SCOUT-O3 Stratosphere-Climate Links with Emphasis on the Upper

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							                SCOUT-O3

 Stratosphere-Climate Links with
Emphasis on the Upper Troposphere
     and Lower Stratosphere
     Publishable Executive Summary - Final draft




                  European Commission
             Framework 6 Integrated Project
                Thematic Priority 1.1.6.3
                 505390-GOCE-CT-2004
              1 May 2004 to 31 August 2009
     Contact

     Prof. J.A. Pyle & Dr N.R.P. Harris
     European Ozone Research Coordinating Unit
     Department of Chemistry
     University of Cambridge
     Lensfield Road
     Cambridge CB2 1EW
     United Kingdom

     Email: Neil.Harris@ozone-sec.ch.cam.ac.uk

     Web: www.ozone-sec.ch.cam.ac.uk


     Design

     Rebecca Penkett
     Marina Tselepi
     Neil Harris


     Acknowledgements

     Many people particiapted in the SCOUT-3 project and they all contributed indirectly to this project summary.
     They are too numerous to mention, but we would like to acknowledge their contributions and thank them for
     it. Here we thank those who contributed directly to the preparation of this summary, namely,

     Alkis Bais, Peter Braesicke, Geir Braathen, Martyn Chipperfield, Thierry Corti, John Crowley, Martin
     Dameris, Andreas Engel, Veronika Eyring, AnnMari Fjaeraa, Peter Haynes, Scott Hosking, Jussi Kaurola,
     Rigel Kivi, Ulrike Langematz, Robert MacKenzie, Virginie Marecal, Hermann Oelhaf, Yvan Orsolini, Thomas
     Peter, Jean-Pierre Pommereau, Thomas Reddmann, Markus Rex, Maria Russo, Cornelius Schiller, Gunther
     Seckmeyer, Harjinder Sembhi, Peter Siegmund, Björn-Martin Sinnhuber, Harry Slaper, Gabi Stiller, Bill
     Sturges, Mark Weber, Jason Williams, ABC, AEMET, DLR, FZJ and FZK.




ii
                                               Preface


The discovery of the Antarctic ‘ozone hole’, nearly 25 years ago, provided confirmation of a major
environmental issue: chlorine- and bromine-containing compounds, with many industrial and domestic uses,
were implicated in the destruction of stratospheric ozone. This discovery led to the Montreal Protocol,
which has become a model for how scientific understanding can contribute to environmental regulation.

European scientists, funded in a series of national and EU research programmes, responded to the developing
scientific challenges. In particular, coordinated, collaborative action, through a number of EU field campaigns,
showed that ozone was also being depleted in the Arctic, and subsequently described the processes by which
middle latitude decreases in ozone, and impacts on UV, were occurring. One of the major successes of this
period was the development of a coherent European stratospheric science community which continues to
play a major role in international science and international assessment for policy.

Europe has also led the developing science agenda into the area of chemistry/climate interactions as scientists
turn their attention to the evolution of the ozone layer during the coming century. This overarching issue is
the major focus of SCOUT-O3, which has involved laboratory, field measurement and modelling scientists.
Major international initiatives have included field campaigns in the tropics and a leading contribution to
international modelling programmes.

70 institutional partners, and more than 400 scientists, have contributed to the SCOUT-O3 project. Thus
far, over 350 scientific papers have been produced, with many more to follow. SCOUT-O3 results, and
scientists, will play a central role in the upcoming WMO/UNEP assessment on the state of the ozone layer.
The EU contribution of 15M€ provided crucial leverage with more than twice this amount coming from
national funding agencies, emphasising SCOUT-O3’s role in bringing together a pan-European community
of scientists. More importantly, the SCOUT-O3 heritage includes a European science community committed
to excellence through collaboration. These are achievements of which we are very proud.

                                     John Pyle, SCOUT-O3 Coordinator
                                              November 2009




                                                                                                                  1
2
                                  Table of Contents


SCOUT-O3 Rationale and Approach                                                4
Laboratory Measurements                                                        6
Observing the Atmosphere                                                       8
Atmospheric Models                                                             10
Coordinated Activity 1: Darwin Campaign                                        12
Coordinated Activity 2: Understanding Clouds, Aerosols and UV                  13
Coordinated Activity 3: SCOUT-O3 / AMMA Campaign                               14
Coordinated Activity 4: SPARC / CCMVal                                         15
Meeting the Objectives                                                         16
Objective 1: Transport Through the Tropical Tropopause Layer (TTL)             18
Objective 2: Clouds in the Tropical Upper Troposphere and Lower Stratosphere   20
Objective 3: Understanding Stratospheric Water Vapour                          22
Objective 4: Stratospheric Aerosol Layer                                       24
Objective 5: Past Surface UV Changes, Variability and Trends                   26
Objective 6: Ozone at Mid-Latitudes                                            28
Objective 7: Polar Ozone in a Changing Atmosphere                              30
Objective 8: The Brewer-Dobson Circulation                                     32
Objective 9: Stratosphere-Troposphere Coupling: Past and Future                34
Objective 10: Predictions of Ozone Recovery on Surface UV                      36
The World Avoided by the Montreal Protocol                                     38
Future Directions for Stratospheric Research                                   40
Data Policy and Database                                                       41
Dissemination, Outreach and Human Capital                                      43
List of Organisations involved with SCOUT-O3                                   46




                                                                                    3
                 SCOUT-O3: Rationale and Approach


                                                    Rationale

    The rationale for the SCOUT-O3 project is to provide scientific knowledge for global assessments on ozone
    depletion and climate change for the Montreal and Kyoto Protocols. European countries and the European
    Union have a responsibility under: the Montreal protocol of the Vienna Convention; the UN Framework
    Convention on Climate Change; and the Kyoto Protocol. The Montreal Protocol has successfully reduced
    emissions and atmospheric concentrations of chloroflorocarbons (CFCs), which are estimated to return to
    their pre-ozone hole concentrations by about 2050. The Kyoto Protocol was the first international measure
    to put a restraint on the galloping rise of carbon dioxide (CO2) emissions caused by industialised nations.

    However, the ozone layer is unlikely to return to its pre-ozone hole state by 2050 and so the remaining
    central question for the Montreal process is: “How and when will ozone and UV radiation recover as CFC
    concentrations fall?”. The answer is required in order to provide essential advice to policy makers in Europe
    and world-wide.

    Such scientific knowledge about the state of the atmosphere and the processes that govern it constitutes the
    basis for political negotiations and decisions concerning the phase-out of ozone depleting substances and
    greenhouse gases emission limits. SCOUT-O3 has contributed to this knowledge, which is necessary to
    formulate a sound environmental protection policy. The improvement of computer models (a central goal
    of the project) is necessary for the prediction of future ozone loss. Such predictions have implications for
    international policies on the phase-out of ozone depleting substances.

    Results from SCOUT-O3 have formed important European input to international assessments, such as the
    Intergovernmental Panel on Climate Change (IPCC), whose fourth assessment report came out in 2007.
    More direct input was made to the IPCC/TEAP report on ‘Safeguarding the ozone layer and the global
    climate system’ in 2005 and to the UNEP/World Meteorolgical Organisation Scientific Assessment of
    Ozone Depletion in 2006. SCOUT-O3 and SCOUT-O3 scientists are also making major contributions to its
    successor which is due out in 2010.




4
              SCOUT-O3: Rationale and Approach


                                        The SCOUT-O3 Approach

The central aim in SCOUT-O3 was to analyse and predict the current status and future evolution of the
ozone layer and surface ultra violet levels with increased confidence. SCOUT-O3 scientists developed and
implemented a science plan which covered the most important component issues. Central to this was the
integration of understanding gained from new and existing measurements using a variety of models operating
on all spatial scales. Doing the job properly requires, for example, knowledge of dramatic individual
thunderstorms extending perhaps 50-100 km for a few hours, as well as the more subtle, hard to define
aspects of the overall atmospheric circulation taking place over the whole globe over many years.

Better understanding of processes in the upper troposphere and lower stratosphere (UTLS) has been
achieved through modelling and data analysis, and studies of the long-term variability in extratropical large
scale transport have been made to improve long-term predictions of mid- and high latitude ozone and ultra
violet. Knowledge about the past and present variability in ultra violet radiation has been improved using
re-evaluated and quality controlled data sets. These have been complemented by focused studies involving
measurements and modelling and used to improve understanding of how clouds and aerosols modify
atmospheric radiation.

Our appreciation of the wide-ranging importance of chemistry/climate feedbacks developed considerably
during the last decade. This is now seen as a crucial component of the ‘earth system’ and one where
further progress is essential for successful prognoses of the future development of the system. SCOUT-
O3 has made a major contribution to global change studies by concentrating on these chemistry/climate
issues. A comprehensive range of scenarios were used in chemistry climate models to provide the basis for
comprehensive studies of the evolution and feedback of the coupled chemistry/climate system.

Lack of knowledge about the tropical stratosphere and upper troposphere, a crucial region when making
predictions, was addressed through tropical field campaigns involving aircraft and balloons which investigated
detailed mechanisms by which air passes from the troposphere to the stratosphere. New fundamental
information about chemical and microphysical processes gained from laboratory studies have been used
in atmospheric models to interpret the measurements of the atmosphere. Understanding of the larger scale
importance is gained through analysis of satellite measurements (e.g. from ENVISAT and CALIPSO),
meteorological analyses and other global fields.

In order to address the central question, 10 scientific objectives were defined which served as a basis for the
science plan. The significant progress made on each objective is reported in the core of this summary and is
complemented by descriptions of how the laboratory, modelling and field measurements were combined in
an integrated way.

SCOUT-O3 has involved the research efforts of 70 partners with more than 100 scientific groups, and it has
taken full advantage of new and existing research facilities developed at a national level. In the next few
pages, prior to discussing the progress made, we give examples of how this large group of scientists have
collaborated to provide real advances in ths area.




                                                                                                                5
                              Laboratory Measurements


               Mimicking the Atmosphere                             The Reaction of HO2 with NO:
                                                                   A New Route to HNO3 Formation
    The behaviour and abundance of trace gases in the
    atmosphere can only be fundamentally understood        The reaction of HO2 with NO (both radicals) has
    by examining the molecular properties of the gases     traditionally been assumed to result in the formation
    concerned. How stable are they? How fast do they       of OH and NO2 (pathway A), the oxidation of NO
    react with other gases? Are they easily adsorbed       to NO2 being an important step in photochemical
    onto particles? Do they react with or on particles?    ozone production. By using a novel “turbulent-
    Similarly, under what conditions do particles form     flow” reactor coupled to a highly sensitive mass
    and evaporate? The answers to these questions          spectrometer, laboratory work in SCOUT-O3
    can only be found by detailed laboratory studies of    has however shown that a small fraction of this
    individual processes. The focus of SCOUT-O3 on         reaction results in generation of nitric acid (HNO3)
    the cold tropopause region has thrown up a great       as written below (pathway B):
    challenge for laboratory work to produce high
    quality datasets within a robust physical/chemical
    framework at temperatures as low as -80ºC.                  HO2 + NO 4           OH + NO2              (A)
                                                                         4           HNO3                  (B)
    Laboratory data enable us to produce accurate
    and transferable parameterisations for use in              The two reaction pathways: B is recently
    models describing this part of the atmosphere.             discovered and takes place just a few
    The laboratory work has covered several aspects            percent of the time.
    of atmospheric chemistry and physics with major
    foci on:
                                                           In pathway B, two radicals are converted to a long
    • gas-phase reactions that generate and remove         lived “reservoir” species, HNO3. Previous studies
      reactive radicals and thus impact on lifetimes       of this reaction were not sensitive enough to
      and abundance of climate gases such as               detect HNO3 as the fraction of reactive collisions
      methane;                                             between HO2 and NO that leads to HNO3 is small
    • the removal of traces gases via interaction with
      cirrus clouds; and
    • the occurrence, properties and persistence of
      cirrus clouds.

    Trace gases from several chemical families have
    been investigated including oxidised organics
    (especially ketones, which are photochemical
    sources of radicals) and inorganic acids (especially
    nitric acid, a major reservoir of radicals). Some
    highlights of the research results are outlined
    below.


                                                                 Cirrus are thin ice clouds that form at altitudes
                                                                    of 7-17 km on existing aerosol particles.




6
(generally less than 1%) and depends on the overall
pressure, humidity and temperature. SCOUT-O3
modelling studies (see Atmospheric Models) show
that the formation of HNO3 even at low yield has
a profound impact on the radical budget of the
tropopause region.


The Interaction of Trace Gases with Cirrus Ice:
  Partitioning between Gas and Ice Phases

Cirrus (ice cloud) coverage in the tropopause
region is high and the ice particles may provide
reactive surfaces for trace gas removal in this part
of the atmosphere. Results on heterogeneous
ice chemistry from SCOUT-O3 have revealed a
strong dependence of the strength of trace gas /
ice interactions on the properties of the trace gas.
Whereas ketones (e.g. acetone) and aldehydes are
weakly associated with ice surfaces, organic (e.g.
acetic) and inorganic acids such as HONO, H2O2
and HNO3 interact strongly.
                                                             The AIDA atmospheric simulation chamber at
For many species a simple empirical relationship        Forschungzentrum Karslruhe can be cooled to low enough
between vapour pressure and ice affinity can be            temperatures (-80ºC!) that “cirrus clouds” can form.
found. The laboratory work shows that nitric acid
(HNO3) has an exceptionally large affinity for ice,      that form at altitudes of 7-17 km. The ice particles
the interaction being associated not only with the      can contain mineral dust arising from deserts
surface but also involving underlying layers of the     and organics originating from natural as well as
bulk ice sample. In order to reconcile laboratory       anthropogenic emissions. One focus of laboratory
findings with field observations a model has been         work within SCOUT-O3 was the investigation
developed that describes the “trapping” of HNO3         of how these different types of aerosol particles
in a growing ice particle under conditions pertinent    affect the ice formation processes. For example,
to the tropopause region. The model captures the        various forms of mineral dust particles facilitate
observed, almost complete HNO3 transfer from the        the formation of ice, while some organics, in
gas to ice phase at sufficiently cold temperatures.      particular the larger water soluble molecules,
                                                        inhibit ice formation, because they become
                                                        “gooey” at the very low temperatures below
 The Formation of Cirrus Ice Clouds: Role of            –70ºC. The laboratory studies were designed to
   Heterogeneous Ice Nuclei and Organics                produce parameterizations for use in atmospheric
                                                        cloud models. The experimental techniques that
The accurate representation of cirrus clouds in         were used range from studies of individual cloud
atmospheric models requires knowledge of the            droplets ~1/100 of a millimetre in size to millions
processes governing their formation, properties         of droplets in chambers several stories high.
and lifetimes. Cirrus clouds consist of ice particles



                                                                                                                 7
                           Observing the Atmosphere


                   Background                          The observing stations in NDACC are global and
                                                       European scientists and institutions make a major
Atmospheric measurements have often led the            contribution (e.g. through the EC GEOMON
way in developing new understanding of the             project). The sites range from the tropics to the
fundamental phenomena - and sometimes even             high latitudes in both hemispheres.
their existence. For example the existence of the
Brewer-Dobson circulation was first suggested by        The scientific aims of NDACC, which align very
measurements of water vapour on high altitude          well with those of SCOUT-O3, are:
aircraft in the 1940s, while the ozone hole was first
                                                       • detecting trends in atmospheric composition;
observed as a result of careful observations being
made in harsh conditions for nearly 30 years.          • studying atmospheric composition variability
                                                         at interannual and longer timescales;
Nowadays, atmospheric observations fall into
three main, complementary categories:                  • establishing links and feedbacks between
                                                         climate change and atmospheric composition;
• long-term measurements;
                                                       • calibrating and validating space-based
• intensive field campaigns;                              measurements of the atmosphere;
• global views from satellites.                        • supporting process-focused scientific field
                                                         campaigns, and
All three types of measurement were involved in
SCOUT-O3.                                              • testing and improving theoretical models of
                                                         the atmosphere.

            Long term Measurements                     There is a paucity of sites in the Tropics and sub-
                                                       tropics, with only 7 sites between 30ºS and 30ºN
The long-term measurements in SCOUT-O3 were            whose area is half the Earth’s surface. One of these,
centred around the Network for the Detection of        at Izaña on Tenerife, opened in 1916 following
Atmosphere Composition Change (NDACC)                  many years of sporadic scientific visits to Tenerife
whose goal is to obtain high quality measurements      including by Darwin and von Humboldt. The
of a broad range of atmospheric chemical species       intensity of measurements picked up in the 1980s
and parameters.                                        and Izaña joined the WMO’s Global Atmospheric
                                                       Watch when it formed in 1989.




8
          Global Views from Satellites                 in the tropical UTLS meant there were real
                                                       opportunities to make new discoveries. In total, 6
The first systematic observations of the Earth’s        field campaigns were organised in SCOUT-O3.
atmosphere by instruments carried on orbiting
satellites started in the late 1960s. Over the years   1. Darwin, Australia, Nov/Dec 2005. Scientists
the capabilities of the instruments have improved      investigated the influence of the strong tropical
enormously, and measurements of the upper              convection on the UTLS using several aircraft.
atmosphere and the Earth’s surface are now of          2. Thessaloniki, Greece, Aug 2006. The interaction
high quality. The upper troposphere and lower          of clouds and aerosol with UV radiation was studied
stratosphere is one of the harder altitude ranges      using aircraft and ground-based instruments.
to observe reliably as there is a lot of atmosphere
above it to look though and strong, complicating       3. Niamey, Niger, Aug/Sept 2006. In collaboration
features such as clouds below and even in it.          with AMMA, the effect of the West African
Since 2000 the ESA Envisat, NASA AURA and              Monsoon on the UTLS was observed with aircraft,
SSC ODIN (below) satellites were launched with         balloons and ground stations.
instruments designed for observing the UTLS.           4. Mahé, Seychelles, Jan/ Feb 2008. Long duration
                                                       balloons capable of carrying instruments in the
In SCOUT-O3 measurements from instruments on           stratosphere were launched.
the satellites, particularly ENVISAT and ODIN,
have been assessed for their quality and used to       5. Teresina, Brazil, June 2005 and June 2008. Large
study of the global and regional variations of many    research balloons were launched with payloads
trace species in the UTLS. The measurements are        which made detailed atmospheric observations
valuable in comparing with the global atmospheric      and validated ESA satellite measurements.
models and providing the large-scale context for
long-term measurements and field campaigns.




         Intensive Field Measurements                  6. Niamey, Niger, Aug 2008. A second campaign
                                                       involving lightweight instruments and small
Field measurement campaigns are invaluable             balloons was organised to look more at the effect
as they allow detailed investigation of critical       of the West African Monsoon on the UTLS.
atmospheric processes. They were the central
experimental activity within SCOUT-O3, with            The measurements from all these campaigns
airborne and balloon-borne measurements in             are being interpreted using other available data
the UTLS focussed on chemical, microphysical,          (e.g. satellite measurements and meteorological
transport and radiative processes in tropical          analyses) as well as SCOUT-O3 models.
regions. The shortage of previous measurements



                                                                                                             9
                                      Atmospheric Models


              What are Atmospheric Models?                  importance for recycling OH and NO2, can also
                                                            follow a reaction pathway which produces nitric
     Our understanding of atmospheric processes is          acid (see Laboratory Measurements).           This
     often encapsulated in numerical models, which          pathway was previously unknown but modelling
     are simply mathematical descriptions of the            studies by SCOUT-O3 scientists showed that,
     atmospheric system formulated on a computer.           although the pathway is followed in only a
     Because the atmosphere is so complex, different        small fraction of the reactions, its importance
     types of model have been developed for different       for atmospheric chemistry is nevertheless very
     uses. Some models contain detailed descriptions        large. The figure shows the change in OH and
     of the chemical processes, e.g. in an isolated         ozone when the reaction is included. The impact
     parcel of air, while others attempt to model the       on the model fields is large, approaching 60% for
     whole of the atmosphere, including all the climate     OH and more than 20% for ozone. Modelling
     and chemistry processes. They can simplify the         has highlighted the imporantance of this reaction.
     atmospheric system, for example, by specifying the     Further investigation of this reaction in modelling
     observed meteorological conditions and focussing       and laboratory studies is merited.
     just on chemical change. Other models attempt
     to model just a local measurement or a local
     process: some of the modelling which supported
     the SCOUT-O3 field measurement campaigns in
     Australia, Africa and South America falls into this
     category. Finally models can be used to study
     how the atmosphere might change in the future:
     chemistry-climate models capable of modelling
     how changes in climate affect atmospheric
     composition particularly in the stratosphere. In
     SCOUT-O3 these are used to investigate how
     the ozone layer is affected by the reductions in
     emissions of ozone-depleting substances and by
     climate change.

     We give examples of these different uses below.


             Including the Latest Information
                   from the Laboratory

     A major objective of SCOUT-O3 was to improve
     our chemistry-climate models. One way of doing
     this is to ensure that the best available laboratory
     data on atmospheric chemical (e.g. reaction
     pathways and rates) and physical processes (e.g.
     properties of atmospheric particles) was included
     in our models. Thus, work by laboratory chemists
     within SCOUT-O3 showed that the reaction of
     HO2 + NO, long known to be of atmospheric



10
            Comparing Models with                          Improving Chemistry-Climate Models
           Atmospheric Observations
                                                      Our improved chemistry-climate models have
A second way in which the models were improved        been used to study how the ozone layer will
was by comparison with atmospheric data. The          recover (and what will be the subsequent impact
concerted collection of data in our various           on surface UV) following further phase-out of
field campaigns was an important part of this          ozone depleting substances. The figure below
exercise. A major SCOUT-O3 research question          gives one example, demonstrating that ‘recovery’
was whether our models represent accurately the       depends not just on the future abundances of the
transport of species from the troposphere to the      ozone depleting substances (ODS) but also on
stratosphere and, especially, whether transport       greenhouse gas concentrations.
through the tropical tropopause, the major path
from troposphere to stratosphere, is treated well.
Air parcel trajectory models, mesoscale models
and global models were used to address these
questions.

One approach was to characterise in detail
the behaviour of the tropical tropopause in
our numerical models. How much transport
occurs through the region and in which specific
directions? Are there important spatial and
temporal differences? Other modelling studies         The variation of tropical and Antartic ozone has
tried to reproduce the aircraft and balloon data      been calculated in a SCOUT-O3 chemistry-climate
collected in tropical field campaigns.                 model. The model reproduces the observed decline
                                                      in ozone and then shows a gradual recovery during
                                                      the 21st century. The increase in greenhouse gas
                                                      concentrations causes the stratosphere to cool
                                                      which slows down the rate of ozone-destroying
                                                      reactions and, hence, leads to a faster recovery of
                                                      the ozone layer.

                                                      Chemistry-climate models can be used to study
                                                      a range of scenarios. In the ‘World Avoided’
                                                      section we show how models are used to address
                                                      what might have happened without the Montreal
                                                      Protocol.



The figure shows an idealized study of the transport
of a gas (this could represent one of the natural
halogen species which are believed to be emitted
by the tropical ocean) emitted in the tropics and
lifted towards the stratosphere.



                                                                                                            11
                                  Coordinated Activity 1:
                                    Darwin Campaign

                  Chasing Hector –                          The campaign was based at the Royal Australian
          The SCOUT-O3 Airborne Experiment                  Air Force base in Darwin in November and
                                                            December 2005. European scientists performed
      The Tropics is the main region where air enters the   extensive measurements of chemical species, of
     stratosphere. An important step is upward transport    aerosol properties and of cloud ice particles from
     into the upper troposphere and occasionally the        the high-flying M-55 Geophysica and the DLR
     lower stratosphere in huge tropical thunderstorms.     Falcon jet. Together with the two aircraft of the
     These are particularly prominent over Indonesia,       UK ACTIVE project and a Swiss Learjet, these
     Micronesia and northern Australia, where strong        activities formed the first phase of the “Tropical
     convection occurs most frequently.                     Warm Pool International Cloud Experiment (TWP-
                                                            ICE)”, which was hosted by the Australian Bureau
     The first campaign in SCOUT-O3 investigated a           of Meteorology and ran from November 2005 to
     storm system called Hector, which occurs almost        February 2006. TWP-ICE involved scientists
     daily during November and December over the            from Australia, Europe, Russia and the USA. The
     Tiwi Islands north of Darwin, Australia (11ºS,         campaign attracted a good deal of press interest
     131ºE). Intense Hectors reach to altitudes of up       and featured in documentaries in Germany and
     to 20 km, clearly in the lower stratosphere. The       Australia as well as numerous press articles.
     regularity and distinctness of Hector mean that
     they have the potential to be studied in isolation.
     Measurements at the bottom and the top give a
     chance to see how quickly and how much travels
     up from the ground.




                                                            The Geophysica left its mark after flying above the
                                                            top of a dissipating Hector. Care had to be taken to
                                                            avoid confusing the Geophysica’s contrail with air

     On 30 November 2005 instruments on the
     Geophysica measured ice particles in the
     stratosphere up to at least the aircraft altitude.
     In this case, “geysers” of ice stretch 600-700 m
     into the stratosphere, seemingly connected to
     the thunderstorm underneath. Other instruments
     confirmed the presence of ice in the stratosphere
     when the aircraft flew through the top of the
     “geysers”.



12
                   Coordinated Activity 2:
            Understanding Clouds, Aerosols and UV

      Thessaloniki Measurement Campaign

Atmospheric particles (aerosols and clouds)
strongly influence the amount of solar radiation
reaching the Earth’s surface.          However, a
quantitative description of how clouds and
aerosols change incoming UV radiation remain
elusive. SCOUT-O3 scientists organised a field
measurement campaign in northern Greece to
examine this in detail. Measurements of spectral
UV radiation, particle concentration, ozone and
other important atmospheric parameters were made
at a network of ground sites and on two aircraft
during two weeks in August 2006, using state of                          Ground instruments used to measure aerosol optical
the art instrumentation. The aircraft measurements                                properties and UV radiation at
                                                                              the Aristotle University of Thessaloniki.
were used to determine the variations of aerosol
optical and physical properties over the wider area
and at different altitudes. New instruments and                      day-to-day aerosol variability which caused
methods for measuring accurately the intensity                       differences in UV radiation of up to 30%.
of UV radiation from the sky were used and were
compared to each other, revealing challenging                        Measurements from the campaign have been
issues to be considered in future.                                   used in conjunction with numerical models
                                                                     describing the propagation of radiation through
The airborne measurements revealed large                             the atmosphere to investigate quantitatively
variability of the aerosols over the wider area and                  the influences of aerosols on various radiative
at different altitudes, both with respect to their                   quantities. Good agreement within the uncertainty
physical and optical properties. However within                      limits has been achieved amongst single scattering
the city the spatial aerosol variations were small,                  albedo retrievals from airborne measurements and
caused by effective mixing of air in the atmospheric                 from the combination of photometric and LIDAR
layer below ~1 km, and showed a marked diurnal                       measurements.
pattern. The ground measurements showed large

                                                                                Advanced 3D model calculations have
                                                                                been used to simulate the polarization of
                                                                                solar radiation by atmospheric particles.
                                                                                By combining model calculations with
                                                                                the measured optical properties of
                                                                                aerosols, vertically resolved properties
                                                                                of aerosols were retrieved. This
                                                                                information can be used in radiation
 Aerosols and clouds up to 3 km detected by the downward-looking Lidar          modelling to improve the accuracy of
   onboard the CESSNA aircraft. Two thin cloud layers in about 3.1 km           UV radiation simulations.
 and 2.5 km were observed during the whole observation period (orange),
 aerosol structures were also visible at 1.5 km over certain areas (green).




                                                                                                                              13
                            Coordinated Activity 3:
                         SCOUT-O3 / AMMA Campaign

                The West African Monsoon                    the effects of intense mesoscale convective systems
                                                            on the upper troposphere and lower stratosphere.
     In July and August 2006 two EU FP6 Integrated          Five scientific flights were successfully carried
     Projects, SCOUT-O3 and AMMA, cooperated in             out on site, and four transfer flights allowed a
     a field measurement campaign investigating the          characterization of the tropopause region along
     effect of the West African Monsoon. The SCOUT-         a latitudinal transect from southern Europe to
     O3 emphasis was on the upper troposphere and           West Africa. These flights were carried out in
     lower stratosphere, while AMMA focussed more on        conjunction with flights of the DLR Falcon. In
     the lower atmosphere including assessing weather       total 7 research balloon flights and 29 lightweight
     forecasting ability, air quality and the impact on     soundings were made at Niamey airport, as well
     disease and agriculture. Overall the campaign          as three low to mid level aircraft in AMMA. The
     involved 5 aircraft, balloons and a network of         research focussed on water vapour transport and
     ground-based measurements.           Of particular     on high altitude clouds. Some balloon experiments
     interest to SCOUT-O3, the M55 Geophysica and           were damaged because of the very difficult
     the DLR Falcon were based at Ouagadougou in            conditions for recovery in a flood region.




     Burkina-Faso, and the research balloons based          The campaign activities, not originally planned
     400 km away at Niamey in Niger.                        in SCOUT-O3, were mainly funded by national
                                                            institutions and exploited scientific and logistic
     The M55 Geophysica flights aimed at a better            infrastructures provided by the EC SCOUT-O3 and
     understanding of the impact of the upward              AMMA projects. This was an excellent example
     transport and redistribution of water, aerosol, dust   of scientific cooperation within Europe as well as
     and chemical species, at assessing the effect of       with the partners in several W. African countries.
     lightning on the NOx production, and at studying




14
                            Coordinated Activity 4:
                           How good are the models?

                    Background                           CCMs represent physical, chemical, and dynamical
                                                         processes. An important element is to understand
When using an atmospheric model for scientific            the ability of CCMs to reproduce past trends and
studies, it is important to know how well it             variability.
performs, especially if the results are used to
inform policymakers – models should always be            The CCMVal activity helps to coordinate CCM
used with their strengths and weaknesses in mind.        model efforts around the world. In this way,
The interaction between the stratosphere and             the CCM community can provide the maximum
climate change is complex, and so a major effort         amount of useful scientific information for
in SCOUT-O3 was to test the models against               the WMO/UNEP and IPCC assessments by
observations and against each other. This effort         developing and maintaining evaluation tools for
involved several different types of model, but a         the models, defining boundary conditions for
particular emphasis was put on the chemistry-            “scenario” experiments, and archiving output
climate models (CCMs) used to simulate the               data from the models. It is currently preparing
effects of different future scenarios as these studies   a report assessing CCM performance which will
require extrapolation from current conditions. This      provide an excellent basis for the UNEP/WMO
work has been based around the participation of          Assessment in 2010. The role CCMVal and other
the SCOUT-O3 CCMs in the international SPARC             SPARC initiatives play in supporting international
CCMVal initiative.                                       Assessments underlies their importance and the
                                                         need to be international themselves.

                 SPARC CCMVal                            The success of such initiatives depends on whether
                                                         individual scientists benefit and get involved.
The goal of CCMVal is to improve understanding           Many SCOUT-O3 scientists have participated
of CCMs by concentrating on specific processes            in CCMVal since its inception with individuals
that are important in determining critical aspects       playing leading roles in its organisation. Three
of the model performance such as Arctic and              workshops were held during SCOUT-O3. 9
Antarctic ozone loss and the Brewer-Dobson               modelling groups are participating through the
Circulation. It also provides a forum for discussion     inclusion of results from their CCM and experts in
and coordinated analysis of science results. One         the collection and analysis of observations provide
outcome has been improvements in how well                the all-important measures to compare with.




                                                                                                               15
       Meeting the Objectives




     Links between SCOUT-O3 Objectives and Activities




16
                             Meeting the Objectives


                                         The Scientific Objectives

In order to address the central aim of SCOUT-O3, ten scientific objectives were identified which served as
the basis for the science plan. These were used to define the organisational structure which consisted of six
scientific and two supporting Activities (see SCOUT-O3 Approach). These are not discussed here as we
want to keep the emphasis on the results rather than the means used to achieve them.


    1. Determination of air residence times in the tropical tropopause layer and assessment of the
       transport of very short-lived ozone-depleting substances through the tropical tropopause layer;

    2. The influence of clouds on the tropical upper troposphere and lower stratosphere;

    3. Understanding the stratospheric water vapour trend and its consequences;

    4. The stratospheric aerosol layer - role of the tropical tropopause layer and possible tropical
       tropopause layer changes;

    5. Past ultraviolet (UV) changes, variability and trends – Improved understanding of UV
       modulation by aerosols and clouds;

    6. Ozone variability and past changes at mid-latitudes;

    7. Interannual variability in polar processes and likely changes in a changing atmosphere;

    8. Improved understanding of the Brewer-Dobson and general stratospheric circulation;

    9. Stratosphere / troposphere coupling - past and future; and

    10. Predictions, based on a new generation of chemistry climate models, to consider (a) ozone
        recovery, (b) the effect of climate change on the recovery, and (c) the impact of the ozone
        change on surface UV




                                                                                                               17
                                               Objective 1:


                          Interest                          kilometers around the globe. Alternatively the very
                                                            strongest thunderstorms can carry air directly into
     The large-scale circulation in the stratosphere        the stratosphere, but the extent to which this can
     is upwards in the tropics and downwards in the         happen is not well known. Two aims in SCOUT-
     extratropics. Air therefore enters the stratosphere    O3 were to (a) quantify the relative importance
     predominantly in the tropics, with the tropical        of these two routes in determining stratospheric
     upper troposphere, now often known as the              composition and (b) provide good estimates of
     Tropical Tropopause Layer (TTL), therefore acting      how long air takes to pass through the Tropical
     as a ‘gateway’ to the stratosphere. Relatively few     Tropopause Layer.
     detailed measurements have been made in the
     TTL region, leaving many open questions. One of
     these is how chemical compounds are transported                             Approach
     from the Earth’s surface into the stratosphere.
     Of particular interest are the very short-lived        Unravelling the different factors that influence how
     substances (VSLS) such as bromoform which              different gases reach the stratosphere is a complex
     could potentially be making an increasingly large      problem. It involves atmospheric processes from
     contribution to the stratospheric bromine amount.      the local (individual thunderstorms) to the global
                                                            scale which operate on timescales from a few
                                                            hours to months and even years. The methods
                                                            used in SCOUT-O3 were:
                                                            • detailed measurements of trace gases lofted by
                                                              convective systems using aircraft and balloons
                                                              in S. America, N. Australia and W. Africa;
                                                            • development and use of models covering local
                                                              areas and scaling up to global models;
                                                            • analysis of satellite measurements to infer
                                                              global patterns; and
                                                            • calculations of uplift in the tropical UTLS
     The quantity of VSLS which reaches the
                                                              using the latest meteorological data.
     stratosphere is affected by a range of chemical and
     meteorological factors. The bottom line is that
                                                            The work on tropical transport has been closely
     they must reach the stratosphere within a few days
                                                            linked with the SCOUT-O3 chemistry-climate
     or weeks of their release into the atmosphere as
                                                            models (e.g. through the SPARC CCMVal
     they will otherwise be removed through oxidation
                                                            initiative) in order to improve their representation of
     and rain-out. Uplift in strong convection is one
                                                            the composition of air entering the stratosphere.
     possibility for this. While most tropical convection
     carries large volumes or air up to 12 km or so,
     most of this will subsequently descend. To reach
                                                                                  Findings
     the stratosphere, air must be taken up in strong
     convective storms to above about 14 km. From
                                                            Many individual studies of transport through the
     here it can be taken up into the stratosphere by
                                                            TTL were made in SCOUT-O3 and only a few
     slower vertical transport, perhaps taking several
                                                            examples can be highlighted here.
     weeks during which time it can travel thousands of



18
   Through the Tropical Tropopause Layer (TTL)


Importance of Convection                                measurements. As such they provide as direct a
The strongest evidence for the injection of air into    comparison as possible with field measurements.
the stratosphere during convective events comes
from in situ measurements of water vapour and
particles. The signatures of local injection of
trace gases such as CO or O3 is harder to identify
in large part because of the influence of air from
further away. It is thus hard to quantify how much
air is injected through strong convective events.




On a larger scale, analysis of satellite measurements   The comparisons (here shown for CO observed
provides stronger evidence for the seasonal             during a flight in the SCOUT-O3 Darwin campaign
importance of strong convection over central Africa     for two CCMs and two other global models) are
during March to May, earlier than and to the south      surprisingly good. The models cannot be expected
of the campaigns in July to September. These            to reproduce all the fine scale structure as their
results are intriguing as they are not explicable       resolution is much coarser, and these results are very
using the best available meteorological data.           encouraging. Complementary work comparing
                                                        SCOUT-O3 and other models with other data is
Measurements around thunderstorms have better           being carried out in SPARC CCMVal and overall
quantified the production rate of nitrogen oxides in     the effect will be a significant improvement in how
tropical storms. Such information was relatively        convection is represented in the models.
sparse previously and it is important because
thunderstorms are one of the natural sources to         Residence Time of Air in the TTL
compare with the emissions from aircraft.               The latest meteorological reanalyses (see
                                                        Objective 3) have been used to provide better
Comparison with CCMs and Other Models                   estimates of how long it takes for air to rise into
A major aim in the latter part of SCOUT-O3 has          the stratosphere from where it emerges from
been to improve the models using the available          convective clouds. These estimates are valuable
measurements. A particular focus has been how           in assessing how much chemical removal of VSLS
models represent transport in convection as they        can take place in air being transported up in this
struggle to provide realistic estimates of the future   way. When coupled with in situ measurements of
input of air into the stratosphere. The trace gas       bromine compounds from aircraft and balloons,
measurements from the field campaigns have been          they provide some useful constraints on the
compared to a range of models, including some           possible global importance of VSLS. Tightening
‘nudged’ CCMs. These models are versions of             these constraints requires further work combining
the CCMs used to look at future scenarios except        both improved estimates of timescales and more
that they are constrained (i.e. nudged) using           precise observations.
meteorological information for the period of the



                                                                                                                 19
                                                 Objective 2:


                           Interest                           TTL on stratospheric ozone. So, SCOUT-O3 set
                                                              itself five goals:
     Clouds are present throughout the Tropics and
     strongly influence the Earth’s energy balance.            • To make measurements of ice clouds and
     They reflect incoming sunlight and absorb                   aerosol particles in the tropical UTLS;
     energy emitted by the underlying land, ocean and         • To carry out laboratory studies of critical
     atmosphere. The processes controlling tropical             processes in ice and aerosol particles;
     cloudiness in a changing climate thus need to be
     understood. Tropical clouds are also critical in         • To undertake computer modelling of ice
     determining how water enters the stratosphere (see         clouds in the tropical UTLS;
     Objective 3) and so influence the ozone layer.            • To assess the role of climate (change) on
                                                                cloudiness in the tropical UTLS; and
                                                              • To produce simple computer modules
                                                                representing the interaction of gases with ice
                                                                particles to improve global climate models.


                                                                                  Findings

                                                              Ice Clouds and Glass Particles
                                                              The tiny aerosol particles that are present in
                                                              the atmosphere promote ice particle formation.
                                                              However, the ability of an aerosol particle to
     The highest clouds in the Tropics are cirrus which       promote ice formation depends very much
     are present at altitudes from 12 to 17 km. About half    on what the particle is made of. Organic
     of them are directly associated with thunderstorms.      compounds make up 60-80% of the mass of
     Humid air is rapidly lofted to high altitudes until      aerosol particles in the upper troposphere where
     the local temperature is low enough that the water       cirrus clouds form; sulfuric acid makes up most
     condenses. Anvils from the top of thunderstorms          of the rest. The organic fraction of the aerosol
     and cirrus clouds often remain as the anvils disperse.   is composed of many different compounds, and
     Most of the thunderstorm remnants occur at about         these mixtures do not crystallise easily. Instead,
     14 km altitude, some 2-3 km below the stratosphere,      they tend to form liquid solutions and non-
     although some very strong storms reach much              crystalline solids (i.e. glasses). Liquids become
     higher (20 km). The rest of the cirrus is produced       very “gooey” (viscous) as temperature decreases:
     by atmospheric motions that lift air more gently.        at 200 K (-73°C) - a temperature typical of the
                                                              upper troposphere - sulfuric acid is about as
                                                              viscous as honey. Organic aerosol particles
                          Approach                            are even more viscous at these temperatures.
                                                              When liquids become so gooey that they act
     To assess how sensitive TTL cloudiness is to             like solids, they have become a glass. During
     climate, it is necessary to understand better the        SCOUT-O3, laboratory work has shown that the
     TTL as it is now. Only then can we quantify the          formation of glassy aerosol particles may have
     feedbacks that control the sensitivity of the TTL        profound effects on ice formation in the upper
     to climate, and assess the impact of clouds in the       troposphere.



20
     Clouds in the tropical upper troposphere and
                  lower stratosphere


Most ice formation in the upper troposphere
comes about by liquid aerosol particles taking up




water as the air cools, until the point is reached
at which ice can form spontaneously in the liquid
particle. If, however, the temperature at which
an aerosol particle turns glassy is higher than the
temperature at which ice formation can occur, then
ice formation will be inhibited.                      decades. As the model is extended in space (i.e.
                                                      from a point in space to 1, 2 and 3D) and time
The Supersaturation Puzzle                            (from hours to decades), the amount of detail about
Another longstanding puzzle connected to              the ice clouds that can be incorporated diminishes.
atmospheric water vapour was the series of in situ    By using a hierarchy of computer models we can
measurements which showed surprisingly large          interpret the observations in detail, and work out
volumes of air where no ice clouds had formed         what is going wrong if the simple ice physics
despite sufficiently low temperatures and high         in the global models misses some part of the
water vapour amounts (supersaturation). While         observed behaviour of the clouds. For example,
this puzzle is still not completely solved, a great   SCOUT-O3 scientists showed that ice is
deal of progress has been made. First, a rigorous     injected into the stratosphere above super-strong
reanalysis of one of the largest available sets of    thunderstorms.
measurements found a reduced incidence of cases
where supersaturation was observed. Second, the       When similar cirrus simulations are carried out
fact that the saturation pressure above glasses is    within climate models, the effect on the Earth’s
greater than above ice (above) might explain some     energy balance can be calculated. This turns out to
of the observed supersaturation (see Objective 2).    be difficult for two reasons: (i) the net effect of ice
                                                      clouds is the relatively small difference between
Simulating Cloudiness                                 the amount of sunlight reflected back to space
SCOUT-O3 has analysed satellite data to provide       and the amount of re-emitted energy absorbed,
global maps of cirrus and aerosol particles. There    and (ii) we don’t have sufficient understanding of
are many new observations with which to compare       the relative importance of different ice formation
computer models and from which, along with the        routes in the upper troposphere. SCOUT-O3 has
laboratory results, to improve those models. The      gone a long way to addressing our uncertainties
computer models of clouds used in SCOUT-O3            about ice-cloudiness, and its impacts, but important
range from relatively simple calculations that        research questions remain.
follow an individual parcel of air, through 3D
simulations that can capture cloud shapes and
properties for a few hours, all the way to global
climate-and-chemistry simulations covering many



                                                                                                               21
                                               Objective 3:


                          Interest                                             Approach

     The stratosphere contains very little water (~5        There are many aspects to understanding water
     parts per million) compared to the troposphere         vapour’s role in the stratosphere, and so a multi-
     (up to a few percent), and the gradient across the     pronged approach has been adopted:
     tropopause is large. There have been vigorous
     discussions about the causes for several decades,      • Studies of the latest re-analysis of historical
     ever since the first stratospheric water vapour           data giving the best picture of the meteorology
     measurements were made in the late 1940s. Air            for the last half century;
     enters the stratosphere in the Tropics where the       • Detailed observations during field
     tropopause is coldest (reaching –90°C), and the low      measurement campaigns in North Australia
     temperatures ‘freeze dry’ the air. However there has     and West Africa;
     not been agreement as to whether this dehydration
     occurs when air is lifted slowly over large areas or   • Process studies using measurements and
     rapidly in large, violent thunderstorms.                 models; and
                                                            • New and improved global measurements from
     Atmospheric measurements indicate that                   satellite instruments.
     stratospheric water vapour concentrations have
     increased. From 1980, when more measurements           The work performed in the approaches has been
     became available, to 2000, stratospheric water         closely integrated with the laboratory work on ice
     vapour increased at a rate of 0.6% per year            particles and the global studies of water vapour
     continuing a previous, though less well observed       using chemistry-climate models.
     trend. In 2000, a sudden drop was identified.
     These are important changes on a global basis and
     need to be understood because of the importance                            Findings
     of water vapour for (a) the radiative balance and
     chemistry of the stratosphere and (b) the feedback     How Water Enters the Stratosphere
     on climate in the troposphere.                         The main factor that determines how much
                                                            water remains in an air parcel which enters the
                                                            stratosphere is the lowest temperature that parcel




                                                             Field work in the Tropics is very
                                                             demanding and frequently means that
                                                             instruments have to be prepared in hot,
                                                             humid conditions (hotter than 30°C, 100%
                                                             relative humidity) in order to make high
                                                             altitude measurements at -90°C in very
                                                             dry air. Here a balloon instrument is
                                                             being prepared in Niamey Airport during




22
       Understanding Stratospheric Water Vapour


experiences. In principle an air parcel could          Recent Changes
pass through the cold tropopause region either         At the start of SCOUT-O3, a great deal of attention
by travelling large distances horizontally while       was being paid to the long-term increase in
rising slowly upward, or in fast upward motion of      stratospheric water vapour. Analyses of satellite
air in, for example, a tropical storm. The latest
meteorological re-analyses are the best current
estimates of the winds, temperatures and other
atmospheric properties for several decades and
can be used to calculate year-to-year variation
of how air moves into the stratosphere, what
temperatures are experienced and the implications
for stratospheric water vapour. These calculations
would be very inaccurate if rapid upward motion
in individual tropical storms was the most
common route into the stratosphere. The excellent
reproduction of the interannual variability in
stratospheric water vapour suggests that most air
                                                       measurements of the past few years shows that
                                                       water vapour was low from 2002-2004, increased
                                                       a little from 2004 onwards, perhaps even reached
                                                       its 2001 value in early 2008. Temperatures at the
                                                       tropical tropopause are broadly consistent with
                                                       these changes. Overall, stratospheric water vapour
enters the stratosphere quasi-horizontally with just   was lower in 2002-2007 than in 1995-2000. This
slow upward movement. In this way it experiences,
and its stratospheric water vapour amount is set
by, the extremely low tropopause temperatures
over the West Pacific.

The Role of Convection
Measurements made in North Australia and in
West Africa show that the super-strong storms
which penetrate into the stratosphere actually
inject water in the form of ice cyrstals that cause
local moistening rather than local drying as was       behaviour appears to be a multi-year dynamical
thought for a long time. It is hard to provide a       variation and there is not compelling evidence of
firm estimate of the global importance of such          any secular trend. It underlines the importance
storms as their size and intensity varies so much      of high quality, long-term measurements and
regionally and seasonally. Preliminary estimates       the value of instrument comparisons such as the
from SCOUT-O3 indicate that the contribution to        SPARC AQUAVIT initiative in which SCOUT-O3
the global stratospheric water vapour budget could     groups are participated.
range from a few percent to a few tens of percent.




                                                                                                             23
                                               Objective 4:


                          Interest                         These have been studied using new in situ
                                                           observations from the tropical field measurement
     Atmospheric aerosol particles are extremely small     campaigns over Australia, Africa and Brazil, as
     solid and liquid particles that play an important     well as remote observations from the lidar onboard
     role in the upper troposphere and the stratosphere.   the CALIPSO US-French satellite.
     They influence the energy budget of the atmosphere
     by scattering incoming solar radiation; they act as   In addition, since the episodic and unpredictable
     condensation nuclei on which cirrus cloud and polar   nature of volcanoes means that their future impact
     stratospheric cloud droplets can form; and they       depends on the halogen loading at the time of the
     provide surfaces for the heterogeneous reactions      eruption, the possible effects of weak and strong
     that play a central role in ozone chemistry.          volcanic eruptions have been assessed in CCMs
                                                           with improved descriptions of the stratospheric
     Most of these aerosol particles result from the       aerosol.
     conversion of gaseous precursor sulphur gases
     (SO2, CS2 and OCS) into sulphuric acid droplets.
     These are particularly enhanced after a major
     volcanic eruption, like that of the Pinatubo in the                        Findings
     Philippines in 1991 which led to low ozone values
     for several years. There have not been any major      Particle composition in the TTL
     volcanoes since Pinatubo and so the stratospheric     The composition of particles in the TTL is important
     aerosol has been relatively unperturbed during        in determining their chemical reactivity and their
     SCOUT-O3. This has confirmed that there is no          ability to grow and/or nucleate cloud particles that
     long-term trend in stratospheric aerosol resulting    can, for example, lead to dehydration of air entering
     from human activities such as aviation. Other         the stratosphere. Particles containing reactive
     classes of aerosol particles include mineral dust     nitrogen have been detected near and below the
     (lofted in storms), sooty smoke from biomass fires     tropopause over Africa by instruments on the M55
     and meteoritic particles. These classes are known     Geophysica. Such nitric acid trihydrate particles
     as non-volatile aerosol particles because — unlike    are similar to the polar stratospheric clouds
     the sulphuric acid droplets — they do not evaporate   forming at low temperature in the Arctic and
     when they are heated to 200°C.                        Antarctic. Satellite observations suggest that they
                                                           might nucleate on ice fed by convective activity.

                         Approach                          Ultra-fine, non-volatile particles have been
                                                           measured in the TTL during the same aircraft
     The main areas of research in SCOUT-O3 are:           flights, with large variations seen near the
     • the fraction of aerosol particles that are non-     tropopause. Though of still unknown nature in the
       volatile,                                           absence of chemical analysis, they are suspected
                                                           to result from deep convection from the boundary
     • the role of the frequent small volcanoes            layer.
       erupting at low altitude;
                                                           Geyser-like injections of ice particles above
     • the convective lifting of mineral dust or smoke
                                                           the tropopause have been observed on several
       and more generally, and
                                                           occasions from aircraft and balloons over land
     • the transport of precursor gases and particles      convective systems. Simultaneous electric field
       into the lower stratosphere.                        measurements on board the same balloon indicate



24
                          Stratospheric Aerosol Layer


                                                           (a) that this plume (as well as a lower altitude one
                                                           from a second volcano, Tavurvur, which erupted
                                                           in October 2006) was then slowly transported
                                                           upward up to 25 km by the Brewer-Dobson
                                                           circulation and (b) that small volcanoes contribute
                                                           to the aerosol load of the mid-stratosphere. These
                                                           measurements also demonstrate the existence of
                                                           a stagnant layer of minimum vertical velocity
                                                           around 20 km, and a surprisingly fast cleansing of
                                                           the lower stratosphere by the injection of particle-
                                                           free air from the troposphere up to 20 km during
                                                           the Southern Hemisphere convective season.

                                                           The future impact of volcanoes
                                                           The size distribution of stratospheric aerosols has
                                                           a strong influence on climate and on stratospheric
                                                           chemistry, and it is important to assess the abilities
that these particles were electrically charged. This       of different descriptions of aerosols in CCMs.
would affect the buoyancy of the particles as well         Under background (low aerosol) conditions the
as their ability either to grow or to evaporate. If this   agreement was good, but there was large scatter in
effect is widespread, this finding would open up a          simulations of volcanic eruptions.
new area of research on the role of thunderstorms
on the stratosphere.                                       The radiative impact of future large volcanoes on
Volcanic eruptions
In August 2006, a layer of sulphuric acid water
droplets was observed over Africa around 20 km
by all aircraft and balloon particle instruments.
These were in the plume following the eruption of




                                                           the stratospheric circulation was studied to see
                                                           if the sensitivity of the stratosphere is likely to
                                                           change as climate changes. In the scenario used
                                                           (large volcanic eruptions in the Tropics in 2025
                                                           and 2035), a faster circulation is found as a result
                                                           of greater tropical upwelling with an indication
                                                           of a larger response in 2035. This process
the Soufrière Hills in the Caribbean in early May.         manifests itself in transient heating in the lower
The evolution of the stratospheric aerosol during the      stratosphere.
two years following the launch of CALIPSO show




                                                                                                                    25
                                               Objective 5:


                          Interest                                              Approach

     Reliable prediction of the future evolution of         The scientific objectives are addressed by:
     surface UV radiation is required to serve European
     policy makers in planning appropriate protection       • exploiting and re-evaluating high quality
     measures for public health. The UV radiation             measurements of UV radiation from across
     levels at the Earth’s surface are controlled mainly      Europe to determine its variability and its
     by atmospheric ozone, clouds, aerosols and               relations with other atmospheric factors;
     albedo. The depletion of stratospheric ozone           • reconstructing old measurement records by
     since the late 1970s has resulted in elevated levels     using state-of-the-art radiative transfer models;
     of UV radiation in many regions worldwide. As
     a result of the successful implementation of the       • making detailed measurements of UV
     Montreal Protocol atmospheric concentrations of          radiation and aerosols from the ground and
     CFCs have started to decrease and the first signs         from the air to improve our knowledge of how
     of ozone recovery have been reported, prompting          aerosols affect how solar UV radiation passes
     the expectation of a corresponding reduction in          through the atmosphere;
     surface UV radiation levels. However, clouds,          • using climate chemistry models in order to
     aerosols and albedo are strongly influenced by            simulate UV radiation in the 21st century,
     climate change and they are expected to either           taking in to consideration also the influence of
     mask or enhance the impact of ozone recovery             climate change on clouds, aerosols and albedo.
     on UV radiation. The way these factors affect
     UV radiation is complex involving synergistic
     processes of absorption and scattering. Taking
     into consideration the complexity of all these
     processes, prediction of future UV radiation levels
     on global scale remains a challenging task.




26
Past Surface UV Changes, Variability and Trends


                                                  Findings

Surface UV measurements made in Thessaloniki, Jokioinen, Sodankylä, Bilthoven, Hradec Kralove,
Norrköping, Potsdam and Lindenberg during the 1990s and 2000s have been re-evaluated and quality
controlled datasets produced. These measurements have been analysed to quantify the changes in surface
UV radiation, resulting from ozone depletion and from changes in clouds and aerosols over Europe. The
cleaning of the atmosphere due to decreasing aerosols results in increasing of UV irradiance counteracting
the effect from the slowdown of ozone depletion.

Reconstruction models have been developed to extend the UV records back to the 1960s providing a longer
period of data for the estimation of long term changes. UV levels have gradually increased over the last
3-4 decades. Ozone depletion has contributed to this change particularly at the high latitude sites, but the
diminishing thickness of aerosols over the same period played an important role. Cloudiness decreased solar
radiation at many sites up to the early 1990s. Since then, decreasing cloudiness has contributed to an increase
in surface UV radiation.

In response to the projected ozone recovery, surface erythemal irradiance under cloud-free skies is projected
to decrease between 2000 and 2100 by up to 5% over northern and 10% over southern mid-latitudes. At
southern high latitudes the average decrease is three times as much. This information is then used to improved
the atmospheric models describing how UV is transmitted through the atmosphere.

Projections of future UV radiation levels have been derived by combining radiative transfer model calculations
with outputs from CCMs. In response to the projected ozone recovery, surface erythemal irradiance under
cloud-free skies is projected to decrease between 2000 and 2100 by up to 5% over northern and 10% over
southern midlatitudes. At southern high latitudes the average decrease is three times as much as a result
of the calculated recovery of the ozone hole. Accounting also for changes in cloudiness derived from one
CCM, the decreases in surface erythemal
irradiance become smaller at mid-latitudes
and increase at high latitudes. Localized
increases are projected in the tropical zone
as a consequence of regional changes in
clouds.

The day-to-day changes of daily erythemal
irradiation doses derived from two CCMs
agree well with those derived from
measurements, except at high latitudes
in the winter months. The agreement is
worse when comparing absolute values,
owing to differences between the actual
and simulated ozone columns and clouds,
but these are encouraging results given that
this is the first time such a study has been
made.




                                                                                                                  27
                                              Objective 6:


                          Interest                         Unravelling the relationship between ODS
                                                           emissions (top), concentrations (middle) and total
     The possibility of depletion of the ozone layer was   ozone (bottom) is needed to see how the Montreal
     first raised in the early 1970s, but there was no      Protocol has affected the mid-latitude ozone
     evidence of a trend in the observations. However,     layer. However, to do so requires quantitative
     by the mid to late 1980s decreasing ozone amounts     understanding of the factors that control the
     were observed at polar and middle latitudes which     variability of ozone which demands great care,
     resulted from the release of Ozone Depleting          even for the longest measurement record from
     Substances (ODS) such as chlorofluorocarbons           Arosa, Switzerland.
     and Halons. Meanwhile, in response to the threat
     of ozone destruction, the Vienna Convention was       It requires, in particular, quantification of the
     signed in 1985. The Montreal Protocol which limits    relative importance of chemical and dynamical
     the emissions of ODS was signed in 1987. The          influences on stratospheric ozone changes.
     implementation of the Montreal Protocol process,      Uncertainty in these limits our ability to interpret
     which allowed for strengthening amendments, has       the past changes of the ozone layer as well as our
     successfully resulted in reduced global production    confidence in predictions of its future evolution.
     of ODS (and, with a small delay, emissions) from
     the end of the 1980s. In turn, this has led to a
     more recent decline of the effective stratospheric                        Approach
     chlorine loading (EESC) by about 6% since its
     peak in the late 1990s.                               The goals in SCOUT-O3 were to


                                                           • quantify the effect of variability in transport
                                                             processes on extra-tropical total O3 variability;
                                                           • quantify the natural and anthropogenic
                                                             influences on the observed past changes;
                                                           • perform multi-decadal simulations of key
                                                             species in past atmosphere; and
                                                           • incorporate new laboratory data into model
                                                             calculations.

                                                           These were achieved by analysis of observations,
                                                           model improvements and model studies



                                                                                Findings

                                                           Interannual variability
                                                           The Brewer-Dobson circulation is critical in
                                                           determining the amount of ozone over middle
                                                           and high latitudes in winter and spring as it
                                                           cause the ozone to increase following its annual



28
                              Ozone at Mid-Latitudes


minimum in autumn. The observed winter ozone              better description of the long-term features in the
gain connected with transport of ozone from               stratospheric circulation. As a result of all these
low to high latitudes has been found to correlate         factors, SCOUT-O3 modellers have made the first
strongly with the upward transfer of energy from          successful multi-decadal simulations of the whole
the troposphere and can be used to diagnose the           stratosphere with reanalysed datasets to quantify
relationship between the state of stratospheric           the role of halogens in global ozone trends.
dynamics and stratospheric ozone depletion.
Analysis of longer time periods indicates a change
of this correlation with time but it is unclear if this         3D Model Calculations of Ozone Changes
change also indicates changes of the circulation.               35N-60N




                                                          The models are much more successful in
                                                          reproducing the observed trends in the Northern
                                                          hemisphere than in the Southern hemisphere.
                                                          Resolving this issue will be needed before we can
                                                          claim a full understanding of the past stratospheric
                                                          ozone changes.
Other studies have investigated the importance of
processes in the lower stratosphere in determining
the ozone amount and variability. In particular
transport from the tropical upper troposphere into
the extratropical lower stratosphere is an important
factor in the annual cycle of ozone.

Improved understanding of trends
Our ability to reproduce past ozone trends has
improved significantly during SCOUT-O3. The
relative roles of transport and chemical depletion
are now much clearer, and the short-lived bromine
compounds have been found to be important
during the period following the eruption of the Mt
Pinatubo in 1991.

A major advance has been the use of the improved
meteorological reanalyses which have led to a



                                                                                                                 29
                                               Objective 7:


                          Interest                          between ozone loss and climate change are
                                                            poorly understood and the importance of climate
     The annual occurrence of the Antarctic ozone           variability and change for the long-term evolution
     hole is probably the best known example of where       of chemical Arctic ozone loss is not known. The
     human activity has had an impact on the Earth’s        objectives of SCOUT-O3 project in polar science
     atmosphere. It is a dramatic feature with all the      were thus to:
     ozone at altitudes between 15 and 20 km destroyed
     each spring over all Antarctica. Smaller, but          • advance our understanding of these processes;
     significant losses (of up to 60% locally occur in       • continue monitoring polar ozone loss in both
     the Arctic winter, albeit with a large interannual       hemispheres;
     variability.
                                                            • assess the impact of climate change on polar
                                                              ozone loss; and
                                                            • provide realistic representations of polar
                                                              processes in chemistry-climate models.



                                                                                Approach

                                                            The SCOUT-O3 approach was threefold. A
                                                            major element was to supplement and coordinate
                                                            nationally funded stratospheric observational
                                                            programmes in polar regions. A second element
                                                            was to analyse all available observations (new and
     Polar stratospheric clouds (PSCs), such as these       existing; ground-based and satellite) in order to
     observed over Sodankyla in Northern Finland,           understand the interannual variability better. The
     must form for rapid chemical ozone loss to occur.      third element was to improve the descriptions of
     Stratospheric conditions are such that the Antarctic   polar ozone loss in chemistry-climate models and
     winter stratosphere is very cold and PSCs form         to make better predictions of ozone will evolve in
     every winter, while the Arctic is warmer and more      the coming decades.
     variable so that PSCs form less regularly. As a
     result, large ozone losses occur every spring in the
     Antarctic and in the Arctic ozone losses are large
     in some winters and small in others.

     The polar ozone losses have potentially large
     effects on the climate system through their impact
     on the radiative balance and the dynamical motions
     of the atmosphere. For example, the ozone hole
     has offset some of the surface warming caused
     by CO2 and other greenhouse gases, an offset that
     will disappear as the ozone hole recovers in the
     coming decades. However, while these effects
     are potentially large, the mutual interactions



30
           Polar Ozone in a Changing Atmosphere


                    Findings                          Polar ozone loss and climate change
                                                      The impact of climate change on Arctic ozone loss
Quantifying ozone loss                                has been assessed using the extended series of
Stratospheric ozone losses in both hemispheres        observed ozone losses in Arctic winters. Early in
have been quantified for each winter during            SCOUT-O3, the climate sensitivity of Arctic ozone
SCOUT-O3 and the related uncertainties have           loss determined from observations was found
been better characterized. For the Arctic, ozone      to be significantly larger than predicted by the
loss has been estimated in near real-time and the     state-of-the-art model at that time. Subsequently,
public was informed when unusually large losses       improvements in the models largely eliminated
occurred. The most notable instance was in spring     this problem and resulted in a much improved
2005 when losses of over 50% occurred at altitudes    representation of the climate sensitivity in the
around 18 km, and there was a 30% depletion in        model, giving greater faith in the model predictions
the atmospheric column of ozone.                      of Arctic ozone loss.

                                                      Finally, SCOUT-O3 scientists found that while
                                                      little change in temperature has occurred in the
                                                      warm Arctic winters, the coldest Arctic winters
                                                      have become significantly colder over the past four
                                                      decades. The role of these changes in stratospheric




Understanding critical processes
A combination of stratospheric observations and
detailed modeling has advanced our theoretical
understanding of the polar ozone loss process
by helping to identify the critical, rate-limiting
processes. In parallel, the year-to-year variation
in the natural dynamical variability (including       climate is to enhance the large Arctic ozone losses
the effect of the Brewer-Dobson Circulation (see      observed in the cold winters since the mid-1990s.
Objective 8) is better quantified. Together, these     The cause of this change is not understood or
have led to better quantitative modelling of polar    reproduced in climate models, but it could lead to
ozone loss in the 3D global models, which can         an amplification of ozone loss in the next decade
now better reproduce the interannual variation of     or so while halogen levels remain high.
chemical ozone losses in the Arctic. In addition,
the chemical and dynamical effects on stratospheric
ozone is responsible for a significant fraction of
the tropospheric climate and ozone variability.




                                                                                                             31
                                                Objective 8:


                           Interest                          and the mean transport time of stratospheric air and
                                                             the correlation of the winter ozone gain and eddy
     Whereas wind speeds in the stratosphere easily          heat flux. Observations are used to evaluate the
     can reach several hundred of kilometre per hour         results derived from CCM simulations. Scenario
     and can sweep air latitudinally around the world        calculations performed with CCMs are used to
     in a few days, air only moves slowly from the           improve our understanding of processes causing
     Tropics to the Poles. As a result, it can take          changes of the Brewer-Dobson circulation and its
     years for tropospheric air parcels from entering        possible future evolution.
     the stratosphere in the tropics to leave it at polar
     latitudes again. Yet it is this circulation (the
     Brewer-Dobson circulation) which determines the                              Findings
     distribution and thickness of the ozone layer, the
     distribution of water vapour in the stratosphere,       Observations of the ‘Age’ of Air
     and the atmospheric lifetimes of many greenhouse        The mean time taken to transport air from the
     gases and ozone depleting substances (ODSs). It         tropical lower stratosphere, where tropospheric
     is characterised by upward motion of air in the         air enters the stratosphere, to any point in the
     tropics from the troposphere into the stratosphere      stratosphere, is called the “age” of air. It can be
     poleward transport in the stratosphere and eventual     found from observations of inert trace gases which
     mixing back into the high latitude troposphere. It      have a clear trend. The spatial distribution of these
     is more pronounced in the winter hemisphere.            transport times results from the Brewer-Dobson
                                                             circulation.
     Climate change is expected to alter the strength
     of the Brewer-Dobson circulation. A stronger
     circulation would tend to warm the extra-tropical
     regions and cool the tropics and, in addition
     would have direct implications for the transport of
     tropospheric source gases into the stratosphere and
     of stratospheric ozone into the troposphere. It is
     therefore important to improve the observational
     and theoretical understanding of the Brewer-
     Dobson circulation.


                          Approach

     Within SCOUT-O3, the approach is to use multi-
     year observations of long-lived trace gases (e.g.       In SCOUT-O3, the first global distribution of the age
     derived from satellite instrument measurements)         of air using observations of sulphur hexafluoride
     in combination with decadal simulations by              (SF6) has been obtained from ESA’s MIPAS/
     numerical models of the atmosphere in order to          ENVISAT instrument. The new measurements
     investigate the variability and long-term temporal      reach all the way to 40 km and allow the age of
     evolution of stratospheric circulation. Important       air to be derived throughout the stratosphere.
     quantities are the tropical ascent rate of air masses   Now spanning seven years of observations these
     which can be determined from different methods          data will provide a basis for future assessment of
     like the H2O tape recorder, diabatic heating rates,     circulation changes.



32
                    The Brewer-Dobson Circulation


Modelling the Current Atmosphere                       the upper troposphere and lower stratosphere,
Several chemical-transport models have been            leading to an enhanced transfer of energy into the
improved following detailed comparisons with           stratosphere.
other models, observations and new estimates
of ascent rates in the tropical lower stratosphere.    The strengthening might be related to higher
In addition strategies were developed to use the       tropical sea surface temperatures which could
meteorological analyses. The resulting multi-          amplify deep convection locally and produce
annual simulations show a slight acceleration of       an intensified upwelling in the tropical upper
the Brewer-Dobson circulation over the past 30         troposphere and lower stratosphere. The transport
years which seems to be in contrast with a new         change in turn would increase the flux of ozone-
analysis of several decades of observations from       poor tropospheric air into the tropical lower
balloons and aircraft which show a small increase      stratosphere.
in the age of air.




                                                       Some CCM calculations indicate that the
The strength of the Brewer-Dobson circulation          intensification of tropical upwelling in the lower
varies considerably from year to year and this has     stratosphere will nearly double between the
been found to have a direct effect on the ozone        periods1960-2000 and 2000-2040 due to the
over middle and higher latitudes (see Objective 6).    combination of the radiative effect of greenhouse
It is important to see how this might change over      gases (GHG) and the impact of higher sea surface
time.                                                  temperatures (SST).

Modelling the Future Atmosphere                        Whether the exact mechanism is correct or not, it
While observations have not provided a complete        is clear that future changes in the Brewer-Dobson
picture of trends of the Brewer-Dobson circulation     circulation (and of ozone and UV radiation) are
to date, several climate model studies indicate that   sensitive to the sea surface temperatures used in
the circulation will strengthen as greenhouse gas      the models. This highlights the importance of
concentrations rise. Although this strengthening       developing and using CCMs which are coupled
is a robust feature of many climate change             with good ocean models in order to determine
simulations, the underlying mechanisms are not         the full response of the stratosphere to climate
sufficiently understood to explain the cause and        change.
effect relationship. The amplification may result
from the calculated increase in the temperature
gradient between lower and higher latitudes in



                                                                                                            33
                                                Objective 9:


                           Interest                                               Findings

     The division of the lower part of the atmosphere into   The Dynamical Effect of the Troposphere on the
     troposphere and stratosphere is a convenience that      Stratosphere
     has been used by meteorologists and atmospheric         The pattern of weather systems in the troposphere
     chemists alike. In practice the troposphere and         produces large-scale waves which disturb the
     stratosphere are strongly coupled, both through         polar vortex and lead to geographical variations of
     dynamics and through chemical transport. The            temperature and chemicals. SCOUT-O3 and other
     coupling is two-way, i.e. the troposphere affects the   work shows a clear link between waves leaving
     stratosphere and vice versa. Tropospheric weather       the troposphere and, for example, column ozone
     and climate both affect the stratosphere and in         in the stratosphere (see Objective 6).
     turn are influenced by it. The troposphere acts as
     a source for chemical species that are important        More challenging is to identify particular patterns
     in the stratosphere, both for ozone distribution        of disturbance in the tropospheric circulation
     and because their distribution in the stratosphere      which have a large effect on the stratosphere. One
     affects the radiation balance of the atmosphere         important aspect of year-to-year variability in the
     as a whole. Conversely the stratosphere is an           stratosphere is the frequency of polar stratospheric
     important source of ozone for the troposphere           cloud (PSC) formation (and hence the potential for
     and model simulations suggest, e.g., that future        chemical ozone loss). SCOUT-O3 has shown this
     changes in stratospheric ozone may significantly         is strongly affected by the large-scale meteorology
     increase background concentrations of ozone in the      in the troposphere and that large PSC volumes are
     troposphere. Concentrations of chemical species         preceded by a tropospheric circulation with higher
     such as ozone and water vapour vary sharply across      than usual pressure over East Asia, associated
     the tropopause, and it is important to understand       with high pressure systems, and lower than usual
     how such steep gradients are maintained.                pressure over the Atlantic.


                          Approach
                                                                                             H
     Understanding the coupling and ensuring that it
     is properly represented in models is an important
     part of understanding observed changes in the
     atmosphere and in making reliable predictions
     about the future. The issue of coupling between the
     stratosphere and troposphere is large and diverse.
     In SCOUT-O3, the effort has been focussed on
     certain important and carefully selected questions
     most closely connected to the overall project goal.
     Broadly these can be classed into three groups:
                                                             The Dynamical Effect of the Stratosphere on the
     • the dynamical effect of the troposphere on the        Troposphere
       stratosphere;                                         Recent observational and modelling studies
     • the dynamical effect of the stratosphere on the       have shown that changes to the stratosphere, e.g.
       troposphere; and                                      destruction of stratospheric ozone in the Southern
                                                             hemisphere spring to form the Ozone Hole, have a
     • chemical coupling.                                    significant effect on tropospheric circulation. Thus


34
              Stratosphere-Troposphere Coupling:
                        Past and Future

stratospheric changes on timescales ranging from       (A)
weeks to decades must be properly represented in
models in order to provide reliable predictions of
weather and climate. Work in SCOUT-O3 relevant
to medium-range weather forecasting has found
that dynamical patterns in the lower stratosphere
can improve predictions of European temperatures.
The work has identified optimal patterns on which
to base such predictions. However it is a complex
issue and the whole subject of what aspects of
stratospheric dynamics and chemistry most need
to be included in models to improve predictions
of surface weather and climate is a fertile area of
investigation for the future.                          (B)

Chemical Coupling
Investigations of the factors influencing chemical
composition around the extratropical tropopause
have been model-based, using particle-based
methods to quantify transport. These provide
estimates of chemical distributions that can be
compared against in situ chemical data and so used
to assess the ability of global chemical models to
reproduce this important atmospheric region.

As an example, the relation between CO and O3          (C)
measured in the UTLS tropics (A - red/pink) and
subtropics (top - pale/dark blue) during the pre-AVE
and AVE campaigns shows anomalous behaviour
in the subtropics (A - orange). The particle
analysis of the origins of these measurements          (D)
(B) shows that they are drawn from two distinct
regions, the lower subtropical troposphere and the
extratropical lower stratosphere.

The particle-based methods have also allowed
mapping of transport pathways showing the strong
latitudinal and longitudinal structure of surface
regions that act as a source for the stratosphere.     (D) and enters the stratosphere after ascent from
For example, air that enters the stratosphere          the outflow from these storms. This information is
in mid- and high latitudes originates from the         now being used to estimate the stratospheric ozone
surface in mid-latitude oceanic regions (C) and        depletion that is likely to result from emission of
ascends in the warm conveyor belt of weather           bromine compounds at different geographical
systems, whereas air that enters the stratosphere      locations.
in the subtropics originates from the surface in the
regions of deepest convective storms in the tropics


                                                                                                             35
                                            Objective 10:


                          Interest                        • specific developments of applied CCMs to
                                                            improve the agreement with observations; and
     Reliable assessment of the future evolution of
     stratospheric ozone and the consequential impact     • use of improved CCMs for new simulations
     on surface ultraviolet (UV) irradiance requires a      to provide the best estimates for assessments
     good understanding of the relevant atmospheric         of temporal evolution of ozone, climate and
     processes. Chemistry-climate models (CCMs) are         surface UV irradiance.
     the principal tool used to make such assessments,
     and they are central to determining whether the
     regulation of ozone depleting substances (ODSs)                           Findings
     by the Montreal Protocol is sufficient to fully
     restore the stratospheric ozone layer in future.     Ten CCMs were used for the first time in an extensive
     The increasing impact of climate change means        set of coordinated, multi-year simulations. These
     that the evolution of the ozone layer in the next    provided the basis for the projections of the future
     few decades will not be a simple reversal of past    evolution of the ozone layer in the UNEP/WMO
     changes, and understanding the coupling between      Scientific Assessment of Ozone Depletion: 2006.
     climate change and stratospheric ozone depletion
     is the central aim in SCOUT-O3.


                        Approach

     Observations in combination with atmospheric
     models were used to investigate recent changes
     of climate, atmospheric composition (especially
     ozone) and surface UV irradiance. The aim is
     to describe and better understand the critical
     processes of the Earth’s atmosphere as well as
     the feedback mechanisms influencing short- and
     long-term changes. In particular, coupled CCMs
     considering the interaction of physical, dynamical
     and chemical processes are used to reproduce
     observed fluctuations and trends as well as to
     perform prognostic studies to assess possible
     future evolution of climate, ozone and surface UV
     irradiance.

     Scientific studies during SCOUT-O3 can be
     divided into three main overlapping phases:          Early in SCOUT-O3, detailed comparisons
                                                          revealed obvious differences in the predictions of
     • evaluation of the performance of CCMs by           ozone, climate, and UV derived from the various
       comparison of CCM results with each other          CCMs. Model calculations have been intensively
       and with observations to identify strengths and    tested with relevant observations. In particular,
       weaknesses of the applied numerical models;        comparisons with the new measurements taken
                                                          during the SCOUT-O3 tropical campaigns have



36
   Predictions of Ozone Recovery and Surface UV


been used to analyse the altitude distribution and    • surface UV irradiance is expected to decrease
variability of chemical species and the influence        due to the anticipated global recovery of
of convection. As a consequence, improvements           stratospheric ozone, surface UV irradiance is
were made to a number of individual CCMs.               expected to decrease. However climate change
                                                        will also influence surface UV irradiance
Near the end of SCOUT-O3 a multitude of                 through changes induced mainly on clouds
improved CCMs has been used to carry out new            and surface reflectivity. This could result in
multi-year simulations, covering the period from        a future increase of surface UV irradiance,
1960 to 2100. These results have been provided          depending on geographical region and season.
to and further investigated for the SPARC
CCMVal report (to be published in early 2010),
the upcoming UNEP/WMO Scientific Assessment
of Ozone Depletion: 2010, and Fifth Assessment
Report of the IPCC. So far the major results are:
• CCMs indicate that future increases of
  greenhouse gas concentrations will contribute
  to a further cooling in the stratosphere;
• Chemical reaction rates in the atmosphere
  cre dependent on temperature and thus
  ozone concentrations are sensitive to climate
                                                      Impact on CCMs and More Generally
  changes;
                                                      Within SCOUT-O3, CCMs have improved
• greenhouse gas induced changes of                   significantly. The intensive evaluation of model
  stratospheric temperature and dynamics are          data with respective observations has enabled
  expected to accelerate the increase of total        modelling groups to identify obvious deficiencies
  global ozone in the next decades. Ozone layer       in model systems applied so far. This has led to
  recovery develops differently in different          a purposeful development of CCMs. Currently
  atmospheric regions and climate change is           available CCMs are still far from being “perfect”
  affecting it. The ozone layer’s recreation is not   model systems describing observed changes in
  a simple reversal of recent development, e.g.       all details, but they have made a big step towards
  decreasing stratospheric temperature in high        more reliable predictions in the last five years.
  latitude regions could lead to a slow down of
  the closure of the Antarctic ozone hole;
• a full recovery of the ozone layer is expected
  around the middle of this century and there is
  a chance for an ozone “super-recovery”, i.e.
  future levels of stratospheric ozone may be
  higher than in the first half of the last century.
  A typical example for achieved results shows
  calculations of column ozone (60°N to 60°S)
  from one model for the period 1960-2050
  compared to two satellite measurements; and




                                                                                                           37
          The World Avoided by the Montreal Protocol


           The Effect of the Montreal Protocol                 gases, and it was recently demonstrated that the
                                                               Montreal Protocol has had a major, beneficial
     From the 1960s onwards, there was a rapid                 climate impact; as in its absence the radiative
     rise in the manufacture and use of a number of            forcing just by ozone-depleting substances would
     halogenated (mainly chlorine- but also bromine-           already have been comparable to that from CO2.
     based) compounds which had a wide range of                Without the Protocol we would effectively be
     industrial and domestic uses. Concerns about their        about a decade further into climate change; the
     environmental impacts began in the 1970s and the          Protocol has brought precious time further drastic
     demonstration of their role in the rapid Antarctic        reductions of other greenhouse gases.
     springtime polar depletion in the 1980s led to
     regulation (phase-out) of these ozone-depleting
     substances under the Montreal Protocol. The
     benefits of the Montreal Protocol for atmospheric              What did the Montreal Protocol Achieve?
     halogen abundances can be seen in the box. The
     original Protocol made a modest impact, slowing           In SCOUT-O3 we have asked questions such as:
     down the rate at which these compounds entered            What ozone depletion, and surface UV increase,
     the atmosphere, but subsequent amendments have            has been avoided by the Protocol? Ozone is a
     led to a trajectory where the atmosphere is slowly        climate gas, so that the avoided ozone depletion
     being cleansed of these industrial halogens.              will also have avoided some climate change. How
                                                               large is this avoided change?
     It is interesting to ask what would have happened
     if the Montreal Protocol had not been enacted and
     if the much higher emissions of ozone-depleting
     substances had occurred. One important aspect is
     that the ozone-depleting substances are greenhouse



                                                          The Montreal Protocol aimed to achieve reductions
                                                          in stratospheric abundances of chlorine and
                                                          bromine through restrictions on the production
                                                          and consumption of manufactured halogen source
                                                          gases. Projections of the future halogen amounts
                                                          are shown assuming 1) no Protocol regulations, 2)
                                                          only the regulations in the original 1987 Montreal
                                                          Protocol, and 3) subsequent changes to the Protocol
                                                          (labelled by where and when changes to the original
                                                          1987 Protocol provisions were agreed). Without the
                                                          Protocol, stratospheric halogen gases were projected
                                                          to increase significantly in the 21st century. The
                                                          “zero emissions” line shows a hypothetical case
                                                          of stratospheric abundances if all emissions were
                                                          reduced to zero beginning in 2007.




38
Avoided Modification of Climate
Without the Protocol the abundance of halogen
species in the atmosphere could have reached
9 part per billion by 2030.              A calculation
with one of the chemistry-climate models in
SCOUT-O3 shows that this increase in the halogens
would have led to further large ozone destruction,
reaching locally to perhaps 40% in both the upper and
lower stratosphere. Changes in stratospheric ozone
have an impact on surface temperatures by influencing
the transmission of solar and infrared radiation through
the atmosphere. The changes in surface temperatures
have a complex spatial pattern (reminiscent in the
Antarctic of observed changes attributed to the ozone
hole) and are large in magnitude.




Avoided Skin Cancers
The large calculated reductions in ozone lead to a large calculated increase in UV (assuming that
cloudiness remains the same) with a consequent impact on human health. This has been assessed in
SCOUT-O3. Models have been used to estimate the global distribution of skin cancer cases avoided
by the Montreal Protocol. The estimate is very large; bearing in mind the possible caveats in the
extrapolation to human health, it is clear that the Montreal protocol has been enormously beneficial for
the human population.




                                                                                                          39
           Future Directions for Stratospheric Research


     Stratospheric science has reached a new, mature phase. In the 25 years since the discovery of the ‘Ozone
     Hole’ we have established the basic understanding of the processes behind Antarctic ozone loss. EU-funded
     research during the 1990s has demonstrated that these processes also occur in the Arctic and can affect
     populated middle latitudes. Within SCOUT-O3, this understanding has been incorporated into climate
     models which have been used to address the issue of stratospheric ozone recovery and the impact on surface
     UV. While our understanding has advanced significantly it would be a mistake to think that the science is
     now settled (just as it would be wrong to think that our understanding of climate change is complete). More
     appropriately, stratospheric science should now be seen to be a central component of Earth System Science.
     We will not be able to make improved projections about global change unless we improve our understanding
     of how the stratosphere couples into the whole system.

     A future research strategy needs to have two components. First, there are still fundamental issues relating to
     the stratospheric science. The UTLS region and the tropical tropopause layer are likely to remain key foci;
     changes here have biggest impact on, e.g., tropospheric chemistry and surface climate. Questions include:
     • the need to improve our understanding of the processes controlling radiatively active components (O3,
       water vapour, aerosols) in the cold UTLS;
     • quantitative understanding of troposphere to stratosphere exchange in the tropics, including the role
       of deep convection, and extratropical stratosphere to troposphere exchange and how these will change
       under climate change;
     • the role of biogenically emitted very short lived halogen substances in the future;
     • the role of growing anthropogenic emission of source gases (e.g methane, nitrous oxide and pollution in
       the tropics)
     • the role of volcanic emissions and solar variations in ozone recovery.

     Secondly, we need to understand quantitatively how changes in the stratosphere impact the whole climate
     system. Questions include:
     • the role of lower stratospheric ozone for regional climate change;
     • how the stratosphere circulation couples to important modes of climate variability, including the North
       Atlantic Oscillation, El Nino and the monsoon circulation;
     • the importance of lower stratosphere for seasonal weather forecasting;
     • the importance of lower stratospheric ozone, and its changes, for tropospheric chemistry and surface
       UV radiation; and
     • how geoengineering of the lower stratosphere could impact surface climate and chemistry of the
       stratosphere.

     In addition, research on UV radiation needs to be more closely integrated with studies of climate change
     and tropospheric composition changes as clouds and tropospheric aerosols are likely to be major factors in
     determining future UV radiation at the Earth’s surface.




40
                          Data Policy and Database


                 General Policy                                        Nadir Database

SCOUT-O3 is a complex project involving many          A major role for the Nadir data centre throughout
sorts of measurements and model calculations          the project is the provision of ancillary information
which had to be integrated to achieve the scientific   such as meteorological analyses and ozone maps.
aims. Accordingly a clear data policy was             The atmospheric context is valuable in interpreting
developed which included support for two central      the atmospheric measurements and so these were
databases in addition to those maintained by many     supplied routinely for the analysis of data from
individual partners. These were the Nadir data        SCOUT-O3 itself as well as in studies of previously
centre at NILU which already stores atmospheric       existing measurements. Two newsletters were
data from many European projects and field             published highlighting the new and existing
measurement campaigns, and the European               products available at the Nadir database.
Database for UV Climatology and Evaluation at
FMI which is the main European repository for         Several tropical field campaigns were organised
UV measurements. A SCOUT-O3 committee                 within SCOUT-O3 to investigate the mechanisms
monitored the effectiveness of the data policy and    by which air passes from the upper troposphere to
suggested new developments.                           the lower stratosphere. A field database was set up


           European Database for
        UV Climatology and Evaluation

The European Database for UV Climatology and
Evaluation has been developed in projects in the
EC’s 4th and 5th Framework Programmes. The
database serves the UV scientist community in
SCOUT-O3, but also reaches out to wider research
communities working on ozone, human health,
and terrestrial and aquatic ecosystems, and various
multi disciplinary research areas. Currently the
database holds over 2.8 million spectra measured      in Darwin for the airborne campaign which took
at 38 stations in 16 European countries.              place in late 2005 in order to support the flight
                                                      planning. Special directories were set up for all
                                                      the SCOUT-O3 field campaigns in order to provide
                                                      easy access for post-campaign analysis.

                                                      The data from all the field measurement campaigns
                                                      (N. Australia, W. Africa and S. America) are stored
                                                      on Nadir. In order to interpret and understand
                                                      the small scale feature in a long-term and global
                                                      context, satellite measurements (e.g. from
                                                      ENVISAT and CALIPSO), measurements from
                                                      ground-based instruments and other global fields
                                                      will be used in conjunction with models from
                                                      regional to global scales.



                                                                                                              41
                                  Dissemination, Outreach


                           General                           contributed well over 500 talks and posters at
                                                             international conferences and meetings including
                                                             those of the European Geophysical Union and
     Scientific research takes place in a broad context
                                                             the American Geophysical Union. These papers
     and so an important aspect of SCOUT-O3 has
                                                             and presentations relate to the many individual
     been to disseminate the project’s scientific results
                                                             research projects which take place within such a
     to a wide audience: other scientists (specialists and
                                                             large enterprise as SCOUT-O3, and of which only
     non-specialists), policy-makers and the public.
                                                             a flavour can be given in this summary. SCOUT-
     This has been in the form of:
                                                             O3 scientists have also written articles for a more
     • scientific journals and meetings;                      general scientific audience in, for example, SPARC
                                                             newsletter and magazines published by their own
     • international scientific assessments; and              institutions or funding agencies.
     • press and public events.

                                                                    Training the scientists of tomorrow
     In addition SCOUT-O3 scientists help train
     the scientists of tomorrow and have actively            A major research project like SCOUT-O3 provides
     participated in programmes to promote science as        an excellent way of involving young scientists in
     a career for women.                                     an international setting. Nearly 40 PhD students
                                                             have been reported as working directly on SCOUT-
                                                             O3-related projects and many more will have been
                   Scientific Discussions                     involved at some level or other. Many early career
                                                             post-doctoral researchers have also taken part.
     Researchers have written or contributed to over 350     The international context is important because it
     peer-reviewed papers (with more in the pipeline) in     exposes the young scientists to many groups and
     over 50 international scientific journals, including     cultures and so lets them build up their own sets of
     Science, Atmospheric Chemistry and Physics and          contacts and colleagues at an early stage.
     the Journal of Geophysical Research. They have




42
                               and Human Capital


           International Assessments                 O3 suggests that such actions are most effective
                                                     as the institutions are responsible for their own
A sound scientific understanding is a necessary       hiring, promoting and employment policies, and
(though not sufficient) criterion for making the      have the best links with their local and national
right decisions on global environmental problems     communities as well as the best understanding of
such as ozone depletion and climate change,          the cultural issues they are dealing with
and SCOUT-O3 was designed to provide this.
In addition to providing important scientific
information in the form of peer-reviewed papers,                   Informing the public
SCOUT-O3 scientists have been personally
involved as contributors, authors or lead authors    Reaching out to a wider audience is important
with international Scientific Assessments.            to maintain the public interest and knowledge
Most notable are the UNEP/WMO Scientific              of science. With this motivation, SCOUT-O3
Assessments of Ozone Depletion in 2006 and           scientists have given many talks at schools and
2010, and there were also significant contributions   within their local communities throughout the
to the IPCC Special Report Safeguarding the          world. They have also been involved in public
Ozone Layer and the Global Climate System, the       outreach events aimed at making science more
IPCC Fourth Assessment Report, UNEP’s GEO-4          accessible to the public as well as encouraging
report and the EEA’s State of the Environment and    children to become more interested in learning
Outlook report 2010.                                 science at university.

                                                     There has been much international press interest
                                                     throughout the project which SCOUT-O3 scientists
                                                     have responded to. The field measurements
                                                     campaigns in West Africa, North Australia and
                                                     South America all received a lot of attention from
                                                     the local and international press.




         Encouraging female scientists

SCOUT-O3, like all EC Integrated Projects,
had a gender action plan which particularly
concentrated on ensuring that within SCOUT-O3
female scientists had equal opportunities when
issues such as positions of responsibility, talks,
etc. were considered. In addition many scientists
were actively involved in initiatives run by their
own institutions. The experience in SCOUT-




                                                                                                          43
     Ozone loss at both poles receives a fair amount
     of attention, and in 2005 SCOUT-O3 issued press
     updates about the large ozone losses in the Arctic
     that year. This received a great deal of attention,
     particularly in Europe and Canada. SCOUT-
     O3 scientists have been asked to comment on
     atmospheric science related articles/items on
     television, radio, newspapers and internet. Overall
     media coverage including television documentaries
     and reports, radio programmes and articles in
     newspaper and popular science magazines.




44
45
        List of Organisations Involved with SCOUT-O3


     Name                                     Country          Name                                     Country

     University of Cambridge                  United Kingdom   Observatory of Neuchâtel                 Switzerland
     Alfred Wegener Institute                 Germany          Paul Scherrer Institute                  Switzerland
     Belgisch Instituut voor Ruimte-                           National Institute for Public Health
            Aëronomie                         Belgium                and Environment                    The Netherlands
     Central Aerological Observatory          Russia           Royal Netherlands Meteorological
     Centre National de Recherches                                   Institute                          The Netherlands
            Scientifique                       France           Sveriges Meteorologiska och
     Chalmers University of Technology        Sweden                 Hydrologiska Institut              Sweden

     Chemical Research Center                 Hungary          Stratosphere-M, Ltd                      Russia

     Consiglio Nazionale delle Ricerche       Italy            University of Bern                       Switzerland

     Czech Hydrometeorological Institute      Czech Republic   University of Bremen                     Germany

     Danish Meteorological Institute          Denmark          University of Buenos Aires               Argentina

     Physical Meteorology Observatory                          University of Crete                      Greece
           of Davos                           Switzerland      Johann Wolfgang Goethe
     Demokritus University of Thrace          Greece                 University of Frankfurt            Germany

     Deutsches Zentrum für Luft                                University of Göteborg                   Sweden
           und Raumfahrt                      Germany          University of Hannover                   Germany
     Deutscher WetterDienst Lindenberg                         University of Heidelberg                 Germany
     Germany                                                   Medizinische Universität Innsbruck       Austria
     Ente per le Nuove Tecnologie,                             University of Karlsruhe                  Germany
           L’Energia e l’Ambiente             Italy
                                                               University of Lancaster                  United Kingdom
     ETH Zürich                               Switzerland
                                                               University of L’Aquila                   Italy
     Finnish Meteorological Institute         Finland
                                                               University of Leeds                      United Kingdom
     Free University of Berlin                Germany
                                                               University of Leicester                  United Kingdom
     Forschungszentrum Jülich GmBH            Germany
                                                               University of Oslo                       Norway
     Forschungszentrum Karlsruhe GmBH         Germany
                                                               Aristotle University of Thessaloniki     Greece
     Imperial College of Science,
           Technology and Medicine            United Kingdom   University of Wyoming                    USA
     Instituto Nacional de Técnica                             University of California at Irvine       USA
             Aeroespacial                     Spain            UK Met Office                             United Kingdom
     Istituto Nazionale di Geofisicae                           University of East Anglia                United Kingdom
             Vulcanologia                     Italy
                                                               Universitaet für Bodenkultur             Austria
     Istituto Nazionale di Ottica Applicata   Italy
                                                               Weather Informatics                      United Kingdom
     Johannes-Gutenberg Universitat Mainz     Germany
                                                               Chemical Processing Research Institute   Greece
     Karl-Franzens-Universitaet Graz          Austria
                                                               Pontif. Univ. Cat. Argentina St Maria
     Max Planck Gesellschaft                  Germany                 de los Buenos Aires               Argentina
     Météo France                             France           University of Utrecht                    The Netherlands
     National and Kapodistrian                                 University of Manchester                 United Kingdom
           University of Athens               Greece
                                                               University of Bielefeld                  Germany
     Norwegian Institute for Air Research     Norway
                                                               University of Wuppertal                  Germany




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