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          CONTINUITY OF IMPROVE CARBON DATA
THROUGH THE 1 JANUARY 2005 INTRODUCTION OF
             NEW ANALYTICAL INSTRUMENTATION*

This is an updated and elaborated version of a presentation sent to DRI in
August 2007 and presented at the IMPROVE Steering Committee meeting
in Durango (http://vista.cira.colostate.edu/improve/Activities/Meetings/2007Pres/C_medians_white.pdf).
It applies to carbon data some of the analytical techniques developed at
CNL to identify temporal instabilities in XRF data. The plots that follow are
snapshots from early stages of a hypothesis-generating exploration, and at
this point are intended only for internal discussions of their interpretation.




WHW, 10/2/07                               *Chow et al. (2007) JA&WMA 57:1015-1023
updated 1/23/08
                                                                     2
 O1         We begin with time series of the ratios
 TC       TOR fraction / total carbon (g/g or mol/mol).
0.15
        VIEWS “raw”, downloaded 9/07

 0.1            VIEWS “preliminary”, downloaded 9/07
                (Babs is not included in VIEWS preliminary data,
                 and so was obtained from CNL’s internal files.)

0.05



   0
        Scales vary from fraction to fraction, but grid intervals
       remain constant (as a visual cue to the differences).
-0.05
    Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                              3
 O1           MEDIAN AND INTERQUARTILE RANGE
               ENTIRE NETWORK, ALL VALID DATA
 TC
0.15



 0.1
                    75th percentile

0.05
               OC 
                                
       median      , k  site 
               TC k
                                

   0                25th percentile



-0.05
    Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                              4
 O1          MEDIAN AND INTERQUARTILE RANGE
              ENTIRE NETWORK, ALL VALID DATA
 TC
0.15

            2001-2003 “NORMAL”:
        for each week {1,2,…,52}, the
 0.1     median of 24h medians from
         that week during 2001-2003

0.05



   0



-0.05
    Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                                          5
 O1              MEDIAN AND INTERQUARTILE RANGE
                  ENTIRE NETWORK, ALL VALID DATA
 TC
0.15
               unsynchronized sampling
               during 2/week  1/3day
               transition: data excluded
 0.1

                                           IMPROVE      IMPROVE_A

0.05                                       (DRI/OGC)   (DRI Model 2001)




   0

   version 1 | version 2
        samplers
-0.05
    Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                              6
 O1          MEDIAN AND INTERQUARTILE RANGE
              ENTIRE NETWORK, ALL VALID DATA
 TC
0.15



 0.1



0.05



   0



-0.05
    Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                             7
O2          MEDIAN AND INTERQUARTILE RANGE
             ENTIRE NETWORK, ALL VALID DATA
TC
0.25



 0.2



0.15



 0.1



0.05
   Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
O1  O 2     MEDIAN AND INTERQUARTILE RANGE
                                                             8
              ENTIRE NETWORK, ALL VALID DATA
  TC
 0.45

  0.4

 0.35

  0.3

 0.25

  0.2

 0.15

  0.1

 0.05

   0
   Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                             9
O3          MEDIAN AND INTERQUARTILE RANGE
             ENTIRE NETWORK, ALL VALID DATA
TC
 0.5

0.45

 0.4

0.35

 0.3

0.25

 0.2

0.15

 0.1

0.05
   Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                            10
O4          MEDIAN AND INTERQUARTILE RANGE
             ENTIRE NETWORK, ALL VALID DATA
TC
 0.3



0.25



 0.2



0.15



 0.1
  Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                                          11
 OP           MEDIAN AND INTERQUARTILE RANGE
               ENTIRE NETWORK, ALL VALID DATA
 TC
 0.4

0.35

 0.3

0.25

 0.2

0.15

 0.1

0.05

  0
  Jan-00   Jan-01   Jan-02   Jan-03   Jan-04   Jan-05   Jan-06   Jan-07
O 4  OP     MEDIAN AND INTERQUARTILE RANGE
                                                              12
              ENTIRE NETWORK, ALL VALID DATA
   TC
  0.6

 0.55

  0.5

 0.45

  0.4

 0.35

  0.3

 0.25

  0.2

 0.15
    Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                            13
E1          MEDIAN AND INTERQUARTILE RANGE
             ENTIRE NETWORK, ALL VALID DATA
TC
 0.5

0.45

 0.4

0.35

 0.3

0.25

 0.2

0.15

 0.1
  Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                            14
E2          MEDIAN AND INTERQUARTILE RANGE
             ENTIRE NETWORK, ALL VALID DATA
TC
 0.2



0.15



 0.1



0.05



  0
  Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                             15
OC          MEDIAN AND INTERQUARTILE RANGE
             ENTIRE NETWORK, ALL VALID DATA
TC
0.95


 0.9


0.85


 0.8


0.75


 0.7


0.65
   Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
EC       OC      MEDIAN AND INTERQUARTILE RANGE
                                                              16
     1          ENTIRE NETWORK, ALL VALID DATA
TC       TC 
 0.35


  0.3


 0.25


  0.2


 0.15


  0.1


 0.05
    Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
                                                                                   17
              O1                        O2                         O4
              TC                        TC                         TC
 0.25                         0.3



  0.2                        0.25



 0.15                         0.2



  0.1                        0.15



  0.05                         0.1
Jan-03 Jan-04 Jan-05 Jan-06 Jan-07 Jan-04 Jan-05 Jan-06 Jan-07
     Jan-00 Jan-01 Jan-02 Jan-03 Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-0

         Some organic fractions changed abruptly on 1 January 2005.
                                                                                18
                     O3                                  OP
                     TC                                  TC
                     0.4

                    0.35

                     0.3

                    0.25

                     0.2

                    0.15

                     0.1

                    0.05

                       0
                      Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07

       Others seemed to anticipate the change in instrumentation.
                                                                                  19
                     OC                                    EC
                     TC                                    TC
                     0.35


                      0.3


                     0.25


                      0.2


                     0.15


                      0.1


                     0.05
                        Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07
Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07

        The changes in OC and EC are neither abrupt nor dramatic, but
        the greater regularity of these aggregates makes them noticeable.
        Winter 2003-4 also appears anomalous.
                                                                     20

We have focused on carbon/carbon ratios up to now.
Total organic carbon, OC, can also be compared against non-
sulfate hydrogen. This is calculated from the A-module PESA
measurement of H and the B-module IC measurement of SO4= on
the assumption that all sulfate is ammonium sulfate. On the
further assumption that ammonium sulfate accounts for all
inorganic hydrogen, non-sulfate hydrogen is referred to as organic
hydrogen, OH.
Total elemental carbon, EC, can be compared against the A-
module HIPS (hybrid integrating plate/sphere) measurement of
light absorption. These data are submitted by CNL as LRNC (the
“NC” stands for non-corrected), and delivered by VIEWS as Babs
in the non-standard units (108 m)-1.
Of course, each measurement added to the comparisons also
carries its own errors and uncertainties.
OC                OC      8          MEDIAN AND INTERQUARTILE     OH21
                      H  SO4       RANGE, ENTIRE NETWORK,
OH                12      96              ALL VALID DATA          OC
          1.4

          1.2

           1                                                                1
mol/mol




          0.8
                                                                        1.5
          0.6
                                                                            2
          0.4
                                                                            3




                                                                        mol/mol
          0.2

           0
           Jan-00    Jan-01 Jan-02   Jan-03 Jan-04   Jan-05 Jan-06 Jan-07
          OC              MEDIAN AND INTERQUARTILE RANGE
                                   0.95                                                              OH22
                           ENTIRE NETWORK, ALL VALID DATA
                                    0.9
          OH                            0.85
                                                                                                     OC
          1.4
                                         0.8


                                        0.75
          1.2                                                           OC
                                         0.7                            TC

                                        0.65
            1                              Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07      1
mol/mol




          0.8
                                                                                                      1.5
          0.6
                                                                                                        2
          0.4
           The new measurements report less OC, not only                                                3
           relative to TC, but also relative to OH – estimated




                                                                                                      mol/mol
          0.2
           wholly independently. Like OP/TC, OC/OH
           seemed to anticipate the instrumentation change.
           0
           Jan-00 Jan-01 Jan-02 Jan-03 Jan-04                             Jan-05 Jan-06 Jan-07
     EC               MEDIAN AND INTERQUARTILE RANGE              Babs 23
                       ENTIRE NETWORK, ALL VALID DATA
    LRNC                                                           EC
          2                                                               5
         1.8
         1.6




                                                                          m2/g
         1.4
g/10m2




         1.2
          1                                                           10
         0.8
         0.6
                                                                      20
         0.4
         0.2
          0
          Jan-00   Jan-01 Jan-02   Jan-03 Jan-04   Jan-05 Jan-06 Jan-07
     EC                MEDIAN AND INTERQUARTILE RANGE                                             Babs 24
                        ENTIRE NETWORK, ALL VALID DATA
    LRNC                             0.35
                                                                      EC
                                                                                                   EC
          2                           0.3                             TC                              5
                                     0.25
         1.8
                                      0.2

         1.6




                                                                                                      m2/g
                                     0.15


         1.4                          0.1
g/10m2




                                     0.05
         1.2                            Jan-00 Jan-01 Jan-02 Jan-03 Jan-04 Jan-05 Jan-06 Jan-07



          1                                                                                          10
         0.8
         0.6
                                                                                                     20
         0.4
         0.2   EC/LRNC trended higher in 2005 than in 2004, but gaps leave the
               record somewhat ambiguous.
          0
          Jan-00   Jan-01 Jan-02        Jan-03 Jan-04                   Jan-05 Jan-06 Jan-07
                                                                              25
TC             MEDIAN AND INTERQUARTILE RANGE
                ENTIRE NETWORK, ALL VALID DATA
FM
0.5


0.4


0.3


0.2


0.1
      Comparison with gravimetric fine mass, considered one of the most
      reliably accurate of the measurements, gives no clear indication that
      TC = EC+OC did exhibit any decrease in 2005.
 0
 Jan-00   Jan-01 Jan-02        Jan-03 Jan-04       Jan-05 Jan-06 Jan-07

				
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