donald r. blake (pi), nicola j. blake, simone meinardi, angela young, andreas beyersdorf, lambert a....
TRANSCRIPT
Donald R. Blake (PI), Nicola J. Blake, Simone Meinardi, Angela Young, Andreas Beyersdorf, Lambert A. Doezema, Brian Novak, Barbara Barletta, Jason Midyett, Michael A Kamboures, Henry Fuelberg (and team), Stephanie Vay, Melody Avery….and the
rest of the INTEX Science Team
Trace Gases in Whole Air Samples Collected on the DC-8 for INTEX-NA
Donald R. Blake (PI), Nicola J. Blake, Simone Meinardi, Angela Young, Andreas Beyersdorf, Lambert A. Doezema, Brian Novak, Barbara Barletta, Jason Midyett, Michael A Kamboures, Henry Fuelberg (and team), Stephanie Vay, Melody Avery….and the
rest of the INTEX Science Team
Trace Gases in Whole Air Samples Collected on the DC-8 for INTEX-NA
Main NMHC/CFC/AN System - 2936 samples
Analysis by GC/ECD/FID/MS at UC-Irvine
Main NMHC/CFC/AN System - 2936 samples
CH4 System - 2263 samples
Analysis by GC/ECD/FID/MS at UC-Irvine
Main NMHC/CFC/AN System - 2936 samples
CO System - 586 samplesCH4 System - 2263 samples
Analysis by GC/ECD/FID/MS at UC-Irvine
Comparison of TRACE-P and INTEX
Expect lower summer levels (OH consumption) - as see for ethyne
0 500 1000 1500 2000 2500
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
Ethyne
Altitude km
Comparison of TRACE-P and INTEX
Expect lower summer levels (OH consumption) - as see for ethyne•But - relatively more ethane for INTEX
(Less combustion/compared to alkane sources?)
0 1000 2000 3000 4000 5000
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
Ethane
0 500 1000 1500 2000 2500
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
Ethyne
Altitude km
Comparison of TRACE-P and INTEX
Expect lower summer levels (OH consumption) - as see for ethyne•But - relatively more ethane for INTEX
(Less combustion/compared to alkane sources?)•Also - INTEX ethane “pumped up”!
0 1000 2000 3000 4000 5000
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
Ethane
0 500 1000 1500 2000 2500
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
Ethyne
Altitude km
Comparison of TRACE-P and INTEX
0 0.5 1 1.5 2
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
CH3I
Altitude km
Comparison of TRACE-P and INTEX
Surprisingly high levels over the continent during INTEX
- terrestrial as well as ocean sources?
0 0.5 1 1.5 2
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
CH3I
Altitude km
Comparison of TRACE-P and INTEX
3 4 5 6 7 8 9 10
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
H-1211
Altitude km
• Fewer low alt plumes than TRACE-P
Comparison of TRACE-P and INTEX
• Fewer low alt plumes than TRACE-P
• High altitude enhancement during INTEX -> long range transport from Asia??
3 4 5 6 7 8 9 10
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
H-1211
Altitude km
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Flight Track with Color-coded Altitude
45
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25
-90 -85 -80 -75 -70
13
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1617
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0
Altitude km
Smaller blue squares correspond to the 6 BL runs
Contrast between Ocean and Land BL Data
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Flight Track with Color-coded Altitude
45
40
35
30
25
-90 -85 -80 -75 -70
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1617
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2
0
Altitude km
Smaller blue squares correspond to the 6 BL runs
• First 3 over Atlantic
1
23
Contrast between Ocean and Land BL Data
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Flight Track with Color-coded Altitude
45
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35
30
25
-90 -85 -80 -75 -70
13
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1617
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4
2
0
Altitude km
Smaller blue squares correspond to the 6 BL runs
• First 3 over Atlantic
• Last 3 over Land
1
23
4
5
6
Contrast between Ocean and Land BL Data
1
23
45
6
1
23
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
45
40
35
30
25
-90 -85 -80 -75 -70
13
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1617
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12
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2
0
Altitude km
1
23
45
6
1
23
4
56
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
45
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35
30
25
-90 -85 -80 -75 -70
13
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Altitude km
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Ethyne Alt P (km)
UTC
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
Tracers: Combustion (ethyne)
0.0
50.0
100.0
150.0
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250.0
300.0
0
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Ethyne Alt P (km)
UTC
15
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30
35
0
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CH2Cl2 Alt P (km)
UTC
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
Tracers: Combustion (ethyne)
& industrial (CH2Cl2)
0.0
50.0
100.0
150.0
200.0
250.0
300.0
0
2
4
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
Ethyne Alt P (km)
UTC
15
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30
35
0
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CH2Cl2 Alt P (km)
UTC
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
Tracers: Combustion (ethyne)
& industrial (CH2Cl2)
• clean MBL
0.0
50.0
100.0
150.0
200.0
250.0
300.0
0
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Ethyne Alt P (km)
UTC
15
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30
35
0
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CH2Cl2 Alt P (km)
UTC
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
Tracers: Combustion (ethyne)
& industrial (CH2Cl2)
• clean MBL
• similar enhancements in the polluted CBL
0.0
0.2
0.4
0.6
0.8
1.0
0
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CH3I Alt P (km)
UTC
4BL leg #4 shows influence from ocean
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
0.0
0.2
0.4
0.6
0.8
1.0
0
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CH3I Alt P (km)
UTC
0
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3500
0
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
IsopreneAlt P (km)
UTC
4BL leg #4 shows influence from ocean and land
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
0.0
0.2
0.4
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0.8
1.0
0
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CH3I Alt P (km)
UTC
0
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3500
0
2
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
IsopreneAlt P (km)
UTC
4
4
BL leg #4 shows influence from ocean and land
- as in trajectory
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
High Levels of organic Br gases from Caribbean
0
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0
2
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CHBr3CH2Br2
Alt P (km)
UTC
33
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
0
2
4
6
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12
14
0
2
4
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CHBr3CH2Br2
Alt P (km)
UTC
3
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
6
8
10
12
14
16
18
20
0
2
4
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CH3Br Alt P (km)
UTC
4 High MeBr associated with ag. regions of FL
Contrast between Ocean and Land BL Data
High Levels of organic Br gases from Caribbean
4
3
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
0
5
10
15
20
0
2
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
i-PrONO22-BuONO2
Alt P (km)
UTC
Leg 4 also has high levels of secondary pollutants
4
4
In BL for past 10 days
0
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200
0
2
4
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
i-PrONO22-BuONO2
Alt P (km)
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
0
5
10
15
20
0
2
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
i-PrONO22-BuONO2
Alt P (km)
UTC
0
1,000
2,000
3,000
4,000
5,000
6,000
7,000
8,000
0
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1,000
1,200
1,400
1,600
13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
acetone_Singh Acetone_UCI
UTC
4
Leg 4 also has high levels of secondary pollutants
4
4
In BL for past 10 days
New UCI acetone data (unarchived) - compare to Singh group acetone
0
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100
150
200
0
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
i-PrONO22-BuONO2
Alt P (km)
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
0
5
10
15
20
0
2
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10
13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
i-PrONO22-BuONO2
Alt P (km)
UTC
0
1,000
2,000
3,000
4,000
5,000
6,000
7,000
8,000
0
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800
1,000
1,200
1,400
1,600
13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
acetone_Singh Acetone_UCI
UTC
4
Leg 4 also has high levels of secondary pollutants
4
4
In BL for past 10 days
New UCI acetone data (unarchived) - compare to Singh group acetone
• strong similarities with i-PrONO2
• both high in Leg #4
350
355
360
365
370
375
380
0
2
4
6
8
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12
13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CO2 (ppmv)
Alt P (km)
UTC
300
350
400
450
500
0
2
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12
13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
OCS Alt P (km)
UTC
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
Both CO2 and OCS show draw-down over land
350
355
360
365
370
375
380
0
2
4
6
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CO2 (ppmv)
Alt P (km)
UTC
300
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500
0
2
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
OCS Alt P (km)
UTC
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
Both CO2 and OCS show draw-down over land
Uptake of OCS and CO2 has common pathway
•through open stomata•transport resistances virtually the same. [Goldan et al. 1988]
350
355
360
365
370
375
380
0
2
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CO2 (ppmv)
Alt P (km)
UTC
300
350
400
450
500
0
2
4
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
OCS Alt P (km)
UTC
Both CO2 and OCS show draw-down over land
Uptake of OCS and CO2 has common pathway
•through open stomata•transport resistances virtually the same. [Goldan et al. 1988]
•Regional variation of OCS uptake uncertain [Kettle et al., 2002]
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
Comparison of TRACE-P and INTEX
Summer vegetation sink for CO2 main difference between missions? (Stephanie/Melody???)
340 350 360 370 380 390 400
INTEX (Summer)TRACE-P (Spring)
0
2
4
6
8
10
12
Mixing Ratio (ppmv)
CO2
Altitude km
Comparison of TRACE-P and INTEX
Like CO2 see vegetation sink for OCS in summer over the US
300 400 500 600 700 800 900 1000
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
OCS
Altitude km
Comparison of TRACE-P and INTEX
Like CO2 see vegetation sink for OCS in summer over the US
Also:
• US much smaller source for OCS?? (much less and cleaner coal
burning)?
300 400 500 600 700 800 900 1000
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
OCS
Altitude km
350
355
360
365
370
375
380
0
2
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CO2 (ppmv)
Alt P (km)
UTC
300
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450
500
0
2
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
OCS Alt P (km)
UTC
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
Both CO2 and OCS show draw-down over land
- Revisited!
450
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600
650
0
2
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13:00:00 15:00:00 17:00:00 19:00:00 21:00:00
CH3Cl Alt P (km)
UTC
350
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365
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380
0
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CO2 (ppmv)
Alt P (km)
UTC
300
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500
0
2
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OCS Alt P (km)
UTC
INTEX-NA Flight 12July 25, 2004 (4th Pease Local)
Contrast between Ocean and Land BL Data
Both CO2 and OCS show draw-down over land
- Revisited!
MeCl also shows clear evidence of uptake over land
•This pathway less well known
>Soil sink?
>Vegetation sink?
Comparison of TRACE-P and INTEX
• US much smaller source for MeCl than Asia (much less biomass/biofuel/coal burning)??
400 500 600 700 800 900100011001200
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
CH3Cl
Altitude km
Comparison of TRACE-P and INTEX
400 500 600 700 800 900100011001200
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
CH3Cl
Altitude km
• US much smaller source for MeCl than Asia (much less biomass/biofuel/coal burning)??
• MeCl frequently influenced by PBL draw-down
Comparison of TRACE-P and INTEX
400 500 600 700 800 900100011001200
TRACE-P (Spring)INTEX (Summer)
0
2
4
6
8
10
12
Mixing Ratio (pptv)
CH3Cl
Altitude km
• US much smaller source for MeCl than Asia (much less biomass/biofuel/coal burning)??
• MeCl frequently influenced by PBL draw-down
• less useful as a biomass burning tracer
54
52
50
48
46
44
42
40
38
-75 -70 -65 -60 -55 -50 -45
14
15 16 17
18
19
20
2122
500
400
300
200
100
0
Ethyne pptv
54
52
50
48
46
44
42
40
38
-75 -70 -65 -60 -55 -50 -45
14
1516 17
18
19
20
2122
12
10
8
6
4
C2Cl4
pptv
Ethyne
C2Cl4
Biomass Burning TracersINTEX-NA Flight 9
July 18, 2004 (1st Pease Local)
Alaska Fire Plume
Alaska Fire Plume
54
52
50
48
46
44
42
40
38
-75 -70 -65 -60 -55 -50 -45
14
1516 17
18
19
20
2122
570
560
550
540
530
520
510
500
CH3Cl
54
52
50
48
46
44
42
40
38
-75 -70 -65 -60 -55 -50 -45
14
15 16 17
18
19
20
2122
500
400
300
200
100
0
Ethyne pptv
Ethyne
CH3Cl
Biomass Burning TracersINTEX-NA Flight 9
July 18, 2004 (1st Pease Local)
Alaska Fire Plume
Alaska Fire Plume
400
450
500
550
600
650
0 100 200 300 400 500 600CO (ppbv)
CH3
Cl (pptv)
Biomass Burning TracersAll INTEX Data
• CO: high in major BB Influence (CO >160 ppb)
400
450
500
550
600
650
0 100 200 300 400 500 600CO (ppbv)
CH3
Cl (pptv)
Biomass Burning TracersAll INTEX Data
0
10
20
30
40
50
60
70
80
0 100 200 300 400 500 600CO (ppbv)
C2
Cl4
(pptv)
• CO: high in major BB Influence (CO >160 ppb)
• C2Cl4: high for urban/industrial
Urban/industrial
400
450
500
550
600
650
0 100 200 300 400 500 600CO (ppbv)
CH3
Cl (pptv)
Biomass Burning TracersAll INTEX Data
0
10
20
30
40
50
60
70
80
0 100 200 300 400 500 600CO (ppbv)
C2
Cl4
(pptv)
• CO: high in major BB Influence (CO >160 ppb)
• C2Cl4: high for urban/industriallow for pure BB
(select for C2Cl4 <10 pptv)
Urban/industrial
Biomass Burning?
400
450
500
550
600
650
0 100 200 300 400 500 600CO (ppbv)
CH3
Cl (pptv)
Biomass Burning TracersAll INTEX Data
0
10
20
30
40
50
60
70
80
0 100 200 300 400 500 600CO (ppbv)
C2
Cl4
(pptv)
• CO: high in major BB Influence (CO >160 ppb)
• C2Cl4: high for urban/industriallow for pure BB
(select for C2Cl4 <10 pptv)
• Large range of CH3Cl for low C2Cl4
Urban/industrial
Biomass Burning?
0
10
20
30
40
50
60
70
80
400 450 500 550 600 650CH
3Cl (pptv)
C2
Cl4
(pptv)
Biomass Burning TracersAll INTEX Data Data Subset: CO >160 ppb, C2Cl4 <10 pptv
100 200 300 400 500 600460
480
500
520
540
560
580
600
CO (ppbv)
CH3
Cl (pptv)
400
450
500
550
600
650
0 100 200 300 400 500 600CO (ppbv)
CH3
Cl (pptv)
0
10
20
30
40
50
60
70
80
0 100 200 300 400 500 600CO (ppbv)
C2
Cl4
(pptv)
0
10
20
30
40
50
60
70
80
400 450 500 550 600 650CH
3Cl (pptv)
C2
Cl4
(pptv)
Few data that look like BB
Biomass Burning TracersAll INTEX Data Data Subset: CO >160 ppb, C2Cl4 <10 pptv
100 200 300 400 500 600460
480
500
520
540
560
580
600
CO (ppbv)
CH3
Cl (pptv)
400
450
500
550
600
650
0 100 200 300 400 500 600CO (ppbv)
CH3
Cl (pptv)
0
10
20
30
40
50
60
70
80
0 100 200 300 400 500 600CO (ppbv)
C2
Cl4
(pptv)
0
10
20
30
40
50
60
70
80
400 450 500 550 600 650CH
3Cl (pptv)
C2
Cl4
(pptv)
Few data that look like BB
0 200 400 600 800 1000 1200 1400 1600460
480
500
520
540
560
580
600
CH3CN (pptv)
CH3
Cl (pptv) MeCl vs. Acetonitrile
Other Tracers:
Biomass Burning TracersAll INTEX Data Data Subset: CO >160 ppb, C2Cl4 <10 pptv
100 200 300 400 500 600460
480
500
520
540
560
580
600
CO (ppbv)
CH3
Cl (pptv)
400
450
500
550
600
650
0 100 200 300 400 500 600CO (ppbv)
CH3
Cl (pptv)
0
10
20
30
40
50
60
70
80
0 100 200 300 400 500 600CO (ppbv)
C2
Cl4
(pptv)
0
10
20
30
40
50
60
70
80
400 450 500 550 600 650CH
3Cl (pptv)
C2
Cl4
(pptv)
Few data that look like BB
0 200 400 600 800 1000 1200 1400 1600460
480
500
520
540
560
580
600
CH3CN (pptv)
CH3
Cl (pptv) MeCl vs. Acetonitrile
Other Tracers:
0 500 1000 1500 2000 2500
HCN_CITHCN_Singh
460
480
500
520
540
560
580
600
HCN (pptv)
CH3
Cl (pptv)MeCl vs. HCN
Biomass Burning TracersAll INTEX Data Data Subset: CO >160 ppb, C2Cl4 <10 pptv
100 200 300 400 500 600460
480
500
520
540
560
580
600
CO (ppbv)
CH3
Cl (pptv)
400
450
500
550
600
650
0 100 200 300 400 500 600CO (ppbv)
CH3
Cl (pptv)
0
10
20
30
40
50
60
70
80
0 100 200 300 400 500 600CO (ppbv)
C2
Cl4
(pptv)
0
10
20
30
40
50
60
70
80
400 450 500 550 600 650CH
3Cl (pptv)
C2
Cl4
(pptv)
Bottom Line:
0 200 400 600 800 1000 1200 1400 1600460
480
500
520
540
560
580
600
CH3CN (pptv)
CH3
Cl (pptv)
0 500 1000 1500 2000 2500
HCN_CITHCN_Singh
460
480
500
520
540
560
580
600
HCN (pptv)
CH3
Cl (pptv)
• No really great BB tracers during INTEX (?)
• Not much BB influence directly sampled during INTEX
“SW” Pollution
Mid-Continental Oil FieldEthane from surface study
[Katzenstein et al., 2003]
SW pollution characterized by:
• High levels of alkanes and daughter alkyl nitrates
• Low levels of urban tracers (such as CO)
“SW” Pollution55
50
45
40
35
30
25
-140 -120 -100 -80 -60 -40
24
22
20
18
16
14
Ratio Ethane/CO (pptv/ppbv)
Air masses with “SW” style oil and gas pollution were widespread during INTEX-NA
• sampled on >15 legs on 10 flights
0
1000
2000
3000
4000
5000
0
2
4
6
8
10
12
15:00:00 17:00:00 19:00:00 21:00:00 23:00:00
EthanePropaneEthyne
Alt P
UTC
INTEX Flight 7July 12, 2004
“SW” Pollution
0
1000
2000
3000
4000
5000
0
2
4
6
8
10
12
15:00:00 17:00:00 19:00:00 21:00:00 23:00:00
EthanePropaneEthyne
Alt P
UTC
INTEX Flight 7July 12, 2004
"SW Pollution"- High ethane & propane- Low ethyne (& CO)
“SW” Pollution
0
1000
2000
3000
4000
5000
0
2
4
6
8
10
12
15:00:00 17:00:00 19:00:00 21:00:00 23:00:00
EthanePropaneEthyne
Alt P
UTC
INTEX Flight 7July 12, 2004
"SW Pollution"- High ethane & propane- Low ethyne (& CO)
“SW” Pollution
Terrestrial Influences on Atmospheric Carbonyl Sulfide and Methyl Chloride over the US during Summertime”, Blake and Blake et al.,
”More Evidence for the Widespread Transport of Light Alkane Pollution from the Southwestern US”, Young, Blake and Blake, Model group, et al.,
"Gaseous Tracers of Convective Uplift during INTEX NA”, Blake and Blake and Fuelburg et al.,
"Coastal Emissions of Bromoform and Dibromomethane during INTEX NA"Blake and Blake et al.,
"Evidence for Long-range Transport of Asian Emissions to the US During Summer”, Blake and Blake and Fuelburg et al.,
First Cut Papers List