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Maria Navarro 1 , E. Atlas 1 , R. Lueb 1 , R. Hendershot 2 , S. Gabbard 2 , X. Zhu 1 , L. Pope 1

Trace gases measurements from the Global Hawk Whole Air Sampler during the Airborne Tropical Tropopause Experiment 2013 ( ATTREX-2) . Maria Navarro 1 , E. Atlas 1 , R. Lueb 1 , R. Hendershot 2 , S. Gabbard 2 , X. Zhu 1 , L. Pope 1

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Maria Navarro 1 , E. Atlas 1 , R. Lueb 1 , R. Hendershot 2 , S. Gabbard 2 , X. Zhu 1 , L. Pope 1

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  1. Trace gases measurements from the Global Hawk Whole Air Sampler during the Airborne Tropical Tropopause Experiment 2013 (ATTREX-2) • Maria Navarro1, E. Atlas1, R. Lueb1, R. Hendershot2, S. Gabbard2, X. Zhu1, L. Pope1 • Division of Marine and Atmospheric Chemistry, Rosenstiel School of Marine and Atmospheric Science, University of Miami, Miami, Florida, USA • 2) Atmospheric Chemistry Division, National Center for Atmospheric Research, Boulder, Colorado, USA with data from MMS and NOAA O3 groups

  2. OBJECTIVES • Characterize variability and distribution of organic trace gases in the UT/LS • Evaluate the chemical gradients in the TTL • Evaluate the budget and partitioning of organic bromine • Examine source signatures and input of natural vs. anthropogenic trace species in the tropical UT

  3. GWAS on ATTREX-2 388 samples 45 vertical profiles RF01 RF03 Altitude (m) RF04 RF05 RF06 UTC (sec)

  4. ATTREX-2 TRACE GAS SPECIES FROM GWAS Longer Lived Species Shorter Lived Species Shorter Lived Species Chlorofluorocarbons Yrs S CFC-11 50 A CFC-12 102 A CFC-113 85 A Halons Halon 1211 20 A Halon 2402 20 A Hydrochlorofluoroarbons/ Hydrofluorocarbons HCFC_141b 9.4 A HCFC-22 13 A HCFC_142b 19.5 A Solvent Carbon Tetrachloride 40 A Methyl chloroform 4.8 A Other Carbonyl Sulfide (COS) 30 N/A/B Methyl Chloride 1.5 N/B Organic nitrates Methyl nitrate 0.08 A/N Ethyl nitrate 0.04 A/N Propyl nitrate 0.03 A/N Non- Methane Halocarbons Ethane (C2H6) 0.2 A Ethyne 0.06 A/B Propane 0.04 A Benzene 0.04 A/B Others 1,2 dichloro ethane 0.3 A Chlorobenzene 0.05 A Solvents YrsS Methylene Chloride 0.3 A Chloroform 0.4 A/N Tetrachloroethylene 0.3 A Trichloroethylene 0.02 A Methyl Halides Bromoform 0.1 N Methyl Bromide 0.8 A/N/B Methylene Bromide 0.4 N Methyl Iodide 0.01 N CHxBryClz 0.1 N Sources A= antropogenic/industrial N= natural/marine B=Biomass burning

  5. AREA OF ANALYSIS 18.3 ALT (Km) 27.0 LAT (deg)

  6. VERTICAL CHEMICAL GRADIENTS LONGER LIVED SPECIES Bins of 10K θ 4% 2% 2% 7% 4% 6%

  7. VERTICAL CHEMICAL GRADIENTS SHORTER LIVED SPECIES Bins of 10K θ 28% 27% 78% 74%

  8. VERTICAL CHEMICAL GRADIENTS SHORTER LIVED SPECIES Bins of 10K θ 75% 80% 69% 36%

  9. (?) ARTIFACT

  10. FRACTIONS AT 366 K 7% 71% 75%

  11. BROMINATED SPECIES Longer Lived Species Shorter Lived Species Shorter Lived Species Halons Halon 1211 Halon2402 Halon 1301 Chlorofluorocarbons CFC-11 50 A CFC-12 102 A CFC-113 85 A Hydrochlorofluoroarbons/ Hydrofluorocarbons HCFC_141b 9.4 A HCFC-22 13 A HCFC_142b 19.5 A Solvent Carbon Tetrachloride 40 A Methyl chloroform 4.8 A Other Carbonyl Sulfide (COS) 30 N/A/B Methyl Chloride 1.5 N/B Yrs S 20 A 20 A Organic nitrates Methyl nitrate 0.08 A/N Ethyl nitrate 0.04 A/N Propyl nitrate 0.03 A/N Non- Methane Halocarbons Ethane (C2H6) 0.2 A Ethyne 0.06 A/B Propane 0.04 A Benzene 0.04 A/B Others 1,2 dichloro ethane 0.3 A Chlorobenzene 0.05 A Methyl Halides Bromoform Methyl Bromide Methylene Bromide Methyl Iodide CHxBryClz Solvents YrsS Methylene Chloride 0.3 A Chloroform 0.4 A/N Tetrachloroethylene 0.3 A Trichloroethylene 0.02 A CBrClF2 0.1 N 0.8 A/N/B 0.4 N 0.01 N 0.1 N CHBr3 CH2Br2 C2Br2F4 CBrF3 Methyl Bromide CH3Br • CHBrCl2 Bromodichloromethane • CHBr2Cl Dibromochloromethane • CH2BrCl Bromochloromethane GROUPS FOR ORGANIC BROMINE BUDGET TOTAL HALONS: HALON 1211+ (2*HALON 2402)+ HALON 1301 CH3Br= CH3Br TOTAL SHOTER LIVED SPECIES (SLS) = (3* CHBr3)+ (2* CH2Br2) + CHBrCl2+ (2*CHBr2CL)+ CH2BrCL Sources A= antropogenic/industrial N= natural/marine B=Biomass burning

  12. TOTAL ORGANIC BROMINE BUDGET Bins of 10K θ TOTAL ORGANIC Br TOTAL HALONS CH3Br TOTAL SLS

  13. ORGANIC BROMINE TENDENCY CR-AVE 2006 ATTREX 2013 pmol Br/mol Measurements Bins of 10K θ Total Organic Bromine Total Halons Total SLS CH3Br Total Organic Bromine Halons Short lived Br CH3Br

  14. ORGANIC BROMINE CONTRIBUTIONS GROUP CONTRIBUTIONS 375-395 K 350-370 K 35% 41% 37% 43% Total Halons Total SLS CH3Br 24% 20% SHORTER LIVED SPECIES DISTRIBUTIONS CH2BrCl CH2Br2 CHBrCl2 6% 5% 31% 41% 54% 46% 6% 6% CHBr2Cl CHBr3 3% 2%

  15. TTL ORGANIC BROMINE COMPARISON

  16. ORGANIC BROMINE FROM CAMPAIGNS 375-395 K 350-370 K ATTREX 2013 10 % SLS 15.2% H1301 35% 41% 37% 23.9% H1211 43% Total Halons Total SLS CH3Br 45.8% CH3Br 24% 20% 2.3% sls 5.2 % CH2Br2 5.2 % H2401 5.2 % H2401 CR-AVE 2006 TC4 2007 17% H1301 5% 47% CH3Br 24% H1211 44% 43% 46%

  17. SHORTER LIVED SPECIES COMPARISON ATTREX 2013 375-395 K 350-370 K CR-AVE 2006 CH2BrCl CH2Br2 CHBrCl2 3.3% 4.1% 6% 5% 6.7% 17.4% 31% 41% 3.7% 54% 46% 6% 6% CHBr2Cl CHBr3 C2H4Br2 Halothane 64.5% 3% 2% WHY THE DIFFERENCES?

  18. ATTREX-2 O3 MIXING RATIOS

  19. O3 AND SLBr SPECIES COMPARISON

  20. NATURAL AND ANTHROPOGENIC SPECIES Longer Lived Species Shorter Lived Species Shorter Lived Species Chlorofluorocarbons Yrs S CFC-11 50 A CFC-12 102 A CFC-113 85 A Halons Halon 1211 20 A Halon 2402 20 A Hydrochlorofluoroarbons/ Hydrofluorocarbons HCFC_141b 9.4 A HCFC-22 13 A HCFC_142b 19.5 A Solvent Carbon Tetrachloride 40 A Methyl chloroform 4.8 A Other Carbonyl Sulfide (COS) 30 N/A/B Methyl Chloride 1.5 N/B Organic nitrates Methyl nitrate 0.08 A/N Ethyl nitrate 0.04 A/N Propyl nitrate 0.03 A/N Non- Methane Halocarbons Ethane (C2H6) 0.2 A Ethyne 0.06 A/B Propane 0.04 A Benzene 0.04 A/B Others 1,2 dichloro ethane 0.3 A Chlorobenzene 0.05 A Solvents YrsS Methylene Chloride 0.3 A Chloroform 0.4 A/N Tetrachloroethylene 0.3 A Trichloroethylene 0.02 A Methyl Halides Bromoform 0.1 N Methyl Bromide 0.8 A/N/B Methylene Bromide 0.4 N Methyl Iodide 0.01 N CHxBryClz0.1 N Sources A= anthropogenic/industrial N= natural/marine B=Biomass burning

  21. LATITUDINAL DISTRIBUTION ETHANE TETRACHLOROETHYLENE pptv pptv BROMOFORM METHYL NITRATE pptv pptv

  22. SUMMARY • LONGER AND SHORTER LIVED SPECIES • Mixing ratios of longer lived species change by less than 10%, while the mixing ratios of shorter lived species change around 70 to 75 % in the TTL • ORGANIC BROMINE BUDGET • Total organic bromine for ATTREX 2013 range between 19.5± 1.4 and 18.3 ± 1.2 pmol of Br/mol for potential temperature ranges of 350-370 and 375-395 K respectively. This value is also in similar to that found in previous campaigns • However, contributions of SLS to the total organic bromine budget are slightly higher during ATTREX 2013. Delivery of 4.8 ±0.7 pmol/mol of organic bromine to the base of the TTL is estimated. Further analysis is needed. • NATURAL AND ANTHROPOGENIC SPECIES • Overall distributions reflect emission sources and lifetimes. Origins of higher concentration features will be diagnosed with trajectory analysis and other tracer correlations.

  23. EXTRA SLIDES

  24. GLOBAL HAWK WHOLE AIR SAMPLER (GWAS) 90 sample canisters (custom Entech Inst.) High vacuum solenoid valves (Parker Series 99) Dual air compressor (Metal Bellows) Computer controller (Custom built) Fig 1: GWAS inside of the Global Hawk (area 61)

  25. GLOBAL HAWK WHOLE AIR SAMPLER (GWAS) • Includes: • High Performance Gas Chromatograph / Mass Selective Detector/ Flame ionization detector / electron capture detector • Unity 2TM Thermal Desorber • CIA Advantage • Variety of compounds analyzed with this instrument ( hydrocarbons, halocarbons, organic nitrates, solvents) • Mixing ratios are calculated based on previous standard measurements and calibrations

  26. LONGITUDINAL DISTRIBUTION

  27. VERTICAL CHEMICAL GRADIENTS

  28. VERTICAL CHEMICAL GRADIENTS

  29. VERTICAL CHEMICAL GRADIENTS

  30. VERTICAL CHEMICAL GRADIENTS

  31. correlations

  32. SF6 N2O

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