Halogen Chemistry at NCAR D. Kinnison, J.Orlando, J-F Lamarque, S. Schaffler, G. Brasseur, R. Garcia, et al… NCAR Alfonso Saiz-Lopez and S. Sander JPL.

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Halogen Chemistry at NCAR D. Kinnison, J.Orlando, J-F Lamarque, S. Schaffler, G. Brasseur, R. Garcia, et al… NCAR Alfonso Saiz-Lopez and S. Sander JPL 11 February D. Kinnison, J.Orlando, J-F Lamarque, S. Schaffler, G. Brasseur, R. Garcia, et al… NCAR Alfonso Saiz-Lopez and S. Sander JPL 11 February

Outline Modeling Tools… Updated Chemistry. UTLS Studies… Ozone Trends (stratosphere; CCMVal) Dynamics and Transport Evaluations of CCMs in UTLS Support START08 and UTLS initiative Polar Troposphere… Ozone Loss (from Bromine Explosions) Support OASIS 2009 Importance of Iodine chemistry (ARCTAS)

+ NCAR Community Climate System Model Atmosphere CAM3 (WACCM3) OceanSea Ice Land Used in decadal and longer simulations

NCAR Community Climate System Model Atmosphere CAM3 (WACCM3) GEOS-5 Met. Fields (U, V, T, etc…). Advantage: Allows direct comparisons with observations. Have fields from 2004-present day (Aura) Process oriented evaluation: SPARC CCMVal

Middle Atmosphere Mechanism (57 species; 148 Gas-phase; 17 Heterogeneous; 47 Photolytic) Long-lived Species: (19-species) Misc:CO 2, CO, CH 4, H 2 O, N 2 O, H 2, O 2 CFCs: CCl 4, CFC-11, CFC-12, CFC-113 HCFCs: HCFC-22 Chlorocarbons:CH 3 Cl, CH 3 CCl 3, Bromocarbons: CH 3 Br Halons: H-1211, H-1301 Constant Species:M, N 2 Short-lived Species: (38-species) O X : O 3, O, O( 1 D) NO X :N, N ( 2 D), NO, NO 2, NO 3, N 2 O 5, HNO 3, HO 2 NO 2 ClO X :Cl, ClO, Cl 2 O 2, OClO, HOCl, HCl, ClONO 2, Cl 2 BrO X :Br, BrO, HOBr, HBr, BrCl, BrONO 2 HO X :H, OH, HO 2, H 2 O 2 HC Species:CH 2 O, CH 3 O 2, CH 3 OOH Ions: N +, N 2 +, NO +, O +, O 2 + Radiatively Active

Whole Atmosphere Mechanism (115 species; 287 Gas-phase; 17 Heterogeneous; 72 photolytic) Additional Surface Source Gases (14 additional) … NHMCs:CH 3 OH, C 2 H 6, C 2 H 4, C 2 H 5 OH, CH 3 CHO C 3 H 8, C 3 H 6, CH 3 COCH 3 (Acetone) C 4 H 8 (BIGENE), C 4 H 8 O (MEK) C 5 H 8 (Isoprene), C 5 H 12 (BIGALK) C 7 H 8 (Toluene) C 10 H 16 (Terpenes) Radicals:Approx. 44 additional species Total ~140 species Next: Additional Organic Bromine (~ 7 species) Organic Iodine Species (~ 8 species) Additional IO X and BrO X radicals (~10 species)

Outline Modeling Tools… Updated Chemistry. UTLS Studies… Ozone Trends (stratosphere; CCMVal) Dynamics and Transport Evaluations of CCMs in UTLS Support START08 and UTLS initiative Polar Troposphere… Ozone Loss (from Bromine Explosions) Support OASIS 2009 Importance of Iodine chemistry (ARCTAS)

Total Inorganic Bromine Loading Taken from Chapter 2, VSLS, WMO, 2006

Total Inorganic Bromine Loading Taken from Chapter 2, VSLS, WMO, 2006

Ozone Trends Taken from Chapter 2, VSLS, WMO, 2006 CCMVal 2008/09 WACCM3 will be used to investigate the impact of enhanced BrOy on model derived ozone trends.

Organic Halogens with varying lifetimes can also tell us about transport pathways in the atmosphere and how well models represent these pathways.

Very Short-lived Substances (VSLS) SG = Organic VSL Source Gas PG = VSL Product gas Xy VSLS = inorganic halogens from organic SG degradation.

TC4, Whole Air Sampler, Schauffler, Atlas, et al., AGU, 2007 Flt km Bromofor m pptv pptv 10 km Convection lofting VSLS into the TTL. Influencing the total inorganic bromine abundance. Transported to ExTL? Org. BrOy Good Profile Data!

Field experiment: Stratosphere-Troposphere Analyses of Regional Transport (START-08)- Spring Goal: Study the transport characteristics of the ExUTLS region. START08 will take advantage of the capabilities of HIAPER and set the stage for more complex and comprehensive field studies of UTLS chemistry and microphysics. START 2008 Modeling: WACCM3 will be used. Chemical characterization of the UTLS will be evaluated. Transport and mixing processes will be examined.

Halogenated Very Short-lived Substances (VSLS) currently being added the WA3 UTLS mechanism Source GasFormula Local Lifetime (days) Main Loss processes WAS BromochloromethaneCH 2 BrCl150OH  Trichloromethane (chloroform) CHCl 3 150OH  Methylene chlorideCH 2 Cl 2 140OH  DibromomethaneCH 2 Br 2 120OH  BromodichloromethaneCHBrCl 2 78OH, hv  DibromochloromethaneCHBr 2 Cl69hv, OH  Tribromomethane (bromoform) CHBr 3 26hv  VSL Organic Bromine Species

Outline Modeling Tools… Updated Chemistry. UTLS Studies… Ozone Trends (stratosphere; CCMVal) Dynamics and Transport Evaluations of CCMs in UTLS Support START08 and UTLS initiative Polar Troposphere… Ozone Loss (from Bromine Explosions) Support OASIS 2009 Importance of Iodine chemistry (ARCTAS)

Ocean sea ice, ~1-2m thick Cl - Br - O3O3 BrO - H+H+ HOBr Br - Br 2 snowpack Br 2 hυhυ 2Br O3O3 BrO HO 2 HOBr Hg HgBr Br HgBr 2 Hg OHgBr HO 2 HOHgBr “bromine explosion” BrX? Hg? O3?O3? Potential ACD Contribution: OH, HO 2, RO 2, VOC/OVOC, CH 2 O H 2 SO 4, aerosol properties, radiation Fast O 3, NO x /NO y, PAN Models (1-D, 3-D) Courtesy of J. Orlando

OASIS Program (Ocean/Atmosphere/Sea Ice/Snowpack) “OASIS program was created to coordinate efforts aimed at determining the importance of OASIS chemical, physical and biological exchange processes on tropospheric chemistry, the cryosphere, and the marine environment”. To address these issues, NCAR ACD is planning to participate in a field campaign under the OASIS umbrella for Spring 2009; at Barrow, AK and the Navy Ice Camp located NE of Barrow. The deployment will consist of measurements of key chemical species active in the Arctic boundary layer: HOx, NOx/NO Y, BrOx, O 3, halocarbons, organics, and aerosols Learn more about the oxidative capacity of the Arctic Troposphere and how bromine explosions impact depletion of Hg  from the atmosphere.

Modeling support for OASIS A connection will be initiated between the OASIS measurement community and the global modeling community at NCAR to examine the impact of of OASIS exchange processes on air quality. Parameterizations of the emissions of halogens and NOx will be incorporated into CAM-CHEM for studies of regional- and hemispheric-scale air quality impacts. We will also conduct climate impacts using CCSM (with chemistry). A major initial focus will be on changing sea ice characteristics, and in particular, first year sea ice which has been shown to correlate with halogen activation. More first year sea ice in the future might mean more ozone depletion.

Trends in Sea Ice Extent, IPCC WG1, Multi-model simulated anomalies.

How important are iodine species in affecting ozone loss in the polar lower troposphere? ACD Collaboration with Alfonso Saiz-Lopez and Stan Sander (JPL).

Observations from Space: Saiz-Lopez et al., GRL, 34, 2007

IO and BrO similar in Antarctica From Saiz-Lopez et al., Boundary Layer Halogen in Coastal Antarctica, Science, Bromine oxide comes from bromine ions found in sea ice. Iodine oxide most likely comes from marine organisms such as phytoplankton and algae, which concentrate the iodide ions that are eventually released in the atmosphere.

Phytoplankton (under Antarctic sea ice) From A. Saiz-Lopez IO has not been observed in the Arctic?!

Source GasFormula Local Lifetime (days) Main Loss processes WAS Methyl iodideCH 3 I7hv  TrifluoroiodomethaneCF 3 I4hv? Ethyl iodideC2H5IC2H5I4hv? 2-Iodopropanei-C 3 H 7 I1.2hv? 1-Iodopropanen-C 3 H 7 I0.5hv? ChloroiodomethaneCH 2 ClI0.1hv? BromoiodomethaneCH 2 BrI0.04hv? DiiodomethaneCH 2 I hv? VSL Iodine Species Halogenated Very Short-lived Substances (VSLS) currently being added the CAM-CHEM, WA3 UTLS mechanism

Summary Implementing organic halogen species in CAM-CHEM / WACCM3. Approximately 140 species total. Examine the impact of enhance BrOy on model derived ozone trends. Connected with ongoing WACCM3 CCMVal activities. Use VSL organic halogens to understand transport pathways in the UTLS region and evaluate model representation of these pathways. Support the START08 field mission. Use specified Met version of CAM-CHEM/WACCM3. Model Halogen activation in polar troposphere. Support both OASIS 2009 (and ARCTAS) field campaigns. Investigate both air quality and climate change issues.

The End