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TROPOSPHERIC CHEMISTRY

TROPOSPHERIC CHEMISTRY TOPSE: Tropospheric Ozone Production About the Spring Equinox Example of a division lead community initiative supported by NSF. The benefit of a critical mass of observational and modeling capabilities. Training opportunity for several young university scientists.

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TROPOSPHERIC CHEMISTRY

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  1. TROPOSPHERIC CHEMISTRY • TOPSE: Tropospheric Ozone Production About the Spring Equinox • Example of a division lead community initiative supported by NSF. • The benefit of a critical mass of observational and modeling capabilities. • Training opportunity for several young university scientists. • Provides useful data for future plans UT/LS. • HANK: ACD’s Regional Chemistry-Transport Model • Application to field campaign analysis • Community based regional model. • ACD Contributions to the NASA TRACE-P Campaign • Leveraging of NSF core funds to develop instruments and gain access to unique capabilities. • Direct involvement of several universities with ACD Investigators • MIRAGE : Megacity Impacts on the Regional And Global Environment • a new initiative with significant societal importance. • Potential for substantial University involvement. • Reactive Carbon Research Initiative. • Building upon existing capabilities to address new issues. • Significant potential for University Involvement. • MOPITT:The MOPITT Experiment on Terra • Enhanced by close relations to ACD. MOZART & HANK data assimilation • A community service funded by NASA & Canadian Agencies

  2. Atmospheric Chemistry DivisionNational Center for Atmospheric Research TOPSE: Tropospheric Ozone Production About the Spring Equinox Chris Cantrell Scientist III – Atmospheric Radical Studies 24-26 October 2001, NSF Review TOPSE: Tropospheric Ozone Production about the Spring Equinox

  3. Primary Objective of TOPSE To investigate the chemical and dynamic evolution of tropospheric chemical composition over mid- to high-latitude continental North America during the winter/spring transition, with particular emphasis on the springtime ozone maximum in the troposphere. TOPSE: Tropospheric Ozone Production about the Spring Equinox

  4. Specific Scientific Questions TOPSE: Tropospheric Ozone Production about the Spring Equinox

  5. TOPSE Development Calendar ACD Internal Retreat March, 1997 Develop Preliminary White Paper Summer/Fall, 1997 Develop Science Proposal Winter, Spring, 1998 Letter of Intent to RAF April, 1998 TOPSE Proposal Distribution (NSF, Universities, Agencies) June, 1998 TOPSE Science Meeting Advertisement (EOS) Aug, 1998 TOPSE Open Workshop October, 1998 Proposal Submission to NSF Jan/Feb, 1999 OFAP Request for Advanced Reservation Spring, 1999 Director’s Fund Request (LIDAR installation) Spring, 1999 NSF Funding Approvals Fall, 1999 Aircraft Integration/Testing Dec, 1999/Jan, 2000 TOPSE Mission Feb – May, 2000 Mid-mission Science Meeting (NCAR) Mar, 2000 First Science Team Meeting (NCAR) Nov, 2000 AGU Special Session May, 2001 Second Science Team Meeting (Boston) May, 2001 Open Access to TOPSE Data Archive June, 2001 TOPSE Manuscripts to JGR (1st round) Oct, 2001 TOPSE: Tropospheric Ozone Production about the Spring Equinox

  6. TOPSE Investigators: Measurements MeasurementInvestigators Remote Ozone/Aerosols (DIAL)Browell et al., NASA Acidic Trace Gases/7-BeTalbot, Dibb, et al. UNH NMHC, Halocarbons, RONO2Blake et al., UCI NO2, PeroxynitratesCohen, Thornton et al., UCB Speciated PeroxidesHeikes, Snow, URI OH, H2SO4Eisele, Mauldin, NCAR HO2, RO2Cantrell, Stephens, NCAR HNO3Zondlo, NCAR NOx, NOy, OzoneRidley, Walega, NCAR CH2O, H2O2Fried, NCAR J valuesShetter, Lefer et al., NCAR PAN, PPNFlocke, Weinheimer, NCAR CO, N2OCoffey, Hannigan, NCAR Ultrafine Aerosols Weber, GIT Mission Scientists/P.I.sAtlas, Cantrell, Ridley, NCAR TOPSE: Tropospheric Ozone Production about the Spring Equinox

  7. TOPSE Investigators: Modeling/Collaboration Modeling/CollaborationInvestigators Regional/Forecast Model (HANK)Klonecki, Hess et al., NCAR Global Model AnalysisTie, Emmons et al., NCAR (MOZART)Brasseur et al., MPI Process and Radiation ModelsMadronich et al., NCAR Global Model/Process StudiesJacob, Evans, Harvard U. Stratosphere/Troposphere Exch.Allen, Pickering, U. Md. Regional/other ModelsWang et al., Rutgers U. Meteorological Forecast/Moody, Cooper, Wimmers, U.Va. Remote Sensing Ozonesonde NetworkMerrill, URI; Fast, PNWL GOME BrORichter, Burrows, U. Bremen Met. Forecasts (UT/LS) Newman, NASA Polar Sunrise Expt., 2000Shepson, Purdue; Bottenheim, Can. Met. Serv. TOPSE: Tropospheric Ozone Production about the Spring Equinox

  8. TOPSE Educational Activities Joel Thornton University of California-Berkeley Graduate student Rebecca Rosen University of California-Berkeley Graduate student Douglas Day University of California-Berkeley Graduate student Jennifer Murphy University of California-Berkeley Graduate student Daniel Murphy New Mexico Tech Undergraduate (Senior Thesis) Julie Snow University of Rhode Island Post-Doctoral Fan Lei University of Maryland Graduate Student Douglas Orsini Georgia Tech Post-Doctoral Baoan Wang Georgia Tech Graduate Student Mat Evans Harvard University Post-Doctoral Andrzej Klonecki NCAR ASP Craig Stroud NCAR ASP Brian Wert University of Colorado Graduate Student Anthony Wimmers University of Virginia Graduate Student Owen Cooper University of Virginia Graduate Student Jennifer Andrews University of Virginia Undergraduate Student Mark Zondlo NCAR ASP John Hair Old Dominion University Post-Doc Alton Jones Old Dominion University Graduate Student Aaron Katzenstein UCI Graduate student Barbara Barletta UCI Graduate student Simone Meinardi UCI Postdoc Alex Choi UCI Graduate student Changsub Shim Rutgers Univ Graduate student Linsey Debell Univ. New Hampshire Graduate student Eric Scheuer Univ. New Hampshire Graduate student Unfunded collaborators: Barkley Sive, Assistant Professor at Central Michigan University Oliver Wingenter, Assistant Professor at New Mexico Tech University Jodye Selco, Assistant Professor at The University of Redlands TOPSE: Tropospheric Ozone Production about the Spring Equinox

  9. TOPSE Flight Tracks TOPSE: Tropospheric Ozone Production about the Spring Equinox

  10. Some TOPSE Highlights • Seasonal variation in trace gases/aerosols • Evolution strong function of altitude and latitude • Decline in NMHC; Spring maximum in sulfate • PAN most significant odd-nitrogen component of NOy • Ozone evolution in the mid-troposphere • Increase about 20 ppb from Feb-May • Covariation in PANs, aerosols; no PV trend • Photochemical/surface sources implicated • Surface ozone depletion • Observations in early spring-May; broad geographical dist’n • Br-catalyzed ozone loss (as in earlier studies, but variable) • Long-range transport of depleted air suggested • Transport processes • Most sampled air masses representative of • background mid-troposphere • Distant pollution sources were encountered in layers TOPSE: Tropospheric Ozone Production about the Spring Equinox

  11. Some TOPSE Highlights (cont’d) • In-situ photochemical processes • Measured radicals consistent with models (so far) • Model/measurement of photolysis frequencies in agreement • Some model/measurement discrepancy for CH2O, H2O2, HNO3 • Calculated increase in in-situ ozone production in spring • Stratosphere-troposphere exchange • Remote sensing (satellite/lidar) indicate folds/streamers/STE(?) • In-situ encounters with lower stratosphere during flights • 7Be measurements suggest significant fraction of tropospheric ozone is from stratosphere. Seasonal modulation by photochemistry, but near constant ozone flux from stratosphere • 3-D modeling • HANK/MOZART • (Models used/evaluated extensively in campaign) • DAO/Harvard (underway) TOPSE: Tropospheric Ozone Production about the Spring Equinox

  12. Median Latitude and Altitude Profiles Latitude Profiles: Altitude Profiles (Blake – UCI) TOPSE: Tropospheric Ozone Production about the Spring Equinox

  13. Evolution of Sulfate Aerosol Vertical Distribution (Scheuer, Talbot, Dibb – UNH) TOPSE: Tropospheric Ozone Production about the Spring Equinox

  14. Ozone vertical profile: Evolution during winter-spring (Ridley, Walega) TOPSE: Tropospheric Ozone Production about the Spring Equinox

  15. Deployment 1 Deployment 3 Deployment 4 Deployment 5 Deployment 6 Deployment 7 Average Ozone Distributions During TOPSE (Browell et al., NASA) TOPSE: Tropospheric Ozone Production about the Spring Equinox

  16. Model calculated O3 production and loss 40 – 60 N; integrated surface to 9 km February 1.7 ppb/mo March 7 ppb/mo May 12 ppb/mo April 14 ppb/mo (Y. Wang, Rutgers Univ) TOPSE: Tropospheric Ozone Production about the Spring Equinox

  17. 7Be – O3 relationship and stratospheric influence during TOPSE 7Be vs O3 Observed “stratospheric influence” (Dibb et al., UNH) TOPSE: Tropospheric Ozone Production about the Spring Equinox

  18. Surface Ozone Depletion Over Baffin Bay ODE from Thule to east side of Baffin Island TOPSE: Tropospheric Ozone Production about the Spring Equinox

  19. Transport of surface ozone hole to Hudson Bay TOPSE: Tropospheric Ozone Production about the Spring Equinox

  20. Summary • An ACD-led field campaign, with observational and numerical modeling components, was organized and carried out • Critical collaborations, in measurements & numerical modeling, with colleagues throughout the scientific community • Important contributions by graduate and post-doctoral students • 1st round of scientific papers to be published mid-to-late 2002. TOPSE: Tropospheric Ozone Production about the Spring Equinox

  21. Atmospheric Chemistry DivisionNational Center for Atmospheric Research HANK: ACD’s Regional Chemistry-Transport Model developed by Peter Hess1 with contributions from A. Klonecki, J.F. Lamarque, M. Barth, L. Smith, S. Madronich 1Theoretical Studies and Modeling Section HANK

  22. HANK - Model Overview Chemical Transport Model driven from MM5 • Resolution: variable (10 x10 km – 250 x 250 km) • Chemistry: flexible gas and aqueous chemistry mechanism (TOPSE: 54 species, 145 reactions, 25 photolysis reactions) • Transport: Deep and shallow convection, boundary layer transport, advection • Physical Removal: Episodic dry and wet deposition • Adjoint model for sensitivity studies • Data assimilation package HANK

  23. HANK SCIENCE • Mauna Loa Photochemistry Experiment1 • Nature of chemical transformations and transport across the Pacific • Subtropical free troposphere is a photochemically active region • Tropospheric Ozone Production about Spring Equinox • Model run in real time and forecast mode • Transport’s role in the spring equinox photochemical transition • Dust transport across Atlantic (UCSB) • Emissions of U.S. Forest Fires (using MOPITT satellite data) 1Hess, P. G., S. Flocke, J.-F. Lamarque, M. C. Barth, and S. Madronich,Episodic modeling of the chemical structure of the troposphere asrevealed during thespring MLOPEX intensive, J. Geophys. Res., 105, 26809-26839, 2000. Vukicevic, T. and P. G. Hess, Analysis of tropospheric transport in the Pacific Basin using theadjoint technique, J. Geophys. Res., 105, 7213-7230, 2000. Hess, P. G., Model and measurement analysis of springtime transport and chemistry of the Pacific basin. J. Geophys. Res., 106, 12689-12717, 2001. Barth, M. C., P. G. Hess, and S. Madronich, Effect of marine boundary layer clouds on tropospheric chemistry as analyzed in a regional chemistry transport model, J. Geophys. Res., submitted, 2001. HANK

  24. Pacific Basin Simulations (MLOPEX) • Adjoint Trajectory for • pollutant plume to Hawaii • Same trajectory in height- • longitude plane • Chemical transformations • and rainout along the • trajectory HANK

  25. TOPSE Simulations CO TRANSPORT OVER POLE • HANK was run in real-time and • forecast mode during TOPSE • Seasonal cycle of constituents • diagnosed • Important changes in both • chemistry and transport • during Spring transition HANK

  26. HANK - Plans • MIRAGE modeling • Real time and forecast modeling of forest fire pollution • Continued development of adjoint technique • applications to data assimilation/inverse modeling • CO2 emissions • Prototype model for WRF-Chem • Coupled meteorological and chemical model • WRF-Chem development group: P. Hess (Lead, NCAR), C. Benkovitz (Brookhaven National Lab), D. W. Byun (University of Houston), G. Carmichael (University of Iowa), K. Schere (EPA), P.-Y. Whung (NOAA ), G. Grell (NOAA, FSL), J. McHenry (NCSC), Carlie Coats (NCSC), M. Trainer (NOAA, AL), B. Skamarock (NCAR), G. Peng, (Aerospace Corporation), J. Wegiel (AFWA), S. Yvon-Lewis (NOAA, AOML) HANK

  27. Atmospheric Chemistry DivisionNational Center for Atmospheric Research ACD Contributions to the NASA TRACE-P* Campaign Fred Eisele Senior Research Associate Photochemical Oxidation & Products 24-26 October 2001, NSF Review *(TRAnsport and Chemical Evolution over the Pacific) ACD contribution to TRACE-P

  28. TRACE-P University Collaborations • University of California-Irvine • Drexel University • Florida State University • Georgia Institute of Technology • Harvard University (mission scientist Daniel Jacob) • University of Hawaii • University of Iowa • Massachusetts Institute of Technology • University of Miami • University of New Hampshire • Pennsylvania State University • University of Rhode Island • Max-Planck-Institut fur Meteorologie • Nagoya University ACD contribution to TRACE-P

  29. MISSION OBJECTIVES Determine Asian outflow pathways Determine the chemical evolution of outflow ACD contribution to TRACE-P

  30. COMMON OBJECTIVES ACD Themes that overlap with TRACE-P objectives MIRAGE Reactive Carbon Biosphere, Chemistry, and Climate Clouds UT/LS Other synergistic activities ACE Asia ACD contribution to TRACE-P

  31. Measurement ACD Participants • Actinic flux Shetter, Lefer, Hall, Cinquini • OH, H2SO4, HNO3, MSA Eisele, Mauldin, Kosciuch, Zondlo • HO2/RO2 Cantrell • Alcohols/Carbonyls Apel • CH2O Fried, Walega, Wert • PAN, PPN, MPAN Flocke/Weinheimer • Organic Nitrates, halocarbons Atlas, Stroud, K. Johnson, Weaver • MOPITT CO Gille et al. ACD contribution to TRACE-P

  32. TRACE-P Data Preliminary Data from TRACE-P This Data is provided for review information only and should not be cited until TRACE-P data is officially released to the public. ACD contribution to TRACE-P

  33. TRACE-P Data Slides are not being included in hard copy or on the web at NASA’s request because this data has not yet been released to the public. ACD contribution to TRACE-P

  34. Measurement University collaboration- Instrument uniqueness Actinic flux only group doing these measurements in US OH, H2SO4,MSA only airborne CIMS technique for OH, HNO3 MSA, and (in US) for H2SO4- Georgia Tech HO2/RO2 only airborne HO2/RO2 CIMS in US Alcohol/Carbonyls only airborne - GC/MS system – U of Miami CH2O only airborne CH2O TDL technique in US - U of Tulsa and U of Colorado PAN etc. no other university airborne GC/ECD for PANs Organic Nitrate unique combination of measurements-UC Irvine MOPITT unique satellite measurements – U of Toronto ACD contribution to TRACE-P

  35. SUMMARY • ACD contributed significantly to the success of TRACE-P • ACD’s unique measurements complemented those of the university research community and broadened mission capabilities • ACD is continuing to develop unique capabilities to fill measure voids ACD contribution to TRACE-P

  36. Future TRACE-P Contributions • Final data submission in December 2001 • Manuscript preparation and submission –Spring/Summer 2002 • TRACE-P data available to the public June 1, 2002 ACD contribution to TRACE-P

  37. Atmospheric Chemistry DivisionNational Center for Atmospheric Research Megacity Impacts on the Regional And Global Environment An integrated multi-disciplinary program to study the export and transformations of pollutants from large metropolitan areas to regional and global scales. Sasha Madronich Senior Scientist Theoretical Studies and Modeling (TSM) MIRAGE

  38. History • 1998 Oct.: Open workshop at NCAR • 1999: Proposal for pilot Mexico City study PI’s: Darrel Baumgardner, Guy Brasseur Reviewed by NSF, not supported at that time __________________________________________________________________ • 2000 Aug.: NCAR decides to revive activity • 2000 Sept.- Nov.: NCAR planning meetings • Develop multidisciplinary plan with 5 focal areas • 2001 Jan. - present: Integrate in ACD Strategic plan • 2001 Spring - present: Define ACD role MIRAGE

  39. Working Groups ACD: C. Cantrell, A. Guenther, P. Hess, S. Madronich, S. Massie, J. Orlando, R. Shetter, G. Tyndall, Frank Flocke ASP: S. Durlak, A. Gettelman MMM: F. Chen, W. Dabberdt, W. Skamarock, T. Warner ESIG: B. Harriss, K. Miller, K. Purvis ATD: L. Radke MIRAGE

  40. New Scientific Foci Gas Phase Chemistry: Export of gaseous pollutants and oxidation intermediates, and their role in regional/global ozone and aerosol budgets. Aerosol Chemistry and Physics: Evolution of aerosol composition and physical properties, their interactions with gas phase species, and their role in climate directly via scattering/absorption and indirectly via cloud formation. Radiation: High pollution levels can alter incident solar radiation, modifying both photochemistry and heating rates. Local and Regional Meteorology: Large urban areas can modify local meteorology, which in turn controls ventilation and the export of gases and aerosols. Urban Metabolism: The mix of pollutants in developing cities is very different from that in large industrialized cities. Future growth of emissions will also differ depending on many socio-economic factors. MIRAGE

  41. Gas Phase Photochemistry - 1 Example of non-linearity of chemistry: Downwind re-inflation of Ox production d[Ox]/dt > 0 when R(OH+CO)>R(OH+NO2) S. Rivale (SOARS) and S. Madronich, unpubl. 1999 MIRAGE

  42. Gas Phase Photochemistry - 2 Example of chemical complexity: Persistence of oxygenated organic intermediates Madronich and Calvert 1990, uptdated by C. Stroud 2001 MIRAGE

  43. Aerosol Physics and Photochemistry Example of aerosol-gas phase coupling: Growth of organic aerosol by dissolution of gas phase species Aumont et al., 2000 MIRAGE

  44. Radiation in Polluted Environments Photolysis rates in polluted conditions: Castro et al. 2001 MIRAGE

  45. Local and Regional Meteorology • Changed Geophysical Properties of Urban Surfaces • Anthropogenic sensible heat flux (up to 200 W m-2) • Anthropogenic latent heat flux (not well known) • Aerodynamic roughness (zo values up to several meters) • Aerodynamic displacement height (tens of meters) • Surface runoff • Heat transfer characteristics of the “ground” (thermal conductivity and volumetric heat capacity); surface and soil wetness • Surface albedo • Potential Interactions with Air Pollution • Radiative (e.g. vertical distributions soot) • Chemical (e.g. amount and type of cloud condensation nuclei) MIRAGE

  46. Urban Metabolism - 1 World’s largest cities MIRAGE

  47. Urban Metabolism - 2 Emissions in developing cities are very different than in developed cities MIRAGE

  48. Site Selection Criteria - 1 Megacity characteristics (ranked by population in 2000) MIRAGE

  49. Site Selection Criteria - 2 CO from MOPPIT • Pollution signal strength relative to background MIRAGE

  50. Site Selection - 5 MIRAGE

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