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Presented by: Rynda Hudman, Harvard University

ICARTT Coordinated Atmospheric Chemistry Campaign Over Eastern North America and North Atlantic in Summer 2004: OBJECTIVES, SEASONAL CONTEXT, AND PRELIMINARY RESULTS.

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Presented by: Rynda Hudman, Harvard University

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  1. ICARTT Coordinated Atmospheric Chemistry Campaign Over Eastern North America and North Atlantic in Summer 2004:OBJECTIVES, SEASONAL CONTEXT, AND PRELIMINARY RESULTS Atmospheric Open SeminarEarth Observation Research and Application CenterJapan Aerospace Exploration Agency (EORC/JAXA)November 26, 2004 Presented by: Rynda Hudman, Harvard University Measurements by L. K. Emmons (NCAR), W. McMillan (U. Maryland), E. Browell, G. B.Pierce, W. Sachse (NASA Langley), J. Holloway (NOAA Aeronomy Lab), D. Blake (Irvine), G. Huey (Georgia Tech), Dibb, A.Fried, and the ICARTT science team Model results provided by Solène Turquety (Harvard), Qinbin Li (JPL), Lyatt Jaeglè (U. Washington), G. Charmichael (U. Iowa) Additional contributions by Daniel Jacob (Harvard) and Jim Crawford (NASA Langley)

  2. ICARTT: COORDINATED ATMOSPHERIC CHEMISTRY CAMPAIGN OVER EASTERN NORTH AMERICA AND NORTH ATLANTIC IN SUMMER 2004 International, multi-agency collaboration • SCIENTIFIC OBJECTIVES • Regional Air Quality:characterize sources and transport of pollution in northeastern North America • Continental Outflow:quantify North American outflow of environmentally important gases and aerosols, relate to sources • Transatlantic Pollution:understand transport and chemical evolution of North American pollution across the Atlantic • Aerosol Radiative Forcing:characterize direct/indirect effects of aerosols over northeastern North America and western North Atlantic

  3. ICARTT Study Collaboration Participants: New England Air Quality Study - Intercontinental Transport and Chemical Transformation (NEAQS-ITCT) 2004 Intercontinental Chemical Transport Experiment - North America (INTEX-NA) CO2 Budget and Rectification Airborne study (COBRA) Meteorological Service of Canada (MSC) Intercontinental Transport of Pollution (ITOP) University of New Hampshire - AIRMAP Harvard Forest, Harvard University University of Massachusetts Robotic Aerostat Research Lab (RARL) Atmospheric Sciences Research Center (ASRC) U.S. Department of Energy (DOE) Atmospheric Chemistry Program California Institute of Technology (Caltech)

  4. ICARTT: Field datahttp://www.al.noaa.gov/ICARTT/FieldOperations INTEX-NA Flight tracks July 1-Aug 8 INTEX flight summaries: http://cloud1.arc.nasa.gov/intex-na ITCT-2K4 flight summaries: https://tropchem.al.noaa.gov/NEAQSITCT2k4P3 ITCT-2K4 Flight tracks Jul 1-Aug 15

  5. ICARTT: Forecast Productshttp://www.al.noaa.gov/ICARTT/FieldOperations • Global and regional models: • GEOS-CHEM • RAQMS (B. Pierce, NASA LaRC) • STEM/CFORS (G. Carmichael, Iowa) • FSU trajectory products (H. Fuelberg, FSU) • MOZART (L. Horowitz, NOAA and L. Emmons, NCAR) • FLEXPART (A. Stohl, NOAA) • WRF-CHEM (G. Grell, NOAA) • Satellite: • NASA Langley Satellite Overpass Predictor • MODIS / PM2.5 forecasting tool • Terra / MOPITT CO data • GOME and SCIAMACHY data • GOES real-time aerosol/smoke product • NOAA Aeronomy Lab Met Products • AIRS CO • TOMS Aerosol product • MODIS real-time images • WF ABBA fire loops • MODISWeb fire mapper • University of Virginia Remotely Sensed • Specific Humidity Products

  6. GEOS forecasts and GEOS-CHEM NRT : Objectiveshttp://coco.atmos.washington.edu/cgi-bin/ion-p?page=geos_intexa.ion • Chemical forecasts (GMAO): • Support flight planning (1X1.25 global resolution!) • Evaluation of transport error • (Dylan B. Jones) • NRT GEOS-CHEM simulations, led by Solène Turquety (Harvard) • Support flight planning: monitor any large deviations between the aircraft observations and our understanding of ozone and aerosol processes that may cause alteration of flight plans, • To provide vertical shape information for NO2 and HCHO concentrations to support near-real-time retrievals of SCIAMACHY column data for these two gases (by Dalhousie University) • Generate a set of preliminary findings by the end of ICARTT – Preliminary findings already presented at IGAC by Solène Turquety! Still running!... • http://coco.atmos.washington.edu/cgi-bin/ion-p?page=geos_nrt.ion

  7. ICARTT GEOS forecasts and GEOS-CHEM NRT analysishttp://coco.atmos.washington.edu/cgi-bin/ion-p?page=geos_intexa.ion Web interface by Lyatt Jaeglé – Univ. Washington

  8. June 2000 Horizontal North American CO Flux June 1998 Anthropogenic pollution outflow at 35ºN-50ºN, while biomass burning outflow at higher latitudes 45ºN-55ºN. Outflow at much lower latitudes in June 1998. Details in Li et. al, 2004: Outflow pathways for N.A. pollution in the summer: A Global 3-D Model Analysis of MODIS and MOPITT observations, submitted to JGR.

  9. Horizontal North American CO Flux July 2000 August 1998 Outflow in July is at lower latitudes than in June, while outflow in August shows features in between June and July. [Li et al., 2004]

  10. 1998 Vertical and Zonal North American CO Flux, July 70ºW 300 hPa 70ºW 70ºW Stronger convective transport than June and August. Line contour – fluxes Filled contour – concentrations [Li et al., 2004]

  11. Seasonal Context: 500 mb Geopotential Height (m): Persistent Deep Trough Over Eastern U.S. July 2004 Long-Term Mean July 1948 - present http://www.cdc.noaa.gov/cdc/reanalysis/reanalysis.shtml

  12. Biomass burning 2004Persistent Alaskan and Canadian burning Canada Canadian National Forest Fire Situation Report Sept 8, 2004(http://www.nrcan.gc.ca/cfs-scf/redirects/fire/) • Wildfires in Alaska: > 2,500,000 Hectares! • Alaska Fire services: “The largest fire season in Alaska’s rich history ” • Alaska ~ 41% total area burned in North America in 2004, • Canada ~ 52% total area burned in North America in 2004. [S. Turquety]

  13. What did we get? • Strong biomass burning signatures further south than normal, mixed with regional pollution (GEOS-CHEM study led by S. Turquety) • Spring-like conditions led to Asian Influence being detected on many flights in the upper troposphere (GEOS-CHEM study led by L. Jaeglè, U.W.) • Convection in the southern U.S. led to first aircraft observations of upper-level ozone maximum predicted by Li et al., 2004. (GEOS-CHEM study led by Q. Li, JPL) • Strong biomass burning signatures led to first successful Lagrangian event to be captured in West, Central and Eastern Atlantic (GEOS-CHEM study by M. Evans U. Leeds and R. Hudman) • Will be able to characterize NOy outflow from different uplift mechanisms along the entire east coast (GEOS-CHEM study led by R. Hudman) • Will be able to characterize CO emissions using MOPITT and aircraft (GEOS-CHEM study by S. Turquety) • What we didn’t get….high regional ozone episode in the east coast due to stagnation  for us…  for population of Northeastern U.S.

  14. (McMillan, UMBC)

  15. Biomass burning 2004: Strong signature during ICARTT MODIS AOD July 18th NOAA Hazard Mapping System Fire and smoke product - July 18th AIRS COColumn July 18th [Courtesy Wallace McMillan] MOPITT CO Column July 16-18th [Courtesy Louisa K. Emmons] è

  16. MODIS AOD July 18, 2004 MODIS Aerosol Optical Depth with EPA AIRNow PM2.5: July 18- July 22, 2004 July 19, 2004 Smoke from Alaskan Forest Fires July 20, 2004 July 21, 2004 July 22, 2004 Link between Alaskan smoke and US AQ?

  17. Biomass burning 2004: Strong signature during ICARTT (ppbv) ITCT P3 flight July 9, 2004 Observations J. Holloway

  18. http://idea.ssec.wisc.edu/ Pierce, LaRC

  19. DC-8 Flight #9: Strong Signature of Biomass Burning 600 ppbv [Observations G. Sachse, LaRC]

  20. Evidence of Upstream Convective Outflow Large Fire Plumes Observed

  21. http://idea.ssec.wisc.edu/ Pierce, LaRC

  22. DC-8 July 20 flight – High Sulfates in the SE (G. Carmichael, U. Iowa) [Huey, Georgia Tech] [Dibb, UNH]

  23. S. Pt. NW Pt. Penn.

  24. S. Pt. NW Pt. Penn. 2 1 Fire Plume Aerosols

  25. http://idea.ssec.wisc.edu/ Pierce, LaRC

  26. MOPITT – MODEL, ICARTT period Comparison GEOS-CHEM / MOPITT Total CO MOPITT CO for July 17-19 GEOS-CHEM NRT x AK July 17-19 1e+18 molec/cm2 • CO columns simulated are under-estimated by ~25% in the location of the biomass burning plume • Area burned ? (2 x reports…) • Type of vegetation burned ? • Fuel loading associated ? • Altitude of the emissions ? [S. Turquety]

  27. Tons CO/ hectare burned How can we improve the comparisons? [S. Turquety] NOAA : use 4.5 tons CO/ hectare burned Underestimation due to peat burning (consider only trees) 1st estimate: x 1.8 for boreal forests in order to account for peat burning • MODIS hot spots : 3 days maximum / 1x1 grid box • Location of fires / region • Daily area burned reports (National Interagency Fire Center http://www.cidi.org/wildfire): • 3 days running averages • Temporal variability / region Emissions = Area burned x [fuel loading x combustion factor x emission factor]

  28. [S. Turquety] Comparison GEOS-CHEM / MOPITT w/ new BB emissions MOPITT CO for July 17-19 GEOS-CHEM NRT x AK July 17-19 (MOPITT-MODEL)/MOPITT

  29. ASIAN POLLUTION PLUME OFF CALIFORNIA sampled by NASA aircraft on July 1, 2004 GEOS forecast Asian CO (9 km) AIRS satellite CO data Asian pollution S. Pawson (NASA), W. McMillan (UMBC), M/ Avery (NASA), S.Turquety (Harvard). L. Jaegle (UW)

  30. (Blake, UC Irvine)

  31. GEOS forecast Asian CO (9 km) ASIAN POLLUTION PLUME OVER EASTERN U.S. Observed O3 (ppbv) Observed CO(ppbv) sampled by NASA aircraft on July 15 Observed O3 = 20-40 ppbv, CO = 20 ppbv GEOS-CHEM O3 = 5-10 ppbv, CO = 10-20 ppbv High Halon-1211 in plume confirms Asian origin

  32. Formaldehyde distributions in the boundary layer and upper troposphere for 6-12 July, 2004 (A. Fried, NCAR) 6-12 km 0-1 km

  33. GEOS-CHEM monthly means at 300 hPa, July 2000 [Li et al., 2004] IS THERE A UT OZONE MAXIMUM OVER SOUTHERN U.S. IN SUMMER? July 2000 ozonesonde data [Newchurch et al., 2003] GEOS- CHEM sondes

  34. DC-8 July 12 flight: 80-110 ppb O3 observed at 6-10 km over SE U.S. model too low by 20-30 ppbv DC8 Model (300 hPa) DIAL O3

  35. IGAC Quasi-Lagrangian Objective • 4 Aircraft: U.S. NASA DC-8, Pease NH U.S. NOAA WP-3D, Pease, NH U.K. ITOP Consortium BAe-146, Azores German DLR Falcon, Creil, France • 3 Major Cross-Atlantic Features Sampled: Alaskan/Canadian Fire Plume (07/18-07/22/2004) New York/Boston Megacity Plume (07/20-07/26/2004) Pre-frontal transport (warm conveyor belt 07/27-8/01/2004)

  36. Alaskan/Canadian Fire Plume: Sampled by DC-8 Sampled by BAe-146 Sampled by DLR Falcon

  37. 27 satellite validation profiles were planned during INTEX Aqua-AIRS 11 underflights (2 aborted due to clouds) Terra-MOPITT 10 underflights Terra-MISR 2 underflights Envisat-SCIAMACHY 4 underflights

  38. 27 satellite validation profiles were planned during INTEX Aqua-AIRS 11 underflights (2 aborted due to clouds) Terra-MOPITT 10 underflights Terra-MISR 2 underflights Envisat-SCIAMACHY 4 underflights

  39. 27 satellite validation profiles were planned during INTEX Aqua-AIRS 11 underflights (2 aborted due to clouds) Terra-MOPITT 10 underflights Terra-MISR 2 underflights Envisat-SCIAMACHY 4 underflights

  40. MOPITT validation example and averaging kernel AIRS validation example

  41. Brief Overview of correlation and inverse analysis during TRACE-P at Harvard University Atmospheric Chemistry Modeling Group Daniel Jacob, Paul I. Palmer, Colette L. Heald, Parvadha N. Suntharalingam, Yaping Xiao All papers as well as contact information are available on group website: www-as.harvard.edu/chemistry/trop/

  42. MOPITT CO columns (Mar-Apr 01) MEAN CO COLUMN FIELDS FROM MOPITT DURING TRACE-P GEOS-CHEM CTM with Duncan et al. [2003]sources Difference Heald et al. [2003]

  43. INVERSION OF TRACE-P AND MOPITT DATA TO QUANTIFY CARBON MONOXIDE SOURCES FROM ASIA Fossil and biofuel [D.R. Streets, ANL] Daily biomass burning (satellite fire counts) TRACE-P CO DATA (G.W. Sachse) A PRIORI EMISSIONS (customized for TRACE-P) chemical forecasts GEOS-CHEM CTM (D.J. Jacob, Harvard) top-down constraints validation INVERSE ANALYSIS • CONCLUSIONS: • A priori Chinese emissions too low by 50% • (domestic burning) • A priori SE Asian biomass burning emissions • too high by 60% • Japan, Korean emissions correct within 20% MOPITT CO March-April 2001

  44. TRACE-P CONSTRAINTS ON ASIAN SOURCES OF CO2 2001 E Asian CO2 source (a priori) Total Fossil fuel (Streets) Biomass burning (Duncan) Balanced biosphere (CASA) TRACE-P period Suntharalingam et al. [2004] ALL DATA CHINA OUTFLOW JAPAN OUTFLOW Observations from Vay et al. [2003] model observed

  45. CO2:CO CORRELATION IN TRACE-P DATA ALLOWS SEPARATION OF CHINESE FOSSIL FUEL vs. BIOSPHERIC SOURCES OF CO2 China outflow data Slope = 25 Slope = 45 observed model (a priori) A priori CO2/CO chinese Source ratios Fitting the observed CO2 concentrations andCO2-CO slopes requires reduction of Chinese net biospheric CO2 source by 45% relative to best a priori information from CASA biogeochemical model Suntharalingam et al. [2004]

  46. TRACE-P CONSTRAINTS ON METHANE SOURCESUSING CH4-C2H6-CO CORRELATIONS C2H6 (D.R. Blake) CH4 (G.W. Sachse) • Strong CH4-C2H6 correlation a dominant contribution of European natural gas sources to Asian outflow of methane; Asian source (mostly livestock in that season) is relatively small • European source must be reduced by 30-50% relative to current inventories (EDGAR2); recent mitigation efforts? Xiao et al. [2004]

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