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)

ICARTT: COORDINATED ATMOSPHERIC CHEMISTRY CAMPAIGN OVER EASTERN NORTH AMERICA AND NORTH ATLANTIC IN SUMMER

2004

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

International, multi-agencycollaboration

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)

INTEX flight summaries: http://cloud1.arc.nasa.gov/intex-na

ITCT-2K4 flight summaries: https://tropchem.al.noaa.gov/NEAQSITCT2k4P3

ICARTT: Field dataICARTT: Field datahttp://www.al.noaa.gov/ICARTT/FieldOperations

ITCT-2K4 Flight tracks Jul 1-Aug 15

INTEX-NA Flight tracks July 1-Aug 8

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 MODIS Web fire mapper University of Virginia Remotely Sensed

Specific Humidity Products

ICARTT: Forecast ProductsICARTT: Forecast Productshttp://www.al.noaa.gov/ICARTT/FieldOperations

GEOS forecasts and GEOS-CHEM NRT : GEOS forecasts and GEOS-CHEM NRT : ObjectivesObjectives

http://coco.http://coco.atmosatmos..washingtonwashington..eduedu//cgicgi-bin/ion-p?page=-bin/ion-p?page=geosgeos__intexaintexa.ion.ion

Chemical forecasts (GMAO):

1. Support flight planning (1X1.25 global resolution!)

2. Evaluation of transport error (Dylan B. Jones)

NRT GEOS-CHEM simulations, led by Solène Turquety (Harvard)

1. 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,

2. 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)

3. 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

ICARTT GEOS forecasts and GEOS-CHEM NRT analysisICARTT GEOS forecasts and GEOS-CHEM NRT analysishttp://coco.atmos.washington.edu/cgi-bin/ion-p?page=geos_intexa.ionhttp://coco.atmos.washington.edu/cgi-bin/ion-p?page=geos_intexa.ion

Web interface by Lyatt Jaeglé – Univ. Washington

Anthropogenic pollution outflow at 35ºN-50ºN, while biomass burning outflow at higher latitudes 45ºN-55ºN. Outflow at much lower latitudes in June 1998.

June 2000

Horizontal North American CO Flux

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.

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.

Horizontal North American CO Flux

[Li et al., 2004]

Vertical and Zonal North American CO Flux, July

Stronger convective transport than June and August.

Line contour – fluxes Filled contour – concentrations

300 hPa

70ºW

70ºW

70ºW

1998

[Li et al., 2004]

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

Biomass burning 2004Biomass burning 2004Persistent Alaskan and Canadian burningPersistent Alaskan and Canadian burning

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.

Canada

[S. Turquety]

What did we get?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.

(McMillan, UMBC)

Biomass burning 2004: Strong signature during ICARTTBiomass burning 2004: Strong signature during ICARTT MODIS AOD July 18th

AIRS CO Column July 18th [Courtesy Wallace McMillan]

MOPITT CO Column July 16-18th [Courtesy Louisa K. Emmons]

NOAA Hazard Mapping System Fire and smoke product - July 18th

è

MODIS Aerosol Optical Depth with EPA AIRNow PM2.5:July 18- July 22, 2004

MODIS AOD July 18, 2004

July 19, 2004

July 20, 2004

July 21, 2004

July 22, 2004

Link between Alaskan smoke and US AQ?

Smoke from Alaskan Forest Fires

Observations J. Holloway

(ppbv)

Biomass burning 2004: Strong signature during ICARTTBiomass burning 2004: Strong signature during ICARTT

ITCT P3 flight July 9, 2004

7 6

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DC-8 Flight Path Aqua (1200 and 1340 LT)

AIRS-swath Terra (1020 and 1200 LT) MOPITT-swath

SCIAMACHY (1110 LT) Rhinelander Lidar Sites

Pierce, LaRChttp://idea.ssec.wisc.edu/

DC-8 Flight #9: Strong Signature of Biomass Burning

600 ppbv

[Observations G. Sachse, LaRC]

Large Fire Plumes Observed

Evidence of Upstream Convective Outflow

76

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DC-8 Flight Path Aqua (1140, 1320, 1500 LT)

AIRS-swath Terra (1005, 1145, 1325 LT) MOPITT-swath

SCIAMACHY (1005 and 1145 LT) MISR-swath Lidar Sites

Pierce, LaRChttp://idea.ssec.wisc.edu/

7so2151515http://nas.

DC-8 July 20 flight – High Sulfates in the SE (G. Carmichael, U. Iowa)

[Huey, Georgia Tech]

[Dibb, UNH]

S. Pt. NW Pt. Penn.

S. Pt. NW Pt. Penn.

Fire Plume Aerosols

1 2

Pierce, LaRChttp://idea.ssec.wisc.edu/

Comparison GEOS-CHEM / MOPITT Total COComparison GEOS-CHEM / MOPITT Total CO

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 ?

MOPITT – MODEL, ICARTT period

MOPITT CO for July 17-19 GEOS-CHEM NRT x AK July 17-19

1e+18 molec/cm2

[S. Turquety]

How can we improve the comparisons?How can we improve the comparisons?

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

Tons CO/ hectare burned

Emissions = Area burned x [fuel loading x combustion factor x emission factor]

[S. Turquety]

Comparison GEOS-CHEM / MOPITT w/ new BB emissionsComparison GEOS-CHEM / MOPITT w/ new BB emissions

MOPITT CO for July 17-19 GEOS-CHEM NRT x AK July 17-19

(MOPITT-MODEL)/MOPITT

[S. Turquety]

ASIAN POLLUTION PLUME OFF CALIFORNIA

sampled by NASA aircraft on July 1, 2004

GEOS forecast Asian CO (9 km) AIRS satellite CO data

Asianpollution

(Blake, UC Irvine)

ASIAN POLLUTION PLUME OVER EASTERN U.S.

sampled by NASA aircraft on July 15

Observed O3 = 20-40 ppbv, CO = 20 ppbvGEOS-CHEM O3 = 5-10 ppbv, CO = 10-20 ppbv

High Halon-1211 in plume confirms Asian origin

0

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13:00 14:00 15:00 16:00 17:00 18:00 19:00 20:00 21:00

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tv)

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GEOS forecast Asian CO (9 km)

Observed O3 (ppbv)

Observed CO (ppbv)

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Median = 0.21 ppbvAverage = 0.24 ppbvStdev = 0.21 ppbvNumber = 394

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76543210CH2O (ppbv)

Median = 2.80 ppbvAverage = 2.99 ppbvStdev = 1.21 ppbvNumber = 280

0-1 km

6-12 km

Formaldehyde distributions in the boundary layer and upper tropospherefor 6-12 July, 2004 (A. Fried, NCAR)

IS THERE A UT OZONE MAXIMUM OVER SOUTHERN U.S. IN SUMMER?

GEOS-CHEM monthly means at 300 hPa, July 2000 [Li et al., 2004]

July 2000 ozonesonde data [Newchurch et al., 2003]

sondes

GEOS-CHEM

DC-8 July 12 flight: 80-110 ppb O3 observed at 6-10 km over SE U.S.

DIAL O3

Model

(300 hPa)

DC8

model too low by 20-30 ppbv

IGAC Quasi-Lagrangian Objective

• 4 Aircraft:U.S. NASA DC-8, Pease NHU.S. NOAA WP-3D, Pease, NHU.K. ITOP Consortium BAe-146, AzoresGerman 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)

Sampled by DC-8

Sampled by BAe-146

Sampled by DLR Falcon

Alaskan/Canadian Fire Plume:

Aqua-AIRS 11 underflights (2 aborted due to clouds)Terra-MOPITT 10 underflightsTerra-MISR 2 underflightsEnvisat-SCIAMACHY 4 underflights

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DC-8 Flight Path Aqua (1305 LT)

AIRS-swath Terra (1125 LT) MOPITT-swath

SCIAMACHY (1100 LT) MISR-dwell Lidar Sites

27 satellite validation profiles were planned during INTEX

Aqua-AIRS 11 underflights (2 aborted due to clouds)Terra-MOPITT 10 underflightsTerra-MISR 2 underflightsEnvisat-SCIAMACHY 4 underflights

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DC-8 Flight Path Aqua (1305 LT)

AIRS-swath Terra (1125 LT) MOPITT-swath

SCIAMACHY (1100 LT) MISR-dwell Lidar Sites

27 satellite validation profiles were planned during INTEX

Aqua-AIRS 11 underflights (2 aborted due to clouds)Terra-MOPITT 10 underflightsTerra-MISR 2 underflightsEnvisat-SCIAMACHY 4 underflights

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DC-8 Flight Path Aqua (1305 LT)

AIRS-swath Terra (1125 LT) MOPITT-swath

SCIAMACHY (1100 LT) MISR-dwell Lidar Sites

27 satellite validation profiles were planned during INTEX

MOPITT validation exampleand averaging kernel

AIRS validation example

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/

MEAN CO COLUMN FIELDS FROM MOPITT DURING TRACE-P

MOPITT CO columns(Mar-Apr 01)

GEOS-CHEMCTM withDuncan et al.[2003]sources

Difference

Heald et al. [2003]

INVERSION OF TRACE-P AND MOPITT DATA TO QUANTIFY CARBON MONOXIDE SOURCES FROM ASIA

TRACE-P CO DATA(G.W. Sachse)

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%

A PRIORIEMISSIONS(customized for TRACE-P)

Fossil and biofuel[D.R. Streets, ANL]

Daily biomass burning(satellite fire counts)

GEOS-CHEM CTM(D.J. Jacob, Harvard)

MOPITT CO March-April 2001

INVERSEANALYSIS

validation

chemicalforecasts

top-downconstraints

TRACE-P CONSTRAINTS ON ASIAN SOURCES OF CO2

2001 E Asian CO2 source (a priori)

ALL DATA JAPAN OUTFLOW

modelobserved

CHINA OUTFLOW

TotalFossil fuel (Streets)Biomass burning (Duncan)Balanced biosphere (CASA)TRACE-P period

Suntharalingamet al. [2004]

Observations from Vay et al. [2003]

CO2:CO CORRELATION IN TRACE-P DATA ALLOWS SEPARATION OF CHINESE FOSSIL FUEL vs. BIOSPHERIC SOURCES OF CO2

Slope = 25Slope = 45

Suntharalingam et al. [2004]

China outflow data

observed model (a priori)

Fitting the observed CO2 concentrations and CO2-CO slopes requires reduction of Chinese net biospheric CO2 source by 45% relative to best a priori information from CASA biogeochemical model

A prioriCO2/COchineseSourceratios

TRACE-P CONSTRAINTS ON METHANE SOURCESUSING CH4-C2H6-CO CORRELATIONS

CH4

(G.W. Sachse)

C2H6 (D.R. Blake)

Xiao et al. [2004]

• Strong CH4-C2H6 correlation 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?