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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
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Page 1: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

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

Page 2: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 2

Atmospheric Chemistry DivisionNational Center for Atmospheric Research

TOPSE: Tropospheric Ozone Production

About the Spring Equinox

Chris Cantrell

Scientist III – Atmospheric Radical Studies24-26 October 2001, NSF Review

Page 3: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Chris Cantrell 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.

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 4

Specific Scientific Questions

1) 2-D morphology and evolution of ozone? 2) Rates of in-situ ozone production? 3) Distribution and evolution of radicals and

reservoirs? 4) Sources and partitioning of reactive odd-

nitrogen? 5) Composition and evolution of volatile organic

compounds? 6) Can models adequately describe and integrate

processes affecting atmospheric chemistry in TOPSE region? In Northern Hemisphere?

Page 5: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 5

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

TOPSE Development Calendar

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 6

TOPSE Investigators: Measurements

Measurement InvestigatorsRemote Ozone/Aerosols (DIAL) Browell et al., NASAAcidic Trace Gases/7-Be Talbot, Dibb, et al. UNHNMHC, Halocarbons, RONO2 Blake et al., UCINO2, Peroxynitrates Cohen, Thornton et al., UCBSpeciated Peroxides Heikes, Snow, URIOH, H2SO4 Eisele, Mauldin, NCARHO2, RO2 Cantrell, Stephens, NCARHNO3 Zondlo, NCARNOx, NOy, Ozone Ridley, Walega, NCARCH2O, H2O2 Fried, NCARJ values Shetter, Lefer et al., NCARPAN, PPN Flocke, Weinheimer, NCARCO, N2O Coffey, Hannigan, NCARUltrafine Aerosols Weber, GITMission Scientists/P.I.s Atlas, Cantrell, Ridley, NCAR

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 7

TOPSE Investigators: Modeling/Collaboration

Modeling/Collaboration InvestigatorsRegional/Forecast Model (HANK) Klonecki, Hess et al., NCARGlobal Model Analysis Tie, Emmons et al., NCAR

(MOZART) Brasseur et al., MPIProcess and Radiation Models Madronich et al., NCARGlobal Model/Process Studies Jacob, Evans, Harvard U.Stratosphere/Troposphere Exch. Allen, Pickering, U. Md.Regional/other Models Wang et al., Rutgers U.Meteorological Forecast/ Moody, Cooper, Wimmers, U.Va.

Remote SensingOzonesonde Network Merrill, URI; Fast, PNWL

GOME BrO Richter, Burrows, U. BremenMet. Forecasts (UT/LS) Newman, NASAPolar Sunrise Expt., 2000 Shepson, Purdue;

Bottenheim, Can. Met. Serv.

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 8

Joel Thornton University of California-Berkeley Graduate studentRebecca Rosen University of California-Berkeley Graduate studentDouglas Day University of California-Berkeley Graduate studentJennifer Murphy University of California-Berkeley Graduate studentDaniel Murphy New Mexico Tech Undergraduate (Senior Thesis)Julie Snow University of Rhode Island Post-DoctoralFan Lei University of Maryland Graduate StudentDouglas Orsini Georgia Tech Post-DoctoralBaoan Wang Georgia Tech Graduate StudentMat Evans Harvard University Post-DoctoralAndrzej Klonecki NCAR ASPCraig Stroud NCAR ASPBrian Wert University of Colorado Graduate StudentAnthony Wimmers University of Virginia Graduate StudentOwen Cooper University of Virginia Graduate StudentJennifer Andrews University of Virginia Undergraduate StudentMark Zondlo NCAR ASPJohn Hair Old Dominion University Post-DocAlton Jones Old Dominion University Graduate StudentAaron Katzenstein UCI Graduate studentBarbara Barletta UCI Graduate studentSimone Meinardi UCI PostdocAlex Choi UCI Graduate studentChangsub Shim Rutgers Univ Graduate studentLinsey Debell Univ. New Hampshire Graduate studentEric Scheuer Univ. New Hampshire Graduate studentUnfunded collaborators:Barkley Sive, Assistant Professor at Central Michigan UniversityOliver Wingenter, Assistant Professor at New Mexico Tech UniversityJodye Selco, Assistant Professor at The University of Redlands

TOPSE Educational Activities

Page 9: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 9

90

80

70

60

50

40

30

Latit

ude

-140 -120 -100 -80 -60 -40 -20Longitude

Denver

Winnipeg

Churchill

Thule

Alert

TOPSE Flight Tracks: Feb - May, 2000

1 2 3 4 5 6 7

Deployment Number

TOPSE Flight Tracks

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 10

• 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

Some TOPSE Highlights

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 11

• 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)

Some TOPSE Highlights (cont’d)

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 12

Median Latitude and Altitude Profiles

(Blake – UCI)

Latitude Profiles: Altitude Profiles

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 13

TOPSE SULFATE MIXING RATIO GEOMETRIC MEAN ALTITUDE PROFILE

(Latitudes 58oN to 85oN)

Aerosol sulfate mixing ratio (pptv)

0 50 100 150 200 250

Pre

ssu

re A

ltitu

de

(m

ete

rs)

0

2000

4000

6000

1

1

1

1

1

1

1

1

2

2

2

2

2

2

2

2

3

3

3

3

3

3

3

3

4

4

4

4

4

4

4

4

5

5

5

5

5

5

5

5

6

6

6

6

6

6

6

6

7

7

7

7

7

7

7

7

1

2

3

4

5

6

7

1988 GTE/ABLE 3A Summertime SO42- Averages

(Scheuer, Talbot, Dibb – UNH)

Evolution of Sulfate Aerosol Vertical Distribution

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 14

6000

4000

2000

0

Pre

ssur

e A

ltitu

de (

m)

250200150100500Ozone (ppbv)

140

120

100

80

60

40

Day of Y

ear

(Ridley, Walega)

Ozone vertical profile: Evolution during winter-spring

BR_O3

52.315 53.8957.04

59.63562.86 63.065

74.61

30

40

50

60

70

80

90

100

0 1 2 3 4 5 6 7 8

Mission

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 15

Deployment 1 Deployment 3

Deployment 6Deployment 5

Deployment 4

Deployment 7

Average Ozone Distributions During TOPSE(Browell et al., NASA)

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 16

February1.7 ppb/mo

May12 ppb/mo

April14 ppb/mo

March7 ppb/mo

(Y. Wang, Rutgers Univ)

Model calculated O3 production and loss40 – 60 N; integrated surface to 9 km

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 17

7Be vs O3

Observed “stratospheric influence”

7Be – O3 relationship and stratospheric influence during TOPSE

(Dibb et al., UNH)

Page 18: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 18ODE from Thule to east side of Baffin Island

Surface Ozone Depletion Over Baffin Bay

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Chris Cantrell TOPSE: Tropospheric Ozone Production about the Spring Equinox 19

Transport of surface ozone hole to Hudson Bay

Page 20: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Chris Cantrell 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.

Page 21: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Peter Hess HANK 37

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

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Peter Hess HANK 38

HANK - Model Overview

Chemical Transport Model driven from MM5

• Resolution: variable (10 x 10 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

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Peter Hess HANK 39

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 as revealed during the spring MLOPEX intensive, J. Geophys. Res., 105, 26809-26839, 2000.

Vukicevic, T. and P. G. Hess, Analysis of tropospheric transport in the Pacific Basin using the adjoint 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.

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Peter Hess HANK 40

Pacific Basin Simulations (MLOPEX)

Adjoint Trajectory forpollutant plume to Hawaii

Same trajectory in height- longitude plane

Chemical transformations and rainout along the trajectory

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Peter Hess HANK 41

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

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Peter Hess HANK 42

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)

Page 27: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Fred Eisele ACD contribution to TRACE-P 43

Atmospheric Chemistry DivisionNational Center for Atmospheric Research

ACD Contributions to the NASA TRACE-P*Campaign

Fred EiseleSenior Research Associate

Photochemical Oxidation & Products

24-26 October 2001, NSF Review

*(TRAnsport and Chemical Evolution over the Pacific)

Page 28: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Fred Eisele ACD contribution to TRACE-P 44

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

Page 29: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Fred Eisele ACD contribution to TRACE-P 45

MISSION OBJECTIVES

Determine Asian outflow pathways

Determine the chemical evolution of outflow

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Fred Eisele ACD contribution to TRACE-P 46

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

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Fred Eisele ACD contribution to TRACE-P 47

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.

Page 32: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Fred Eisele ACD contribution to TRACE-P 48

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.

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Fred Eisele ACD contribution to TRACE-P 49

• 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.

Page 34: 1 TROPOSPHERIC CHEMISTRY  TOPSE: Tropospheric Ozone Production About the Spring Equinox –Example of a division lead community initiative supported by.

Fred Eisele ACD contribution to TRACE-P 50

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

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Fred Eisele ACD contribution to TRACE-P 51

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

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Fred Eisele ACD contribution to TRACE-P 52

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

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Sasha Madronich MIRAGE 53

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 MadronichSenior ScientistTheoretical Studies and Modeling (TSM)

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Sasha Madronich MIRAGE 54

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

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Sasha Madronich MIRAGE 55

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

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Sasha Madronich MIRAGE 56

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.

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Sasha Madronich MIRAGE 57

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)

0

200

400

600

800

0 1 2 3

Time, days

Co

nce

ntr

atio

n, p

pb

O3

NO2

O3+NO2

S. Rivale (SOARS) and S. Madronich, unpubl. 1999

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Sasha Madronich MIRAGE 58

Gas Phase Photochemistry - 2

Example of chemical complexity:

Persistence of oxygenated organic intermediates

Madronich and Calvert 1990, uptdated by C. Stroud 2001

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Sasha Madronich MIRAGE 59

Aerosol Physics and Photochemistry

Example of aerosol-gas phase coupling:

Growth of organic aerosol by dissolution of gas phase species

Aumont et al., 2000

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Sasha Madronich MIRAGE 60

Radiation in Polluted Environments

Photolysis rates in polluted conditions:

Outside Mexico City (Tres Marias) 15 April 94

6 9 12 15 18

Local time, hrs.

Mexico City 11 Feb 94

0.E+00

2.E-03

4.E-03

6.E-03

8.E-03

1.E-02

6 9 12 15 18

Local time, hrs

J NO

2, s

-1

JNO2_exp

clean

wo=0.95

wo=0.80

Castro et al. 2001

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Sasha Madronich MIRAGE 61

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)

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Sasha Madronich MIRAGE 62

Urban Metabolism - 1

World’s largest cities

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Sasha Madronich MIRAGE 63

Urban Metabolism - 2

Emissions in developing cities are very different than in developed cities

Urban NOx Emissions

0

20

40

60

80

100

1980 2000 2020 2040 2060 2080

Year

% to

t NO

x fr

om

urb

an 30-40N

16-23N

Mayer et al. 2000

Aerosol Emissions

0

20

40

60

80

100

1980 2000 2020 2040

Year

% o

f Tot

al

Underdeveloped

Developed

240Tg/yr

513 Tg/yr

Wolf et al. 1997

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Sasha Madronich MIRAGE 64

Site Selection Criteria - 1

Megacity characteristics (ranked by population in 2000)

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Sasha Madronich MIRAGE 65

Site Selection Criteria - 2

Pollution signal strength relative to background

CO from MOPPIT

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Sasha Madronich MIRAGE 66

Site Selection - 5

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Sasha Madronich MIRAGE 67

ACD’s Capability-based Foci

• Distributions– Local emissions and concentrations– Surrounding emissions and concentrations– UV radiation

• Processes– Gas phase photo-chemistry, esp. evolution of oxygenated

and nitrogenated organics– Aerosol growth and interactions with gas-phase

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Sasha Madronich MIRAGE 68

The Next Steps

• Tentative site selection

• Identify key collaborators (esp. at site)

• Develop proposal, distribute for critique by community with call for input, collaborations

• Hold community workshop

• Develop implementation plan

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Elliot Atlas Reactive Carbon Research Initiative 69

Atmospheric Chemistry DivisionNational Center for Atmospheric Research

Reactive Carbon Research Initiative

Elliot AtlasSenior Scientist

Stratospheric/Tropospheric Measurements Group

24-26 October 2001, NSF Review

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Elliot Atlas Reactive Carbon Research Initiative 70

Significance

•Impact on tropospheric oxidant cycles•Urban, regional, global scales•Upper troposphere/lower stratosphere

•Biosphere-atmosphere exchanges•Carbon exchange•Nitrogen cycling

•Role in aerosol processes and climate•Aerosol organic composition/processing•Hygroscopic properties/nucleation

•Impact on stratospheric chemistry•Organic halogen •Methane/water vapor

Reactive Carbon in the Atmosphere

From P. Shepson

From A. Guenther

From J. SeinfeldFrom P. Newman/SOLVE

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Elliot Atlas Reactive Carbon Research Initiative 71

MotivationTo better understand the evolution, fate and interactions of reactive carbon in the atmosphere.

Issues1. What are products of biogenic and anthropogenic carbon

oxidation? What is the distribution of these products in the atmosphere?

2. What are links between carbon oxidation and the nitrogen cycle?3. How does reactive carbon oxidation and product formation affect

atmospheric oxidant production and loss?4. How do reactive carbon oxidation products influence aerosol

production, composition, and growth?5. What are the significant sources (and sinks) of reactive carbon?

What is variation of surface exchanges and controlling variables?

Reactive Carbon Research Initiative

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Elliot Atlas Reactive Carbon Research Initiative 72

Reactive Carbon Research Initiative

Approach

Coordination of ACD and community research to address specific questions using a combination of existing and developing measurement technology, model simulations, laboratory studies and field investigations.

Focus on quantitative understanding of selected trace gases representative of different major sources.

Biogenic – Isoprene and selected terpenesAnthropogenic – Toluene; Selected others

Implementation in process studies and incorporation in larger field efforts.

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Elliot Atlas Reactive Carbon Research Initiative 73

Reactive Carbon Research Initiative

Research Foci:

– Atmospheric history of reactive carbon

– Carbon – nitrogen interactions

– Aerosol processes and organic interactions

– Radicals and oxidants

– Emission and deposition fluxes

– Development of tools and techniques

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Elliot Atlas Reactive Carbon Research Initiative 74

Reactive Carbon Research Initiative

Atmospheric history of reactive carbonLaboratory Investigations:

Basic alkoxy/peroxy radical investigationsAromatics oxidationIsoprene/Terpene product studies

Model Investigations:Updated Master MechanismGas-aerosol partitioning

Field Investigations:Process studies: Predicted vs. measured productsSurvey studies: Investigations related to specific

source regions (MIRAGE, etc.) Source profiles from developing regions. Effects of land-use change.

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Elliot Atlas Reactive Carbon Research Initiative 75

HCHO Yield

0.00 0.25 0.50 0.75 1.00 1.25 1.50 1.75 2.00

z (k

m)

0

2

4

6

8

10

12

14

16

NCAR

1997 evaluation

Most Models

Formaldehyde Yield From OH + Ethene

Temperature effects on CH2O yield

(G. Tyndall, J. Orlando)

1997 evaluation

NCAR

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Elliot Atlas Reactive Carbon Research Initiative 76

Isoprene and oxidation products in Houston

OH and O3

Cl

CH3

CH2 CH2

+ CH3

OCH CH2

MVK

CH2 C

CH3

CH

O

MACR

H2CO

Formaldehyde

OH or O3

Isoprene

ClCl

C

CH3

CH CH

O

CMBA isomers

CH3

CH2 CH2

+ CH2 C

CH3

C CH2Cl

O

CMBOIsoprene

9/1/2000 00:00 9/1/2000 12:00 9/2/2000 00:00 9/2/2000 12:00 9/3/2000 00:001E-3

0.01

0.1

1

10Houston 2000

pp

b

time (local)

Isoprene Methacrolein Methyl Vinyl Ketone CMBO CMBA

Daniel Riemer, UMEric Apel, NCAR

Isoprene

Methacrolein

Methyl Vinyl Ketone

CMBO/CMBA

Chloromethylbutenone(CMBO)

Chloromethylbutenalisomers (CMBA)

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Elliot Atlas Reactive Carbon Research Initiative 77

Reactive Carbon Research Initiative

Carbon – nitrogen interactions

Laboratory Investigations:Product/yield studies:

Hydroxy-, multifunctional nitratesPANs

Model Investigations:Updated Master MechanismGas-aerosol partitioning

Field Investigations:Process studies: Predicted vs. measured productsSurvey studies: Investigations related to specific

source regions (Biogenic emissions),Role of PANs in UT/LS region

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Elliot Atlas Reactive Carbon Research Initiative 78

Initial pathways for isoprene oxidation

(from Sprengnether et al., submitted)

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Elliot Atlas Reactive Carbon Research Initiative 79

-Pinene oxidation scheme

(Kamens and Jaoui, 2001)

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Elliot Atlas Reactive Carbon Research Initiative 80

Overlaid Chromatogram Plots

File: f:\bear_vg data_aug_01\aug 29 2001 #012.smsSample: L1- 1st Operator: AtlasScan Range: 1 - 4860 Time Range: 3.33 - 32.73 min. Date: 8/29/01 3:26 PMSample Notes: 3 ul int std, 8/22 -23 2319-1105

5 10 15 20 25minutes

10%

20%

30%

40%

50%

Norm Ion: 46 all aug 29 2001 #012.sms -0.046971 min offsetIon: 62 all aug 29 2001 #012.sms 0.028137 min offsetIon: 169 all aug 29 2001 #012.sms 0.109292 min offset

46 = NO2-

62 = NO3-

Isoprene + multifunctionalnitrates

C4-C6 + alkyl nitrates Terpene

nitrates?

m/e=169

GC-NICI-MS of complex organic nitrates in Blodgett Forest

(Cohen,Day –UCB;Atlas,Flocke – NCAR)

CH3

CH3

CH3OH

ONO2

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Elliot Atlas Reactive Carbon Research Initiative 81

Reactive Carbon Research Initiative

Aerosol processes and organic interactions

Laboratory Investigations:Organic acid formationSecondary product/aerosol reactionsRole of organics in nucleation

Model Investigations:Updated mechanismGas-aerosol partitioningIncorporation in larger scale models

Field Investigations:Process studies: Predicted vs. measured productsSurvey studies: Investigations related to specific

source regions (Biogenic emissions/Urban plume)

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Elliot Atlas Reactive Carbon Research Initiative 82

74%

3%6%

11%

6%

Anhydrosugars

Sugars/sugar alcohols

Di-/triacids

Oxo-/hydroxyacids

Aromatics

(Graham et al., JGR)

Anhydrosugars Di-/tricarboxylic acidsArabinosan Malonic acidXylosan Methylmalonic acidGalactosan Maleic acidMannosan Succinic acidLevoglucosan Methylsuccinic acid1,6-Anhydro-b-D-glucofuranose Fumaric acidN -Acetyl-2-aminoglucosan Glutaric acid

Sugars/sugar alcohols Adipic acidGlycerol Tricarballylic acidThreitol Azelaic acidErythritol Oxo-/hydroxyacidsXylose Glyoxylic acidArabitol Pyruvic acidFructose Lactic acidMannose Glycolic acidGalactose Glyceric acidGlucose Malic acidMannitol Hydroxymalonic acidSorbitol 2-Ketoglutaric acidInositol 2-Hydroxyglutaric acidSucrose Threonic acidTrehalose Tartaric acid

4-Ketopimelic acidAromatic acids

3-Hydroxybenzoic acid4-Hydroxybenzoic acidVanillinPhthalic acidVanillic acidSyringaldehyde3,4-Dihydroxybenzoic acidVanilethanediolSyringic acid

Composition of WSOC in biomass burning aerosol from Amazonia

Sample F12, 0.17 µg m-3

identified

Sample P2, 10.50 µg m-3

identified

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Elliot Atlas Reactive Carbon Research Initiative 83

Organics…A role in new particle formation?

Critical nucleation cluster (tentative identification)

NH3 H2SO4 H2SO4(Hanson and Eisele)

Amines vs. ammonia? Organic acids vs. sulfuric?

RNH2 R(OH)COOH

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Elliot Atlas Reactive Carbon Research Initiative 84

Reactive Carbon Research Initiative

Radicals and oxidants

Laboratory Investigations:Photochemically active organics as radical sourceRO2 speciation as tool to understand reactive carbon

degradation

Model Investigations:Role of reactive carbon in cycling OH/HO2/RO2

Model update and prediction of oxidant production

Field Investigations:Process studies: Predicted vs. measured radical

sources/sinks and oxidant production.

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Elliot Atlas Reactive Carbon Research Initiative 85

M easured Species Calspan Oct 19, 1998

0

50

100

150

200

250

300

10:00 11:00 12:00 13:00 14:00

Tim e of Day

Co

nce

ntr

ati

on

a-pinene, ppbv*10 RO2, pptv NO, ppbv*50 NOx, ppbv*50O3, ppbv CN/200 RH% LW C*500

Figure 2.

Observations of RO2 – cloud interactions

Cantrell et al.

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Elliot Atlas Reactive Carbon Research Initiative 86

Reactive Carbon Research Initiative

Emission and deposition fluxes

Laboratory Investigations:Leaf/Branch level emission studies

Model Investigations:Flux parameterization/Controlling variablesGas-aerosol partitioningIncorporation in larger scale models

Field Investigations:Process studies: Evaluation of emission fluxes from different environments; Estimation of deposition fluxesSurvey studies: Improved estimation of speciated VOC emissions/oxidation products (esp. biogenic VOC)

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Elliot Atlas Reactive Carbon Research Initiative 87

OxyVOC emissions from a Colorado alfalfa field before and after cutting

1.2

1.0

0.8

0.6

0.4

0.2

0.0

-0.2

-0.4

ace

tald

eh

yde

, ace

ton

(m

g/m

^2

*h)

12:008/12/00

12:008/13/00

12:008/14/00

12:008/15/00

Datatime

10

5

0

me

tha

no

l (mg

/m^

2*h

)

acetaldehyde methanol aceton

Cutting

growing

drying

Rinne et al. GRL 28: 3139-3142 (2001)

e

(Rinne, Guenther)

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Elliot Atlas Reactive Carbon Research Initiative 88

Reactive Carbon Research Initiative

Development of tools and techniques

LaboratoryFlow tube and smog chamberIntegrated MS techniquesGas-aerosol partitioning

ModelIncorporation and update with relevant results

Field Gas phase chemistry:

PTR/MS, MS/MS, Fast GC/MS, TDLemissions and oxidation products

Aerosol organic chemistry:Aerosol Ion Trap: particle compositionLC/MS: water soluble organic carbon

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Elliot Atlas Reactive Carbon Research Initiative 89

New instrument development (examples)

Aeros ol I n le t

(15 lpm )

Sam pleC ollec t ion

F ilam ent

Sheath G as

(1 lpm )

L inear

Ac tuator Ion izat ionR egion

C ollis ion

C ham ber

To Mas sSpec t rom eter

34"

Ultrafine OrganicAerosol Instrument(J. Smith)

LC/MS/MS for water soluble organics (E. Atlas)

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Elliot Atlas Reactive Carbon Research Initiative 90

Reactive Carbon Research Initiative

Relationship to existing and planned research

MIRAGEFocus on reactive carbon evolution/TracersAerosol characterization/reactionsLaboratory investigations

UT/LSVOC as sources of ROx VOC as transport tracers/halogen sources

CloudsWater soluble organic characteristicsVOC partitioningSource tracer measurement

Biosphere, Chemistry and ClimateFlux estimates of VOC from different environments

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John C. Gille The MOPITT Experiment on Terra 91

Atmospheric Chemistry DivisionNational Center for Atmospheric Research

John GilleSenior ScientistMOPITT and HIRDLS Groups24-26 October 2001, NSF Review

The MOPITT Experiment on Terra

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John C. Gille The MOPITT Experiment on Terra 92

MOPITT OVERVIEW

Measurements Of Pollution In The Troposphere• Joint University of Toronto/NCAR satellite instrument project• Developed from Prof. James Drummond’s sabbatical at NCAR

in 1987• University of Toronto and NCAR supporting project with their

expertise

Measurement Goals: Obtain long term global measurements of:

Profiles and columns of Tropospheric CO Total columns of CH4

Demonstrate capability to make and use measurements of tropospheric composition from space

Applications: Improve knowledge of sources, sinks and transformationsTesting and improvement of model transport and chemistry

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John C. Gille The MOPITT Experiment on Terra 93

MOPITT Investigators

Principal Investigator - James Drummond, UT (CSA Funding) Instrument development, calibration, orbital operation Lead U.S. Investigator - John Gille, NCAR (NASA Funding) Develop, test, apply and update data processing algorithms

Co-Investigators

G.P. Brasseur, Max Planck Institute G.R. Davis, University of Saskatoon J.C. McConnell, York University G.D. Peskett, Oxford University H.G. Reichle, North Carolina State University N. Roulet, McGill University

Further information at

http://www.eos.ucar.edu/mopitt/home.html

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John C. Gille The MOPITT Experiment on Terra 94

John Gille US Principal Investigator David Edwards NCAR Project Leader

Jarmei Chen Merritt Deeter Louisa Emmons Gene Francis David Grant Alan Hills Shu-peng Ho Boris Khattatov

Jean-Francois Lamarque Debbie Mao Jianguo Niu Dan Packman BarbTunison Juying Warner Valery Yudin Dan Ziskin

The NCAR/ACD MOPITT Team

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95The MOPITT Experiment on TerraJohn C. Gille

History of MOPITT

• 1987 - Prof. James Drummond takes sabbatical at NCAR with John Gille Possibilities for measurement of tropospheric CO discussed• 1988 - MOPITT proposed to NASA• 1989 - Provisional acceptance, beginning of retrieval studies at NCAR• 1990 - Acceptance for development

– Development and testing of retrieval algorithms and operational code at NCAR

• 1999 - Launch in December• 2000 - (March) Reach final orbit, begin data collection (September) Filter position determined, initial good data retrievals• 2001 - (May) Cooler failure, instrument in Safe Mode (June) Begin testing Retrieval Beta version (July) Instrument restarted with single cooler (August) PMC modulation increased

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John C. Gille The MOPITT Experiment on Terra 96

MOPITT Instrument

MOPITT Instrument: 8 channel nadir viewing gas correlation radiometer

4 channels @ 4.7 m - thermal emission from atmosphere and sfc.

4 channels @ 3.3 m - reflected solar radiation Gas correlation radiometer reduces effects of interfering species, at

the expense of radiative transfer complexity Sensitivity to small radiance changes

The MOPITT instrument and the measurement technique are new: Lessons are being learned in both instrument operation and data processing

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John C. Gille The MOPITT Experiment on Terra 97

- Level 1 data products - Calibrated and geo-located radiances

- Level 2 data products - Tropospheric CO profiles with a 22 km horizontal resolution

Mixing ratios at surface, 850, 700, 500, 350, 250, 150 hPa with 10% precision

- CO total column with 10% precision

- CH4 total column with 1% precision

- Level 3 data products (initially a research product) - Gridded global CO distribution

- Gridded global CH4 distribution

MOPITT StandardScientific Products

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John C. Gille The MOPITT Experiment on Terra 98

MOPITT Data Processing

1.00.80.60.40.2

2240222022002180216021402120

1.5

1.0

0.5

2240222022002180216021402120

CO

H2O

Other

Tran

smit

tan

ceR

adia

nce

(x1

0-3)

[W/(

m2 s

r c

m-1

)]

Wavenumber (cm-1)

MOPITT Thermal Channel Gas Transmittances

Top of Atmosphere Radiance and Channel Response

Wavenumber (cm-1)

L1

NCEP

Clim

Input Cloud Retrieval L2

Forward Model Maximum

Likelihood

method

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John C. Gille The MOPITT Experiment on Terra 100

March

Dec

June

Sept

Monthly mean (2000) CO 700 mb

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John C. Gille The MOPITT Experiment on Terra 101

MOPITT Level 2 CO Column

MOPITT Level 2 CO total column shows:

Aug 20-27 2000

• High CO amounts correlate with areas of industrial pollution and biomass burning

• Inter-continental transport• Good comparison with in-

situ aircraft and FTIR data

Plumes from western forest fires clearly seen

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John C. Gille The MOPITT Experiment on Terra 102

MOPITT Data Assimilation in MOZART 2

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John C. Gille The MOPITT Experiment on Terra 103

Accomplishments Since Launch

• Diagnosis and correction of instrument artifacts, development of preliminary algorithm

• Public release of preliminary CO total column and profile retrievals in September 2001

• Validation begun with comparisons against Trace-P, CMDL and other profiles and FTIR total column

• Real-time data provided for TRACE-P flight planning in February-March 2001

• Assimilation of MOPITT data with the MOZART-2 CTM

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John C. Gille The MOPITT Experiment on Terra 105

Initial Example of Single Cooler Data

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John C. Gille The MOPITT Experiment on Terra 106

Future plans

Three Major Thrusts

• Algorithm improvements

– e.g. Retrieve CH4 column data

– Reduce retrieval bias, other artifacts– Cloud detection and clearing, using MODIS data

• Data quality assessment (“Validation”)– vs. A/C profile measurements fromTrace-P, CMDL, other– vs. ground based FTIR column measurements

• Application of data– To studies of transports, sources, chemical impacts– Inverse modeling to constrain surface emissions– Participation in campaign planning (e.g. MIRAGE)

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John C. Gille The MOPITT Experiment on Terra 107

Future Outlook

Studies of tropospheric chemistry from space is in its infancy, but offers great promise

Data assimilation will be extremely important in scientific studies

ACD has expertise in remote sounding and data assimilation, and plans to remain involved in this kind of activity

Possible future activities• Involvement in SCIAMACHY validation and data use • Interactions with Tropospheric Emission Spectrometer

on Aura• “MOPITT - 2” under discussion• Evaluation of other instrumental approaches• Collaboration with other experimental groups