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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
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
slide2

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

slide3

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

slide4

Specific Scientific Questions

TOPSE: Tropospheric Ozone Production about the Spring Equinox

slide5

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

slide6

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

slide7

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

slide8

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

slide9

TOPSE Flight Tracks

TOPSE: Tropospheric Ozone Production about the Spring Equinox

slide10

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

slide11

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

slide12

Median Latitude and Altitude Profiles

Latitude Profiles:

Altitude Profiles

(Blake – UCI)

TOPSE: Tropospheric Ozone Production about the Spring Equinox

slide13

Evolution of Sulfate Aerosol Vertical Distribution

(Scheuer, Talbot,

Dibb – UNH)

TOPSE: Tropospheric Ozone Production about the Spring Equinox

slide14

Ozone vertical profile: Evolution during winter-spring

(Ridley, Walega)

TOPSE: Tropospheric Ozone Production about the Spring Equinox

slide15

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

slide16

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

slide17

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

slide18

Surface Ozone Depletion Over Baffin Bay

ODE from Thule to east side of Baffin Island

TOPSE: Tropospheric Ozone Production about the Spring Equinox

slide19

Transport of surface ozone hole to Hudson Bay

TOPSE: Tropospheric Ozone Production about the Spring Equinox

summary
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

atmospheric chemistry division national center for atmospheric research
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

hank model overview
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

hank science
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

slide24

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

slide25

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

hank plans
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

atmospheric chemistry division national center for atmospheric research27
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

trace p university collaborations
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

mission objectives
MISSION OBJECTIVES

Determine Asian outflow pathways

Determine the chemical evolution of outflow

ACD contribution to TRACE-P

common objectives
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

measurement acd participants
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

trace p data
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

slide33
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

slide34

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

summary35
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

future trace p contributions
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

atmospheric chemistry division national center for atmospheric research37
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

history
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

working groups
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

new scientific foci
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

gas phase photochemistry 1
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

gas phase photochemistry 2
Gas Phase Photochemistry - 2

Example of chemical complexity:

Persistence of oxygenated organic intermediates

Madronich and Calvert 1990, uptdated by C. Stroud 2001

MIRAGE

aerosol physics and photochemistry
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

radiation in polluted environments
Radiation in Polluted Environments

Photolysis rates in polluted conditions:

Castro et al. 2001

MIRAGE

local and regional meteorology
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

urban metabolism 1
Urban Metabolism - 1

World’s largest cities

MIRAGE

urban metabolism 2
Urban Metabolism - 2

Emissions in developing cities are very different than in developed cities

MIRAGE

site selection criteria 1
Site Selection Criteria - 1

Megacity characteristics (ranked by population in 2000)

MIRAGE

site selection criteria 2
Site Selection Criteria - 2

CO from MOPPIT

  • Pollution signal strength relative to background

MIRAGE

acd s capability based foci
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

MIRAGE

the next steps
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

MIRAGE

atmospheric chemistry division national center for atmospheric research53
Atmospheric Chemistry DivisionNational Center for Atmospheric Research

Reactive Carbon Research Initiative

Elliot Atlas

Senior Scientist

Stratospheric/Tropospheric Measurements Group

24-26 October 2001, NSF Review

Reactive Carbon Research Initiative

slide54

Reactive Carbon in the Atmosphere

  • 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

From P. Shepson

From A. Guenther

From J. Seinfeld

From P. Newman/SOLVE

Reactive Carbon Research Initiative

slide55

Reactive Carbon Research Initiative

  • Motivation
  • To better understand the evolution, fate and interactions of reactive carbon in the atmosphere.
  • Issues
  • What are products of biogenic and anthropogenic carbon oxidation? What is the distribution of these products in the atmosphere?
  • What are links between carbon oxidation and the nitrogen cycle?
  • How does reactive carbon oxidation and product formation affect atmospheric oxidant production and loss?
  • How do reactive carbon oxidation products influence aerosol production, composition, and growth?
  • What are the significant sources (and sinks) of reactive carbon? What is variation of surface exchanges and controlling variables?

Reactive Carbon Research Initiative

reactive carbon research initiative
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 terpenes

Anthropogenic – Toluene; Selected others

Implementation in process studies and incorporation in larger field efforts.

Reactive Carbon Research Initiative

reactive carbon research initiative57
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

Reactive Carbon Research Initiative

slide58

Reactive Carbon Research Initiative

Atmospheric history of reactive carbon

Laboratory Investigations:

Basic alkoxy/peroxy radical investigations

Aromatics oxidation

Isoprene/Terpene product studies

Model Investigations:

Updated Master Mechanism

Gas-aerosol partitioning

Field Investigations:

Process studies: Predicted vs. measured products

Survey studies: Investigations related to specific source regions (MIRAGE, etc.) Source profiles from developing regions. Effects of land-use change.

Reactive Carbon Research Initiative

slide59

Temperature effects on CH2O yield

NCAR

1997evaluation

(G. Tyndall, J. Orlando)

Reactive Carbon Research Initiative

slide60

Isoprene and oxidation products in Houston

OH and O3

Cl

Isoprene

Methyl Vinyl Ketone

Methacrolein

CMBO/CMBA

Daniel Riemer, UM

Eric Apel, NCAR

Chloromethylbutenone

(CMBO)

Chloromethylbutenal

isomers (CMBA)

Reactive Carbon Research Initiative

slide61

Reactive Carbon Research Initiative

Carbon – nitrogen interactions

Laboratory Investigations:

Product/yield studies:

Hydroxy-, multifunctional nitrates

PANs

Model Investigations:

Updated Master Mechanism

Gas-aerosol partitioning

Field Investigations:

Process studies: Predicted vs. measured products

Survey studies: Investigations related to specific source regions (Biogenic emissions),

Role of PANs in UT/LS region

Reactive Carbon Research Initiative

slide62

Initial pathways for isoprene oxidation

(from Sprengnether et al., submitted)

Reactive Carbon Research Initiative

slide63

a-Pinene oxidation scheme

(Kamens and Jaoui, 2001)

Reactive Carbon Research Initiative

slide64

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

C4-C6 + alkyl nitrates

Isoprene + multifunctional

nitrates

46 = NO2-

Terpene nitrates?

62 = NO3-

m/e=169

(Cohen,Day –UCB;

Atlas,Flocke – NCAR)

Reactive Carbon Research Initiative

slide65

Reactive Carbon Research Initiative

Aerosol processes and organic interactions

Laboratory Investigations:

Organic acid formation

Secondary product/aerosol reactions

Role of organics in nucleation

Model Investigations:

Updated mechanism

Gas-aerosol partitioning

Incorporation in larger scale models

Field Investigations:

Process studies: Predicted vs. measured products

Survey studies: Investigations related to specific source regions (Biogenic emissions/Urban plume)

Reactive Carbon Research Initiative

slide66

Composition of WSOC in biomass burning

aerosol from Amazonia

(Graham et al., JGR)

Reactive Carbon Research Initiative

slide67

Organics…A role in new particle formation?

Critical nucleation cluster (tentative identification)

NH3

(Hanson and Eisele)

H2SO4 H2SO4

Amines vs. ammonia?

Organic acids vs. sulfuric?

RNH2

R(OH)COOH

Reactive Carbon Research Initiative

slide68

Reactive Carbon Research Initiative

Radicals and oxidants

Laboratory Investigations:

Photochemically active organics as radical source

RO2 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.

Reactive Carbon Research Initiative

slide69

Observations of RO2 – cloud interactions

Cantrell et al.

Reactive Carbon Research Initiative

slide70

Reactive Carbon Research Initiative

Emission and deposition fluxes

Laboratory Investigations:

Leaf/Branch level emission studies

Model Investigations:

Flux parameterization/Controlling variables

Gas-aerosol partitioning

Incorporation in larger scale models

Field Investigations:

Process studies: Evaluation of emission fluxes from different environments; Estimation of deposition fluxes

Survey studies: Improved estimation of speciated VOC emissions/oxidation products (esp. biogenic VOC)

Reactive Carbon Research Initiative

slide71

drying

e

Cutting

growing

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

OxyVOC emissions from a Colorado alfalfa field before and after cutting

(Rinne, Guenther)

Reactive Carbon Research Initiative

slide72

Reactive Carbon Research Initiative

Development of tools and techniques

Laboratory

Flow tube and smog chamber

Integrated MS techniques

Gas-aerosol partitioning

Model

Incorporation and update with relevant results

Field

Gas phase chemistry:

PTR/MS, MS/MS, Fast GC/MS, TDL

emissions and oxidation products

Aerosol organic chemistry:

Aerosol Ion Trap: particle composition

LC/MS: water soluble organic carbon

Reactive Carbon Research Initiative

slide73

New instrument development (examples)

Ultrafine Organic

Aerosol Instrument

(J. Smith)

LC/MS/MS for water soluble organics

(E. Atlas)

Reactive Carbon Research Initiative

slide74

Reactive Carbon Research Initiative

Relationship to existing and planned research

MIRAGE

Focus on reactive carbon evolution/Tracers

Aerosol characterization/reactions

Laboratory investigations

UT/LS

VOC as sources of ROx

VOC as transport tracers/halogen sources

Clouds

Water soluble organic characteristics

VOC partitioning

Source tracer measurement

Biosphere, Chemistry and Climate

Flux estimates of VOC from different environments

Reactive Carbon Research Initiative

atmospheric chemistry division national center for atmospheric research75
Atmospheric Chemistry DivisionNational Center for Atmospheric Research

The MOPITT Experiment on Terra

John Gille

Senior Scientist

MOPITT and HIRDLS Groups

24-26 October 2001, NSF Review

The MOPITT Experiment on Terra

mopitt overview
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 transformations

Testing and improvement of model transport and chemistry

The MOPITT Experiment on Terra

mopitt investigators
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

The MOPITT Experiment on Terra

slide78

The NCAR/ACD MOPITT Team

  • 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 MOPITT Experiment on Terra

history of mopitt
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

The MOPITT Experiment on Terra

mopitt instrument
MOPITT Instrument:

8 channel nadir viewing gas correlation radiometer

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

4 channels @ 3.3 mm - 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

MOPITT Instrument

The MOPITT Experiment on Terra

mopitt standard scientific products
MOPITT StandardScientific Products

- 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

The MOPITT Experiment on Terra

mopitt data processing
MOPITT Data Processing

L1

L2

NCEP

Input

Cloud

Retrieval

Clim

Forward Model

Maximum

Likelihood

method

The MOPITT Experiment on Terra

monthly mean 2000 co 700 mb
Monthly mean (2000) CO 700 mb

June

March

Sept

Dec

The MOPITT Experiment on Terra

mopitt level 2 co column
MOPITT Level 2 CO Column

Plumes from western forest fires clearly seen

MOPITT Level 2 CO total column shows:

  • High CO amounts correlate with areas of industrial pollution and biomass burning
  • Inter-continental transport
  • Good comparison with in-situ aircraft and FTIR data

Aug 20-27 2000

The MOPITT Experiment on Terra

slide85

MOPITT Data Assimilation in MOZART 2

The MOPITT Experiment on Terra

accomplishments since launch
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

The MOPITT Experiment on Terra

slide87

Initial Example of Single Cooler Data

The MOPITT Experiment on Terra

future plans
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)

The MOPITT Experiment on Terra

future outlook

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

The MOPITT Experiment on Terra