continental outflow and intercontinental transport at northern midlatitudes (and a few ut/ls topics)...
TRANSCRIPT
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CONTINENTAL OUTFLOW AND INTERCONTINENTAL CONTINENTAL OUTFLOW AND INTERCONTINENTAL TRANSPORT AT NORTHERN MIDLATITUDES TRANSPORT AT NORTHERN MIDLATITUDES
(and a few UT/LS topics)(and a few UT/LS topics)
Daniel J. Jacob
Atmospheric Chemistry Modeling Group
Harvard University
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ARE ATMOSPHERIC OBSERVATIONS OF ACETONEARE ATMOSPHERIC OBSERVATIONS OF ACETONECONSISTENT WITH CURRENT UNDERSTANDINGCONSISTENT WITH CURRENT UNDERSTANDING
OF SOURCES AND SINKS?OF SOURCES AND SINKS?
TRACE-A
SONEX
ABLE-3B PEM
-WB
PEM-TB
Surface sites
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GLOBAL BUDGET OF ATMOSPHERIC ACETONEGLOBAL BUDGET OF ATMOSPHERIC ACETONE
Singh et al. Jacob et al. [2002]
[2000] (a priori) (a posteriori)
SOURCES (Tg yr-1) 56 (37-80) 78 (49-105) 95 (80-110)
Terrestrial vegetation 15 (10-20) 26 (0-52) 33 (24-42)
Plant decay 6 (4-8) 9 (0-18) 2 (-3-7)
Biomass burning 5 (3-10) 3 (2-5) 5 (3-7)
Industry 2 (1-3) 1 (1-2) 1 (1-2)
Oceans 0 10 (0-20) 27 (21-33)
Oxidation of isoalkanes 17 (12-24) 20 (10-30) 21 (16-26)
Oxidation of terpenes, MBO 11 (7-15) 9 (3-15) 7 (3-11)
SINKS (Tg yr-1) 56 (37-80) 78 95
Photolysis 36 (24-51) 44 46
Oxidation by OH 13 (9-19) 25 27
Deposition to land 7 (4-10) 9 9
Uptake by ocean 0 0 14
LIFETIME 16 days 20 days 15 days
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OCEANIC SIGNATURE OCEANIC SIGNATURE IN ATMOSPHERIC ACETONE OBSERVATIONSIN ATMOSPHERIC ACETONE OBSERVATIONS
Low winter values over Europe imply ocean sink
southern Norway[Solberg et al., 1996]
High values over South Pacific imply large ocean source
South Pacific[Singh et al., 2001]
a priori sources/sinks; 2 = 1.3 a posteriori sources/sinks(including “microbial” ocean sink,photochemical ocean source); 2 = 0.39
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SURFACE AIR ACETONE CONCENTRATIONSSURFACE AIR ACETONE CONCENTRATIONSIN IN A POSTERIORIA POSTERIORI SIMULATION SIMULATION
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METHYL IODIDE: TRACER OF MARINE CONVECTION IN METHYL IODIDE: TRACER OF MARINE CONVECTION IN GLOBAL ATMOSPHERIC MODELSGLOBAL ATMOSPHERIC MODELS
Loss by photolysis (~4 days), relatively uniform ocean Loss by photolysis (~4 days), relatively uniform ocean source, large aircraft data base [D.R. Blake, UCI]source, large aircraft data base [D.R. Blake, UCI]
Simple modelfor ocean source
Observations
Model(GEOS-CHEM)
Define Marine Convection Index (MCI) as ratio of upper tropospheric (8-12 km)to lower tropospheric (0-2.5 km) CH3I concentrations
• MCI over Pacific ranges from 0.11 (Easter Island dry season) to 0.40 (observations over tropical Pacific • GEOS-CHEM reproduces observed MCI with little global bias (+11%) but poor correlation (r2 = 0.15, n=11)
Bell et al. [2002]
MCI: 0.40 (obs) 0.22 (mod)
MCI: 0.16 (obs) 0.14 (mod)
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SURFACE OZONE BACKGROUND IN THE U.S. SURFACE OZONE BACKGROUND IN THE U.S. IMPORTED FROM OUTSIDE IS A SIZABLE INCREMENT IMPORTED FROM OUTSIDE IS A SIZABLE INCREMENT
TOWARDS VIOLATION OF U.S. AIR QUALITY STANDARDSTOWARDS VIOLATION OF U.S. AIR QUALITY STANDARDS(even more so in Europe!)(even more so in Europe!)
0 20 40 60 80 100 120 ppbv
Europe(seasonal)
U.S.(8-h avg.)
U.S.(1-h avg.)
preindustrial presentbackground
Europe (8-h avg.)
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OZONE BACKGROUND OVER U.S. IS GENERALLY DEPLETED OZONE BACKGROUND OVER U.S. IS GENERALLY DEPLETED DURING REGIONAL POLLUTION EPISODESDURING REGIONAL POLLUTION EPISODES
due to deposition and chemical loss under stagnant conditionsdue to deposition and chemical loss under stagnant conditions
Background(clean conditions)
O3 vs. (NOy-NOx) At Harvard Forest,
Massachusetts
Background(pollution episodes)
Observed (J.W. Munger)model (GEOS-CHEM)model background
Pollution coordinateFiore et al. [2002]
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RANGE OF ASIAN/EUROPEAN POLLUTION RANGE OF ASIAN/EUROPEAN POLLUTION SURFACE OZONE ENHANCEMENTS OVER THE U.S. IN SUMMERSURFACE OZONE ENHANCEMENTS OVER THE U.S. IN SUMMER
asas determined from a simulation with these emissions shut offdetermined from a simulation with these emissions shut off
Max Asian/European pollution enhancements(up to 14 ppbv) occur at intermediate ozone levels (50-70 ppbv)
MAJOR CONCERNIF U.S. OZONE STANDARDWERE TO DECREASE!
Fiore et al. [2002]
tropical air
Subsidence of Asian pollution+ local production
stagnation
U.S. standardEuropean standards
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NORTH AMERICAN OZONE OUTFLOW IN SURFACE AIR NORTH AMERICAN OZONE OUTFLOW IN SURFACE AIR (GEOS-CHEM model results for 1997)(GEOS-CHEM model results for 1997)
Li et al. [2002]
APRIL
JULY
LL
HH
HH
LL
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OZONE DATA AT MACE HEAD, IRELANDOZONE DATA AT MACE HEAD, IRELAND
Observed[Simmonds]
GEOS-CHEMmodel
N.America pollutionevents in model
Time series, Mar-Aug 1997
Model vs. observedstats, 1993-1997
Li et al. [2002]
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FORECASTING TRANSATLANTIC TRANSPORT OF FORECASTING TRANSATLANTIC TRANSPORT OF NORTH AMERICAN POLLUTION TO EUROPE WITH THENORTH AMERICAN POLLUTION TO EUROPE WITH THE
NORTH ATLANTIC OSCILLATION (NAO) INDEXNORTH ATLANTIC OSCILLATION (NAO) INDEX
NAO IndexNorth American ozone pollution enhancementAt Mace Head, Ireland (GEOS-CHEM model)
r = 0.57
NAO index = normalized surface P anomaly between Iceland and Azores
Li et al.[2002]
Greenhouse warming NAO index shift change in transatlantic transport of pollution
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EFFECT OF NORTH AMERICAN SOURCESEFFECT OF NORTH AMERICAN SOURCESON VIOLATIONS OF EUROPEAN AIR QUALITY ON VIOLATIONS OF EUROPEAN AIR QUALITY
STANDARD (55 ppbv, 8-h average)STANDARD (55 ppbv, 8-h average)GEOS-CHEM modelresults, summer 1997
Number of violation days(out of 92)
# of violation days thatwould not have beenin absence of N.American emissions
Li et al. [2002]
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Enhancements in Asian surface ozone due to European Enhancements in Asian surface ozone due to European anthropogenic emissions (GEOS-CHEM, 1996)anthropogenic emissions (GEOS-CHEM, 1996)
Liu et al.[2002]
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GLOBAL MODEL ANALYSIS OF OZONESONDE GLOBAL MODEL ANALYSIS OF OZONESONDE OBSERVATIONS ALONG THE PACIFIC RIM (1993-1997)OBSERVATIONS ALONG THE PACIFIC RIM (1993-1997)
observationsGEOS-CHEM model
High UT variability at Hong Kong in winter-spring reflects alternance of tropical and stratospheric influences
Liu et al. [2002]
Spring enhancementfrom SE Asian biomass burning
Hong Kong, 1996
300-120 hPa
700-300 hPa
850-700 hPa
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ALTERNANCE OF TROPICAL AND STRATOSPHERIC ALTERNANCE OF TROPICAL AND STRATOSPHERIC INFLUENCES IN WINTER UT OVER HONG KONG:INFLUENCES IN WINTER UT OVER HONG KONG:
comparison of Dec 24, 1996 and Jan 6, 1997comparison of Dec 24, 1996 and Jan 6, 1997
ObservedGEOS-CHEM
Sonde and model profiles
Model ozone concentrations and fluxes, 200 hPa
Stratospheric ozone tracer at longitude of Hong Kong
Liu et al. [2002]
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200 hPa ozone fluxes across Pacific Rim (GEOS-CHEM, 1996) 200 hPa ozone fluxes across Pacific Rim (GEOS-CHEM, 1996) • Tropical and midlatitude influences• Easterly circulation away from Pacific in summer
Liu et al.[2002]
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SUMMER UT OZONE POLLUTION EVENT OVER HONG KONGSUMMER UT OZONE POLLUTION EVENT OVER HONG KONGAugust 21, 1996August 21, 1996
ObservedGEOS-CHEM
Asianpollution
Sonde and model profiles
Model enhancement of ozone concentrationsand fluxes due to Asian anthropogenic sources
Liu et al. [2002]
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WHAT OBSERVATIONS AND MODELS ARE NEEDEDWHAT OBSERVATIONS AND MODELS ARE NEEDEDTO BETTER QUANTIFY INTERCONTINENTAL TRANSPORT?TO BETTER QUANTIFY INTERCONTINENTAL TRANSPORT?
3-D CHEMICAL TRACER MODELS
INTERCONTINENTAL TRANSPORT:INTERCONTINENTAL TRANSPORT:CONCENTRATIONS AND FLUXESCONCENTRATIONS AND FLUXES
SATELLITE OBSERVATIONSGlobal and continuous but few species, low resolution
AIRCRAFT OBSERVATIONSHigh resolution, targeted flights
provide critical snapshots for model testing
SURFACE OBSERVATIONShigh resolution but spatially limited
Source/sinkinventories
Assimilated meteorological
data
Chemical and aerosolprocesses
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TRACE-P MISSIONTRACE-P MISSION(Mar-Apr 2001)(Mar-Apr 2001)
Emissions-Fossil fuel-Biomass burning-Biosphere, dust
Long-range transport fromEurope, N. America, Africa
ASIA PACIFIC
P-3
Satellite datain near-real time:MOPITTTOMSSEAWIFSAVHRRLIS
DC-8
3D chemical model forecasts: - ECHAM - GEOS-CHEM - Iowa/Kyushu - Meso-NH -LaRC/U. Wisconsin
FLIGHTPLANNING
Boundary layerchemical/aerosolprocessing
ASIANOUTFLOW
Stratosphericintrusions
PACIFIC
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GOME daily data of NOGOME daily data of NO22 and HCHO and HCHO
tropospheric columns during TRACE-P (3/15 - )tropospheric columns during TRACE-P (3/15 - )
Randall Martin
Mean slant NO2 column, 3/16-4/15 Slant HCHO column, singleorbit on 3/27
Thomas Kurosu/Kelly Chance
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CARBON MONOXIDE CONCENTRATIONSCARBON MONOXIDE CONCENTRATIONSMEASURED IN TRACE-PMEASURED IN TRACE-P
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40
30
20
10
160150140130120110100
14
12
10
8
6
4
2
Perchlorethylene (pptv)
>15
HONG KONG
TOKYO
<1
Distribution of Perchlorethylene (C2Cl4) Measured During TRACE P
Don Blake, UCI
Symbol size 1/altitude
CC22ClCl44 CONCENTRATIONS MEASURED IN TRACE-P CONCENTRATIONS MEASURED IN TRACE-P
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INVERSE ANALYSIS OF CO SET UP FOR TRACE-PINVERSE ANALYSIS OF CO SET UP FOR TRACE-Pa priori a priori Asian emissions appear low but not outrageously soAsian emissions appear low but not outrageously so
Paul Palmer,Harvard
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PRELIMINARY GLOBAL (GEOS-CHEM) 3-D MODEL PRELIMINARY GLOBAL (GEOS-CHEM) 3-D MODEL ANALYSIS OF TRACE-P OBSERVATIONS ANALYSIS OF TRACE-P OBSERVATIONS
Mat Evans,Harvard
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GLOBAL MODEL ANALYSIS OF TRACE-P OBSERVATIONS: GLOBAL MODEL ANALYSIS OF TRACE-P OBSERVATIONS: SENSITIVITY TO SOURCESSENSITIVITY TO SOURCES
Mat Evans, Harvard
Median model/observed Median model/observed
OZONE CO
Median model/observed
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• To quantify the North American import and export of
(1) atmospheric oxidants and their precursors, (2) aerosols and their
precursors, (3) long-lived greenhouse gases
• To relate this import/export to surface sources/sinks and to
continental boundary layer chemistry
INTERCONTINENTAL TRANSPORT EXPERIMENT – INTERCONTINENTAL TRANSPORT EXPERIMENT – NORTH AMERICA (INTEX-NA)NORTH AMERICA (INTEX-NA)
OBJECTIVES:
TWO PHASES:• Summer 2004:
- active photochemistry, biosphere- aerosol radiative forcing- carbon uptake
• Spring 2006:- maximum Asian inflow- contrast with summer
TWO AIRCRAFT: NASA DC-8 and P-3
The next NASA Global Tropospheric Experiment (GTE) mission
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DR
RL BG
BR
AZWL
DC-8
P-3B
HI
NO
Ozonesonde sites
INTEX NOMINAL FLIGHT TRACKS FOR PHASE A (SUMMER)INTEX NOMINAL FLIGHT TRACKS FOR PHASE A (SUMMER)
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INTEX-NA HAS LINKAGES WITH A NUMBER OF INTEX-NA HAS LINKAGES WITH A NUMBER OF ATMOSPHERIC PROGRAMSATMOSPHERIC PROGRAMS
• In situ– North American Carbon Program (2002-)
– NOAA Northeast U.S. Study (2004)
– European UT/LS program (-2005) - LET’S TALK!!!
– Asian APARE program (ongoing)
• Satellites– Terra [MOPITT] (1999-)
– Envisat [SCIAMACHY, MIPAS] (2002-)
– NMP/GIFTS (2004-)
– Aura [TES, OMI, HRDLS, TES] (2004-)
• Modeling– EPA OAQPS/ORD climate change/air quality initiative (2001-2010)