RAQMS global chemical composition assimilation and regional ozone/aerosol forecasting during the 2004 NASA INTEX-NA field campaign

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Regional Air Quality Modeling System (RAQMS) Ozone Assimilation/Prediction February 27, 2001 RAQMS global chemical

Retrievals Global Assimilation R. Bradley Pierce 1, Jassim Al-Saadi 1, Chieko Kittaka 1, Todd K. Schaack 2,Donald R.

Lenzen 2, Matt Hitchman 3,Greg Tripoli 3,Marcus Buker 3 Regional Prediction Insitu data provided by: M. Avery (LaRC), R.

Szykman (USEPA) 1 NASA Langley Research Center 2 University of Wisconsin, Space Science and Engineering Center, 3

1 Regional Air Quality Modeling System (RAQMS) Ozone Assimilation/Prediction February 27, 2001 RAQMS global chemical composition assimilation and regional ozone/aerosol forecasting during the 2004 NASA INTEX-NA field campaign Satellite Retrievals Global Assimilation R. Bradley Pierce 1, Jassim Al-Saadi 1, Chieko Kittaka 1, Todd K. Schaack 2,Donald R. Johnson 2, Tom H. Zapotocny 2,Allen J. Lenzen 2, Matt Hitchman 3,Greg Tripoli 3,Marcus Buker 3 Regional Prediction Insitu data provided by: M. Avery (LaRC), R. Cohen (UC Berkley) Satellite data provided by: R. McPeters (GSFC) EPA Surface data provided by: J. Szykman (USEPA) 1 NASA Langley Research Center 2 University of Wisconsin, Space Science and Engineering Center, 3 University of Wisconsin, Atmospheric and Oceanic Sciences Validation RAQMS [Pierce et al., 2003] is a nested globalto regional-scale meteorological and chemical modeling system for assimilating and predicting the chemical state of the atmosphere (air quality).

RAQMS G Chemical Assimilation Chem/Met Forecast Cycle EPTOMS O3 Column 24hr chemical assimilation 72hr Chem/Met Forecast 12Z 18Z 00Z 06Z 12Z GFS Analyses May 11- Aug 31, 2004 ICARTT Focus areas:

(INTEX-NA) mission EU Intercontinental Transport of Ozone and Precursors (ITOP) North Atlantic Study RAQMS provided daily on-line global meteorological and chemical forecasts, initialized with

2 RAQMS G Chemical Assimilation Chem/Met Forecast Cycle EPTOMS O3 Column 24hr chemical assimilation 72hr Chem/Met Forecast 12Z 18Z 00Z 06Z 12Z GFS Analyses May 11- Aug 31, 2004 ICARTT Focus areas: regional air quality, intercontinental transport, and radiation balance NOAA New England Air Quality Study (NEAQS) mission NASA Intercontinental Chemical Transport Experiment- North America (INTEX-NA) mission EU Intercontinental Transport of Ozone and Precursors (ITOP) North Atlantic Study RAQMS provided daily on-line global meteorological and chemical forecasts, initialized with assimilated ozone distributions, to the NASA INTEX-NA science team for mission flight planning. 2 o x2.5 o Global component of the LaRC/UW-Madison Regional Air Quality Modeling System (RAQMS) uses the UW- Hybrid dynamical core, LaRC unified strat/trop chemistry, and Statistical Digital Filtering (SFD) for real-time TOMS Ozone assimilation and chemical/dynamical predictions. [36 levels (12 eta, 24 theta, ~3km stratospheric resolution]

3 Verification of RAQMS Upper Air O3 Analysis: INTEX RAQMS/DC8 Insitu O3 (M. Avery, LaRC) July 2004 RAQMS TOC and DC8 Flight Tracks July 2004 distribution of tropospheric ozone column (TOC) over the continental US was determined by local and remote (Alaskan Fires, Asian, European) emissions of O3 precusors (NOx, NMHC) and significant STE. RAQMS O3 analysis shows very good agreement with in-situ O3 except for overestimates associated with tropopause encounters

4 Verification of RAQMS Surface O3 Forecast: July 2004 RAQMS Analysis/48hr Forecast

5 Verification of RAQMS Upper Air NO2/PAN Analysis: INTEX RAQMS/DC8 Insitu NO2/PAN (R. Cohen, UC-Berkley) RAQMS NO2 analysis shows very good agreement with in-situ NO2 except for upper tropospheric underestimates associated with convectively influenced airmasses (BL lofting & lightning NOx) RAQMS PAN analysis shows fair agreement with in-situ PAN except near 800mb where it is underestimated by a factor of 4, possibly due to influences from Alaskan fires.

6 Moderate-Unhealthy O3 AQI over TX on July 20, spread to the SE US on July 21, and then NE by July 22, EPA AIRNow Ozone AQI: July 18- July 22, 2004

BL O3 July 18, 2004 RAQMS N Average Boundary

80Km Continental US EDAS Met BC/IC RAQMS G

7 BL O3 July 18, 2004 RAQMS N Average Boundary Layer Ozone: July 18-22, 2004 July 19, 2004 July 20, 2004 July 21, 2004 RAQMS N regional Chemical simulation: UWNMS Dynamical Core 80Km Continental US EDAS Met BC/IC RAQMS G Chem BC/IC Initialized on July 15, 2004 July 22, 2004

8 Verification of Surface RAQMS N O3 Forecast: July 22, 2004 RAQMS/AIRNOW EPA AIRNow Peak AQI-Ozone July 22, 2004

9 Moderate PM2.5 AQI on July 20, Unhealthy for sensitive groups in Great Lakes on 21 st then SE-NE by July 22, EPA AIRNow PM25 AQI: July 18- July 22, 2004

10 MODIS AOD July 18, 2004 MODIS Aerosol Optical Depth: July 18- July 22, 2004 MODIS AOD July 19, 2004 MODIS AOD July 20, 2004 Smoke from Alaskan Forest Fires MODIS Data Gap MODIS AOD July 21, 2004 MODIS AOD July 22, 2004 Link between Alaskan smoke and US AQ?

RAQMS N Average Boundary Layer Carbonaceous (BC+OC) Aerosol: July 18-July 22, 2004 Total Column Carbon Aerosol July 18, 2004 BL Column Carbon Aerosol July 19, 2004 RAQMS N regional Aerosol

11 RAQMS N Average Boundary Layer Carbonaceous (BC+OC) Aerosol: July 18-July 22, 2004 Total Column Carbon Aerosol July 18, 2004 BL Column Carbon Aerosol July 19, 2004 RAQMS N regional Aerosol simulation: Same Dynamics as chemical simulation GOCART Aerosol Module GOCART background climatological IC/BC MODIS BC+OC & SO4 perturbations added above BL at 18Z July 18, 2004 BL Column Carbon Aerosol July 20, 2004 BL Column Carbon Aerosol July 21, 2004 BL Column Carbon Aerosol July 22, 2004

12 Verification of Surface RAQMS N Aerosol Forecast: July 22, 2004 RAQMS/AIRNOW EPA AIRNow Peak AQI-Ozone July 22, 2004

High Resolution Dynamics Limb Sounder (HIRDLS) limb scans in the vertical at multiple azimuth angles, measures infrared emissions in 21 channels ranging

5THz Ability to see through upper tropospheric clouds NASA Earth Observing System (EOS) Aura Satellite Ozone Monitoring Instrument (OMI) hyperspectral (740

km Tropospheric Emission Spectrometer (TES) high-resolution infrared-imaging Fourier transform spectrometer capability to make both limb and nadir

13 High Resolution Dynamics Limb Sounder (HIRDLS) limb scans in the vertical at multiple azimuth angles, measures infrared emissions in 21 channels ranging from 6.12 mm to mm. Microwave Limb Sounder (MLS) 5 microwave channels (118, 190, 240, 640 GHz, and 2.5THz Ability to see through upper tropospheric clouds NASA Earth Observing System (EOS) Aura Satellite Ozone Monitoring Instrument (OMI) hyperspectral (740 wavelength bands)imaging solar backscatter (visible and ultraviolet) radiometer Large swath large provides global coverage in 14 orbits (1 day) at 13 x 24 km Tropospheric Emission Spectrometer (TES) high-resolution infrared-imaging Fourier transform spectrometer capability to make both limb and nadir observations. Each of the Auras instrument team's Algorithm Theoretical Basis Documents (ATBD) are now available after having gone through peer review. They can be found at:

14 Conclusions: July 22 nd 2004 PM2.5 AQI over the SE and NE US was strongly influenced and O3 AQI was enhanced by entrainment of carbonaceous aerosols, O3, and O3 precusors from the Alaskan Fires.

15 Extra Figures

16 Verification of RAQMS Total Column O3 Analysis: July 2004 RAQMS/EPTOMS Partial TOMS coverage NH mid-latitude: zonal mean errors are +/- 2DU RMS errors are ~3% anomoly correlations are >0.8 Tropics: zonal mean subtropical low bias of 5DU RMS errors are ~1-2% anomoly correlations are ~0.6

17 Verification of RAQMS 800mb O3 Forecast: July 2004 RAQMS Analysis/48hr Forecast

18 Verification of Surface RAQMS O3 Analysis: July 2004 RAQMS/AIRNOW Good agreement (r>0.6, daytime biases <10ppbv) in SE, NE, Midwestern US associated with strong synoptic forcing of regional pollution events. Largest errors in Ohio River valley which shows high (>20ppbv) daytime biases due to neglect of clouds in photolysis rate calculations and low (<0.0) correlations due to weak synoptic forcing of local emissions

19 RAQMS Surface O3 Timeseries: July 2004 RAQMS/AIRNOW Best Case: relatively cloud free strong synoptic forcing Worst Case: Frequent cloudiness Low synoptic variability Regional emission source

NASA Air Quality Applications* Goal: Improved capability to Air Quality managers to assess, plan & implement sound-science, emissions control strategies, policy, & air quality forecasts.

20 NASA Air Quality Applications* Goal: Improved capability to Air Quality managers to assess, plan & implement sound-science, emissions control strategies, policy, & air quality forecasts. The primary partners for the Air Quality Management program are the US Environmental Protection Agency (EPA) and the National Oceanic and Atmospheric Administration (NOAA). *From NASA Earth Science Enterprise Applications Plan

RAQMS NMHC Treatment Explicit treatment of C 2 H 6 (ethane), C 2 H 4 (ethene) and CH 3 OH (methanol) oxidation [Sander et al., 2003].

C 4 and larger alkanes and C 3 and larger alkenes are lumped via a carbon-bond approach [Zaveri and Peters, 1999] which accounts for long-lived species and their

July, Med O3, High NOx 10-day diurnal equilibrium runs with/without NMHC conducted as part of the NASA Global Modeling Initiative (GMI) unified chemistry

21 RAQMS NMHC Treatment Explicit treatment of C 2 H 6 (ethane), C 2 H 4 (ethene) and CH 3 OH (methanol) oxidation [Sander et al., 2003]. C 3 H 8 (propane) is handled semi-explicitly. C 4 and larger alkanes and C 3 and larger alkenes are lumped via a carbon-bond approach [Zaveri and Peters, 1999] which accounts for long-lived species and their intermediates based on the Carbon Bond Mechanism IV [Gery et al., 1989]. Isoprene is modeled after the Carter 4-product mechanism as modified for RADM2. July, Med O3, High NOx 10-day diurnal equilibrium runs with/without NMHC conducted as part of the NASA Global Modeling Initiative (GMI) unified chemistry development. GMI Harvard mechanism [Bey et al., 2001] with Gear solver for 80 species (all transported in GMI) LaRC Run Versions Standard Revised 1: Remove NO3 + peroxy radical rxns Revised 2: Revised Peroxide oxidation branching matched to GMI Organic nitrate production matched to GMI RO2 + NO branching matched to GMI

22 RAQMS unified (strat/trop) chemistry (55 species/families explicitly transported, 86 calculated, PCE assumptions for fast species) 1) Ox 2) Noy 3) Cly 4) Bry 5) HNO3 6) N2O5 7) H2O2 8) HCl 9) ClONO2 10) OClO 11) N2O 12) CFCl3 (F11) 13) CF2Cl2 (F12) 14) CCl4 15) CH3Cl 16) CH3CCl3 (MTCFM) 17) CH3Br 18) CF3Br (H1301) 19) CF2ClBr (H1211) 20) HF 21) CFClO 22) CF2O 23) CH4 24) HNO4 25) HOCl 26) H2O 27) NO3 28) NO2 29) CH2O 30) CH3OOH 31) CO 32) HBr 33) BrONO2 34) HOBr 35) BrCl 36) Cl2 Stratosphere+CH4&CO oxidation 37) C2H6 (ethane, 2C) 38) ALD2 (acetaldehyde+higher group, 2C) 39) ETHOOH (ethyl hydrogen peroxide, 2C) 40) PAN (2C) 41) PAR (paraffin carbon bond group, 1C) 42) ONIT (organic nitrate group, 1C) 43) AONE (acetone, 3C) 44) ROOH (C3+hydrogen peroxides group, 1C) 45) MGLY (methylglyoxal, 3C) 46) ETH (ethene, 2C) 47) XOLET (terminal olefin carbon group, 2C) 48) XOLEI (internal olefin carbon group, 2C) 49) XISOP (isoprene, 5C) 50) XISOPRD (isoprene oxidation product-long lived, 5C) 51) PROP_PAR (propane paraffin, 1C) 52) CH3OH (methanol) 53) XMVK (methyl vinyl ketone, 4C) 54) XMACR (methacrolein, 4C) 55) XMPAN (peroxymethacryloyl nitrate, 4C) NMHC Chemistry Chemical families Ox=O(1D)+O(3P)+O3+NO2+HNO3+2(NO3)+3(N2O5)+HNO4+PAN+MPAN NOy=N+NO+NO2+NO3+2(N2O5)+HNO3+HNO4+BrNO3+ClNO3+PAN+ONIT+MPAN Cly=HCl+ClONO2+ClO+2(Cl2O2)+OClO+ClO2+2(Cl2)+BrCl+HOCl+Cl Bry=HBr+BrONO2+BrO+BrCl+HOBr+Br

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