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A new parameterization of biogenic SOA formation based on smog chamber data: 3D testing in CMAQ

A new parameterization of biogenic SOA formation based on smog chamber data: 3D testing in CMAQ. Manuel Santiago 1 , Ariel F. Stein 2 , Marta G. Vivanco 1 , Yunsoo Choi 3 and Rick Saylor 4 1 CIEMAT (Research Center for Energy, Environment and Technology). Madrid. SPAIN

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A new parameterization of biogenic SOA formation based on smog chamber data: 3D testing in CMAQ

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  1. A new parameterization of biogenic SOA formation based on smog chamber data: 3D testing in CMAQ Manuel Santiago1,Ariel F. Stein2, Marta G. Vivanco1, Yunsoo Choi3 and Rick Saylor4 1 CIEMAT (Research Center for Energy, Environment and Technology). Madrid. SPAIN 2 ERT on assignment of NOAA/ARL, Silver Spring MD 3 NOAA/ARL, Silver Spring, MD 4 NOAA/ARL, Atmospheric Turbulence and Diffusion Division, Oak Ridge, TN 2011 CMAS Conference manuel.santiago@ciemat.es

  2. Motivation • Biogenic SOA, accounts for the largest fraction of the global atmospheric aerosol • EUPHORE smog chamber experiments: CMAQ paramaters that • govern SOA originated by terpenes clearly overestimate our • experimental data. • Here, a semi-empirical parameterization based on product • distribution given by BVOCs oxidation pathways is presented for • a-pinene + limonene SOA

  3. Terpene SOA in CMAQ v4.7 • Based on the partition parameters obtained by Griffin et al. 1999 Two Product Model for different BVOCs Griffin et al., 1999

  4. Terpene SOA in CMAQ v4.7 Compound wght alpha1 Kom1 alpha2 Kom2 ---------- ---- ------ ------ ------ ------ a-pinene 0.4 .038 .171 .326 .0040 b-pinene 0.25 .13 .044 .406 .0049 d3-carene 0.15 .054 .043 .517 .0042 sabinene 0.1 .067 .258 .399 .0038 limonene 0.1 .239 .055 .363 .0053 alpha1 cstar1 alpha2 cstar2 ------ ------ ------ ------ CMAQ TERPENE .1123 7.466 .5013 110.77 Why two-product model? • Straighforward implementation • Lack of known of the product distributions for all the identified SOA precursor pathways

  5. Semiempirical Parameterization Theoretical Kom,i calculation for individual SOA constituents a-pin + limo yield calculation Two product model fit (Based on theoretical constraints) Comparison with current CMAQ parameters

  6. Smog Chamber Experiments • Outdoor chamber EUPHORE (CEAM, Valencia, Spain) • Approximated volume of 200 m3 • Biogenic VOCs mixture photooxidation experiments: • (isoprene + a-pinene + limonene) + HONO

  7. Smog Chamber Experiments ppbCHAMBER : ppbRURAL ATM. = 102 – 103

  8. Individual Kom,i calculation The contribution method SIMPOL.1 (Pankow and Asher, 2008) was used for the calculation of individual poL,i and Kom,i 0.1 m3/mg < Kom,1 < 0.5 m3/mg 0.01 m3/mg < Kom,2 < 0.001 m3/mg

  9. a-pin + limo Yield Calculation Yisoprene = 0.02 a1= 0.1939 Kom,1 = 0.1106 m3.mg-1 a2= 0.2 Kom,2= 0.0056 m3.mg-1

  10. Model Description • CMAQ v4.7 simplified version: only gas phase chemistry and aerosol formation • Domain: 4 x 4 cell grid located in Valencia, Spain (LAT: 39, LON: 0) • Meteorology: Hourly T, P and QV values measured in the chamber • CCTM Conditions: • Gas/Aerosol mechanism: CB05-AERO5 • Solver: SMVGEAR • Temporal Resolution: 000100 (hhmmss)

  11. Parameterizations to test TRP_original : Current parameters in CMAQ v4.7 (scale up of ai to consider 1.3 g/cc density) TRP_revised: re-derived parameters for 1.3 g/cc density (Carlton et al.2010) TRP_fit: parameters obtained in this work (Santiago et al., 2011, submitted to ES&T)

  12. Model Description orgaer5.f data alpha / 0.0718, ! SV_ALK & 0.0386, 0.1119, ! SV_XYL1, SV_XYL2 & 0.0758, 0.1477, ! SV_TOL1, SV_TOL2 & 0.0942, 1.162, ! SV_BNZ1, SV_BNZ2 & 0.1123, 0.5013, ! SV_TRP1, SV_TRP2 & 0.232, 0.0288, ! SV_ISO1, SV_ISO2 & 1.3 / ! SV_SQT data cstar / 0.020, ! SV_ALK & 1.314, 34.483, ! SV_XYL1, SV_XYL2 & 2.326, 21.277, ! SV_TOL1, SV_TOL2 & 0.302, 111.11, ! SV_BNZ1, SV_BNZ2 & 7.466, 110.77, ! SV_TRP1, SV_TRP2 & 116.01, 0.617, ! SV_ISO1, SV_ISO2 & 12.193 / ! SV_SQT

  13. Chamber Experiments Simulations

  14. Normalized Mean Bias (%)

  15. CMAQ v4.7 3D Settings • Study Period: August 2009 • Emissions: based on NEI 2005 • Meteorology: NAM • Horizontal/Vertical Resolution: 12 km/22 layers • Boundary Conditions: GEOSCHEM monthly average • Chemical/Aerosol Mechanism: CB05-AE5

  16. TRP_original SOA Monthly Average

  17. Effect of different parameters TRP_original – TRP_revised TRP_original – TRP_fit -1 -1

  18. Summary SMOG CHAMBER EXPERIMENTS • A 2 product parameterization for SOA from a-pinene and limonene has been calculated with a mixed theoretical-experimental approach • Mechanistic considerations considered in TRP_fit represent an improvement of the treatment of SOA from a-pinene and limonene • Parameters re-derived by Carlton et al. 2010 (TRP_revised) reduce original parameters • bias by 50%. Still an overprediction is observed (NOx dependent SOA?) 3-D AUGUST 2009 SIMULATION • Differences in the chamber experiment simulations do not drive to substantial • changes on the model response on SOA monthly average concentration • TRP_revised and TRP_fit show a similar reduction of the original CMAQ values • (TRP_original). • Only a-pinene and limonene parameters have been calculated in this work. The • same procedure should be done for the rest of terpenes

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