Modeling of Organic Aerosol during the MEGAPOLI Summer Campaign in the Paris Region CHIMERE - Volatility Basis Set approach CHIMERE - Volatility Basis Set approach Q.J.Zhang (1)*, M.Beekmann (1), L. Poulain (2), A. Held (2), A. Wiedensohler (2) , K. Kamilli (2), H. Herrmann (2), P. de Carlo (3), M. Crippa (3), R. Chirico (3), M. Heringa (3), Claudia Mohr (3), A. Prevot (3), U. Baltensperger (3), E. Freney (4), A. Schwarzenboeck (4), K. Sellegri (4), J.M. Pichon (4), L. Gomes (5), B. Bessagnet (6), S. Pandis (7), A. Hodzic(8) zhang@lisa.univ-paris12.fr (1) Laboratoire Interuniversitaire des Systèmes Atmosphériques (LISA), Université Paris Est et 7, CNRS, Créteil, France Créteil, France (2) Institute for Troposphärenforschung, Leipzig, Germany, (3) Paul Scherrer Institut, Villingen, Switzerland, (4) Laboratoire de Météorologie Physique, Clermont-Ferrand, France (5) Centre National de Recherche Météorologique, Toulouse, France (6) Institut National de l'EnviRonnement industriel et des rISques, Verneuil en Halatte, France (7) Foundation for Research and Technology, Hellas, University of Patras, Greece (8) National Center for Atmospheric Research, USA. * Also Aria technologies 1 Harmo13, Paris 2010/06/03
Context & Objective • SOA (Secondary Organic Aerosol): under-estimated in Chemistry Transport Models Comparison Model / Measurement, 05/2007-06/2007 LHVP , (urban MEGAPOLI site) LHVP , (urban MEGAPOLI site) Observed SOA (J. Sciare, LSCE) Simulated SOA (classic) Simulated anthropogenic SOA (classic) Volkamer et al., GRL, 2006 MEGAPOLI Paris Campaign : Quantify primary and secondary sources of organic aerosols, in urban and in plume Objective: Improve Volatility Basis Set approach ( VBS) ) simulation of SOA in Lane et al. 2008 Robinson et al., 2007 CHIMERE (regional CTM) Compare with MEGAPOLI measurements 2
MEGAPOLI Campaign - Measurements Forest ATR - 42 ����� ����� ������� ����� ����� � PARIS Matthias.BEEKMANN ����!�� ���� ������� ����� (Tuesday 14h, 20km Harmo13) Forest ������ � ���� ����� => suite of in situ measurements / + meteo at SIRTA. 3 primary sites 3 secondary sites 3 secondary sites => lidar and spectroscopic measurements / or in situ => lidar and spectroscopic measurements / or in situ 3 mobile labs => full in situ measurements (PSI + MPI) + Univ Duisburg 1 mobile lab => lidar measurements (CEA) 1 mobile lab => MAXDOAS (MPI) 1 aircraft ATR-42 => full in situ measurements (SAFIRE, CNRS, MPI)
SOA scheme in CHIMERE Classic scheme based on “two-product” approach of Odum et al. 1996 • α∑ SVOC (Surrogated Semi-volatile OH, VOC precursors O3, VOC species with distinct volatilities) NO3 (Pun et Seigneur,2006, Bessagnet et al. 2008) Phase Phase Aerosol transfer VBS « Volatility Basis-Set » approach • OH n ∑ SVOC with defined volatility bins VOC precursors (Robinson et al., 2007, Lane et al. 2008, Murphy and Pandis. 2009) 4
VBS approach main features Classic POA partitioning of POA (SVOC) emissions additional IVOC emission emissions 1 1 0.8 0.9 0.8 0.7 Chemical aging 0.030.060.090.140.18 0.3 0.4 0.5 0.4 0.5 Normalized Normalized 0.6 0.6 +OH +OH 0.5 emission 0.4 Robinson et factor with 0.3 respect to al., 2007, 0.2 classic POA 0.1 Murphy et 0 emission Pandis. 2009 C* (µg m-3) at 298K Saturation concentration ∆ Hv (kJ mol-1) ∆ Hv (kJ mol-1) 150 112 106 106 94 88 82 76 70 64 Semivolatile-SOA (S-SOA) 5
Model configuration Gocart/LMDz Meteorology GFS/MM5 domain Resolution CONT 0.5 °× 0.5 ° CHIMERE CHIMERE GN9 9km × 9km Gas phase mechanism, MELCHIOR2 50 species,120 reactions CONT3 CONT3 Inorganic mechanism ISORROPIA (Nenes et al., 1998) GN9 GN9 Paris Paris Two-product method / SOA Scheme VBS approach EMEP MEGAN Emissions Anthropo Biogenic genic 6
Model simulations Simulations with classic scheme (POA non-volatile) � Simulations with VBS � Total SOA=Oxygenated OA Biogenic SOA (BSOA) Semivolatile-SOA Anthropogenic SOA VBS VBS Classic Lumped VOC Isoprene, Terpene, α - Partitioning of POA (Aromatics, Higher pinene, β -pinene, emissions (SVOC) + Alkanes, etc.) Limonene, Ocimene, additional IVOC according to SAPRC Humunene 4 volatility bins Chemical aging Chemical aging (Lane et al. 2008) (Pun and Seigneur, 2006; (Robinson et al., 2007, Murphy Bessagnet al. 2008) and Pandis. 2009) 7
AMS measurements Aerodyne aerosol Mass spectrometer (AMS) � � Organic Aerosol (OA=POA+SOA) � � LHVP: by IFT (urban site) Paris Preliminary simplified PMF (Positive Matrix) Factorization (Poor man’s PMF) Factorization (Poor man’s PMF) � Hydrocarbon-like Organic Aerosol (HOA) � Biomass Burning Organic Aerosol (BBOA) HOA+BBOA � Primary Organic Aerosol (POA) � Oxygenated Organic Aerosol (OOA) OOA � SOA(S-SOA+ASOA+BSOA) OA –LaMP (µg/m 3 ) SIRTA: upwind of Paris agglomeration, by PSI (suburban site) Flight: by LaMP 8
9 Paris 7-22 7-22 7/22 OOA Model -VBS 7-22 7-22 7-22 HOA Model-VBS 7-21 7/21 7-21 7-21 7-21 7-21 7-20 7/20 7-20 7-20 7-20 7-20 7/19 7-19 7-19 7-19 7-19 7-19 In VBS, POA � SVOC+IVOC => reduce POA levels 7-18 7-18 7/18 7-18 7-18 7-18 7/17 7-17 7-17 7-17 7-17 7-17 7-16 7/16 7-16 7-16 7-16 7-16 POA Model-Classic SOA Model -Classic 7/15 7-15 7-15 7-15 7-15 7-15 Simulation results (LHVP-Urban site) 7-14 7/14 7-14 7-14 7-14 7-14 7/13 7-13 7-13 7-13 7-13 7-13 vs. ground based AMS measurements 7/12 7-12 7-12 7-12 7-12 7-12 7/11 7-11 7-11 7-11 7-11 7-11 7/10 7-10 7-10 7-10 7-10 7-10 HOA/BBOA AMS Poor man’s PMF 7-9 7-9 7/9 7-9 7-9 7-9 7/8 7-8 7-8 7-8 7-8 7-8 OOA AMS Poor man’s PMF 7-7 7/7 7-7 7-7 7-7 7-7 7/6 7-6 7-6 7-6 7-6 7-6 Local 7-5 7/5 7-5 7-5 7-5 7-5 7/4 7-4 7-4 7-4 7-4 7-4 Continental 7/3 7-3 7-3 7-3 7-3 7-3 µg/m 3 µg/m 3 7/2 7-2 7-2 7-2 7-2 7-2 TIME TIME TIME TIME TIME TIME 25 25 25 20 20 20 15 15 15 10 10 10 5 5 5 0 0 0 -5 12 12 12 9 9 9 6 6 6 3 3 3 0 0 0
10 POA_VBS OPOA_VBS ASOA_VBS S-SOA_VBS July 22 J u ly 2 2 OA_Classic BSOA BSOA OA_VBS July 21 J u ly 2 1 OA-AMS July 20 J u ly 2 0 July 19 J u ly 1 9 July 18 J u ly 1 8 POA+BSOA July 17 J u ly 1 7 J u ly 1 6 July 16 VBS � close at peaks, underestimate Classic � over-estimate peaks, close July 15 J u ly 1 5 July 14 J u ly 1 4 July 13 J u ly 1 3 at background concentration OA =HOA+OOA (LHVP-Urban site) background concentration J u ly 1 2 July 12 J u ly 1 1 July 11 J u ly 1 0 July 10 J u ly 0 9 July 09 J u ly 0 8 July 08 J u ly 0 7 July 07 J u ly 0 6 July 06 S-SOA+BSOA J u ly 0 5 July 05 J u ly 0 4 July 04 Continental J u ly 0 3 July 03 µg/m 3 µg/m 3 J u ly 0 2 July 02 J u ly 0 1 July 01 30 25 20 15 10 10 5 0 12 10 8 8 6 4 2 0
11 11 Paris July 22 S-SOA_VBS July 22 BS BS BS July 21 _V _V _V July 21 OPOA BSOA SOA POA July 20 July 20 A Upwind => background concentration is low July 19 OA Model -VBS July 19 July 18 July 18 July 17 July 17 July 16 Simulation results (SIRTA-Suburban site) July 16 July 15 July 15 July 14 July 14 Mostly BSOA July 13 vs. ground based AMS measurements July 13 OA Model -Classic July 12 July 12 July 11 July 11 July 10 July 10 July 09 July 09 July 08 July 08 July 07 July 07 July 06 July 06 July 05 July 05 July 04 July 04 OA AMS Continental Downwind July 03 July 03 µg/m 3 µg/m 3 July 02 July 02 July 01 July 01 20 16 12 12 9 6 6 3 0 8 4 4 0
Diurnal Variation of OA (LHVP-Urban site) µg/m 3 14 OA_Classic_Diurnal_Variation OA_VBS_Diurnal_Variation OA_AMS_Diurnal_Variation 12 10 10 8 6 4 2 0 0 1 2 3 4 5 6 7 8 9 10 11 12 13 14 15 16 17 18 19 20 21 22 23 24 Daytime (Hr ) Classic scheme: Wrong morning peak due to primary emissions (non-volatile) With VBS scheme: Peak in the morning corrected <=> distribution of POA into S/IVOC But OOA lacks in the evening 12
High yield case (LHVP-Urban site) Paris - POA-SVOC/IVOC emissions *2 - Anthropogenic SOA yield *2 OA-AMS-Poor man's PMF OA_VBS OA_VBS_HY 25,00 20,00 15,00 10,00 5,00 0,00 TIME 7/2 7/3 7/4 7/5 7/6 7/7 7/8 7/9 7/10 7/11 7/12 7/13 7/14 7/15 7/16 7/17 7/18 7/19 7/20 7/21 7/22 7/23 Background concentration underestimated Peak overestimated 13
Regional influence on OOA plume Anthropogenic Biogenic Local 14 14
Local formation of OA vs. measurements on flight Flight 32 Measurement 20090721 µg/m3 100KM 14 14 14 14 y = 0,1631x - 2,4517 y = 0,1631x - 2,4517 µg/m 3 µg/m 3 12 12 10 10 Measurement 8 8 6 6 OA Model VBS 4 4 y = 0,0695x - 3,2018 µg/m3 Model-VBS Background 2 2 concentration 0 0 0 0 ppb 0 0 10 10 20 20 30 30 40 40 50 50 60 60 70 70 80 80 90 90 Ox=O3+NO2 15 15
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