Organics in the global troposphere: Recent advances and future plans at ECPL
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1 Organics in the global troposphere: Recent advances and future plans at ECPL Environmental Chemical Processes Laboratory (ECPL) Department of Chemistry University of Crete, Heraklion, Greece Maria Kanakidou Stelios Myriokefalitakis PhD defense June 2009 Nikos Daskalakis AEROCOM OA exercise Kostas Tsigaridis NASA-GISS / lumping/simplifying SOA Maria Kanakidou ECPL Univ of Crete mariak@chemistry.uoc.gr
2 TM4-ECPL Model description Explicit chemical mechanism (Glyoxal studies Myriokefalitakis et al., ACP 2008) (59 gases + about 20 aerosol species +? Radicals) Marine Aerosol OA (Vignati et al AE 2009) + SOA (Myriokefalitakis et al...) Isorropia II equilibrium model for inorganic aerosols Aqueous phase chemistry of glycolaldehyde, glyoxal & methylglyoxal Ageing of SOA (by OH as Tsigaridis& Kanakidou ACP 2003, K OH =1E-12) Ageing of OA (by O3 as Tsigaridis& Kanakidou, ACP 2003) Impact of heterogeneous chemistry Myriokefalitakis, PhD Thesis, June 2009
3 Studied heterogeneous reactions N 2 O 5 γ i =0.04 γ o = HNO 3 HO 2 H 2 O NO 3 γ i =0.2 γ o = H 2 O H 2 O SO 4=, NO 3-, MS -, NH + 4+, H 2 O H 2 O γ i = γ o =0.005 OC, BC H 2 O H 2 O H 2 O 2 H 2 O HNO 3 γ:on humid surfaces of inorganic (γ i ) and organic/black carbon (γ o ) NO 2 γ i =5x10-7 γ o =2x HNO HNO 2 Myriokefalitakis, PhD Thesis, June 2009
4 Impact of heterogeneous reactions Ο 3 και SO = 4 % Impact of heterogeneous reactions on Ο 3-10% Myriokefalitakis, PhD The esis, June 2009 % Impact of heterogeneous reactions on SO 4 = -10% SO 2 + O 3 SO 4 =
5 Impact of heterogeneous reactions on ΝΟ 3- andνη + 4 % Impact of heterogeneous reactions on ΝO % Myriokefalitakis, PhD The esis, June 2009 Ν 2 O 5 ΗΝΟ 3 ΝΟ 3 - % Impact of heterogeneous reactions onνη 4 + SΟ 4 = ΝΗ 3 +10% ΗΝΟ 3 + ΝΗ 3 ΝΗ 4 +
6 Impact of heterogeneous reactions on ΟΑ % Impact of heterogeneous reactions on ΟΑ esis, June 2009 Myriokefalitakis, PhD The +3%
7 Impact of studied heterogeneous reactions on- ΟΑ % Impact of heterogeneous reactions on ΟΑ +3% Seinfeld and Pankow, 2003
8 Impact of heterogeneous reactions atmospheric loading without with Myriokefalitakis, PhD The esis, June 2009 TM4 Global Burden (Tg) % -4.6% 12% 0.6% 0.9% 0.0 Ο 3 *10-2 SO 4 = NO 3 - NH 4 + SOA
9 Impact of heterogeneous reactions Myriokefalitakis, PhD Th hesis, June 2009 Προσομοίωση Προσομοίωσης χωρίς με ετερογενείς ετερογενείς %Συνεισφορά Ένωση αντιδράσεις αντιδράσεις ετερογενών Ατμοσφαιρικό αντιδράσεων Ατμοσφαιρικό Φορτίο (Τg) Φορτίο (Τg) Τροποσφαιρικό Ο 3 SO = NO ΝΗ SOA
10 Cloud chemistry
11 Glyoxal& methylglyoxal chemistry in clouds SOA based on Ervenset al., 2007 and Carlton et al., 2007 adopted in TM4-ECPL global model Myriokefalitakis, PhD thesis 2009 Lim et al., Tg/y from isoprene Fu et al., TgC/y from glyoxal from methylglyoxal, 90% clouds Cloud LWC Pressure (hpa a) Aqueous-phase glyoxal oxidation pathways. Glyoxal, glyoxylic acid and glyoxylate are predominantly hydrated in Solution Carlton et al., AE, 2007
12 Aqueous phase impact - oxalate in TM4-ECPL ng(oxl)/m³ ng(oxl)/m³ Ιαν Schauinsland (47.55N, 7.54E) ΤΜ4 obs Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Φεβ Μαρ Απρ ΤΜ4 obs Μαϊ Ιουν Ιουλ Αυγ Αυγ Finokalia (35.3N, 25.7E) Σεπ Οκτ Νοε εκ ng(oxl)/m³ ng(oxl)/m³ ΤΜ4 obs Pay de Dome (45.46N, 2.57E) Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Ιαν Φεβ Μαρ Απρ ΤΜ4 obs Μαϊ Ιουν Ιουλ Αυγ Αυγ Amsterdam Island (37.5S, 77.3E) Σεπ Οκτ Νοε εκ Myriokefalitakis, PhD Thesis s, June Ιαν Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Φεβ Μαρ Απρ Μαϊ Ιουν Ιουλ Αυγ Αυγ Σεπ Οκτ Νοε εκ 0 Jan Feb Mar Apr May Jun Jul Aug Sep Oct Nov Dec Ιαν Φεβ Μαρ Απρ Μαϊ Ιουν Ιουλ Αυγ Αυγ Σεπ Οκτ Νοε εκ
13 Updated global view of OA TM4-ECPL model JJA SOA/OA DJF Myriokefalitakis, PhD Th hesis, June 2009 Maria Kanakidou Goldschmidt Conference Davos 25 June 2009
14 Myriokefalitakis, PhD The esis, June 2009 Maria Kanakidou Goldschmidt Conference Davos 25 June 2009
15 TM4-ECPL 6x4 versus3x2
16 O3 6 x4 OH 3 x2 1E6 rad/cm3
17 CO 6 x4 isoprene 3 x2
18 BCsol 6 x4 POCsol 3 x2
19 TM4-ECPL vs Measurements
20 6 x4 Mean value of the stations in each grid box The biggest differences in urban areas 3 x2 Smaller grid box, most accurate measurement values Differences in urban areas are even more visible.
21 6 x4 3 x2 Good agreement of the measured values and the model results on most sites.
22 An AEROCOM intercomparison exercise in organic aerosol modeling Kostas Tsigaridis, Maria Kanakidou and a lot of contributors
23 Contributors CAM-Oslo Alf Kirkevåg GISS MATRIX* Susanne Bauer GISS modele* Kostas Tsigaridis, Dorothy Koch GLOMAP Graham Mann SPRINTARS Toshi Takemura GEOS-Chem Gabriele Curci TM3 Kostas Tsigaridis, Maria Kanakidou TM4* Nikos Daskalakis, Maria Kanakidou Measurements Lynn Russell, Jose-Luis Jimenez, Ranjit Bahadur, Qi Zhang * Preliminary results includes aerosol microphysics
24 100% 90% 80% 70% 60% 50% 40% 30% 20% 10% 0% Modified from Textor et al., 2006 OA within AEROCOM Fraction of global aerosol composition H2O POM BC SO4 SS DUST 100% 90% 80% 70% 60% 50% 40% 30% 20% 10% 0% Fraction of global fine dry aerosol composition POM BC SO4 ARQM DLR GISS GOCART KYU LOA LSCE MATCH MOZGN MPI_HAM PNNL TM5_B UIO_CTM UIO_GCM ULAQ UMI ARQM DLR GISS GOCART KYU LOA LSCE MATCH MOZGN MPI_HAM PNNL TM5_B UIO_CTM UIO_GCM ULAQ UMI
25 Aerosol microphysics Detailed SOA Most detailed OA Model results annual mean CAM-Oslo GISS-MATRIX GISS-SOA GISS GEOS-Chem GLOMAP TM3 TM4-F TM4-C
26 All measurements, January CAM-Oslo GISS-MATRIX GISS-SOA GISS GEOS-Chem GLOMAP TM3 TM4-F TM4-C
27 All measurements, July CAM-Oslo GISS-MATRIX GISS-SOA GISS GEOS-Chem GLOMAP TM3 TM4-F TM4-C
28 TM4-C All measurements January
29 TM4-C All measurements July
30 TM4-F 2006 All IMPROVE Marine Urban July January
31 Comparison with station data (2006) Preliminary analysis
32 TM4-F GEOS-Chem GLOMAP IMPROVE Urban All measurements
33 Future work-aerocom Include more models Include more stations Compare with high altitude measurements Study budgets: sources, burden, removal, lifetime Study regions Compare with HOA/OOA/WSOC/WIOC Compare AOD
34 On going projects at ECPL Reduction of SOA scheme CIRCE -JRC emission database for CIRCE EDGAR CITYZEN Megacities / East Mediterranean Lateral boundaries from TM4-ECPL + WRF-CHEM GFEDv2 (?3) database for biomass burning 1 x1 simulations? TM5 (+size distribution) Coupling with MEGAN Publications
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