Supplement of Inversion of and
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1 Supplement of Inversion of and emissions using the adjoint of the IMAGES model J.-F. Müller and T. Stavrakou Belgian Institute for Space Aeronomy, Brussels, Belgium
2 Abstract This supplement contains three tables. The chemical species included in the IMAGES model are presented in Table. The chemical reaction mechanism of the model is described in Table. References for the reaction rates are also given. In Table we present the photodissociations included in the model, as well as references for their cross sections, quantum yields, and products. Correspondence to: J.-F. Müller
3 ' Table. Chemical species included in the model. Chemical species included in the model Species Category Chemical Formula Name : 0.9 oxygen : 79.0 nitrogen Fixed (from ECMWF) water : 0 ppbv hydrogen : ppbv nitrous oxide : 0. ppbv carbonyl sulfide ozone hydrogen peroxide nitric acid nitrogen oxides (family) methane ethane ethylene propane propylene!" isoprene # $ "$& -pinene ( other hydrocarbons carbon monoxide methanol formaldehyde acetaldehyde )*, # *.-/" 0 glycolaldehyde - # *.- " 4 " 4 hydroxy carbonyls from ISOP # 7" Long-lived methylacrolein (transported) acetone # 8" hydroxy acetone " < :9 ; methylvinylketone methyl peroxide ethyl peroxide " peroxide from propylene peracetic acid = peroxide from propane # >( " peroxide from acetone " peroxide from ISOP # " < peroxide from MACR
4 - Chemical species included in the model (continued) Species Category Chemical Formula Name 0 < peroxide from # " peroxy-acetyl nitrate # " < peroxymethacrylic nitrate ( " substituted organic nitrate from ISOP sulfur dioxide non-sea-salt sulfate " < dimethyl sulfide carbon disulfide hydrogen sulfide - oxygen atom (excited state) hydroxyl radical hydroperoxyl radical nitrogen oxide nitrogen dioxide pernitric acid nitrogen trioxide nitrogen hemipentoxide Short-lived methylglyoxal methylperoxy radical " peroxy radical from propylene # >( " peroxy radical from acetone < peroxy radical from HYDRALDOH and ISOPOOHOH ethylperoxy radical = propylperoxy radical peroxy radical from ISOP # " peroxy radical from MACROH acetylperoxy radical " peroxymethacrylic radical
5 Table. Chemical reaction mechanism and kinetic rates. Chemical reaction mechanism and kinetic rates Reaction Rate Ref. - <., -!!. -! - -!! ", -! # "$" < $ & " '& ()$ "! -!! *. $)! &,! -<. 0/ &! < 4 & (!!. )!! $. ** (.!*.!! $ $...! " -. -,. *!! * -$,..!! (. $! $. $) & -. / 7 " <. / 4 & (! & 8 9;:<, 8 9,:= &,.<!. &),! ($ -,. $) &> (* -<. /?& ". 0/ 4 & (! ) $! $ 4
6 Chemical reaction mechanism and kinetic rates (continued) *! $ $ $ * # # # # # Reaction Rate Ref.! < ($ <. & -. / 7. &/ ) 4 ; ( ) )& ADC!! $ $) <.$!! (*.. 8! $.!! (,.)!)!!!!.! '& "! #& (*.!!! <!!!!. )$*)!! ($ #& (!!! (*. $) 4 <..$ < ($ 8!.! #& & < & < '&!! (*, < '&, '& (*. & < '&!! *. $) = 4 '& <..$ =, & <! ($& = = 8! #& (* $ )) = 7! (*. = = 7! >(. $ ) 4 >(!!! (*.. >( >( * (!. >( < #& ("!! ($..$
7 Chemical reaction mechanism and kinetic rates (continued) # $ # # $ $ $ $ # # / / &! $ # # Reaction & Rate Ref. & " <! >(! >( * 7! &;*. / 4 ; ( < ) 4 &! # $,!'& #& (! $ $ & (* '& $!!# & < < '& $ <! &,. / ; ) 4 & * 4!!!'&!#,! & #& < < ".$,!! $ 8 ) $! #& ($ #& ($ '& *!! $!.& 4 < *! 4!! * ) <! & 8 &;* ($.) 7 <. ) 4 & < ; ( ) ADC '& #& & ) & " < #& (! < $.$! #& ( < (.$ & #& ( '& <! #& ($ * & #& ($, $ < < '& # '& # ) ()$, :9 ; & () #& (!!# & #& )! '& # " ( #& )! '& ( ()!) :9 ; &!) '& ()!# "
8 Chemical reaction mechanism and kinetic rates (continued) Reaction Rate Ref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
9 Chemical reaction mechanism and kinetic rates (continued) Reaction Rate Ref. # <. 0/ & # ;. C <! *..*!!. *!) # $!? " <.<,7 # $! '&!* # '& $. - :9 ;, & #& $ #& ( #& ($&< #& & #, # $? " (..$!$), (! '& $ ($ <, - # * -!#& ($ ( - # *.-. *!) - # * -4 (*! <. $)? $!..$ & $ #!!)*, # * - $! ($,8 & $ #!!)*, # * - (*. 8! #& ( < $.<) & " #&, & #!!!)*, # *.-!!! <? $ (..! & $ #!!)*, # * -!! (. 9!!! (!. $) 9! '& $ #& ($ (*.!!!.! #! #& ($ # &;* ). / ; < 4 & ($ #!! 8, # <!!)*, # *.-#& (* #, #& (! <!!. -$)!!. ),0 - <.!,0 - '&!..$ ' ' 4 & &! '&, ($ ' 7 $ &<!)8 9;: 8
10 ( Chemical reaction mechanism and kinetic rates (continued) Reaction Rate Ref. - (..$,0!! * (*!. 0!! &; &<. / 7 $ ) 4! in-cloud 0!! & 4,! & (& 4,! # $ & 4, Read < as.4 ; =temperature (K); 8 9,: is the air density ( ); is the atmospheric pressure. ; is the reaction probability on aerosols. Units for first-, second-, and third-order reactions are,. and $ respectively. # &!'( )!"*,.-!/0 Three-body reaction rates are calculated with!". Rates for equilibrium reactions calculated C is the equilibrium ADC, where is the rate of the formation reaction and References:, DeMore et al. (997);, Sander et al. (000);, Tyndall et al. (00); 4, Atkinson et al. (999);, Horowitz et al. (00);, Müller and Brasseur (99); 7, Brasseur et al. (998); 8, Saunders et al. (00); 9, Brocheton (999); 0, Pham et al. (99);, Ravishankara et al. (00);, Atkinson (994);, Martinez et al. (999); 4, Jacob (000). Notes.. Rate assumed equal to the rate of the corresponding reaction of.. Rate assumed equal to the rate of the corresponding reaction of <.. Based on Horowitz et al. (00) assuming that the peroxy radical produced in this reaction reacts with. The conversion of to is neglected.. Rate assumed equal to the rate of the corresponding reaction of <.. Products as in Horowitz et al. (00), except that is replaced by, a more likely product in the -addition pathway of alkyl nitrates (Atkinson, 994).. Adapted from Brasseur et al. (998).. OTHC represents all non-methane VOCs (NMVOCs) non explicitly included in the mechanism. See article for details.. The heterogenous reaction of a gas on sulphate aerosols is represented as a pseudosecond-order reaction between the gas and particulate sulphate. 9
11 Table. Photodissocations included in the model. Photodissociations - # # # * # # # # # Reaction Cross section Quantum yield Products!!,4!!! 4!,,7 4!! 8!! 8 <! )*, *.-!!!! < <!! 4 '&! 9 9 & (!) "!! # " '& " :9 ; & ( # 9 #& (!" & "! 4 (!! 0!!!! # = >(!!!!!! '& * 7 &!!!?! & (*, #& (*, 7 &! >( 0
12 Photodissociations (continued) Reaction Cross section Quantum yield Products References:, DeMore et al. (997);, Atkinson et al. (00);, Molina and Molina (98); 4, Sander et al. (000);, Johnston et al. (99);, Knight et al. (00); 7, Roehl et al. (00); 8, Meller et al. (000); 9, Raber and Moortgat (99); 0, Atkinson et al. (999);, Martinez et al. (99);, Gierczak et al. (998);, Bacher et al. (00); 4, Kockarts (994);, Warneck (00);, Horowitz et al. (00); 7, Brocheton (999). Notes: ) Hertzberg continuum (0-40 nm) ) Schumann-Runge bands (7-0 nm) ) Quantum yield is taken equal to. ) Oxygen and hydrogen atoms as well as and radicals produced in the mechanism are assumed to react instantly with, an excellent approximation in the troposphere. ) nm temperature-independent cross sections ) 80-0 nm temperaturedependent cross sections ) The contribution of near-ir radiation to the photolysis of is about. during daytime throughout the atmosphere (Roehl et al., 00; Salawitch et al., 00). ) Use the corresponding photolysis quantum yield increased by a factor of. (Bacher ( et al., 00). ) is assumed to photolyse as -. ) Constant value of 0.0 " " & * # (upper limit) ) ) ) )
13 References Atkinson, R.: Gas-Phase tropospheric chemistry of organic compounds, J. Phys. Chem. Ref. Data, Monograph No., 994. Atkinson, R., Baulch, D. L., Cox, R. A., Hampson, R. F., Kerr, Jr., J. A., Rossi, M. J., and Troe, J.: Evaluated Kinetic and Photochemical Data for Atmospheric Chemistry, IUPAC Subcommittee on gas kinetic data evaluation for atmospheric chemistry, J. Phys. Chem. Ref. Data, 8, 9 9, 999. Atkinson, R., Baulch, D. L., Cox, R. A., Crowley, J. N., Hampson, R. F.(Jr), Kerr, J. A., Rossi, M. J., and Troe, J.: Summary of Evaluated Kinetic and Photochemical Data for Atmospheric Chemistry, IUPAC Subcommittee on gas kinetic data evaluation for atmospheric chemistry, Bacher, C., Tyndall, G. S. and Orlando, J. J.: The atmospheric chemistry of glycolaldehyde, J. Atmos. Chem., 9, 7 89, 00. Brasseur, G. P., Hauglustaine, D. A., Walters, S., Rasch, P. J., Müller, J.-F., Granier, C. and Tie X.: MOZART, a global chemical transport model for ozone and related tracers,. Model Description, J. Geophys. Res., 0, 8 889, 998. Brocheton, F.: Représentation des émissions anthropiques dans les modèles de chimie-transport: Sensibilité à la représentation spatiale des émissions et au degré de raffinement du schéma chimique, Ph.D., Université Paris - Val de Marne, 999. DeMore, W. B., Sander, S. P., Golden, D. M., Hampson, R. F., Kurylo, M. J., Howard, C. J., Ravishankara, A. R., Kolb, C. E. and Molina, M. J.: Chemical Kinetics and Photochemical Data for Use in Stratospheric Modeling, Evaluation number, NASA panel for data evaluation, JPL Publication 97-4, Jet Propulsion Laboratory, Pasadena, 997. Dentener, F. J. and Crutzen, P. J.: Reaction of on tropospheric aerosols: impact on the global distributions of,, and, J. Geophys. Res., 98, 749 7, 99. Gierczak, T., Burkholder, J. B., Bauerle, S. and Ravishankara, A. R., Photochemistry of acetone under tropospheric conditions, Chem. Phys.,, 9 44, 998. Jacob, D. J.: Heterogeneous Chemistry and Tropospheric Ozone, Atmos. Environ., 4, 9, 000. Johnston, H. S. Davis and Lee, Y. T.: photolysis product channels: quantum yields from observed energy thresholds, J. Phys. Chem., 00, 47 47, 99. Horowitz, L. W., Walters, S., Mauzerall, D. L., Emmons, L. K., Rasch, P. J., Granier, C., Tie X., Lamarque, J.-F., Schultz, M. G., Tyndall, G. S., Orlando, J. J. and Brasseur, G. P.: A global simulation of tropospheric ozone and related tracers: description and evaluation of Mozart, version, 08, No. D4, 4784, doi:0.09/00jd008, 00. Kockarts, G.: The penetration of solar radiation in the Schumann-Runge bands of molecular oxygen: a robust approximation, Ann. Geophysicae,, 07 7, 994. Knight, G., Ravishankara, A. R. and Burkholder, J.: UV absorption cross section of between 4 and 7 K, Phys. Chem. Chem. Phys., 4, 4 47, 00. Martinez, E., Cabanas, B., Aranda, A., Martin, P. and Salgado, S.: Absolute rate coefficients for the gas-phase reactions of radical with a series of monoterpenes at T=98 to 4 K, J. Atmos. Chem.,, 8, 999. Martinez, R. D., Buitrago, A. A., Howell, N. W., Hearn, C. H. and Joens J. A.: The near U.V. absorption spectra
14 of several aliphatic aldehydes and ketones at 00 K, Atmos. Environ.,, 78 79, 99. Meller, R. and Moortgat, G. K.: Temperature dependence of the absorption cross sections of formaldehyde between and K in the wavelength range -7 nm, J. Geophys. Res., 0, , 000. Middleton, P., Stockwell, W. R. and Carter, W. P.: Aggregation and analysis of volatile organic compound emissions for regional modeling, Atmos. Environ., 4, 07, 990. Molina, L. T. and Molina M. J.: Absolute absorption cross sections of ozone in the 8- to 0-nm wavelength range, J. Geophys. Res., 9, , 98. Müller, J.-F. and Brasseur, G. P.: IMAGES: A three-dimensional chemical transport model of the global troposphere, J. Geophys. Res., 00, , 99. Pham, M., Müller, J.-F., Brasseur, G. P., Granier, C., and Mégie, G.: A three-dimensional study of the tropospheric sulfur cycle, J. Geophys. Res., 00, 0 09, 99. Raber, W. H. and Moortgat, G. K.: Photodissociation of selected carbonyl compounds in air: methy ethyl ketone, methyl vinyl ketone, methacrolein and methylglyoxal, in Progress and problems in atmospheric chemistry, Barker, J. R., ed., pp. 8 7, World Scientific Publ. Co., Singapore, 99. Ravishankara, A. R., Dunlea, E. J., Blitz, M. A., Dillon, T. J., Heard, D. E., Pilling, M. J., Strekowski, R. S., Nicovich, J. M. and Wine, P. H.: Redetermination of the rate coefficient for the reaction with, Geophys. Res. Lett., 9, 0.09/00GL0480, 00. Roehl, C. A., Nizkorodov, S. A., Zhang, H., Blake, G. and Wennberg, P. O.: Photodissociation of in the near IR, J. Phys. Chem. A., 0, 7 77, 00. Salawitch, R. J., Wennberg, P. O., Toon, G. C., Sen, B. and Blavier, J.-F.: Near IR photolysis of : Implications for, Geophys. Res. Lett., 9, 0.09/00GL000, 00. Sander, S. P., Friedl, R. R., DeMore, W. B., Golden, D. M., Kurylo, M. J., Hampson, R. F., Huie, R. E., Moortgat, G. K., Ravishankara, A. R., Kolb, C. E. and Molina, M. J.: Chemical Kinetics and Photochemical Data for Use in Stratospheric Modeling, Evaluation number, NASA panel for data evaluation, JPL Publication 00-, Jet Propulsion Laboratory, Pasadena, 000. Saunders, S. M., Jenkin, M. E., Derwent, R. G. and Pilling, M. J.: Protocol for the development of the Master Chemical Mechanism, MCM v (Part A): tropospheric degradation of non-aromatic volatile organic compounds, Atmos. Chem. Phys.,, 80, 00. Tyndall, G. S., Cox, R. A., Granier, C., Lesclaux, R., Moortgat, G. K., Pilling, M. J., Ravishankara, A. R. and Wallington, T. J.: Atmospheric chemistry of small organic peroxy radicals, J. Geophys. Res., 0, D, 7 8, 00. Warneck, P.: Photodissociation of acetone in the troposphere: an algorithm for the quantum yield, Atmos. Environ.,, , 00.
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