Reactive uptake coefficients for N2O5 determined from aircraft measurements during the Second Texas Air Quality Study: Comparison to current model parameterizations

被引:112
作者
Brown, Steven S. [1 ,4 ]
Dube, William P. [1 ,4 ]
Fuchs, Hendrik [1 ,4 ]
Ryerson, Thomas B. [1 ]
Wollny, Adam G. [1 ,4 ]
Brock, Charles A. [1 ]
Bahreini, Roya [1 ,4 ]
Middlebrook, Ann M. [1 ]
Neuman, J. Andrew [1 ,4 ]
Atlas, Elliot [2 ]
Roberts, James M. [1 ]
Osthoff, Hans D. [1 ,4 ]
Trainer, Michael [1 ]
Fehsenfeld, Frederick C. [1 ,4 ]
Ravishankara, A. R. [1 ,3 ]
机构
[1] NOAA, Earth Syst Res Lab, Boulder, CO 80305 USA
[2] Univ Miami, RSMAS, Miami, FL 33149 USA
[3] Univ Colorado, Dept Chem & Biochem, Boulder, CO 80309 USA
[4] Univ Colorado, Cooperat Inst Res Environm Sci, Boulder, CO 80309 USA
关键词
MARINE BOUNDARY-LAYER; LONG-TERM OBSERVATION; IN-SITU MEASUREMENTS; GAS-PHASE REACTION; HETEROGENEOUS HYDROLYSIS; AQUEOUS AEROSOLS; GASEOUS N2O5; ORGANIC-COMPOUNDS; NITRATE RADICALS; SULFURIC-ACID;
D O I
10.1029/2008JD011679
中图分类号
P4 [大气科学(气象学)];
学科分类号
0706 ; 070601 ;
摘要
This paper presents determinations of reactive uptake coefficients for N2O5, gamma( N2O5), on aerosols from nighttime aircraft measurements of ozone, nitrogen oxides, and aerosol surface area on the NOAA P-3 during Second Texas Air Quality Study (TexAQS II). Determinations based on both the steady state approximation for NO3 and N2O5 and a plume modeling approach yielded gamma(N2O5) substantially smaller than current parameterizations used for atmospheric modeling and generally in the range 0.5-6 x 10(-3). Dependence of gamma(N2O5) on variables such as relative humidity and aerosol composition was not apparent in the determinations, although there was considerable scatter in the data. Determinations were also inconsistent with current parameterizations of the rate coefficient for homogenous hydrolysis of N2O5 by water vapor, which may be as much as a factor of 10 too large. Nocturnal halogen activation via conversion of N2O5 to ClNO2 on chloride aerosol was not determinable from these data, although limits based on laboratory parameterizations and maximum nonrefractory aerosol chloride content showed that this chemistry could have been comparable to direct production of HNO3 in some cases.
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页数:16
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