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000020323 084__ $$2WoS$$aMeteorology & Atmospheric Sciences
000020323 1001_ $$0P:(DE-HGF)0$$aKanaya, Y.$$b0
000020323 245__ $$aComparisons of observed and modeled OH and HO2 concentrations during the ambient measurement period of the HOxComp field campaign
000020323 260__ $$aKatlenburg-Lindau$$bEGU$$c2012
000020323 300__ $$a2567 - 2585
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000020323 440_0 $$09601$$aAtmospheric Chemistry and Physics$$v12$$x1680-7316
000020323 500__ $$3POF3_Assignment on 2016-02-29
000020323 500__ $$aHelpful comments by two anonymous reviewers are greatly appreciated. This work was supported by the EU FP-6 program EUROCHAMP (grant no. RII3-CT-2004-505968), ACCENT (Priority 1.1.6.3. Global Change and Ecosystems, grant no. GOCE-CT-2004-505337), a Grant-in-Aid for Scientific Research (KAKENHI) (B) 22310018 and RR2002 of the Kyosei Project by the Ministry of Education, Science, Sports, and Culture of Japan. We thank F. J. Johnen for assistance with the experiments and K. D. Lu for discussions.
000020323 520__ $$aA photochemical box model constrained by ancillary observations was used to simulate OH and HO2 concentrations for three days of ambient observations during the HO(x)Comp field campaign held in Julich, Germany in July 2005. Daytime OH levels observed by four instruments were fairly well reproduced to within 33% by a base model run (Regional Atmospheric Chemistry Mechanism with updated isoprene chemistry adapted from Master Chemical Mechanism ver. 3.1) with high R-2 values (0.72-0.97) over a range of isoprene (0.3-2 ppb) and NO (0.1-10 ppb) mixing ratios. Daytime HO2(*) levels, reconstructed from the base model results taking into account the sensitivity toward speciated RO2 (organic peroxy) radicals, as recently reported from one of the participating instruments in the HO2 measurement mode, were 93% higher than the observations made by the single instrument. This also indicates an overprediction of the HO2 to OH recycling. Together with the good model-measurement agreement for OH, it implies a missing OH source in the model. Modeled OH and HO2(*) could only be matched to the observations by addition of a strong unknown loss process for HO2(*) that recycles OH at a high yield. Adding to the base model, instead, the recently proposed isomerization mechanism of isoprene peroxy radicals (Peeters and Muller, 2010) increased OH and HO2(*) by 28% and 13% on average. Although these were still only 4% higher than the OH observations made by one of the instruments, larger overestimations (42-70%) occurred with respect to the OH observations made by the other three instruments. The overestimation in OH could be diminished only when reactive alkanes (HC8) were solely introduced to the model to explain the missing fraction of observed OH reactivity. Moreover, the overprediction of HO2(*) became even larger than in the base case. These analyses imply that the rates of the isomerization are not readily supported by the ensemble of radical observations. One of the measurement days was characterized by low isoprene concentrations (similar to 0.5 ppb) and OH reactivity that was well explained by the observed species, especially before noon. For this selected period, as opposed to the general behavior, the model tended to underestimate HO2(*). We found that this tendency is associated with high NOx concentrations, suggesting that some HO2 production or regeneration processes under high NOx conditions were being overlooked; this might require revision of ozone production regimes.
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000020323 7001_ $$0P:(DE-HGF)0$$aMiyamoto, K.$$b12
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000020323 7001_ $$0P:(DE-HGF)0$$aWatanabe, K.$$b14
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000020323 7001_ $$0P:(DE-HGF)0$$aKubistin, D.$$b16
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000020323 7001_ $$0P:(DE-HGF)0$$aKleffmann, J.$$b24
000020323 7001_ $$0P:(DE-HGF)0$$aElshorbany, Y.$$b25
000020323 7001_ $$0P:(DE-HGF)0$$aSchurath, U.$$b26
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