期刊
ATMOSPHERIC CHEMISTRY AND PHYSICS
卷 16, 期 5, 页码 3041-3059出版社
COPERNICUS GESELLSCHAFT MBH
DOI: 10.5194/acp-16-3041-2016
关键词
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资金
- California Air Resources Board [12-312]
- NOAA [NA13OAR4310058]
- CARB [11-305]
- EPA STAR [83587701-0]
The influence of losses of organic vapors to chamber walls during secondary organic aerosol (SOA) formation experiments has recently been established. Here, the influence of such losses on simulated ambient SOA concentrations and properties is assessed in the University of California at Davis / California Institute of Technology (UCD/CIT) regional air quality model using the statistical oxidation model (SOM) for SOA. The SOM was fit to laboratory chamber data both with and without accounting for vapor wall losses following the approach of Zhang et al. (2014). Two vapor wall-loss scenarios are considered when fitting of SOM to chamber data to determine best-fit SOM parameters, one with low and one with high vapor wall-loss rates to approximately account for the current range of uncertainty in this process. Simulations were run using these different parameterizations (scenarios) for both the southern California/South Coast Air Basin (SoCAB) and the eastern United States (US). Accounting for vapor wall losses leads to substantial increases in the simulated SOA concentrations from volatile organic compounds (VOCs) in both domains, by factors of similar to aEuro parts per thousand aEuro-2-5 for the low and similar to aEuro parts per thousand aEuro-5-10 for the high scenarios. The magnitude of the increase scales approximately inversely with the absolute SOA concentration of the no loss scenario. In SoCAB, the predicted SOA fraction of total organic aerosol (OA) increases from similar to aEuro parts per thousand aEuro-0.2 (no) to similar to aEuro parts per thousand aEuro-0.5 (low) and to similar to aEuro parts per thousand aEuro-0.7 (high), with the high vapor wall-loss simulations providing best general agreement with observations. In the eastern US, the SOA fraction is large in all cases but increases further when vapor wall losses are accounted for. The total OAaEuro-a center dot aEuro-Delta CO ratio captures the influence of dilution on SOA concentrations. The simulated OAaEuro-a center dot aEuro-Delta CO in SoCAB (specifically, at Riverside, CA) is found to increase substantially during the day only for the high vapor wall-loss scenario, which is consistent with observations and indicative of photochemical production of SOA. Simulated OaEuro-:aEuro-C atomic ratios for both SOA and for total OA increase when vapor wall losses are accounted for, while simulated HaEuro-:aEuro-C atomic ratios decrease. The agreement between simulations and observations of both the absolute values and the diurnal profile of the OaEuro-:aEuro-C and HaEuro-:aEuro-C atomic ratios for total OA was greatly improved when vapor wall-losses were accounted for. These results overall demonstrate that vapor wall losses in chambers have the potential to exert a large influence on simulated ambient SOA concentrations, and further suggest that accounting for such effects in models can explain a number of different observations and model-measurement discrepancies.
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