Radicals in the marine boundary layer during NEAQS 2004: A model study of day-time and night-time sources and sinks

Sommariva, R., Osthoff, H. D., Brown, S. S., Bates, T. S., Baynard, T., Coffman, D., de Gouw, J. A., Goldan, P. D., Kuster, W. C., Lerner, B. M., Stark, H., Warneke, C., Williams, E. J., Fehsenfeld, F. C., Ravishankara, A. R. and Trainer, M. (2009) Radicals in the marine boundary layer during NEAQS 2004: A model study of day-time and night-time sources and sinks. Atmospheric Chemistry and Physics, 9 (9). pp. 3075-3093.

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Abstract

This paper describes a modelling study of several HOx and NOx species (OH, HO2, organic peroxy radicals, NO 3 and N2O5) in the marine boundary layer. A model based upon the Master Chemical Mechanism (MCM) was constrained to observations of chemical and physical parameters made onboard the NOAA ship R/V Brown as part of the New England Air Quality Study (NEAQS) in the summer of 2004. The model was used to calculate [OH] and to determine the composition of the peroxy radical pool. Modelled [NO3] and [N 2O5] were compared to in-situ measurements by Cavity Ring-Down Spectroscopy. The comparison showed that the model generally overestimated the measurements by 30g€"50%, on average. The model results were analyzed with respect to several chemical and physical parameters, including uptake of NO3 and N 2O5 on fog droplets and on aerosol, dry deposition of NO3 and N2O5, gas-phase hydrolysis of N 2O5 and reactions of NO3 with NMHCs and peroxy radicals. The results suggest that fog, when present, is an important sink for N2O5 via rapid heterogeneous uptake. The comparison between the model and the measurements were consistent with values of the heterogeneous uptake coefficient of N2O5 (I3N 2O5)>1×10-2, independent of aerosol composition in this marine environment. The analysis of the different loss processes of the nitrate radical showed the important role of the organic peroxy radicals, which accounted for a significant fraction (median: 15%) of NO3 gas-phase removal, particularly in the presence of high concentrations of dimethyl sulphide (DMS).

Item Type:	Article
Additional Information:	© Author(s) 2009. This work is distributed under the Creative Commons Attribution 3.0 License.
Uncontrolled Keywords:	sdg 14 - life below water ,/dk/atira/pure/sustainabledevelopmentgoals/life_below_water
Faculty \ School:	Faculty of Science > School of Environmental Sciences
Depositing User:	Rosie Cullington
Date Deposited:	23 Feb 2011 11:40
Last Modified:	24 Sep 2024 09:26
URI:	https://ueaeprints.uea.ac.uk/id/eprint/24425
DOI:	10.5194/acp-9-3075-2009

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