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Title: Effect of sea salt aerosol on tropospheric bromine chemistry
Abstract. Bromine radicals influence global tropospheric chemistryby depleting ozone and by oxidizing elemental mercury and reduced sulfurspecies. Observations typically indicate a 50 % depletion of sea saltaerosol (SSA) bromide relative to seawater composition, implying that SSAdebromination could be the dominant global source of tropospheric bromine.However, it has been difficult to reconcile this large source with therelatively low bromine monoxide (BrO) mixing ratios observed in the marineboundary layer (MBL). Here we present a new mechanistic description of SSAdebromination in the GEOS-Chem global atmospheric chemistry model with adetailed representation of halogen (Cl, Br, and I) chemistry. We show thatobserved levels of SSA debromination can be reproduced in a mannerconsistent with observed BrO mixing ratios. Bromine radical sinks from theHOBr + S(IV) heterogeneous reactions and from ocean emission ofacetaldehyde are critical in moderating tropospheric BrO levels. Theresulting HBr is rapidly taken up by SSA and also deposited. Observations of SSA debromination at southern midlatitudes in summer suggest that modeluptake of HBr by SSA may be too fast. The model provides a successfulsimulation of free-tropospheric BrO in the tropics and midlatitudes in summer,where the bromine radical sink from the HOBr + S(IV) reactions iscompensated for by more efficient HOBr-driven recycling in clouds compared toprevious GEOS-Chem versions. Simulated BrO in the MBL is generally muchhigher in winter than in summer due to a combination of greater SSA emissionand slower conversion of bromine radicals to HBr. An outstanding issue inthe model is the overestimate of free-tropospheric BrO in extratropicalwinter–spring, possibly reflecting an overestimate of the HOBr∕HBr ratiounder these conditions where the dominant HOBr source is hydrolysis ofBrNO3.  more » « less
Award ID(s):
1643217 1702266
PAR ID:
10109064
Author(s) / Creator(s):
; ; ; ; ; ; ; ; ; ; ; ; ; ;
Date Published:
Journal Name:
Atmospheric Chemistry and Physics
Volume:
19
Issue:
9
ISSN:
1680-7324
Page Range / eLocation ID:
6497 to 6507
Format(s):
Medium: X
Sponsoring Org:
National Science Foundation
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