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. Fluxes of halogenated volatile organic compounds (VOCs) over the SouthernOcean remain poorly understood, and few atmospheric measurements exist toconstrain modeled emissions of these compounds. We present observations of CHBr3 , CH2Br2 , CH3I , CHClBr2 , CHBrCl2 , and CH3Br during the O2∕N2 Ratio and CO2 Airborne SouthernOcean (ORCAS) study and the second Atmospheric Tomography mission(ATom-2) in January and February of 2016 and 2017. Good model–measurementcorrelations were obtained between these observations and simulations fromthe Community Earth System Model (CESM) atmospheric component with chemistry(CAM-Chem) for CHBr3 , CH2Br2 , CH3I , and CHClBr2 butall showed significant differences in model : measurement ratios. Themodel : measurement comparison for CH3Br was satisfactory and for CHBrCl2 the low levels present precluded us from making a completeassessment. Thereafter, we demonstrate two novel approaches to estimatehalogenated VOC fluxes; the first approach takes advantage of the robustrelationships that were found between airborne observations of O2 and CHBr3 , CH2Br2 , and CHClBr2 . We use these linearregressions with O2 and modeled O2 distributions to infer abiological flux of halogenated VOCs. The second approach uses the StochasticTime-Inverted Lagrangian Transport (STILT) particle dispersion model toexplore the relationships between observed mixing ratios and the product ofthe upstream surface influence of sea ice, chl  a , absorption due todetritus, and downward shortwave radiation at the surface, which in turnrelate to various regional hypothesized sources of halogenated VOCs such asmarine phytoplankton, phytoplankton in sea-ice brines, and decomposingorganic matter in surface seawater. These relationships can help evaluatethe likelihood of particular halogenated VOC sources and in the case ofstatistically significant correlations, such as was found for CH3I , maybe used to derive an estimated flux field. Our results are consistent with abiogenic regional source of CHBr3 and both nonbiological andbiological sources of CH3I over these regions.

Novel approaches to improve estimates of short-lived halocarbon emissions during summer from the Southern Ocean using airborne observations