The role of ice in the formation of chemically active halogens in the environment requires a full understanding because of its role in atmospheric chemistry, including controlling the regional atmospheric oxidizing capacity in specific situations. In particular, ice and snow are important for facilitating multiphase oxidative chemistry and as media upon which marine algae live. This paper reviews the nature of environmental ice substrates that participate in halogen chemistry, describes the reactions that occur on such substrates, presents the field evidence for ice-mediated halogen activation, summarizes our best understanding of ice-halogen activation mechanisms, and describes the current state of modeling these processes at different scales. Given the rapid pace of developments in the field, this paper largely addresses advances made in the past five years, with emphasis given to the polar boundary layer. The integrative nature of this field is highlighted in the presentation of work from the molecular to the regional scale, with a focus on understanding fundamental processes. This is essential for developing realistic parameterizations and descriptions of these processes for inclusion in larger scale models that are used to determine their regional and global impacts
Abstract. The physical, chemical, and biological processes involving organics in ice in the environment impact a number of atmospheric and biogeochemical cycles. Organic material in snow or ice may be biological in origin, deposited from aerosols or atmospheric gases, or formed chemically in situ. In this manuscript, we review the current state of knowledge regarding the sources, properties, and chemistry of organic materials in environmental ices. Several outstanding questions remain to be resolved and fundamental data gathered before an accurate model of transformations and transport of organic species in the cryosphere will be possible. For example, more information is needed regarding the quantitative impacts of chemical and biological processes, ice morphology, and snow formation on the fate of organic material in cold regions. Interdisciplinary work at the interfaces of chemistry, physics and biology is needed in order to fully characterize the nature and evolution of organics in the cryosphere and predict the effects of climate change on the Earth's carbon cycle.
Context. Millimetric observations have measured high degrees of molecular deuteration in several species seen around low-mass protostars. The Herschel Space Telescope, launched in 2009, is now providing new measures of the deuterium fractionation of water, the main constituent of interstellar ices. Aims. We aim at theoretically studying the formation and the deuteration of water, which is believed to be formed on interstellar grain surfaces in molecular clouds. Methods. We used our gas-grain astrochemical model GRAINOBLE, which considers the multilayer formation of interstellar ices. We varied several input parameters to study their impact on water deuteration. We included the treatment of ortho-and para-states of key species, including H 2 , which affects the deuterium fractionation of all molecules. The model also includes relevant laboratory and theoretical works on the water formation and deuteration on grain surfaces. In particular, we computed the transmission probabilities of surface reactions using the Eckart model, and we considered ice photodissociation following molecular dynamics simulations. Results. The use of a multilayer approach allowed us to study the influence of various parameters on the abundance and the deuteration of water. Deuteration of water is found to be very sensitive to the ortho-to-para ratio of H 2 and to the total density, but it also depends on the gas/grain temperatures and the visual extinction of the cloud. Since the deuteration is very sensitive to the physical conditions, the comparison with sub-millimetric observation towards the low-mass protostar IRAS 16293 allows us to suggest that water ice is formed together with CO 2 in molecular clouds with limited density, whilst formaldehyde and methanol are mainly formed in a later phase, where the condensation becomes denser and colder.
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