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3. An Overview of Snow Photochemistry: Evidence, Mechanisms and Impacts

Author

Grannas, A. M, Jones, A. E, Dibb, J, Ammann, M, Anastasio, C, Beine, H. J, Bergin, M, Bottenheim, J, Boxe, C. S, Carver, G, Chen, G, Crawford, J. H, Domine, F, Frey, M. M, Guzman, M. I, Heard, D. E, Helmig, D, Hoffmann, M. R, Honrath, R. E, Huey, L. G, Hutterli, M, Jacobi, H.-W, Klan, P, McConnell, J, and Plane, J

Subjects
Meteorology And Climatology
Abstract

It has been shown that sunlit snow and ice plays an important role in processing atmospheric species. Photochemical production of a variety of chemicals has recently been reported to occur in snow/ice and the release of these photochemically generated species may significantly impact the chemistry of the overlying atmosphere. Nitrogen oxide and oxidant precursor fluxes have been measured in a number of snow covered environments, where in some cases the emissions significantly impact the overlying boundary layer. For example, photochemical ozone production (such as that occurring in polluted mid-latitudes) of 3-4 ppbv/day has been observed at South Pole, due to high OH and NO levels present in a relatively small boundary layer. Field and laboratory experiments have determined that the origin of the observed NOx flux is the photochemistry of nitrate within the snowpack, however some details of the mechanism have not yet been elucidated. A variety of low molecular weight organic compounds have been shown to be emitted from sunlit snowpacks, the source of which has been proposed to be either direct or indirect photo-oxidation of natural organic materials present in the snow. Although myriad studies have observed active processing of species within irradiated snowpacks, the fundamental chemistry occurring remains poorly understood. Here we consider the nature of snow at a fundamental, physical level; photochemical processes within snow and the caveats needed for comparison to atmospheric photochemistry; our current understanding of nitrogen, oxidant, halogen and organic photochemistry within snow; the current limitations faced by the field and implications for the future.

Published
2007

5. An overview of snow photochemistry: evidence, mechanisms and impacts

Author

Grannas, A. M., Jones, A. E., Dibb, J., Ammann, M., Anastasio, C., Beine, H. J., Bergin, M., Bottenheim, J., Boxe, C. S., Carver, G., Chen, G., Crawford, J. H., Dominé, F., Frey, M. M., Guzmán, M. I., Heard, D. E., Helmig, D., Hoffmann, M. R., Honrath, R. E., Huey, L. G., Hutterli, M., Jacobi, H. W., Klán, P., Lefer, B., McConnell, J., Plane, J., Sander, R., Savarino, J., Shepson, P. B., Simpson, W. R., Sodeau, J. R., von Glasow, R., Weller, R., Wolff, E. W., Zhu, T., Grannas, A. M., Jones, A. E., Dibb, J., Ammann, M., Anastasio, C., Beine, H. J., Bergin, M., Bottenheim, J., Boxe, C. S., Carver, G., Chen, G., Crawford, J. H., Dominé, F., Frey, M. M., Guzmán, M. I., Heard, D. E., Helmig, D., Hoffmann, M. R., Honrath, R. E., Huey, L. G., Hutterli, M., Jacobi, H. W., Klán, P., Lefer, B., McConnell, J., Plane, J., Sander, R., Savarino, J., Shepson, P. B., Simpson, W. R., Sodeau, J. R., von Glasow, R., Weller, R., Wolff, E. W., and Zhu, T.

Abstract

It has been shown that sunlit snow and ice plays an important role in processing atmospheric species. Photochemical production of a variety of chemicals has recently been reported to occur in snow/ice and the release of these photochemically generated species may significantly impact the chemistry of the overlying atmosphere. Nitrogen oxide and oxidant precursor fluxes have been measured in a number of snow covered environments, where in some cases the emissions significantly impact the overlying boundary layer. For example, photochemical ozone production (such as that occurring in polluted mid-latitudes) of 3–4 ppbv/day has been observed at South Pole, due to high OH and NO levels present in a relatively shallow boundary layer. Field and laboratory experiments have determined that the origin of the observed NOx flux is the photochemistry of nitrate within the snowpack, however some details of the mechanism have not yet been elucidated. A variety of low molecular weight organic compounds have been shown to be emitted from sunlit snowpacks, the source of which has been proposed to be either direct or indirect photo-oxidation of natural organic materials present in the snow. Although myriad studies have observed active processing of species within irradiated snowpacks, the fundamental chemistry occurring remains poorly understood. Here we consider the nature of snow at a fundamental, physical level; photochemical processes within snow and the caveats needed for comparison to atmospheric photochemistry; our current understanding of nitrogen, oxidant, halogen and organic photochemistry within snow; the current limitations faced by the field and implications for the future.

Published
2007

8. A comparison of Arctic BrO measurements by chemical ionization mass spectrometry and long path-differential optical absorption spectroscopy

Author

Liao, J., primary, Sihler, H., additional, Huey, L. G., additional, Neuman, J. A., additional, Tanner, D. J., additional, Friess, U., additional, Platt, U., additional, Flocke, F. M., additional, Orlando, J. J., additional, Shepson, P. B., additional, Beine, H. J., additional, Weinheimer, A. J., additional, Sjostedt, S. J., additional, Nowak, J. B., additional, Knapp, D. J., additional, Staebler, R. M., additional, Zheng, W., additional, Sander, R., additional, Hall, S. R., additional, and Ullmann, K., additional

Published
2011
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10. An overview of snow photochemistry: evidence, mechanisms and impacts

Author

Grannas, A. M., primary, Jones, A. E., additional, Dibb, J., additional, Ammann, M., additional, Anastasio, C., additional, Beine, H. J., additional, Bergin, M., additional, Bottenheim, J., additional, Boxe, C. S., additional, Carver, G., additional, Chen, G., additional, Crawford, J. H., additional, Dominé, F., additional, Frey, M. M., additional, Guzmán, M. I., additional, Heard, D. E., additional, Helmig, D., additional, Hoffmann, M. R., additional, Honrath, R. E., additional, Huey, L. G., additional, Hutterli, M., additional, Jacobi, H. W., additional, Klán, P., additional, Lefer, B., additional, McConnell, J., additional, Plane, J., additional, Sander, R., additional, Savarino, J., additional, Shepson, P. B., additional, Simpson, W. R., additional, Sodeau, J. R., additional, von Glasow, R., additional, Weller, R., additional, Wolff, E. W., additional, and Zhu, T., additional

Published
2007
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19. Small HONO emissions from snow surfaces at Browning Pass, Antarctica.

Author

Beine, H. J., Amoroso, A., Dominé, F., King, M. D., Nardino, M., Ianniello, A., and France, J. L.

Abstract

Measured Fluxes of nitrous acid at Browning Pass, Antarctica were very low, despite conditions that are generally understood as favorable for HONO emissions, including: acidic snow surfaces, an abundance of NO3- anions in the snow surface, and abundant UV light for NO3- photolysis. Photochemical modeling suggests noon time HONO fluxes of 5-10 nmol m-2h-1; the measured fluxes, however, were close to zero throughout the campaign. The analysis of soluble mineral ions in snow reveals that the NO-3 ion is probably present in aged snows as NaNO3. This is peculiar to our study site, and we suggest that this may affect the photochemical reactivity of NO3-, by preventing the release of products, or providing a reactive medium for newly formed HONO. In 10 fresh snow, the NO3- ion is probably present as dissolved or adsorbed HNO3 and yet, no HONO emissions were observed. We speculate that HONO formation from NO3- photolysis may involve electron transfer reactions of NO2 from photosensitized organics and that fresh snows at our site had insufficient concentrations of adequate organic compounds to favor this reaction. [ABSTRACT FROM AUTHOR]

Published
2006
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20. An overview of snow photochemistry: evidence, mechanisms and impacts

Author

Grannas, A. M., Jones, A. E., Dibb, J., Ammann, M., Anastasio, C., Beine, H. J., Bergin, M., Bottenheim, J., Boxe, C. S., Carver, G., Chen, G., Crawford, J. H., Dominé, F., Frey, M. M., Guzmán, M. I., Heard, D. E., Helmig, D., Hoffmann, M. R., Honrath, R. E., Huey, L. G., Hutterli, M., Hans-Werner Jacobi, Klán, P., Lefer, B., Mcconnell, J., Plane, J., Sander, R., Savarino, J., Shepson, P. B., Simpson, W. R., Sodeau, J. R., Glasow, R., Weller, R., Wolff, E. W., Zhu, T., Department of Chemistry, Villanova University, British Antarctic Survey (BAS), Natural Environment Research Council (NERC), Institute for Study of Earth, Oceans and Space, University of New Hampshire (UNH), Laboratory for Radio- and Environmental Chemistry, Department of Land, Air {&} Water Resources, Consiglio Nazionale delle Ricerche [Roma] (CNR), School of Earth and Atmospheric Sciences [Atlanta], Georgia Institute of Technology [Atlanta], Air Quality Research Branch, Environment and Climate Change Canada, W. M. Keck Laboratories, California Institute of Technology (CALTECH), Centre for Atmospheric Science [Cambridge, UK], Department of Chemistry [Cambridge, UK], University of Cambridge [UK] (CAM)-University of Cambridge [UK] (CAM), NASA Langley Research Center [Hampton] (LaRC), Laboratoire de glaciologie et géophysique de l'environnement (LGGE), Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut national des sciences de l'Univers (INSU - CNRS)-Centre National de la Recherche Scientifique (CNRS)-Université Grenoble Alpes (UGA)-Centre National de la Recherche Scientifique (CNRS), School of Engineering, University of California [Merced], University of California-University of California, School of Chemistry [Leeds], University of Leeds, Institute of Arctic and Alpine Research (INSTAAR), University of Colorado [Boulder], Department of Civil and Environmental Engineering [Michigan] (CEE), Michigan Technological University (MTU), Department of Bentho-pelagic processes, Alfred-Wegener-Institut, Helmholtz-Zentrum für Polar- und Meeresforschung (AWI), Masaryk University, Department of Geosciences [Houston], University of Houston, Department of Earth and Space Science and Engineering [York University - Toronto] (ESSE), York University [Toronto], Atmospheric Chemistry Department [MPIC], Max Planck Institute for Chemistry (MPIC), Max-Planck-Gesellschaft-Max-Planck-Gesellschaft, Department of Chemistry [West Lafayette], Purdue University [West Lafayette], Department of Chemistry and Geophysical Institute, University of Alaska [Fairbanks] (UAF), School of Environmental Sciences [Norwich], University of East Anglia [Norwich] (UEA), Institute of Environmental Physics [Heidelberg] (IUP), Universität Heidelberg [Heidelberg], College of Environmental Sciences and Engineering [Peking], Peking University [Beijing], Air & Water Resources, Department of Earth, Atmospheric, and Planetary Sciences [West Lafayette] (EAPS), University of Cambridge [UK] (CAM), Centre National de la Recherche Scientifique (CNRS)-Institut national des sciences de l'Univers (INSU - CNRS)-Observatoire des Sciences de l'Univers de Grenoble (OSUG), Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national des sciences de l'Univers (INSU - CNRS)-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS)-Université Joseph Fourier - Grenoble 1 (UJF)-Institut polytechnique de Grenoble - Grenoble Institute of Technology (Grenoble INP )-Institut national de recherche en sciences et technologies pour l'environnement et l'agriculture (IRSTEA)-Université Savoie Mont Blanc (USMB [Université de Savoie] [Université de Chambéry])-Centre National de la Recherche Scientifique (CNRS), and Masaryk University [Brno] (MUNI)

Subjects
lcsh:Chemistry, [SDU.OCEAN]Sciences of the Universe [physics]/Ocean, Atmosphere, lcsh:QD1-999, 010504 meteorology & atmospheric sciences, 13. Climate action, 010501 environmental sciences, 01 natural sciences, lcsh:Physics, lcsh:QC1-999, Caltech Library Services, 0105 earth and related environmental sciences
Abstract

International audience; It has been shown that sunlit snow and ice plays an important role in processing atmospheric species. Photochemical production of a variety of chemicals has recently been reported to occur in snow/ice and the release of these photochemically generated species may significantly impact the chemistry of the overlying atmosphere. Nitrogen oxide and oxidant precursor fluxes have been measured in a number of snow covered environments, where in some cases the emissions significantly impact the overlying boundary layer. For example, photochemical ozone production (such as that occurring in polluted mid-latitudes) of 3–4 ppbv/day has been observed at South Pole, due to high OH and NO levels present in a relatively shallow boundary layer. Field and laboratory experiments have determined that the origin of the observed NOx flux is the photochemistry of nitrate within the snowpack, however some details of the mechanism have not yet been elucidated. A variety of low molecular weight organic compounds have been shown to be emitted from sunlit snowpacks, the source of which has been proposed to be either direct or indirect photo-oxidation of natural organic materials present in the snow. Although myriad studies have observed active processing of species within irradiated snowpacks, the fundamental chemistry occurring remains poorly understood. Here we consider the nature of snow at a fundamental, physical level; photochemical processes within snow and the caveats needed for comparison to atmospheric photochemistry; our current understanding of nitrogen, oxidant, halogen and organic photochemistry within snow; the current limitations faced by the field and implications for the future.

21. Microorganisms in dry polar snow are involved in the exchanges of reactive nitrogen species with the atmosphere.

Author

Amoroso A, Domine F, Esposito G, Morin S, Savarino J, Nardino M, Montagnoli M, Bonneville JM, Clement JC, Ianniello A, and Beine HJ

Subjects
Arctic Regions, Atmosphere, Nitrogen, Oxygen, Photochemical Processes, Seasons, Reactive Oxygen Species metabolism, Snow microbiology
Abstract

The snowpack is a complex photochemical reactor that emits a wide variety of reactive molecules to the atmosphere. In particular, the photolysis of nitrate ions, NO(3)(-), produces NO, NO(2), and HONO, which affects the oxidative capacity of the atmosphere. We report measurements in the European High Arctic where we observed for the first time emissions of NO, NO(2), and HONO by the seasonal snowpack in winter, in the complete or near-complete absence of sunlight and in the absence of melting. We also detected unusually high concentrations of nitrite ions, NO(2)(-), in the snow. These results suggest that microbial activity in the snowpack is responsible for the observed emissions. Isotopic analysis of NO(2)(-) and NO(3)(-) in the snow confirm that these ions, at least in part, do not have an atmospheric origin and are most likely produced by the microbial oxidation of NH(4)(+) coming from clay minerals into NO(2)(-) and NO(3)(-). These metabolic pathways also produce NO. Subsequent dark abiotic reactions lead to NO(2) and HONO production. The snow cover is therefore not only an active photochemical reactor but also a biogeochemical reactor active in the cycling of nitrogen and it can affect atmospheric composition all year round.

Published
2010
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