气候变化领域集成服务门户(CCPortal): Laboratory measurements of HDO/H2O isotopic fractionation during ice deposition in simulated cirrus clouds

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DOI	10.1073/pnas.1618374114
	Laboratory measurements of HDO/H2O isotopic fractionation during ice deposition in simulated cirrus clouds
	Lamb K.D.; Clouser B.W.; Bolot M.; Sarkozy L.; Ebert V.; Saathoff H.; Möhler O.; Moyer E.J.
发表日期	2017
ISSN	0027-8424
起始页码	5612
结束页码	5617
卷号	114 期号:22
英文摘要	The stable isotopologues of water have been used in atmospheric and climate studies for over 50 years, because their strong temperature-dependent preferential condensation makes them useful diagnostics of the hydrological cycle. However, the degree of preferential condensation between vapor and ice has never been directly measured at temperatures below 233 K (-40 °C), conditions necessary to form cirrus clouds in the Earth's atmosphere, routinely observed in polar regions, and typical for the near-surface atmospheric layers of Mars. Models generally assume an extrapolation from the warmer experiments of Merlivat and Nief [Merlivat L, Nief G (1967) Tellus 19:122-127]. Nonequilibrium kinetic effects that should alter preferential partitioning have also not been well characterized experimentally. We present here direct measurements of HDO/H2O equilibrium fractionation between vapor and ice (αeq) at cirrus-relevant temperatures, using in situ spectroscopic measurements of the evolving isotopic composition of water vapor during cirrus formation experiments in a cloud chamber. We rule out the recent proposed upward modification of αeq, and find values slightly lower than Merlivat and Nief. These experiments also allow us to make a quantitative validation of the kinetic modification expected to occur in supersaturated conditions in the ice-vapor system. In a subset of diffusion-limited experiments, we show that kinetic isotope effects are indeed consistent with published models, including allowing for small surface effects. These results are fundamental for inferring processes on Earth and other planets from water isotopic measurements. They also demonstrate the utility of dynamic in situ experiments for studying fractionation in geochemical systems.
英文关键词	Cirrus clouds; Diffusivity ratio; Ice deposition; Isotopic fractionation; Water vapor
语种	英语
scopus关键词	deuterium oxide; ice; Article; astronomy; atmospheric deposition; cloud; fractionation; low temperature; priority journal; temperature dependence; validation study; vapor; water vapor
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/160632
作者单位	Lamb, K.D., Department of Physics, University of Chicago, Chicago, IL 60637, United States, Chemical Sciences Division, Earth System Research Laboratory, National Oceanic and Atmospheric Administration, Boulder, CO 80305, United States; Clouser, B.W., Department of Physics, University of Chicago, Chicago, IL 60637, United States; Bolot, M., Department of the Geophysical Sciences, University of Chicago, Chicago, IL 60637, United States, Program in Atmospheric and Oceanic Sciences, Princeton University, Princeton, NJ 08540, United States; Sarkozy, L., Department of the Geophysical Sciences, University of Chicago, Chicago, IL 60637, United States; Ebert, V., Physikalisch-Technische Bundesanstalt, Braunschweig, 38116, Germany; Saathoff, H., Institute for Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, 76021, Germany; Möhler, O., Institute for Meteorology and Climate Research, Karlsruhe Institute of Technology, Karlsruhe, 76021, Germany; Moyer, E.J., Department of the Geop...
推荐引用方式 GB/T 7714	Lamb K.D.,Clouser B.W.,Bolot M.,et al. Laboratory measurements of HDO/H2O isotopic fractionation during ice deposition in simulated cirrus clouds[J],2017,114(22).
APA	Lamb K.D..,Clouser B.W..,Bolot M..,Sarkozy L..,Ebert V..,...&Moyer E.J..(2017).Laboratory measurements of HDO/H2O isotopic fractionation during ice deposition in simulated cirrus clouds.Proceedings of the National Academy of Sciences of the United States of America,114(22).
MLA	Lamb K.D.,et al."Laboratory measurements of HDO/H2O isotopic fractionation during ice deposition in simulated cirrus clouds".Proceedings of the National Academy of Sciences of the United States of America 114.22(2017).