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DOI | 10.1073/pnas.1618374114 |
Laboratory measurements of HDO/H2O isotopic fractionation during ice deposition in simulated cirrus clouds | |
Lamb, Kara D.1,5; Clouser, Benjamin W.1; Bolot, Maximilien2,6; Sarkozy, Laszlo2; Ebert, Volker3; Saathoff, Harald4; Moehler, Ottmar4; Moyer, Elisabeth J.2 | |
2017-05-30 | |
发表期刊 | PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
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ISSN | 0027-8424 |
出版年 | 2017 |
卷号 | 114期号:22页码:5612-5617 |
文章类型 | Article |
语种 | 英语 |
国家 | USA; Germany |
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 degrees 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 (alpha(eq)) 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 alpha(eq), 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 | isotopic fractionation water vapor cirrus clouds ice deposition diffusivity ratio |
领域 | 地球科学 ; 气候变化 ; 资源环境 |
收录类别 | SCI-E |
WOS记录号 | WOS:000402296700040 |
WOS关键词 | WATER-VAPOR ; EQUILIBRIUM FRACTIONATION ; MARTIAN ATMOSPHERE ; HDO ; PRECIPITATION ; NUCLEATION ; GROWTH ; MODEL ; O-18 |
WOS类目 | Multidisciplinary Sciences |
WOS研究方向 | Science & Technology - Other Topics |
URL | 查看原文 |
引用统计 | |
文献类型 | 期刊论文 |
条目标识符 | http://119.78.100.173/C666/handle/2XK7JSWQ/204722 |
专题 | 地球科学 资源环境科学 气候变化 |
作者单位 | 1.Univ Chicago, Dept Phys, Chicago, IL 60637 USA; 2.Univ Chicago, Dept Geophys Sci, Chicago, IL 60637 USA; 3.Phys Tech Bundesanstalt, D-38116 Braunschweig, Germany; 4.Karlsruhe Inst Technol, Inst Meteorol & Climate Res, D-76021 Karlsruhe, Germany; 5.NOAA, Earth Syst Res Lab, Chem Sci Div, Boulder, CO 80305 USA; 6.Princeton Univ, Program Atmospher & Ocean Sci, Princeton, NJ 08540 USA |
推荐引用方式 GB/T 7714 | Lamb, Kara D.,Clouser, Benjamin W.,Bolot, Maximilien,et al. Laboratory measurements of HDO/H2O isotopic fractionation during ice deposition in simulated cirrus clouds[J]. PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA,2017,114(22):5612-5617. |
APA | Lamb, Kara D..,Clouser, Benjamin W..,Bolot, Maximilien.,Sarkozy, Laszlo.,Ebert, Volker.,...&Moyer, Elisabeth 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),5612-5617. |
MLA | Lamb, Kara 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):5612-5617. |
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