期刊
JOURNAL OF PHYSICAL CHEMISTRY C
卷 117, 期 6, 页码 2944-2951出版社
AMER CHEMICAL SOC
DOI: 10.1021/jp311986m
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资金
- Oxford University Clarendon Fund
- St. Edmund Hall
- European Commission (Marie Curie IEF) [PIEF-GA-2010-272402]
- Wolfson Foundation
- Royal Society
Isotope fractionation between different phases is a subtle but very important phenomenon that is related to the quantum nature of light nuclei, and that has important consequences for geochemistry, hydrology, and biology. Here we present a joint experimental/theoretical investigation of the differential segregation of hydrogen and deuterium at the liquid/vapor interface of mixtures of light and heavy water. We use both vibrational sum-frequency spectroscopy and path integral molecular dynamics simulations to quantitatively assess this phenomenon. The experimental and theoretical results indicate that the last layer of water molecules at the liquid/vapor interface is enriched in hydrogen. We discuss in detail the extent, the physical origin, and the implications of this surface-specific isotope effect.
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