Reduced Near-Resonant Vibrational Coupling at the Surfaces of Liquid Water and Ice

被引:25
作者
Smit, Wilbert J. [1 ,3 ]
Versluis, Jan [1 ]
Backus, Ellen H. G. [2 ]
Bonn, Mischa [2 ]
Bakker, Huib J. [1 ]
机构
[1] AMOLF, Sci Pk 104, NL-1098 XG Amsterdam, Netherlands
[2] Max Planck Inst Polymer Res, Ackermannweg 10, D-55128 Mainz, Germany
[3] PSL Res Univ, ESPCI Paris, UMR CBI 8231, 10 Rue Vauquelin, F-75005 Paris, France
关键词
FREQUENCY GENERATION SPECTROSCOPY; AIR INTERFACE; CONSEQUENCES; ORIENTATION; H2O; D2O;
D O I
10.1021/acs.jpclett.7b03359
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
We study the resonant interaction of the OH stretch vibrations of water molecules at the surfaces of liquid water and ice using heterodyne-detected sum-frequency generation (HD-SFG) spectroscopy. By studying different isotopic mixtures of H2O and D2O, we vary the strength of the interaction, and we monitor the resulting effect on the HD-SFG spectrum of the OH stretch vibrations. We observe that the near-resonant coupling effects are weaker at the surface than in the bulk, for both water and ice, indicating that for both phases of water the OH vibrations are less strongly delocalized at the surface than in the bulk.
引用
收藏
页码:1290 / 1294
页数:9
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