Terahertz-field-induced second-harmonic generation measurements of liquid dynamics

被引:102
作者
Cook, DJ [1 ]
Chen, JX [1 ]
Morlino, EA [1 ]
Hochstrasser, RM [1 ]
机构
[1] Univ Penn, Dept Chem, Philadelphia, PA 19104 USA
基金
美国国家卫生研究院; 美国国家科学基金会;
关键词
D O I
10.1016/S0009-2614(99)00668-5
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
A new third-order non-linear THz pump-optical probe measurement of liquid dynamics is reported. Terahertz-field-induced second-harmonic generation (TFISH) measures the correlations between the hyperpolarizability and dipole moment fluctuations at equilibrium. This method is analyzed in the Born-Oppenheimer approximation, and is shown to measure diffusive orientational dynamics as [P-1(cos theta)]. Measurements of water and acetonitrile yield relaxation time constants of 13 and 9.6 ps, respectively. Signals were also obtained from thin polymer films and surfaces, suggesting a number of applications for this method. (C) 1999 Elsevier Science B.V. All rights reserved.
引用
收藏
页码:221 / 228
页数:8
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