Theoretical study on surface vibrational infrared-visible sum-frequency generation spectroscopy applied to adsorbed molecules

被引:14
作者
Kato, T
Hayashi, M
Villaeys, AA
Lin, SH
机构
[1] ACAD SINICA, INST ATOM & MOL SCI, TAIPEI 106, TAIWAN
[2] INST PHYS & CHIM MAT STRASBOURG, F-67037 STRASBOURG, FRANCE
[3] UNIV STRASBOURG 1, F-67037 STRASBOURG, FRANCE
来源
PHYSICAL REVIEW A | 1997年 / 56卷 / 01期
关键词
D O I
10.1103/PhysRevA.56.980
中图分类号
O43 [光学];
学科分类号
070207 ; 0803 ;
摘要
A comprehensive theory of sum-frequency generation (SFG) spectroscopies with infrared pump and infrared-visible probe is presented in a systematic way based on the Markovian master equation approach. A description of SFG as a five-wave mixing process is given by using a perturbation theory for both the stationary and time-resolved experiments. A criterion for the validity of the perturbation treatment is also presented in terms of the saturation parameter. Simple expressions are derived by introducing the rotating-wave approximation for a four-level model system of the adsorbed molecule. It is shown that the fourth-order induced nonlinear polarization at the SF can be expressed as a sum of three components which are induced by different field-molecule interactions. Numerical calculations for the recent experimental results of the SFG spectroscopy applied to C-H stretch modes on the hydrogen-terminated H/C(111) (1 x 1) surface are performed to show the applicability of our expressions as well.
引用
收藏
页码:980 / 993
页数:14
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