Fifth-order Raman spectrum of an atomic liquid: Simulation and instantaneous-normal-mode calculation

被引：85

作者：

Ma, A ^{[1
]}

Stratt, RM ^{[1
]}

机构：

[1] Brown Univ, Dept Chem, Providence, RI 02912 USA

来源：

PHYSICAL REVIEW LETTERS | 2000年 / 85卷 / 05期

关键词：

D O I：

10.1103/PhysRevLett.85.1004

中图分类号：

O4 [物理学];

学科分类号：

0702 ;

摘要：

Experimental artifacts and technical difficulties in carrying out theoretical calculations have consistently frustrated attempts to obtain the two-dimensional (5th-order) Raman spectrum of a liquid. We report here a new theoretical development: the first microscopic numerical simulation of the 5th-order Raman signal in a liquid. Comparison with an instantaneous-normal-mode treatment, a fully microscopic model which interprets liquid dynamics as arising from coherent harmonic modes, shows that the 5th-order spectrum reveals profound effects stemming from dynamical anharmonicity.

引用

页码：1004 / 1007

页数：4

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