用于计算时间分辨和频率分辨四波混频信号的高效方法及其在光子回波光谱学中的应用。

Efficient method for the calculation of time- and frequency-resolved four-wave mixing signals and its application to photon-echo spectroscopy.

作者信息

Gelin Maxim F, Egorova Dassia, Domcke Wolfgang

机构信息

Department of Chemistry, Technical University of Munich, D-85747 Garching, Germany.

出版信息

J Chem Phys. 2005 Oct 22;123(16):164112. doi: 10.1063/1.2062188.

DOI:10.1063/1.2062188

PMID:16268686

Abstract

An efficient method has been developed for the calculation of third-order time- and frequency-resolved optical signals. To obtain the general four-wave mixing signal, seven auxiliary density matrices have to be propagated in time. For the special cases of two-pulse photon-echo and transient-grating signals, two or three density matrices, respectively, are required. The method is limited to weak laser fields (it is thus valid within the third-order perturbation theory) but allows for any pulse durations and automatically accounts for pulse-overlap effects. To illustrate the method, we present the explicit derivation of the three-pulse photon-echo signal. Any other third-order optical signal can be calculated in the same manner. As an example, two- and three-pulse photon-echo and transient-grating signals for a weakly damped displaced harmonic oscillator have been calculated.

摘要

已经开发出一种用于计算三阶时间和频率分辨光信号的有效方法。为了获得一般的四波混频信号，必须及时传播七个辅助密度矩阵。对于双脉冲光子回波和瞬态光栅信号的特殊情况，分别需要两个或三个密度矩阵。该方法限于弱激光场（因此在三阶微扰理论内有效），但允许任何脉冲持续时间，并自动考虑脉冲重叠效应。为了说明该方法，我们给出了三脉冲光子回波信号的显式推导。任何其他三阶光信号都可以以相同的方式计算。作为一个例子，已经计算了弱阻尼位移谐振子的双脉冲和三脉冲光子回波以及瞬态光栅信号。