Optical response functions with semiclassical dynamics

Optical response functions with semiclassical dynamics
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半经典动力学的光学响应函数

DOI:
10.1063/1.1577319
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发表时间:
2003
影响因子:
4.4
通讯作者:
Roger F Loring
Roger F Loring
中科院分区:
化学2区
文献类型:
--
作者:
W. Noid;G. S. Ezra;Roger F Loring

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非线性光谱测量中的可观测值可以根据响应函数计算,其形式为涉及控制辐射-物质相互作用的算子的嵌套换向器的平均值。我们提出了光学非线性响应函数的半经典公式,采用 Herman-Kluk 冻结高斯近似来表示相干态表示中的量子传播器。这种半经典近似允许根据经典轨迹和稳定性矩阵计算响应函数,并提供对经典力学和量子力学中非线性响应之间关系的深入了解。非简谐振子的线性响应计算表明,半经典方法再现了量子结果和经典结果之间的显着差异。
Observables in nonlinear spectroscopic measurements may be calculated from response functions, which have the form of averages of nested commutators involving the operator governing the radiation–matter interaction. We present a semiclassical formulation of the optical nonlinear response function, employing the Herman–Kluk frozen Gaussian approximation to the quantum propagator in the coherent states representation. This semiclassical approximation permits the response function to be computed from classical trajectories and stability matrices, and provides insight into the relationship between nonlinear response in classical and quantum mechanics. Linear response calculations for an anharmonic oscillator illustrate that the semiclassical approach reproduces the significant differences between quantum and classical results.
DOI: 10.1016/s0006-3495(02)75669-5
发表时间: 2002-06-01
影响因子: 3.4
作者:
Merchant, KA;Thompson, DE;Fayer, MD
通讯作者: Fayer, MD