Molecular response properties from explicitly time-dependent configuration interaction methods.
Molecular response properties from explicitly time-dependent configuration interaction methods.
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来自明确时间依赖性构型相互作用方法的分子响应特性。
DOI：
10.1063/1.2749503
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发表时间：
2007
期刊：
影响因子：
--
通讯作者：
P. Saalfrank
中科院分区：
文献类型：
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作者：
Pascal Krause;T. Klamroth;P. Saalfrank
本文报道了用显式含时组态相互作用（TD-CI）方法计算分子的电响应性质。这些方法的优点是适用于任意形状和强度的含时扰动（在含时薛定谔方程的限制范围内）。用三种方法求解含时电子薛定谔方程，即TD-CIS（只包含单激发）、TD-CISD（包含单激发和双激发）和TD-CIS（D）（单激发和双激发的微扰处理）方法，并应用于小分子H（2）和H（2）O的计算。在计算中，缓慢变化的非共振电场施加到分子和线性（极化率）和非线性（超极化率，谐波产生）的响应特性从随时间变化的偶极矩。
In this paper we report the calculation of molecular electric response properties with the help of explicitly time-dependent configuration interaction (TD-CI) methods. These methods have the advantage of being applicable (within the limitations of the time-dependent Schrodinger equation) to time-dependent perturbations of arbitrary shape and strength. Three variants are used to solve the time-dependent electronic Schrodinger equation, namely, the TD-CIS (inclusion of single excitations only), TD-CISD (inclusion of single and double excitations), and TD-CIS(D) (single excitations and perturbative treatment of double excitations) methods and applied for illustration to small molecules, H(2) and H(2)O. In the calculation, slowly varying off-resonant electric fields are applied to the molecules and linear (polarizabilities) and nonlinear (hyperpolarizabilities, harmonic generation) response properties are determined from the time-dependent dipole moments.