Rehn Dirk R, Dreuw Andreas
Interdisciplinary Center for Scientific Computing and Physical-Chemistry Institute, Ruprecht-Karls University, Im Neuenheimer Feld 205, 69120 Heidelberg, Germany.
J Chem Phys. 2019 May 7;150(17):174110. doi: 10.1063/1.5085117.
Analytic gradient expressions for the algebraic diagrammatic construction (ADC) scheme for the polarization propagator up to third order are derived using a Lagrangian approach. An implementation within the Q-CHEM electronic structure package for excited-state nuclear gradients of the ADC(2), ADC(2)-x, and ADC(3) models based on restricted and unrestricted Hartree-Fock references is presented. Details of the implementation and the applicability of the newly derived gradients for geometry optimizations and the quality of the resulting structures are discussed.
利用拉格朗日方法推导了极化传播子的代数图解构造（ADC）方案直至三阶的解析梯度表达式。介绍了在Q-CHEM电子结构软件包中基于受限和非受限Hartree-Fock参考对ADC(2)、ADC(2)-x和ADC(3)模型的激发态核梯度的实现。讨论了实现细节以及新推导的梯度在几何优化中的适用性和所得结构的质量。
