Accelerating convergence of equation-of-motion coupled-cluster computations using the semi-stochastic CC( P ; Q ) formalism
Accelerating convergence of equation-of-motion coupled-cluster computations using the semi-stochastic CC( P ; Q ) formalism
复制标题
使用半随机 CC( P ; Q ) 形式加速运动方程耦合簇计算的收敛
DOI：
10.1080/00268976.2020.1817592
复制
发表时间：
2020
影响因子：
1.7
通讯作者：
Piecuch, Piotr
中科院分区：
文献类型：
--
作者：
Yuwono, Stephen H.;Chakraborty, Arnab;Emiliano Deustua, J.;Shen, Jun;Piecuch, Piotr
最近提出的计算激发电子态的方法，其中确定性运动方程耦合团簇(EOMCC)框架与随机组态相互作用量子蒙特卡罗(CIQMC)计算相结合[J.E.Deustuaet等人，J.Chem.Phys.150,111101(2019年)]，与从CC(P；Q)形式导出的非迭代能量校正相结合。通过研究平衡状态下CH+中的垂直激发，以及CH和CnC中的伸展几何结构和绝热激发，我们证明了所得到的半随机CC(P；Q)方法在CIQMC传播的早期阶段收敛于目标高能级能级，在本研究中用EOMCC方法表示为单、双和三重。
The recently proposed approach to excited electronic states, in which the deterministic equation-of-motion coupled-cluster (EOMCC) framework is merged with stochastic configuration interaction Quantum Monte Carlo (CIQMC) computations [J.E. Deustuaet al., J. Chem. Phys.150, 111101 (2019)], is combined with the noniterative energy corrections derived from the CC(P;Q) formalism. By examining vertical excitations in CH+at the equilibrium and stretched geometries and adiabatic excitations in CH and CNC, we demonstrate that the resulting semi-stochastic CC(P;Q) methodology converges target high-level energetics, represented in this study by the EOMCC method with singles, doubles, and triples, in the early stages of CIQMC propagations.