激发态
可见的
系统间交叉
波函数
密度泛函理论
单重态
物理
化学
联轴节(管道)
基态
自旋(空气动力学)
分子轨道
自旋轨道相互作用
原子物理学
计算化学
量子力学
材料科学
分子
冶金
热力学
作者
Momir Mališ,Eva Vandaele,Sandra Luber
标识
DOI:10.1021/acs.jctc.1c01046
摘要
A procedure for the calculation of spin-orbit coupling (SOC) at the delta self-consistent field (ΔSCF) level of theory is presented. Singlet and triplet excited electronic states obtained with the ΔSCF method are expanded into a linear combination of singly excited Slater determinants composed of ground electronic state Kohn-Sham orbitals. This alleviates the nonorthogonality between excited and ground electronic states and introduces a framework, similar to the auxiliary wave function at the time-dependent density functional theory (TD-DFT) level, for the calculation of observables. The ΔSCF observables of the formaldehyde system were compared to reference TD-DFT values. Our procedure gives all components (energies, gradients, nonadiabatic couplings, and SOC terms) at the ΔSCF level of theory for conducting efficient, full-atomistic nonadiabatic molecular dynamics with intersystem crossing, particularly in condensed phase systems.
科研通智能强力驱动
Strongly Powered by AbleSci AI