伪谱方法中解析非绝热导数耦合的高效实现。

Highly efficient implementation of analytic nonadiabatic derivative couplings within the pseudospectral method.

作者信息

Cao Yixiang, Halls Mathew D, Friesner Richard A

机构信息

Schrödinger Inc., 1540 Broadway, 24th Floor, New York, New York 10036, USA.

Schrödinger Inc., 9868 Scranton, Suite 3200, San Diego, California 92121, USA.

出版信息

J Chem Phys. 2024 Feb 28;160(8). doi: 10.1063/5.0188277.

DOI:10.1063/5.0188277

PMID:38385510

Abstract

A pseudospectral implementation of nonadiabatic derivative couplings in the Tamm-Dancoff approximation is reported, and the accuracy and efficiency of the pseudospectral nonadiabatic derivative couplings are studied. Our results demonstrate that the pseudospectral method provides mean absolute errors of 0.2%-1.9%, while providing a significant speedup. Benchmark calculations on fullerenes (Cn, n up to 100) using B3LYP achieved 10- to 15-fold, 8- to 17-fold, and 43- to 75-fold speedups for 6-31G**, 6-31++G**, and cc-pVTZ basis sets, respectively, when compared to the conventional spectral method.

摘要

报道了在Tamm-Dancoff近似下非绝热导数耦合的拟谱实现，并研究了拟谱非绝热导数耦合的准确性和效率。我们的结果表明，拟谱方法提供了0.2%-1.9%的平均绝对误差，同时显著提高了速度。与传统谱方法相比，使用B3LYP对富勒烯（Cn，n高达100）进行基准计算时，对于6-31G**、6-31++G**和cc-pVTZ基组，分别实现了10至15倍、8至17倍和43至75倍的加速。