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

Yixiang Cao; Mathew D Halls; Richard A Friesner

doi:10.1063/5.0188277

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

J Chem Phys. 2024 Feb 28;160(8):084106. doi: 10.1063/5.0188277.

Authors

Yixiang Cao¹, Mathew D Halls², Richard A Friesner³

Affiliations

¹ Schrödinger Inc., 1540 Broadway, 24th Floor, New York, New York 10036, USA.
² Schrödinger Inc., 9868 Scranton, Suite 3200, San Diego, California 92121, USA.
³ Department of Chemistry, Columbia University, New York, New York 10027, USA.

PMID: 38385510
DOI: 10.1063/5.0188277

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.