GPU-Accelerated State-Averaged Complete Active Space Self-Consistent Field Interfaced with Ab Initio Multiple Spawning Unravels the Photodynamics of Provitamin D3

James W. Snyder, Basile F E Curchod, Todd J. Martínez*

*Corresponding author for this work

Research output: Contribution to journalArticle (Academic Journal)

33 Citations (Scopus)

Abstract

Excited-state molecular dynamics is essential to the study of photochemical reactions, which occur under nonequilibrium conditions. However, the computational cost of such simulations has often dictated compromises between accuracy and efficiency. The need for an accurate description of both the molecular electronic structure and nuclear dynamics has historically stymied the simulation of medium- to large-size molecular systems. Here, we show how to alleviate this problem by combining ab initio multiple spawning (AIMS) for the nuclear dynamics and GPU-accelerated state-averaged complete active space self-consistent field (SA-CASSCF) for the electronic structure. We demonstrate the new approach by first-principles SA-CASSCF/AIMS nonadiabatic dynamics simulation of photoinduced electrocyclic ring-opening in the 51-atom provitamin D3 molecule.

Original languageEnglish
Pages (from-to)2444-2449
Number of pages6
JournalJournal of Physical Chemistry Letters
Volume7
Issue number13
DOIs
Publication statusPublished - 7 Jul 2016

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