GPU-Accelerated State-Averaged Complete Active Space Self-Consistent Field Interfaced with Ab Initio Multiple Spawning Unravels the Photodynamics of Provitamin D-3

Snyder Jr., James W.; Curchod, Basile F.E.; Martinez, Todd J.

doi:10.1021/acs.jpclett.6b00970

GPU-Accelerated State-Averaged Complete Active Space Self-Consistent Field Interfaced with Ab Initio Multiple Spawning Unravels the Photodynamics of Provitamin D-3

Snyder Jr., James W.; Curchod, Basile F.E.; Martinez, Todd J.

Authors

James W. Snyder Jr.

Dr Basile Curchod basile.f.curchod@durham.ac.uk
Academic Visitor

Todd J. Martinez

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.

Citation

Snyder Jr., J. W., Curchod, B. F., & Martinez, T. J. (2016). GPU-Accelerated State-Averaged Complete Active Space Self-Consistent Field Interfaced with Ab Initio Multiple Spawning Unravels the Photodynamics of Provitamin D-3. Journal of Physical Chemistry Letters, 7(13), 2444-2449. https://doi.org/10.1021/acs.jpclett.6b00970

Journal Article Type	Article
Acceptance Date	Jun 7, 2016
Online Publication Date	Jun 16, 2016
Publication Date	Jul 7, 2016
Deposit Date	Nov 6, 2017
Publicly Available Date	Dec 8, 2017
Journal	Journal of Physical Chemistry Letters
Publisher	American Chemical Society
Peer Reviewed	Peer Reviewed
Volume	7
Issue	13
Pages	2444-2449
DOI	https://doi.org/10.1021/acs.jpclett.6b00970

Files

Accepted Journal Article (3.9 Mb)
PDF

Copyright Statement
This document is the Accepted Manuscript version of a Published Work that appeared in final form in Journal of Physical Chemistry Letters, copyright © American Chemical Society after peer review and technical editing by the publisher. To access the final edited and published work see https://doi.org/10.1021/acs.jpclett.6b00970.