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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. and Curchod, Basile F. E. and Martinez, Todd 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). pp. 2444-2449.

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.

Item Type:Article
Full text:(AM) Accepted Manuscript
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Status:Peer-reviewed
Publisher Web site:https://doi.org/10.1021/acs.jpclett.6b00970
Publisher 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.
Date accepted:07 June 2016
Date deposited:08 December 2017
Date of first online publication:16 June 2016
Date first made open access:08 December 2017

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