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Title: An atomic orbital-based formulation of analytical gradients and nonadiabatic coupling vector elements for the state-averaged complete active space self-consistent field method on graphical processing units

Abstract

We recently presented an algorithm for state-averaged complete active space self-consistent field (SA-CASSCF) orbital optimization that capitalizes on sparsity in the atomic orbital basis set to reduce the scaling of computational effort with respect to molecular size. Here, we extend those algorithms to calculate the analytic gradient and nonadiabatic coupling vectors for SA-CASSCF. Combining the low computational scaling with acceleration from graphical processing units allows us to perform SA-CASSCF geometry optimizations for molecules with more than 1000 atoms. The new approach will make minimal energy conical intersection searches and nonadiabatic dynamics routine for molecular systems with O(10{sup 2}) atoms.

Authors:
; ;
Publication Date:
OSTI Identifier:
22493123
Resource Type:
Journal Article
Journal Name:
Journal of Chemical Physics
Additional Journal Information:
Journal Volume: 143; Journal Issue: 15; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA); Journal ID: ISSN 0021-9606
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ALGORITHMS; ATOMS; COUPLING; MOLECULES; SELF-CONSISTENT FIELD; VECTORS

Citation Formats

Snyder, James W., Hohenstein, Edward G., Luehr, Nathan, Martínez, Todd J., E-mail: toddjmartinez@gmail.com, and SLAC National Accelerator Laboratory, Menlo Park, California 94025. An atomic orbital-based formulation of analytical gradients and nonadiabatic coupling vector elements for the state-averaged complete active space self-consistent field method on graphical processing units. United States: N. p., 2015. Web. doi:10.1063/1.4932613.
Snyder, James W., Hohenstein, Edward G., Luehr, Nathan, Martínez, Todd J., E-mail: toddjmartinez@gmail.com, & SLAC National Accelerator Laboratory, Menlo Park, California 94025. An atomic orbital-based formulation of analytical gradients and nonadiabatic coupling vector elements for the state-averaged complete active space self-consistent field method on graphical processing units. United States. https://doi.org/10.1063/1.4932613
Snyder, James W., Hohenstein, Edward G., Luehr, Nathan, Martínez, Todd J., E-mail: toddjmartinez@gmail.com, and SLAC National Accelerator Laboratory, Menlo Park, California 94025. 2015. "An atomic orbital-based formulation of analytical gradients and nonadiabatic coupling vector elements for the state-averaged complete active space self-consistent field method on graphical processing units". United States. https://doi.org/10.1063/1.4932613.
@article{osti_22493123,
title = {An atomic orbital-based formulation of analytical gradients and nonadiabatic coupling vector elements for the state-averaged complete active space self-consistent field method on graphical processing units},
author = {Snyder, James W. and Hohenstein, Edward G. and Luehr, Nathan and Martínez, Todd J., E-mail: toddjmartinez@gmail.com and SLAC National Accelerator Laboratory, Menlo Park, California 94025},
abstractNote = {We recently presented an algorithm for state-averaged complete active space self-consistent field (SA-CASSCF) orbital optimization that capitalizes on sparsity in the atomic orbital basis set to reduce the scaling of computational effort with respect to molecular size. Here, we extend those algorithms to calculate the analytic gradient and nonadiabatic coupling vectors for SA-CASSCF. Combining the low computational scaling with acceleration from graphical processing units allows us to perform SA-CASSCF geometry optimizations for molecules with more than 1000 atoms. The new approach will make minimal energy conical intersection searches and nonadiabatic dynamics routine for molecular systems with O(10{sup 2}) atoms.},
doi = {10.1063/1.4932613},
url = {https://www.osti.gov/biblio/22493123}, journal = {Journal of Chemical Physics},
issn = {0021-9606},
number = 15,
volume = 143,
place = {United States},
year = {Wed Oct 21 00:00:00 EDT 2015},
month = {Wed Oct 21 00:00:00 EDT 2015}
}