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Title: Interfacing the Ab initio multiple spawning method with electronic structure methods in GAMESS: Photodecay of trans-Azomethane

Abstract

This work presents a nonadiabatic molecular dynamics study of the nonradiative decay of photoexcited trans-azomethane, using the ab initio multiple spawning (AIMS) program that has been interfaced with the General Atomic and Molecular Electronic Structure System (GAMESS) quantum chemistry package for on-the-fly electronic structure evaluation. The interface strategy is discussed, and the capabilities of the combined programs are demonstrated with a nonadiabatic molecular dynamics study of the nonradiative decay of photoexcited trans-azomethane. Energies, gradients, and nonadiabatic coupling matrix elements were obtained with the state-averaged complete active space self-consistent field method, as implemented in GAMESS. The influence of initial vibrational excitation on the outcome of the photoinduced isomerization is explored. Increased vibrational excitation in the CNNC torsional mode shortens the excited state lifetime. Depending on the degree of vibrational excitation, the excited state lifetime varies from ~60–200 fs. As a result, these short lifetimes are in agreement with time-resolved photoionization mass spectroscopy experiments.

Authors:
 [1];  [2];  [3];  [4];  [1]
+ Show Author Affiliations
  1. Ames Laboratory (AMES), Ames, IA (United States); Iowa State Univ., Ames, IA (United States)
  2. Univ. of Pittsburgh, Pittsburgh, PA (United States)
  3. Univ. of Nevada, Reno, NV (United States)
  4. Stanford Univ., Stanford, CA (United States)
Publication Date:
Research Org.:
Ames Laboratory (AMES), Ames, IA (United States)
Sponsoring Org.:
USDOE
OSTI Identifier:
1233235
Report Number(s):
IS-J-8543
Journal ID: ISSN 1089-5639
Grant/Contract Number:  
AC02-07CH11358
Resource Type:
Accepted Manuscript
Journal Name:
Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory
Additional Journal Information:
Journal Volume: 118; Journal Issue: 46; Journal ID: ISSN 1089-5639
Publisher:
American Chemical Society
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY

Citation Formats

Gaenko, Alexander, DeFusco, Albert, Varganov, Sergey A., Martínez, Todd J., and Gordon, Mark S. Interfacing the Ab initio multiple spawning method with electronic structure methods in GAMESS: Photodecay of trans-Azomethane. United States: N. p., 2014. Web. doi:10.1021/jp508242j.
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Gaenko, Alexander, DeFusco, Albert, Varganov, Sergey A., Martínez, Todd J., & Gordon, Mark S. Interfacing the Ab initio multiple spawning method with electronic structure methods in GAMESS: Photodecay of trans-Azomethane. United States. https://doi.org/10.1021/jp508242j
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Gaenko, Alexander, DeFusco, Albert, Varganov, Sergey A., Martínez, Todd J., and Gordon, Mark S. Mon . "Interfacing the Ab initio multiple spawning method with electronic structure methods in GAMESS: Photodecay of trans-Azomethane". United States. https://doi.org/10.1021/jp508242j. https://www.osti.gov/servlets/purl/1233235.
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@article{osti_1233235,
title = {Interfacing the Ab initio multiple spawning method with electronic structure methods in GAMESS: Photodecay of trans-Azomethane},
author = {Gaenko, Alexander and DeFusco, Albert and Varganov, Sergey A. and Martínez, Todd J. and Gordon, Mark S.},
abstractNote = {This work presents a nonadiabatic molecular dynamics study of the nonradiative decay of photoexcited trans-azomethane, using the ab initio multiple spawning (AIMS) program that has been interfaced with the General Atomic and Molecular Electronic Structure System (GAMESS) quantum chemistry package for on-the-fly electronic structure evaluation. The interface strategy is discussed, and the capabilities of the combined programs are demonstrated with a nonadiabatic molecular dynamics study of the nonradiative decay of photoexcited trans-azomethane. Energies, gradients, and nonadiabatic coupling matrix elements were obtained with the state-averaged complete active space self-consistent field method, as implemented in GAMESS. The influence of initial vibrational excitation on the outcome of the photoinduced isomerization is explored. Increased vibrational excitation in the CNNC torsional mode shortens the excited state lifetime. Depending on the degree of vibrational excitation, the excited state lifetime varies from ~60–200 fs. As a result, these short lifetimes are in agreement with time-resolved photoionization mass spectroscopy experiments.},
doi = {10.1021/jp508242j},
journal = {Journal of Physical Chemistry. A, Molecules, Spectroscopy, Kinetics, Environment, and General Theory},
number = 46,
volume = 118,
place = {United States},
year = {Mon Oct 20 00:00:00 EDT 2014},
month = {Mon Oct 20 00:00:00 EDT 2014}
}
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https://doi.org/10.1021/jp508242j
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