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First-order nonadiabatic couplings in extended systems by time-dependent density functional theory

We propose an ab initio formulation that enables a rigorous calculation of the first-order nonadiabatic couplings (NAC) between electronic states based on time-dependent density functional theory in conjunction with planewave bases, projector augmented-wave pseudopotentials, and hybrid exchange-corr... Full description

Journal Title: The Journal of Chemical Physics 28 December 2018, Vol.149(24)
Main Author: Zhang, Xu
Other Authors: Lu, Gang
Format: Electronic Article Electronic Article
Language: English
Subjects:
ID: ISSN: 0021-9606 ; E-ISSN: 1089-7690 ; DOI: 10.1063/1.5065504
Link: http://dx.doi.org/10.1063/1.5065504
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recordid: aip_complete10.1063/1.5065504
title: First-order nonadiabatic couplings in extended systems by time-dependent density functional theory
format: Article
creator:
  • Zhang, Xu
  • Lu, Gang
subjects:
  • Articles
ispartof: The Journal of Chemical Physics, 28 December 2018, Vol.149(24)
description: We propose an ab initio formulation that enables a rigorous calculation of the first-order nonadiabatic couplings (NAC) between electronic states based on time-dependent density functional theory in conjunction with planewave bases, projector augmented-wave pseudopotentials, and hybrid exchange-correlation functionals. The linear and quadratic time-dependent response theory is used to derive analytic expressions for the NAC matrix elements. In contrast to the previous formulation in atomic basis sets, the present formulation eliminates explicit references to Kohn-Sham virtual orbitals. With the introduction of Lagrangian functionals, the present formulation circumvents expensive derivative calculations of Kohn-Sham orbitals with respect to ionic coordinates. As a validation of the formulation, the NAC matrix elements of small molecules LiH and HeH + are calculated and compared to previous results with the atomic orbital basis. This development paves the way for accurate ab initio nonadiabatic molecular dynamics in extended systems.
language: eng
source:
identifier: ISSN: 0021-9606 ; E-ISSN: 1089-7690 ; DOI: 10.1063/1.5065504
fulltext: fulltext
issn:
  • 0021-9606
  • 1089-7690
  • 00219606
  • 10897690
url: Link


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descriptionWe propose an ab initio formulation that enables a rigorous calculation of the first-order nonadiabatic couplings (NAC) between electronic states based on time-dependent density functional theory in conjunction with planewave bases, projector augmented-wave pseudopotentials, and hybrid exchange-correlation functionals. The linear and quadratic time-dependent response theory is used to derive analytic expressions for the NAC matrix elements. In contrast to the previous formulation in atomic basis sets, the present formulation eliminates explicit references to Kohn-Sham virtual orbitals. With the introduction of Lagrangian functionals, the present formulation circumvents expensive derivative calculations of Kohn-Sham orbitals with respect to ionic coordinates. As a validation of the formulation, the NAC matrix elements of small molecules LiH and HeH + are calculated and compared to previous results with the atomic orbital basis. This development paves the way for accurate ab initio nonadiabatic molecular dynamics in extended systems.
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descriptionWe propose an ab initio formulation that enables a rigorous calculation of the first-order nonadiabatic couplings (NAC) between electronic states based on time-dependent density functional theory in conjunction with planewave bases, projector augmented-wave pseudopotentials, and hybrid exchange-correlation functionals. The linear and quadratic time-dependent response theory is used to derive analytic expressions for the NAC matrix elements. In contrast to the previous formulation in atomic basis sets, the present formulation eliminates explicit references to Kohn-Sham virtual orbitals. With the introduction of Lagrangian functionals, the present formulation circumvents expensive derivative calculations of Kohn-Sham orbitals with respect to ionic coordinates. As a validation of the formulation, the NAC matrix elements of small molecules LiH and HeH + are calculated and compared to previous results with the atomic orbital basis. This development paves the way for accurate ab initio nonadiabatic molecular dynamics in extended systems.
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abstractWe propose an ab initio formulation that enables a rigorous calculation of the first-order nonadiabatic couplings (NAC) between electronic states based on time-dependent density functional theory in conjunction with planewave bases, projector augmented-wave pseudopotentials, and hybrid exchange-correlation functionals. The linear and quadratic time-dependent response theory is used to derive analytic expressions for the NAC matrix elements. In contrast to the previous formulation in atomic basis sets, the present formulation eliminates explicit references to Kohn-Sham virtual orbitals. With the introduction of Lagrangian functionals, the present formulation circumvents expensive derivative calculations of Kohn-Sham orbitals with respect to ionic coordinates. As a validation of the formulation, the NAC matrix elements of small molecules LiH and HeH + are calculated and compared to previous results with the atomic orbital basis. This development paves the way for accurate ab initio nonadiabatic molecular dynamics in extended systems.
pubAIP Publishing LLC
doi10.1063/1.5065504
pages244103
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date2018-12-28