# Non-adiabatic excited-state time-dependent <i>GW</i> molecular dynamics (TD<i>GW</i>) satisfying extended Koopmans’ theorem: An accurate description of methane photolysis

https://mdr.nims.go.jp/datasets/b3b036ee-95b4-433c-b531-740a0efb3f39

## File

- [JChemPhys160(2024)184102.pdf](https://mdr.nims.go.jp/filesets/119c4e1e-3e82-44ac-9f61-cb8e57dae12b/download) ([Detail](https://mdr.nims.go.jp/filesets/119c4e1e-3e82-44ac-9f61-cb8e57dae12b.md))

## Id

b3b036ee-95b4-433c-b531-740a0efb3f39

## Local identifier



## Visibility

open_to_public

## State

published

## Created at

2024-06-03T01:27:25.538107Z

## Updated at

2025-05-13T23:30:07.720331Z

## Published at

2025-05-13T23:19:52.659448Z

## Doi



## First published url

https://doi.org/10.1063/5.0202590

## Date published

2024-05-14

## Recorded date published

2024-5-14

## Resource type

journal_article

## Manuscript type

vor

## Collection



## Title

- title: 'Non-adiabatic excited-state time-dependent <i>GW</i> molecular dynamics
    (TD<i>GW</i>) satisfying extended Koopmans’ theorem: An accurate description of
    methane photolysis'
  title_type: original
  lang: en

## Description

- description: There is a longstanding difficulty that time-dependent density functional
    theory relying on adiabatic local density approximation is not applicable to the
    electron dynamics, for example, for an initially excited state, such as in photochemical
    reactions. To overcome this, we develop non-adiabatic excited-state time-dependent
    <i>GW</i> molecular dynamics (TD<i>GW</i>) on the basis of the extended quasiparticle
    theory. Replacing Kohn–Sham orbitals/energies with correlated, interacting quasiparticle
    orbitals/energies allows the full correspondence to the excited-state surfaces
    and corresponding total energies, with satisfying extended Koopmans’ theorem.
    We demonstrate the power of TD<i>GW</i>using methane photolysis, CH<sub>4 </sub>→
    CH<sub>3</sub><sup>●</sup> + H, an important initiation reaction for combustion/pyrolysis
    and hydrogen production of methane. We successfully explore several possible pathways
    and show how this reaction dynamics is captured accurately through simultaneously
    time-tracing all quasiparticle levels. TD<i>GW</i> scales as O(N<sub>B</sub><sup>3-4</sup>),
    where <i>N</i><sub>B</sub> is the number of basis functions, which is distinctly
    advantageous to performing dynamics using configuration interaction and coupled
    cluster methods.
  description_type: abstract
  lang: und

## Creator

- name: Aaditya Manjanath
  role: author
  orcid: https://orcid.org/0000-0003-2223-5954
  organization: National Institute for Materials Science
  ror: https://ror.org/026v1ze26
- name: Ryoji Sahara
  role: author
  orcid: https://orcid.org/0000-0003-0788-2985
  organization: National Institute for Materials Science
  ror: https://ror.org/026v1ze26
- name: Kaoru Ohno
  role: author
  orcid: https://orcid.org/0000-0002-1980-5971
- name: Yoshiyuki Kawazoe
  role: author

## Contact agent



## Publisher

organization: AIP Publishing

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## Keyword

- subject: Molecular dynamics
  schema: not_defined
- subject: Methane photolysis
  schema: not_defined
- subject: Excited states
  schema: not_defined
- subject: time-dependent density functional theory
  schema: not_defined
- subject: GW approximation
  schema: not_defined

## Rights

- description: This article may be downloaded for personal use only. Any other use
    requires prior permission of the author and AIP Publishing. This article appeared
    in Aaditya Manjanath et al., J. Chem. Phys. 160, 184102 (2024) and may be found
    at https://doi.org/10.1063/5.0202590
  identifier: http://rightsstatements.org/vocab/InC/1.0/

## Other identifier(s)



## Data origin

- data_origin_type: other

## Embargo

start_date: 2024-05-14
end_date: 2025-05-14

## Journal

- title: The Journal of Chemical Physics
  issn: '00219606'
  volume: '160'
  issue: '18'
  article_number: '184102'

## Conference



## Related item



## Funding

- identifier: 19S0501
  funder_name: Institute for Materials Research, Tohoku University
- identifier: 20S0505
  funder_name: Institute for Materials Research, Tohoku University
- identifier: 202308-SCKGE-0216
  funder_name: Institute for Materials Research, Tohoku University
- identifier: 202212-SCKXX-0506
  funder_name: Institute for Materials Research, Tohoku University
- identifier: 21H01607
  funder_name: Japan Society for the Promotion of Science
- identifier: 21H01877
  funder_name: Japan Society for the Promotion of Science
- identifier: FA2386-21-1-4024
  funder_name: Asian Office of Aerospace Research and Development
- identifier: '90465'
  funder_name: National Science, Research and Innovation Fund
- funder_name: Thailand Science Research and Innovation
- funder_name: Suranaree University of Technology

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## Fileset

- id: 119c4e1e-3e82-44ac-9f61-cb8e57dae12b
  filename: JChemPhys160(2024)184102.pdf
  content_type: application/pdf
  size: 7835529
  md5: 52a9e273ea3ec85b627e998d43a18910

## Thumbnail

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filename: JChemPhys160(2024)184102.pdf