Cargando…

Electronic excited states in deep variational Monte Carlo

Obtaining accurate ground and low-lying excited states of electronic systems is crucial in a multitude of important applications. One ab initio method for solving the Schrödinger equation that scales favorably for large systems is variational quantum Monte Carlo (QMC). The recently introduced deep Q...

Descripción completa

Detalles Bibliográficos
Autores principales: Entwistle, M. T., Schätzle, Z., Erdman, P. A., Hermann, J., Noé, F.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: Nature Publishing Group UK 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9845370/
https://www.ncbi.nlm.nih.gov/pubmed/36650151
http://dx.doi.org/10.1038/s41467-022-35534-5
_version_ 1784870891548573696
author Entwistle, M. T.
Schätzle, Z.
Erdman, P. A.
Hermann, J.
Noé, F.
author_facet Entwistle, M. T.
Schätzle, Z.
Erdman, P. A.
Hermann, J.
Noé, F.
author_sort Entwistle, M. T.
collection PubMed
description Obtaining accurate ground and low-lying excited states of electronic systems is crucial in a multitude of important applications. One ab initio method for solving the Schrödinger equation that scales favorably for large systems is variational quantum Monte Carlo (QMC). The recently introduced deep QMC approach uses ansatzes represented by deep neural networks and generates nearly exact ground-state solutions for molecules containing up to a few dozen electrons, with the potential to scale to much larger systems where other highly accurate methods are not feasible. In this paper, we extend one such ansatz (PauliNet) to compute electronic excited states. We demonstrate our method on various small atoms and molecules and consistently achieve high accuracy for low-lying states. To highlight the method’s potential, we compute the first excited state of the much larger benzene molecule, as well as the conical intersection of ethylene, with PauliNet matching results of more expensive high-level methods.
format Online
Article
Text
id pubmed-9845370
institution National Center for Biotechnology Information
language English
publishDate 2023
publisher Nature Publishing Group UK
record_format MEDLINE/PubMed
spelling pubmed-98453702023-01-19 Electronic excited states in deep variational Monte Carlo Entwistle, M. T. Schätzle, Z. Erdman, P. A. Hermann, J. Noé, F. Nat Commun Article Obtaining accurate ground and low-lying excited states of electronic systems is crucial in a multitude of important applications. One ab initio method for solving the Schrödinger equation that scales favorably for large systems is variational quantum Monte Carlo (QMC). The recently introduced deep QMC approach uses ansatzes represented by deep neural networks and generates nearly exact ground-state solutions for molecules containing up to a few dozen electrons, with the potential to scale to much larger systems where other highly accurate methods are not feasible. In this paper, we extend one such ansatz (PauliNet) to compute electronic excited states. We demonstrate our method on various small atoms and molecules and consistently achieve high accuracy for low-lying states. To highlight the method’s potential, we compute the first excited state of the much larger benzene molecule, as well as the conical intersection of ethylene, with PauliNet matching results of more expensive high-level methods. Nature Publishing Group UK 2023-01-17 /pmc/articles/PMC9845370/ /pubmed/36650151 http://dx.doi.org/10.1038/s41467-022-35534-5 Text en © The Author(s) 2023 https://creativecommons.org/licenses/by/4.0/Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) .
spellingShingle Article
Entwistle, M. T.
Schätzle, Z.
Erdman, P. A.
Hermann, J.
Noé, F.
Electronic excited states in deep variational Monte Carlo
title Electronic excited states in deep variational Monte Carlo
title_full Electronic excited states in deep variational Monte Carlo
title_fullStr Electronic excited states in deep variational Monte Carlo
title_full_unstemmed Electronic excited states in deep variational Monte Carlo
title_short Electronic excited states in deep variational Monte Carlo
title_sort electronic excited states in deep variational monte carlo
topic Article
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9845370/
https://www.ncbi.nlm.nih.gov/pubmed/36650151
http://dx.doi.org/10.1038/s41467-022-35534-5
work_keys_str_mv AT entwistlemt electronicexcitedstatesindeepvariationalmontecarlo
AT schatzlez electronicexcitedstatesindeepvariationalmontecarlo
AT erdmanpa electronicexcitedstatesindeepvariationalmontecarlo
AT hermannj electronicexcitedstatesindeepvariationalmontecarlo
AT noef electronicexcitedstatesindeepvariationalmontecarlo