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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...
Autores principales: | , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2023
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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 |
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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 |
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