Bootstrap Embedding for Molecules
Fragment embedding is one way to circumvent the high computational scaling of accurate electron correlation methods. The challenge of applying fragment embedding to molecular systems primarily lies in the strong entanglement and correlation that prevent accurate fragmentation across chemical bonds....
| Main Authors: | , , , |
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| Other Authors: | |
| Format: | Article |
| Language: | English |
| Published: |
American Chemical Society (ACS)
2019
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| Online Access: | https://hdl.handle.net/1721.1/122290 |
| _version_ | 1811073060471570432 |
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| author | Ye, Hongzhou Ricke, Nathan Darrell Tran, Henry K. Van Voorhis, Troy |
| author2 | Massachusetts Institute of Technology. Department of Chemistry |
| author_facet | Massachusetts Institute of Technology. Department of Chemistry Ye, Hongzhou Ricke, Nathan Darrell Tran, Henry K. Van Voorhis, Troy |
| author_sort | Ye, Hongzhou |
| collection | MIT |
| description | Fragment embedding is one way to circumvent the high computational scaling of accurate electron correlation methods. The challenge of applying fragment embedding to molecular systems primarily lies in the strong entanglement and correlation that prevent accurate fragmentation across chemical bonds. Recently, Schmidt decomposition has been shown effective for embedding fragments that are strongly coupled to a bath in several model systems. In this work, we extend a recently developed quantum embedding scheme, bootstrap embedding (BE), to molecular systems. The resulting method utilizes the matching conditions naturally arising from using overlapping fragments to optimize the embedding. Numerical simulation suggests that the accuracy of the embedding improves rapidly with fragment size for small molecules, whereas larger fragments that include orbitals from different atoms may be needed for larger molecules. BE scales linearly with system size (apart from an integral transform) and hence can potentially be useful for large-scale calculations. |
| first_indexed | 2024-09-23T09:27:58Z |
| format | Article |
| id | mit-1721.1/122290 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T09:27:58Z |
| publishDate | 2019 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1222902022-09-30T14:34:22Z Bootstrap Embedding for Molecules Ye, Hongzhou Ricke, Nathan Darrell Tran, Henry K. Van Voorhis, Troy Massachusetts Institute of Technology. Department of Chemistry Fragment embedding is one way to circumvent the high computational scaling of accurate electron correlation methods. The challenge of applying fragment embedding to molecular systems primarily lies in the strong entanglement and correlation that prevent accurate fragmentation across chemical bonds. Recently, Schmidt decomposition has been shown effective for embedding fragments that are strongly coupled to a bath in several model systems. In this work, we extend a recently developed quantum embedding scheme, bootstrap embedding (BE), to molecular systems. The resulting method utilizes the matching conditions naturally arising from using overlapping fragments to optimize the embedding. Numerical simulation suggests that the accuracy of the embedding improves rapidly with fragment size for small molecules, whereas larger fragments that include orbitals from different atoms may be needed for larger molecules. BE scales linearly with system size (apart from an integral transform) and hence can potentially be useful for large-scale calculations. National Science Foundation (U.S.) (Grant CHE-1464804) 2019-09-25T20:36:01Z 2019-09-25T20:36:01Z 2019-07 2019-05 2019-09-20T13:58:51Z Article http://purl.org/eprint/type/JournalArticle 1549-9618 1549-9626 https://hdl.handle.net/1721.1/122290 Ye, Hong-Zhou et al. "Bootstrap Embedding for Molecules." Journal of Chemical Theory and Computing 15, 8 (July 2019): 4497-4506 © 2019 American Chemical Society en http://dx.doi.org/10.1021/acs.jctc.9b00529 Journal of Chemical Theory and Computation Creative Commons Attribution-NonCommercial-NoDerivs License http://creativecommons.org/licenses/by-nc-nd/4.0/ application/pdf American Chemical Society (ACS) ACS |
| spellingShingle | Ye, Hongzhou Ricke, Nathan Darrell Tran, Henry K. Van Voorhis, Troy Bootstrap Embedding for Molecules |
| title | Bootstrap Embedding for Molecules |
| title_full | Bootstrap Embedding for Molecules |
| title_fullStr | Bootstrap Embedding for Molecules |
| title_full_unstemmed | Bootstrap Embedding for Molecules |
| title_short | Bootstrap Embedding for Molecules |
| title_sort | bootstrap embedding for molecules |
| url | https://hdl.handle.net/1721.1/122290 |
| work_keys_str_mv | AT yehongzhou bootstrapembeddingformolecules AT rickenathandarrell bootstrapembeddingformolecules AT tranhenryk bootstrapembeddingformolecules AT vanvoorhistroy bootstrapembeddingformolecules |