Local Embedding and Effective Downfolding in the Auxiliary-Field Quantum Monte Carlo Method
Abstract
A local embedding and effective downfolding scheme has been developed and implemented in the auxiliary-field quantum Monte Carlo (AFQMC) method. A local cluster in which electrons are fully correlated is defined, and the frozen orbital method is used on the remainder of the system to construct an effective Hamiltonian, which operates within the local cluster. Local embedding, which involves only the occupied sector, has previously been employed in the context of Co/graphene. Here, the methodology is extended in order to allow for effective downfolding of the virtual sector, thus allowing for significant reduction in the computational effort required for AFQMC calculations. The system size, which can be feasibly treated with AFQMC, is therefore greatly extended as only a single local cluster is explicitly correlated at the AFQMC level of theory. The approximation is controlled by the separate choice of the spatial size of the active occupied region (Ro) and of the active virtual region (Rv). In conclusion, the systematic dependence of the AFQMC energy on Ro and Rv is investigated, and it is found that relative AFQMC energies of physical and chemical interest converge rapidly to the full AFQMC treatment (i.e., using no embedding or downfolding).
- Authors:
-
- College of William and Mary, Williamsburg, VA (United States)
- College of William and Mary, Williamsburg, VA (United States); The Flatiron Institute, New York, NY (United States)
- Publication Date:
- Research Org.:
- College of William and Mary, Williamsburg, VA (United States)
- Sponsoring Org.:
- USDOE Office of Science (SC), Basic Energy Sciences (BES). Chemical Sciences, Geosciences, and Biosciences Division
- OSTI Identifier:
- 1544771
- Grant/Contract Number:
- SC0001303
- Resource Type:
- Accepted Manuscript
- Journal Name:
- Journal of Chemical Theory and Computation
- Additional Journal Information:
- Journal Volume: 15; Journal Issue: 7; Journal ID: ISSN 1549-9618
- Publisher:
- American Chemical Society
- Country of Publication:
- United States
- Language:
- English
- Subject:
- 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 97 MATHEMATICS AND COMPUTING
Citation Formats
Eskridge, Brandon, Krakauer, Henry, and Zhang, Shiwei. Local Embedding and Effective Downfolding in the Auxiliary-Field Quantum Monte Carlo Method. United States: N. p., 2019.
Web. doi:10.1021/acs.jctc.8b01244.
Eskridge, Brandon, Krakauer, Henry, & Zhang, Shiwei. Local Embedding and Effective Downfolding in the Auxiliary-Field Quantum Monte Carlo Method. United States. https://doi.org/10.1021/acs.jctc.8b01244
Eskridge, Brandon, Krakauer, Henry, and Zhang, Shiwei. Tue .
"Local Embedding and Effective Downfolding in the Auxiliary-Field Quantum Monte Carlo Method". United States. https://doi.org/10.1021/acs.jctc.8b01244. https://www.osti.gov/servlets/purl/1544771.
@article{osti_1544771,
title = {Local Embedding and Effective Downfolding in the Auxiliary-Field Quantum Monte Carlo Method},
author = {Eskridge, Brandon and Krakauer, Henry and Zhang, Shiwei},
abstractNote = {A local embedding and effective downfolding scheme has been developed and implemented in the auxiliary-field quantum Monte Carlo (AFQMC) method. A local cluster in which electrons are fully correlated is defined, and the frozen orbital method is used on the remainder of the system to construct an effective Hamiltonian, which operates within the local cluster. Local embedding, which involves only the occupied sector, has previously been employed in the context of Co/graphene. Here, the methodology is extended in order to allow for effective downfolding of the virtual sector, thus allowing for significant reduction in the computational effort required for AFQMC calculations. The system size, which can be feasibly treated with AFQMC, is therefore greatly extended as only a single local cluster is explicitly correlated at the AFQMC level of theory. The approximation is controlled by the separate choice of the spatial size of the active occupied region (Ro) and of the active virtual region (Rv). In conclusion, the systematic dependence of the AFQMC energy on Ro and Rv is investigated, and it is found that relative AFQMC energies of physical and chemical interest converge rapidly to the full AFQMC treatment (i.e., using no embedding or downfolding).},
doi = {10.1021/acs.jctc.8b01244},
journal = {Journal of Chemical Theory and Computation},
number = 7,
volume = 15,
place = {United States},
year = {Tue Jun 25 00:00:00 EDT 2019},
month = {Tue Jun 25 00:00:00 EDT 2019}
}
Web of Science
Figures / Tables:
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