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Accurate many-body electronic structure near the basis set limit: Application to the chromium dimer

Li, Junhao and Yao, Yuan and Holmes, Adam A. and Otten, Matthew and Sun, Qiming and Sharma, Sandeep and Umrigar, C. J. (2020) Accurate many-body electronic structure near the basis set limit: Application to the chromium dimer. Physical Review Research, 2 (1). Art. No. 012015. ISSN 2643-1564. doi:10.1103/physrevresearch.2.012015.

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We describe a method for computing near-exact energies for correlated systems with large Hilbert spaces. The method efficiently identifies the most important basis states (Slater determinants) and performs a variational calculation in the subspace spanned by these determinants. A semistochastic approach is then used to add a perturbative correction to the variational energy to compute the total energy. The size of the variational space is progressively increased until the total energy converges to within the desired tolerance. We demonstrate the power of the method by computing a near-exact potential energy curve for a very challenging molecule: the chromium dimer.

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URLURL TypeDescription Paper
Sun, Qiming0000-0003-0528-6186
Sharma, Sandeep0000-0002-6598-8887
Additional Information:© 2020 Published by the American Physical Society. Published by the American Physical Society under the terms of the Creative Commons Attribution 4.0 International license. Further distribution of this work must maintain attribution to the author(s) and the published article’s title, journal citation, and DOI. Received 2 October 2019; revised manuscript received 20 November 2019; published 15 January 2020. This work was supported by the AFOSR under Grant No. FA9550-18-1-0095 and by the NSF under Grants No. ACI-1534965 and No. CHE-1800584. The computations were performed on the Bridges cluster at the Pittsburgh Supercomputing Center supported by NSF Grant No. ACI-1445606, as part of the XSEDE program supported by NSF Grant No. ACI-1548562, and on the Google Cloud Platform. We thank N. Dattani for sharing the Cr₂ PEC he deduced from experimental data, A. Mahajan for help with using pyscf, and G. Chan, A. Savin, and J. Toulouse for valuable discussions.
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Air Force Office of Scientific Research (AFOSR)FA9550-18-1-0095
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Record Number:CaltechAUTHORS:20200115-105617962
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:100734
Deposited By: Tony Diaz
Deposited On:15 Jan 2020 19:41
Last Modified:16 Nov 2021 17:56

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