Bootstrap Embedding For Large Molecular Systems

doi:10.1021/acs.jctc.0c00438

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Bootstrap Embedding For Large Molecular Systems

2020-06-26

PRE

Hong‐Zhou Ye

Henry K. Tran

Troy Van Voorhis *

DOI：10.1021/acs.jctc.0c00438

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Abstract

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Recent developments in quantum embedding theories have provided attractive approaches to correlated calculations for large systems. In this work, we extend our previous work [J. Chem. Theory Comput. 2019, 15, 4497-4506; J. Phys. Chem. Lett. 2019, 10, 6368-6374] on bootstrap embedding (BE) to enable correlated ab initio calculations at the coupled cluster with singles and doubles (CCSD) level for large molecules. We introduce several new algorithmic developments that significantly reduce the computational cost of BE, while maintaining its accuracy. The resulting implementation scales as O(N-3) for the integral transform and O(N) for the CCSD calculation. Numerical results on a series of conjugated molecules suggest that BE with reasonably sized fragments can recover more than 99.5% of the total correlation energy of a full CCSD calculation, while the required computational resources (time and storage) compare favorably to one popular local correlation scheme: domain localized pair natural orbital (DLPNO). The largest BE calculation in this work involves similar to 2900 basis functions and can be performed on a single node with 16 CPU cores and 64 GB of memory in a few days. We anticipate that these developments represent an important step toward the application of BE to solve practical problems.

Keywords:

AUXILIARY BASIS-SETS

COUPLED-CLUSTER SINGLES

ELECTRON CORRELATION METHODS

AB-INITIO CALCULATIONS

PERTURBATION-THEORY

DENSITY

SPACE

DOUBLES

LOCALIZATION

PERFORMANCE

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