Henry K Tran, Leah P Weisburn, Minsik Cho, Shaun Weatherly, Hong-Zhou Ye, Troy Van Voorhis
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引用次数: 0
Abstract
Quantum embedding methods are powerful tools to exploit the locality of electron correlation, but thus far many wave function-in-wave function methods have focused on small (e.g., minimal) basis sets. One major challenge for extended basis sets lies in defining consistent atom- or fragment-localized orbitals in spite of the larger spatial extent of the underlying atomic orbitals. In this work, we modify a particular form of quantum embedding, bootstrap embedding (BE), to the case of extended basis sets. We find that using intrinsic atomic orbital (IAO) localization schemes alongside BE converges to ∼99.7% of the CCSD correlation energy in 3-21G, 6-311G, and cc-pVDZ basis sets for reasonably sized fragments. These results mark an important first step in extending the success of embedding methods to properly studying dynamic correlation.
期刊介绍：
The Journal of Chemical Theory and Computation invites new and original contributions with the understanding that, if accepted, they will not be published elsewhere. Papers reporting new theories, methodology, and/or important applications in quantum electronic structure, molecular dynamics, and statistical mechanics are appropriate for submission to this Journal. Specific topics include advances in or applications of ab initio quantum mechanics, density functional theory, design and properties of new materials, surface science, Monte Carlo simulations, solvation models, QM/MM calculations, biomolecular structure prediction, and molecular dynamics in the broadest sense including gas-phase dynamics, ab initio dynamics, biomolecular dynamics, and protein folding. The Journal does not consider papers that are straightforward applications of known methods including DFT and molecular dynamics. The Journal favors submissions that include advances in theory or methodology with applications to compelling problems.
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