{"title":"Periodic Local Coupled-Cluster Theory for Insulators and Metals","authors":"Hong-Zhou Ye, Timothy C. Berkelbach","doi":"10.1021/acs.jctc.4c00936","DOIUrl":null,"url":null,"abstract":"We describe the implementation details of periodic local coupled-cluster theory with single and double excitations (CCSD) and perturbative triple excitations [CCSD(T)] using local natural orbitals (LNOs) and <i>k</i>-point symmetry. We discuss and compare several choices for orbital localization, fragmentation, and LNO construction. By studying diamond and lithium, we demonstrate that periodic LNO-CC theory can be applied with equal success to both insulators and metals, achieving speedups of 2 to 3 orders of magnitude even for moderately sized <i>k</i>-point meshes. Our final predictions of the equilibrium cohesive energy, lattice constant, and bulk modulus for diamond and lithium are in good agreement with previous theoretical predictions and experimental results.","PeriodicalId":45,"journal":{"name":"Journal of Chemical Theory and Computation","volume":null,"pages":null},"PeriodicalIF":5.7000,"publicationDate":"2024-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Theory and Computation","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.jctc.4c00936","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
We describe the implementation details of periodic local coupled-cluster theory with single and double excitations (CCSD) and perturbative triple excitations [CCSD(T)] using local natural orbitals (LNOs) and k-point symmetry. We discuss and compare several choices for orbital localization, fragmentation, and LNO construction. By studying diamond and lithium, we demonstrate that periodic LNO-CC theory can be applied with equal success to both insulators and metals, achieving speedups of 2 to 3 orders of magnitude even for moderately sized k-point meshes. Our final predictions of the equilibrium cohesive energy, lattice constant, and bulk modulus for diamond and lithium are in good agreement with previous theoretical predictions and experimental results.
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.