Zeynep Gündoğar*, , , Mads Greisen Ho̷jlund*, , , Kasper Green Larsen*, , and , Ove Christiansen*,
{"title":"递归线性张量展开式的自然占用分析。","authors":"Zeynep Gündoğar*, , , Mads Greisen Ho̷jlund*, , , Kasper Green Larsen*, , and , Ove Christiansen*, ","doi":"10.1021/acs.jctc.5c01101","DOIUrl":null,"url":null,"abstract":"<p >We introduce an innovative recursive tensor decomposition method that draws inspiration from quantum chemical theories. This approach integrates ideas such as natural occupation numbers and natural basis, much like natural orbitals, and employs truncations that parallel the excitation-level truncations in the linear expansions of configuration interaction theory. The framework features recursive algorithms that combine linear expansion with natural basis transformations at each step, ensuring convergence to the original tensor. Consequently, a numerical technique is developed that reconstructs the initial tensor with precision within a predetermined tolerance, using only subtensors of limited dimension and a series of matrix transformations. An initial Python implementation has been created for the 3D tensor scenario where 3D tensors are decomposed to be represented using vectors and matrices alone. We illustrate the behavior of the final Recursive Linear Tensor Expansion in Natural basis algorithm in processing random data sets, experimental data sets from diverse sources with both real and complex tensors, and data sets representing both time-independent and time-dependent anharmonic vibrational wave functions of water. Finally, the systematic accuracy control is illustrated for density fitting two-electron repulsion integrals and tested for the second-order correlation energy of molecular nitrogen and benzene.</p>","PeriodicalId":45,"journal":{"name":"Journal of Chemical Theory and Computation","volume":"21 19","pages":"9270–9289"},"PeriodicalIF":5.5000,"publicationDate":"2025-09-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Recursive Linear Tensor Expansion with Natural Occupation Analysis\",\"authors\":\"Zeynep Gündoğar*, , , Mads Greisen Ho̷jlund*, , , Kasper Green Larsen*, , and , Ove Christiansen*, \",\"doi\":\"10.1021/acs.jctc.5c01101\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p >We introduce an innovative recursive tensor decomposition method that draws inspiration from quantum chemical theories. This approach integrates ideas such as natural occupation numbers and natural basis, much like natural orbitals, and employs truncations that parallel the excitation-level truncations in the linear expansions of configuration interaction theory. The framework features recursive algorithms that combine linear expansion with natural basis transformations at each step, ensuring convergence to the original tensor. Consequently, a numerical technique is developed that reconstructs the initial tensor with precision within a predetermined tolerance, using only subtensors of limited dimension and a series of matrix transformations. An initial Python implementation has been created for the 3D tensor scenario where 3D tensors are decomposed to be represented using vectors and matrices alone. We illustrate the behavior of the final Recursive Linear Tensor Expansion in Natural basis algorithm in processing random data sets, experimental data sets from diverse sources with both real and complex tensors, and data sets representing both time-independent and time-dependent anharmonic vibrational wave functions of water. Finally, the systematic accuracy control is illustrated for density fitting two-electron repulsion integrals and tested for the second-order correlation energy of molecular nitrogen and benzene.</p>\",\"PeriodicalId\":45,\"journal\":{\"name\":\"Journal of Chemical Theory and Computation\",\"volume\":\"21 19\",\"pages\":\"9270–9289\"},\"PeriodicalIF\":5.5000,\"publicationDate\":\"2025-09-17\",\"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://pubs.acs.org/doi/10.1021/acs.jctc.5c01101\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Theory and Computation","FirstCategoryId":"92","ListUrlMain":"https://pubs.acs.org/doi/10.1021/acs.jctc.5c01101","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Recursive Linear Tensor Expansion with Natural Occupation Analysis
We introduce an innovative recursive tensor decomposition method that draws inspiration from quantum chemical theories. This approach integrates ideas such as natural occupation numbers and natural basis, much like natural orbitals, and employs truncations that parallel the excitation-level truncations in the linear expansions of configuration interaction theory. The framework features recursive algorithms that combine linear expansion with natural basis transformations at each step, ensuring convergence to the original tensor. Consequently, a numerical technique is developed that reconstructs the initial tensor with precision within a predetermined tolerance, using only subtensors of limited dimension and a series of matrix transformations. An initial Python implementation has been created for the 3D tensor scenario where 3D tensors are decomposed to be represented using vectors and matrices alone. We illustrate the behavior of the final Recursive Linear Tensor Expansion in Natural basis algorithm in processing random data sets, experimental data sets from diverse sources with both real and complex tensors, and data sets representing both time-independent and time-dependent anharmonic vibrational wave functions of water. Finally, the systematic accuracy control is illustrated for density fitting two-electron repulsion integrals and tested for the second-order correlation energy of molecular nitrogen and benzene.
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.