{"title":"单一耦合簇Ansatz的能量景观。","authors":"Choy Boy, Maria-Andreea Filip, David J Wales","doi":"10.1021/acs.jctc.4c01667","DOIUrl":null,"url":null,"abstract":"<p><p>The unitary coupled cluster (UCC) approach has been one of the most popular wavefunction parametrizations for the variational quantum eigensolver due to the relative ease of optimization compared to hardware-efficient ansätze. In this contribution, we explore the energy landscape of the unitary coupled cluster singles and doubles (UCCSD) wavefunction for two commonly employed benchmark systems, lithium hydride and the nitrogen dimer. We investigate the organization of the solution space in terms of local minima and show how it changes as the number and order of operators of the UCC ansatz are varied. Surprisingly, we find that in all cases, the UCCSD energy has numerous low-lying minima connected by high energy transition states. Additionally, the energy spread of the minima that lie in the same band as the global minimum may exceed chemical accuracy, making the location of the true global minimum especially challenging.</p>","PeriodicalId":45,"journal":{"name":"Journal of Chemical Theory and Computation","volume":" ","pages":"1739-1751"},"PeriodicalIF":5.5000,"publicationDate":"2025-02-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11866750/pdf/","citationCount":"0","resultStr":"{\"title\":\"Energy Landscapes for the Unitary Coupled Cluster Ansatz.\",\"authors\":\"Choy Boy, Maria-Andreea Filip, David J Wales\",\"doi\":\"10.1021/acs.jctc.4c01667\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>The unitary coupled cluster (UCC) approach has been one of the most popular wavefunction parametrizations for the variational quantum eigensolver due to the relative ease of optimization compared to hardware-efficient ansätze. In this contribution, we explore the energy landscape of the unitary coupled cluster singles and doubles (UCCSD) wavefunction for two commonly employed benchmark systems, lithium hydride and the nitrogen dimer. We investigate the organization of the solution space in terms of local minima and show how it changes as the number and order of operators of the UCC ansatz are varied. Surprisingly, we find that in all cases, the UCCSD energy has numerous low-lying minima connected by high energy transition states. Additionally, the energy spread of the minima that lie in the same band as the global minimum may exceed chemical accuracy, making the location of the true global minimum especially challenging.</p>\",\"PeriodicalId\":45,\"journal\":{\"name\":\"Journal of Chemical Theory and Computation\",\"volume\":\" \",\"pages\":\"1739-1751\"},\"PeriodicalIF\":5.5000,\"publicationDate\":\"2025-02-25\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11866750/pdf/\",\"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.4c01667\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"2025/2/16 0:00:00\",\"PubModel\":\"Epub\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Chemical Theory and Computation","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1021/acs.jctc.4c01667","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"2025/2/16 0:00:00","PubModel":"Epub","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Energy Landscapes for the Unitary Coupled Cluster Ansatz.
The unitary coupled cluster (UCC) approach has been one of the most popular wavefunction parametrizations for the variational quantum eigensolver due to the relative ease of optimization compared to hardware-efficient ansätze. In this contribution, we explore the energy landscape of the unitary coupled cluster singles and doubles (UCCSD) wavefunction for two commonly employed benchmark systems, lithium hydride and the nitrogen dimer. We investigate the organization of the solution space in terms of local minima and show how it changes as the number and order of operators of the UCC ansatz are varied. Surprisingly, we find that in all cases, the UCCSD energy has numerous low-lying minima connected by high energy transition states. Additionally, the energy spread of the minima that lie in the same band as the global minimum may exceed chemical accuracy, making the location of the true global minimum especially challenging.
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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