{"title":"远程相互作用模型中未取代和取代多烯链单线态裂变的精确波包动力学","authors":"Suryoday Prodhan, S. Ramasesha","doi":"10.1103/PhysRevB.96.075142","DOIUrl":null,"url":null,"abstract":"Singlet fission is a potential pathway for significant enhancement of efficiency in organic solar cells. In this article, we have studied singlet fission in a pair of polyene molecules employing exact many-body wave packet dynamics. The individual molecules are treated within Hubbard and Pariser-Parr-Pople (PPP) models and the interaction between them involves transfer terms, intersite electron repulsions and site charge-bond charge repulsion terms. Initial wave packet is constructed from excited singlet state of one molecule and ground state of the other. Time development of this wave packet under the influence of intermolecular interactions is followed within the Schr\\\"{o}dinger picture by an efficient predictor-corrector scheme. In unsubstituted Hubbard and PPP chains, $2{}^1A$ excited singlet state leads to significant fission yield while the $1{}^1B$ state gives negligible fission yield. On substitution by donor-acceptor groups of moderate strength, singlet state derived from $1{}^1B$ state also gives significant fission yield within PPP model. Furthermore, we find the fission yield depends considerably on the stacking arrangement of the polyene molecules.","PeriodicalId":8439,"journal":{"name":"arXiv: Chemical Physics","volume":null,"pages":null},"PeriodicalIF":0.0000,"publicationDate":"2016-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"4","resultStr":"{\"title\":\"Exact Wave Packet Dynamics of Singlet Fission in Unsubstituted and Substituted Polyene Chains within Long-Range Interacting Models\",\"authors\":\"Suryoday Prodhan, S. Ramasesha\",\"doi\":\"10.1103/PhysRevB.96.075142\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Singlet fission is a potential pathway for significant enhancement of efficiency in organic solar cells. In this article, we have studied singlet fission in a pair of polyene molecules employing exact many-body wave packet dynamics. The individual molecules are treated within Hubbard and Pariser-Parr-Pople (PPP) models and the interaction between them involves transfer terms, intersite electron repulsions and site charge-bond charge repulsion terms. Initial wave packet is constructed from excited singlet state of one molecule and ground state of the other. Time development of this wave packet under the influence of intermolecular interactions is followed within the Schr\\\\\\\"{o}dinger picture by an efficient predictor-corrector scheme. In unsubstituted Hubbard and PPP chains, $2{}^1A$ excited singlet state leads to significant fission yield while the $1{}^1B$ state gives negligible fission yield. On substitution by donor-acceptor groups of moderate strength, singlet state derived from $1{}^1B$ state also gives significant fission yield within PPP model. Furthermore, we find the fission yield depends considerably on the stacking arrangement of the polyene molecules.\",\"PeriodicalId\":8439,\"journal\":{\"name\":\"arXiv: Chemical Physics\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":0.0000,\"publicationDate\":\"2016-10-03\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"4\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"arXiv: Chemical Physics\",\"FirstCategoryId\":\"1085\",\"ListUrlMain\":\"https://doi.org/10.1103/PhysRevB.96.075142\",\"RegionNum\":0,\"RegionCategory\":null,\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"\",\"JCRName\":\"\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"arXiv: Chemical Physics","FirstCategoryId":"1085","ListUrlMain":"https://doi.org/10.1103/PhysRevB.96.075142","RegionNum":0,"RegionCategory":null,"ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"","JCRName":"","Score":null,"Total":0}
引用次数: 4
摘要
单线态裂变是提高有机太阳能电池效率的潜在途径。本文用精确多体波包动力学研究了一对多烯分子的单线态裂变。单个分子在Hubbard和parier - parr - people (PPP)模型中进行处理,它们之间的相互作用涉及转移项、位点间电子排斥和位点电荷-键电荷排斥项。初始波包是由一个分子的激发态和另一个分子的基态构成的。在分子间相互作用的影响下,该波包的时间发展在薛定谔图中被一个有效的预测-校正方案所跟踪。在未取代的Hubbard链和PPP链中,$2{}^1A$激发态导致显著的裂变产额,而$1{}^1B$的裂变产额可以忽略不计。在中等强度的供体-受体基团取代下,由$1{}^1B$状态衍生出的单重态在PPP模型中也给出了显著的裂变产额。此外,我们发现裂变产率在很大程度上取决于多烯分子的堆叠排列。
Exact Wave Packet Dynamics of Singlet Fission in Unsubstituted and Substituted Polyene Chains within Long-Range Interacting Models
Singlet fission is a potential pathway for significant enhancement of efficiency in organic solar cells. In this article, we have studied singlet fission in a pair of polyene molecules employing exact many-body wave packet dynamics. The individual molecules are treated within Hubbard and Pariser-Parr-Pople (PPP) models and the interaction between them involves transfer terms, intersite electron repulsions and site charge-bond charge repulsion terms. Initial wave packet is constructed from excited singlet state of one molecule and ground state of the other. Time development of this wave packet under the influence of intermolecular interactions is followed within the Schr\"{o}dinger picture by an efficient predictor-corrector scheme. In unsubstituted Hubbard and PPP chains, $2{}^1A$ excited singlet state leads to significant fission yield while the $1{}^1B$ state gives negligible fission yield. On substitution by donor-acceptor groups of moderate strength, singlet state derived from $1{}^1B$ state also gives significant fission yield within PPP model. Furthermore, we find the fission yield depends considerably on the stacking arrangement of the polyene molecules.