{"title":"第一原理水平 QED-TDDFT 计算的分子激子极化子光学发射光谱","authors":"Shanhao Deng, Junjie Yang, Yihan Shao, Qi Ou, Prof. Zhigang Shuai","doi":"10.1002/cptc.202400117","DOIUrl":null,"url":null,"abstract":"<p>In microcavity, strong coupling between light and molecules leads to the formation of hybrid excitations, i. e., the polaritons, or exciton-polaritons. Such coupling may alter the energy landscape of the system and the optical properties of the material, making it an effective approach for controlling the light emission from molecular materials. However, due to the complexity of vibrational modes, spectroscopic calculations for organic exciton-polaritons remain to be challenging. In this work, based on the linear-response quantum-electrodynamical time-dependent density functional theory (QED-TDDFT), we employ the thermal vibrational correlation function (TVCF) formalism to calculate the molecular optical spectrum of the lower polaritons (LP) at first-principles level for three molecules, i. e., anthracene, distyrylbenzenes (DSB), and rubrene. The polaron decoupling effect is confirmed from our first-principles computations. The theoretical emission spectra of LP provide new insights for aiding molecular and device design in microcavities that are otherwise hindered due to the lack of vibrational information.</p>","PeriodicalId":10108,"journal":{"name":"ChemPhotoChem","volume":"8 12","pages":""},"PeriodicalIF":3.0000,"publicationDate":"2024-07-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Optical Emission Spectra of Molecular Excitonic Polariton Computed at the First-Principles Level QED-TDDFT\",\"authors\":\"Shanhao Deng, Junjie Yang, Yihan Shao, Qi Ou, Prof. Zhigang Shuai\",\"doi\":\"10.1002/cptc.202400117\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p>In microcavity, strong coupling between light and molecules leads to the formation of hybrid excitations, i. e., the polaritons, or exciton-polaritons. Such coupling may alter the energy landscape of the system and the optical properties of the material, making it an effective approach for controlling the light emission from molecular materials. However, due to the complexity of vibrational modes, spectroscopic calculations for organic exciton-polaritons remain to be challenging. In this work, based on the linear-response quantum-electrodynamical time-dependent density functional theory (QED-TDDFT), we employ the thermal vibrational correlation function (TVCF) formalism to calculate the molecular optical spectrum of the lower polaritons (LP) at first-principles level for three molecules, i. e., anthracene, distyrylbenzenes (DSB), and rubrene. The polaron decoupling effect is confirmed from our first-principles computations. The theoretical emission spectra of LP provide new insights for aiding molecular and device design in microcavities that are otherwise hindered due to the lack of vibrational information.</p>\",\"PeriodicalId\":10108,\"journal\":{\"name\":\"ChemPhotoChem\",\"volume\":\"8 12\",\"pages\":\"\"},\"PeriodicalIF\":3.0000,\"publicationDate\":\"2024-07-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ChemPhotoChem\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://onlinelibrary.wiley.com/doi/10.1002/cptc.202400117\",\"RegionNum\":4,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q3\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ChemPhotoChem","FirstCategoryId":"92","ListUrlMain":"https://onlinelibrary.wiley.com/doi/10.1002/cptc.202400117","RegionNum":4,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q3","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Optical Emission Spectra of Molecular Excitonic Polariton Computed at the First-Principles Level QED-TDDFT
In microcavity, strong coupling between light and molecules leads to the formation of hybrid excitations, i. e., the polaritons, or exciton-polaritons. Such coupling may alter the energy landscape of the system and the optical properties of the material, making it an effective approach for controlling the light emission from molecular materials. However, due to the complexity of vibrational modes, spectroscopic calculations for organic exciton-polaritons remain to be challenging. In this work, based on the linear-response quantum-electrodynamical time-dependent density functional theory (QED-TDDFT), we employ the thermal vibrational correlation function (TVCF) formalism to calculate the molecular optical spectrum of the lower polaritons (LP) at first-principles level for three molecules, i. e., anthracene, distyrylbenzenes (DSB), and rubrene. The polaron decoupling effect is confirmed from our first-principles computations. The theoretical emission spectra of LP provide new insights for aiding molecular and device design in microcavities that are otherwise hindered due to the lack of vibrational information.
ChemPhotoChemChemistry-Physical and Theoretical Chemistry
CiteScore
5.80
自引率
5.40%
发文量
165
期刊介绍:
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