{"title":"不对称三层过渡金属二卤化物异质结构中的多种激子现象","authors":"Zhe Zhang, Shudong Wang","doi":"10.1021/acs.jpclett.4c02526","DOIUrl":null,"url":null,"abstract":"Interlayer excitons formed in two-dimensional transition metal dichalcogenide (TMD) heterostructures can be easily tuned due to the large spatial separation. In this work, we discuss the electronic and excitonic optical properties of trilayer heterostructures MoS<sub>2</sub>/MoSSe/WSe<sub>2</sub> and MoS<sub>2</sub>/MoSSe/MoSe<sub>2</sub> using state-of-the-art <i>GW</i>+BSE calculations. In both trilayer geometries, we discover a variety of exciton states, including interlayer excitons, every-other-layer excitons, and their hybridized states, <i>h</i>-IX. Importantly, the <i>h</i>-IXs are optically bright through hybridizing with the intralayer excitons, and the radiative lifetimes of <i>h</i>-IXs range from subnanoseconds to tens of microseconds at 77 K, depending on their compositions. We also reveal that the diversity of the low-lying IXs in MoS<sub>2</sub>/MoSSe/MoSe<sub>2</sub> is higher than that of MoS<sub>2</sub>/MoSSe/WSe<sub>2</sub>, because more energy levels participate in transitions in MoS<sub>2</sub>/MoSSe/MoSe<sub>2</sub>. Our findings demonstrate that the appropriate energy alignment via manipulating the Janus layer is crucial for realizing rich excitonic states in trilayer TMD heterostructures.","PeriodicalId":62,"journal":{"name":"The Journal of Physical Chemistry Letters","volume":null,"pages":null},"PeriodicalIF":4.8000,"publicationDate":"2024-09-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Diverse Excitonic Phenomena in Asymmetric Trilayer Transition Metal Dichalcogenide Heterostructures\",\"authors\":\"Zhe Zhang, Shudong Wang\",\"doi\":\"10.1021/acs.jpclett.4c02526\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Interlayer excitons formed in two-dimensional transition metal dichalcogenide (TMD) heterostructures can be easily tuned due to the large spatial separation. In this work, we discuss the electronic and excitonic optical properties of trilayer heterostructures MoS<sub>2</sub>/MoSSe/WSe<sub>2</sub> and MoS<sub>2</sub>/MoSSe/MoSe<sub>2</sub> using state-of-the-art <i>GW</i>+BSE calculations. In both trilayer geometries, we discover a variety of exciton states, including interlayer excitons, every-other-layer excitons, and their hybridized states, <i>h</i>-IX. Importantly, the <i>h</i>-IXs are optically bright through hybridizing with the intralayer excitons, and the radiative lifetimes of <i>h</i>-IXs range from subnanoseconds to tens of microseconds at 77 K, depending on their compositions. We also reveal that the diversity of the low-lying IXs in MoS<sub>2</sub>/MoSSe/MoSe<sub>2</sub> is higher than that of MoS<sub>2</sub>/MoSSe/WSe<sub>2</sub>, because more energy levels participate in transitions in MoS<sub>2</sub>/MoSSe/MoSe<sub>2</sub>. Our findings demonstrate that the appropriate energy alignment via manipulating the Janus layer is crucial for realizing rich excitonic states in trilayer TMD heterostructures.\",\"PeriodicalId\":62,\"journal\":{\"name\":\"The Journal of Physical Chemistry Letters\",\"volume\":null,\"pages\":null},\"PeriodicalIF\":4.8000,\"publicationDate\":\"2024-09-27\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"The Journal of Physical Chemistry Letters\",\"FirstCategoryId\":\"1\",\"ListUrlMain\":\"https://doi.org/10.1021/acs.jpclett.4c02526\",\"RegionNum\":2,\"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":"The Journal of Physical Chemistry Letters","FirstCategoryId":"1","ListUrlMain":"https://doi.org/10.1021/acs.jpclett.4c02526","RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Diverse Excitonic Phenomena in Asymmetric Trilayer Transition Metal Dichalcogenide Heterostructures
Interlayer excitons formed in two-dimensional transition metal dichalcogenide (TMD) heterostructures can be easily tuned due to the large spatial separation. In this work, we discuss the electronic and excitonic optical properties of trilayer heterostructures MoS2/MoSSe/WSe2 and MoS2/MoSSe/MoSe2 using state-of-the-art GW+BSE calculations. In both trilayer geometries, we discover a variety of exciton states, including interlayer excitons, every-other-layer excitons, and their hybridized states, h-IX. Importantly, the h-IXs are optically bright through hybridizing with the intralayer excitons, and the radiative lifetimes of h-IXs range from subnanoseconds to tens of microseconds at 77 K, depending on their compositions. We also reveal that the diversity of the low-lying IXs in MoS2/MoSSe/MoSe2 is higher than that of MoS2/MoSSe/WSe2, because more energy levels participate in transitions in MoS2/MoSSe/MoSe2. Our findings demonstrate that the appropriate energy alignment via manipulating the Janus layer is crucial for realizing rich excitonic states in trilayer TMD heterostructures.
期刊介绍:
The Journal of Physical Chemistry (JPC) Letters is devoted to reporting new and original experimental and theoretical basic research of interest to physical chemists, biophysical chemists, chemical physicists, physicists, material scientists, and engineers. An important criterion for acceptance is that the paper reports a significant scientific advance and/or physical insight such that rapid publication is essential. Two issues of JPC Letters are published each month.