Na Liu, Licheng Xiao, Yuxing Liu, Yunong Tang, Yichen Ma, Seyed Sepehr Mohajerani, Yue Luo, James Hone, Stefan Strauf
{"title":"WSe2均匀层中禁光层间量子发射体的增亮","authors":"Na Liu, Licheng Xiao, Yuxing Liu, Yunong Tang, Yichen Ma, Seyed Sepehr Mohajerani, Yue Luo, James Hone, Stefan Strauf","doi":"10.1021/acsnano.4c14574","DOIUrl":null,"url":null,"abstract":"Interlayer excitons (IXs) in layered van der Waals materials are promising for quantum technologies and fundamental studies such as exciton-polariton condensation due to their large permanent dipole moments. However, their indirect bandgap optical transition through the Q-K channel renders them momentum forbidden and thus less relevant for optical applications. Here, we demonstrate a method for brightening momentum indirect Q-K transitions from IX quantum emitters (QEs) in 2H-stacked bilayer WSe<sub>2</sub> by simultaneously employing local strain and plasmonic nanocavity coupling. Initially, long <i>T</i><sub>1</sub> lifetimes up to 140 ns are indicative of momentum indirect transitions. Magneto-photoluminescence data show a striking bimodal distribution of <i>g</i>-factors between mono- and bilayer QEs, with a well-defined value of <i>g</i> = 9.5 for IX, highlighting their momentum indirect nature and decoupling from local strain variations. In addition, angle-resolved PL measurements reveal that local curvature on the nanostressor induces a dipole orientation tilt of the QEs, affecting cavity coupling. By embedding these strained QEs into plasmonic cavities, we achieve a 10-fold increase in emission intensity and a 24-fold enhancement in the <i>T</i><sub>1</sub> lifetime in the best case (12-fold average), leading to bright single-photon emission rates up to 1.45 ± 0.1 MHz into the first lens. Moreover, the demonstrated brightening of IX transitions allowed to push the emission wavelength reliably to around 810 nm that enables free-space quantum optical communication.","PeriodicalId":21,"journal":{"name":"ACS Nano","volume":"1 1","pages":""},"PeriodicalIF":16.0000,"publicationDate":"2025-02-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Brightening of Optical Forbidden Interlayer Quantum Emitters in WSe2 Homobilayers\",\"authors\":\"Na Liu, Licheng Xiao, Yuxing Liu, Yunong Tang, Yichen Ma, Seyed Sepehr Mohajerani, Yue Luo, James Hone, Stefan Strauf\",\"doi\":\"10.1021/acsnano.4c14574\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Interlayer excitons (IXs) in layered van der Waals materials are promising for quantum technologies and fundamental studies such as exciton-polariton condensation due to their large permanent dipole moments. However, their indirect bandgap optical transition through the Q-K channel renders them momentum forbidden and thus less relevant for optical applications. Here, we demonstrate a method for brightening momentum indirect Q-K transitions from IX quantum emitters (QEs) in 2H-stacked bilayer WSe<sub>2</sub> by simultaneously employing local strain and plasmonic nanocavity coupling. Initially, long <i>T</i><sub>1</sub> lifetimes up to 140 ns are indicative of momentum indirect transitions. Magneto-photoluminescence data show a striking bimodal distribution of <i>g</i>-factors between mono- and bilayer QEs, with a well-defined value of <i>g</i> = 9.5 for IX, highlighting their momentum indirect nature and decoupling from local strain variations. In addition, angle-resolved PL measurements reveal that local curvature on the nanostressor induces a dipole orientation tilt of the QEs, affecting cavity coupling. By embedding these strained QEs into plasmonic cavities, we achieve a 10-fold increase in emission intensity and a 24-fold enhancement in the <i>T</i><sub>1</sub> lifetime in the best case (12-fold average), leading to bright single-photon emission rates up to 1.45 ± 0.1 MHz into the first lens. Moreover, the demonstrated brightening of IX transitions allowed to push the emission wavelength reliably to around 810 nm that enables free-space quantum optical communication.\",\"PeriodicalId\":21,\"journal\":{\"name\":\"ACS Nano\",\"volume\":\"1 1\",\"pages\":\"\"},\"PeriodicalIF\":16.0000,\"publicationDate\":\"2025-02-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"ACS Nano\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://doi.org/10.1021/acsnano.4c14574\",\"RegionNum\":1,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"CHEMISTRY, MULTIDISCIPLINARY\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"ACS Nano","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1021/acsnano.4c14574","RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, MULTIDISCIPLINARY","Score":null,"Total":0}
引用次数: 0
摘要
层间激子(IXs)由于具有较大的永久偶极矩,在量子技术和基础研究(如激子-极化子凝聚)中具有广阔的应用前景。然而,它们通过Q-K通道的间接带隙光学跃迁使得它们的动量被禁止,因此与光学应用的相关性较小。在这里,我们展示了一种通过同时使用局部应变和等离子体纳米腔耦合来增强2h堆叠双层WSe2中IX量子发射体(QEs)的动量间接Q-K跃迁的方法。最初,长达140ns的长T1寿命表明了动量的间接转变。磁光致发光数据显示,单层和双层QEs之间的g因子具有显著的双峰分布,对于IX, g = 9.5的值明确定义,突出了它们的动量间接性质和与局部应变变化的解耦。此外,角分辨PL测量结果显示,纳米应力源的局部曲率导致量子点偶极子取向倾斜,影响腔耦合。通过将这些应变量子阱嵌入等离子体腔中,我们在最佳情况下实现了10倍的发射强度和24倍的T1寿命增强(平均12倍),导致明亮的单光子发射率高达1.45±0.1 MHz进入第一透镜。此外,所演示的IX跃迁增亮允许将发射波长可靠地推至810 nm左右,从而实现自由空间量子光通信。
Brightening of Optical Forbidden Interlayer Quantum Emitters in WSe2 Homobilayers
Interlayer excitons (IXs) in layered van der Waals materials are promising for quantum technologies and fundamental studies such as exciton-polariton condensation due to their large permanent dipole moments. However, their indirect bandgap optical transition through the Q-K channel renders them momentum forbidden and thus less relevant for optical applications. Here, we demonstrate a method for brightening momentum indirect Q-K transitions from IX quantum emitters (QEs) in 2H-stacked bilayer WSe2 by simultaneously employing local strain and plasmonic nanocavity coupling. Initially, long T1 lifetimes up to 140 ns are indicative of momentum indirect transitions. Magneto-photoluminescence data show a striking bimodal distribution of g-factors between mono- and bilayer QEs, with a well-defined value of g = 9.5 for IX, highlighting their momentum indirect nature and decoupling from local strain variations. In addition, angle-resolved PL measurements reveal that local curvature on the nanostressor induces a dipole orientation tilt of the QEs, affecting cavity coupling. By embedding these strained QEs into plasmonic cavities, we achieve a 10-fold increase in emission intensity and a 24-fold enhancement in the T1 lifetime in the best case (12-fold average), leading to bright single-photon emission rates up to 1.45 ± 0.1 MHz into the first lens. Moreover, the demonstrated brightening of IX transitions allowed to push the emission wavelength reliably to around 810 nm that enables free-space quantum optical communication.
期刊介绍:
ACS Nano, published monthly, serves as an international forum for comprehensive articles on nanoscience and nanotechnology research at the intersections of chemistry, biology, materials science, physics, and engineering. The journal fosters communication among scientists in these communities, facilitating collaboration, new research opportunities, and advancements through discoveries. ACS Nano covers synthesis, assembly, characterization, theory, and simulation of nanostructures, nanobiotechnology, nanofabrication, methods and tools for nanoscience and nanotechnology, and self- and directed-assembly. Alongside original research articles, it offers thorough reviews, perspectives on cutting-edge research, and discussions envisioning the future of nanoscience and nanotechnology.