Xu David D, Vong Albert F, Lebedev Dmitry, Ananth Riddhi, Wong Alexa M, Brown Paul T, Hersam Mark C, Mirkin Chad A, Weiss Emily A
Department of Chemistry, Northwestern University, 2145 Sheridan Road, Evanston, IL, 60208, USA.
International Institute for Nanotechnology, Northwestern University, 2145 Sheridan Road, Evanston, IL, 60208, USA.
Adv Mater. 2023 Feb;35(5):e2208066. doi: 10.1002/adma.202208066. Epub 2022 Dec 14.
Solid-state single photon emitters (SPEs) within atomically thin transition metal dichalcogenides (TMDs) have recently attracted interest as scalable quantum light sources for quantum photonic technologies. Among TMDs, WSe monolayers (MLs) are promising for the deterministic fabrication and engineering of SPEs using local strain fields. The ability to reliably produce isolatable SPEs in WSe is currently impeded by the presence of numerous spectrally overlapping states that occur at strained locations. Here nanoparticle (NP) arrays with precisely defined positions and sizes are employed to deterministically create strain fields in WSe MLs, thus enabling the systematic investigation and control of SPE formation. Using this platform, electron beam irradiation at NP-strained locations transforms spectrally overlapped sub-bandgap emission states into isolatable, anti-bunched quantum emitters. The dependence of the emission spectra of WSe MLs as a function of strain magnitude and exposure time to electron beam irradiation is quantified and provides insight into the mechanism for SPE production. Excitons selectively funnel through strongly coupled sub-bandgap states introduced by electron beam irradiation, which suppresses spectrally overlapping emission pathways and leads to measurable anti-bunched behavior. The findings provide a strategy to generate isolatable SPEs in 2D materials with a well-defined energy range.
原子级薄的过渡金属二卤化物(TMDs)中的固态单光子发射器(SPEs)最近作为量子光子技术中可扩展的量子光源引起了人们的关注。在TMDs中,WSe单分子层(MLs)有望利用局部应变场来确定性地制造和设计SPEs。目前,由于在应变位置存在大量光谱重叠的状态,在WSe中可靠地产生可分离的SPEs的能力受到了阻碍。在这里,具有精确定义位置和尺寸的纳米颗粒(NP)阵列被用于在WSe MLs中确定性地创建应变场,从而能够对SPE形成进行系统的研究和控制。利用这个平台,在NP应变位置的电子束辐照将光谱重叠的亚带隙发射态转变为可分离的、反聚束的量子发射器。对WSe MLs发射光谱随应变幅度和电子束辐照暴露时间的依赖性进行了量化,并为SPE产生的机制提供了深入了解。激子选择性地通过电子束辐照引入的强耦合亚带隙态进行漏斗传输,这抑制了光谱重叠的发射途径并导致可测量的反聚束行为。这些发现提供了一种在具有明确能量范围的二维材料中产生可分离的SPEs的策略。