Luo Weijun, Lawrie Benjamin J, Puretzky Alexander A, Tan Qishuo, Gao Hongze, Lingerfelt David B, Eichman Gage, Mcgee Edward, Swan Anna K, Liang Liangbo, Ling Xi
Department of Chemistry, Boston University, Boston, Massachusetts 02215, United States.
Center for Nanophase Materials Sciences, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States.
ACS Nano. 2023 Dec 12;17(23):23455-23465. doi: 10.1021/acsnano.3c05250. Epub 2023 Dec 3.
Nanoscale strain control of exciton funneling is an increasingly critical tool for the scalable production of single photon emitters (SPEs) in two-dimensional materials. However, conventional far-field optical microscopies remain constrained in spatial resolution by the diffraction limit and thus can provide only a limited description of nanoscale strain localization of SPEs. Here, we quantify the effects of nanoscale heterogeneous strain on the energy and brightness of GaSe SPEs on nanopillars with correlative cathodoluminescence, photoluminescence, and atomic force microscopy, supported by density functional theory simulations. We report the strain-localized SPEs have a broad range of emission wavelengths from 620 to 900 nm. We reveal substantial strain-controlled SPE wavelength tunability over a ∼100 nm spectral range and 2 orders of magnitude enhancement in the SPE brightness at the pillar center due to Type-I exciton funneling. In addition, we show that radiative biexciton cascade processes contribute to observed CL photon superbunching. Also, the GaSe SPEs show excellent stability, where their properties remain unchanged after electron beam exposure. We anticipate that this comprehensive study on the nanoscale strain control of two-dimensional SPEs will provide key insights to guide the development of truly deterministic quantum photonics.
激子漏斗的纳米级应变控制是二维材料中可扩展生产单光子发射器(SPEs)的一种日益关键的工具。然而,传统的远场光学显微镜在空间分辨率上仍受衍射极限的限制,因此只能对SPEs的纳米级应变定位提供有限的描述。在此,我们通过相关的阴极发光、光致发光和原子力显微镜,并结合密度泛函理论模拟,量化了纳米级非均匀应变对纳米柱上GaSe SPEs的能量和亮度的影响。我们报告应变局域化的SPEs具有从620到900 nm的宽发射波长范围。我们揭示了由于I型激子漏斗效应,在约100 nm的光谱范围内,应变控制的SPE波长具有显著的可调谐性,并且在柱中心处SPE亮度提高了2个数量级。此外,我们表明辐射双激子级联过程导致了观察到的阴极发光光子超聚束。而且,GaSe SPEs表现出优异的稳定性,在电子束照射后其性质保持不变。我们预计,这项关于二维SPEs纳米级应变控制的全面研究将为指导真正确定性量子光子学的发展提供关键见解。