Puchert Robin P, Hofmann Felix J, Angerer Hermann S, Vogelsang Jan, Bange Sebastian, Lupton John M
Institut für Experimentelle und Angewandte Physik, Universität Regensburg, 93053, Regensburg, Germany.
Small. 2021 Feb;17(5):e2006425. doi: 10.1002/smll.202006425. Epub 2021 Jan 15.
Break junctions in noble-metal films can exhibit electroluminescence (EL) through inelastic electron tunneling. The EL spectrum can be tuned by depositing a single-layer crystal of a transition-metal dichalcogenide (TMDC) on top. Whereas the emission from the gaps between silver or gold nanoparticles formed in the break junction is spectrally broad, the hybrid metal/TMDC structure shows distinct luminescence from the TMDC material. The EL from individual hotspots is found to be linearly polarized, with a polarization axis apparently oriented randomly. Surprisingly, the degree of polarization is retained in the EL from the TMDC monolayer at room temperature. In analogy to polarized photoluminescence experiments, such polarized EL can be interpreted as a signature of valley-selective transitions, suggesting that spin-flip transitions and dephasing for excitons in the K valleys are of limited importance. However, polarized EL may also originate from the metal nanoparticles formed under electromigration which constitute optical antenna structures. Such antennae can apparently change over time since jumps in the polarization are observed in bare silver-nanoparticle films. Remarkably, photon-correlation spectroscopy reveals that gold-nanoparticle films exhibit signatures of deterministic single-photon emission in the EL, suggesting a route to designing room-temperature polarized single-photon sources with tunable photon energy through the choice of TMDC overlayer.
贵金属薄膜中的断裂结可通过非弹性电子隧穿表现出电致发光(EL)。通过在顶部沉积过渡金属二硫属化物(TMDC)的单层晶体,可以调节EL光谱。在断裂结中形成的银或金纳米颗粒之间的间隙发射光谱较宽,而金属/TMDC混合结构则显示出TMDC材料独特的发光。发现来自单个热点的EL是线偏振的,偏振轴明显随机取向。令人惊讶的是,在室温下,TMDC单层的EL中仍保留着偏振度。类似于偏振光致发光实验,这种偏振EL可以解释为谷选择性跃迁的特征,这表明K谷中激子的自旋翻转跃迁和退相作用的重要性有限。然而,偏振EL也可能起源于电迁移过程中形成的金属纳米颗粒,这些颗粒构成了光学天线结构。由于在裸银纳米颗粒薄膜中观察到偏振的跳跃,这种天线显然会随时间变化。值得注意的是,光子相关光谱显示,金纳米颗粒薄膜在EL中表现出确定性单光子发射的特征,这表明通过选择TMDC覆盖层,有望设计出具有可调光子能量的室温偏振单光子源。