Walter Schottky Institute and Physics-Department, Technical University of Munich, Am Coulombwall 4a, 85748, Garching, Germany.
Nanosystems Initiative Munich (NIM), Schellingstr. 4, 80799, München, Germany.
Nat Commun. 2019 Feb 18;10(1):807. doi: 10.1038/s41467-019-08764-3.
Charge carriers in semiconducting transition metal dichalcogenides possess a valley degree of freedom that allows for optoelectronic applications based on the momentum of excitons. At elevated temperatures, scattering by phonons limits valley polarization, making a detailed knowledge about strength and nature of the interaction of excitons with phonons essential. In this work, we directly access exciton-phonon coupling in charge tunable single layer MoS devices by polarization resolved Raman spectroscopy. We observe a strong defect mediated coupling between the long-range oscillating electric field induced by the longitudinal optical phonon in the dipolar medium and the exciton. This so-called Fröhlich exciton phonon interaction is suppressed by doping. The suppression correlates with a distinct increase of the degree of valley polarization up to 20% even at elevated temperatures of 220 K. Our result demonstrates a promising strategy to increase the degree of valley polarization towards room temperature valleytronic applications.
在半导体过渡金属二卤族化合物中,电荷载流子具有谷自由度,这使得基于激子动量的光电器件应用成为可能。在高温下,声子的散射限制了谷极化,因此详细了解激子与声子相互作用的强度和性质是至关重要的。在这项工作中,我们通过偏振分辨拉曼光谱直接研究了可调控电荷的单层 MoS 器件中的激子-声子耦合。我们观察到在偶极介质中长程振荡的纵向光学声子诱导的电场与激子之间存在很强的缺陷介导耦合。这种所谓的 Fröhlich 激子-声子相互作用被掺杂所抑制。这种抑制与谷极化度的明显增加相关,即使在 220 K 的高温下,谷极化度也高达 20%。我们的结果表明了一种很有前途的策略,即通过增加谷极化度来实现室温谷电子学应用。