Scharf Benedikt, Perebeinos Vasili
Institute for Theoretical Physics and Astrophysics and Würzburg-Dresden Cluster of Excellence ct.qmats, University of Würzburg, Am Hubland, 97074 Würzburg, Germany.
Department of Electrical Engineering, University at Buffalo, Buffalo, New York 14228, USA.
J Chem Phys. 2024 Oct 7;161(13). doi: 10.1063/5.0230578.
The competition between the radiative and nonradiative lifetimes determines the optical quantum yield and plays a crucial role in the potential optoelectronic applications of transition metal dichalcogenides (TMDCs). Here, we show that, in the presence of free carriers, an additional nonradiative decay channel opens for excitons in TMDC monolayers. Although the usual Auger decay channel is suppressed at low doping levels by the simultaneous momentum and energy conservation laws, exciton-phonon coupling relaxes this suppression. By solving a Bethe-Salpeter equation, we calculate the phonon-assisted Auger decay rates in four typical TMDCs as a function of doping, temperature, and dielectric environment. We find that even for a relatively low doping of 1012 cm-2, the nonradiative lifetime ranges from 16 to 165 ps in different TMDCs, offering competition to the radiative decay channel.
辐射寿命和非辐射寿命之间的竞争决定了光学量子产率,并且在过渡金属二硫属化物(TMDCs)潜在的光电子应用中起着至关重要的作用。在此,我们表明,在存在自由载流子的情况下,TMDC单层中的激子会开启一个额外的非辐射衰变通道。尽管通常的俄歇衰变通道在低掺杂水平下会因动量和能量守恒定律同时作用而受到抑制,但激子 - 声子耦合会缓解这种抑制。通过求解贝特 - 萨尔皮特方程,我们计算了四种典型TMDCs中声子辅助的俄歇衰变率随掺杂、温度和介电环境的变化关系。我们发现,即使对于相对较低的10^12 cm^-2掺杂水平,不同TMDCs中的非辐射寿命在16到165皮秒之间,这对辐射衰变通道构成了竞争。