School of Physics and Astronomy, The University of Manchester , Manchester M13 9PL, U.K.
ACS Nano. 2015 Dec 22;9(12):12004-10. doi: 10.1021/acsnano.5b04804. Epub 2015 Nov 4.
We report the dynamics of photoinduced carriers in a free-standing MoS2 laminate consisting of a few layers (1-6 layers) using time-resolved optical pump-terahertz probe spectroscopy. Upon photoexcitation with the 800 nm pump pulse, the terahertz conductivity increases due to absorption by the photoinduced charge carriers. The relaxation of the non-equilibrium carriers shows fast as well as slow decay channels, analyzed using a rate equation model incorporating defect-assisted Auger scattering of photoexcited electrons, holes, and excitons. The fast relaxation time occurs due to the capture of electrons and holes by defects via Auger processes, resulting in nonradiative recombination. The slower relaxation arises since the excitons are bound to the defects, preventing the defect-assisted Auger recombination of the electrons and the holes. Our results provide a comprehensive understanding of the non-equilibrium carrier kinetics in a system of unscreened Coulomb interactions, where defect-assisted Auger processes dominate and should be applicable to other 2D systems.
我们使用时间分辨光泵太赫兹探针光谱法报告了由几层(1-6 层)组成的独立 MoS2 层压板中光致载流子的动力学。在 800nm 泵浦脉冲的光激发下,由于光致电荷载流子的吸收,太赫兹电导率增加。使用包含缺陷辅助光激电子、空穴和激子的俄歇散射的速率方程模型分析了非平衡载流子的弛豫,表现出快速和缓慢的衰减通道。快速弛豫时间是由于电子和空穴通过俄歇过程被缺陷捕获,导致非辐射复合。较慢的弛豫是由于激子与缺陷结合,阻止了电子和空穴的缺陷辅助俄歇复合。我们的结果提供了对非屏蔽库仑相互作用体系中非平衡载流子动力学的全面理解,其中缺陷辅助俄歇过程占主导地位,并且应该适用于其他二维体系。