Kaviraj Bhaskar, Sahoo Dhirendra
Department of Physics, School of Natural Sciences, Shiv Nadar University NH91, Gautam Budh Nagar Greater Noida Uttar Pradesh 201314 India
RSC Adv. 2019 Aug 16;9(44):25439-25461. doi: 10.1039/c9ra03769a. eCollection 2019 Aug 13.
Two-dimensional (2D) group-VI transition metal dichalcogenide (TMD) semiconductors, such as MoS, MoSe, WS and others manifest strong light matter coupling and exhibit direct band gaps which lie in the visible and infrared spectral regimes. These properties make them potentially interesting candidates for applications in optics and optoelectronics. The excitons found in these materials are tightly bound and dominate the optical response, even at room temperatures. Large binding energies and unique exciton fine structure make these materials an ideal platform to study exciton behaviors in two-dimensional systems. This review article mainly focuses on studies of mechanisms that control dynamics of excitons in 2D systems - an area where there remains a lack of consensus in spite of extensive research. Firstly, we focus on the kinetics of dark and bright excitons based on a rate equation model and discuss on the role of previous 'unsuspected' dark excitons in controlling valley polarization. Intrinsically, dark and bright exciton energy splitting plays a key role in modulating the dynamics. In the second part, we review the excitation energy-dependent possible characteristic relaxation pathways of photoexcited carriers in monolayer and bilayer systems. In the third part, we review the extrinsic factors, in particular the defects that are so prevalent in single layer TMDs, affecting exciton dynamics, transport and non-radiative recombination such as exciton-exciton annihilation. Lastly, the optical response due to pump-induced changes in TMD monolayers have been reviewed using femtosecond pump-probe spectroscopy which facilitates the analysis of underlying physical process after the excitation.
二维(2D)的VI族过渡金属二硫属化物(TMD)半导体,如MoS、MoSe、WS等,表现出强烈的光与物质耦合,并呈现出位于可见光和红外光谱区域的直接带隙。这些特性使其成为光学和光电子学应用中潜在的有趣候选材料。在这些材料中发现的激子束缚紧密,即使在室温下也主导着光学响应。大的结合能和独特的激子精细结构使这些材料成为研究二维系统中激子行为的理想平台。这篇综述文章主要关注二维系统中控制激子动力学机制的研究——尽管进行了广泛研究,但在这个领域仍缺乏共识。首先,我们基于速率方程模型关注暗激子和亮激子的动力学,并讨论先前“未被怀疑”的暗激子在控制谷极化中的作用。本质上,暗激子和亮激子的能量分裂在调节动力学中起着关键作用。在第二部分,我们综述了单层和双层系统中光激发载流子与激发能量相关的可能特征弛豫途径。在第三部分,我们综述了外部因素,特别是单层TMD中普遍存在的缺陷,这些缺陷会影响激子动力学、传输和非辐射复合,如激子 - 激子湮灭。最后,使用飞秒泵浦 - 探测光谱对TMD单层中泵浦诱导变化引起的光学响应进行了综述,这有助于分析激发后潜在的物理过程。