State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University, 2699 Qianjin Street, Changchun 130012, China.
Department of Electrical &Computer Engineering, National University of Singapore, 4 Engineering Drive 3, Singapore 117583, Singapore.
Nat Commun. 2017 Jan 5;8:13906. doi: 10.1038/ncomms13906.
In emerging optoelectronic applications, such as water photolysis, exciton fission and novel photovoltaics involving low-dimensional nanomaterials, hot-carrier relaxation and extraction mechanisms play an indispensable and intriguing role in their photo-electron conversion processes. Two-dimensional transition metal dichalcogenides have attracted much attention in above fields recently; however, insight into the relaxation mechanism of hot electron-hole pairs in the band nesting region denoted as C-excitons, remains elusive. Using MoS monolayers as a model two-dimensional transition metal dichalcogenide system, here we report a slower hot-carrier cooling for C-excitons, in comparison with band-edge excitons. We deduce that this effect arises from the favourable band alignment and transient excited-state Coulomb environment, rather than solely on quantum confinement in two-dimension systems. We identify the screening-sensitive bandgap renormalization for MoS monolayer/graphene heterostructures, and confirm the initial hot-carrier extraction for the C-exciton state with an unprecedented efficiency of 80%, accompanied by a twofold reduction in the exciton binding energy.
在新兴的光电应用中,如水的光解、激子分裂以及涉及低维纳米材料的新型光伏技术,热载流子弛豫和提取机制在其光电转换过程中起着不可或缺的作用。二维过渡金属二硫属化物在上述领域引起了广泛关注;然而,对于带嵌套区域(C-激子)中热电子-空穴对的弛豫机制,仍不清楚。本文使用 MoS 单层作为二维过渡金属二硫属化物体系的模型,报告了 C-激子的热载流子冷却速度比带边激子慢。我们推断,这种效应源于有利的能带排列和瞬态激发态库仑环境,而不仅仅是二维体系中的量子限制。我们确定了 MoS 单层/石墨烯异质结构的屏蔽敏感带隙重整化,并通过前所未有的 80%的初始热载流子提取效率证实了 C-激子态的初始热载流子提取,同时激子结合能降低了两倍。