Slow cooling and efficient extraction of C-exciton hot carriers in MoS2 monolayer

Lei Wang, Zhuo Wang, Hai-Yu Wang (), Gustavo Grinblat, Yu-Li Huang, Dan Wang, Xiao-Hui Ye, Xian-Bin Li, Qiaoliang Bao, AndrewThye-Shen Wee, Stefan A Maier, Qi-Dai Chen, Min-Lin Zhong, Cheng-Wei Qiu () and Hong-Bo Sun ()
Additional contact information
Lei Wang: State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University
Zhuo Wang: National University of Singapore
Hai-Yu Wang: State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University
Gustavo Grinblat: The Blackett Laboratory, Imperial College London
Yu-Li Huang: National University of Singapore
Dan Wang: State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University
Xiao-Hui Ye: Laser Materials Processing Research Center, School of Materials Science and Engineering, Tsinghua University
Xian-Bin Li: State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University
Qiaoliang Bao: Monash University
AndrewThye-Shen Wee: National University of Singapore
Stefan A Maier: The Blackett Laboratory, Imperial College London
Qi-Dai Chen: State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University
Min-Lin Zhong: Laser Materials Processing Research Center, School of Materials Science and Engineering, Tsinghua University
Cheng-Wei Qiu: National University of Singapore
Hong-Bo Sun: State Key Laboratory on Integrated Optoelectronics, College of Electronic Science and Engineering, Jilin University

Nature Communications, 2017, vol. 8, issue 1, 1-8

Abstract: Abstract 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 MoS2 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 MoS2 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.

Date: 2017
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DOI: 10.1038/ncomms13906

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