Ultrafast formation of interlayer hot excitons in atomically thin MoS2/WS2 heterostructures

Hailong Chen, Xiewen Wen, Jing Zhang, Tianmin Wu, Yongji Gong, Xiang Zhang, Jiangtan Yuan, Chongyue Yi, Jun Lou, Pulickel M. Ajayan, Wei Zhuang (), Guangyu Zhang () and Junrong Zheng ()
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Hailong Chen: College of Chemistry and Molecular Engineering, Beijing National Laboratory for Molecular Sciences, Peking University
Xiewen Wen: College of Chemistry and Molecular Engineering, Beijing National Laboratory for Molecular Sciences, Peking University
Jing Zhang: Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences
Tianmin Wu: University of Science and Technology of China
Yongji Gong: Rice University
Xiang Zhang: Rice University
Jiangtan Yuan: Rice University
Chongyue Yi: Rice University
Jun Lou: Rice University
Pulickel M. Ajayan: Rice University
Wei Zhuang: State Key Laboratory of Structural Chemistry, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences
Guangyu Zhang: Beijing National Laboratory for Condensed Matter Physics and Institute of Physics, Chinese Academy of Sciences
Junrong Zheng: College of Chemistry and Molecular Engineering, Beijing National Laboratory for Molecular Sciences, Peking University

Nature Communications, 2016, vol. 7, issue 1, 1-8

Abstract: Abstract Van der Waals heterostructures composed of two-dimensional transition-metal dichalcogenides layers have recently emerged as a new family of materials, with great potential for atomically thin opto-electronic and photovoltaic applications. It is puzzling, however, that the photocurrent is yielded so efficiently in these structures, despite the apparent momentum mismatch between the intralayer/interlayer excitons during the charge transfer, as well as the tightly bound nature of the excitons in 2D geometry. Using the energy-state-resolved ultrafast visible/infrared microspectroscopy, we herein obtain unambiguous experimental evidence of the charge transfer intermediate state with excess energy, during the transition from an intralayer exciton to an interlayer exciton at the interface of a WS2/MoS2 heterostructure, and free carriers moving across the interface much faster than recombining into the intralayer excitons. The observations therefore explain how the remarkable charge transfer rate and photocurrent generation are achieved even with the aforementioned momentum mismatch and excitonic localization in 2D heterostructures and devices.

Date: 2016
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DOI: 10.1038/ncomms12512

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