Auger‐Assisted Secondary Hot Carrier Transfer in a Type I MoS2/PtSe2 Heterostructure

Author:

Yang Jin1,Gong Shaokuan2,Zhang Xiaguang3,Liu Jianxun4,Luo Wen1,Lu Zhouguang1,Liu Yanjun4,Chen Xihan2,Lienau Christoph5ORCID,Zhong Jin‐Hui1

Affiliation:

1. Department of Materials Science and Engineering Southern University of Science and Technology Shenzhen 518055 China

2. SUSTech Energy Institute for Carbon Neutrality Department of Mechanical and Energy Engineering Southern University of Science and Technology Shenzhen 518055 China

3. Key Laboratory of Green Chemical Media and Reactions Ministry of Education Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals College of Chemistry and Chemical Engineering Henan Normal University Xinxiang 453007 China

4. Department of Electrical and Electronic Engineering Southern University of Science and Technology Shenzhen 518055 China

5. Institut für Physik Carl von Ossietzky Universität 26129 Oldenburg Germany

Abstract

AbstractCharge transfer is vital in determining the optoelectronic properties of atomically thin materials, yet remains elusive in type I heterostructures. Here, distinct two‐step charge transfer processes in a type I MoS2/PtSe2 heterostructure are reported. By exclusively exciting the smaller bandgap PtSe2, strong exciton photobleaching peaks of the larger bandgap MoS2 are observed, indicating primary hot carrier transfer from PtSe2 to MoS2 within 70 fs. More importantly, the amplitude of the exciton peaks shows a secondary increase after the initial rapid decay. These dynamics are distinctly different from the monotonic decrease in monolayer MoS2 and indicate a secondary charge transfer process that is attributed to hot carriers re‐generated in PtSe2 by intralayer Auger recombination. Concurrently, the exciton energy blue shifts within 100 ps, probing the dynamic buildup of a charge‐transfer induced electric field across the heterostructure interface, which displaces electron and hole wavefunctions of MoS2 excitons and reduces the exciton binding energy. The results are corroborated by carrier dynamics and transient absorption spectra simulations by considering the two‐step charge transfer processes. The work reveals Auger‐assisted hot carrier transfer processes in type I heterostructures and suggests the possibility for optoelectronic and photocatalytic applications by optical sub‐bandgap excitation.

Funder

National Natural Science Foundation of China

Basic and Applied Basic Research Foundation of Guangdong Province

Shenzhen Science and Technology Innovation Program

National Basic Research Program of China

Natural Science Foundation of Henan Province

China Postdoctoral Science Foundation

Niedersächsische Ministerium für Wissenschaft und Kultur

Volkswagen Foundation

Publisher

Wiley

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