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Band alignment and interlayer hybridization in monolayer organic/WSe2 heterojunction

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Abstract

Semiconducting heterojunctions (HJs), comprised of atomically thin transition metal dichalcogenides (TMDs), have shown great potentials in electronic and optoelectronic applications. Organic/TMD hybrid bilayers hold enhanced pumping efficiency of interfacial excitons, tunable electronic structures and optical properties, and other superior advantages to these inorganic HJs. Here, we report a direct probe of the interfacial electronic structures of a crystalline monolayer (ML) perylene-3,4,9,10-tetracarboxylic-dianhydride (PTCDA)/ML-WSe2 HJ using scanning tunneling microscopy, photoluminescence, and first-principle calculations. Strong PTCDA/WSe2 interfacial interactions lead to appreciable hybridization of the WSe2 conduction band with PTCDA unoccupied states, accompanying with a significant amount of PTCDA-to-WSe2 charge transfer (by 0.06 e/PTCDA). A type-II band alignment was directly determined with a valence band offset of ∼ 1.69 eV, and an apparent conduction band offset of ∼ 1.57 eV. Moreover, we found that the local stacking geometry at the HJ interface differentiates the hybridized interfacial states.

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Acknowledgements

This work was supported by the National Key R&D Program of China (Nos. 2018FYA0305800 and 2018YFA0703700), the National Natural Science Foundation of China (Nos. 11774268 and 11974012), and the Strategic Priority Research Program of Chinese Academy of Sciences (No. XDB30000000). W. J. gratefully acknowledges financial support from the Fundamental Research Funds for the Central Universities, China, and the Research Funds of Renmin University of China (Nos. 16XNLQ01 and 19XNQ025). Calculations were performed at the Physics Lab of High-Performance Computing of Renmin University of China, Shanghai Supercomputer Center.

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  1. Yanping Guo, Linlu Wu, and Jinghao Deng contributed equally to this work.

Authors and Affiliations

  1. Key Laboratory of Artificial Micro- and Nano-structures of Ministry of Education and School of Physics and Technology, Wuhan University, Wuhan, 430027, China

    Yanping Guo, Jinghao Deng, Wei Jiang, Shuangzan Lu, Da Huo, Jiamin Ji, Yusong Bai, Xiaoyu Lin, Shunping Zhang, Hongxing Xu & Chendong Zhang

  2. Department of Physics and Beijing Key Laboratory of Optoelectronic Functional Materials and Micro-Nano Devices, Renmin University of China, Beijing, 100872, China

    Linlu Wu, Linwei Zhou & Wei Ji

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  1. Yanping Guo
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Guo, Y., Wu, L., Deng, J. et al. Band alignment and interlayer hybridization in monolayer organic/WSe2 heterojunction. Nano Res. 15, 1276–1281 (2022). https://doi.org/10.1007/s12274-021-3648-9

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