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    Moiré-Orbital-Resolved Excitonic Mott Insulating States and Their Optical and Electric Control in van der Waals Heterostructures

    Lanyu Huang1,2, Cuihuan Ge2, Boyi Xu2, Yufan Wang2, Siyao Li2, Xinyi Luo2, Haipeng Zhao2, Danliang Zhang2, Zhouxiaosong Zeng2 et al.

    Qingjun Tong2,*, Dong Li1, Xiaoli Zhu1, Kai Braun3, Tingge Gao4, Xiao Wang1,2,†, and Anlian Pan1,5,‡

    • 1Key Laboratory for Micro-Nano Physics and Technology of Hunan Province, College of Materials Science and Engineering, Hunan University, Changsha 410082, China
    • 2School of Physics and Electronics, Hunan University, Changsha 410082, China
    • 3Institute of Physical and Theoretical Chemistry and LISA+, University of Tübingen, Auf der Morgenstelle 18, 72076 Tübingen, Germany
    • 4Department of Physics, School of Science, Tianjin University, Tianjin 300072, China
    • 5School of Physics and Electronics, Hunan Normal University, Changsha 410081, China

    • *Contact author: tongqj@hnu.edu.cn
    • †Contact author: xiao_wang@hnu.edu.cn
    • ‡Contact author: anlian.pan@hnu.edu.cn

    Phys. Rev. Lett. 135, 096902 – Published 27 August, 2025

    DOI: https://doi.org/10.1103/gg98-1vhp

    Abstract

    Moiré potential formed in van der Waals heterostructures is predicted to feature multiple local minima functioning as orbital degree of freedom, which is an important ingredient for understanding intriguing strong correlation phenomena. However, an experimental demonstration of this moiré-orbital enabled quantum state engineering is still unexplored. Here, we report clear evidence of moiré-orbital resolved excitonic Mott insulating states in multiannealing H-type WSe2/WS2 heterobilayers and demonstrate their application in generating spatially ordered excitonic quantum phases. This moiré orbital is evidenced by interlayer exciton emissions with an energy separation of ∼65  meV and further supported by our multiple field-dependent characterizations. Remarkably, the moiré orbital allows a sequential formation of correlated Mott insulating states, with the extracted onsite Hubbard interaction reaching ∼30  meV. A combined optical and electric doping allows control of strongly correlated quantum phases with various spatially ordered fermionic-bosonic orbital components.

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