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    Interlayer-coupling control of high-harmonic generation in bilayer WS2

    Xiaoteng Tang1, Zhongxue Ren1, Yue Lang1, Jing Zhao1,*, and Zengxiu Zhao1,2,3,†

    • 1College of Science, National University of Defense Technology, Changsha 410073, China
    • 2Hunan Key Laboratory of Extreme Matter and Applications, Changsha 410073, China
    • 3Hunan Research Center of the Basic Discipline for Physical States, Changsha 410073, China

    • *Contact author: jzhao@nudt.edu.cn
    • †Contact author: zhaozengxiu@nudt.edu.cn

    Phys. Rev. A 114, 033115 – Published 25 September, 2026

    DOI: https://doi.org/10.1103/yzdw-vsf5

    Abstract

    We investigate how interlayer coupling shapes high-harmonic generation (HHG) in AA-stacked bilayer WS2 using real-time time-dependent density functional theory and semiconductor Bloch equations. The bilayer harmonic yield is found to depart from the coherent layer-number enhancement expected for independent layers, with the departure growing continuously as the interlayer distance is reduced. We trace this behavior to coupling-induced band splitting, which opens two electron-hole recombination pathways whose relative dynamical phase is set by the interlayer coupling. As the coupling increases, the two pathways evolve from nearly constructive toward partially destructive interference. Time-frequency analysis and two-color field probing show that their recombination timing shifts accordingly. Interlayer coupling thus provides continuous structural control over recombination-pathway interference, allowing the amplitude, phase, and timing of solid-state high-harmonic emission to be tailored.

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