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    Structural evolution and continuous band-gap narrowing in layered-like framework LaCuS2 under pressure

    Boyang Fu1, Wenbo Qiu1, Shuangjiang Du1, Junhui Liang1, Long Zhang1,*, Fuyang Liu2, Luhong Wang3, Haozhe Liu2, and Weizhao Cai1,†

    • *Contact author: zhangl@uestc.edu.cn
    • †Contact author: wzhcai@uestc.edu.cn

    Phys. Rev. B 114, 214102 – Published 5 October, 2026

    DOI: https://doi.org/10.1103/hx9l-y2xj

    Abstract

    LaCuS2 is a Cu-based rare-earth chalcogenide semiconductor whose structural robustness and pressure-dependent electronic evolution remain largely unexplored. Here, we investigate its structural, optical, and transport properties under compression by combining high-pressure experiments with first-principles calculations. LaCuS2 retains its monoclinic P21/c structure up to 70.1 GPa without the emergence of a phase transition. Nevertheless, compression induces subtle local structural reorganization, including Cu-site disordering-to-ordering and an anisotropic lattice anomaly near 5.0 GPa associated with flattening of the corrugated corner-sharing Cu2S6 layers. Concurrently, the optical band-gap decreases continuously from 2.39 to 0.93 eV upon compression to 48.6 GPa, accompanied by distinct piezochromism and a progressive redshift of the photoluminescence emission. First-principles calculations reveal that the band-gap narrowing originates from the continuous evolution of the Cu 3d−S 3p derived valence states and La 5d derived conduction states under compression. Electrical transport measurements show that LaCuS2 remains semiconducting up to 64.1 GPa, while photocurrent retains the same polarity throughout the investigated pressure range. These results establish LaCuS2 as an unusual pressure-robust semiconductor in which substantial band-edge engineering is achieved through continuous local structural evolution without a phase transformation, providing a model system for exploring pressure-induced electronic tuning in Cu-based rare-earth chalcogenides.

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