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    Band-spin-valley coupled exciton physics in antiferromagnetic MnPS3

    Dan Wang1, Haowei Chen1, Yu Pang2, Xiaolong Zou2,*, and Wenhui Duan1,3,4

    • 1State Key Laboratory of Low Dimensional Quantum Physics and Department of Physics, Tsinghua University, Beijing 100084, People’s Republic of China
    • 2Shenzhen Geim Graphene Center & Shenzhen Key Laboratory of Advanced Layered Materials for Value-added Applications, Institute of Materials Research, Tsinghua Shenzhen International Graduate School, Tsinghua University, Shenzhen 518055, People's Republic of China
    • 3Institute for Advanced Study, Tsinghua University, Beijing 100084, People's Republic of China
    • 4Frontier Science Center for Quantum Information, Beijing 100084, People's Republic of China

    • *Contact author: xlzou@sz.tsinghua.edu.cn

    Phys. Rev. B 112, 075306 – Published 26 August, 2025

    DOI: https://doi.org/10.1103/wbnk-ywn2

    Abstract

    The introduction of intrinsic magnetic order in two-dimensional (2D) semiconductors offers great opportunities for investigating correlated excitonic phenomena. Here, we employ full-spinor GW plus Bethe-Salpeter equation methodology to reveal rich exciton physics in a prototypical 2D Néel-type antiferromagnetic semiconductor MnPS3, enabled by the interplay among inverted dispersion of the second valence band, spin-valley coupling and magnetic order. The negative hole mass increases the reduced mass of the lowest-energy bright exciton, leading to exchange splitting enhancement of the bright exciton relative to band-edge dark exciton. Notably, such splitting couples with spontaneous valley polarization to generate distinct excitonic fine structure between K and −K valleys, which dictate distinct relaxation behaviors. Crucially, magnetic order transition from Néel antiferromagnetic to ferromagnetic state induces significant quasiparticle band structure reconstruction and excitonic transitions modification, with low-energy optical excitations being exclusively contributed by majority-spin channel. These findings establish 2D antiferromagnetic semiconductors as an intriguing platform to study band-spin-valley coupled exciton physics.

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