Despite extensive studies on magnetic proximity effects, the fundamental excitonic properties of the 2D semiconductor‐magnet heterostructures remain elusive. Here, the presence of localized excitons in MoSe2/CrSBr heterostructures is unveiled, represented by a new photoluminescence emission feature, X*. Our findings reveal that X* originates from excitons confined by intrinsic defects in the CrSBr layer. Additionally, the degrees of valley polarization of the X* and trion peaks exhibit opposite polarities under a magnetic field and closely correlate with the magnetic order of CrSBr. This is attributed to spin‐dependent charge transfer across the heterointerface, supported by density functional theory calculations which reveal a type‐II band alignment. Furthermore, the strong in‐plane anisotropy of CrSBr induces unique polarization‐dependent responses in MoSe2 emissions. This study highlights the crucial role of defects in shaping excitonic properties and offers valuable insights into spectrally resolved proximity effects in semiconductor‐magnet van der Waals heterostructures.

中文翻译：

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MoSe2/CrSBr 异质结构中的内禀定位激子


尽管对磁邻近效应进行了广泛的研究，但 2D 半导体-磁体异质结构的基本激子特性仍然难以捉摸。在这里，揭示了 MoSe₂/CrSBr 异质结构中局域激子的存在，由新的光致发光发射特征 X^* 表示。我们的研究结果表明，X^* 起源于 CrSBr 层中受本征缺陷限制的激子。此外，X^* 和 trion 峰的谷极化程度在磁场下表现出相反的极性，与 CrSBr 的磁序密切相关。这归因于跨异质界面的自旋依赖性电荷转移，并得到密度泛函理论计算的支持，该计算揭示了 II 型能带对齐。此外，CrSBr 的强面内各向异性在 MoSe₂ 发射中诱导独特的偏振依赖性响应。这项研究强调了缺陷在塑造激子特性中的关键作用，并为半导体-磁体范德华异质结构中的光谱分辨邻近效应提供了有价值的见解。