AI 中文总结
研究针对室温自旋光电器件的性能瓶颈，利用团簇组装的V4S9X4二维磁性半导体，实现了兼具强铁磁性与巨激子结合能的特性，可用于制备室温自旋光子及量子信息器件。
AI 中文摘要
室温自旋光电器件需要兼具强铁磁性和巨激子结合能，但传统半导体中因磁性局域会屏蔽激子，二者难以共存，形成了瓶颈。团簇组装的V4S9X4（X=F、Cl、Br、I）单分子层通过分级设计突破该瓶颈：团簇内局域态同时承载局域磁矩和强电子-空穴相互作用，团簇间耦合介导长程铁磁性。这些二维半导体具有本征铁磁性，居里温度最高达507.6 K。以V4S9Br4单分子层为例，其巨激子结合能为1.85 eV，最低激子为暗态（DI），辐射寿命1.20 ns；首个亮激子（BI）则表现出86.87 ps的超快辐射衰减，这种显著的寿命对比可实现超快光学响应与长寿命自旋信息存储的同步。最值得注意的是，铁磁与反铁磁序的切换可对激子寿命进行宽范围调控，且巨结合能几乎保持不变。本研究确立了团簇组装为设计下一代室温自旋光子及量子信息器件的强大范式。
英文摘要
Room-temperature spin-optoelectronic devices require a combination of robust ferromagnetism and giant exciton binding, a pairing mutually exclusive in conventional semiconductors due to magnetic localization that screens excitons. Cluster-assembled V4S9X4 (X = F, Cl, Br and I) monolayers overcome this bottleneck via a hierarchical design, that is, intra-cluster localized states host both local magnetic moments and strong electron-hole interactions, while inter-cluster coupling mediates long-range ferromagnetism. Remarkably, these two-dimensional semiconductors exhibit intrinsic ferromagnetism with Curie temperature up to 507.6 K. As a prototype, V4S9Br4 monolayer possesses a giant exciton binding energy of 1.85 eV. Its lowest exciton is a dark state (DI) with a radiative lifetime of 1.20 ns, whereas the first bright exciton (BI) exhibits an ultrafast radiative decay of 86.87 ps. This stark lifetime contrast enables simultaneous ultrafast optical response and long-lived spin information storage. Most notably, switching between ferromagnetic and antiferromagnetic order allows for wide-range tuning of exciton lifetime, with the giant binding energy remaining nearly intact. Our findings establish cluster assembly as a powerful paradigm for designing next-generation spin-photonic and quantum information devices operating at room temperature.
