发表机构
Instituto de Ciencia Molecular, Universitat de València（瓦伦西亚大学分子科学研究所）
机构由 AI 辅助整理，请以论文原文为准。AI 中文总结
本研究通过密度泛函计算，提出利用自旋交叉机制在层状范德华MOFs中按需切换交变磁性，为可重构自旋电子器件提供了新平台。
AI 中文摘要
交变磁性的动态控制是将其独特的自旋相关功能转化为实用自旋电子器件的关键要求，然而有效的切换机制在很大程度上仍未得到探索。在此，我们开辟了一条基于自旋交叉的前所未有、通用且可编程的途径，用于按需切换分子材料中的交变磁性。利用密度泛函计算，我们证明了层状范德华MOFs MnX$_2$(tdz)$_2$（X = Cl, Br；tdz = 噻二唑）中存在交变磁性基态，该基态由各向异性的层间交换相互作用稳定，从而产生特征性的d波动量空间自旋劈裂以及相关的自旋劈裂器输运响应。我们的研究结果表明，在静水压力下，高自旋到低自旋的转变重新配置了Mn d轨道占据，从而改变了磁交换网络，并稳定了一个不同的反铁磁基态，其对称性抑制了非相对论性自旋劈裂。至关重要的是，自旋交叉不是通过直接改变电子结构，而是通过改变磁基态的对称性来切换交变磁性。这些结果确立了分子自旋交叉交变磁体作为外部可重构自旋电子器件平台的地位。
英文摘要
Dynamical control of altermagnetism is a key requirement for translating its unique spin-dependent functionalities into practical spintronic devices, yet effective switching mechanisms remain largely unexplored. Here, we open an unprecedented, versatile and programmable route based on spin-crossover to switch altermagnetism on demand in molecular materials. Using density functional calculations, we demonstrate an altermagnetic ground state in the layered van der Waals MOFs MnX$_2$(tdz)$_2$ (X = Cl, Br; tdz = thiadiazole), stabilized by anisotropic interlayer exchange interactions, which gives rise to a characteristic d-wave momentum-space spin splitting and an associated spin-splitter transport response. Our findings reveal that under hydrostatic pressure, a high-spin to low-spin transition reconfigures the Mn d-orbital occupation, thus modifying the magnetic exchange network, and stabilizing a different antiferromagnetic ground state whose symmetry suppresses the nonrelativistic spin splitting. Crucially, spin-crossover switches altermagnetism not by directly altering the electronic structure, but by changing the symmetry of the magnetic ground state. These results establish molecular spin-crossover altermagnets as a platform for externally reconfigurable spintronic devices.
