Magnetic transition metal dichalcogenide (TMD) films have recently emerged as promising candidates in hosting novel magnetic phases relevant to next-generation spintronic devices. However, systematic control of the magnetization orientation, or anisotropy, and its thermal stability characterized by Curie temperature $\left(T_{\mathrm{C}}\right)$, remains to be achieved in such films. Here we present self-intercalated epitaxial ${\mathrm{Cr}}_{1+\delta }{\mathrm{Te}}_2$ films as a platform for achieving systematic/smooth magnetic tailoring in TMD films. Using a molecular-beam epitaxy based technique, we have realized epitaxial ${\mathrm{Cr}}_{1+\delta }{\mathrm{Te}}_2$ films with smoothly tunable δ over a wide range (0.33–0.82), while maintaining NiAs-type crystal structure. With increasing δ, we found monotonic enhancement of $T_{\mathrm{C}}$ from 160 to 350 K, and the rotation of magnetic anisotropy from out-of-plane to in-plane easy-axis configuration for fixed film thickness. Contributions from conventional dipolar and orbital moment terms are insufficient to explain the observed evolution of magnetic behavior with δ. Instead, ab initio calculations suggest that the emergence of antiferromagnetic interactions with δ, and its interplay with conventional ferromagnetism, may play a key role in the observed trends. This demonstration of tunable $T_{\mathrm{C}}$ and magnetic anisotropy across room temperature in TMD films paves the way for engineering different magnetic phases for spintronic applications.

中文翻译：

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自嵌入Cr1 +δTe2外延膜的定制磁性

磁性过渡金属二硫化碳（TMD）膜最近成为托管与下一代自旋电子器件相关的新型磁性相的有前途的候选者。然而，以居里温度为特征的磁化取向或各向异性及其热稳定性的系统控制$（{Ť}_{\mathrm{C}}）$在此类影片中仍有待实现。在这里，我们介绍了自插外延${\mathrm{铬}}_{\mathrm{1个}+\delta }{\mathrm{特}}_2$薄膜作为在TMD薄膜中实现系统/平滑磁剪裁的平台。使用基于分子束外延的技术，我们实现了外延${\mathrm{铬}}_{\mathrm{1个}+\delta }{\mathrm{特}}_2$在保持NiAs型晶体结构的同时，在宽范围（0.33–0.82）范围内具有平滑可调δ的薄膜。随着δ的增加，我们发现单调增强${Ť}_{\mathrm{C}}$从160到350 K，磁各向异性从平面外旋转到平面内易轴配置，以固定膜厚度。传统偶极和轨道力矩项的贡献不足以解释观察到的磁行为随δ的变化。相反，从头算计算表明与δ的反铁磁相互作用的出现以及其与常规铁磁的相互作用可能在观察到的趋势中起关键作用。本示范可调${Ť}_{\mathrm{C}}$ TMD薄膜在室温下的磁各向异性以及为自旋电子应用工程化不同磁相铺平了道路。