Modifying the Dzyaloshinskii-Moriya Interaction Via Disruption of Ordered Intercalation in a Van Der Waals Magnet.

Yangrui Liu, Jianxiong Zhang,Ying Liu,Jiadong Dan, Luyang Wang,Wei Liu,Lei Zhang, Fengshan Zheng,Haifeng Du,Binghui Ge,Jin-Zhu Zhao,Dongsheng Song

Nano Letters（2025）SCI 1区SCI 2区

NUS Centre for Bioimaging Sciences

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Abstract

The intercalation of magnetic atoms into van der Waals (vdW) gaps offers a unique opportunity to manipulate the Dzyaloshinskii-Moriya interaction (DMI) and magnetic structures by modifying the local atomic structures in vdW magnets. Herein, a new strategy is proposed for modifying DMI by disrupting the atomic-scale order within the Cr sublattice of Cr-intercalated 2H-TaS2, i.e., Cr1/3TaS2, which enables significant and efficient DMI modulation across a wide range by controlling the degree of atomic disorder. Lorentz transmission electron microscopy reveals pronounced variations in spin-helix periods, which are correlated with changes in the degree of Cr ordering within the vdW gaps, as shown by atomic-resolution imaging and principal component analysis. First-principles calculations confirm that this structural ordering affects the DMI strength, thereby notably altering the spin textures and magnetic transition behaviors. These findings are further supported by macroscopic magnetic measurements and micromagnetic simulations, highlighting new pathways for controlling magnetic properties of vdW materials.

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【要点】：论文提出了一种通过破坏层状范德瓦尔斯磁体中Cr子晶格的原子级有序性来调控Dzyaloshinskii-Moriya相互作用（DMI）的新策略，实现了DMI的显著和高效调制。

【方法】：通过控制Cr原子在范德瓦尔斯间隙中的有序程度，使用原子分辨率成像和主成分分析来观察Cr子晶格的有序性变化，结合第一性原理计算和宏观磁性测量来验证DMI强度的变化。

【实验】：实验采用Lorentz透射电子显微镜观测了Cr1/3TaS2中自旋螺旋周期的变化，并与原子分辨率成像和主成分分析结果相关联，同时使用宏观磁性测量和微磁模拟来支持研究结果。数据集来源于原子级成像和计算模拟的结果。