Atomically Unveiling the Phase Evolution in Weakly Coupled Layered Transition-Metal Phosphorus Trichalcogenide by Chalcogen Doping

IF 9.1 1区材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY

Nano Letters Pub Date : 2025-04-04 DOI:10.1021/acs.nanolett.5c00826

Wing Ni Cheng, Ruihuan Duan, Mengmeng Niu, Xiaocang Han, Song Huang, Yu Liang, Jun Zhao, Zheng Liu, Jingsi Qiao, Xiaoxu Zhao

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Abstract

The stacking configuration significantly influences the properties of van der Waals (vdW) layered magnets by dictating crystallographic and magnetic symmetries. Transition-metal phosphorus trichalcogenides (MPX₃, X = S, Se) intrinsically exhibit diverse stacking polytypes, being an optimal platform for magnetic phase engineering. Unlike MX₂, where chalcogen doping has a minimal impact on stacking, MPX₃ allows stacking control via elemental substitution. However, the atomic-scale mechanisms governing stacking variations remain unclear. Using scanning transmission electron microscopy (STEM) and density functional theory (DFT) calculations, we reveal that in 3d transition metal MPX₃, tuning the S/Se ratio induces a transition from the C2/m to R3̅ phase due to modified interlayer S–S/Se–Se and P–P interactions. In contrast, stacking control becomes challenging for 4d CdPX₃, due to relatively weak interlayer coupling. These insights provide a stacking basis for stacking polytypes in MPX₃, paving the way for tuning magnetic couplings via stackingtronics.

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用硫掺杂原子揭示弱耦合层状过渡金属三卤代磷的相演化

堆叠构型通过决定晶体学和磁对称性，对范德华（vdW）层状磁体的特性产生重大影响。过渡金属磷三钙化物（MPX3，X = S、Se）本质上表现出多种堆叠多型性，是磁相工程的最佳平台。与 MX2 不同，MPX3 允许通过元素替代来控制堆叠，而 MX2 中掺杂的查尔根对堆叠的影响微乎其微。然而，有关堆叠变化的原子尺度机制仍不清楚。利用扫描透射电子显微镜（STEM）和密度泛函理论（DFT）计算，我们揭示了在 3d 过渡金属 MPX3 中，由于层间 S-Se/Se-Se 和 P-P 相互作用的改变，调整 S/Se 比率可诱导从 C2/m 到 R3̅ 相的转变。相比之下，由于层间耦合相对较弱，4d CdPX3 的堆叠控制变得具有挑战性。这些见解为 MPX3 的堆叠多类型提供了堆叠基础，为通过堆叠电子学调整磁耦合铺平了道路。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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来源期刊

Nano Letters 工程技术-材料科学：综合

CiteScore

16.80

自引率

2.80%

发文量

1182

审稿时长

1.4 months

期刊介绍： Nano Letters serves as a dynamic platform for promptly disseminating original results in fundamental, applied, and emerging research across all facets of nanoscience and nanotechnology. A pivotal criterion for inclusion within Nano Letters is the convergence of at least two different areas or disciplines, ensuring a rich interdisciplinary scope. The journal is dedicated to fostering exploration in diverse areas, including: - Experimental and theoretical findings on physical, chemical, and biological phenomena at the nanoscale - Synthesis, characterization, and processing of organic, inorganic, polymer, and hybrid nanomaterials through physical, chemical, and biological methodologies - Modeling and simulation of synthetic, assembly, and interaction processes - Realization of integrated nanostructures and nano-engineered devices exhibiting advanced performance - Applications of nanoscale materials in living and environmental systems Nano Letters is committed to advancing and showcasing groundbreaking research that intersects various domains, fostering innovation and collaboration in the ever-evolving field of nanoscience and nanotechnology.