以原子方式揭示过渡金属三卤化物中的多型图谱,Journal of the American Chemical Society

当前位置： X-MOL 学术 › J. Am. Chem. Soc. › 论文详情

Our official English website, www.x-mol.net, welcomes your feedback! (Note: you will need to create a separate account there.)

以原子方式揭示过渡金属三卤化物中的多型图谱
Journal of the American Chemical Society ( IF 14.4 ) Pub Date : 2023-02-03 , DOI: 10.1021/jacs.2c12801
Xiaocang Han ₁ , Jing-Yang You ₂ , Shengqiang Wu ₁ , Runlai Li ₃ , Yuan Ping Feng ₂ , Kian Ping Loh ₄ , Xiaoxu Zhao ₁

Affiliation

过渡金属三卤化物 MX ₃（M = Cr、Ru；X = Cl、Br 和 I）属于新型二维 (2D) 磁体家族，具有拓扑磁振子和电磁特性，因此在未来具有广阔前景代自旋电子器件。_{在 MX 3}系列中观察到的丰富磁性基态被认为与标志性的 Kagome 晶格和从不同堆叠顺序产生的层间范德华耦合密切相关。_{然而，MX 3}固有的空气不稳定性使其直接原子级分析具有挑战性。_{因此，有关 MX 3}的堆叠注册表相关磁性的信息仍然难以捉摸，这极大地阻碍了所需阶段的工程。_{在这里，我们报告了一种无损转移方法并成功实现了双层 MX 3}的完整转移，扫描透射电子显微镜 (STEM) 证明了这一点。在调查了数百个 MX _{3薄片之后，我们提供了 MX}₃中具有原子精度的完整堆叠顺序谱，并计算了它们相关的磁性基态，结合 STEM 和密度泛函理论 (DFT) 揭示了这一点。除了有据可查的相外，我们还在MX ₃中广泛存在的反铁磁 (AFM) 结构中发现了一种新的单斜晶系C 2/ c相。丰富的堆叠多类型，包括C2/ c、C 2/ m、R 3̅ 、P 3 ₁ 12等在 MX ₃中提供丰富而独特的磁性基态。_{此外，在所有 MX 3}中始终发现高密度的应变孤子边界，结合可能的倒置结构，允许在大多数 MX ₃中进行 AFM 到铁磁 (FM) 跃迁。因此，我们的研究阐明了 MX _{3中不同磁阶的结构基础，为}通过堆叠工程调制磁耦合铺平了道路。

"点击查看英文标题和摘要"

Atomically Unveiling an Atlas of Polytypes in Transition-Metal Trihalides

Transition-metal trihalides MX₃ (M = Cr, Ru; X = Cl, Br, and I) belong to a family of novel two-dimensional (2D) magnets that can exhibit topological magnons and electromagnetic properties, thus affording great promises in next-generation spintronic devices. Rich magnetic ground states observed in the MX₃ family are believed to be strongly correlated to the signature Kagome lattice and interlayer van der Waals coupling raised from distinct stacking orders. However, the intrinsic air instability of MX₃ makes their direct atomic-scale analysis challenging. Therefore, information on the stacking-registry-dependent magnetism for MX₃ remains elusive, which greatly hinders the engineering of desired phases. Here, we report a nondestructive transfer method and successfully realize an intact transfer of bilayer MX₃, as evidenced by scanning transmission electron microscopy (STEM). After surveying hundreds of MX₃ thin flakes, we provide a full spectrum of stacking orders in MX₃ with atomic precision and calculated their associated magnetic ground states, unveiled by combined STEM and density functional theory (DFT). In addition to well-documented phases, we discover a new monoclinic C2/c phase in the antiferromagnetic (AFM) structure widely existing in MX₃. Rich stacking polytypes, including C2/c, C2/m, R3̅, P3₁12, etc., provide rich and distinct magnetic ground states in MX₃. Besides, a high density of strain soliton boundaries is consistently found in all MX₃, combined with likely inverted structures, allowing AFM to ferromagnetic (FM) transitions in most MX₃. Therefore, our study sheds light on the structural basis of diverse magnetic orders in MX₃, paving the way for modulating magnetic couplings via stacking engineering.

更新日期：2023-02-03

点击分享查看原文

点击收藏

阅读更多本刊新发论文本刊介绍/投稿指南