Xiang Xu#, Pengbin Liu#, Cong Wang#, Yudi Dai#, Bin Cheng#, Yan Jiang#, Hao Luo, Jinsong Wu, Shi-Jun Liang, Wei Ji*, Feng Miao*, Tianyou Zhai*, and Xing Zhou*
Abstract:
Two-dimensional (2D) lateral magnetic heterostructures offer a promising platform for exploring interfacial magnetism and related physical phenomena. Current synthesis strategies primarily rely on sequential edge-epitaxy. However, the second-step chemical vapor deposition process inevitably introduces various interfacial defects, disrupting the intrinsic magnetic properties. Here we propose an interface-driven endotaxy method that enables the synthesis of 2D lateral magnetic heterostructures (e.g., CuCrSe2, CuCr2Se4, AgCrSe2-CrSe2, CuCrS2-CuCr2S4) with atomically sharp interfaces. The growth of the second phase is triggered by a controlled interfacial phase transition, as revealed by in situ imaging of the growth, systematic microstructure characterizations, and theoretical calculations. The obtained heterointerfaces feature coherent lattice and symmetry breaking, leading to unique magnetic phenomena such as proximity-induced ferromagnetism near the interface and the topological Hall effect in CuCrSe2-CuCr2Se4. Moreover, in AgCrSe2-CrSe2, the synthesized CrSe2 exhibits a previously unreported defect spinel structure and room-temperature ferromagnetism at the heterointerface. The interface-driven endotaxy growth method opens a rational pathway for fabricating 2D lateral magnetic heterostructures, providing a robust material platform for fundamental studies and the development of magnetoelectronic and spintronic devices.
Mao-Peng Miao, Nanshu Liu, Wen-Hao Zhang, Jian-Wang Zhou, Dao-Bo Wang, Cong Wang, Wei Ji, and Ying-Shuang Fu
Abstract:
Noncollinear magnetic orders in monolayer van der Waals magnets are crucial for probing delicate magnetic interactions under minimal spatial constraints and advancing miniaturized spintronic devices. Despite their significance, achieving atomic-scale identification remains challenging. In this study, we utilized spin-polarized scanning tunneling microscopy and density functional theory calculations to identify spin-spiral orders in mono- and bi-layer NiI2, grown on graphene-covered SiC(0001) substrates. We discovered two distinct spin-spiral states with Q vectors aligning and deviating by 7° from the lattice direction, exhibiting periodicities of 4.54 and 5.01 times the lattice constant, respectively. These findings contrast with bulk properties and align closely with our theoretical predictions. Surprisingly, the finite sizes of monolayers induce incommensurability with the spin-spiral period, facilitating collective spin switching behavior under magnetic fields. Our research reveals intrinsic noncollinear magnetism at the monolayer limit with unprecedented resolution, paving the way for exploring novel spin phenomena.
Shuo Mi#, Manyu Wang#, Bingxian Shi#, Songyang Li, Xiaoxiao Pei, Yanyan Geng, Shumin Meng, Rui Xu, Li Huang, Wei Ji, Fei Pang, Peng Cheng*, Jianfeng Guo*, and Zhihai Cheng*
Abstract:
Strain engineering offers a compelling route to modulate magnetism in two-dimensional (2D) materials, yet most approaches rely on externally applied strain. An in-plane anisotropic 2D-layered ferromagnet FePd2Te2 provides a suitable platform to study intrinsic strain-magnetism coupling due to its twinning domains. Here, we report spatially modulated internal compressive/tensile(C/T) strain regions in FePd2Te2 and their strong impact on local magnetic properties in real space by using atomic/magnetic force microscopy (AFM/MFM) combined with scanning tunneling microscopy (STM). Field- and strain-dependent spin transformations reveal the modulation of its intrinsic C/T regions. Notably, C regions retain intact Fe zigzag chains and exhibit larger, abruptly switching magnetic moments, while T regions display fragmented chains with reduced, gradually rotating spins. The intrinsic strain-induced intact ferromagnetic (FM), field-induced polarized-FM states, and their transitions are comparatively discussed during magnetic measurements. Temperature- and field-dependent evolution are further investigated in the FM and paramagnetic (PM) states and summarized to obtain an H-T phase diagram of FePd2Te2. Our work provides key results for understanding real-space tunable magnetic states through internal structural heterogeneity and suggests potential strategies for manipulating intrinsic strain-engineered magnetic devices.
Xiaoqing Chen#, Huijuan Zhao#, Ruixiang Fei, Chun Huang, Jingsi Qiao, Cheng Sun, Haiming Zhu, Li Zhan, Zehua Hu, Songlin Li, Li Yang, Zemin Tang, Lianhui Wang, Yi Shi, Wei Ji, Jian-Bin Xu, Li Gao*, Xuetao Gan* & Xinran Wang*
Abstract:
Two-dimensional (2D) materials offer strong light-matter interaction and design flexibility beyond bulk semiconductors, but an intrinsic limit is the low absorption imposed by the atomic thickness. A long-sought-after goal is to achieve complementary absorption enhancement through energy transfer (ET) to break this limit. However, it is found challenging due to the competing charge transfer (CT) process and lack of resonance in exciton states. Here, we report highly efficient ET in a 2D hybrid organic-inorganic heterostructure (HOIST) of Me-PTCDI/WS2. Resonant ET is observed leading to enhanced WS2 photoluminescence (PL) by 124 times. We identify Dexter exchange between the Frenkel state in donor and an excited 2s state in acceptor as the main ET mechanism, as supported by density functional theory calculations. We further demonstrate ET-enhanced phototransistor devices with enhanced responsivity by nearly 1000 times without sacrificing the response time. Our results expand the understanding of interlayer relaxation processes in 2D materials and open opportunities in optoelectronic devices.
Kagome materials have attracted extensive attention due to their correlated properties. The breathing kagome material system Nb3F8, Nb3Cl8, Nb3Br8, Nb3I8 is regarded as a Mott insulator. However, studies on the influence of interlayer coupling on its magnetic and Mott properties are lacking. In this work, we investigated the effect of interlayer coupling on bilayer properties of each Nb3X8 (X = F, Cl, Br, I) compound via density functional theory (DFT) calculations, considering 24 stacking configurations per material. We found that each bilayer material is a Mott insulator. Due to the competition between interlayer Pauli repulsion and hopping, most interlayer magnetism is AFM, a small number of cases show AFM-FM degeneracy, and the magnetic ground state of 3 configurations is interlayer FM, i.e., tunable interlayer magnetism occurs. This robustness of Mott states coexisting with tunable interlayer magnetism provide novel and comprehensive analysis and insights for the research of breathing kagome Mott insulators.
