Chen Ye, Cong Wang, Qiong Wu, Sheng Liu, Jiayuan Zhou, Guopeng Wang, Aljoscha Söll, Zdenek Sofer, Ming Yue, Xue Liu, Mingliang Tian, Qihua Xiong, Wei Ji & Xiao Renshaw Wang
Abstract
Magnetic van der Waals (vdW) materials possess versatile spin configurations stabilized in reduced dimensions. One magnetic order is the interlayer antiferromagnetism in A-type vdW antiferromagnet, which may be effectively modified by the magnetic field, stacking order, and thickness scaling. However, atomically revealing the interlayer spin orientation in the vdW antiferromagnet is highly challenging, because most of the material candidates exhibit an insulating ground state or instability in ambient conditions. Here, we report the layer-dependent interlayer antiferromagnetic spin reorientation in air-stable semiconductor CrSBr using magnetotransport characterization and first-principles calculations. We reveal an odd–even layer effect of interlayer spin reorientation, which originates from the competitions among interlayer exchange, magnetic anisotropy energy, and extra Zeeman energy of uncompensated magnetization. Furthermore, we quantitatively constructed the layer-dependent magnetic phase diagram with the help of a linear-chain model. Our work uncovers the layer-dependent interlayer antiferromagnetic spin reorientation engineered by magnetic field in the air-stable semiconductor. (DOI: 10.1021/acsnano.2c01151)
Pingfan Gu, Yujia Sun, Cong Wang, Yuxuan Peng, Yaozheng Zhu, Xing Cheng, Kai Yuan, Chao Lyu, Xuelu Liu, Qinghai Tan, Qinghua Zhang, Lin Gu, Zhi Wang, Hanwen Wang, Zheng Han, Kenji Watanabe, Takashi Taniguchi, Jinbo Yang, Jun Zhang, Wei Ji, Ping-Heng Tan & Yu Ye
Abstract
Materials with a quasi-one-dimensional stripy magnetic order often exhibit low crystal and magnetic symmetries, thus allowing the presence of various energy coupling terms and giving rise to macroscopic interplay between spin, charge, and phonon. In this work, we performed optical, electrical and magnetic characterizations combined with first-principles calculations on a van der Waals antiferromagnetic insulator chromium oxychloride (CrOCl). We detected the subtle phase transition behaviors of exfoliated CrOCl under varying temperature and magnetic field and clarified its controversial spin structures. We found that the antiferromagnetism and its air stability persist down to few-layer samples, making it a promising candidate for future 2D spintronic devices. Additionally, we verified the magnetoelastic coupling effect in CrOCl, allowing for the potential manipulation of the magnetic states via electric field or strain. These virtues of CrOCl provide us with an ideal platform for fundamental research on spin-charge, spin-phonon coupling, and spin-interactions.
Intrinsic antiferromagnetism in van der Waals (vdW) monolayer (ML) crystals enriches our understanding of two-dimensional (2D) magnetic orders and presents several advantages over ferromagnetism in spintronic applications. However, studies of 2D intrinsic antiferromagnetism are sparse, owing to the lack of net magnetisation. Here, by combining spin-polarised scanning tunnelling microscopy and first-principles calculations, we investigate the magnetism of vdW ML CrTe2, which has been successfully grown through molecular-beam epitaxy. We observe a stable antiferromagnetic (AFM) order at the atomic scale in the ML crystal, whose bulk is ferromagnetic, and correlate its imaged zigzag spin texture with the atomic lattice structure. The AFM order exhibits an intriguing noncollinear spin reorientation under magnetic fields, consistent with its calculated moderate magnetic anisotropy. The findings of this study demonstrate the intricacy of 2D vdW magnetic materials and pave the way for their in-depth analysis.
Two-dimensional magnetic semiconductors provide a platform for studying physical phenomena at atomically thin limit, and promise magneto-optoelectronic devices application. Here, we report light helicity detectors based on graphene-CrI3-graphene vdW heterostructures. We investigate the circularly polarized light excited current and reflective magnetic circular dichroism (RMCD) under various magnetic fields in both monolayer and multilayer CrI3 devices. The devices exhibit clear helicity-selective photoresponse behavior determined by the magnetic state of CrI3. We also find abnormal negative photocurrents at higher bias in both monolayer and multilayer CrI3. A possible explanation is proposed for this phenomenon. Our work reveals the interplay between magnetic and optoelectronic properties in CrI3 and paves the way to developing spin-optoelectronic devices.
The discovery of intrinsic ferromagnetism in ultrathin two-dimensional van der Waals crystals opens up exciting prospects for exploring magnetism in the ultimate two-dimensional limit. Here, we show that environmentally stable CrSe2 nanosheets can be readily grown on a dangling-bond-free WSe2 substrate with systematically tunable thickness down to the monolayer limit. These CrSe2/WSe2 heterostructures display high-quality van der Waals interfaces with well-resolved moiré superlattices and ferromagnetic behaviour. We find no apparent change in surface roughness or magnetic properties after months of exposure in air. Our calculations suggest that charge transfer from the WSe2 substrate and interlayer coupling within CrSe2 play a critical role in the magnetic order in few-layer CrSe2 nanosheets. The highly controllable growth of environmentally stable CrSe2 nanosheets with tunable thickness defines a robust two-dimensional magnet for fundamental studies and potential applications in magnetoelectronic and spintronic devices.
