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.

Beijing Academy of Quantum Information Sciences Beijing 100193 China

Beijing Innovation Center for Future Chips Tsinghua University Beijing 100084 China

Beijing Key Laboratory of Optoelectronic Functional Materials and Micro Nano Devices Department of Physics Renmin University of China Beijing 100872 China

Department of Inorganic Chemistry Faculty of Chemical Technology University of Chemistry and Technology Prague Technická 5 16628 6 Prague Czech Republic

Division of Physics and Applied Physics School of Physical and Mathematical Sciences Nanyang Technological University Singapore 637371

Faculty of Materials and Manufacturing Key Laboratory of Advanced Functional Materials Ministry of Education of China Beijing University of Technology Beijing 100124 China

Frontier Science Center for Quantum Information Beijing 100084 China

Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of Education Institutes of Physical Science and Information Technology Anhui University Hefei 230601 China

Okinawa Institute of Science and Technology Onna Okinawa Prefecture 904 0412 Japan

School of Electrical and Electronic Engineering Nanyang Technological University 50 Nanyang Avenue Singapore 639798

School of Physics and Optoelectronics Engineering Anhui University Hefei 230601 China

State Key Laboratory of Low Dimensional Quantum Physics and Department of Physics Tsinghua University Beijing 100084 China

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