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Abstract Antiferromagnetic van der Waals‐typeM2P2X6compounds provide a versatile material platform for studying 2D magnetism and relevant phenomena. Establishing ferromagnetism in 2D materials is technologically valuable. Though magnetism is generally tunable via a chemical way, it is challenging to induce ferromagnetism with isovalent chalcogen and bimetallic substitutions inM2P2X6. Here, we report co‐substitution of Cu1+and Cr3+for Ni2+in Ni2P2S6, creating CuxNi2(1‐x)CrxP2S6medium‐entropy alloys spanning a full substitution range (x= 0 to 1). Such substitution strategy leads to a unique evolution in crystal structure and magnetic phases that are distinct from traditional isovalent bimetallic doping, with Cu and Cr co‐substitution enhancing ferromagnetic correlations and generating a weak ferromagnetic phase in intermediate compositions. This aliovalent substitution strategy offers a universal approach for tuning layered magnetism in antiferromagnetic systems, which along with the potential for light‐matter interaction and high‐temperature ferroelectricity, can enable multifunctional device applications.
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High‐Throughput Screening Assisted Discovery of a Stable Layered Anti‐Ferromagnetic Semiconductor: CdFeP 2 Se 6
Abstract Recent advances in 2D magnetism have heightened interest in layered magnetic materials due to their potential for spintronics. In particular, layered semiconducting antiferromagnets exhibit intriguing low‐dimensional semiconducting behavior with both charge and spin as carrier controls. However, synthesis of these compounds is challenging and remains rare. Here, first‐principles based high‐throughput search is conducted to screen potentially stable mixed metal phosphorous trichalcogenides (MM′P2X6, where M and M′are transition metals and X is a chalcogenide) that have a wide range of tunable bandgaps and interesting magnetic properties. Among the potential candidates, a stable semiconducting layered magnetic material, CdFeP2Se6, that exhibits a short‐range antiferromagnetic order atTN = 21 K with an indirect bandgap of 2.23 eV is successfully synthesized . This work suggests that high‐throughput screening assisted synthesis can be an effective method for layered magnetic materials discovery.
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- Award ID(s):
- 2210933
- PAR ID:
- 10469519
- Publisher / Repository:
- Wiley-VCH GmBH
- Date Published:
- Journal Name:
- Advanced Functional Materials
- Volume:
- 33
- Issue:
- 9
- ISSN:
- 1616-301X
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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- Free Publicly Accessible Full Text
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Accepted Manuscript
- Journal Article:
- https://doi.org/10.1002/adfm.202210965
