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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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This content will become publicly available on July 28, 2026
Is the single-ion conductor cubic Li 7 La 3 Zr 2 O 12 a binary ionic electrolyte?
Garnet-type cubic Li7La3Zr2O12(c-LLZO) is a single-ion conductor, but the electrochemically generated charged vacancies make it a binary ionic electrolyte, which explains the current- and thickness-dependent lithium dendrite initiation dynamics.
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- Award ID(s):
- 2203994
- PAR ID:
- 10633497
- Publisher / Repository:
- Royal Society of Chemistry
- Date Published:
- Journal Name:
- Materials Horizons
- Volume:
- 12
- Issue:
- 15
- ISSN:
- 2051-6347
- Page Range / eLocation ID:
- 5453 to 5458
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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