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Van der Waals (VdW) materials have opened new directions in the study of low dimensional magnetism. A largely unexplored arena is the intrinsic tuning of VdW magnets toward new ground states. Chromium trihalides provided the first such example with a change of interlayer magnetic coupling emerging upon exfoliation. Here, we take a different approach to engineer previously unknown ground states, not by exfoliation, but by tuning the spin-orbit coupling (SOC) of the nonmagnetic ligand atoms (Cl, Br, I). We synthesize a three-halide series, CrCl 3 − x − y Br x I y , and map their magnetic properties as a function of Cl, Br, and I content. The resulting triangular phase diagrams unveil a frustrated regime near CrCl 3 . First-principles calculations confirm that the frustration is driven by a competition between the chromium and halide SOCs. Furthermore, we reveal a field-induced change of interlayer coupling in the bulk of CrCl 3 − x − y Br x I y crystals at the same field as in the exfoliation experiments.
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Designing Magnetic Properties in CrSBr through Hydrostatic Pressure and Ligand Substitution
Abstract Magnetic van der Waals (vdW) materials are a promising platform for producing atomically thin spintronic and optoelectronic devices. The A‐type antiferromagnet CrSBr has emerged as a particularly exciting material due to its high magnetic ordering temperature, semiconducting electrical properties, and enhanced chemical stability compared to other vdW magnets. Exploring mechanisms to tune its magnetic properties will facilitate the development of nanoscale devices based on vdW materials with designer magnetic properties. Here it is investigated how the magnetic properties of CrSBr change under pressure and ligand substitution. Pressure compresses the unit cell, increasing the interlayer exchange energy while lowering the Néel temperature. Ligand substitution, realized synthetically through Cl alloying, anisotropically compresses the unit cell and suppresses the Cr‐halogen covalency, reducing the magnetocrystalline anisotropy energy and decreasing the Néel temperature. A detailed structural analysis combined with first‐principles calculations reveals that alterations in the magnetic properties are intricately related to changes in direct Cr–Cr exchange interactions and the Cr–anion superexchange pathways. Further, it is demonstrated that Cl alloying enables chemical tuning of the interlayer coupling from antiferromagnetic to ferromagnetic, which is unique among known two‐dimensional magnets.
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- Award ID(s):
- 1751949
- PAR ID:
- 10439625
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- Advanced Physics Research
- Volume:
- 2
- Issue:
- 11
- ISSN:
- 2751-1200
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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