Designing Magnetic Properties in CrSBr through Hydrostatic Pressure and Ligand Substitution

Telford, Evan J.; Chica, Daniel G.; Ziebel, Michael E.; Xie, Kaichen; Manganaro, Nicholas S.; Huang, Chun‐Ying; Cox, Jordan; Dismukes, Avalon H.; Zhu, Xiaoyang; Walsh, James P. S.; Cao, Ting; Dean, Cory R.; Roy, Xavier

doi:10.1002/apxr.202300036

Title: Designing Magnetic Properties in CrSBr through Hydrostatic Pressure and Ligand Substitution

Journal Article · 06 August 2023 · Advanced Physics Research

DOI: https://doi.org/10.1002/apxr.202300036 · OSTI ID:1994007

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Department of Chemistry Columbia University New York NY 10027 USA, Department of Physics Columbia University New York NY 10027 USA
Department of Chemistry Columbia University New York NY 10027 USA
Department of Materials Science and Engineering University of Washington Seattle WA 98195 USA
Department of Chemistry University of Massachusetts Amherst Amherst MA 01003 USA
Department of Physics Columbia University New York NY 10027 USA

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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Sponsoring Organization:: USDOE

Grant/Contract Number:: FG02-94ER14466

OSTI ID:: 1994007

Journal Information:: Advanced Physics Research, Journal Name: Advanced Physics Research Journal Issue: 11 Vol. 2; ISSN 2751-1200

Publisher:: Wiley Blackwell (John Wiley & Sons)Copyright Statement

Country of Publication:: Germany

Language:: English

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