Extreme sensitivity of the magnetic ground state to halide composition in FeCl3-xBrx

Andrew Cole; Alenna Streeter; Adolfo O. Fumega; Xiaohan Yao; Zhi Cheng Wang; Erxi Feng; Huibo Cao; Jose L. Lado; Stephen E. Nagler; Fazel Tafti

doi:10.1103/PhysRevMaterials.7.064401

Extreme sensitivity of the magnetic ground state to halide composition in FeCl3-xBrx

Andrew Cole, Alenna Streeter, Adolfo O. Fumega, Xiaohan Yao, Zhi Cheng Wang, Erxi Feng, Huibo Cao, Jose L. Lado, Stephen E. Nagler, Fazel Tafti

Single Crystal Diffraction

Research output: Contribution to journal › Article › peer-review

3 Scopus citations

Abstract

Mixed halide chemistry has recently been utilized to tune the intrinsic magnetic properties of transition-metal halides - one of the largest families of magnetic van der Waals materials. Prior studies have shown that the strength of exchange interactions, hence the critical temperature, can be tuned smoothly with halide composition for a given ground state. Here we show that the ground state itself can be altered by a small change of halide composition in FeCl3-xBrx. Specifically, we find a threefold jump in the Néel temperature and a sign change in the Weiss temperature at x=0.08 corresponding to only 3% bromine doping. Using neutron scattering, we reveal a change of the ground state from spiral order in FeCl3 to A-type antiferromagnetic order in FeBr3. From first-principles calculations, we show that a delicate balance between nearest and next-nearest neighbor interactions is responsible for such a transition. These results demonstrate how varying the halide composition can tune the competing interactions and change the ground state of a spiral spin liquid system.

Original language	English
Article number	064401
Journal	Physical Review Materials
Volume	7
Issue number	6
DOIs	https://doi.org/10.1103/PhysRevMaterials.7.064401
State	Published - Jun 2023

Funding

The work at Boston College was supported by the National Science Foundation under Award No. DMR-2203512. J.L.L. and A.F. acknowledge the computational resources provided by the Aalto Science-IT project, the financial support from the Academy of Finland Projects No. 331342, No. 336243, and No. 349696, and the Jane and Aatos Erkko Foundation. S.N. was supported by the Quantum Science Center (QSC), a National Quantum Information Science Research Center of the U.S. Department of Energy (DOE). E.F. and H.B.C. were supported by the U.S. Department of Energy (DOE), Office of Science, Office of Basic Energy Sciences, Early Career Research Program Award No. KC0402020, under Contract No. DE-AC05-00OR22725. A portion of this research used resources at the High Flux Isotope Reactor, a DOE Office of Science User Facility operated by the Oak Ridge National Laboratory.

Funders	Funder number
National Quantum Information Science Research Center
Quantum Science Center
National Science Foundation	DMR-2203512
U.S. Department of Energy
Office of Science
Basic Energy Sciences	DE-AC05-00OR22725, KC0402020
Academy of Finland	336243, 349696, 331342
Jane ja Aatos Erkon Säätiö

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10.1103/PhysRevMaterials.7.064401

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title = "Extreme sensitivity of the magnetic ground state to halide composition in FeCl3-xBrx",

abstract = "Mixed halide chemistry has recently been utilized to tune the intrinsic magnetic properties of transition-metal halides - one of the largest families of magnetic van der Waals materials. Prior studies have shown that the strength of exchange interactions, hence the critical temperature, can be tuned smoothly with halide composition for a given ground state. Here we show that the ground state itself can be altered by a small change of halide composition in FeCl3-xBrx. Specifically, we find a threefold jump in the N{\'e}el temperature and a sign change in the Weiss temperature at x=0.08 corresponding to only 3% bromine doping. Using neutron scattering, we reveal a change of the ground state from spiral order in FeCl3 to A-type antiferromagnetic order in FeBr3. From first-principles calculations, we show that a delicate balance between nearest and next-nearest neighbor interactions is responsible for such a transition. These results demonstrate how varying the halide composition can tune the competing interactions and change the ground state of a spiral spin liquid system.",

author = "Andrew Cole and Alenna Streeter and Fumega, {Adolfo O.} and Xiaohan Yao and Wang, {Zhi Cheng} and Erxi Feng and Huibo Cao and Lado, {Jose L.} and Nagler, {Stephen E.} and Fazel Tafti",

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AU - Streeter, Alenna

AU - Fumega, Adolfo O.

AU - Yao, Xiaohan

AU - Wang, Zhi Cheng

AU - Feng, Erxi

AU - Cao, Huibo

AU - Lado, Jose L.

AU - Nagler, Stephen E.

AU - Tafti, Fazel

PY - 2023/6

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AB - Mixed halide chemistry has recently been utilized to tune the intrinsic magnetic properties of transition-metal halides - one of the largest families of magnetic van der Waals materials. Prior studies have shown that the strength of exchange interactions, hence the critical temperature, can be tuned smoothly with halide composition for a given ground state. Here we show that the ground state itself can be altered by a small change of halide composition in FeCl3-xBrx. Specifically, we find a threefold jump in the Néel temperature and a sign change in the Weiss temperature at x=0.08 corresponding to only 3% bromine doping. Using neutron scattering, we reveal a change of the ground state from spiral order in FeCl3 to A-type antiferromagnetic order in FeBr3. From first-principles calculations, we show that a delicate balance between nearest and next-nearest neighbor interactions is responsible for such a transition. These results demonstrate how varying the halide composition can tune the competing interactions and change the ground state of a spiral spin liquid system.

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Extreme sensitivity of the magnetic ground state to halide composition in FeCl3-xBrx

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