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

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

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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 languageEnglish
Article number064401
Pages (from-to)1-6
Number of pages6
JournalPhysical Review Materials
Issue number6
Publication statusPublished - 2 Jun 2023
MoE publication typeA1 Journal article-refereed


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