Thermal evolution of spin excitations in honeycomb Ising antiferromagnetic FePSe3

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Abstract

We use elastic and inelastic neutron scattering (INS) to study the antiferromagnetic (AF) phase transitions and spin excitations in the two-dimensional (2D) zig-zag antiferromagnet FePSe3. By determining the magnetic order parameter across the AF phase transition, we conclude that the AF phase transition in FePSe3 is first-order in nature. In addition, our INS measurements reveal that the spin waves in the AF ordered state have a large easy-axis magnetic anisotropy gap, consistent with an Ising Hamiltonian, and possible biquadratic magnetic exchange interactions. On warming across TN, we find that dispersive spin excitations associated with three-fold rotational symmetric AF fluctuations change into FM spin fluctuations above TN. These results suggest that the first-order AF phase transition in FePSe3 may arise from the competition between C3 symmetric AF and C1 symmetric FM spin fluctuations around TN, in place of a conventional second-order AF phase transition.

Original languageEnglish
Article number40
Journalnpj Quantum Materials
Volume9
Issue number1
DOIs
StatePublished - Dec 2024

Funding

The work at the University of California, Berkeley was supported by the U.S. DOE under contract no. DE-AC02-05-CH11231 within the Quantum Materials Program (KC2202) (R.J.B.). The neutron scattering and single-crystal synthesis work at Rice was supported by US NSF-DMR-2100741, NSF-DMR-2418154 (P.D.) and by the Robert A. Welch Foundation under grant no. C-1839 (P.D.), respectively. A part of this research is supported by the Edinburgh-Rice Strategic Collaboration Award (P.D.). X.T. and M.Y. are supported by the Gordon and Betty Moore Foundation’s EPiQS Initiative through grant No. GBMF9470 and the Robert A. Welch Foundation Grant No. C-2175. The work of J.-H.C. was supported by the National Research Foundation (NRF) of Korea (Grant nos. 2020R1A5A1016518 and 2022R1F1A1074321). The research at Hangzhou Normal University is supported by The Open Project of Guangdong Provincial Key Laboratory of Magnetoelectric Physics and Devices, no. 2022B1212010008, Startup Project of Hangzhou Normal University (Grant no. 2020QDL026) and the Natural Science Foundation of Zhejiang Province (Grant no. LY22A040009). A portion of this research used resources at the Spallation Neutron Source, a DOE Office of Science User Facility operated by Oak Ridge National Laboratory.

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