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Magnetic order, field-induced melting, and role of spin-lattice coupling in two-dimensional Van der Waals materials: A case study of CrSiTe3

Smita Gohil, Saswata Halder, Karthik K. Iyer, Shankar Ghosh, A. Thamizhavel, and Kalobaran Maiti*

  • *Contact author: kbmaiti@tifr.res.in

Phys. Rev. B 111, L100407 – Published 25 March, 2025

DOI: https://doi.org/10.1103/PhysRevB.111.L100407

Abstract

Two-dimensional (2D) Van der Waals compounds exhibit interesting electronic and magnetic properties due to complex intralayer and interlayer interactions, which are of immense importance in realizing exotic physics as well as advanced technology. Various experimental and theoretical studies led to significantly different ground state properties often contrasting each other. Here, we studied a novel 2D material, CrSiTe3, employing magnetic, specific heat, and Raman measurements. Experimental results reveal evidence of incipient antiferromagnetism below 1 kOe concomitant to ferromagnetic order at 33 K. Antiferromagnetic and ferromagnetic interactions coexist at low field in the temperature regime 15–33 K. Low-field data reveal an additional magnetic order below 15 K, which melts on application of external magnetic field and remains dark in the heat capacity data. Raman spectra exhibit anomalies at the magnetic transitions, evidence of strong spin-lattice coupling. Below 15 K, Eg modes exhibit hardening while Ag modes become significantly softer, suggesting weakening of the interlayer coupling at low temperatures which might be a reason for the unusual magnetic ground state and field-induced melting of the magnetic order. These results reveal evidence of exceptional ground state properties linked to spin-lattice coupling and also suggest a pathway to study complex magnetism in such technologically important materials.

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