Unusual magnetic order, field induced melting and role of spin-lattice coupling in 2D Van der Waals materials: a case study of CrSiTe3

Two-dimensional (2D) Van der Waals compounds exhibit interesting electronic and magnetic properties due to complex intra-layer and inter-layer 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 coexists 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 remain dark in the heat capacity data. Raman spectra exhibit anomalies at the magnetic transitions; an evidence of strong spin-lattice coupling. Below 15 K, Eg modes exhibit hardening while Ag modes become significantly softer suggesting weakening of the inter-layer 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.