Structural phase transitions in the van der Waals ferromagnets Fe${}_x$Pd${}_y$Te${}_2$

Abstract

Here, we provide a detailed study of the crystal structure and physical properties of the recently discovered vdW ferromagnet FePd${}_2$Te${}_2$. We find this compound has a relatively wide width of formation, and grow single crystals with compositions Fe${}_x$Pd${}_y$Te${}_2$ where $x$ ranges from 0.9 to 1.1 and $y$ from 1.8 to 2.5, respectively. Temperature-dependent X-ray diffraction and transport measurements reveal that a first-order structural transition occurs in the range of $T$ = 360-420 K. Above the transition, the compounds with Pd fraction $y>2$ adopt a disordered derivative of the tetragonal FeTe structure, with the Fe layer showing mixed Fe/Pd occupancy and the extra Pd atoms partially occupying interstitial sites. Below 370 K, the structure is incommensurately modulated. For $y<2$, the composition Fe${}_{1.1}$Pd${}_{1.8}$Te${}_2$ has monoclinic symmetry at room temperature that is consistent with the reported structure of FePd${}_2$Te${}_2$. This phase undergoes a structural transition at 420 K for which the high temperature structure is yet to be determined; however, based on the similarities with the $y>2$ compounds, we speculate that this composition also adopts a tetragonal structure above 420\,K. All compounds investigated in the Fe${}_x$Pd${}_y$Te${}_2$ series show metallic behavior, with magnetic characterization indicating that they are easy-plane, hard, ferromagnets with $T_C$ spanning 98--180 K. Both the critical temperature for the structural transition and the Curie temperature are moderately suppressed with increasing Pd fraction $y$ and corresponding decreasing Fe fraction $x$, indicating that synthetic control over $x$ and $y$ paves way for the further exploration of these compounds.