Lattice Transformation from 2D to Quasi 1D and Phonon Properties of Exfoliated ZrS₂ and ZrSe₂

Abstract Recent reports on thermal and thermoelectric properties of emerging 2D materials have shown promising results. Among these materials are Zirconium‐based chalcogenides such as zirconium disulfide (ZrS₂), zirconium diselenide (ZrSe₂), zirconium trisulfide (ZrS₃), and zirconium triselenide (ZrSe₃). Here, the thermal properties of these materials are investigated using confocal Raman spectroscopy. Two different and distinctive Raman signatures of exfoliated ZrX₂ (where X = S or Se) are observed. For 2D‐ZrX₂, Raman modes are in alignment with those reported in literature. However, for quasi 1D‐ZrX₂, Raman modes are identical to exfoliated ZrX₃ nanosheets, indicating a major lattice transformation from 2D to quasi‐1D. Raman temperature dependence for ZrX₂ are also measured. Most Raman modes exhibit a linear downshift dependence with increasing temperature. However, for 2D‐ZrS₂, a blueshift for A1g mode is detected with increasing temperature. Finally, phonon dynamics under optical heating for ZrX₂ are measured. Based on these measurements, the calculated thermal conductivity and the interfacial thermal conductance indicate lower interfacial thermal conductance for quasi 1D‐ZrX₂ compared to 2D‐ZrX₂, which can be attributed to the phonon confinement in 1D. The results demonstrate exceptional thermal properties for Zirconium‐based materials, making them ideal for thermoelectric device applications and future thermal management strategies.