Anomalous Raman Response in 2D Magnetic FeTe Under Uniaxial Strain: Tetragonal and Hexagonal Polymorphs

Abstract 2D Fe‐chalcogenides emerge with rich structures, magnetisms, and superconductivities, which spark the growing research interests in the torturous transition mechanism and tunable properties for their potential applications in nanoelectronics. Uniaxial strain can produce a lattice distortion to study symmetry breaking induced exotic properties in 2D magnets. Herein, the anomalous Raman spectrum of 2D tetragonal ( t −) and hexagonal ( h −) FeTe is systematically investigated via uniaxial strain engineering strategy. It is found that both t ‐ and h ‐FeTe keep the structural stability under different uniaxial tensile or compressive strain up to ± 0.4%. Intriguingly, the lattice vibrations along both in‐plane and out‐of‐plane directions exceptionally harden (softened) under tensile (compressive) strain, distinguished from the behaviors of many conventional 2D systems. Further, the difference in thickness‐dependent strain effect can be well explained by their structural discrepancy between two polymorphs of FeTe. These results can supply a unique platform to explore the vibrational properties of many novel 2D materials.