First-principles study on structural, thermal, mechanical and dynamic stability of T'-MoS₂

Using first-principles density functional theory calculations, we investigate the structure, stability, optical modes and electronic band gap of a distorted tetragonal MoS₂ monolayer (T'-MoS₂). Our simulated scanning tunnel microscopy (STM) images of T'-MoS₂ are dramatically similar to those STM images which were identified as K _x (H₂O) _y MoS₂ from a previous experimental study. This similarity suggests that T'-MoS₂ might have already been experimentally observed, but due to being unexpected was misidentified. Furthermore, we verify the stability of T'-MoS₂ from the thermal, mechanical and dynamic aspects, by ab initio molecular dynamics simulation, elastic constants evaluation and phonon band structure calculation based on density functional perturbation theory, respectively. In addition, we calculate the eigenfrequencies and eigenvectors of the optical modes of T'-MoS₂ at [Formula: see text] point and distinguish their Raman and infrared activity by pointing out their irreducible representations using group theory. At the same time, we compare the Raman modes of T'-MoS₂ with those of H-MoS₂ and T-MoS₂. Our results provide useful guidance for further experimental identification and characterization of T'-MoS₂.