First-principles Study on Structural, Thermal, Mechanical and Dynamic Stability of T'-MoS$_2$

TL;DR

This study uses first-principles calculations to explore the structure, stability, and vibrational properties of T'-MoS$_2$, suggesting it may have been previously observed but misidentified, and provides guidance for future experimental work.

Contribution

It is the first comprehensive theoretical investigation of T'-MoS$_2$'s stability, optical modes, and electronic properties, linking simulations with experimental observations.

Findings

T'-MoS$_2$ is thermally, mechanically, and dynamically stable.

Simulated STM images match experimental images previously attributed to other compounds.

Distinct Raman and infrared modes are identified and compared with other MoS$_2$ phases.

Abstract

Using first-principles density functional theory calculations, we investigate the structure, stability, optical modes and electronic band gap of a distorted tetragonal MoS$_2$ monolayer (T'-MoS$_2$). Our simulated scanning tunnel microscopy (STM) images of T'-MoS$_2$ are dramatically similar with those STM images which were identified as K$_{x}$(H$_{2}$O)$_{y}$MoS$_{2}$ from a previous experimental study. This similarity suggests that T'-MoS$_2$ might have already been observed in experiment but was unexpectedly misidentified. Furthermore, we verify the stability of T'-MoS$_2$ from thermal, mechanical and dynamic aspects, by \emph{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'-MoS$_2$ at $\Gamma$ 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'-MoS$_2$ with those of H-MoS$_2$ and T-MoS$_2$. Our results provide a useful guidance for further experimental identification and characterization of T'-MoS$_2$.