Lattice equations and dielectric function for optical lattice vibrations in monolayer transition metal dichalcogenides

Abstract

Using a microscopic dipole lattice model including electronic polarization (EP) of ions and local field effects (LFEs) self-consistently, two sets of three equations are deduced for long wavelength in-plane and out-of-plane optical lattice vibrations in monolayer (ML) transition metal dichalcogenides (TMDs). Expressions for the lattice vibrational energy density are obtained for the two-dimensional (2D) crystals. The linear coefficients of the lattice equations can be determined by first-principles calculation, making these equations very useful for studying the lattice dynamical properties. The two pairs of equations describing the polar vibrations have the same forms as those for ML hexagonal BN and also resemble Huang's equations for bulk [Proc. Roy. Soc. A 208, 352 (1951)]. Each pair of the equations are solved simultaneously with the equation of electrostatics, and explicit expressions are obtained for the in-plane longitudinal and transverse optical (LO and TO) modes and out-of-plane optical (ZO) modes. The LO phonon dispersion relation is identical to the analytical expression of Sohier et al. [Nano Lett. 17, 3758 (2017)]. All the optical phonon branches except for LO are nondispersive at the long wavelengths. A 2D longitudinal lattice dielectric function $\epsilon(k,\omega)$ is deduced, allowing one to rederive the LO phonon dispersion simply from $\epsilon(k,\omega)=0$. A 2D Lyddane--Sachs--Teller relation and a frequency--susceptibility relation are obtained for in-plane and out-of-plane vibrations, respectively, through which the phonon frequencies are related to the 2D dielectric functions or susceptibilities. The explicit expressions are applied to calculate various dynamical properties when knowing three first-principles calculated parameters, and the ionic EP and LFEs are studied thoroughly.