Two-dimensional excitons in monolayer transition metal dichalcogenides from simple models and variational calculations

TL;DR

This paper investigates exciton spectra in monolayer transition metal dichalcogenides using simple models and variational calculations, revealing limitations of the screened hydrogen model and providing close agreement with experimental data.

Contribution

It introduces a combined numerical and variational approach to accurately model exciton energies and radii, highlighting the model's strengths and limitations in describing exciton properties.

Findings

SHM describes nonhydrogenic Rydberg series well

SHM fails to capture m-dependence of exciton energy

Calculated exciton energies agree with experimental data

Abstract

Exciton spectra of monolayer transition metal dichalcogenides (TMDs) in various dielectric environments are studied. The screened hydrogen model (SHM) [Phys. Rev. Lett. 116, 056401 (2016)] is examined by comparing its exciton spectra with the radial equation (RE) solutions. While the SHM is found to describe the nonhydrogenic exciton Rydberg series reasonably well, it fails to account for the linear decrease of the exciton energy with the orbital quantum number $m$. The exciton Bohr orbit shrinks as $\lvert m\rvert$ becomes larger resulting in increased strength of the electron-hole interaction and a decrease of the exciton energy. The exciton effective radius expression of the SHM can characterize the exciton radius's dependence on $n$, but it cannot properly describe the exciton radius's dependence on $m$, which is the cause of the SHM's poor description of the exciton energy's $m$-dependence. For monolayer WS$_2$ on the SiO$_2$ substrate, our calculated $s$ exciton Rydberg series agrees closely with that measured by optical reflection spectroscopy [Phys. Rev. Lett. 113, 076802 (2014)], while the calculated $p$ excitons offer an explanation for the two broad features of a two-photon absorption spectrum [Nature 513, 214 (2014)]. Our calculated exciton energies for monolayer TMDs in various dielectric environments compare favourably with experimental data. Variational wave functions are obtained for a number of strongly bound exciton states and further used to study the Stark effects in monolayer TMDs, an analytical expression being deduced which yields a redshift of the ground state energy to a good accuracy. The numerical solution of the RE combined with the variational method provides a simple and effective approach for the study of excitons in monolayer TMDs.