Optical Emission from Light-like and Particle-like Excitons in Monolayer Transition Metal Dichalcogenides

Abstract

Several monolayer transition metal dichalcogenides (TMDs) are direct band gap semiconductors and potentially efficient emitters in light emitting devices. Photons are emitted when strongly bound excitons decay radiatively, and accurate models of such excitons are important for a full understanding of the emission. Importantly, photons are emitted in directions uniquely determined by the exciton center of mass momentum and with lifetimes determined by the exciton transition matrix element. The exciton band structures of two-dimensional hexagonal materials, including TMDs, are highly unusual with coexisting particle- and light-like bands. The latter is non-analytic with emission selection rules essentially opposite to the particle-like states, but has been ignored in analyses of TMD light emission so far. In the present work, we analyse the temperature and angular dependence of light emission from both exciton species and point out several important consequences of the unique exciton band structure. Within a first-principles Density-Functional-Theory+Bethe-Salpeter-Equation framework, we compute exciton band structures and optical matrix elements for the important TMDs MoS2, MoSe2, WS2, and WSe2. At low temperature, only the particle-like band is populated and our results agree with previous work. However, at slightly elevated temperatures, a significant population of the light-like band leads to modified angular emission patterns and lifetimes. Clear experimental fingerprints are predicted and explained by a simple four-state model incorporating spin-orbit as well as intervalley exchange coupling.

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• Theoretical methods for excitonic physics in two-dimensional materials
• Exciton absorption, band structure, and optical emission in biased bilayer graphene
• Electron energy-loss spectrum and exciton band structure of ${\mathrm{WSe}}_2$ monolayer studied by ab initio Bethe-Salpeter equation calculations
• Anisotropic linear and non-linear excitonic optical properties of buckled monolayer semiconductors
• Effect of intravalley and intervalley electron-hole exchange on the nonlinear optical response of monolayer MoSe${}_2$
• Searching for Unconventional Superfluid in Excitons of Monolayer Semiconductors
• Dimensionality-Dependent Exciton Dispersion in a Single-Band Mott Insulator