Engineering the Radiative Dynamics of Thermalized Excitons with Metal Interfaces

TL;DR

This paper investigates how excitons in monolayer TMDCs near metal interfaces emit light, revealing how temperature, momentum distribution, and cavity effects influence their radiative properties, which is crucial for optoelectronic device optimization.

Contribution

It provides a comprehensive analysis of exciton emission near metal interfaces, highlighting the impact of temperature and momentum distribution on radiative rates, and suggests pathways for long-lifetime exciton states.

Findings

Emission rates at high temperatures resemble point dipoles.

Low-temperature excitons show significantly different emission behavior.

Nanoscale cavities can enhance exciton lifetimes.

Abstract

As a platform for optoelectronic devices based on exciton dynamics, monolayer transition metal dichalcogenides (TMDCs) are often placed near metal interfaces or inside planar cavities. While the radiative properties of point dipoles at metal interfaces has been studied extensively, those of excitons, which are delocalized and exhibit a temperature-dependent momentum distribution, lack a thorough treatment. Here, we analyze the emission properties of excitons in TMDCs near planar metal interfaces and explore their dependence on exciton center-of-mass momentum, transition dipole orientation, and temperature. Defining a characteristic energy scale $k_B T_c = (\hbar k)^2/2m$~($k$ being the radiative wavevector and $m$ the exciton mass), we find that at temperatures $T\gg T_c$ and low densities where the momentum distribution can be characterized by Maxwell-Boltzmann statistics, the modified emission rates~(normalized to free space) behave similarly to point dipoles at temperatures $T\gg T_c$. This similarity in behavior arises due to the broad nature of wavevector components making up the exciton and point dipole emission. On the other hand, the narrow momentum distribution of excitons for $T<T_c$ can result in significantly different emission behavior as compared to point dipoles. These differences can be further amplified by considering excitons with a Bose Einstein distribution at high phase space densities. We find suppression or enhancement of emission relative to the point dipole case by several orders of magnitude. These insights can help optimize the performance of optoelectronic devices that incorporate 2D semiconductors near metal electrodes and can inform future studies of exciton radiative dynamics at low temperatures. Additionally, these studies show that nanoscale optical cavities are a viable pathway to generating long-lifetime exciton states in TMDCs.