Polaritonic Bottleneck in Colloidal Quantum Dots

TL;DR

This paper investigates how placing colloidal quantum dots in an optical cavity creates a polariton-induced phonon bottleneck, significantly slowing exciton relaxation compared to free space, with implications for controlling exciton dynamics.

Contribution

It demonstrates that multiphonon emission causes a phonon bottleneck in cavity-embedded quantum dots, revealing a new mechanism to control exciton relaxation timescales.

Findings

Relaxation times are slowed by orders of magnitude in cavities.

Multiphonon emission dominates exciton decay.

Photon fraction has a secondary effect on relaxation.

Abstract

Controlling the relaxation dynamics of excitons is key to improving the efficiencies of semiconductor--based applications. Confined semiconductor nanocrystals (NCs) offer additional handles to control the properties of excitons, for example, by changing their size or shape, resulting in a mismatch between excitonic gaps and phonon frequencies. This has led to the hypothesis of a significant slowing--down of exciton relaxation in strongly confined NCs, but in practice due to increasing exciton--phonon coupling and rapid multiphonon relaxation channels, the exciton relaxation depends only weakly on the size or shape. Here, we focus on elucidating the nonradiative relaxation of excitons in NCs placed in an optical cavity. We find that multiphonon emission of carrier governs the decay resulting in a polariton--induced phonon bottleneck with relaxation timescales that are slower by orders of magnitude compared to the cavity--free case, while the photon fraction plays a secondary role.