Polariton assisted incoherent to coherent excitation energy transfer between colloidal nanocrystal quantum dots

TL;DR

This paper investigates how optical microcavities can control energy transfer between colloidal nanocrystal quantum dots, enabling a switch from incoherent to coherent transfer regimes through cavity coupling and nonadiabatic effects.

Contribution

It introduces a novel method to tune energy transfer regimes in quantum dots using cavity coupling and models the dynamics with a non-Markovian quantum Redfield approach.

Findings

Demonstrates tunable transition from Förster to coherent energy transfer regimes.

Shows rapid energy transfer rates in the underdamped regime.

Provides a detailed atomistic and quantum dynamical model for the system.

Abstract

We explore the dynamics of energy transfer between two nanocrystal quantum dots placed within an optical microcavity. By adjusting the coupling strength between the cavity photon mode and the quantum dots, we have the capacity to fine-tune the effective coupling between the donor and acceptor. Introducing a nonadiabatic parameter, $\gamma$, governed by the coupling to the cavity mode, we demonstrate the system's capability to shift from the overdamped Forster regime ($\gamma \ll 1$) to an underdamped coherent regime ($\gamma \gg 1$). In the latter regime, characterized by swift energy transfer rates, the dynamics are influenced by decoherence times. To illustrate this, we study the exciton energy transfer dynamics between two closely positioned CdSe/CdS core/shell quantum dots with sizes and separations relevant to experimental conditions. Employing an atomistic approach, we calculate the excitonic level arrangement, exciton-phonon interactions, and transition dipole moments of the quantum dots within the microcavity. These parameters are then utilized to define a model Hamiltonian. Subsequently, we apply a generalized non-Markovian quantum Redfield equation to delineate the dynamics within the polaritonic framework.