Perspective on Coupled Colloidal Quantum Dot Molecules

TL;DR

This paper explores the electronic hybridization in coupled colloidal quantum dot molecules, revealing how their structure influences optical properties and potential applications in quantum technologies.

Contribution

It introduces a model for fused core-shell nanocrystal dimers, analyzing how structural parameters affect hybridization energy and optical behavior.

Findings

Hybridization energy correlates with structural continuity and barrier thickness.

Hybridization modifies photon emission statistics, including decay rates and photon bunching.

Fused nanocrystals exhibit altered Auger recombination pathways.

Abstract

Electronic coupling and hence hybridization of atoms serve as the basis for the rich properties of the endless library of naturally occurring molecules. Colloidal quantum dots (CQDs) manifesting quantum strong confinement, possess atomic like characteristics with s and p electronic levels, which popularized the notion of CQDs as artificial atoms. Continuing this analogy, when two atoms are close enough to form a molecule so that their orbitals start overlapping, the orbitals' energies start to split into bonding and anti-bonding states made out of hybridized orbitals. The same concept is also applicable for two fused core-shell nanocrystals in close proximity. Their band-edge states, which dictate the emitted photon energy, start to hybridize changing their electronic and optical properties. Thus, an exciting direction of artificial molecules emerges leading to a multitude of possibilities for creating a library of new hybrid nanostructures with novel optoelectronic properties with relevance towards diverse applications including quantum technologies. In a model fused core-shell homodimer molecule, the hybridization energy is strongly correlated with the extent of structural continuity, the delocalization of the exciton wavefunction, and the barrier thickness as calculated numerically. The hybridization impacts the emitted photon statistics manifesting a faster radiative decay rate, photon bunching effect, and modified Auger recombination pathway compared to the monomer artificial atoms. Future perspectives for the nanocrystals chemistry paradigm are highlighted.