Resonant Spectroscopy of II-VI Self-Assembled Quantum Dots: Excited States and Exciton-LO Phonon Coupling

TL;DR

This study investigates carrier excitation mechanisms and exciton-LO phonon coupling in CdTe/ZnTe and CdSe/ZnSe quantum dots using resonant photoluminescence spectroscopy, revealing size-dependent interactions and energy distributions.

Contribution

It provides new insights into the size-dependent exciton-LO phonon coupling and excited state distributions in self-assembled quantum dots through resonant spectroscopy.

Findings

Excited state energies are shifted by 100 meV above ground states in CdTe quantum dots.

LO phonon-assisted absorption shows size selectivity, with stronger coupling in smaller dots.

Annealing increases dot size, altering exciton-LO phonon interactions to reflect energy distribution.

Abstract

Using resonantly excited photoluminescence along with photoluminescence excitation spectroscopies, we study the carrier excitation processes in CdTe/ZnTe and CdSe/ZnSe self-assembled quantum dots. Photoluminescence excitation spectra of single CdTe quantum dots reflect two major mechanisms for carrier excitation: The first, associated with the presence of sharp and intense lines in the spectrum, is a direct excited state ? ground state transition. The second, associated with the appearance of up to four much broader excitation lines, is a LO phonon-assisted absorption directly into the quantum dot ground states. LO phonons with energies of both quantum dots and ZnTe barrier material are identified in the photoluminescence excitation spectra. Resonantly excited PL measurements for the dot ensemble as a function of excitation energy makes it possible to separate the contributions of these two mechanisms. We find that for CdTe quantum dots the distribution of excited states coupled to the ground states reflects the energy distribution of the quantum dot emission, but shifted up in energy by 100 meV. This large splitting between excited and ground states in CdTe quantum dots suggests strong spatial confinement. In contrast, the LO phonon-assisted absorption shows significant size selectivity. In the case of CdTe dots the exciton-LO phonon coupling is strongly enhanced for smaller-sized dots which have higher emission energies. In contrast, for CdSe quantum dots the exciton-LO phonon coupling is uniform over the ensemble ? that is, the energy distribution determines the intensities of LO phonon replicas. We show that for CdTe quantum dots after annealing, that is after an increase in the average dot size, the exciton-LO phonon interaction reflects the dot energy distribution, as observed for CdSe quantum dots.