Exciton Dephasing by Phonon-Induced Scattering between Bright Exciton States in InP/ZnSe Colloidal Quantum Dots

ACS Nano. 2023 Jul 11;17(13):12118-12126. doi: 10.1021/acsnano.2c12182. Epub 2023 Jun 16.

Abstract

Decoherence or dephasing of the exciton is a central characteristic of a quantum dot (QD) that determines the minimum width of the exciton emission line and the purity of indistinguishable photon emission during exciton recombination. Here, we analyze exciton dephasing in colloidal InP/ZnSe QDs using transient four-wave mixing spectroscopy. We obtain a dephasing time of 23 ps at a temperature of 5 K, which agrees with the smallest line width of 50 μeV we measure for the exciton emission of single InP/ZnSe QDs at 5 K. By determining the dephasing time as a function of temperature, we find that exciton decoherence can be described as a phonon-induced, thermally activated process. The deduced activation energy of 0.32 meV corresponds to the small splitting within the nearly isotropic bright exciton triplet of InP/ZnSe QDs, suggesting that the dephasing is dominated by phonon-induced scattering within the bright exciton triplet.

Keywords: Colloidal quantum dots; InP; dephasing; fine structure; four-wave mixing; homogeneous line width; zero phonon line.