Two-phonon assisted exciton spin relaxation due to exchange interaction in spherical quantum dots

TL;DR

This study investigates spin relaxation in spherical CdS quantum dots, revealing a novel phonon-assisted mechanism driven by exchange interaction that explains nanosecond spin-relaxation times at room temperature.

Contribution

The paper introduces a new phonon-assisted exciton spin relaxation mechanism involving exchange interaction, supported by both experimental data and theoretical calculations.

Findings

Spin relaxation time of several nanoseconds at room temperature.

Agreement between calculated transition rates and experimental results.

Identification of a phonon-assisted spin-flip process driven by exchange interaction.

Abstract

Spin relaxation in undoped quasi-spherical CdS quantum dots at zero magnetic fields is investigated using time- and polarization-resolved transient absorption measurements. Unlike in previous studies of these systems, the measured signals were corrected for spin-insensitive contributions to the exciton bleaching dynamics, {allowing us to determine} the pure spin-related exciton dynamics. To explain the observed room-temperature spin-relaxation time of several nanoseconds, we propose a novel mechanism based on intralevel exciton transitions with the emission of one LO phonon, the absorption of another LO phonon, and an electron spin flip, which is driven by the electron-hole exchange interaction. The transition rates, calculated in the present work for different sizes of quantum dots and temperatures, are in fair agreement with our experimental results.