Hole-Acceptor-Manipulated Electron Spin Dynamics in CdSe Colloidal Quantum Dots

Electron spin dynamics in CdSe quantum dots with hole acceptors are investigated by time-resolved ellipticity spectroscopy. Two types of hole acceptors, Li­[Et₃BH] and 1-octanethiol, result in distinctly different electron spin dynamics. The differences include electron g factors, spin dephasing/relaxation times, and mechanisms. In CdSe quantum dots with Li­[Et₃BH], the electron spin dephasing and relaxation are dominated by electron–nuclear hyperfine interactions in zero and weak magnetic fields. In contrast, hyperfine interactions, electron carrier lifetimes, and exchange interactions between electrons and holes or surface dangling bond spins control the electron spin dynamics in CdSe quantum dots with 1-octanethiol. Inhomogeneous dephasing limits the spin coherence time in larger transverse magnetic fields for both hole acceptor cases, but with distinct different g-factor inhomogeneity. These findings manifest that surface conditions play an important role in the spin dynamics and that thereby the surface and its surroundings can be exploited to control the spin in colloidal nanostructures.