Origin of Two Larmor Frequencies in the Coherent Spin Dynamics of Colloidal CdSe Quantum Dots Revealed by Controlled Charging

TL;DR

This study reveals that the two Larmor frequencies observed in the coherent spin dynamics of colloidal CdSe quantum dots originate from electrons localized differently within the QD, influenced by surface states and controlled charging.

Contribution

It demonstrates that surface states and controlled photocharging determine the two distinct Larmor frequencies in colloidal CdSe QDs, clarifying their spin dynamics origin.

Findings

Surface states influence the spin signals in CdSe QDs.

Controlled charging enhances specific spin components.

Core/shell QDs show weaker spin signals.

Abstract

Coherent spin dynamics in colloidal CdSe quantum dots (QDs) typically show two spin components with different Larmor frequencies, whose origin is an open question. We exploit the photocharging approach to identify their origin and find that surface states play a key role in the appearance of the spin signals. By controlling the photocharging with electron or hole acceptors, we show that the specific spin component can be enhanced by the choice of acceptor type. In core/shell CdSe/ZnS QDs, the spin signals are significantly weaker. Our results exclude the neutral exciton as the spin origin and suggest that both Larmor frequencies are related to the coherent spin precession of electrons in photocharged QDs. The lower frequency is due to the electron confined in the middle of the QD, and the higher frequency to the electron additionally localized in the vicinity of the surface.