Methods for Obtaining One Single Larmor Frequency, Either or , in the Coherent Spin Dynamics of Colloidal Quantum Dots.

The coexistence of two spin components with different Larmor frequencies in colloidal CdSe and CdS quantum dots (QDs) leads to the entanglement of spin signals, complicating the analysis of dynamic processes and hampering practical applications. Here, we explored several methods, including varying the types of hole acceptors, air or anaerobic atmosphere and laser repetition rates, in order to facilitate the obtention of one single Larmor frequency in the coherent spin dynamics using time-resolved ellipticity spectroscopy at room temperature. In an air or nitrogen atmosphere, manipulating the photocharging processes by applying different types of hole acceptors, e.g., Li[EtBH] and 1-octanethiol (OT), can lead to pure spin components with one single Larmor frequency. For as-grown QDs, low laser repetition rates favor the generation of the higher Larmor frequency spin component individually, while the lower Larmor frequency spin component can be enhanced by increasing the laser repetition rates. We hope that the explored methods can inspire further investigations of spin dynamics and related photophysical processes in colloidal nanostructures.