Optical control of an individual Cr spin in a semiconductor quantum dot

TL;DR

This paper demonstrates optical control of a single Cr atom's spin in a quantum dot, revealing its magnetic properties, relaxation dynamics, and tunability, with potential applications in hybrid spin-mechanical systems.

Contribution

It introduces a method for optically initializing and controlling a single Cr spin in a quantum dot, including spin state tuning via the optical Stark effect, which is novel in this context.

Findings

Cr spin exhibits large magnetic anisotropy due to local strain.

Single Cr spin can be prepared and monitored by resonant optical pumping.

Cr spin relaxation time is in the microsecond range.

Abstract

We demonstrate that the spin of a Cr atom in a quantum dot (QD) can be controlled optically and we discuss the main properties of this single spin system. The photoluminescence of individual Cr-doped QDs and their evolution in magnetic field reveal a large magnetic anisotropy of the Cr spin induced by local strain. This results in a splitting of the Cr spin states and in a thermalization on the lower energy states states S$_z$=0 and S$_z$=$\pm$1. The magneto-optical properties of Cr-doped QDs can be modelled by an effective spin Hamiltonian including the spin to strain coupling and the influence of the QD symmetry. We also show that a single Cr spin can be prepared by resonant optical pumping. Monitoring the intensity of the resonant fluorescence of the QD during this process permits to probe the dynamics of the optical initialization of the spin. Hole-Cr flip-flops induced by an interplay of the hole-Cr exchange interaction and the coupling with acoustic phonons are the main source of relaxation that explains the efficient resonant optical pumping. The Cr spin relaxation time is measured in the $\mu s$ range. We evidence that a Cr spin couples to non-equilibrium acoustic phonons generated during the optical excitation inside or near the QD). Finally we show that the energy of any spin state of an individual Cr atom can be independently tuned by a resonant single mode laser through the optical Stark effect. All these properties make Cr-doped QDs very promising for the development of hybrid spin-mechanical systems where a coherent mechanical driving of an individual spin in an oscillator is required.