Optical Orientation of Mn$^{2+}$ Spins in Bulk (Zn, Mn)Se Induced by Magnetic Field

TL;DR

This study demonstrates optical orientation of Mn$^{2+}$ spins in bulk (Zn, Mn)Se under magnetic field using circularly polarized light, revealing complex spin dynamics influenced by Jahn-Teller effects and symmetry considerations.

Contribution

It provides a theoretical model explaining the selection rules and spin orientation mechanisms for Mn$^{2+}$ ions during optical excitation in a bulk semiconductor.

Findings

Non-monotonic circular polarization dependence on magnetic field

Jahn-Teller coupling causes energy splitting of spin states

Optical orientation depends on Jahn-Teller configurations and relaxation times

Abstract

The optical orientation of Mn$^{2+}$ spins in the first excited state $^4$T$_1$ was experimentally observed in bulk (Zn, Mn)Se ($x_\mathrm{Mn}=0.01$) in the an external magnetic field of up to $6\,$T in Faraday geometry. This occurred during quasi-resonant continuous wave circularly polarized photoexcitation of the intracenter d-d transitions. A non-monotonic dependence of the thermal circular polarization of the intracenter photoluminescence on the magnetic field was observed. A theoretical model is proposed to describe the selection rules for resonant optical d-d transitions of an isolated Mn$^{2+}$ ion in a ZnSe cubic crystal. These rules are based on the analysis of the total angular momentum symmetry for the ground ($^6$A$_1$) and first excited ($^4$T$_1$) states of the Mn$^{2+}$ ion. This discussion neglects the specific mechanism for spin-flip processes in a d-shell of the ion during optical excitation. The analysis is founded on the rotational symmetry of the effective total angular momenta and parity for each state as a whole. Additionally, the Jahn-Teller coupling of the excited state orbital parts with tetragonal ($e$-type) local distortions of the crystal lattice is considered. This coupling results in the segregation of cubic axes and spin projections on these axes due to weak spin-orbit and spin-spin coupling in the excited state. This leads to energy splitting for spin states with their projections of $\pm 1/2$ and $\pm 3/2$ on each axis distinguished by specific Jahn-Teller distortion in the corresponding atomic potential minimum. By introducing two different times of relaxation to reach thermodynamic equilibrium for $\pm 1/2$ and $\pm 3/2$ states in each Jahn-Teller configuration, an angle dependent optical orientation contribution in photoluminescence polarization arises in the presence of a magnetic field.