Spin-lattice relaxation processes of transition metal ions in a heavily cobalt doped ZnO: Phonon heating effect

Abstract

Inversion recovery with electron spin-echo detection has been used to study the electron spin-lattice relaxation rates 1/T1 for transition metal impurities in heavily cobalt-doped hydrothermally grown ZnO single crystals. The relaxation dynamics of Co2+ ions dominates the phonon bottleneck effect in the Orbach-Aminov process, which involves the modulation of the zero-field-splitting tensor. The relaxation mechanism may be treated in terms of phonon heating with fast rate of energy pump from Co2+ spins into the lattice phonon modes. The measurements reveal the cross-relaxation process in which the single Co2+ ions cross-relax to exchange-coupled clusters of cobalt ions. The higher temperature relaxation of Co2+ indicates an additional Orbach-Aminov process via a state of ∼226 cm−1 above the ground state Kramers doublet. It is shown that in this system Co2+ ions play a role of the rapidly relaxing centers, strongly mediating the spin-lattice relaxation of the other transition metal impurities, such as Mn2+ and Fe3+.