Quadratic Zeeman effect and spin-lattice relaxation of Tm$^{3+}$:YAG at high magnetic fields

TL;DR

This study investigates the quadratic Zeeman effect and spin-lattice relaxation in Tm$^{3+}$:YAG at high magnetic fields, revealing site-specific shifts, relaxation behaviors, and confirming theoretical phonon coupling predictions.

Contribution

It provides detailed measurements of the quadratic Zeeman effect and spin relaxation in Tm$^{3+}$:YAG, including the first observation of magnetic field dependence of the Orbach process at high fields.

Findings

Large anisotropic quadratic Zeeman shifts enable spectral resolution of ion subsets.

Spin lifetime decreases rapidly at high magnetic fields, indicating weak direct-phonon contribution.

Observed magnetic field dependence of the Orbach process explains changes in electronic energy levels.

Abstract

Anisotropy of the quadratic Zeeman effect for the $^3{\rm H}_6 \rightarrow \, ^3{\rm H}_4$ transition at 793 nm wavelength in $^{169}$Tm$^{3+}$-doped Y$_3$Al$_5$O$_{12}$ is studied, revealing shifts ranging from near zero up to + 4.69 GHz/T$^2$ for ions in magnetically inequivalent sites. This large range of shifts is used to spectrally resolve different subsets of ions and study nuclear spin relaxation as a function of temperature, magnetic field strength, and orientation in a site-selective manner. A rapid decrease in spin lifetime is found at large magnetic fields, revealing the weak contribution of direct-phonon absorption and emission to the nuclear spin-lattice relaxation rate. We furthermore confirm theoretical predictions for the phonon coupling strength, finding much smaller values than those estimated in the limited number of past studies of thulium in similar crystals. Finally, we observe a significant -- and unexpected -- magnetic field dependence of the two-phonon Orbach spin relaxation process at higher field strengths, which we explain through changes in the electronic energy-level splitting arising from the quadratic Zeeman effect.