Measurement of the Thulium Ion Spin Hamiltonian Within a Yttrium Gallium Garnet Host Crystal

We characterize the magnetic properties for thulium ion energy levels in the Y₃Ga₅O₁₂ (Tm:YGG) lattice with the goal to improve decoherence and reduce line-width broadening caused by local host spins and crystal imperfections. More precisely, we measure hyperfine tensors for the lowest level of the, ³H₆, and excited, ³H₄, states using a combination of spectral hole burning, absorption spectroscopy, and optically detected nuclear magnetic resonance. By rotating the sample through a series of angles with an applied external magnetic field, we measure and analyze the orientation dependence of the Tm³⁺ ion's spin-Hamiltonian. Using this spin-Hamiltonian, we propose a set of orientations to improve material properties that are important for light-matter interaction and quantum information applications. Our results yield several important external field directions: some to extend optical coherence times, another to improve spin inhomogeneous broadening, and yet another that maximizes mixing of the spin states for specific sets of ions, which allows improving optical pumping and creation of lambda systems in this material.