Rare-earth ion-doped crystals are of great interest for quantum memories, a central component in future quantum repeaters. To assess the promise of 1 % Tm ³⁺-doped yttrium gallium garnet (Tm:YGG), we report measurements of optical coherence and energy-level lifetimes of its ³H 6 ↔ 3 H ₄ transition at a temperature of around 500 mK and various magnetic fields. Using spectral hole burning (SHB), we find hyperfine ground-level (Zeeman level) lifetimes of several minutes at magnetic fields of less than 1000 G. We also measure coherence time exceeding one millisecond using two-pulse photon echoes. Three-pulse photon echo and SHB measurements reveal that due to spectral diffusion, the effective coherence time reduces to a few µs over a timescale of around two hundred seconds. Finally, temporal and frequency-multiplexed storage of optical pulses using the atomic frequency comb protocol is demonstrated. Our results suggest Tm:YGG to be promising for multiplexed photonic quantum memory for quantum repeaters.

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The creation of well-understood structures using spectral hole burning is an important task in the use of technologies based on rare-earth ion-doped crystals. We apply a series of different techniques to model and improve the frequency dependent population change in the atomic level structure of thulium yttrium gallium garnet (Tm:YGG). In particular we demonstrate that, at zero applied magnetic field, numerical solutions to frequency-dependent three-level rate equations show good agreement with spectral hole-burning results. This allows us to predict spectral structures given a specific hole-burning sequence, the underpinning spectroscopic material properties, and the relevant laser parameters. This enables us to largely eliminate power-dependent hole broadening through the use of adiabatic hole-burning pulses. Although this system of rate equations shows good agreement at zero field, the addition of a magnetic field results in unexpected spectral diffusion proportional to the induced Tm ion magnetic-dipole moment and average magnetic-field strength, which, through the quadratic Zeeman effect, dominates the optical spectrum over long timescales. Our results allow optimization of the preparation process for spectral structures in a large variety of rare-earth ion-doped materials for quantum memories and other applications.

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We characterize the optical coherence and energy-level properties of the 795-nm H63 to H43 transition of Tm3+ in a Ti4+:LiNbO3 waveguide at temperatures as low as 0.65 K. Coherence properties are measured with varied temperature, magnetic field, optical excitation power and wavelength, and measurement timescale. We also investigate nuclear spin-induced hyperfine structure and population dynamics with varying magnetic field and laser excitation power. Except for accountable differences due to different Ti4+- and Tm3+-doping concentrations, we find that the properties of Tm3+:Ti4+:LiNbO3 produced by indiffusion doping are consistent with those of a bulk-doped Tm3+:LiNbO3 crystal measured under similar conditions. Our results, which complement previous work in a narrower parameter space, support using rare-earth ions for integrated optical and quantum signal processing.

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We characterize the magnetic properties for thulium ion energy levels in the (Tm:YGG) lattice with the goal to improve decoherence and reduce linewidth broadening caused by local host spins and crystal imperfections. More precisely, we measure hyperfine tensors for the lowest level of and excited 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 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.

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Nanostructured rare-earth-ion-doped materials are increasingly being investigated for on-chip implementations of quantum information processing protocols as well as commercial applications such as fluorescent lighting. However, achieving high-quality and optimized materials at the nanoscale is still challenging. Here we present a detailed study into the restriction of phonon processes in the transition from bulk crystals to small (≤40-nm) nanocrystals by observing the relaxation dynamics between crystal-field levels of Tb3+:Y3Al5O12. We find that the population relaxation dynamics are modified as the particle size is reduced, consistent with our simulations of inhibited relaxation through a modified vibrational density of states and hence modified phonon emission. However, our experiments also indicate that nonradiative processes not driven by phonons are also present in the smaller particles, causing transitions and rapid thermalization between the levels on a time scale of <100ns.@en