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Nanoscale Pr3+: Y2O3 for optical quantum technologies (Conference Presentation)

Diana Serrano, Chetan Deshmukh, Shuping Liu, Alexandre Tallaire, Alban Ferrier, Hugues de Riedmatten, Philippe Goldner

Published Mar 30, 2020• 0 citations
Publisher

Abstract

Nanoscale systems possessing long-lived spins and the ability to coherently couple to light are highly demanded for quantum devices implementations. Several approaches, like NV centers in diamond, semiconductor quantum dots are intensively investigated in the field, where an outstanding challenge is to preserve properties, and especially optical and spin coherence lifetimes, at the nanoscale. In this context, chemically synthesized Eu3+ doped Y2O3 nanoparticles have demonstrated great potential for quantum technologies based on their narrow optical homogeneous linewidth, down to the 10 kHz level, and millisecond-long spin coherence time. Here, we investigate an alternative nanoscale material: Pr3+: Y2O3. We first determine the Pr3+ hyperfine structure in Y2O3 by spectral hole burning and then measure photon and spin echoes from nanoparticles down to 150 nm. Spin T2 up to 880 μs was obtained for the ±3/2↔±5/2 hyperfine transition at 10.42 MHz, a value which exceeds that of bulk Pr3+doped crystals so far reported. These promising results confirm nanoscale Pr3+:Y2O3 as a very appealing candidate to integrate quantum devices.

DOI
10.1117/12.2555835

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Nanoscale systems possessing long-lived spins and the ability to coherently couple to light are highly demanded for quantum devices implementations. Several approaches, like NV centers in diamond, semiconductor quantum dots are intensively investigated in the field, where an outstanding challenge is to preserve properties, and especially optical and spin coherence lifetimes, at the nanoscale. In this context, chemically synthesized Eu3+ doped Y2O3 nanoparticles have demonstrated great potential for quantum technologies based on their narrow optical homogeneous linewidth, down to the 10 kHz level, and millisecond-long spin coherence time. Here, we investigate an alternative nanoscale material: Pr3+: Y2O3. We first determine the Pr3+ hyperfine structure in Y2O3 by spectral hole burning and then measure photon and spin echoes from nanoparticles down to 150 nm. Spin T2 up to 880 μs was obtained for the ±3/2↔±5/2 hyperfine transition at 10.42 MHz, a value which exceeds that of bulk Pr3+doped crystals so far reported. These promising results confirm nanoscale Pr3+:Y2O3 as a very appealing candidate to integrate quantum devices.
We investigate the potential for optical quantum technologies of Pr3+:Y2O3{\mathrm{Pr}}^{3+}:\phantom{\rule{0.28em}{0ex}}{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Pr3+:Y2​O3​ in the form of monodisperse spherical nanoparticles. We measured optical inhomogeneous lines of 27 GHz and optical homogeneous linewidths of 108 and 315 kHz in particles with 400- and 150-nm average diameters, respectively, for the $^{1}D_{2}(0)\ensuremath{\leftrightarrow}^{3}H_{4}(0)$ transition at 1.4 K. Furthermore, ground-state and 1D2^{1}D_{2}1D2​ excited-state hyperfine structures in Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}\phantom{\rule{0.16em}{0ex}}Y2​O3​ are here determined by spectral hole burning and modeled by complete Hamiltonian calculations. Ground-state spin transitions have energies of 5.99 and 10.42 MHz, for which we demonstrate spin inhomogeneous linewidths of 42 and 45 kHz, respectively. Spin T2{T}_{2}T2​ up to $880\phantom{\rule{0.28em}{0ex}}\ensuremath{\mu}\mathrm{s}$ was obtained for the $\ifmmode\pm\else\textpm\fi{}3/2\ensuremath{\leftrightarrow}\ifmmode\pm\else\textpm\fi{}5/2$ transition at 10.42 MHz, a value which exceeds that of bulk Pr3+{\mathrm{Pr}}^{3+}Pr3+-doped crystals reported so far. These promising results confirm nanoscale Pr3+:Y2O3{\mathrm{Pr}}^{3+}:\phantom{\rule{0.28em}{0ex}}{\mathrm{Y}}_{2}{\mathrm{O}}_{3}\phantom{\rule{0.16em}{0ex}}Pr3+:Y2​O3​ is a very appealing candidate to integrate quantum devices. In particular, we discuss the possibility of using this material for realizing spin-photon interfaces emitting indistinguishable single photons.
Rare earth (RE) doped crystals are promising materials for quantum information processing (QIP). In particular, Eu3+:Y2O3 bulk crystals present long optical coherent lifetimes (T2), a fundamental parameter for QIP. In this thesis, we investigated this system at the nanoscale, which could be used to build hybrid devices where RE are coupled to other quantum systems. This work focuses on the development of Eu3+: Y2O3 particles with sub-wavelength size and on the static and dynamical contributions to Eu3+ optical linewidth. Systems with different particle and crystallite sizes were prepared using homogeneous precipitation. Optical inhomogeneous linewidths were found to decrease with high temperature annealing and reached values close to those of bulk crystals, showing that low defect concentrations can be obtained. A quasi-linear correlation with Raman linewidths was also observed. T1 population decays were measured by fluorescence and found longer than in the bulk, in good agreement with a model based on an effective refractive index model. Optical T2 were investigated by photon echo (PE) and holeburning techniques. We observed a coherence lifetime of 7.1 µs at 1.7 K in a 0.5 % Eu3+ doped sample, the highest value reported for any nanocrystal. Temperature dependence and spectral diffusion studies indicate that structure fluctuations and spin flips dominate dephasing.
Rare earth ions (REI) in solid materials are among the leading systems for quantum technology applications. However, developing practical REI quantum devices with long-lived coherent states remains challenging due to great difficulties in growing high-quality REI materials and incomplete understanding of their decoherence mechanisms. In this work, we report a long optical coherence time of 422 ± 11 μs for the 7F0 → 5D0 transition, as well as a lifetime exceeding 30 hours for the 7F0 hyperfine spin states in Eu3+:Y2O3 optical ceramics. We identify the absence of two-level-system induced optical decoherence in short-range-ordered crystals and a decoherence mechanism caused by perturbing magnetic centers that were not detected previously below 1.5 K. Furthermore, we demonstrate coherent light storage over 5 μs by using the atomic frequency comb protocol. These results provide a promising proof-of-principle demonstration of quantum memory using Eu3+:Y2O3 optical ceramic system, highlighting its significant potential for practical quantum applications. Rare earth ions (REI) in solids are promising for quantum technologies. Here, the authors demonstrate a record optical coherence lifetime and the absence of two-level-system induced decoherence in Eu3+:Y2O3 optical ceramics. These findings advance the optimization of REI-based quantum systems and enable tailored material designs.
Abstract Nanoscale systems that coherently couple to light and possess spins offer key capabilities for quantum technologies. However, an outstanding challenge is to preserve properties, and especially optical and spin coherence lifetimes, at the nanoscale. Here, we report optically controlled nuclear spins with long coherence lifetimes (T2) in rare-earth-doped nanoparticles. We detect spins echoes and measure a spin coherence lifetime of 2.9 ± 0.3 ms at 5 K under an external magnetic field of 9 mT, a T2 value comparable to those obtained in bulk rare-earth crystals. Moreover, we achieve spin T2 extension using all-optical spin dynamical decoupling and observe high fidelity between excitation and echo phases. Rare-earth-doped nanoparticles are thus the only nano-material in which optically controlled spins with millisecond coherence lifetimes have been reported. These results open the way to providing quantum light-atom-spin interfaces with long storage time within hybrid architectures.