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Journal of Physics Condensed Matter

Nuclear spin coherence properties of 151 Eu 3+ and 153 Eu 3+ in a Y 2 O 3 transparent ceramic

Jenny Karlsson, Nathalie Kunkel, Akio Ikesue, Alban Ferrier, Philippe Goldner

Published Feb 8, 2017• 19 citations
Publisher

Abstract

Abstract We have measured inhomogeneous linewidths and coherence times ( T 2 ) of nuclear spin transitions in a Eu 3+ :Y 2 O 3 transparent ceramic by an all-optical spin echo technique. The nuclear spin echo decay curves showed a strong modulation which was attributed to interaction with Y nuclei in the host. The coherence time of the 29 MHz spin transition in 151 Eu 3+ was 16 ms in a small applied magnetic field. Temperature dependent measurements showed that the coherence time was constant up to 18 K and was limited by spin-lattice relaxation for higher temperatures. Nuclear spin echoes in 153 Eu 3+ gave much weaker signals than for the case of 151 Eu 3+ . The spin coherence time for the 73 MHz spin transition in 153 Eu 3+ was estimated to 14 ms in a small magnetic field. The study shows that the spin transitions of ceramic Eu 3+ :Y 2 O 3 have coherence properties comparable to the best rare-earth-doped materials available.

DOI
10.1088/1361-648x/aa529a

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We identify and analyze dephasing mechanisms that broaden the optical transitions of rare-earth ions in randomly oriented transparent ceramics. The study examines the narrow $^{7}F_{0}\phantom{\rule{4pt}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{4pt}{0ex}}^{5}D_{0}$ transition of ${\mathrm{Eu}}^{3+}$ dopants in a series of ${\mathrm{Y}}_{2}{\mathrm{O}}_{3}$ ceramic samples prepared under varying conditions. We characterize the temperature and magnetic field dependence of the homogeneous linewidth, as well as long-term spectral diffusion on time scales up to 1 s. The results highlight significant differences between samples with differing thermal treatments and ${\mathrm{Zr}}^{4+}$ additive concentrations. In particular, several distinct magnetic interactions from defect centers are observed, which are clearly distinguished from the broadening due to interactions with two-level systems and phonons. By minimizing the broadening due to the different defect centers, linewidths of the order of 4 kHz are achieved for all samples. The linewidths are limited by temperature-dependent interactions and by an interaction that is yet to be identified. Although the homogeneous linewidth can be narrowed further in these ceramic samples, the broadening is now comparable to the linewidths achieved in rare-earth-ion--doped single crystals. Thus, this work emphasizes the usefulness of studying ceramics to gain insights into dephasing mechanisms relevant to single crystals and suggests that ceramics may be an interesting alternative for applications in classical and quantum information processing.

Physical review. B./Physical review. B•Nov 1, 2016•30 citations
Abstract We have measured inhomogeneous linewidths and coherence times ( T 2 ) of nuclear spin transitions in a Eu 3+ :Y 2 O 3 transparent ceramic by an all-optical spin echo technique. The nuclear spin echo decay curves showed a strong modulation which was attributed to interaction with Y nuclei in the host. The coherence time of the 29 MHz spin transition in 151 Eu 3+ was 16 ms in a small applied magnetic field. Temperature dependent measurements showed that the coherence time was constant up to 18 K and was limited by spin-lattice relaxation for higher temperatures. Nuclear spin echoes in 153 Eu 3+ gave much weaker signals than for the case of 151 Eu 3+ . The spin coherence time for the 73 MHz spin transition in 153 Eu 3+ was estimated to 14 ms in a small magnetic field. The study shows that the spin transitions of ceramic Eu 3+ :Y 2 O 3 have coherence properties comparable to the best rare-earth-doped materials available.
ABSTRACT Rare‐earth‐ion‐doped solid materials have attracted considerable interest for quantum technologies. However, achieving robust spin coherence in polycrystalline systems remains challenging due to structural disorder and limited understanding spin environments. Here, we report high‐quality : optical ceramics with optical inhomogeneous of GHz and sub‐kHz homogeneous linewidths, indicating a spectrally quiet optical environment. At cryogenic temperatures, spin‐dynamics measurements show that decoherence is strongly influenced by the surrounding nuclear spin bath. Magnetic‐field‐dependent studies, combined with radio‐frequency spectroscopy, reveal the sensitivity of spin coherence to weak magnetic perturbations and enable selective addressing of the bath spins. By applying an all‐optical Raman dynamical decoupling protocol, we substantially prolong the observed nuclear‐spin coherence decay, yielding a slow decay component of 224 ms. These results establish : ceramics as a promising platform for solid‐state quantum memories and highlight the potential of spin‐bath engineering in polycrystalline rare‐earth‐ion systems.
We show that the coherence properties of the nuclear spin states of rare-earth ions in solids can be manipulated by small applied electric fields. This was done by measuring the Stark effect on the nuclear quadrupole transitions of 151Eu^{151}\mathrm{Eu}151Eu in Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ (YSO) using a combination of Raman heterodyne optical detection and Stark modulated quadrupole echoes to achieve high sensitivity. The measured Stark coefficients were 0.42 and 1.0  Hz cm/V1.0\text{ }\text{ }\mathrm{Hz}\text{ }\mathrm{cm}/\mathrm{V}1.0  Hz cm/V for the two quadrupole transitions at 34.54 and 46.20 MHz, respectively. The long decoherence time of the nuclear spin states (25 ms) allowed us to make the measurements in very low electric fields of $\ensuremath{\sim}10\text{ }\text{ }\mathrm{V}/\mathrm{cm}$, which produced 100% modulation of the nuclear spin echo, and to measure Stark shifts of $\ensuremath{\sim}1\text{ }\text{ }\mathrm{Hz}$ or 20 ppm of the inhomogeneous linewidth.
We report a low-temperature spectroscopic characterization of the ground-state hyperfine transitions in 151Eu3+:Y2SiO5{}^{151}\mathrm{Eu}{}^{3+}{\mathrm{:Y}}_{2}{\mathrm{SiO}}_{5}151Eu3+:Y2​SiO5​ via coherent Raman scattering. Inhomogeneous linewidths of 21 and 38 kHz were measured for the ${I}_{z}=\ifmmode\pm\else\textpm\fi{}\frac{1}{2}$ $\ensuremath{\leftrightarrow}$ $\ifmmode\pm\else\textpm\fi{}\frac{3}{2}$ and the $\ifmmode\pm\else\textpm\fi{}\frac{3}{2}$ $\ensuremath{\leftrightarrow}$ $\ifmmode\pm\else\textpm\fi{}\frac{5}{2}$ ground-state transitions, respectively. Spin-echo decays were recorded for the ${I}_{z}=\ifmmode\pm\else\textpm\fi{}\frac{1}{2}$ $\ensuremath{\leftrightarrow}$ $\ifmmode\pm\else\textpm\fi{}\frac{3}{2}$ transition at zero field and for a small static magnetic field. In the latter case, analysis by a simple model gave an amplitude of 284 Hz and a correlation time of 3.5 ms for the transition frequency fluctuations. Application of a dynamical decoupling sequence resulted in coherence lifetimes up to 474 ms, an 18-fold increase compared to the spin intrinsic phase memory time of 26 ms.
Inhomogeneous and homogeneous linewidth are reported in a Eu3+{}^{3+}3+ doped transparent Y2{}_{2}2​O3{}_{3}3​ ceramic for the 7{}^{7}7F0{}_{0}0​-5{}^{5}5D0{}_{0}0​ transition, using high-resolution coherent spectroscopy. The 8.7-GHz inhomogeneous linewidth is close to that of single crystals, as is the 59-kHz homogeneous linewidth at 3 K (T2{T}_{2}T2​ === 5.4 $\ensuremath{\mu}$s). The homogeneous linewidth exhibits a temperature dependence that is typical of a crystalline environment, and additional dephasing observed in the ceramic is attributed to magnetic impurities or defects introduced during the synthesis process. The absence of Eu3+{}^{3+}3+segregation at the grain boundaries, evidenced through confocal microfluorescence, further indicates that the majority of Eu3+{}^{3+}3+ions in the ceramic experience an environment comparable to a single crystal. The obtained results suggest that ceramic materials can be competitive with single crystals for applications in quantum information and spectral hole burning devices, beyond their current applications in lasers and scintillators.
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.
We identify and analyze dephasing mechanisms that broaden the optical transitions of rare-earth ions in randomly oriented transparent ceramics. The study examines the narrow $^{7}F_{0}\phantom{\rule{4pt}{0ex}}\ensuremath{\leftrightarrow}\phantom{\rule{4pt}{0ex}}^{5}D_{0}$ transition of Eu3+{\mathrm{Eu}}^{3+}Eu3+ dopants in a series of Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​ ceramic samples prepared under varying conditions. We characterize the temperature and magnetic field dependence of the homogeneous linewidth, as well as long-term spectral diffusion on time scales up to 1 s. The results highlight significant differences between samples with differing thermal treatments and Zr4+{\mathrm{Zr}}^{4+}Zr4+ additive concentrations. In particular, several distinct magnetic interactions from defect centers are observed, which are clearly distinguished from the broadening due to interactions with two-level systems and phonons. By minimizing the broadening due to the different defect centers, linewidths of the order of 4 kHz are achieved for all samples. The linewidths are limited by temperature-dependent interactions and by an interaction that is yet to be identified. Although the homogeneous linewidth can be narrowed further in these ceramic samples, the broadening is now comparable to the linewidths achieved in rare-earth-ion--doped single crystals. Thus, this work emphasizes the usefulness of studying ceramics to gain insights into dephasing mechanisms relevant to single crystals and suggests that ceramics may be an interesting alternative for applications in classical and quantum information processing.