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arXiv:1911.05058 · Physical review. B./Physical review. B

Subkilohertz optical homogeneous linewidth and dephasing mechanisms in Er3+ : Y2O3 ceramics

Rikuto Fukumori, Yizhong Huang, Jun Mo Yang, Haitao Zhang, Tian Zhong

Published Jun 8, 2020• 32 citations
arXivHTMLPDF

Abstract

Rare-earth dopants in solids are conducive of sharp optical transitions and long spin coherence at cryogenic temperatures. While superb coherences are routine in high-quality bulk crystals, the more versatile materials such as rare-earth doped nanoparticles and ceramics have suffered from excessive decoherence due to disorder. This work reports a surprisingly narrow linewidth of Er in Y${}_{2}$O${}_{3}$ ceramics made with industry-standard synthesis technique, putting it on par with the best single crystalline counterpart. The ultranarrow linewidth also helps clarify decoherence pathways within the matrix.

DOI
10.1103/physrevb.101.214202

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Rare-earth dopants in solids are conducive of sharp optical transitions and long spin coherence at cryogenic temperatures. While superb coherences are routine in high-quality bulk crystals, the more versatile materials such as rare-earth doped nanoparticles and ceramics have suffered from excessive decoherence due to disorder. This work reports a surprisingly narrow linewidth of Er in Y2{}_{2}2​O3{}_{3}3​ ceramics made with industry-standard synthesis technique, putting it on par with the best single crystalline counterpart. The ultranarrow linewidth also helps clarify decoherence pathways within the matrix.
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.
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.
La3+ is used as an index modifier to tune the refractive index of Er3+ doped Y2O3 transparent ceramics without reducing the coherence lifetime of Er3+ 4I13/2−4I15/2 transition. La3+ and Er3+ are incorporated into Y2O3 through a solution-phase nanoparticle synthesis and nanoparticles are sintered into transparent ceramics by hot isostatic press. The maximum La3+ doping concentration is about 10%, which increases the refractive index of Y2O3 by 0.009 (Δn/n = 0.48%). La3+ doping doesn’t reduce Er3+ optical coherence lifetime. The homogeneous linewidth of Er3+(20 ppm) 4I13/2−4I15/2 transition in La3+ doped Y2O3 ceramics is about 10 kHz at 2 K and 0.65 T, which is close to the reported homogeneous linewidth in Er3+ doped Y2O3 ceramics and single crystals. Such La3+ Er3+ co-doped Y2O3 ceramics are proper materials to fabricate optical waveguides for quantum memory applications.
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.
Rare-earth emitters in solids are well suited for implementing efficient, long-lived quantum memory coupled to integrated photonics for scalable quantum technologies. They are typically introduced as dopants in a solid-state host, but this introduces disorder and limits the available density of emitters. Stoichiometric materials can offer high densities with narrow optical linewidths. The regular spacing of emitters also opens possibilities for quantum information processing and collective effects. Here, we show narrow optical linewidths in a layered stoichiometric crystalline material, NaEu(IO_{3})_{4}. We observed an inhomogeneous linewidth of 2.2(1) GHz and a homogeneous linewidth of 120(4) kHz. Using spectral hole-burning techniques, we observe a hyperfine spin lifetime of 1.9(4) s. Furthermore, we demonstrate an atomic frequency comb delay of up to 800 ns.
Ultralong-lived Coherent States in Eu3+^{3+}3+:Y2_22​O3_33​ Optical Ceramics for Quantum Memories
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 growth difficulties of high-quality REI materials and a lack of comprehensive understanding of REI's decoherence mechanisms. Here we realize a record optical coherence time of 421.5 ±\pm± 10.5 μμμs for the 7^77F0→5_0\rightarrow^50​→5D0_00​ transition and more than 30 hours lifetime for the 7^77F0_00​ hyperfine spin states in Eu3+^{3+}3+:Y2_22​O3_33​ optical ceramics. We report the elimination of two-level-system induced optical decoherence in short-range ordered crystals. Meanwhile, a new decoherence mechanism caused by new kinds of perturbing magnetic centers is identified below 1.5 K. We further demonstrate the coherent light storage over 5 μμμs by using the atomic frequency comb protocol. These results open up prospects for the realization of practical quantum memories and large scale quantum communications with REI optical ceramics.