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Physical Review B

Narrow inhomogeneous and homogeneous optical linewidths in a rare earth doped transparent ceramic

Alban Ferrier, Charles W. Thiel, Biagio Tumino, Mariola O. Ramírez, L. E. Bausá, R. L. Cone, Akio Ikesue, Philippe Goldner

Published Jan 11, 2013• 29 citations
Publisher

Abstract

Inhomogeneous and homogeneous linewidth are reported in a Eu${}^{3+}$ doped transparent Y${}_{2}$O${}_{3}$ ceramic for the ${}^{7}$F${}_{0}$-${}^{5}$D${}_{0}$ 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 (${T}_{2}$ $=$ 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 Eu${}^{3+}$segregation at the grain boundaries, evidenced through confocal microfluorescence, further indicates that the majority of Eu${}^{3+}$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.

DOI
10.1103/physrevb.87.041102

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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 \ensuremathμ\ensuremath{\mu}\ensuremathμs). 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.
Homogeneous linewidths below 10 kHz are reported for the first time in high-quality Eu3+ doped Y 2O3 transparent ceramics. This result is obtained on the 7F0→5D0 transition in Eu3+ doped Y 2O3 ceramics and corresponds to an improvement of nearly one order of magnitude compared to previously reported values in transparent ceramics. Furthermore, we observed spectral hole lifetimes of ∼15 min that are long enough to enable efficient optical pumping of the nuclear hyperfine levels. Additionally, different Eu3+ concentrations (up to 1.0%) were studied, resulting in an increase of up to a factor of three in the peak absorption coefficient. These results suggest that transparent ceramics can be useful in applications where narrow and deep spectral holes can be burned into highly absorbing lines, such as quantum information processing and spectral filtering.
We present a case study on Eu 3+ -doped Y 2 O 3 transparent ceramics in which high-resolution laser spectroscopy is used as a material characterization tool. By comparing the results from coherent and incoherent optical spectroscopy with other characterization methods, we show that optical techniques can deliver supplementary information about the local environment of the activator ions in materials. Thus, high-resolution spectroscopy may be of interest for the investigation of a wider range of rare earth doped optical materials beyond materials studied for quantum information technology. The refinement of optical spectroscopy for the study of narrow optical transitions in rare earth ion single crystals has demonstrated that these techniques are extremely sensitive tools for probing the local environment of the rare earth ion. These techniques, such as photon echo experiments, have been important in developing materials for quantum information technology and spectral filtering applications. Here, we apply these techniques to transparent ceramic samples and compare the results with information gained from conventional material characterization techniques. Our present study demonstrates the high sensitivity of laser spectroscopic methods to microstructural strain and the presence of defects. In particular, the sensitivity is sufficient to detect small changes introduced by different thermal treatments in nominally equivalent materials. The results of our work show that it is possible to relate high-resolution optical measurements to defects and microstructural strain.
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.
Rare Earth (RE) ion doped nanomaterials are promising candidates for a range of quantum technology applications. Among RE ions, the so-called Kramers' ions possess spin transitions in the GHz range at low magnetic fields, which allows for high-bandwidth multimode quantum storage, fast qubit operations as well as interfacing with superconducting circuits. They also present relevant optical transitions in the infrared. In particular, Er3+{\mathrm{Er}}^{3+}Er3+ has an optical transition in the telecom band, while Nd3+{\mathrm{Nd}}^{3+}Nd3+ presents a high-emission-rate transition close to 890 nm. In this paper, we measure spectroscopic properties that are of relevance to using these materials in quantum technology applications. We find the inhomogeneous linewidth to be 10.7 GHz for Er3+{\mathrm{Er}}^{3+}Er3+ and 8.2 GHz for Nd3+{\mathrm{Nd}}^{3+}Nd3+, and the excited state lifetime T1{T}_{1}T1​ to be 13.68 ms for Er3+{\mathrm{Er}}^{3+}Er3+ and $540\phantom{\rule{0.16em}{0ex}}\textmu{}\mathrm{s}$ for Nd3+{\mathrm{Nd}}^{3+}Nd3+. We study the dependence of homogeneous linewidth on temperature for both samples, with the narrowest linewidth being 379 kHz (T2=839{T}_{2}=839T2​=839 ns) for Er3+{\mathrm{Er}}^{3+}Er3+ measured at 3 K, and 62 kHz (${T}_{2}=5.14\phantom{\rule{4pt}{0ex}}\textmu{}\mathrm{s}$) for Nd3+{\mathrm{Nd}}^{3+}Nd3+ measured at 1.6 K. Further, we investigate time-dependent homogeneous linewidth broadening due to spectral diffusion and the dependence of the homogeneous linewidth on magnetic field to get additional clarity of mechanisms that can influence the coherence time. In light of our results, we discuss two applications: single qubit-state readout and a Fourier-limited single photon source.
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.