We present the characterization of stoichiometric europium materials as progress towards realizing long-lived, ensemble-based quantum memory devices. The candidate materials demonstrate inhomogeneous optical linewidths similar to those in doped materials with 1000x larger densities.
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.
Abstract Quantum memory is a core enabling device for large-scale quantum networks, serving as the fundamental building block for quantum repeaters and transportable quantum memories. Among various physical platforms, rare-earth-ion-doped crystals stand out as one of the most promising solid-state candidates for long-lived photonic quantum memories, owing to their exceptionally long spin coherence time and their compatibility with integration. In this review, we first introduce the physical mechanisms underlying long-lived spin coherence in rare-earth systems, with particular emphasis on the zero-first-order-Zeeman transition and dynamical decoupling techniques. We then review the experimental progress in this field, highlighting three distinct lifetimes—the spin coherence time, the light storage time, and the quantum storage time—and covering experiments that have achieved hour-scale spin coherence, minute- to hour-scale light storage, and minute-scale single-photon-level quantum storage. Finally, we discuss the remaining challenges that hinder the realization of practical long-lived quantum memories, explore potential strategies to overcome these obstacles, and outline the prospects for their future applications in quantum networks.
Rare-earth ion dopants in solid-state hosts are ideal candidates for quantum communication technologies, such as quantum memories, due to the intrinsic spin–photon interface of the rare-earth ion combined with the integration methods available in the solid state. Erbium-doped cerium oxide (Er:CeO2) is a particularly promising host material platform for such a quantum memory, as it combines the telecom-wavelength (∼1.5μm) 4f–4f transition of erbium, a predicted long electron spin coherence time when embedded in CeO2, and a small lattice mismatch with silicon. In this work, we report on the epitaxial growth of Er:CeO2 thin films on silicon using molecular beam epitaxy, with controlled erbium concentration between 2 and 130 parts per million (ppm). We carry out a detailed microstructural study to verify the CeO2 host structure and characterize the spin and optical properties of the embedded Er3+ ions as a function of doping density. In as-grown Er:CeO2 in the 2–3 ppm regime, we identify an EPR linewidth of 245(1) MHz, an optical inhomogeneous linewidth of 9.5(2) GHz, an optical excited state lifetime of 3.5(1) ms, and a spectral diffusion-limited homogeneous linewidth as narrow as 4.8(3) MHz. We test the annealing of Er:CeO2 films up to 900 °C, which yields narrowing of the inhomogeneous linewidth by 20% and extension of the excited state lifetime by 40%.
We obtain a low optical inhomogeneous linewidth of 25 MHz in the stoichiometric rare-earth crystal EuCl_{3}·6H_{2}O by isotopically purifying the crystal in ^{35}Cl. With this linewidth, an important limit for stoichiometric rare-earth crystals is surpassed: the hyperfine structure of ^{153}Eu is spectrally resolved, allowing the whole population of ^{153}Eu^{3+} ions to be prepared in the same hyperfine state using hole-burning techniques. This material also has a very high optical density, and can have long coherence times when deuterated. This combination of properties offers new prospects for quantum information applications. We consider two of these: quantum memories and quantum many-body studies. We detail the improvements in the performance of current memory protocols possible in these high optical depth crystals, and describe how certain memory protocols, such as off-resonant Raman memories, can be implemented for the first time in a solid-state system. We explain how the strong excitation-induced interactions observed in this material resemble those seen in Rydberg systems, and describe how these interactions can lead to quantum many-body states that could be observed using standard optical spectroscopy techniques.
Development of a Scalable Quantum Memory Platform -- Materials Science of Erbium-Doped TiO2 Thin Films on Silicon
Rare-earth ions (REI) have emerged as an attractive candidate for solid-state qubits, particularly as a quantum memory. Their 4f-4f transitions are shielded by filled 5s and 5p orbitals, offering a degree of protection from external electric fields. Embedded within a thin film oxide host, REIs could enable a qubit platform with significant memory capabilities. Furthermore, a silicon-compatible thin film form factor would enable the use of standard semiconductor fabrication processes to achieve chip-based integrability and scalability for functional quantum networks. Towards this goal, we have carried out optical and microstructural studies of erbium-doped polycrystalline and epitaxial TiO2 thin films on Si (100), r-sapphire, and SrTiO3 (100). We observe that the inhomogeneous optical linewidth of the Er photoluminescence is comparable or better for polycrystalline Er:TiO2(grown on Si) in comparison to single crystal epitaxial films on sapphire or SrTiO3, implying a relative insensitivity to extended defects. We investigated the effect of the film/substrate and film/air interface and found that the inhomogeneous linewidth and spectral diffusion can be significantly improved via bottom buffer and top capping layers of undoped TiO2. Using such approaches, we obtain inhomogeneous linewidths of 5.2 GHz and spectral diffusion of 180 MHz in Er:TiO2 /Si(100) films and have demonstrated the engineerability of quantum-relevant properties in these thin films.
Dense rare-earth spin ensembles in solids offer strong collective light-matter coupling for scalable quantum technologies but are typically incompatible with long coherence times due to strong dipolar interactions. Here we challenge this paradigm by showing long-lived coherence in such systems. In a stoichiometric EuCl_{3}·6H_{2}O crystal, we achieve hyperfine coherence times T_{2}^{CPMG} of up to 15 s at 4 K, extending the zero-field value T_{2} of 1.28 ms by more than four orders of magnitude using dynamical decoupling at a zero-first-order Zeeman (ZEFOZ) transition. Homogeneous linewidth measurements reveal a substantial suppression of resonant Eu^{3+}-Eu^{3+} spin interactions introduced by the full concentration near the ZEFOZ point. Coherence remains resilient to strong local perturbations, with a 32 ms coherence time for Eu^{3+} ions adjacent to Er^{3+} dopants. These results establish stoichiometric rare-earth crystals as a promising platform for quantum memories and spin-photon interfaces, demonstrating that intrinsically high optical depth and long-lived spin coherence can coexist in a fully concentrated ensemble.