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NTT technical review

Magnetically Purified Erbium-doped Oxide Crystal--Towards Creating a Quantum-information-manipulation Platform

Takehiko Tawara, Tomohiro Inaba

Published Oct 1, 2019• 1 citation
Publisher

Abstract

Erbium (Er) is a rare-earth element that is expected to be a platform for manipulation of quantum information by utilizing telecommunication-wavelength photons.However, high-quality epitaxial growth of Er-doped host crystals is difficult, and the memory time of quantum information, which determines the performance of quantum manipulation, is much shorter than theoretically predicted.We investigated a good-compatibility rare-earth oxide as a host crystal for Er.The host oxide crystal, cerium oxide (CeO 2 ), had its nuclear spin removed (i.e., magnetically purified).The nuclear spin is the main factor that shortens the lifetime of quantum-information retention time.In this article, we describe high-quality epitaxial growth of CeO 2 and its optical properties as a thin film grown on a silicon substrate.

DOI
10.53829/ntr201910fa3

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Erbium (Er) is a rare-earth element that is expected to be a platform for manipulation of quantum information by utilizing telecommunication-wavelength photons.However, high-quality epitaxial growth of Er-doped host crystals is difficult, and the memory time of quantum information, which determines the performance of quantum manipulation, is much shorter than theoretically predicted.We investigated a good-compatibility rare-earth oxide as a host crystal for Er.The host oxide crystal, cerium oxide (CeO 2 ), had its nuclear spin removed (i.e., magnetically purified).The nuclear spin is the main factor that shortens the lifetime of quantum-information retention time.In this article, we describe high-quality epitaxial growth of CeO 2 and its optical properties as a thin film grown on a silicon substrate.
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%.
Quantum memory is a key device for quantum repeaters that are a prerequisite for building global quantum networks. In particular for on-chip quantum memory operating at the telecommunication wavelength, Er-doped CeO2(Er:CeO2)\mathrm{CeO}_{2}\left(\mathrm{Er}: \mathrm{CeO}_{2}\right)CeO2​(Er:CeO2​) is a promising material platform, in which a long coherence time is expected. This is because the Er ions are dilutely embedded in the nuclear-spin-free CeO2matrix (crystal). Although we have prepared high-quality Er: CeO2crystals on Si substrates by molecular beam epitaxy, further improvement of their optical properties is desired. Here, we introduced a post-growth annealing process and explored the optimum annealing conditions using Bayesian optimization with a view to increasing the intensity and narrowing the optical absorption linewidth. The post-growth annealing process turned out to be effective, and the resultant improvement in the optical properties can be attributed to improved crystallinity of the host material CeO2that contributes to providing a uniform environment around the Er ions.
Robust spin-photon interfaces with optical transitions in the telecommunication band are essential for quantum networking technologies. Erbium (Er) ions are the ideal candidate with environmentally protected transitions in telecom-C band. Finding the right technologically compatible host material to enable long-lived spins remains a major hurdle. We introduce a new platform based on Er ions in cerium dioxide (CeO 2 ) as a nearly-zero nuclear spin environment (0.04%) epitaxially grown on silicon, offering silicon compatibility for opto-electrical devices. Our studies focus on Er 3+ ions and show a narrow homogeneous linewidth of 440 kHz with an optical coherence time of 0.72 μs at 3.6 K. The reduced nuclear spin noise enables a slow spin-lattice relaxation with a spin relaxation time up to 2.5 ms and an electron spin coherence time of 0.66 μs (in the isolated ion limit) at 3.6 K. These findings highlight the potential of Er 3+ :CeO 2 platform for quantum networks applications.
Coherent quantum devices play a central role in quantum science and engineering. Rare-earth ions such as erbium in solids feature numerous 4f- intra-shell transitions that are effectively shielded from their crystalline surroundings by closed outer shells, allowing for long spin coherence times and narrow optical transitions. Recent ensemble experiments have established the rare-earth doped crystals as the leading materials for optical quantum memories. However, the development of large-scale quantum devices based on rare-earth doped materials has remained a challenge. Here we describe a scalable quantum photonic platform based on epitaxially grown oxide thin films doped with trivalent ions on silicon substrates. The platform builds upon the recent developments of high quality epitaxial rare-earth doped oxides on silicon, and highlights the integration of quantum coherent materials with existing silicon technologies for ultimate device scalability. The proposed device platform builds upon our capability to epitaxially grow high quality, near-lattice-matched Y2O3 thin films on silicon. The epitaxial thin film is of high structural quality and offers several distinct advantages: (1) significantly less optical loss and better quantum emitter coherence; (2) atomic precision placement of rare-earth emitters (via delta doping) with respect to the photonic mode for controllable ion-photon coupling; (3) scalable top-down device fabrication using standard lithography and etching techniques; (4) heterogeneous integration with silicon takes full advantage of existing silicon photonics technologies for routing, tuning, and modulation of the quantum emission from rare-earth ions.
The obtention of quantum-grade rare-earth-doped oxide thin films that can be integrated with optical cavities and microwave resonators is of great interest for the development of scalable quantum devices. Among the different growth methods, chemical vapor deposition (CVD) offers high flexibility and has demonstrated the ability to produce oxide films hosting rare-earth ions with narrow linewidths. However, growing epitaxial films directly on silicon is challenging by CVD due to a native amorphous oxide layer formation at the interface. In this manuscript, we investigate the CVD growth of erbium-doped yttrium oxide (Er:Y2O3) thin films on different substrates, including silicon, sapphire, quartz, or yttria stabilized zirconia (YSZ). Alternatively, growth was also attempted on an epitaxial Y2O3 template layer on Si (111) prepared by molecular beam epitaxy (MBE) in order to circumvent the issue of the amorphous interlayer. We found that the substrate impacts the film morphology and the crystalline orientations, with different textures observed for the CVD film on the MBE-oxide/Si template (111) and epitaxial growth on YSZ (001). In terms of optical properties, Er3+ ions exhibit visible and IR emission features that are comparable for all samples, indicating a high-quality local crystalline environment regardless of the substrate. Our approach opens interesting prospects to integrate such films into scalable devices for optical quantum technologies.