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arXiv:2309.16785 · npj Quantum Information

Optical and spin coherence of Er spin qubits in epitaxial cerium dioxide on silicon

Jiefei Zhang, Gregory D. Grant, Ignas Masiulionis, Michael T. Solomon, Jonathan C. Marcks, Jasleen K. Bindra, Jens Niklas, Alan Dibos, Oleg G. Poluektov, F. Joseph Heremans, Supratik Guha, D. D. Awschalom

Published Nov 20, 2024• 19 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1038/s41534-024-00903-z

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Millisecond electron spin coherence time for erbium ions in silicon

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Spins in silicon that are accessible via a telecom-compatible optical transition are a versatile platform for quantum information processing that can leverage the well-established silicon nanofabrication industry. Key to these applications are long coherence times on the optical and spin transitions to provide a robust system for interfacing photonic and spin qubits. Here, we report telecom-compatible Er3+ sites with long optical and electron spin coherence times, measured within a nuclear spin-free silicon crystal (<0.01% 29Si) using optical detection. We investigate two sites and find 0.1 GHz optical inhomogeneous linewidths and homogeneous linewidths below 70 kHz for both sites. We measure the electron spin coherence time of both sites using optically detected magnetic resonance and observe Hahn echo decay constants of 0.8 ms and 1.2 ms at around 11 mT. These optical and spin properties of Er3+:Si are an important milestone towards using optically accessible spins in silicon for a broad range of quantum information processing applications.

arXiv:2307.10021•Jul 19, 2023•7 citations
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.
Developing telecom-compatible spin-photon interfaces is essential towards scalable quantum networks. Erbium ions (Er^{3+}) exhibit a unique combination of a telecom (1.5 μm) optical transition and an effective spin-1/2 ground state, but identifying a host that enables heterogeneous device integration while preserving long optical and spin coherence remains an open challenge. We explore the potential of Er^{3+}:CeO_{2} films on silicon and study the Er^{3+} spin coherence, offering low nuclear spin density and the potential for on-chip integration. We demonstrate a 38.8 μs spin coherence, which can be extended to 176.4 μs with dynamical decoupling. Pairing experiments with cluster correlation expansion calculations, we identify spectral diffusion induced by bath Er^{3+} spin flip-flops as the dominant decoherence mechanism and provide pathways to millisecond-scale coherence.
Clock-transition-enabled long electron spin coherence of telecom emitters in CeO2_22​
Rare-earth-ion-doped crystals has emerged as a promising platform for quantum technologies, owing to their narrow telecom-band optical emission, long spin memory, and compatibility with silicon integrated photonic architectures. However, the realization of scalable quantum devices requires host materials with intrinsically dilute spin environments to suppress decoherence. In this context, erbium (Er3+^{3+}3+) doped cerium oxide (CeO2_22​) is an attractive candidate due to the ultra-low concentration of nuclear spins in the host matrix and its compatibility with silicon-based technologies. Here we perform a comprehensive investigation of the coherence properties of Er3+^{3+}3+ electron spin qubit in CeO2_22​ via semiclassical as well as detailed cluster correlation expansion simulations. By systematically exploring magnetic field strength, pulse sequences, erbium concentration, and spin temperature, we identify regimes where decoherence from the spin bath is strongly suppressed. Our investigations illustrate that at dilute doping concentration (of the order of 10 ppb) and sub-Kelvin temperatures, operation near clock transitions enables Hahn-echo coherence times to approach the second timescale even at natural isotopic abundance. Importantly, from a practical standpoint, coherence times on the order of ∼10\sim 10∼10 ms are expected even at liquid helium temperature (about 2 K) for similar concentrations. Moreover, we demonstrate that an additional enhancement can be obtained with conventional multi-πππ-pulse dynamical decoupling protocols. Thus, our findings establish Er3+^{3+}3+ doped CeO2_22​ as a front-runner for realizing spin qubits, quantum memories, and integrated quantum networks.
Spin decoherence dynamics of Er3+^{3+}3+ in CeO2_22​ film
Developing telecom-compatible spin-photon interfaces is essential towards scalable quantum networks. Erbium ions (Er3+^{3+}3+) exhibit a unique combination of a telecom (1.5 μμμm) optical transition and an effective spin-1/21/21/2 ground state, but identifying a host that enables heterogeneous device integration while preserving long optical and spin coherence remains an open challenge. We explore a new platform of Er3+^{3+}3+:CeO2_22​ films on silicon, offering low nuclear spin density and the potential for on-chip integration. We demonstrate a 38.8 μμμs spin coherence, which can be extended to 176.4\nobreakspace μμμs with dynamical decoupling. Pairing experiments with cluster correlation expansion calculations, we identify spectral diffusion-induced Er3+^{3+}3+ spin flips as the dominant decoherence mechanism and provide pathways to millisecond-scale coherence.
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%.
Spins in silicon that are accessible via a telecom-compatible optical transition are a versatile platform for quantum information processing that can leverage the well-established silicon nanofabrication industry. Key to these applications are long coherence times on the optical and spin transitions to provide a robust system for interfacing photonic and spin qubits. Here, we report telecom-compatible Er 3+ sites with long optical and electron spin coherence times, measured within a nuclear spin-free silicon crystal (<0.01 % 29 Si) using optical detection. We investigate two sites and find 0.1 GHz optical inhomogeneous linewidths and homogeneous linewidths below 70 kHz for both sites. We measure the electron spin coherence time of both sites using optically detected magnetic resonance and observe Hahn echo decay constants of 0.8 ms and 1.2 ms at ~ 11 mT. These optical and spin properties of Er 3+ :Si are an important milestone towards using optically accessible spins in silicon for a broad range of quantum information processing applications.
Spins in silicon that are accessible via a telecom-compatible optical transition are a versatile platform for quantum information processing that can leverage the well-established silicon nanofabrication industry. Key to these applications are long coherence times on the optical and spin transitions to provide a robust system for interfacing photonic and spin qubits. Here, we report telecom-compatible Er3+ sites with long optical and electron spin coherence times, measured within a nuclear spin-free silicon crystal (<0.01% 29Si) using optical detection. We investigate two sites and find 0.1 GHz optical inhomogeneous linewidths and homogeneous linewidths below 70 kHz for both sites. We measure the electron spin coherence time of both sites using optically detected magnetic resonance and observe Hahn echo decay constants of 0.8 ms and 1.2 ms at around 11 mT. These optical and spin properties of Er3+:Si are an important milestone towards using optically accessible spins in silicon for a broad range of quantum information processing applications.