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arXiv:1709.01959 · Physical Review Letters

Selective Optical Addressing of Nuclear Spins through Superhyperfine Interaction in Rare-Earth Doped Solids

B. Car, Lucile Veissier, Anne Louchet-Chauvet, J.-L. Le Gouët, T. Chanelière

Published May 10, 2018• 36 citations
arXivHTMLPDF

Abstract

In Er^{3+}:Y_{2}SiO_{5}, we demonstrate the selective optical addressing of the ^{89}Y^{3+} nuclear spins through their superhyperfine coupling with the Er^{3+} electronic spins possessing large Landé g factors. We experimentally probe the electron-nuclear spin mixing with photon echo techniques and validate our model. The site-selective optical addressing of the Y^{3+} nuclear spins is designed by adjusting the magnetic field strength and orientation. This constitutes an important step towards the realization of long-lived solid-state qubits optically addressed by telecom photons.

DOI
10.1103/physrevlett.120.197401

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In Er^{3+}:Y_{2}SiO_{5}, we demonstrate the selective optical addressing of the ^{89}Y^{3+} nuclear spins through their superhyperfine coupling with the Er^{3+} electronic spins possessing large Landé g factors. We experimentally probe the electron-nuclear spin mixing with photon echo techniques and validate our model. The site-selective optical addressing of the Y^{3+} nuclear spins is designed by adjusting the magnetic field strength and orientation. This constitutes an important step towards the realization of long-lived solid-state qubits optically addressed by telecom photons.
Individually addressed Er 3+ ions in solid-state hosts are promising resources for quantum repeaters, because of their direct emission in the telecom band and their compatibility with silicon photonic devices.While the Er 3+ electron spin provides a spin-photon interface, ancilla nuclear spins could enable multiqubit registers with longer storage times.In this work, we demonstrate coherent coupling between the electron spin of a single Er 3+ ion and a single I = 1/2 nuclear spin in the solid-state host crystal, which is a fortuitously located proton ( 1 H).We control the nuclear spin using dynamical-decoupling sequences applied to the electron spin, implementing one-and two-qubit gate operations.Crucially, the nuclear spin coherence time exceeds the electron coherence time by several orders of magnitude, because of its smaller magnetic moment.These results provide a path toward combining long-lived nuclear spin quantum registers with telecom-wavelength emitters for long-distance quantum repeaters.
Echo-based spectroscopy of the superhyperfine interaction of an electronic spin with nuclear spins in its surroundings enables detailed insights into the microscopic magnetic environment of spins in solids. Still, it is an outstanding challenge to resolve individual nuclear spins in a dense bath, in which many of them exhibit a comparable coupling strength. This simultaneously requires a high spectral resolution and a large signal-to-noise ratio. However, when probing spin ensembles, dipolar interactions between the dopants can lead to a concentration-dependent trade-off between resolution and signal. Here, we fully eliminate this limitation of previous optical-echo-envelope-modulation spectroscopy experiments by integrating the emitters into a high-finesse resonator, which allows for strong optical echoes even at very low concentrations. To demonstrate its potential, the technique is applied to erbium dopants in yttrium orthosilicate ( Er : YSO ). Achieving an unprecedented spectral resolution enables precise measurements of the superhyperfine interaction with four of the Y nuclear spins densely surrounding each emitter. The achieved boost of the signal, enabled by the resonator, allows for extending the approach to the lowest concentration possible—to the level of single dopants, thereby providing a tool for detecting and studying individual nuclear spins. Thus, our technique paves the way for an improved understanding of dense nuclear-spin baths in solids.
Solid-state impurity spins with optical control are currently investigated for quantum networks and repeaters. Among these, rare-earth-ion doped crystals are promising as quantum memories for light, with potentially long storage time, high multimode capacity, and high bandwidth. However, with spins there is often a tradeoff between bandwidth, which favors electronic spin, and memory time, which favors nuclear spins. Here, we present optical storage experiments using highly hybridized electron-nuclear hyperfine states in ^{171}Yb^{3+}:Y_{2}SiO_{5}, where the hybridization can potentially offer both long storage time and high bandwidth. We reach a storage time of 1.2 ms and an optical storage bandwidth of 10 MHz that is currently only limited by the Rabi frequency of the optical control pulses. The memory efficiency in this proof-of-principle demonstration was about 3%. The experiment constitutes the first optical storage using spin states in any rare-earth ion with electronic spin. These results pave the way for rare-earth based quantum memories with high bandwidth, long storage time, and high multimode capacity, a key resource for quantum repeaters.
Abstract Nanoscale systems that coherently couple to light and possess spins offer key capabilities for quantum technologies. However, an outstanding challenge is to preserve properties, and especially optical and spin coherence lifetimes, at the nanoscale. Here, we report optically controlled nuclear spins with long coherence lifetimes ( T 2 ) in rare-earth-doped nanoparticles. We detect spins echoes and measure a spin coherence lifetime of 2.9 ± 0.3 ms at 5 K under an external magnetic field of 9 mT, a T 2 value comparable to those obtained in bulk rare-earth crystals. Moreover, we achieve spin T 2 extension using all-optical spin dynamical decoupling and observe high fidelity between excitation and echo phases. Rare-earth-doped nanoparticles are thus the only nano-material in which optically controlled spins with millisecond coherence lifetimes have been reported. These results open the way to providing quantum light-atom-spin interfaces with long storage time within hybrid architectures.
Abstract Nanoscale systems that coherently couple to light and possess spins offer key capabilities for quantum technologies. However, an outstanding challenge is to preserve properties, and especially optical and spin coherence lifetimes, at the nanoscale. Here, we report optically controlled nuclear spins with long coherence lifetimes (T2) in rare-earth-doped nanoparticles. We detect spins echoes and measure a spin coherence lifetime of 2.9 ± 0.3 ms at 5 K under an external magnetic field of 9 mT, a T2 value comparable to those obtained in bulk rare-earth crystals. Moreover, we achieve spin T2 extension using all-optical spin dynamical decoupling and observe high fidelity between excitation and echo phases. Rare-earth-doped nanoparticles are thus the only nano-material in which optically controlled spins with millisecond coherence lifetimes have been reported. These results open the way to providing quantum light-atom-spin interfaces with long storage time within hybrid architectures.
Rare-earth related electron spins in crystalline hosts are unique material systems, as they can potentially provide a direct interface between telecom band photons and long-lived spin quantum bits. Specifically, their optically accessible electron spins in solids interacting with nuclear spins in their environment are valuable quantum memory resources. Detection of nearby individual nuclear spins, so far exclusively shown for few dilute nuclear spin bath host systems such as the nitrogen-vacancy center in diamond or the silicon vacancy in silicon carbide, remained an open challenge for rare earths in their host materials, which typically exhibit dense nuclear spin baths. Here, we present the electron spin spectroscopy of single Ce^{3+} ions in a yttrium orthosilicate host, featuring a coherence time of T_{2}=124 μs. This coherent interaction time is sufficiently long to isolate proximal ^{89}Y nuclear spins from the nuclear spin bath of ^{89}Y. Furthermore, it allows for the detection of a single nearby ^{29}Si nuclear spin, native to the host material with ∼5% abundance. This study opens the door to quantum memory applications in rare-earth ion related systems based on coupled environmental nuclear spins, potentially useful for quantum error correction schemes.