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Optical Materials X

Optical and spin inhomogeneous linewidths in 171Yb 3 + :Y 2 SiO5

Eloïse Lafitte-Houssat, Alban Ferrier, Sacha Welinski, Loïc Morvan, Mikael Afzelius, Perrine Berger, Philippe Goldner

Published Apr 27, 2022• 4 citations
Publisher

Abstract

Single crystals of 171Yb3+:Y2SiO5 are promising systems for quantum technologies as an efficient optical to spin interface. This is due to the long optical and spin coherence lifetimes, or narrow homogeneous linewidths, observed in this material at zero magnetic field. Inhomogeneous linewidths are also of importance since they affect peak absorption, available bandwidth or spin–spin interactions. In this work, we investigate inhomogeneous linewidths in a series of 171Yb3+:Y2SiO5 single crystals grown by the Czochralski method with the purpose of identifying the broadening mechanisms in the regime of ultra-low doping, i.e. in the ppm range. In a series of samples obtained with varying doping level, growth atmosphere, and cut at different locations in a crystal boule, optical inhomogeneous linewidths between 0.6 and 1.3 GHz are observed. This study suggests that these variations are due to changes in dislocation densities. Spin inhomogeneous linewidths, recorded using electron paramagnetic resonance, did not show the differences between samples observed in the optical domain. They were otherwise found to vary as a function of magnetic field orientation, enabling determination of directions that minimize e.g. detrimental spin–spin interactions. These results suggest ways to reduce optical inhomogeneous linewidths in 171Yb3+:Y2SiO5, which is of interest for high efficiency quantum memories and optical to microwave quantum transducers.

DOI
10.1016/j.omx.2022.100153

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Однородные и неоднородные ширины линий в оптических спектрах кристалла Y-=SUB=-2-=/SUB=-SiO-=SUB=-5-=/SUB=- : -=SUP=-171-=/SUP=-Yb-=SUP=-3+-=/SUP=-

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Abstract The coherent interaction of solid-state spins with both optical and microwave fields provides a platform for a range of quantum technologies, such as quantum sensing, microwave-to-optical quantum transduction and optical quantum memories. Rare-earth ions with electronic spins are interesting in this context. In this work, we use a loop-gap microwave resonator to coherently drive optical and microwave clock transitions simultaneously in a 171 Yb 3+ :Y 2 SiO 5 crystal, achieving a Rabi frequency of 0.56 MHz at 2.497 GHz over a 1-cm long crystal. Furthermore, we provide insights into the spin dephasing at very low fields, showing that superhyperfine-induced collapse of the Hahn echo plays an important role. Our calculations and measurements reveal that the effective magnetic moment can be manipulated in 171 Yb 3+ :Y 2 SiO 5 , which suppresses the superhyperfine interaction at the clock transition. At a doping concentration of 2 ppm and 3.4 K, we achieve spin coherence time of 10.0 ± 0.4 ms.

arXiv:2209.04196•npj Quantum Information•Mar 2, 2023•18 citations
Single crystals of 171Yb3+:Y2SiO5 are promising systems for quantum technologies as an efficient optical to spin interface. This is due to the long optical and spin coherence lifetimes, or narrow homogeneous linewidths, observed in this material at zero magnetic field. Inhomogeneous linewidths are also of importance since they affect peak absorption, available bandwidth or spin–spin interactions. In this work, we investigate inhomogeneous linewidths in a series of 171Yb3+:Y2SiO5 single crystals grown by the Czochralski method with the purpose of identifying the broadening mechanisms in the regime of ultra-low doping, i.e. in the ppm range. In a series of samples obtained with varying doping level, growth atmosphere, and cut at different locations in a crystal boule, optical inhomogeneous linewidths between 0.6 and 1.3 GHz are observed. This study suggests that these variations are due to changes in dislocation densities. Spin inhomogeneous linewidths, recorded using electron paramagnetic resonance, did not show the differences between samples observed in the optical domain. They were otherwise found to vary as a function of magnetic field orientation, enabling determination of directions that minimize e.g. detrimental spin–spin interactions. These results suggest ways to reduce optical inhomogeneous linewidths in 171Yb3+:Y2SiO5, which is of interest for high efficiency quantum memories and optical to microwave quantum transducers.
Rare earth ions are actively investigated as optically addressable spin systems for quantum technologies thanks to their long optical and spin coherence lifetimes. 171Yb3+, which has 1/2 electron and nuclear spins, recently raised interest for its simple hyperfine structure that moreover can result in long coherence lifetimes at zero magnetic field, an unusual property for paramagnetic rare earth ions. Here, we report on the optical inhomogeneous and homogeneous linewidths in 171Yb3+:Y2SiO5 (site 2) for different doping concentrations. While inhomogeneous linewidth is not correlated to 171Yb3+ concentration, the homogeneous one strongly decreases between 10 and 2 ppm doping level, reaching 255 Hz at 3 K. This is attributed to a slowing down of 171Yb3+ ground state spin flip-flops.
The transportable quantum memory is a feasible solution for realizing the long-distance quantum communication, which requires a storage lifetime of the order of hours. The isotope-enriched 151Eu3+:Y2SiO5 crystal is a promising candidate for this application. However, its optical storage efficiency and spin storage lifetime are limited by the wide inhomogeneous linewidth. In this work, we successfully grow isotope-enriched 151Eu3+:Y2SiO5 crystals with varying doping concentrations by utilizing the Czochralski method. The optical inhomogeneous broadening and spin inhomogeneous broadening are measured by the optical absorption spectroscopy and optically detected magnetic resonance tests, respectively. Notably, in the undoped samples, we identify a baseline level of inhomogeneous linewidths, happening at (390 ± 15) MHz for optical inhomogeneous broadening and (4.6 ± 0.2) kHz for spin inhomogeneous broadening. Our findings reveal that the point defects, induced by the doping ions, significantly contribute to the inhomogeneous broadening. For every increase of 10–6 in doping concentration, the optical inhomogeneous broadening increases by 0.97 MHz, and the spin inhomogeneous broadening increases by 0.014 kHz. Furthermore, we discuss the influence of dislocations on inhomogeneous broadening and propose potential strategies to further mitigate these effects. These advancements are expected to promote the development of ultra-long-lifetime transportable quantum memory applications.
Optical coherence and spin population dynamics in 171^{171}171Yb3+^{3+}3+:Y2_22​SiO5_55​ single crystals
171^{171}171Yb3+^{3+}3+-doped Y2_22​SiO5_55​ crystals are a promising platform for optical quantum memories in long-distance quantum communications. The relevance of this material lies in 171^{171}171Yb long optical and spin coherence times, along with a large hyperfine splitting, enabling long quantum storage over large bandwidths. Mechanisms affecting the optical decoherence are however not precisely known, especially since low-temperature measurements have so far focused on the 2 to 4 K range. In this work, we performed two- and three-pulse photon echoes and spectral hole burning to determine optical homogeneous linewidths in two 171 Yb:YSO crystals doped at 2 and 10 ppm. Experiments were performed in the 40 mK to 18 K temperature range, leading to linewidths between 320 Hz, among the narrowest reported for rare-earth ions, and several MHz. Our results show that above 6 K the homogeneous linewidth is mainly due to an elastic two-phonon process which results in a slow broadening with temperature, the homogeneous linewidth reaching only 25 kHz at 10 K. At lower temperatures, interactions with 89^{89}89Yb nuclear spin-flips, paramagnetic defects or impurities, and also Yb-Yb interactions for the higher concentrated crystal, are likely the main limiting factor to the homogeneous linewidth. In particular, we conclude that the direct effect of spin and optical excited state lifetime is a minor contribution to optical decoherence in the whole temperature range studied. Our results indicate possible paths and regimes for further decreasing the homogeneous linewidths or maintaining narrow lines at higher 171^{171}171Yb concentration.
Rare earth ions are actively investigated as optically addressable spin systems for quantum technologies thanks to their long optical and spin coherence lifetimes. 171Yb3+, which has 1/2 electron and nuclear spins, recently raised interest for its simple hyperfine structure that moreover can result in long coherence lifetimes at zero magnetic field, an unusual property for paramagnetic rare earth ions. Here, we report on the optical inhomogeneous and homogeneous linewidths in 171Yb3+:Y2SiO5 (site 2) for different doping concentrations. While inhomogeneous linewidth is not correlated to 171Yb3+ concentration, the homogeneous one strongly decreases between 10 and 2 ppm doping level, reaching 255 Hz at 3 K. This is attributed to a slowing down of 171Yb3+ ground state spin flip-flops.
Rare-earth doped crystals are promising systems for quantum information processing. In particular, paramagnetic rare earths could be used to build coherent interfaces with optical and microwave photons. In addition, isotopes with nonzero nuclear spins could provide long-lived states for quantum state storage and processing. Yb3+{\mathrm{Yb}}^{3+}Yb3+ is particularly interesting in this respect since it is the only paramagnetic rare earth with a spin-12\frac{1}{2}21​ isotope, which corresponds to the simplest possible level structure. In this paper, we report on the optical and magnetic properties of Yb3+{\mathrm{Yb}}^{3+}Yb3+ in the two sites of Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​, a commonly used crystal for quantum applications. We measured optical inhomogeneous linewidths, peak absorption coefficients, oscillator strengths, and excited-state lifetimes. The Zeeman tensors were also determined in the ground and excited states, as well as the ground-state hyperfine tensor for the 171Yb3+^{171}\mathrm{Yb}^{3+}171Yb3+ (I=12I=\frac{1}{2}I=21​) isotope. These results suggest that Yb3+{\mathrm{Yb}}^{3+}Yb3+:Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ is a promising material for applications like solid-state optical and microwave quantum memories.
Abstract The coherent interaction of solid-state spins with both optical and microwave fields provides a platform for a range of quantum technologies, such as quantum sensing, microwave-to-optical quantum transduction and optical quantum memories. Rare-earth ions with electronic spins are interesting in this context. In this work, we use a loop-gap microwave resonator to coherently drive optical and microwave clock transitions simultaneously in a 171 Yb 3+ :Y 2 SiO 5 crystal, achieving a Rabi frequency of 0.56 MHz at 2.497 GHz over a 1-cm long crystal. Furthermore, we provide insights into the spin dephasing at very low fields, showing that superhyperfine-induced collapse of the Hahn echo plays an important role. Our calculations and measurements reveal that the effective magnetic moment can be manipulated in 171 Yb 3+ :Y 2 SiO 5 , which suppresses the superhyperfine interaction at the clock transition. At a doping concentration of 2 ppm and 3.4 K, we achieve spin coherence time of 10.0 ± 0.4 ms.