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Physical review. B./Physical review. B

Optical coherence and spin population dynamics in Yb3+171 : Y2SiO5 single crystals

F. Chiossi, Eloïse Lafitte-Houssat, Alban Ferrier, Sacha Welinski, Loïc Morvan, Perrine Berger, Diana Serrano, Mikael Afzelius, Philippe Goldner

Published Mar 22, 2024• 8 citations
Publisher

Abstract

Rare earth doped crystals are a promising platform for long-distance quantum communications, where they can perform quantum light storage. Among different systems, ${}^{171}$Yb${}^{3+}$-doped Y${}_{2}$SiO${}_{5}$ (YSO) crystals stand out because of long optical and spin coherence times, and large hyperfine splitting, enabling long-time storage over large bandwidths. Here, the authors study the mechanisms affecting the optical decoherence in a broad range of temperatures (40 mK to 18 K) using high-resolution spectroscopic techniques, and identify ways to further improve the crystal's properties.

DOI
10.1103/physrevb.109.094114

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Optical coherence and spin population dynamics in $^{171}$Yb$^{3+}$:Y$_2$SiO$_5$ single crystals

F. Chiossi, Eloïse Lafitte-Houssat, Alban Ferrier +6 more

$^{171}$Yb$^{3+}$-doped Y$_2$SiO$_5$ crystals are a promising platform for optical quantum memories in long-distance quantum communications. The relevance of this material lies in $^{171}$Yb 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 $^{89}$Yb 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 $^{171}$Yb concentration.

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Optical investigation of ultra-slow spin relaxation in 171 Yb 3+ :Y 2 SiO 5 single crystals

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Abstract We report a detailed investigation of spin relaxation dynamics in the rare-earth-doped crystal 171 Yb:Y 2 SiO 5 , a promising platform for quantum memory based on atomic frequency combs. The population dynamics among the four ground-state hyperfine levels were studied in the 50 mK–6 K temperature range by optically modifying the spin populations and monitoring their return to thermal equilibrium via absorption spectroscopy. Below 1 K, population rethermalization occurs on timescales of several hours and is governed by direct spin-phonon relaxation. In contrast, the lifetime of individual spin states is strongly reduced by spin-spin interactions, ranging from seconds in low-doped (2 ppm) samples to milliseconds at higher doping (10 ppm). These results provide clear guidelines for optimizing doping concentration and operating temperature, indicating that atomic frequency comb lifetimes on the order of one hour are achievable in 171 Yb:Y 2 SiO 5 crystals with Yb concentrations not much lower than 2 ppm and at temperatures at or below 1 K.

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Coherent spin dynamics of ytterbium ions in yttrium orthosilicate

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Rare-earth spins in optical crystals like yttrium orthosilicate (YSO) are of much interest for providing coherent interfaces with both microwave and optical photons. Here, the authors study the spin dynamics of a new system, Yb in YSO, which has favorable optical properties and strong hyperfine coupling to the ${}^{171}$Yb (spin-1/2) and ${}^{173}$Yb (spin-5/2) isotopes. The results demonstrate long coherence times for both the electron and nuclear spins (~1 ms). Employing a range of pulsed electron spin resonance measurements as well as comparison with relevant theory, the study elucidates a number of spin relaxation and decoherence mechanisms at work.

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Spectroscopic study of hyperfine properties in Yb3+171:Y2SiO5

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Rare-earth ion-doped crystals are promising systems for quantum communication and quantum information processing. In particular, paramagnetic rare-earth centers can be utilized to realize quantum coherent interfaces simultaneously for optical and microwave photons. In this paper, we study hyperfine and magnetic properties of a ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ crystal doped with $^{171}\mathrm{Yb}^{3+}$ ions. This isotope is particularly interesting since it is the only rare--earth ion having electronic spin $S=\frac{1}{2}$ and nuclear spin $I=\frac{1}{2}$, which results in the simplest possible hyperfine level structure. In this work, we determine the hyperfine tensors for the ground and excited states on the optical $^{2}\mathrm{F}_{7/2}(0)\ensuremath{\longleftrightarrow}^{2}\mathrm{F}_{5/2}(0)$ transition by combining spectral hole burning and optically detected magnetic resonance techniques. The resulting spin Hamiltonians correctly predict the magnetic-field dependence of all observed optical-hyperfine transitions, from zero applied field up to fields where the Zeeman interaction is dominating the hyperfine interaction. Using the optical absorption spectrum, we can also determine the order of the hyperfine levels in both states. These results pave the way for realizing solid-state optical and microwave quantum memories based on a $^{171}\mathrm{Yb}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ crystal.

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High-resolution optical spectroscopy and magnetic properties of Yb 3 + in Y 2 SiO 5

Sacha Welinski, Alban Ferrier, Mikael Afzelius +1 more

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. ${\mathrm{Yb}}^{3+}$ is particularly interesting in this respect since it is the only paramagnetic rare earth with a spin-$\frac{1}{2}$ isotope, which corresponds to the simplest possible level structure. In this paper, we report on the optical and magnetic properties of ${\mathrm{Yb}}^{3+}$ in the two sites of ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$, 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 $^{171}\mathrm{Yb}^{3+}$ ($I=\frac{1}{2}$) isotope. These results suggest that ${\mathrm{Yb}}^{3+}$:${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ is a promising material for applications like solid-state optical and microwave quantum memories.

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Investigation of the Electronic Structure and Optical, EPR, and ODMR Spectroscopic Properties for 171Yb3+-Doped Y2SiO5 Crystal: A Combined Theoretical Approach

Xiaonan Zhou, Hong-Gang Liu, Z. Y. He +2 more

Various spectroscopic properties of Yb 3+ -doped Y 2 SiO 5 crystal have been extensively investigated due to its promising application in quantum information processing. However, the local structure, electronic structure of Yb 3+:Y 2 SiO 5 crystal, and its optical and magnetic properties have not been comprehensively studied from a theoretical viewpoint. In this work, the geometric and electronic structures of Yb 3+ that replaces two crystallographic Y 3+ sites in the Y 2 SiO 5 crystal are first obtained by the method of density functional theory (DFT). Then, the optical, electron paramagnetic resonance (EPR), and optically detected magnetic resonance (ODMR) spectra for 171 Yb 3+ (nuclear spin I = 1/2) at such two sites are simultaneously calculated in the framework of the complete diagonalization (of energy) matrix (CDM) based on the optimized local structure around 171 Yb 3+ ion by DFT. The various calculated spectroscopic properties by such combined theoretical approach are consistent with the experimental ones, which demonstrates that CDM is effective and particularly suitable for calculating hyperfine A -tensors under zero, low, and intermediate magnetic field. More importantly, based on the obtained accurate hyperfine structure of 171 Yb 3+ in Y 2 SiO 5 crystal, the possible “clock transitions”, which can enhance the optical coherence time, can be assigned or predicted by the present approach. This study successfully explains the spectroscopic properties of 171 Yb 3+ -doped Y 2 SiO 5 and provides a feasible method to design and search for practical rare-earth-doped quantum information materials for the community.

Inorganic Chemistry•Aug 31, 2020•23 citations
Rare earth doped crystals are a promising platform for long-distance quantum communications, where they can perform quantum light storage. Among different systems, 171{}^{171}171Yb3+{}^{3+}3+-doped Y2{}_{2}2​SiO5{}_{5}5​ (YSO) crystals stand out because of long optical and spin coherence times, and large hyperfine splitting, enabling long-time storage over large bandwidths. Here, the authors study the mechanisms affecting the optical decoherence in a broad range of temperatures (40 mK to 18 K) using high-resolution spectroscopic techniques, and identify ways to further improve the crystal's properties.
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.
Abstract We report a detailed investigation of spin relaxation dynamics in the rare-earth-doped crystal 171 Yb:Y 2 SiO 5 , a promising platform for quantum memory based on atomic frequency combs. The population dynamics among the four ground-state hyperfine levels were studied in the 50 mK–6 K temperature range by optically modifying the spin populations and monitoring their return to thermal equilibrium via absorption spectroscopy. Below 1 K, population rethermalization occurs on timescales of several hours and is governed by direct spin-phonon relaxation. In contrast, the lifetime of individual spin states is strongly reduced by spin-spin interactions, ranging from seconds in low-doped (2 ppm) samples to milliseconds at higher doping (10 ppm). These results provide clear guidelines for optimizing doping concentration and operating temperature, indicating that atomic frequency comb lifetimes on the order of one hour are achievable in 171 Yb:Y 2 SiO 5 crystals with Yb concentrations not much lower than 2 ppm and at temperatures at or below 1 K.
Rare-earth spins in optical crystals like yttrium orthosilicate (YSO) are of much interest for providing coherent interfaces with both microwave and optical photons. Here, the authors study the spin dynamics of a new system, Yb in YSO, which has favorable optical properties and strong hyperfine coupling to the 171{}^{171}171Yb (spin-1/2) and 173{}^{173}173Yb (spin-5/2) isotopes. The results demonstrate long coherence times for both the electron and nuclear spins (~1 ms). Employing a range of pulsed electron spin resonance measurements as well as comparison with relevant theory, the study elucidates a number of spin relaxation and decoherence mechanisms at work.
Rare-earth ion-doped crystals are promising systems for quantum communication and quantum information processing. In particular, paramagnetic rare-earth centers can be utilized to realize quantum coherent interfaces simultaneously for optical and microwave photons. In this paper, we study hyperfine and magnetic properties of a Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ crystal doped with 171Yb3+^{171}\mathrm{Yb}^{3+}171Yb3+ ions. This isotope is particularly interesting since it is the only rare--earth ion having electronic spin S=12S=\frac{1}{2}S=21​ and nuclear spin I=12I=\frac{1}{2}I=21​, which results in the simplest possible hyperfine level structure. In this work, we determine the hyperfine tensors for the ground and excited states on the optical $^{2}\mathrm{F}_{7/2}(0)\ensuremath{\longleftrightarrow}^{2}\mathrm{F}_{5/2}(0)$ transition by combining spectral hole burning and optically detected magnetic resonance techniques. The resulting spin Hamiltonians correctly predict the magnetic-field dependence of all observed optical-hyperfine transitions, from zero applied field up to fields where the Zeeman interaction is dominating the hyperfine interaction. Using the optical absorption spectrum, we can also determine the order of the hyperfine levels in both states. These results pave the way for realizing solid-state optical and microwave quantum memories based on a 171Yb3+:Y2SiO5^{171}\mathrm{Yb}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}171Yb3+:Y2​SiO5​ crystal.
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.
Various spectroscopic properties of Yb 3+ -doped Y 2 SiO 5 crystal have been extensively investigated due to its promising application in quantum information processing. However, the local structure, electronic structure of Yb 3+:Y 2 SiO 5 crystal, and its optical and magnetic properties have not been comprehensively studied from a theoretical viewpoint. In this work, the geometric and electronic structures of Yb 3+ that replaces two crystallographic Y 3+ sites in the Y 2 SiO 5 crystal are first obtained by the method of density functional theory (DFT). Then, the optical, electron paramagnetic resonance (EPR), and optically detected magnetic resonance (ODMR) spectra for 171 Yb 3+ (nuclear spin I = 1/2) at such two sites are simultaneously calculated in the framework of the complete diagonalization (of energy) matrix (CDM) based on the optimized local structure around 171 Yb 3+ ion by DFT. The various calculated spectroscopic properties by such combined theoretical approach are consistent with the experimental ones, which demonstrates that CDM is effective and particularly suitable for calculating hyperfine A -tensors under zero, low, and intermediate magnetic field. More importantly, based on the obtained accurate hyperfine structure of 171 Yb 3+ in Y 2 SiO 5 crystal, the possible “clock transitions”, which can enhance the optical coherence time, can be assigned or predicted by the present approach. This study successfully explains the spectroscopic properties of 171 Yb 3+ -doped Y 2 SiO 5 and provides a feasible method to design and search for practical rare-earth-doped quantum information materials for the community.