Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Log inSign up
Challenges
Datasets
Workspaces
Papers
Discussions
Leaderboard
Blog
Job Board
Q3AS

© 2026 Aqora Quantum S.A.S.

TermsPrivacyLegal Notice

Physical Review Letters

Optical Measurement of the Effect of Electric Fields on the Nuclear Spin Coherence of Rare-Earth Ions in Solids

R. M. Macfarlane, Andrea Arcangeli, Alban Ferrier, Philippe Goldner

Published Oct 7, 2014• 25 citations
Publisher

Abstract

We show that the coherence properties of the nuclear spin states of rare-earth ions in solids can be manipulated by small applied electric fields. This was done by measuring the Stark effect on the nuclear quadrupole transitions of $^{151}\mathrm{Eu}$ in ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ (YSO) using a combination of Raman heterodyne optical detection and Stark modulated quadrupole echoes to achieve high sensitivity. The measured Stark coefficients were 0.42 and $1.0\text{ }\text{ }\mathrm{Hz}\text{ }\mathrm{cm}/\mathrm{V}$ for the two quadrupole transitions at 34.54 and 46.20 MHz, respectively. The long decoherence time of the nuclear spin states (25 ms) allowed us to make the measurements in very low electric fields of $\ensuremath{\sim}10\text{ }\text{ }\mathrm{V}/\mathrm{cm}$, which produced 100% modulation of the nuclear spin echo, and to measure Stark shifts of $\ensuremath{\sim}1\text{ }\text{ }\mathrm{Hz}$ or 20 ppm of the inhomogeneous linewidth.

DOI
10.1103/physrevlett.113.157603

Related papers

Nuclear spin coherence properties of 151 Eu 3+ and 153 Eu 3+ in a Y 2 O 3 transparent ceramic

Jenny Karlsson, Nathalie Kunkel, Akio Ikesue +2 more

Abstract We have measured inhomogeneous linewidths and coherence times ( T 2 ) of nuclear spin transitions in a Eu 3+ :Y 2 O 3 transparent ceramic by an all-optical spin echo technique. The nuclear spin echo decay curves showed a strong modulation which was attributed to interaction with Y nuclei in the host. The coherence time of the 29 MHz spin transition in 151 Eu 3+ was 16 ms in a small applied magnetic field. Temperature dependent measurements showed that the coherence time was constant up to 18 K and was limited by spin-lattice relaxation for higher temperatures. Nuclear spin echoes in 153 Eu 3+ gave much weaker signals than for the case of 151 Eu 3+ . The spin coherence time for the 73 MHz spin transition in 153 Eu 3+ was estimated to 14 ms in a small magnetic field. The study shows that the spin transitions of ceramic Eu 3+ :Y 2 O 3 have coherence properties comparable to the best rare-earth-doped materials available.

Journal of Physics Condensed Matter•Feb 8, 2017•19 citations

Precision measurements of electric-field-induced frequency displacements of an ultranarrow optical transition in ions in a solid

S. Zhang, Nemanja Lučić, Nicolas Galland +5 more

We report a series of measurements of the effect of an electric field on the frequency of the ultranarrow linewidth F70→ D50 optical transition of Eu3+ ions in an Y2SiO5 matrix at cryogenic temperatures. We provide linear Stark coefficients along two dielectric axes and for the two different substitution sites of the Eu3+ ions, with an unprecedented accuracy and an upper limit for the quadratic Stark shift. The measurements, which indicate that the electric field sensitivity is a factor of seven larger for site 1 relative to site 2 for a particular direction of the electric field, are of direct interest in the context of both quantum information processing and laser frequency stabilization with rare-earth doped crystals, in which electric fields can be used to engineer experimental protocols by tuning transition frequencies.

arXiv:2101.10169•Applied Physics Letters•Nov 30, 2020•10 citations

Spectroscopic study of rare earth ions in antiferromagnets

Masaya Hiraishi

Microwave and optical transitions of rare-earth ions enable microwave-to-optical frequency transduction. This transduction is a coherent process; therefore, the narrow linewidths and long coherence times of rare-earth ions are crucial for achieving efficient frequency conversion. Particularly long coherence times can be achieved with small-spin materials, as unpaired electronic and nuclear spins introduce magnetic noise, serving as a decoherent source of the transitions. However, complete spin-free rare-earth materials cannot exist without charge compensation. Consequently, residual spins in existing rare-earth materials act as a bottleneck, limiting both their spin and optical coherence times. Rather than focusing on nearly spin-free materials, this thesis investigates the microwave and optical transitions of rare-earth ions in materials that are fully concentrated with electronic spins. Recent studies on rare-earth magnetic materials have demonstrated narrow optical linewidths resulting from magnetic ordering and a particularly strong coupling between microwave cavity modes and the collective excitations of rare-earth ions. Although these recent studies are noteworthy, the energy-level transitions, especially optical transitions, of rare-earth ions in magnetic materials remain largely unexamined. In this thesis, various spectroscopic studies are employed to characterise their transition properties and to develop a model of energy levels. The model presented is expected to be applicable to other rare-earth magnetic materials, thereby opening avenues for further investigation in this class of systems. Two types of rare-earth magnetic materials are investigated: neodymium gallate with a stoichiometric concentration of neodymium ions, and gadolinium vanadate doped with a low (ppm) concentration of erbium ions. Microwave and optical transmission spectroscopy are employed under externally applied magnetic fields to characterise the energy-state transitions of the rare-earth ions in both materials. The magnetic phases and corresponding spin configurations influence the observed spectra, making conventional approaches to spectral simulation inadequate. To address this challenge, mean field and magnon-coupled crystal-field models are developed in this thesis to predict magnon and optical transition spectra. These simulations exhibit good agreement with experimental results, allowing for the characterisation of transition properties. Following the characterisation of the material, a new transduction approach is introduced, developed, and implemented using doped rare-earth ions in a magnetic material. In this scheme, coherent conversion between microwave and optical modes is achieved by exciting an optical transition of the doped ions.

•May 14, 2025•0 citations

Raman heterodyne detection of nuclear magnetic resonance

N. C. Wong, Emily S. Kintzer, J. Mlynek +2 more

A novel coherent Raman effect induced by a laser and a radio-frequency (rf) field is used to detect cw and pulsed nuclear magnetic resonance (NMR) in ground and excited electronic states. The effect is illustrated in the impurity-ion solid ${\mathrm{Pr}}^{3+}$: La${\mathrm{F}}_{3}$ at 1.6 K utilizing the ${\mathrm{Pr}}^{3+}$ optical transition $^{3}H_{4}({\ensuremath{\Gamma}}_{1})\ensuremath{\rightarrow}^{1}D_{2}({\ensuremath{\Gamma}}_{1})$. The laser field of frequency ${\ensuremath{\omega}}_{E}$ and the rf field (${\ensuremath{\omega}}_{H}$) induce a light wave at the sum ${\ensuremath{\omega}}_{E}+{\ensuremath{\omega}}_{H}$ (anti-Stokes) and difference ${\ensuremath{\omega}}_{E}\ensuremath{-}{\ensuremath{\omega}}_{H}$ (Stokes) frequencies, generating an absorptive or dispersive heterodyne beat signal (${\ensuremath{\omega}}_{H}$) with the laser field at a photodetector. The theory of this effect is characterized in a new three-level perturbation calculation which requires, unlike the usual stimulated Raman effect, that all three transitions be electric- or magnetic-dipole allowed. Detailed predictions are confirmed by cw measurements of the ${\mathrm{Pr}}^{3+}$: La${\mathrm{F}}_{3}$ hyperfine splittings where the optical heterodyne signals are shot-noise limited. The ${\mathrm{Pr}}^{3+}$ nuclear quadrupole parameters are obtained for the $^{3}H_{4}$ and $^{1}D_{2}$ states where the line centers are determined with kilohertz precision. The corresponding wave functions show significant hyperfine-state mixing, as required for all three transitions to be dipole allowed. The cw line shapes are narrow (30-160 kHz), inhomogeneously broadened by nuclear magnetic interactions, and reveal either a Gaussian or an anomalous second-derivative---like line shape. The spin-echo measurements for the $^{3}H_{4}$ and $^{1}D_{2}$ hyperfine transitions yield homogeneous line shapes which are Lorentzian, and rather surprisingly, linewidths in the narrow range 10-20 kHz, a result which tests current line-broadening theories.

Physical review. B, Condensed matter•Nov 1, 1983•110 citations

Optical and spin manipulation of non-Kramers rare-earth ions in a weak magnetic field for quantum memory applications

Jean Etesse, Adrian Holzäpfel, Antonio Ortu +1 more

Rare-earth ion doped crystals have proven to be solid platforms for implementing quantum memories. Their potential use for integrated photonics with large multiplexing capability and unprecedented coherence times is at the core of their attractiveness. The best performances of these ions are, however, usually obtained when subjected to a DC magnetic field, but consequences of such fields on the quantum memory protocols have only received little attention. In this paper, we focus on the effect of a DC bias magnetic field on the population manipulation of non-Kramers ions with nuclear quadrupole states, both in the spin and optical domains, by developing a simple theoretical model. We apply this model to explain experimental observations in a $^{151}\mathrm{Eu}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ crystal, and highlight specific consequences on the atomic frequency comb spin-wave protocol. The developed analysis should allows predicting optimal magnetic field configurations for various protocols.

arXiv:2011.05114•Physical Review A•Feb 26, 2021•19 citations

Nuclear Spin Coherence and All‐Optical Dynamical Decoupling in Eu 3+ :Y 2 O 3 Ceramics

Miaomiao Ren, Anonymous, Jun Wang +7 more

ABSTRACT Rare‐earth‐ion‐doped solid materials have attracted considerable interest for quantum technologies. However, achieving robust spin coherence in polycrystalline systems remains challenging due to structural disorder and limited understanding spin environments. Here, we report high‐quality : optical ceramics with optical inhomogeneous of GHz and sub‐kHz homogeneous linewidths, indicating a spectrally quiet optical environment. At cryogenic temperatures, spin‐dynamics measurements show that decoherence is strongly influenced by the surrounding nuclear spin bath. Magnetic‐field‐dependent studies, combined with radio‐frequency spectroscopy, reveal the sensitivity of spin coherence to weak magnetic perturbations and enable selective addressing of the bath spins. By applying an all‐optical Raman dynamical decoupling protocol, we substantially prolong the observed nuclear‐spin coherence decay, yielding a slow decay component of 224 ms. These results establish : ceramics as a promising platform for solid‐state quantum memories and highlight the potential of spin‐bath engineering in polycrystalline rare‐earth‐ion systems.

Advanced Quantum Technologies•Sep 1, 2026•0 citations
We show that the coherence properties of the nuclear spin states of rare-earth ions in solids can be manipulated by small applied electric fields. This was done by measuring the Stark effect on the nuclear quadrupole transitions of 151Eu^{151}\mathrm{Eu}151Eu in Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ (YSO) using a combination of Raman heterodyne optical detection and Stark modulated quadrupole echoes to achieve high sensitivity. The measured Stark coefficients were 0.42 and 1.0  Hz cm/V1.0\text{ }\text{ }\mathrm{Hz}\text{ }\mathrm{cm}/\mathrm{V}1.0  Hz cm/V for the two quadrupole transitions at 34.54 and 46.20 MHz, respectively. The long decoherence time of the nuclear spin states (25 ms) allowed us to make the measurements in very low electric fields of \ensuremath∼10  V/cm\ensuremath{\sim}10\text{ }\text{ }\mathrm{V}/\mathrm{cm}\ensuremath∼10  V/cm, which produced 100% modulation of the nuclear spin echo, and to measure Stark shifts of \ensuremath∼1  Hz\ensuremath{\sim}1\text{ }\text{ }\mathrm{Hz}\ensuremath∼1  Hz or 20 ppm of the inhomogeneous linewidth.
Abstract We have measured inhomogeneous linewidths and coherence times ( T 2 ) of nuclear spin transitions in a Eu 3+ :Y 2 O 3 transparent ceramic by an all-optical spin echo technique. The nuclear spin echo decay curves showed a strong modulation which was attributed to interaction with Y nuclei in the host. The coherence time of the 29 MHz spin transition in 151 Eu 3+ was 16 ms in a small applied magnetic field. Temperature dependent measurements showed that the coherence time was constant up to 18 K and was limited by spin-lattice relaxation for higher temperatures. Nuclear spin echoes in 153 Eu 3+ gave much weaker signals than for the case of 151 Eu 3+ . The spin coherence time for the 73 MHz spin transition in 153 Eu 3+ was estimated to 14 ms in a small magnetic field. The study shows that the spin transitions of ceramic Eu 3+ :Y 2 O 3 have coherence properties comparable to the best rare-earth-doped materials available.
We report a series of measurements of the effect of an electric field on the frequency of the ultranarrow linewidth F70→ D50 optical transition of Eu3+ ions in an Y2SiO5 matrix at cryogenic temperatures. We provide linear Stark coefficients along two dielectric axes and for the two different substitution sites of the Eu3+ ions, with an unprecedented accuracy and an upper limit for the quadratic Stark shift. The measurements, which indicate that the electric field sensitivity is a factor of seven larger for site 1 relative to site 2 for a particular direction of the electric field, are of direct interest in the context of both quantum information processing and laser frequency stabilization with rare-earth doped crystals, in which electric fields can be used to engineer experimental protocols by tuning transition frequencies.
Microwave and optical transitions of rare-earth ions enable microwave-to-optical frequency transduction. This transduction is a coherent process; therefore, the narrow linewidths and long coherence times of rare-earth ions are crucial for achieving efficient frequency conversion. Particularly long coherence times can be achieved with small-spin materials, as unpaired electronic and nuclear spins introduce magnetic noise, serving as a decoherent source of the transitions. However, complete spin-free rare-earth materials cannot exist without charge compensation. Consequently, residual spins in existing rare-earth materials act as a bottleneck, limiting both their spin and optical coherence times. Rather than focusing on nearly spin-free materials, this thesis investigates the microwave and optical transitions of rare-earth ions in materials that are fully concentrated with electronic spins. Recent studies on rare-earth magnetic materials have demonstrated narrow optical linewidths resulting from magnetic ordering and a particularly strong coupling between microwave cavity modes and the collective excitations of rare-earth ions. Although these recent studies are noteworthy, the energy-level transitions, especially optical transitions, of rare-earth ions in magnetic materials remain largely unexamined. In this thesis, various spectroscopic studies are employed to characterise their transition properties and to develop a model of energy levels. The model presented is expected to be applicable to other rare-earth magnetic materials, thereby opening avenues for further investigation in this class of systems. Two types of rare-earth magnetic materials are investigated: neodymium gallate with a stoichiometric concentration of neodymium ions, and gadolinium vanadate doped with a low (ppm) concentration of erbium ions. Microwave and optical transmission spectroscopy are employed under externally applied magnetic fields to characterise the energy-state transitions of the rare-earth ions in both materials. The magnetic phases and corresponding spin configurations influence the observed spectra, making conventional approaches to spectral simulation inadequate. To address this challenge, mean field and magnon-coupled crystal-field models are developed in this thesis to predict magnon and optical transition spectra. These simulations exhibit good agreement with experimental results, allowing for the characterisation of transition properties. Following the characterisation of the material, a new transduction approach is introduced, developed, and implemented using doped rare-earth ions in a magnetic material. In this scheme, coherent conversion between microwave and optical modes is achieved by exciting an optical transition of the doped ions.
A novel coherent Raman effect induced by a laser and a radio-frequency (rf) field is used to detect cw and pulsed nuclear magnetic resonance (NMR) in ground and excited electronic states. The effect is illustrated in the impurity-ion solid Pr3+{\mathrm{Pr}}^{3+}Pr3+: LaF3{\mathrm{F}}_{3}F3​ at 1.6 K utilizing the Pr3+{\mathrm{Pr}}^{3+}Pr3+ optical transition $^{3}H_{4}({\ensuremath{\Gamma}}_{1})\ensuremath{\rightarrow}^{1}D_{2}({\ensuremath{\Gamma}}_{1})$. The laser field of frequency ${\ensuremath{\omega}}_{E}$ and the rf field (${\ensuremath{\omega}}_{H}$) induce a light wave at the sum ${\ensuremath{\omega}}_{E}+{\ensuremath{\omega}}_{H}$ (anti-Stokes) and difference ${\ensuremath{\omega}}_{E}\ensuremath{-}{\ensuremath{\omega}}_{H}$ (Stokes) frequencies, generating an absorptive or dispersive heterodyne beat signal (${\ensuremath{\omega}}_{H}$) with the laser field at a photodetector. The theory of this effect is characterized in a new three-level perturbation calculation which requires, unlike the usual stimulated Raman effect, that all three transitions be electric- or magnetic-dipole allowed. Detailed predictions are confirmed by cw measurements of the Pr3+{\mathrm{Pr}}^{3+}Pr3+: LaF3{\mathrm{F}}_{3}F3​ hyperfine splittings where the optical heterodyne signals are shot-noise limited. The Pr3+{\mathrm{Pr}}^{3+}Pr3+ nuclear quadrupole parameters are obtained for the 3H4^{3}H_{4}3H4​ and 1D2^{1}D_{2}1D2​ states where the line centers are determined with kilohertz precision. The corresponding wave functions show significant hyperfine-state mixing, as required for all three transitions to be dipole allowed. The cw line shapes are narrow (30-160 kHz), inhomogeneously broadened by nuclear magnetic interactions, and reveal either a Gaussian or an anomalous second-derivative---like line shape. The spin-echo measurements for the 3H4^{3}H_{4}3H4​ and 1D2^{1}D_{2}1D2​ hyperfine transitions yield homogeneous line shapes which are Lorentzian, and rather surprisingly, linewidths in the narrow range 10-20 kHz, a result which tests current line-broadening theories.
Rare-earth ion doped crystals have proven to be solid platforms for implementing quantum memories. Their potential use for integrated photonics with large multiplexing capability and unprecedented coherence times is at the core of their attractiveness. The best performances of these ions are, however, usually obtained when subjected to a DC magnetic field, but consequences of such fields on the quantum memory protocols have only received little attention. In this paper, we focus on the effect of a DC bias magnetic field on the population manipulation of non-Kramers ions with nuclear quadrupole states, both in the spin and optical domains, by developing a simple theoretical model. We apply this model to explain experimental observations in a 151Eu:Y2SiO5^{151}\mathrm{Eu}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}151Eu:Y2​SiO5​ crystal, and highlight specific consequences on the atomic frequency comb spin-wave protocol. The developed analysis should allows predicting optimal magnetic field configurations for various protocols.
ABSTRACT Rare‐earth‐ion‐doped solid materials have attracted considerable interest for quantum technologies. However, achieving robust spin coherence in polycrystalline systems remains challenging due to structural disorder and limited understanding spin environments. Here, we report high‐quality : optical ceramics with optical inhomogeneous of GHz and sub‐kHz homogeneous linewidths, indicating a spectrally quiet optical environment. At cryogenic temperatures, spin‐dynamics measurements show that decoherence is strongly influenced by the surrounding nuclear spin bath. Magnetic‐field‐dependent studies, combined with radio‐frequency spectroscopy, reveal the sensitivity of spin coherence to weak magnetic perturbations and enable selective addressing of the bath spins. By applying an all‐optical Raman dynamical decoupling protocol, we substantially prolong the observed nuclear‐spin coherence decay, yielding a slow decay component of 224 ms. These results establish : ceramics as a promising platform for solid‐state quantum memories and highlight the potential of spin‐bath engineering in polycrystalline rare‐earth‐ion systems.