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arXiv:2507.05140 · Physical review. B./Physical review. B

Optical pumping simulations and optical Rabi frequency measurements in Eu 151 3 + : Y 2 SiO 5 under magnetic field

Jingjing Chen, Mikael Afzelius

Published Nov 24, 2025• 0 citations
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Abstract

Europium-doped crystal ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ is an interesting platform for optical quantum memories, due to its long optical and spin coherence times. In this work, we investigate ${^{151}\mathrm{Eu}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ under the application of magnetic field, a complex system with 36 different optical-hyperfine transitions. We present a simple numerical simulator for calculating the effect of optical pumping schemes that allow the isolation of a single-frequency class of ions, applicable to any multilevel atom with inhomogeneous broadening. Experimentally, we develop methodologies for estimating the magnetic field vector, demonstrating high precision in predicting spectral features based on the known spin Hamiltonians. We measured the optical Rabi frequency of 21 transitions among the 36 possible optical-hyperfine transitions, allowing for the construction of a $6\ifmmode\times\else\texttimes\fi{}6$ branching ratio matrix of relative transition strengths. From the Rabi frequency measurements, we derive the optical dipole moment for the $^{7}F_{0}\ensuremath{\leftrightarrow}^{5}D_{0}$ transition, yielding a value of $(6.94\ifmmode\pm\else\textpm\fi{}0.09)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}33}\phantom{\rule{0.28em}{0ex}}\mathrm{C}\phantom{\rule{0.16em}{0ex}}\mathrm{m}$. Our results provide a critical test of the spin Hamiltonian models, demonstrating high precision in predicting energy levels and relative transition strengths, which are key abilities for quantum applications with ${^{151}\mathrm{Eu}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ under magnetic field.

DOI
10.1103/vwjk-x1ny

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Europium-doped crystal Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ is an interesting platform for optical quantum memories, due to its long optical and spin coherence times. In this work, we investigate 151Eu3+:Y2SiO5{^{151}\mathrm{Eu}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}151Eu3+:Y2​SiO5​ under the application of magnetic field, a complex system with 36 different optical-hyperfine transitions. We present a simple numerical simulator for calculating the effect of optical pumping schemes that allow the isolation of a single-frequency class of ions, applicable to any multilevel atom with inhomogeneous broadening. Experimentally, we develop methodologies for estimating the magnetic field vector, demonstrating high precision in predicting spectral features based on the known spin Hamiltonians. We measured the optical Rabi frequency of 21 transitions among the 36 possible optical-hyperfine transitions, allowing for the construction of a 6\ifmmode×\else\texttimes\fi66\ifmmode\times\else\texttimes\fi{}66\ifmmode×\else\texttimes\fi6 branching ratio matrix of relative transition strengths. From the Rabi frequency measurements, we derive the optical dipole moment for the 7F0\ensuremath↔5D0^{7}F_{0}\ensuremath{\leftrightarrow}^{5}D_{0}7F0​\ensuremath↔5D0​ transition, yielding a value of (6.94\ifmmode±\else\textpm\fi0.09)\ifmmode×\else\texttimes\fi10\ensuremath−33Cm(6.94\ifmmode\pm\else\textpm\fi{}0.09)\ifmmode\times\else\texttimes\fi{}{10}^{\ensuremath{-}33}\phantom{\rule{0.28em}{0ex}}\mathrm{C}\phantom{\rule{0.16em}{0ex}}\mathrm{m}(6.94\ifmmode±\else\textpm\fi0.09)\ifmmode×\else\texttimes\fi10\ensuremath−33Cm. Our results provide a critical test of the spin Hamiltonian models, demonstrating high precision in predicting energy levels and relative transition strengths, which are key abilities for quantum applications with 151Eu3+:Y2SiO5{^{151}\mathrm{Eu}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}151Eu3+:Y2​SiO5​ under magnetic field.
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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 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.
We report a low-temperature spectroscopic characterization of the ground-state hyperfine transitions in 151Eu3+:Y2SiO5{}^{151}\mathrm{Eu}{}^{3+}{\mathrm{:Y}}_{2}{\mathrm{SiO}}_{5}151Eu3+:Y2​SiO5​ via coherent Raman scattering. Inhomogeneous linewidths of 21 and 38 kHz were measured for the ${I}_{z}=\ifmmode\pm\else\textpm\fi{}\frac{1}{2}$ $\ensuremath{\leftrightarrow}$ $\ifmmode\pm\else\textpm\fi{}\frac{3}{2}$ and the $\ifmmode\pm\else\textpm\fi{}\frac{3}{2}$ $\ensuremath{\leftrightarrow}$ $\ifmmode\pm\else\textpm\fi{}\frac{5}{2}$ ground-state transitions, respectively. Spin-echo decays were recorded for the ${I}_{z}=\ifmmode\pm\else\textpm\fi{}\frac{1}{2}$ $\ensuremath{\leftrightarrow}$ $\ifmmode\pm\else\textpm\fi{}\frac{3}{2}$ transition at zero field and for a small static magnetic field. In the latter case, analysis by a simple model gave an amplitude of 284 Hz and a correlation time of 3.5 ms for the transition frequency fluctuations. Application of a dynamical decoupling sequence resulted in coherence lifetimes up to 474 ms, an 18-fold increase compared to the spin intrinsic phase memory time of 26 ms.
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.
Efficient optical pumping is an important tool for state initialization in quantum technologies, such as optical quantum memories. In crystals doped with Kramers rare-earth ions, such as erbium and neodymium, efficient optical pumping is challenging due to the relatively short population lifetimes of the electronic Zeeman levels, of the order of 100 ms at around 4 K. In this article we show that optical pumping of the hyperfine levels in isotopically enriched 145 Nd :Y 2 SiO 5 crystals is more efficient, owing to the longer population relaxation times of hyperfine levels. By optically cycling the population many times through the excited state a nuclear spin flip can be forced in the ground state hyperfine manifold, in which case the population is trapped for several seconds before relaxing back to the pumped hyperfine level. To demonstrate the effectiveness of this approach in applications we perform an atomic frequency comb memory experiment with 33% storage efficiency in 145 Nd :Y 2 SiO 5 , which is on a par with results obtained in non-Kramers ions, e.g. europium and praseodymium, where optical pumping is generally efficient due to the quenched electronic spin. Efficient optical pumping in neodymium-doped crystals is also of interest for spectral filtering in biomedical imaging, as neodymium has an absorption wavelength compatible with tissue imaging. In addition to these applications, our study is of interest for understanding spin dynamics in Kramers ions with nuclear spin.