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arXiv:1611.05444 · Physical review. B./Physical review. B

Spectral hole lifetimes and spin population relaxation dynamics in neodymium-doped yttrium orthosilicate

Emmanuel Zambrini Cruzeiro, Alexey Tiranov, Imam Usmani, Cyril Laplane, Jonathan Lavoie, Alban Ferrier, Philippe Goldner, Nicolas Gisin, Mikael Afzelius

Published May 11, 2017• 23 citations
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Abstract

We present a detailed study of the lifetime of optical spectral holes due to population storage in Zeeman sublevels of ${\mathrm{Nd}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$. The lifetime is measured as a function of magnetic field strength and orientation, temperature, and ${\mathrm{Nd}}^{3+}$ doping concentration. At the lowest temperature of 3 K we find a general trend where the lifetime is short at low field strengths, then increases to a maximum lifetime at a few hundred mT, and then finally decays rapidly for high field strengths. This behavior can be modeled with a relaxation rate dominated by ${\mathrm{Nd}}^{3+}\ensuremath{-}{\mathrm{Nd}}^{3+}$ cross relaxation at low fields and spin lattice relaxation at high magnetic fields. The maximum lifetime depends strongly on both the field strength and orientation, due to the competition between these processes and their different angular dependencies. The cross relaxation limits the maximum lifetime for concentrations as low as 30 ppm of ${\mathrm{Nd}}^{3+}$ ions. By decreasing the concentration to less than 1 ppm we could completely eliminate the cross relaxation, reaching a lifetime of 3.8 s at 3 K. At higher temperatures the spectral hole lifetime is limited by the magnetic-field-independent Raman and Orbach processes. In addition we show that the cross relaxation rate can be strongly reduced by creating spectrally large holes of the order of the optical inhomogeneous broadening. Our results are important for the development and design of new rare-earth-ion doped crystals for quantum information processing and narrow-band spectral filtering for biological tissue imaging.

DOI
10.1103/physrevb.95.205119

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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.
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Detailed site-selective spectroscopy has been performed as a function of temperature on the ${}^{7}{F}_{0}{\ensuremath{\leftrightarrow}}^{5}{D}_{0}$ transition of Eu3+:Y2SiO5{\mathrm{Eu}}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Eu3+:Y2​SiO5​ for Eu3+{\mathrm{Eu}}^{3+}Eu3+ concentrations of 0.02%, 0.1%, 0.5%, and 1%. Time-domain optical dephasing, spectral hole lifetimes, anisotropic absorption coefficients, inhomogeneous linewidths, and fluorescence lifetimes for Eu3+{\mathrm{Eu}}^{3+}Eu3+ ions at both crystallographic sites were measured. The temperature dependence of the optical dephasing, transition energy, and linewidth of the ${}^{7}{\stackrel{\ensuremath{\rightarrow}}{{F}_{0}}}^{5}{D}_{0}$ absorption was measured and interpreted in terms of Raman scattering of phonons. Photon echo measurements of optical dephasing gave T2{T}_{2}T2​ values as long as 2.6 ms, approaching the limit set by the fluorescence decay time. Spectral hole lifetimes were measured for temperatures from 2 K to 18 K, with observed lifetimes varying from 1 s at 18 K to an estimated value of greater than 20 days at 2 K. Anisotropic absorption coefficients were measured, and an increase in Eu3+{\mathrm{Eu}}^{3+}Eu3+ concentration from 0.02% to 7% produced an increase in the inhomogeneous linewidth ${\ensuremath{\Gamma}}_{\mathrm{inh}}$ from 0.5 GHz to \ensuremath{\sim}150 GHz, indicating that Eu3+{\mathrm{Eu}}^{3+}Eu3+ doping induces significant strain in the crystal. New determinations of many energy levels of 7FJ{}^{7}{F}_{J}7FJ​ multiplets have been made for J=0J=0J=0 to 6.
We use spectral hole burning to investigate spin dynamics within the electronic Zeeman sublevels of the ground state of the erbium ions in erbium-doped fibers (EDF). Conducted at ultra-low temperatures and under varying magnetic fields, our study reveals distinct changes in spin relaxation dynamics across different conditions. We identified three decay components at approximately 7 mK, with one achieving spin lifetimes of over 9 hours under optimal conditions, while two components were observed at higher temperatures. The fairly stable relative weights of the decay components across conditions suggest distinct ion populations contributing to the observed relaxation dynamics. While earlier studies struggled to account for all decay components at higher temperatures, our approach successfully models spin dynamics across all observed decay components, using a consistent set of underlying mechanisms, including spin flip-flop interactions, direct coupling to two-level systems, and Raman-type processes, and distinguishes the decay components by the strengths with which these mechanisms contribute. These results suggest EDFs' potential as a promising candidate for quantum memory applications, with further room for optimization.