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arXiv:1712.02682 · New Journal of Physics

Efficient optical pumping using hyperfine levels in 145 Nd 3+ :Y 2 SiO 5 and its application to optical storage

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

Published Apr 16, 2018• 22 citations
arXivHTMLPDF

Abstract

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.

DOI
10.1088/1367-2630/aabe3b

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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.
Erbium-doped solids are potential candidates for the realization of a quantum memory for photons at telecommunication wavelengths. The implementation of quantum memory proposals in rare-earth-ion-doped solids require spectral tailoring of the inhomogeneous absorption profile by efficient population transfer between ground-state levels (spin polarization) using optical pumping. In this paper we investigate the limiting factors of efficient optical pumping between ground-state Zeeman levels in an erbium-doped Y2SiO5{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}Y2​SiO5​ crystal. We introduce two methods to overcome these limiting factors: stimulated emission using a second laser and spin mixing using radio frequency excitation. Both methods significantly improve the degree of spin polarization. Population transfer between two Zeeman levels with less than 10% of the total population in the initial ground state is achieved, corresponding to a spin polarization greater than 90%. In addition, we demonstrate spectral tailoring by isolating a narrow absorption peak within a large transparency window.
Abstract Optical quantum memories are essential components for realizing the full potential of quantum networks. Among these, rare-earth-doped crystal memories stand out due to their large multimode storage capabilities. To maximize the multimode capacity in the time domain, it is key to simultaneously achieve large memory bandwidth and long optical storage time. Here, we demonstrate an atomic frequency comb optical memory in 171 Yb 3+ :Y 2 SiO 5 , with a memory bandwidth of 250 MHz and a storage time of up to 125 µ s. The efficiency reaches 20% at short storage times, and 5% at 125 µ s. These results were enabled by an optimized optical pumping scheme, guided by numerical modelling. Our approach is specifically designed for future spin-wave storage experiments, with the theoretical bandwidth limit set at 288 MHz by the hyperfine structure of 171 Yb 3+ :Y 2 SiO 5 . Additionally, we introduce an efficient method for synthesizing the optical pumping waveforms required for generating combs with tens of thousands of teeth, as well as a simple yet frequency-agile laser setup for optical pumping across a 10 GHz bandwidth.
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.
Spin dynamics are investigated in several rare-earth-ion-doped crystals, both for so-called Kramers ions and non-Kramers ions. I have studied two illustrative examples of such systems, Neodymium (Kramers) and Europium (non-Kramers). The main motivation behind these studies is the search for long relaxation and coherence times in solid state atomic ensembles. To this end I employ spectroscopic techniques to probe different kinds of interactions and relaxation mechanisms taking place in the samples. I perform spectroscopy of Neodymium (Kramers) in two different crystal lattices, yttrium orthosilicate and yttrium orthovanadate. I propose new methods to improve the relaxation lifetimes, and make precise characterizations of the interactions taking place within the atomic ensemble. In particular we achieve the most precise measurement of a kind of interaction which has received considerable attention recently in other areas of physics, the Dzyaloshinskii-Moriya interaction. These spectroscopic studies are of course of fundamental interest, but they can also be applied to quantum communication and computation. In this context, we were able to increase the efficiency of a quantum memory based on a Kramers ion (Nd) to be on par with the best non-Kramers (Eu,Pr) memories. Using Neodymium ions, I have certified that multi-dimensional entanglement can be stored in a quantum memory. The second part of this thesis concerns the study of Europium (non-Kramers), starting with a characterization of the Zeeman and quadrupole interactions. I believe these studies will pave the way for long duration (100 ms or more) quantum storage in a rare-earth-ion-doped crystal.
Rare-earth-ion doped crystals are state-of-the-art materials for optical quantum memories and quantum transducers between optical and microwave photons. Here we describe our progress towards a nanophotonic quantum memory based on a rare-earth (Neodymium) doped yttrium orthosilicate (YSO) photonic crystal resonator. The Purcell-enhanced coupling of the 883 nm transitions of Neodymium (Nd3+) ions to the nano-resonator results in increased optical depth, which could in principle facilitate highly efficient photon storage via cavity impedance matching. The atomic frequency comb (AFC) memory protocol can be implemented in the Nd:YSO nano-resonator by efficient optical pumping into the long-lived Zeeman state. Coherent optical signals can be stored and retrieved from the AFC memory. We currently measure a storage efficiency on par with a bulk crystal Nd:YSO memory that is millimeters long. Our results will enable multiplexed on-chip quantum storage and thus quantum repeater devices using rare-earth-ions.
Solid-state impurity spins with optical control are currently investigated for quantum networks and repeaters. Among these, rare-earth-ion doped crystals are promising as quantum memories for light, with potentially long storage time, high multimode capacity, and high bandwidth. However, with spins there is often a tradeoff between bandwidth, which favors electronic spin, and memory time, which favors nuclear spins. Here, we present optical storage experiments using highly hybridized electron-nuclear hyperfine states in ^{171}Yb^{3+}:Y_{2}SiO_{5}, where the hybridization can potentially offer both long storage time and high bandwidth. We reach a storage time of 1.2 ms and an optical storage bandwidth of 10 MHz that is currently only limited by the Rabi frequency of the optical control pulses. The memory efficiency in this proof-of-principle demonstration was about 3%. The experiment constitutes the first optical storage using spin states in any rare-earth ion with electronic spin. These results pave the way for rare-earth based quantum memories with high bandwidth, long storage time, and high multimode capacity, a key resource for quantum repeaters.