Erbium-doped crystals are promising candidates for fiber-compatible quantum memories due to their optical transition in the telecommunication C-band. Here, we investigate the optical decoherence dynamics of isotopically enriched 167Er3+:Y2SiO5 (YSO) at sub-Kelvin temperatures and low magnetic fields (<1 T). We observed an optical homogeneous linwidth of 100 Hz at 100 mK and 0.2 T – significantly narrower than previous values obtained at 7 T in a sample with the same 167Er3+ concentration. We analyze the dependence of coherence properties on magnetic field orientation and temperature, identifying spectral diffusion resulted from the host spin bath as key decoherence mechanisms. We further identified that superhyperfine interactions between the 167Er3+ and the host bath spins pose challenges for long-term storage protocols requiring precise spectral tailoring. To address this issue, we propose a strategy that combined the Stark modulation memory scheme with noiseless photon echo storage protocol, which is expected to achieve spin-wave quantum storage with lower noise and higher efficiency.
Erbium-doped crystals are promising candidates for fiber-compatible quantum memories due to their optical transition in the telecommunication C-band. Here, we investigate the optical decoherence dynamics of isotopically enriched 167Er3+:Y2SiO5 (YSO) at sub-Kelvin temperatures and low magnetic fields (<1 T). We observed an optical homogeneous linwidth of 100 Hz at 100 mK and 0.2 T – significantly narrower than previous values obtained at 7 T in a sample with the same 167Er3+ concentration. We analyze the dependence of coherence properties on magnetic field orientation and temperature, identifying spectral diffusion resulted from the host spin bath as key decoherence mechanisms. We further identified that superhyperfine interactions between the 167Er3+ and the host bath spins pose challenges for long-term storage protocols requiring precise spectral tailoring. To address this issue, we propose a strategy that combined the Stark modulation memory scheme with noiseless photon echo storage protocol, which is expected to achieve spin-wave quantum storage with lower noise and higher efficiency.
Erbium-167-doped yttrium orthosilicate (167Er3+:Y2SiO5) is a rare-earth-ion-doped crystal which possesses unique properties that would make it an ideal microwave-addressed quantum memory. It has an optical transition at 1.5 µm, which lies in the telecom C-band where much of the optical telecommunications infrastructure is already operating. It also possesses both nuclear and electron spin states, and hyperfine structure with transitions at microwave frequencies. The hyperfine structure exhibits microwave frequency transitions with or without an applied magnetic field, which would allow for a memory compatible with superconducting systems. However, the complicated hyperfine structure has prevented the transitions of 167Er3+:Y2SiO5 from being fully utilised.\nWith the recent publication of new spin Hamiltonian parameters for the ground state of 167Er3+:Y2SiO5, we can predict which transitions should have the longest coherence time at zero field. Based on calculations using these spin Hamiltonian parameters, we used Raman heterodyne spectroscopy to investigate the hyperfine structure of 167Er3+:Y2SiO5 for small magnetic fields and for energy level differences from 600 to 1200 MHz. We observed many transitions from the 4I15/2 ground state, as well as the 4I13/2 excited state that until now has had little investigation regarding its hyperfine structure.\nBy comparing our spectra to the existing ground state spin Hamiltonian parameters, and unpublished excited state parameters, we identified the origin of many of the transitions. We observed differences between the predicted transition frequencies from both sets of parameters and the experimental data. The data obtained using Raman heterodyne was used to improve both ground and excited state parameters to give a better description of the zero-field hyperfine splittings.\nIn addition, we identified transitions from both the 4I15/2 ground and 4I13/2 excited state that have a small dependence on magnetic field. These transitions, with zero field frequencies of 879.4 MHz and 896.7 MHz respectively, yielded coherence times of 67 µs and 300 µs at 3.2 K, when measured with a two-pulse spin echo sequence. By using a dynamic decoupling sequence, we extending the coherence times of the transitions at 879.4 MHz to 380 µs and for the transitions at 896.7 MHz, to 1.4 ms.\nThese coherence time measurements demonstrate an improvement of a previous zero field coherence measurement in 167Er3+:Y2SiO5. By operating at lower temperatures, reducing the 167Er3+ ion concentration or using a different transition, it should be possible to extend the coherence time of 167Er3+:Y2SiO5 even further.
Optical coherence and spin population dynamics in 171Yb3+:Y2SiO5 single crystals
171Yb3+-doped Y2SiO5 crystals are a promising platform for optical quantum memories in long-distance quantum communications. The relevance of this material lies in 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 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 171Yb concentration.
Abstract 167Er3+ doped solids are a promising platform for quantum technology due to erbium’s telecom C-band optical transition and its long hyperfine coherence times. We experimentally study the spin Hamiltonian and dynamics of 167Er3+ spins in Y2O3 using electron paramagnetic resonance (EPR) spectroscopy. The anisotropic electron Zeeman, hyperfine and nuclear quadrupole matrices are fitted using data obtained by X-band (9.5 GHz) EPR spectroscopy. We perform pulsed EPR spectroscopy to measure spin relaxation time T 1 and coherence time T 2 for the 3 principal axes of an anisotropic g tensor. Long electronic spin coherence time up to 24.4 μs is measured for lowest g transition at 4 K, exceeding previously reported values at much lower temperatures. Measurements of decoherence mechanism indicates T 2 limited by spectral diffusion and instantaneous diffusion. Long spin coherence times, along with a strong anisotropic hyperfine interaction makes 167Er3+:Y2O3 a rich system and an excellent candidate for spin-based quantum technologies.
Rare earth doped crystals are a promising platform for long-distance quantum communications, where they can perform quantum light storage. Among different systems, 171Yb3+-doped Y2SiO5 (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.
Quantum information processing has been developing rapidly in the last two decades as a way to overcome the limitations of classical electronics. Several components to generate, process and send quantum information are needed. In this context, optical quantum memories appear as principal components to communicate quantum information at long distances by overcoming the losses of the optical fibers in the so-called quantum repeater scheme. During the last decade several storage protocols to store quantum information have been proposed and tested. In this thesis, I present the Revival of Silenced Echo (ROSE) protocol implemented in an Er3+:Y2SiO5 crystal. This material is a good candidate for a quantum memory because of its transition in the C-band of the telecom wavelengths where the losses in optical fibers are minimized. In this work, I evaluate the ROSE performances with weak classical pulses. I measure efficiency, bandwidth and storage time which are the typical figures of merit for an optical quantum memory. Starting with a fixed bandwidth, I demonstrate experimentally a good efficiency. Additionally, I measure the bandwidth dependence of the protocol. For this latter, the dipole-dipole interactions between erbium ions appears as limiting factors. Finally, I implement the ROSE protocol with a few photons per pulse to show its potential as a quantum memory. I report good efficiencies with a moderate signal to noise ratio.I finish this work with a series of measurements in new materials (doped or codoped with erbium), to extend the processing bandwidth of Er doped samples compatible the telecom wavelength range.
In the context of quantum information technologies superconducting qubits (SQs) are very attractive devices for the manipulation of quantum states, and present themselves as one of our best candidates to build a quantum processor. They couple naturally to microwave photons, for which suitable quantum memories or a long distance propagation channel don’t exist. A way around these limitations is to turn these microwave photons into optical ones by building a quantum frequency converter: a device by which the frequency of a photon can be changed while preserving its non-classical correlations. Then, optical fibres could be used to link distant SQ-based devices together, facilitating the creation of a network of quantum computers. Moreover, SQs could then be coupled to quantum memories compatible with photons at optical frequencies, which are the most well developed kind of quantum memories at the present time. This thesis explores the possibility to convert single microwave photons into optical photons using erbium doped in a yttrium orthosilicate crystal (Er3+:Y2SiO5). Er3+:Y2SiO5 is a good candidate because it has a naturally occurring optical transition near 1536 nm close to the point where silica optical fibres show their minimum loss. A microwave transition can be found in two different ways: one way is to use the 167 isotope of erbium, which is the only stable isotope that shows hyperfine splitting as it has non-zero nuclear spin. The hyperfine structure of the ground state of 167Er3+:Y2SiO5 spans over about 5 GHz. The other possibility is to use the other stable isotopes of erbium and Zeeman split their ground state using an external magnetic field. A microwave transition near 5 GHz can be achieved with moderate magnetic fields due to the high 𝑔-factors of Er3+:Y2SiO5. The physical process of interest is a three wave mixing process involving two fields at optical frequencies and one field at microwave frequencies. In order to boost the efficiency of the frequency conversion process the Er3+:Y2SiO5 crystal is placed inside a microwave and an optical resonator. The problem is first explored from the theoretical point of view, where a nonlinear coefficient Λ(2) is derived (analogous to the 𝜒(2) often used in nonlinear optics), and the interaction between cavity modes and the nonlinear medium is studied. It is predicted that with a sample cooled down to millikelvin temperatures total frequency conversion between microwave and optical fields can be achieved. A preliminary hole burning spectroscopy experiment is performed with the objective of reconstructing the hyperfine structure of the excited state of 167Er3+:Y2SiO5, but the complexity of the problem makes it too difficult to achieve this goal. Then a series of experiments are shown, aimed at determining whether or not frequency conversion at the single photon level is achievable using the even isotopes of erbium in a magnetic field. These experiments are based in the Raman heterodyne spectroscopy technique, which is used in combination with electron paramagnetic resonance and optical absorption spectroscopy. In all experiments the sample is cooled down to cryogenic temperatures near 4 K. A first experiment shows that the frequency conversion process exists in Er3+:Y2SiO5, in a setup where only a microwave resonator is used, but not an optical one. A second experiment is performed in a similar setup, this time presenting a quantitative study of the properties of the frequency conversion process, and its comparison with the theoretical model previously derived. A third experiment is performed, which incorporates an optical cavity to the system. The interaction between the erbium ions and the optical cavity introduces a whole new range of experimental complications, which are studied and discussed. Then, the frequency conversion signal is studied anew, showing an unexpected highly non-linear scaling behaviour with the input powers. A hypothesis explaining this unexpected behaviour is given, referring to stray optical absorption in the inhomogeneous line of Er3+:Y2SiO5 (and in particular 167Er3+:Y2SiO5), which can be bleached out under certain circumstances due to spectral hole burning effects. The overall maximum frequency conversion efficiency observed is of 3 × 10^−4 per Watt of pump laser power. While this value is still far from the target several ways of improvement are proposed, including cooling down the system to millikelvin temperatures, increasing the dopant concentration and modifying the geometry of the resonators.