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Hyperfine Structure and Coherent Properties of Erbium-167-doped Yttrium Orthosilicate

Jelena V. Rakonjac

Published Jan 1, 2018• 3 citations
OpenAlex

Abstract

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its hyperfine structure.\nBy comparing our spectra to the existing ground state spin Hamiltonian parameters, and unpublished excited state parameters, we identified the origin of many of the transitions.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.

Related papers

Spin echoes in the ground and an optically excited state of $^{167}$Er$^{3+}$:Y$_2$SiO$_5$ at near-zero magnetic fields using Raman heterodyne spectroscopy

Jelena V. Rakonjac, Yuhui Chen, Sebastian P. Horvath +1 more

Erbium-167-doped yttrium orthosilicate is an ideal candidate for a microwave-addressed quantum memory due to its telecom wavelength optical transition and hyperfine structure with and without an applied magnetic field. However, to date there has been little investigation in coherence times for transitions around zero magnetic field, or for hyperfine structure other than from the ground state. Through the use of Raman heterodyne spectroscopy, we have identified transitions at zero magnetic field with a small dependence on field that are suitable for detecting spin echoes for both the ground and excited state. We measured coherence times of transitions at 879.4 MHz and 896.7 MHz as 370 $\mu$s and 1.4 ms respectively at 3.2 K. This is a 100-fold increase in coherence time compared to previous measurements at the same dopant concentration and 200 times greater than the even isotopes of erbium-doped yttrium orthosilicate previously used to demonstrate a microwave memory.

•Feb 12, 2018•0 citations

Coherent Frequency Conversion from Microwave to Optical Fields in an Erbium Doped Y2SiO5 Crystal: Towards the Single Photon Regime

Xavier Fernandez-Gonzalvo

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.

•Jan 1, 2017•1 citation

Spectroscopic study of hyperfine properties in Yb3+171:Y2SiO5

Alexey Tiranov, Antonio Ortu, Sacha Welinski +4 more

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 ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ crystal doped with $^{171}\mathrm{Yb}^{3+}$ ions. This isotope is particularly interesting since it is the only rare--earth ion having electronic spin $S=\frac{1}{2}$ and nuclear spin $I=\frac{1}{2}$, 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 $^{171}\mathrm{Yb}^{3+}:{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ crystal.

arXiv:1712.08616•Physical review. B./Physical review. B•Nov 8, 2018•36 citations

Decoherence characterization and quantum memory design in 167Er3+:Y2SiO5

Mucheng Guo, Qiangrui Li, Zhehao Xu +3 more

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.

Frontiers of Physics•Oct 31, 2025•1 citation

Hyperfine interactions and coherent spin dynamics of isotopically purified 167Er3+ in polycrystalline Y2O3

Tijana Rajh, Lei Sun, Shobhit Gupta +3 more

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.

Materials for Quantum Technology•Nov 1, 2022•12 citations

A comprehensive understanding of ground and optically-excited hyperfine structure of ¹⁶⁷Er³+:Y2SiO5

Horvath Sp, Jelena V. Rakonjac, Chen Yh +4 more

Using high-performance computing techniques and targeted experimental investigation we have developed a predictive crystal-field model of the complex hyperfine structure of ¹⁶⁷Er³+:Y2SiO5 We simultaneously match site-selective spectroscopic data up to 20,000 cm-¹, rotational Zeeman data, and ground- and excited-state hyperfine structure determined from high-resolution Raman-heterodyne spectroscopy on the 1.5 μm telecom transition. We achieve agreement of better than 50 MHz for assigned hyperfine transitions. The successful analysis of the complex hyperfine patterns opens the possibility of systematically searching this whole class of materials for the ZEFOZ transitions that have proved so useful in quantum information applications.

•Jan 1, 2018•0 citations
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.
Spin echoes in the ground and an optically excited state of 167^{167}167Er3+^{3+}3+:Y2_22​SiO5_55​ at near-zero magnetic fields using Raman heterodyne spectroscopy
Erbium-167-doped yttrium orthosilicate is an ideal candidate for a microwave-addressed quantum memory due to its telecom wavelength optical transition and hyperfine structure with and without an applied magnetic field. However, to date there has been little investigation in coherence times for transitions around zero magnetic field, or for hyperfine structure other than from the ground state. Through the use of Raman heterodyne spectroscopy, we have identified transitions at zero magnetic field with a small dependence on field that are suitable for detecting spin echoes for both the ground and excited state. We measured coherence times of transitions at 879.4 MHz and 896.7 MHz as 370 μ\muμs and 1.4 ms respectively at 3.2 K. This is a 100-fold increase in coherence time compared to previous measurements at the same dopant concentration and 200 times greater than the even isotopes of erbium-doped yttrium orthosilicate previously used to demonstrate a microwave memory.
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.
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.
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.
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.
Using high-performance computing techniques and targeted experimental investigation we have developed a predictive crystal-field model of the complex hyperfine structure of ¹⁶⁷Er³+:Y2SiO5 We simultaneously match site-selective spectroscopic data up to 20,000 cm-¹, rotational Zeeman data, and ground- and excited-state hyperfine structure determined from high-resolution Raman-heterodyne spectroscopy on the 1.5 μm telecom transition. We achieve agreement of better than 50 MHz for assigned hyperfine transitions. The successful analysis of the complex hyperfine patterns opens the possibility of systematically searching this whole class of materials for the ZEFOZ transitions that have proved so useful in quantum information applications.