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Physical Review B

Spin Hamiltonian characterization and refinement for Pr 3 + :YAlO 3 and Pr 3 + :Y 2 SiO 5

Marko Lovrić, Philipp Glasenapp, Dieter Suter

Published Jan 24, 2012• 24 citations
Publisher

Abstract

Rare-earth ions in dielectric crystals play an important role in high-resolution laser spectroscopy and are interesting candidates for storing quantum states of photons. We characterize the praseodymium hyperfine interaction of the ground-state (${}^{3}$H${}_{4}$) and one excited-state (${}^{1}$D${}_{2}$) for two important compounds: praseodymium doped in yttrium aluminum perovskite and praseodymium doped in yttrium orthosilicate. The spin Hamiltonian parameters are determined by numerical analysis of Raman-heterodyne spectra, which were collected for a range of static external magnetic field strengths and orientations. For Pr${}^{3+}$:YAlO${}_{3}$, we present a full analysis without restrictions for the Zeeman and quadrupole tensors, and our new characterization for Pr${}^{3+}$:Y${}_{2}$SiO${}_{5}$ resolves a controversy in the literature.

DOI
10.1103/physrevb.85.014429

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•Jan 1, 2018•3 citations
Rare-earth ions in dielectric crystals play an important role in high-resolution laser spectroscopy and are interesting candidates for storing quantum states of photons. We characterize the praseodymium hyperfine interaction of the ground-state (3{}^{3}3H4{}_{4}4​) and one excited-state (1{}^{1}1D2{}_{2}2​) for two important compounds: praseodymium doped in yttrium aluminum perovskite and praseodymium doped in yttrium orthosilicate. The spin Hamiltonian parameters are determined by numerical analysis of Raman-heterodyne spectra, which were collected for a range of static external magnetic field strengths and orientations. For Pr3+{}^{3+}3+:YAlO3{}_{3}3​, we present a full analysis without restrictions for the Zeeman and quadrupole tensors, and our new characterization for Pr3+{}^{3+}3+:Y2{}_{2}2​SiO5{}_{5}5​ resolves a controversy in the literature.
Rare-earth ions in dielectric crystals are interesting candidates for storing quantum states of photons. A limiting factor on the optical density and thus the conversion efficiency is the distortion introduced in the crystal by doping elements of one type into a crystal matrix of another type. Here we investigate the system Pr3+{}^{3+}3+:La2{}_{2}2​(WO4{}_{4}4​)3{}_{3}3​, where the similarity of the ionic radii of Pr and La minimizes distortions due to doping. We characterize the praseodymium hyperfine interaction of the ground-state (3{}^{3}3HHH4{}_{4}4​) and one excited state (1{}^{1}1DDD2{}_{2}2​) and determine the spin Hamiltonian parameters by numerical analysis of Raman-heterodyne spectra, which were collected for a range of static external magnetic-field strengths and orientations. On the basis of a crystal-field analysis, we discuss the physical origin of the experimentally determined quadrupole and Zeeman tensor characteristics. We show the potential for quantum memory applications by measuring the spin coherence lifetime in a magnetic field that is chosen such that additional magnetic fields do not shift the transition frequency in first order. Experimental results demonstrate a spin coherence lifetime of 158 ms --- almost 3 orders of magnitude longer than in zero field.
We show that crystal-field calculations for C_{1} point-group symmetry are possible, and that such calculations can be performed with sufficient accuracy to have substantial utility for rare-earth based quantum information applications. In particular, we perform crystal-field fitting for a C_{1}-symmetry site in ^{167}Er^{3+}:Y_{2}SiO_{5}. The calculation simultaneously includes 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 an agreement of better than 50 MHz for assigned hyperfine transitions. The success of this analysis opens the possibility of systematically evaluating the coherence properties, as well as transition energies and intensities, of any rare-earth ion doped into Y_{2}SiO_{5}.
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.
In many important situations, the dominant dephasing mechanism in cryogenic rare-earth-metal-ion--doped systems is due to magnetic field fluctuations from spins in the host crystal. Operating at a magnetic field where a transition has a zero first-order Zeeman (ZEFOZ) shift can greatly reduce this dephasing. Here we identify the location of transitions with a zero first-order Zeeman shift for optical transitions in Pr3+{}^{3+}3+:YAG and for spin transitions in Er3+{}^{3+}3+:Y2{}_{2}2​SiO5{}_{5}5​. The long coherence times that ZEFOZ can enable would make Pr3+{}^{3+}3+:YAG a strong candidate for achieving the strong-coupling regime of cavity QED, and would be an important step forward in creating long-lived telecommunications wavelength quantum memories in Er3+{}^{3+}3+:Y2{}_{2}2​SiO5{}_{5}5​. This work relies mostly on published spin-Hamiltonian parameters, but Raman heterodyne spectroscopy was performed on Pr3+{}^{3+}3+:YAG to measure the parameters for the excited state.
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.