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arXiv:2206.09080 · Physical review. B./Physical review. B

Prediction of optical polarization and high-field hyperfine structure via a parametrized crystal-field model for low-symmetry centers in Er3+ -doped Y2SiO5

Nicholas Jobbitt, J.‐P. R. Wells, Michael F. Reid, Sebastian P. Horvath, Philippe Goldner, Alban Ferrier

Published Oct 13, 2021• 15 citations
arXivHTMLPDF

Abstract

We report on the development and application of a parametrized crystal-field model for both ${\mathrm{C}}_{1}$ symmetry centers in trivalent erbium-doped ${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$. High-resolution Zeeman and temperature dependent absorption spectroscopy was performed to acquire the necessary experimental data. The obtained data, in addition to the ground $(^{4}\mathrm{I}_{15/2}{\mathrm{Z}}_{1})$ state and exited $(^{4}\mathrm{I}_{13/2}{\mathrm{Y}}_{1})$ state Zeeman and hyperfine structure, were simultaneously fitted in order to refine an existing crystal-field interpretation of the ${\mathrm{Er}}^{3+}$:${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ system. We demonstrate that it is possible to account for the electronic, magnetic, and hyperfine structure of the full $4{f}^{11}$ configuration of ${\mathrm{Er}}^{3+}$:${\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}$ and further, that it is possible to predict both optical polarization behavior and high magnetic field hyperfine structure of transitions in the $1.5\text{\ensuremath{-}}\ensuremath{\mu}\mathrm{m}$ telecommunications band.

DOI
10.1103/physrevb.104.155121

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We report on the development and application of a parametrized crystal-field model for both C1{\mathrm{C}}_{1}C1​ symmetry centers in trivalent erbium-doped Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​. High-resolution Zeeman and temperature dependent absorption spectroscopy was performed to acquire the necessary experimental data. The obtained data, in addition to the ground (4I15/2Z1)(^{4}\mathrm{I}_{15/2}{\mathrm{Z}}_{1})(4I15/2​Z1​) state and exited (4I13/2Y1)(^{4}\mathrm{I}_{13/2}{\mathrm{Y}}_{1})(4I13/2​Y1​) state Zeeman and hyperfine structure, were simultaneously fitted in order to refine an existing crystal-field interpretation of the Er3+{\mathrm{Er}}^{3+}Er3+:Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ system. We demonstrate that it is possible to account for the electronic, magnetic, and hyperfine structure of the full 4f114{f}^{11}4f11 configuration of Er3+{\mathrm{Er}}^{3+}Er3+:Y2SiO5{\mathrm{Y}}_{2}{\mathrm{SiO}}_{5}Y2​SiO5​ and further, that it is possible to predict both optical polarization behavior and high magnetic field hyperfine structure of transitions in the 1.5\ensuremath-\ensuremathμm1.5\text{\ensuremath{-}}\ensuremath{\mu}\mathrm{m}1.5\ensuremath-\ensuremathμm telecommunications band.
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 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.
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.
Rare-earth doped insulators have been widely recognized as excellent candidate materials for optical quantum computing and information processing. This is principally due to a combination of optical coherence times of up to milliseconds and ground-state hyperfine coherence times of seconds exhibited by rare-earth 4𝑓 𝑁 states. A key contender among rare-earth doped materials is Er3+:Y2SiO5, for which homogeneous linewidths as narrow as 50 Hz have been reported, and for which transitions between the ground and first excited states fall within the 1.5 𝜇m telecommunications wavelength band. However, attempts to utilize this material for spin-wave storage have been hampered by the complexity of the excited-state hyperfine structure, which inhibits the necessary theoretical work required to predict the location of zero first-order zeeman transitions. To address this, a novel crystal-field fitting method was developed to allow an accurate analysis of the 𝐶1 point-group symmetry sites of Y2SiO5. This work was complemented with spectral hole-burning spectroscopy, which revealed ground-state hyperfine level storage with a lifetime of 1.6 ± 0.4 seconds for the 4I15/2𝑍1 → 4F9/2𝐷1 transition. This type of storage time is uncharacteristic for erbium without an external magnetic field, since spin-flips of the unpaired electron in nearby Er3+ ions are typically understood to lead to fast hole filling. The development process of the theoretical and experimental tools required to perform the above work enabled several additional investigations. In particular, the novel crystal-field fitting methods were applied to the 𝑆4 site of Ce3+:LiYF4 and to the 𝐶2𝑣 site of Sm3+:Na+/Li+:CaF2/SrF2. These studies consisted of excellent tests for the developed methods yet also amounted to interesting investigations in their own respect. Similarly, the experimental work afforded an opportunity to directly determine the hyperfine splittings of the 5I8𝑍1 → 5F5𝐷1 transition in Ho3+:KY3F10. This was achieved using high-resolution excitation spectroscopy. Furthermore, the experimentally determined hyperfine structure could be accurately reproduced using a crystal field model. Finally, a lifetime measurement of the 6H7/2 state of Sm3+:LiYF4 was conducted. By utilizing an infrared free-electron laser, pico-second pump-probe spectroscopy allowed for a direct measurements of one of the shortest lifetimes of an RE3+ doped insulator reported in the literature to date. This confirmed the previously suggested two-gradient modification required for the energy-gap law at very short time scales.
We performed high-resolution magneto-optical spectroscopy of the hyperfine transitions from 4I15/2^{4}I_{15/2}4I15/2​ to the 4I13/2^{4}I_{13/2}4I13/2​ and 4I9/2^{4}I_{9/2}4I9/2​ multiplets of 167Er3+^{167}\mathrm{Er}^{3+}167Er3+ and 166Er3+^{166}\mathrm{Er}^{3+}166Er3+ in an isotopically purified 7LiYF4^{7}\mathrm{LiYF}_{4}7LiYF4​ crystal in various external magnetic fields up to 0.7 T. The obtained experimental results are interpreted in the framework of the generalized theoretical approach. The derived model successfully explains all the experimentally observed optical hyperfine transitions by using a single set of basic parameters found for the crystal-field interaction, magnetic dipole and electric quadrupole hyperfine interactions, together with Zeeman interactions at different orientations of the external magnetic field. A number of the studied quantum transitions appears to be promising for use in Raman quantum storage at optical telecommunication wavelengths.
Erbium-doped solids are a promising platform for quantum technology due to the Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+ 1.5-\textmu{}m optical transition in the telecom C band that can offer long coherence times. To characterize the intrinsic C2{\mathrm{C}}_{2}C2​ site of Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+ in Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​ for quantum information and photonic signal-processing applications, absorption and site-selective fluorescence spectroscopy were used to assign the Er3+4I15/2\mathrm{E}{\mathrm{r}}^{3+}\phantom{\rule{4pt}{0ex}}^{4}I_{15/2}Er3+4I15/2​$\ensuremath{\leftrightarrow}$4I13/2^{4}I_{13/2}4I13/2​ transitions. The lowest-to-lowest transition occurs at 1535.608 nm and laser absorption determined an inhomogeneous linewidth of 780 MHz in a 0.005%-doped crystal at 3.4 K. Time-resolved fluorescence established an upper limit for the excited-state lifetime of 8.5 ms. Angular-dependent Zeeman absorption was used to determine ground- and excited-state ggg tensors. The C2{\mathrm{C}}_{2}C2​-site ggg tensor components for the ground state are gx=1.60{g}_{x}=1.60gx​=1.60, gy=4.71{g}_{y}=4.71gy​=4.71, and gz=11.93{g}_{z}=11.93gz​=11.93 with a tipping angle of \ensuremath{\alpha} = $2.{06}^{\ensuremath{\circ}}$, whereas for the excited state the components are gx=1.08{g}_{x}=1.08gx​=1.08, gy=4.36{g}_{y}=4.36gy​=4.36, and gz=10.07{g}_{z}=10.07gz​=10.07 with a tipping angle of \ensuremath{\alpha} = $\ensuremath{-}11.{7}^{\ensuremath{\circ}}$. Optical decoherence can be suppressed by the application of a magnetic field parallel to $\ensuremath{\langle}111\ensuremath{\rangle}$ crystal axes where all C2{\mathrm{C}}_{2}C2​ sites become nearly magnetically equivalent with large ggg values so that spin flips of neighboring Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+ ions can be simultaneously suppressed. Using this magnetic field direction, two-pulse photon echoes gave a homogeneous linewidth of 5 kHz for an applied magnetic field of 0.5 T, narrowing and saturating at 2.5 kHz at 3.5 T. Decoherence over intermediate magnetic fields was described by spectral diffusion due to $\mathrm{E}{\mathrm{r}}^{3+}\text{\ensuremath{-}}\mathrm{E}{\mathrm{r}}^{3+}$ magnetic dipole interactions driven by the direct phonon process. With Er3+\mathrm{E}{\mathrm{r}}^{3+}Er3+:Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​ absorption at a convenient telecom laser wavelength and the ability to fabricate waveguides, our study suggests that this is a promising material system for quantum information and spectral hole-burning signal-processing applications.