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Journal of Physics Condensed Matter

Hyperfine structure of Ho3+levels and electron–phonon coupling in Y PO4single crystals

Margherita Mazzera, R. Capelletti, Andrea Baraldi, E. Buffagni, Nicola Magnani, Marco Bettinelli

Published Apr 18, 2012• 12 citations
Publisher

Abstract

High resolution spectroscopy (the finest being 0.01 cm(-1)) was applied in the 75-25,000 cm(-1) and 9-300 K ranges to a 1 mol% holmium doped Y PO(4) single crystal with two purposes: (1) to study the hyperfine splitting of Ho(3+) energy levels of interest for possible quantum manipulation media and (2) to analyze the electron-phonon interaction. The hyperfine structure was clearly revealed for a high number of lines in a wide wavenumber range (up to ~21,500 cm(-1)) and for a large number of multiplets. Several hyperfine patterns were monitored, differing in the number of components (a maximum of 16 could be easily distinguished in a single beautiful pattern), in their separation, and in their relative statistical weight. These features were all understood in terms of a crystal-field model, whose results are in good agreement with experiments and account for the involved level symmetry, the type of transitions (electric and magnetic dipole allowed), and the contribution of a second-order (pseudoquadrupolar) hyperfine coupling between close levels. The electron-phonon interaction, investigated through the thermally induced line shift, was critically discussed in the framework of single phonon coupling and of two phonon Raman scattering models.

DOI
10.1088/0953-8984/24/20/205501

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High resolution spectroscopy (the finest being 0.01 cm(-1)) was applied in the 75-25,000 cm(-1) and 9-300 K ranges to a 1 mol% holmium doped Y PO(4) single crystal with two purposes: (1) to study the hyperfine splitting of Ho(3+) energy levels of interest for possible quantum manipulation media and (2) to analyze the electron-phonon interaction. The hyperfine structure was clearly revealed for a high number of lines in a wide wavenumber range (up to ~21,500 cm(-1)) and for a large number of multiplets. Several hyperfine patterns were monitored, differing in the number of components (a maximum of 16 could be easily distinguished in a single beautiful pattern), in their separation, and in their relative statistical weight. These features were all understood in terms of a crystal-field model, whose results are in good agreement with experiments and account for the involved level symmetry, the type of transitions (electric and magnetic dipole allowed), and the contribution of a second-order (pseudoquadrupolar) hyperfine coupling between close levels. The electron-phonon interaction, investigated through the thermally induced line shift, was critically discussed in the framework of single phonon coupling and of two phonon Raman scattering models.
High-resolution spectroscopy (as fine as $0.01\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$) was applied to a 1mol1\phantom{\rule{0.3em}{0ex}}\mathrm{mol}\phantom{\rule{0.2em}{0ex}}%1mol holmium-doped single crystal of yttrium aluminum tetraborate with the purpose of studying the hyperfine splitting of Ho3+{\mathrm{Ho}}^{3+}Ho3+ energy levels of interest for possible quantum manipulation media. The hyperfine structure was clearly revealed for a high number of lines in a wide wave number range (up to $\ensuremath{\simeq}21\phantom{\rule{0.2em}{0ex}}300\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$) and for a large number of multiplets. Several different hyperfine patterns were monitored, differing in the number of lines, in their separation, and in their relative statistical weight. These features were all understood by a crystal-field model, whose results are in very good agreement with experiments and account for the involved level symmetry, the type of transitions (electric and magnetic dipole allowed), the possibility of a second-order (pseudoquadrupolar) hyperfine coupling between close levels, and a slight distortion of the local D3{D}_{3}D3​ symmetry in Ho-occupied sites.
Abstract Resolved hyperfine structure and narrow inhomogeneously broadened lines in the optical spectra of a rare-earth-doped crystal are favorable for the implementation of various sensors. Here, a well-resolved hyperfine structure in the photoluminescence spectra of LiYF 4 :Ho single crystals and the anticrossings of hyperfine levels in a magnetic field are demonstrated using a self-made setup based on a Bruker 125HR high-resolution Fourier spectrometer. This is the first observation of the resolved hyperfine structure and anticrossing hyperfine levels in the luminescence spectra of a crystal. The narrowest spectral linewidth is only 0.0022 cm −1 . This fact together with a large value of the magnetic g factor of several crystal-field states creates prerequisites for developing magnetic field sensors, which can be in demand in modern quantum information technology devices operating at low temperatures. Very small random lattice strains characterizing the quality of a crystal can be detected using anticrossing points.
Rare-earth-doped crystals can be attractive materials for quantum information processing, because of the long coherence times that can be expected, in particular, from non-Kramers ions. In this paper, Ho3+-doped yttrium and lutetium vanadate single crystals have been investigated using linear and coherent optical spectroscopy. For Ho3+:YVO4, the crystal-field levels of the I-5(8), F-5, F-5(4) and S-5(2) multiplets have been determined and compared with crystal-field level calculations. This allowed us to unambiguously assign most of the observed transitions, although some results suggest that the site symmetry of the Ho3+ ion could deviate from D-2d. Similar conclusions were reached for Ho3+:LuVO4. Hole burning measurements indicate that the coherence time of the I-5(8)-F-5(5) optical transitions is rather short in both compounds (around 40 ns). Assuming that the coherence is limited by spin interactions, this is accounted for by the high nuclear moment of the nearby vanadium ions, since the large crystal-field level splittings of the I-5(8) and F-5(5) multiplets do not favour a large enhanced nuclear Zeeman effect.
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.
We report on a high-resolution optical and magneto-optical spectroscopy, luminescence, and electron paramagnetic resonance (EPR) studies of yttrium orthophosphate single crystals doped with erbium, which are promising telecom-wavelength materials for applications in quantum electronics and quantum information processing. An observation of the hyperfine structure in optical spectra of 167Er^{167}\mathrm{Er}167Er isotope in Er:YPO4{\mathrm{Er}:\mathrm{YPO}}_{4}Er:YPO4​ is presented. Energies and symmetries of 40 crystal-field levels of Er3+{\mathrm{Er}}^{3+}Er3+ in Er:YPO4{\mathrm{Er}:\mathrm{YPO}}_{4}Er:YPO4​ and ggg factors of some of them were determined and successfully modeled on the basis of crystal-field calculations. The obtained set of crystal-field parameters was used in modeling the hyperfine structure observed in the optical and EPR spectra of Er:YPO4{\mathrm{Er}:\mathrm{YPO}}_{4}Er:YPO4​ single crystals.
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}.