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Physical Review B

Hyperfine interactions in YAB:Ho3+ : A high-resolution spectroscopy investigation

Andrea Baraldi, R. Capelletti, Margherita Mazzera, Nicola Magnani, I. Földvári, Elena Beregi

Published Oct 26, 2007• 43 citations
Publisher

Abstract

High-resolution spectroscopy (as fine as $0.01\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}$) was applied to a $1\phantom{\rule{0.3em}{0ex}}\mathrm{mol}\phantom{\rule{0.2em}{0ex}}%$ holmium-doped single crystal of yttrium aluminum tetraborate with the purpose of studying the hyperfine splitting of ${\mathrm{Ho}}^{3+}$ 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 ${D}_{3}$ symmetry in Ho-occupied sites.

DOI
10.1103/physrevb.76.165130

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High-resolution spectroscopy (as fine as 0.01cm\ensuremath−10.01\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}0.01cm\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≃21300cm\ensuremath−1\ensuremath{\simeq}21\phantom{\rule{0.2em}{0ex}}300\phantom{\rule{0.3em}{0ex}}{\mathrm{cm}}^{\ensuremath{-}1}\ensuremath≃21300cm\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.
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.
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.
High-Resolution Spectroscopy of 173^{173}173Yb+^{+}+ Ions
Compared to other stable isotopes of Yb+\rm{Yb}^+Yb+, 173Yb+^{173}\rm{Yb}^+173Yb+ has a richer hyperfine structure, which leads to more favorable clock transitions, spectroscopic techniques for probing new physics, and more sophisticated quantum computing architectures. However, to date, its electronic spectrum remains poorly characterized. Here, we report on efficient laser cooling, state preparation, and detection of a single trapped 173Yb+^{173}\rm{Yb}^+173Yb+ ion. The previously unobserved 2 ⁣S1/2→2 ⁣D3/2^2\!S_{1/2} \rightarrow {}^2\!D_{3/2}2S1/2​→2D3/2​ electric quadrupole transition at 436 nm is coherently excited, and the isotope shift between 171Yb+^{171}\rm{Yb}^+171Yb+ and 173Yb+^{173}\rm{Yb}^+173Yb+ on this transition is determined with an uncertainty of 1.4 Hz. Using microwave spectroscopy, we resolve the hyperfine structure (HFS) of the 2 ⁣D3/2{}^2\!D_{3/2}2D3/2​ state with a relative uncertainty below 10−810^{-8}10−8. From the HFS measurement data, we infer for 173{}^{173}173Yb a nuclear magnetic octupole moment Ω=−0.062(8) (b×μN)Ω= -0.062(8)\,({\rm b} \times μ_N)Ω=−0.062(8)(b×μN​) with uncertainty reduced by more than 2 orders of magnitude compared to previous studies. The data also allow us to determine hyperfine anomalies for the 2 ⁣S1/2{}^2\!S_{1/2}2S1/2​ and 2 ⁣D3/2{}^2\!D_{3/2}2D3/2​ states.
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.
Most of the experiments related to quantum information applications, involving rare-earth doped inorganic crystals, are performed on yttrium orthosilicate single crystals. The work presented here is motivated by the search of new compounds which can be used in the field of quantum computing and/or quantum storage. Relaxation times and hyperfine structure of the $^{3}H_{4}(0)\ensuremath{\rightarrow}^{1}D_{2}(0)$ transition in 1.4% Pr3+:La2(WO4)3{\mathrm{Pr}}^{3+}:{\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}Pr3+:La2​(WO4​)3​ at 4K4\phantom{\rule{0.3em}{0ex}}\mathrm{K}4K have been measured by photon-echo and spectral-hole-burning techniques. The hyperfine splittings of the ground 3H4(0)^{3}H_{4}(0)3H4​(0) and the excited 1D2(0)^{1}D_{2}(0)1D2​(0) states are $14.9\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $24.6\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$ and $5.0\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, $7.3\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{MHz}$, respectively. An inhomogeneous linewidth of $18.8\ifmmode\pm\else\textpm\fi{}0.1\phantom{\rule{0.3em}{0ex}}\mathrm{GHz}$ was measured. A homogeneous linewidth of $25.3\ifmmode\pm\else\textpm\fi{}2.0\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}$ was obtained with or without an external magnetic field of about 14mT14\phantom{\rule{0.3em}{0ex}}\mathrm{mT}14mT. The fluorescence dynamics of the 1D2^{1}D_{2}1D2​ level obtained by a direct excitation in the $^{3}H_{4}\ensuremath{\rightarrow}^{1}D_{2}$ transition gives a nonexponential decay which indicates energy-transfer processes. This decay can be accurately fitted by the Inokuti-Hirayama model [J. Chem. Phys. 43, 1978 (1965)] with a radiative lifetime of $61\ifmmode\pm\else\textpm\fi{}1\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{s}$ giving a minimal homogeneous linewidth of 2.6kHz2.6\phantom{\rule{0.3em}{0ex}}\mathrm{kHz}2.6kHz. The spectral-hole lifetime due to population redistribution within the ground hyperfine levels is $16\ifmmode\pm\else\textpm\fi{}2\phantom{\rule{0.3em}{0ex}}\mathrm{s}$. The results obtained for the La2(WO4)3{\mathrm{La}}_{2}{(\mathrm{W}{\mathrm{O}}_{4})}_{3}La2​(WO4​)3​ compound make this crystal an interesting host for quantum 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.