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Laser Physics

Intensities of inter-Stark transitions in YAG-Yb3+ crystals

Gagik G. Demirkhanyan

Published Jun 28, 2006• 33 citations
Publisher

Abstract

The line strengths of indirect electric dipole and magnetic dipole transitions between Stark sublevels of the Yb 3+ impurity ion in a YAG crystal are calculated. The intensity’s parameters are determined, and the spectroscopic characteristics of inter-Stark transitions (probabilities of spontaneous transitions and radiative lifetimes of Stark sublevels of excited multiplet, fluorescence branching ratios, transition cross sections, and absorption coefficients) are computed. Quantitative calculations of spectroscopic parameters revealed a quite reasonable agreement with experimental data.

DOI
10.1134/s1054660x0607005x

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The line strengths of indirect electric dipole and magnetic dipole transitions between Stark sublevels of the Yb 3+ impurity ion in a YAG crystal are calculated. The intensity’s parameters are determined, and the spectroscopic characteristics of inter-Stark transitions (probabilities of spontaneous transitions and radiative lifetimes of Stark sublevels of excited multiplet, fluorescence branching ratios, transition cross sections, and absorption coefficients) are computed. Quantitative calculations of spectroscopic parameters revealed a quite reasonable agreement with experimental data.
(Yb:YLF) for the application of laser cooling. Time-dependent fluorescence spectroscopy reveals a temperature dependence of the radiative lifetime which we explain by the Boltzmann distribution of excited ions in the upper Stark levels. The emission cross sections of Yb:YLF from 17 K to 440 K are revised using the temperature-dependent radiative lifetimes from fluorescence spectra. We provide fit equations for the peak values of important transitions as a function of temperature, which is also useful for the design of Yb:YLF laser oscillators and amplifiers operated at cryogenic temperatures. Based on our spectroscopic data, we show the prerequisite crystal purity to achieve laser cooling below liquid nitrogen temperatures.
The spectra of luminescence and magnetic circular polarization of luminescence in the 1 D 2 → 3 F 4 emission band in thulium:yttrium-aluminum garnet Tm3+:YAG (Tm3+:Y3Al5O12) have been investigated at temperatures T = 78 and 293 K, respectively. Based on the analysis of the magnetooptical and optical spectra, the optical transitions between the Stark sublevels of the 3 F 4 and 1 D 2 multiplets in Tm3+:YAG were identified. It is shown that the symmetry and energies of the Stark sublevels of the 3 F 4, 1 D 2, and 3 H 6 multiplets, found experimentally from magnetic and magnetooptical studies, confirm the results of theoretical calculations of the energy spectrum of the rare earth Tm3+ ion in YAG.
The wavefunctions, matrix elements, and probabilities of radiative transitions between Stark sub-levels of atomic multiplets are calculated as a function of the strength of a dc electric field. The general expressions for the wavefunction of a multiplet state in a field obtained by perturbation theory for close-lying levels with the use of completely reduced Green’s function allow one to determine the field dependence of both the dipole-allowed and dipole-forbidden radiation amplitudes. A decomposition of the second-order amplitude for the transition between fine-structure sublevels of two levels of equal parity into irreducible components is obtained. Numerical calculations of the probabilities of radiative transitions between triplet states of helium show the possibility of experimental observation of the emergence and vanishing of Stark lines of radiative transitions in the vicinity of anticrossing fields.
A scheme is proposed for computing the probability of the dipole-forbidden f – f transition at the interaction of the RE 3+ impurity ion with the field of an inhomogeneous exciting radiation. It is shown that in the case under consideration, the prohibition on electric dipole transitions can be repealed without involving the Judd–Ofelt theory of induced electric dipole transitions. The quantitative estimation of the absorption cross-section of YAG:Er 3+ crystal at the wavelength of 1530 nm ( 4 I 15/2 → 4 I 13/2 ) was carried out for the simplest model of the inhomogeneous exciting radiation.
The $^{2}F_{7/2}\ensuremath{\leftrightarrow}^{2}F_{5/2}$ optical transitions of Yb3+\mathrm{Y}{\mathrm{b}}^{3+}Yb3+ doped into Y3Al5O12{\mathrm{Y}}_{3}\mathrm{A}{\mathrm{l}}_{5}{\mathrm{O}}_{12}Y3​Al5​O12​ (YAG) were studied for potential quantum information and photonic signal processing applications. Absorption and fluorescence spectroscopy located the energy levels of the ground 2F7/2^{2}F_{7/2}2F7/2​ and excited 2F5/2^{2}F_{5/2}2F5/2​ manifolds, allowing inconsistencies between previous assignments of crystal field splittings in the literature to be resolved. These measurements reveal an unusually large splitting between the first and second levels in both the ground and excited multiplets, potentially providing for reduced sensitivity to thermally induced decoherence and spin-lattice relaxation. Spectral hole burning through two-level saturation was observed, determining the excited state lifetime to be 860 \ensuremath{\mu}s and resolving ambiguities in previous fluorescence measurements that were caused by the large radiation trapping effects in this material. Optical decoherence measurements using two-pulse photon echoes gave a homogeneous linewidth of 18 kHz for an applied magnetic field of 1 T, narrowing to 5 kHz at 2.5 T. The observed decoherence was described by spectral diffusion attributed to $\mathrm{Y}{\mathrm{b}}^{3+}\mathrm{\ensuremath{-}}\mathrm{Y}{\mathrm{b}}^{3+}$ magnetic dipole interactions. Laser absorption determined an inhomogeneous linewidth of 3.6 GHz for this transition in this 0.05%-doped crystal, which is narrower than for any other rare-earth-ion transition previously studied in the YAG host. The temperature dependence of the transition energy and linewidth of the lowest 2F7/2^{2}F_{7/2}2F7/2​ to lowest 2F5/2^{2}F_{5/2}2F5/2​ transition centered at 968.571 nm measured from 4 K to 300 K was well described by phonon scattering at higher temperatures, with an additional anomalous linear temperature-dependent broadening at temperatures below 80 K. Two magnetically inequivalent subgroups of Yb3+\mathrm{Y}{\mathrm{b}}^{3+}Yb3+ ions were identified when a magnetic field was applied along the $\ensuremath{\langle}111\ensuremath{\rangle}$ axis, as expected for the D2{D}_{2}D2​ sites in the cubic symmetry crystal, with ground and excited state effective ggg-values of gg=3.40{g}_{\mathrm{g}}=3.40gg​=3.40 (3.34) and ge=1.04{g}_{\mathrm{e}}=1.04ge​=1.04 (2.01), respectively. Together with the convenient diode laser wavelength of this transition, our study suggests that Yb3+\mathrm{Y}{\mathrm{b}}^{3+}Yb3+:YAG is a promising material system for spectral hole burning and quantum information applications.
A detailed spectroscopic study of Yb3+:CaF2{\text{Yb}}^{3+}:{\text{CaF}}_{2}Yb3+:CaF2​ is made by using laser selective excitation, low-temperature time-resolved fluorescence, and Raman techniques. Three dominant types of Yb3+{\text{Yb}}^{3+}Yb3+ isolated ion centers are identified at very low (0.03 at. (0.03\text{ }\text{at}\text{.}\text{ }%)(0.03 at.  dopant concentration: two of them with cubic and tetragonal symmetries and the third one not clearly identified but likely of trigonal symmetry. Fluorescence decays strongly differ from one site to another. The overall measured positions of the Stark sublevels of the 2F7/2{^{2}F}_{7/2}2F7/2​ and 2F5/2{^{2}F}_{5/2}2F5/2​ multiplets are satisfactorily explained by the crystal-field calculations. On the other hand, at higher dopant concentrations, only one dominant class of Yb3+{\text{Yb}}^{3+}Yb3+ centers occurs which corresponds to some hexameric cluster in which the Yb3+{\text{Yb}}^{3+}Yb3+ ions site in nearly tetragonal crystal-field environments and whose energy-level positions are discussed and compared with those previously reported in the literature.