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Physical review. B, Condensed matter

Determination of spectral linewidths by Voigt profiles in Yb3+ -doped fluorozirconate glasses

Gang Lei, J. E. Anderson, M. I. Buchwald, B. C. Edwards, Richard I. Epstein

Published Apr 1, 1998• 55 citations
Publisher

Abstract

Homogeneous and inhomogeneous spectral linewidths of the ${(}^{2}{F}_{5/2}{)}_{1}\ensuremath{-}{(}^{2}{F}_{7/2}{)}_{1}$ transition in ${\mathrm{Yb}}^{3+}$-doped fluorozirconate glasses are determined by fitting Voigt profiles to the inhomogeneously broadened emission and absorption spectra between 10 and 300 K. The homogeneous linewidth varied as $(12\ifmmode\pm\else\textpm\fi{}2)\ifmmode\times\else\texttimes\fi{}{T}^{(1.9\ifmmode\pm\else\textpm\fi{}0.1)}\mathrm{MHz}$ for emission and $(10\ifmmode\pm\else\textpm\fi{}1)\ifmmode\times\else\texttimes\fi{}{T}^{1.9\ifmmode\pm\else\textpm\fi{}0.1}$ for absorption over the entire temperature range, similar to that of other rare-earth-doped systems previously studied by fluorescence line narrowing and photon echoes. The inhomogeneous linewidths were nearly independent of temperature, but different by $\ensuremath{\sim}30%$ between emission and absorption. The structural and dynamic properties in this disordered system are discussed.

DOI
10.1103/physrevb.57.7673

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Homogeneous and inhomogeneous spectral linewidths of the (2F5/2)1\ensuremath−(2F7/2)1{(}^{2}{F}_{5/2}{)}_{1}\ensuremath{-}{(}^{2}{F}_{7/2}{)}_{1}(2F5/2​)1​\ensuremath−(2F7/2​)1​ transition in Yb3+{\mathrm{Yb}}^{3+}Yb3+-doped fluorozirconate glasses are determined by fitting Voigt profiles to the inhomogeneously broadened emission and absorption spectra between 10 and 300 K. The homogeneous linewidth varied as (12\ifmmode±\else\textpm\fi2)\ifmmode×\else\texttimes\fiT(1.9\ifmmode±\else\textpm\fi0.1)MHz(12\ifmmode\pm\else\textpm\fi{}2)\ifmmode\times\else\texttimes\fi{}{T}^{(1.9\ifmmode\pm\else\textpm\fi{}0.1)}\mathrm{MHz}(12\ifmmode±\else\textpm\fi2)\ifmmode×\else\texttimes\fiT(1.9\ifmmode±\else\textpm\fi0.1)MHz for emission and (10\ifmmode±\else\textpm\fi1)\ifmmode×\else\texttimes\fiT1.9\ifmmode±\else\textpm\fi0.1(10\ifmmode\pm\else\textpm\fi{}1)\ifmmode\times\else\texttimes\fi{}{T}^{1.9\ifmmode\pm\else\textpm\fi{}0.1}(10\ifmmode±\else\textpm\fi1)\ifmmode×\else\texttimes\fiT1.9\ifmmode±\else\textpm\fi0.1 for absorption over the entire temperature range, similar to that of other rare-earth-doped systems previously studied by fluorescence line narrowing and photon echoes. The inhomogeneous linewidths were nearly independent of temperature, but different by \ensuremath∼30\ensuremath{\sim}30%\ensuremath∼30 between emission and absorption. The structural and dynamic properties in this disordered system are discussed.
We have measured the homogeneous linewidth of the 2F5/2^{2}\mathrm{F}_{5/2}2F5/2​(1)${\mathrm{\ensuremath{-}}}^{2}$F7/2{\mathrm{F}}_{7/2}F7/2​(1) transition of Yb3+{\mathrm{Yb}}^{3+}Yb3+ in silicate and phosphate glasses using fluorescence line narrowing between 6.5 and 70 K. The linewidth is observed to vary as ${T}^{1.9\ifmmode\pm\else\textpm\fi{}0.1}$ at high temperature, changing to ${T}^{1.3\ifmmode\pm\else\textpm\fi{}0.1}$ below 40 K. This behavior is compared to that observed in other systems and examined in light of current theories of dephasing in disordered systems.
Resonance-fluorescence-line-narrowing studies have been performed on a representative group of Er3+ -doped glasses for excitation in both the 1530 and 980-nm bands at 4.2, 77, 200, and 300 K. Fluorozirconate, fluorophosphate, phosphate, silicate, Ge/P-doped and A1/P-doped silica preforms, and Al/P-doped and Ge-doped fibers were examined. At 77 K the homogeneous linewidths were found to be relatively insensitive to composition. In particular, they vary from 1.4 to 1.8 cm-1 for the different hosts using excitation at 1531 nm. At 300 K weak resonant features were observed in most samples, consistent with a small inhomogeneous contribution to a predominantly homogeneous fluorescence emission.
The role of disorder on the inhomogeneous and homogeneous linewidths of Eu3+{\mathrm{Eu}}^{3+}Eu3+ in single crystals with various degrees of disorder is described for samples grown by LHPG (laser-heated pedestal growth). Emission spectra, hole-burning spectra, and results of the two-pulse photon echo are reported for ${\mathrm{Y}}_{2\mathrm{\ensuremath{-}}\mathit{x}}$Scx{\mathrm{Sc}}_{\mathit{x}}Scx​O3{\mathrm{O}}_{3}O3​ (x=0.04,0.3,1) and YSZ (yttria-stabilized zirconia). For the ${\mathrm{Y}}_{2\mathrm{\ensuremath{-}}\mathit{x}}$Scx{\mathrm{Sc}}_{\mathit{x}}Scx​O3{\mathrm{O}}_{3}O3​ system, the inhomogeneous linewidths increase with x while the homogeneous linewidths are nearly independent of x. Dynamics associated with low-frequency excitations observed previously in x=0 LHPG samples are nearly absent for x>0. However, both the static and dynamic properties of YSZ show behavior which is characteristic of amorphous systems like silicate glass.
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.
The relation between absorption and emission spectra in a rare-earth doped solid is explored analytically and through numerical simulations on a model system. It is found that the widely used theory of McCumber [D. E. McCumber, Phys. Rev. 136, A954 (1964)] is strictly valid only when the linewidth of each individual transition between Stark levels is ≪kBT. When this assumption is relaxed, deviations between actual simulated spectra and McCumber-calculated spectra are found for both homogeneous and inhomogeneous broadening. The McCumber transform introduces a characteristic distortion of each component transition, in which the low-energy side of the spectrum is increased, and the high-energy side is decreased. The average degree of distortion for the model system is calculated to be 5% for a homogeneous width of 50 cm−1 at room temperature, but only 1% for a purely inhomogeneous width of 50 cm−1. For both homogeneous and inhomogeneous spectra, the distortion varies with the linewidth Δν as (Δν)3/2. The dependence of the distortion on temperature is different for the two types of line shapes, however: ∼T2 for homogeneous and ∼T−1 for inhomogeneous broadening. For most rare-earth doped glasses and crystals at room temperature, the average degree of distortion is expected to be on the order of 5% or less, although the actual discrepancy in the spectral wings can be much larger. The effects described here are likely to be of importance when using McCumber’s theory to obtain accurate cross section values in the spectral wings of rare-earth transitions.
We show that rare-earth (RE-) doped glasses can have homogeneous linewidths as narrow as 287 kHz at (4)He temperatures. This is far narrower than others reported in glasses in the same temperature range and is suitable for precise spectral hole burning and spatial-spectral holographic applications. It is known that cw spectral hole burning linewidth measurements of RE ions in glasses are hindered by the presence of spectral diffusion but, even in glasses, application of a magnetic field can freeze out RE spin-spin interactions responsible for spectral diffusion and isolate the remaining contribution of two-level systems (TLSs). The Er(3+):2G2S glasses have unusually low TLS contributions, making it possible to study the real homogeneous linewidth using photon echo measurements. The contribution from TLSs is only 170 T(1.3) kHz when subjected to a field of 5 T.