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Physical review. B, Condensed matter

Homogeneous and inhomogeneous linewidths of Eu 3 + in disordered crystalline systems

Kiwan Jang, Richard S. Meltzer

Published Sep 1, 1995• 30 citations
Publisher

Abstract

The role of disorder on the inhomogeneous and homogeneous linewidths of ${\mathrm{Eu}}^{3+}$ 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}}$${\mathrm{Sc}}_{\mathit{x}}$${\mathrm{O}}_{3}$ (x=0.04,0.3,1) and YSZ (yttria-stabilized zirconia). For the ${\mathrm{Y}}_{2\mathrm{\ensuremath{-}}\mathit{x}}$${\mathrm{Sc}}_{\mathit{x}}$${\mathrm{O}}_{3}$ 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.

DOI
10.1103/physrevb.52.6431

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Conference on Lasers and Electro-Optics•Jan 1, 2000•0 citations
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}}$${\mathrm{Sc}}_{\mathit{x}}$${\mathrm{O}}_{3} (x=0.04,0.3,1) and YSZ (yttria-stabilized zirconia). For the {\mathrm{Y}}_{2\mathrm{\ensuremath{-}}\mathit{x}}$${\mathrm{Sc}}_{\mathit{x}}$${\mathrm{O}}_{3} 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.
Two-pulse photon-echo measurements were made on the 7^{7}7F0{\mathit{F}}_{0}F0​${\mathrm{\ensuremath{\leftrightarrows}}}^{5}$D0{\mathit{D}}_{0}D0​ optical transition in a number of crystalline samples of Y2{\mathrm{Y}}_{2}Y2​O3{\mathrm{O}}_{3}O3​:Eu3+{\mathrm{Eu}}^{3+}Eu3+ prepared by three different crystal-growth techniques. For crystals prepared by a laser-heated pedestal growth or arc-imaging furnace process, we report the observation of an additional sample-dependent contribution to the optical dephasing in comparison with a crystal grown by flame fusion. The dephasing rate 1/Tm{\mathit{T}}_{\mathit{m}}Tm​ at 1.4 K is up to two orders of magnitude faster than that previously reported for the flame-fusion-grown crystal, and is uncorrelated with concentration. Measurements up to 14 K show that 1/Tm{\mathit{T}}_{\mathit{m}}Tm​ increases linearly with temperature, in contrast to the expected T7{\mathit{T}}^{7}T7 behavior due to a two-phonon Raman process. The linear temperature dependence is similar to that seen in glasses and disordered crystalline systems, suggesting the presence of disorder in the samples with more rapid dephasing. The crystals were examined by x-ray diffraction, excitation spectroscopy, and near-field optical microscopy to provide information on the nature of the disorder. The effect of annealing on the crystal dynamics is also investigated.
Homogeneous and inhomogeneous spectral linewidths of the ${(}^{2}{F}_{5/2}{)}_{1}\ensuremath{-}{(}^{2}{F}_{7/2}{)}_{1}$ 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 $(12\ifmmode\pm\else\textpm\fi{}2)\ifmmode\times\else\texttimes\fi{}{T}^{(1.9\ifmmode\pm\else\textpm\fi{}0.1)}\mathrm{MHz}$ 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.
Inhomogeneous and homogeneous linewidth are reported in a Eu3+{}^{3+}3+ doped transparent Y2{}_{2}2​O3{}_{3}3​ ceramic for the 7{}^{7}7F0{}_{0}0​-5{}^{5}5D0{}_{0}0​ transition, using high-resolution coherent spectroscopy. The 8.7-GHz inhomogeneous linewidth is close to that of single crystals, as is the 59-kHz homogeneous linewidth at 3 K (T2{T}_{2}T2​ === 5.4 $\ensuremath{\mu}$s). The homogeneous linewidth exhibits a temperature dependence that is typical of a crystalline environment, and additional dephasing observed in the ceramic is attributed to magnetic impurities or defects introduced during the synthesis process. The absence of Eu3+{}^{3+}3+segregation at the grain boundaries, evidenced through confocal microfluorescence, further indicates that the majority of Eu3+{}^{3+}3+ions in the ceramic experience an environment comparable to a single crystal. The obtained results suggest that ceramic materials can be competitive with single crystals for applications in quantum information and spectral hole burning devices, beyond their current applications in lasers and scintillators.
Optical hole burning is used to study optical dephasing of the 7F0 ⇒ 5D0 transition in samples of Y2O3:Eu3+ grown by both flame fusion and laser-heated pedestal growth. The samples exhibited a wide variation in their low-temperature hole widths, and the measured hole linewidths were in reasonable agreement with homogeneous linewidths obtained from values of T2 that were determined with two-pulse photon echoes. The sample that had the longest value of T2 (510 μs) from the echo measurements gave a hole width of 3.5 kHz. This is believed to be the narrowest spectral feature observed directly in the frequency domain for a solid. Other samples produced wider holes that were not correlated with the Eu3+ impurity concentrations. Time-resolved hole burning in one of the samples showed a slow and continuous broadening of the spectral hole from 130 kHz at 3 ms to 900 kHz at 10 s after hole burning. It is suggested that the additional broadening is associated with some form of disorder modes in this ordered crystalline solid.
A homogeneous linewidth of $85.6\ifmmode\pm\else\textpm\fi{}4.4\text{ }\text{ }\mathrm{kHz}$ is reported in 60 nm Eu3+{\mathrm{Eu}}^{3+}Eu3+ doped Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​ nanocrystals at 1.3 K. This linewidth was measured by two-pulse photon echoes on highly scattering powders using heterodyne detection. Spectral diffusion was also investigated by three-pulse photon echoes and resulted in a limited broadening of the homogenous linewidth of about 250 kHz over $120\text{ }\text{ }\ensuremath{\mu}\mathrm{s}$. Compared to achievable Rabi frequencies, in the range of several MHz, these values show that rare earth doped nanocrystals can be useful for applications in optical quantum information processing.
Summary form only given. Congruent lithium niobate has a disordered, lithium-deficient structure in which Nb/sub Li/ antisites provide charge compensation for lithium vacancies. The disorder is produced by departures from stoichiometry, which play an important role in the photorefractive properties of lithium niobate, particularly two-color photorefractivity at ambient temperatures. Disorder also increases the inhomogeneous linewidth (/spl Gamma//sub inhom/) of optical transitions of impurity centers, which gives a desirable increase in bandwidth for applications involving low temperature spatial-spectral holography where the frequency and time-domain phenomena of spectral hole burning and photon echoes are combined with that of spatial holography. However it also has the potential to increase the homogeneous linewidth (/spl Gamma//sub hom/) by inducing low frequency tunneling modes or "two-level systems" (TLS), reducing the figure of merit for the time-bandwidth product: F=/spl Gamma//sub inhom///spl Gamma//sub hom/. We investigate the role of disorder in lithium niobate by measuring both the inhomogeneous and homogeneous broadening of optical transitions in Pr/sup 3+/ and Er/sup 3+/ doped lithium niobate where the rare-earth ions are generally accepted to substitute for Li/sup +/ ions in sites of nominally C/sub 3/ symmetry.