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Conference on Lasers and Electro-Optics

Inhomogeneous and homogeneous broadening in Pr/sup 3+/- and Er/sup 3+/-doped lithium niobate

R. M. Macfarlane, Y. Sun, Flurin Könz, R. L. Cone

Published Jan 1, 2000• 0 citations
Publisher

Abstract

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.

DOI
10.1109/cleo.2000.907295

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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.
The subgigahertz spectral bandwidth of the lowest energy $1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$ Er3+{\mathrm{Er}}^{3+}Er3+ $^{4}I_{15∕2}\ensuremath{\rightarrow}^{4}I_{13∕2}$ optical transition in Er3+:Y2SiO5{\mathrm{Er}}^{3+}:{\mathrm{Y}}_{2}\mathrm{Si}{\mathrm{O}}_{5}Er3+:Y2​SiO5​ has been increased to $\ensuremath{\sim}22\phantom{\rule{0.3em}{0ex}}\mathrm{GHz}$ by intentionally introducing compositional disorder through codoping with Eu3+{\mathrm{Eu}}^{3+}Eu3+ impurity ions. This illustrates a general bandwidth control technique for spectral hole burning device applications including spatial-spectral holography and quantum computing. Coherence measurements by stimulated photon echoes demonstrated that the increased disorder does not perturb the dynamical properties of the Er3+{\mathrm{Er}}^{3+}Er3+ transition and, thus, gives the desired bandwidth enhancement without penalty in other properties. The echo measurements and model analysis also show that phonon-driven spin flips of Er3+{\mathrm{Er}}^{3+}Er3+ ions in the ground state are responsible for the spectral diffusion that was observed for the optical transition. These results collectively give a better understanding of both the nature of disorder and of the ion-ion interactions in doped materials, and they also enable the high bandwidths required for signal processing and memory applications at $1.5\phantom{\rule{0.3em}{0ex}}\ensuremath{\mu}\mathrm{m}$ based on spectral hole burning.
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.
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.
The nature of inhomogeneous broadening in rare earth systems plays an important role in the dynamical optical properties of ions in crystals. For this reason much of the work on the nature of the inhomogeneous broadening in rare earth doped systems has concentrated on the investigation of ion-ion interactions such as spectral transfer and up conversion processes.1,3 Variations in homogeneous optical dephasing times across the inhomogeneous optical line have also been reported.4 These studies concentrate on the variations of collective effects of ion- ion interactions at different positions in the inhomogeneous optical line in relatively heavily doped rare earth systems. We report variations in optically detected NQR (ODNQR) linewidths and shifts of Pr3+ hyperfme transitions in the optical ground state as a function of position in the inhomogeneous optical line and for satellite transitions of the 1D2-3H4 transition in lightly doped (0.5 at. %) Pr3+:LaF3.
Solids containing rare earth (RE) ions have attracted spectroscopists' attention since the beginning of this century.In the last 30 years, their extremely narrow spectral features in combination with the use of non linear spectroscopy have served to sensitively measure ion-solid interactions and to progressively observe narrower homogeneous linewidths.The potential for using RE ion doped crystals as optical storage materials and processors has lately been a driving force in their investigations, Here, the ratio of inhomogeneous to homogeneous linewidth is regarded as an adequate measure of storage density and can become as big as 10 7 at cryogenic temperatures.Therefore, the analysis of line broadening is of fundamental as well as applied interest.This work is concerned with the investigation of interactions of RE ions with their environment.By means of a laser with a kilohertz resolution and non-linear spectroscopy, spectral dynamics as a function of intrinsic, external electric field, or light-pulse induced perturbations are analyzed on different time scales.In the first part, the theoretical background for the spectroscopy of RE ion doped crystals is outlined.The energy levels are presented and it is shown that due to their electronic properties RE ions have spectrally narrow electronic transitions, sometimes in the sub-kHz regime.The investigations of these narrow spectral features on the seconds to minutes time scale require very stable tunable laser sources.At present, such devices are not commercially available.In the second part, the performance of ahorne built laser system is characterized using persistent spectral holes, The results show that frequency selective materials can be used as powerful tools for the high resolution Vlll Abstract spectral analysis of laser sources.Complementary to that, they give a measure for the long term evolution of the spectral holes for the particular hole burning substance.In the third part, the effect of an external electric field on RE ion doped crystals is investigated.It is shown that for these systems the electric field induced frequency shifts are fully reversible.A general theory of Stark splittings of RE doped crystals is introduced and two methods are presented which allow for the determination of the magnitude and orientation of the electric dipole moment differences with sub-degree accuracy.Finally in the last part, spectral line broadening mechanisms of RE ion doped crystals are discussed and investigated by means of two-pulse photon echoes.Through variation of the experimental parameters, a discrimination between the different contributions is partly achieved and characteristic properties for different dephasing mechanisms are presented.In combination with the measurements from the third part, quantitative predictions of the electric dipole-dipole induced broadening are carried out, which are compared to the experimental results,
We investigated the hole-burning phenomena and homogeneous linewidth in Pr3+{\mathrm{Pr}}^{3+}Pr3+-doped Y2O3{\mathrm{Y}}_{2}{\mathrm{O}}_{3}Y2​O3​-based crystals under the systematic control of disorder in the crystal. When divalent ions are doped into an Y2O3:Pr3+{\mathrm{Y}}_{2}{\mathrm{O}}_{3}{:\mathrm{P}\mathrm{r}}^{3+}Y2​O3​:Pr3+ crystal, holes due to rearrangement of local structure around Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions are burned. The burning curves are successfully analyzed in terms of a distributed tunneling rate model for hole formation. The burning efficiency from this analysis and the homogeneous linewidth become larger as the crystal includes a larger amount of divalent ions. The interaction of Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions with oxygen vacancies is thought to be one of the origins of the hole production and the line broadening. The interaction length between Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions and oxygen vacancies is discussed.