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Journal of the Optical Society of America

Some Studies of Relaxation Processes in Tb^3+ Using Pulsed Excitation

GEORGE E. PETERSON, Paul M. Bridenbaugh

Published Oct 1, 1963• 57 citations
Publisher

Abstract

In this paper the relaxation paths of Tb3+ in two hosts, SrMoO4 and Na0.5Eu0.5WO4, are studied using pulsed and continuous illumination. In the molybdate structure we find that resonance coupling between the host lattice and the rare earths strongly influences the energy levels excited. The doping of Na0.5Eu0.5WO4 with Tb results in a rare-earth-ion–rare-earth-ion resonance-coupled system in which the Eu may be excited by pumping the Tb.

DOI
10.1364/josa.53.001129

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Physical Review Letters•Feb 16, 1998•23 citations
In this paper the relaxation paths of Tb3+ in two hosts, SrMoO4 and Na0.5Eu0.5WO4, are studied using pulsed and continuous illumination. In the molybdate structure we find that resonance coupling between the host lattice and the rare earths strongly influences the energy levels excited. The doping of Na0.5Eu0.5WO4 with Tb results in a rare-earth-ion–rare-earth-ion resonance-coupled system in which the Eu may be excited by pumping the Tb.
Narrow line optical absorption and emission spectra have been observed in Nd3+- and Er3+-doped In2S3, CdIn2S4, and ZnIn2S4. All three spectra show essentially the same structure, and this indicates that the rare-earth ions occupy the same type of environment in the three lattices. The sites most probably have octohedral symmetry, since electron spin resonance results show that the site for CdIn2S4is octohedral. Fluorescence has been observed from all the Er3+- levels almost up to the host lattice band-gap energy above the ions ground state, under both X-ray and ultraviolet excitation. This fluorescence shows the same dependance on rare-earth concentration, method of excitation, and intensity for all three doped host lattices, provided the emission frequency is well removed from the band-gap frequency. The temperature dependance of the fluorescence, however, increases as the emission frequency approaches the host lattice band-gap frequency, and this indicates that a relationship may exist between the extent of the temperature dependance and the magnitude of the band-gap frequency.
Eu-doped yttrium orthosilicate (Eu(3+) : Y2SiO5) had been a subject being investigated for coherent time-domain optical memory and information processing applications since its ultraslow optical dephasing was discovered several years ago. In this crystal the weakly allowed (7)F0 - (5)D0 transition of europium ions exhibits a sufficient long dephasing time and no spectral difli.usion on a time scale of several hours at low temperature, thus an information pattern or data can be stored as a population grating in the ground state hyperfine levels. On the other hand, the study on photon-echo relaxation shows that the dephasing time T2 of Eu (3+) and other rare-earth ions doped YAG, YAlO3 strongly depends on the intensity of the excitation pulses. In Eu (3+) :YAlO3, an exponential decay of photon-echo with T2 = 53 microseconds if the excitation pulses are weak (5 vJ/pulse) was observed. However, when the excitation pulses are strong (80 pJ/pulse) they observed a much shortened T2 with a highly nonexponential decay pattern. The conclusion they derived is that the intensity-dependent dephasing rate effects are quite general, and it depends on how much the excitation intensity varies. In this paper we use transient grating formation technique showing that a temporal lattice distortion may only occur along crystal c axis, caused by EU (3+) excitation. At high excitation level the produced exciton in conduction band may also couple to the dynamical lattice relaxation process, giving rise to an apparently much shortened dephasing time.
We describe a general numerical method for calculating short-pulse laser propagation in rare-earth-doped materials, which are very important as gain materials for solid-state lasers, fiber lasers and optical amplifiers. The split-step, finite difference method simultaneously calculates changes in the laser pulse as it propagates through the material and calculates the dynamic populations of the rare-earth energy levels at any position within the material and for times during and after the laser pulse has passed through the material. Many traditional theoretical and numerical analyses of laser pulse propagation involve approximations and assumptions that limit their applicability to a narrow range of problems. Our numerical method, however, is more comprehensive and includes the processes of single- and multi-photon absorption, excited state absorption (ESA), energy transfer, upconversion, stimulated emission, cross relaxation, radiative relaxation and non-radiative relaxation. In the models, the rare-earth dopants can have an arbitrary number of energy levels. We are able to calculate the electron population density of every electronic level as a function of, for example, pulse energy, dopant concentration and sample thickness. We compare our theoretical results to published experimental results for rare-earth ions such as Er3+, Yb3+, Tm3+ and Ho3+.
Photon-echo-relaxation measurements made on the 3H4^{3}\mathrm{H}_{4}3H4​${\mathrm{\ensuremath{-}}}^{3}$P0{\mathrm{P}}_{0}P0​ transition of 0.01 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG (where YAG represents yttrium aluminum garnet), 3H4^{3}\mathrm{H}_{4}3H4​${\mathrm{\ensuremath{-}}}^{1}$D2{\mathrm{D}}_{2}D2​ transition in 0.1 at. % Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​, and 7F0^{7}\mathrm{F}_{0}7F0​${\mathrm{\ensuremath{-}}}^{5}$D0{\mathrm{D}}_{0}D0​ transition in 0.25 at. % Eu3+{\mathrm{Eu}}^{3+}Eu3+:YAlO3{\mathrm{YAlO}}_{3}YAlO3​ show that the photon-echo relaxation rate increases when the intensities of the excitation pulses are increased. Although a part of the relaxation-rate increase in Pr3+{\mathrm{Pr}}^{3+}Pr3+:YAG may be attributed to an instantaneous spectral diffusion (ISD) in which the presence of excited neighboring Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions change the local field and the absorption frequency of the rare-earth ions, our data deviate significantly from the ISD-model predictions. An additional intensity-dependent relaxation mechanism is required to explain the results.
Excited-state absorption spectra of erbium and thulium doped gallium lanthanum sulfide glasses reveal transitions whose final 4f4f4f states do not appear in the ground state absorption spectra due to resonance with the fundamental absorption of the glass host. The results give direct evidence for the model of isolated rare-earth ions with highly shielded 4f4f4f levels showing no noticeable interaction with the host material despite resonance. Only the energy splitting of the 4f4f4f levels is relevant for energy transfer processes between rare-earth ions and the host material, whereas the absolute energetic position is unimportant.