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Proceedings of SPIE, the International Society for Optical Engineering/Proceedings of SPIE

Correlation-induced spectroscopy of rare-earth ions doped in crystals

Hem Chandra Kandpal, K.C. Joshi, J.S. Vaishya

Published Jul 1, 1990• 0 citations
Publisher

Abstract

Auxillary optics used to measure the spectral properties of ions doped in crystal may play a dominant role in causing the shift of the peak frequency of the spectrum emitted by the ions. Therefore consideration has to be to the contribution to this spectral shift due to source correlation in addition to the shift caused by phonon scattering crystal field and tnperature effects etc.

DOI
10.1117/12.34821

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Auxillary optics used to measure the spectral properties of ions doped in crystal may play a dominant role in causing the shift of the peak frequency of the spectrum emitted by the ions. Therefore consideration has to be to the contribution to this spectral shift due to source correlation in addition to the shift caused by phonon scattering crystal field and tnperature effects etc.
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 study the optical properties of rare-earth-ion-doped inorganic crystals with an emphasis on the dependence of two-pulse photon echoes on the excitation density in the system. The experimental investigations concentrate on Pr3+{\mathrm{Pr}}^{3+}Pr3+:Nd3+{\mathrm{Nd}}^{3+}Nd3+:Eu3+{\mathrm{Eu}}^{3+}Eu3+ codoped Y2{\mathrm{Y}}_{2}Y2​SiO5{\mathrm{O}}_{5}O5​ and YAlO3{\mathrm{O}}_{3}O3​ crystals at low temperatures. With two pulses of one laser the echo is induced in one ion species and with a third, "scrambler" pulse of a second laser another species is excited. These scrambler excitations lead to a dephasing and thus to an echo attenuation which depends on the strength, frequency, and time of the scrambler pulse. The spectral sensitivity of the echo attenuation is used for a spectroscopic technique: "photon-echo attenuation spectroscopy." As a function of the delay time ts{t}_{s}ts​ between the scrambler pulse and the onset of the two-pulse echo sequence the attenuation shows a very specific behavior dictated by the excitation-induced frequency shifts (EFS's). For ts{t}_{s}ts​ between the two echo-inducing pulses the echo intensity is partially regained by the "dephasing-rephasing balancing" of the reversible EFS's. For the theoretical description a stochastic model is introduced and the dephasing by excitation-induced lattice vibrations and by EFS's are analyzed in detail. The present results are discussed in the light of previous experimental and theoretical investigations.