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physica status solidi (a)

Application of two-photon spectroscopy in the study of trivalent rare-earth ions in crystals

A. G. Makhanek, G. A. Skripko

Published May 16, 1979• 28 citations
Publisher

Abstract

To study the role of stepwise and relaxation processes under effective excitation of anti-Stokes luminescence of rare-earth (RE) ions in crystals the time-shifted pulse method is used. It is shown that direct comparison of measured single- and two-photon luminescence excitation spectra often enables one to make immediate conclusions on the position and classification of electron levels of RE ions. The Tb3+ and Eu3− level structures (crystal CaF2) in the near ultraviolet are considered as an example. The peculiarities connected with the polarization characteristics of the two-photon absorption of radiation by the trivalent RE ions in a crystal matrix are discussed. To obtain the two-photon spectra a frequency-tunable organic dye solution laser (ODSL) is used.

DOI
10.1002/pssa.2210530127

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Abstract Theoretical and experimental investigations are made of two‐photon absorption spectra of trivalent rare‐earth ions in crystals. Effective cross‐sections, selection rules, and relative intensities of the components are found. The most intensive two‐photon transitions are established. Two‐photon excitation spectra of luminescence of Er3+ and Ho3+ ions in CaF2 are obtained and effective excitation cross‐sections are measured using a tunable dye laser (715 to 850 nm). It is shown that the spectra have a peculiar structure which differs considerably from that of the one‐photon absorption spectra. The experimental results agree with theory. It is established that one of the levels in Ho3+ is the level 5G6 rather than 3K7 usually assumed.

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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 ${\mathrm{Pr}}^{3+}$:${\mathrm{Nd}}^{3+}$:${\mathrm{Eu}}^{3+}$ codoped ${\mathrm{Y}}_{2}$Si${\mathrm{O}}_{5}$ and YAl${\mathrm{O}}_{3}$ 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 ${t}_{s}$ 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 ${t}_{s}$ 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.

Physical review. B, Condensed matter•Dec 15, 1996•22 citations
To study the role of stepwise and relaxation processes under effective excitation of anti-Stokes luminescence of rare-earth (RE) ions in crystals the time-shifted pulse method is used. It is shown that direct comparison of measured single- and two-photon luminescence excitation spectra often enables one to make immediate conclusions on the position and classification of electron levels of RE ions. The Tb3+ and Eu3− level structures (crystal CaF2) in the near ultraviolet are considered as an example. The peculiarities connected with the polarization characteristics of the two-photon absorption of radiation by the trivalent RE ions in a crystal matrix are discussed. To obtain the two-photon spectra a frequency-tunable organic dye solution laser (ODSL) is used.
Abstract Theoretical and experimental investigations are made of two‐photon absorption spectra of trivalent rare‐earth ions in crystals. Effective cross‐sections, selection rules, and relative intensities of the components are found. The most intensive two‐photon transitions are established. Two‐photon excitation spectra of luminescence of Er3+ and Ho3+ ions in CaF2 are obtained and effective excitation cross‐sections are measured using a tunable dye laser (715 to 850 nm). It is shown that the spectra have a peculiar structure which differs considerably from that of the one‐photon absorption spectra. The experimental results agree with theory. It is established that one of the levels in Ho3+ is the level 5G6 rather than 3K7 usually assumed.
Abstract Using wave functions which are transformed in irreducible representations of corresponding point groups of symmetry, an analysis is carried out of the tensor structure of resonance cubic susceptibility. Polarization characteristics are found of a four‐photon parametric process in the conditions of two‐photon resonance between the components of fine structure of trivalent rare‐earth ions in crystals. The number of independent and nonzero tensor components of resonance cubic susceptibility is determined and their number is shown to be much smaller than it follows from the general features of the crystal symmetry. The signs of resonance cubic susceptibility are calculated for concrete two‐photon transitions.
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,
Abstract Emission and visible photoluminescence excitation spectra of CaF2:Er (0.5 at %) crystals have been studied under different optical pumping conditions. The results demonstrate that anti-Stokes luminescence of the erbium-doped crystals has higher intensity in the case of pumping of the 4I13/2 metastable state of the dopant. Resonance IR photon wavelengths have been determined for two-photon excitation of visible emission in CaF2:Er. A method has been developed for the optical modulation of anti-Stokes luminescence, which allows the nature of the corresponding electron transitions in emission centers to be identified.
Crystals of the composition Ca1–x Er x F2 + x (0 < x ≤ 0.02) have been grown from the melt by the Bridgman method. The absorption, luminescence excitation, and photoluminescence spectra of this material in the case of the Stokes and anti-Stokes mechanisms of the optical excitation from two radiation sources simultaneously have been analyzed. It has been found that the visible luminescence manifests itself upon sequential absorption of two resonance infrared photons with different energies. This effect is associated with the fact that, in this material, there are metastable states of the excited levels 4 I 11/2 of the Er3+ ions, from which transitions to higher energy levels occur due to the absorption of infrared photons.
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.