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Soviet Journal of Quantum Electronics

Selective excitation of activator centers in condensed media with inhomogeneous spectral line broadening

Evgenii M Dianov, Aleksandr Ya Karasik, Ivan A Shcherbakov

Published May 31, 1977• 5 citations
Publisher

Abstract

Neodymium (Nd 3+ ) ions in mixed yttrofluorite crystals were excited by Y 3 Al 5 O 12 :Nd 3+ laser radiation. Luminescence spectra of these ions were recorded in 5x10 –6 sec after a delay time (relative to a short excitation pulse), which was varied within the range from 3 × 10 –5 to 2 × 10 –3 sec. The spectra recorded during the initial stages of the decay of the 4 F 3/2 metastable state were quite different from the spectra recorded under nonselective excitation conditions. The selectively excited spectra varied with time because of the migration of energy between metastable states but this migration was completed in a time of the order of 10 –3 sec at T = 300°K when the concentration of NdF 3 was 1 wt.%. The results indicated a correlation between the spectra of the energy levels of Nd 3+ in yttrofluorite crystals and structural disorder.

DOI
10.1070/qe1977v007n05abeh012566

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Journal of Applied Physics•Oct 15, 1994•20 citations
Neodymium (Nd 3+ ) ions in mixed yttrofluorite crystals were excited by Y 3 Al 5 O 12 :Nd 3+ laser radiation. Luminescence spectra of these ions were recorded in 5x10 –6 sec after a delay time (relative to a short excitation pulse), which was varied within the range from 3 × 10 –5 to 2 × 10 –3 sec. The spectra recorded during the initial stages of the decay of the 4 F 3/2 metastable state were quite different from the spectra recorded under nonselective excitation conditions. The selectively excited spectra varied with time because of the migration of energy between metastable states but this migration was completed in a time of the order of 10 –3 sec at T = 300°K when the concentration of NdF 3 was 1 wt.%. The results indicated a correlation between the spectra of the energy levels of Nd 3+ in yttrofluorite crystals and structural disorder.
This paper shows that the satellite lines that appear in the absorption and fluorescence spectra of neodymium ions in a LaF3 crystal at concentrations of about 0.5 at.% and the accompanying lines of the isolated ion are caused by pairwise interaction of the Nd3+ ions. Double optical resonance is used to study the structure of the satellite lines in the neighborhood of the 4I9/2→4G5/2 transition of the isolated ion (wavelength 5777.1 Å), hidden by inhomogeneous broadening. When neodymium ion pairs are excited by resonance laser radiation, the presence of anti-Stokes components is recorded in the fluorescence spectrum (up-conversion). It is shown that the main up-conversion mechanism is cumulative pair excitation. These results are convincing evidence that the suppression of absorption from excited levels can be experimentally observed in condensed media.
The time and temperature dependences of the probability of deactivation of the excited state of the Yb 3+ ions in mixed yttrium-ytterbium garnets of various compositions were investigated in the temperature range 1.7–300°K. An analysis indicated that these dependences were governed by the excitation energy migration, which was the "bottleneck" in the process of nonradiative deactivation of the excited state. A strong rise (by more than an order of magnitude) of the migration probability was observed when the temperature was raised from 1.7 to 4.2°K. The diffusion theory, applicable to migration processes in the case of homogeneous broadening of spectral lines, was generalized to inhomogeneous broadening. The theoretical results were in good agreement with the experimental data.
The detailed site-selective and time-resolved fluorescence laser spectroscopy and kinetic measurements with high spectral and nanosecond temporal resolution were applied to analyze the M and N absorption bands at the 4I9/2(1) yields 4G5/2(1) crystal field (CF) transition in the CaF2:Nd3+ crystal at 4.2 K. It was found that at helium temperatures the dynamically split spectral line at the 4I9/2(1) yields 4G5/2(1) CF transition of coherently coupled Nd3+ ions in the pair M- and quartet N-centers is inhomogeneously broadened. Small variation of fluorescence lifetimes of the 4F3/2 and 4D3/2 levels due to small variation of distances between Nd3+ ions in the pairs was found. Approximately 1 percent variation of the Nd-Nd distance in the pair -center was determined form lifetime variation of the 4F3/2 manifold.
The spectral and lasing parameters of Yb 3+ ions in zirconium dioxide crystals with a stabilised cubic structure (fianites) are studied. It is found that the absorption and luminescence spectra of Yb 3+ in these crystals are characterised by a considerable inhomogeneous broadening. The nature of this broadening is investigated and the model of optical centres consistent with the properties of the inhomogeneous spectra of Yb 3+ in the cubic zirconium dioxide crystal is proposed. It is shown that fianites can be used in solid-state lasers. Lasing in Yb 3+ ions in diode-pumped fianite crystals was obtained and studied.
The photoluminescence spectra of Yb-implanted InP samples were studied under pulsed and cw excitations using an Ar+-ion laser (above band-gap excitation) at different temperatures and excitation intensities. The photoluminescence spectrum of the 4f transitions 2F5/2–2F7/2 consists of a sharp peak at 1001 nm and broader peaks in the spectral range between 1002.5 and 1010 nm. Time-resolved spectra were recorded at different temperatures. Using a tunable Ti:sapphire laser (above and below band-gap excitation) the photoluminescence excitation spectra were investigated for different emission lines. Study of the rise and decay time under intrinsic excitation (band to band) show that the rise time is a function of excitation intensity, which reflects an indirect excitation process for Yb3+. The experimental data are explained using a kinetics model of energy transfer from the host lattice to the localized core excited states of rare-earth isoelectronic structured traps. The numerically simulated luminescence rise and decay times show a good general quantitative agreement with experimental data, over a wide range of generation rates. The photoluminescence spectra and decay time were also studied as a function of temperature. A quenching mechanism of ytterbium luminescence involving Yb and Fe ions is proposed. Finally, the electric-field quenching of InP:Yb photoluminescence is investigated.