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

Inhomogeneous broadening of the dynamically split Kramers spectral line and up-conversion in the pair and quartet centers in CaF 2 :Nd3+

Yu.V. Orlovskii, Tasoltan T. Basiev, A.G. Papashvili, Ivan N. Vorob'ev, Olimkhon K. Alimov, Vyacheslav V Osiko, Johann Heber

Published Jul 12, 2002• 0 citations
Publisher

Abstract

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.

DOI
10.1117/12.475335

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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.
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.
Accumulated photon echoes have been used to investigate the mechanisms of optical dephasing in CaF2 crystals activated by Nd3+ ions. Tunable picosecond laser radiation, which permits the selective excitation of various Nd3+ optical centers in the 4 I 9/2→4 G 5/2, 2 G 7/2 transition, is used. The optical phase relaxation times measured at temperatures from 9 to 50 K permit determination of the homogeneous widths of the transitions between the low-lying 4 I 9/2 Stark level and three excited 4 G 5/2, 2 G 7/2 levels, and calculation of the constants of the inter-Stark relaxation transitions in the ground and excited multiplets for the rhombic N and M Nd3+ centers in CaF2 crystals. An analysis of the temperature dependence of the homogeneous linewidth of the transitions between low-lying Stark levels of the ground and excited states shows that the mechanism of optical dephasing in the crystals investigated is described well by direct relaxation processes with resonant inter-Stark absorption of one phonon in the ground and excited states. At T=9 K, the homogeneous linewidth Γh in CaF2 crystals is almost an order of magnitude smaller than Γh in disordered CaF2-YF3 crystals. This difference can be attributed to the significantly greater spectral phonon density of states in disordered crystals.
The temporal dependence of the fluorescence line shape of Pr ion diluted in LaF3{\mathrm{F}}_{3}F3​ has been studied in detail. The line-shape study is based on the assumption that the cross relaxation between Pr ions dominates the nonradiative process. The ion-ion interaction has been directly probed by the two-ion cooperative absorption process under which a 3P0^{3}P_{0}3P0​ level lifetime dilation has been observed. The dilation effect can be suppressed when the spectral energy transfer is switched on by raising the temperature of the host crystal. The temporal behavior of the fluorescence line shape of the 1D2^{1}D_{2}1D2​ level has been systematically investigated. The "inhomogeneous" linewidth is found to be composed of a main central peak and a series of ion-pair satellites. The shorter decay lifetime of the ion-pair states results in the narrowing of the emission line shape at later times. The energy positions of the ion-pair states have been measured from the 1D2^{1}D_{2}1D2​ ion pairs up-conversion fluorescence process. The lifetime of the ion-pair states is determined by the coupling strength of the cross relaxation from an excited ion to its partner ion and hence varies according to the ion-pair separation. The decay under the inhomogeneous width is nonexponential in general. Based on the number of the distinguished ion pair levels, a concept of the sphere of influence is introduced. Following this model, an approach has been developed which allows us to study the decay characteristics. Systematical trends emerge from such analysis. The cross-relaxation coupling constants for ion pairs have been extracted from the decay curves and profiles of the ion-pairs line shape have been mapped out. Their peak positions agree with those obtained from 1D2^{1}D_{2}1D2​ ion-pair up-conversion fluorescence measurements.
By measuring the absorption and fluorescence spectra and the fluorescence lifetime of ^{4}F_{3/2} state of Nd^{3+} ions in YVO_{4} (2 at.-{\%}) crystal at different temperature, the effects of temperature on the spectra and the lifetime of ^{4}F_{3/2} state have been investigated. As the temperature is increased, the line width of the ^{4}F_{3/2}-->^4I_{11/2} transitions is found to increase and the spectral line toward the longer wavelength, which are duo to the ion-phonon interaction. The variation fluorescence lifetime of the ^{4}F_{3/2} state of Nd:YVO_{4} is found to be anomalous in the measured range 8-300 K. It is about 81 us at room temperature and decreases to 30 us at 8 K. The experimental results are explained by ascribing to the thermal mixing between the two Stark levels of ^{4}F_{3/2} state with different lifetime.
We have observed extremely fast nonradiative relaxation (picosecond to femtosecond) between closely spaced crystal field states derived from the 4G5/2,2G7/2 Stark manifold of Nd3+ in glassy media. The relaxation is significantly faster than that predicted by an indiscriminate application of the energy-gap law, and it is highly wavelength-dependent. Femtosecond accumulated-photon-echo techniques were used at 13 K, revealing single and nonexponential echo decays. Relaxation was found to involve single phonon processes. Generally, the dephasing rate increased as higher-lying crystal field states were excited, reflecting the larger number of available terminal levels for the relaxation and the phonon density of states. However, a detailed plot of the dephasing rate versus wavelength revealed considerable unexpected structure. As higher-lying states were excited, the relaxation rate did not increase in the expected monotonic fashion. Surprisingly, the relaxation rate decreased in various spectral regions as the excitation energy was increased. By using T2-selective dynamic-excitation spectroscopy, we assigned these regions to the spectral locations of the inhomogeneously broadened crystal field states in the Stark manifold. Site-dependent electron-phonon interaction and a strong correlation between the inhomogeneous broadening of the crystal field states are deduced from the data.