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Journal of Optical Technology

Resonance laser spectroscopy of ion pairs in a Nd^3+: LaF_3 crystal

Ахмеджанов Ринат Абдулхаевич, A. A. Bondartsev, Л. А. Гущин, V. V. Chernov

Published May 31, 2011• 1 citation
Publisher

Abstract

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.

DOI
10.1364/jot.78.000346

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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.
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.
Using the energy level shift induced by a Nd3+ ion on a neighbour ion, the selective excitation of a class of (Nd, Nd) pairs is possible in weakly doped samples with a spectrally narrow laser. The observation of an anti-Stokes fluorescence shows that a pair can absorb two photons. From experiments with a magnetic field, it is shown that using a single laser, the double excitation of moderatly coupled pairs is essentially induced by a double quantum process by which two photons are simultaneously absorbed. The strongly coupled pairs, on the contrary, can only be doubly excited by two lasers of different frequencies. Orders of magnitude of the coupling strength between the two ions are deduced from the difference between these frequencies.
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 nature of inhomogeneous broadening in rare earth systems plays an important role in the dynamical optical properties of ions in crystals. For this reason much of the work on the nature of the inhomogeneous broadening in rare earth doped systems has concentrated on the investigation of ion-ion interactions such as spectral transfer and up conversion processes.1,3 Variations in homogeneous optical dephasing times across the inhomogeneous optical line have also been reported.4 These studies concentrate on the variations of collective effects of ion- ion interactions at different positions in the inhomogeneous optical line in relatively heavily doped rare earth systems. We report variations in optically detected NQR (ODNQR) linewidths and shifts of Pr3+ hyperfme transitions in the optical ground state as a function of position in the inhomogeneous optical line and for satellite transitions of the 1D2-3H4 transition in lightly doped (0.5 at. %) Pr3+:LaF3.
Anti-Stokes fluorescence from the 3 P 0 level of impurity ions was detected in Pr 3+ : Y 2 SiO 5 , Pr 3+ : Lu 2 SiO 5 , and Pr 3+ : Gd 2 SiO 5 crystals non-resonantly pumped by laser radiation with a certain power density. The integrated intensity of the anti-Stokes fluorescence depends nonlinearly on the pump power density. As the atomic concentration of impurity ions was increased from 0.3% to 0.6% and 1.8%, the anti-Stokes fluorescence intensity was saturated due to the concentration quenching of the 1 D 2 term of the impurity Pr 3+ ions. The anti-Stokes fluorescence and quenching of the 1 D 2 term occur due to the cross relaxation of the electronic energy of excited terms of the Pr 3+ ions.
Laser-induced fluorescence line narrowing has been observed for the first time in a nonresonantly excited rare-earth system. Excitation with the 4727-\AA{} A+{A}^{+}A+ line into the 4G112^{4}G_{\frac{11}{2}}4G211​​ level of Nd3+{\mathrm{Nd}}^{3+}Nd3+ in glass results in narrowing of transitions from the 4F32^{4}F_{\frac{3}{2}}4F23​​ to both the 4I92^{4}I_{\frac{9}{2}}4I29​​ ground manifold and the 4I112^{4}I_{\frac{11}{2}}4I211​​ excited manifold. The concentration dependence of the line narrowing provides information regarding resonant ion-ion energy transfer within the inhomogeneously broadened system.