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Journal of the Optical Society of America

Thermal Shifts in the Energy Levels of LaF_3:Nd^3+*

Steve A. Johnson, H. G. Freie, ARTHUR L. SCHAWLOW, William M. Yen

Published Jun 1, 1967• 53 citations
Publisher

Abstract

We have measured the temperature dependence of the linewidths and positions for a number of transitions in the spectrum of LaF3:Nd3+. As the temperature increases, all lines broaden because of relaxation and Raman scattering of phonons. Relative to the ground state, all observed levels shift to lower energies as the temperature increases. Most lines show the usual shifts to the red. All these effects are qualitatively attributable to lattice vibrations. In general, the level shifts increase for the higher levels so that, ordinarily, line shifts are to the red with increasing temperatures. However, because of irregularities of the magnitudes of the level shifts, a few lines show shifts to the blue with increasing temperature, over some temperature ranges.

DOI
10.1364/josa.57.000734

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Le Journal de Physique Colloques•Oct 1, 1985•0 citations
We have measured the temperature dependence of the linewidths and positions for a number of transitions in the spectrum of LaF3:Nd3+. As the temperature increases, all lines broaden because of relaxation and Raman scattering of phonons. Relative to the ground state, all observed levels shift to lower energies as the temperature increases. Most lines show the usual shifts to the red. All these effects are qualitatively attributable to lattice vibrations. In general, the level shifts increase for the higher levels so that, ordinarily, line shifts are to the red with increasing temperatures. However, because of irregularities of the magnitudes of the level shifts, a few lines show shifts to the blue with increasing temperature, over some temperature ranges.
Temperature dependences of backward photon echo intensity have been measured from 5°K to 13°K on the 3P0–3H4 (4778 Å) and 1D2–3H4 (5925 Å) transitions of LaF3:Pr3+. Over six orders of magnitude (on the 3P0–3H4 transition) and three orders of magnitude (on the 1D2–3H4 transition) of the photon echo intensity, the experimental results are explained by the one-phonon process (the direct process) taking into account the energy differences between the echo levels and their adjacent levels. Preliminary measurements have also been made on the 4G7/2–4I9/2 (5221 Å) and 4G5/2–4I9/2 (5775 Å) transitions of LaF3:Nd3+.
Phonon-ion interactions have recently been shown to satisfactorily explain the temperature dependence of widths and positions of the RRR lines of some 3d3d3d ions in crystals. These interactions give rise to phonon relaxation processes and are investigated here as the mechanisms responsible for the widths and positions of sharp optical transitions in (4f4f4f) ions, in particular LaF3{\mathrm{F}}_{3}F3​: Pr3+{\mathrm{Pr}}^{3+}Pr3+. The widths of transitions originating or terminating in the metastable 3P0^{3}P_{0}3P0​ state and involving the 3H4^{3}H_{4}3H4​, 3H6^{3}H_{6}3H6​, 3F2^{3}F_{2}3F2​, and 3F4^{3}F_{4}3F4​ states of Pr3+{\mathrm{Pr}}^{3+}Pr3+ in LaF3{\mathrm{F}}_{3}F3​ have been investigated as a function of temperature and are found to be both qualitatively and quantitatively explainable in terms of lifetime broadening of the interacting states via nonradiative processes. Temperature-dependent shifts have also been measured for the above four groups of transitions and are shown to be in qualitative agreement with theoretical predictions. Additional features of the LaF3{\mathrm{F}}_{3}F3​: Pr3+{\mathrm{Pr}}^{3+}Pr3+ spectrum, including several unreported weak transitions and vibrational sidebands, are also reported.
We report nuclear quadrupole resonance (NQR) frequency and linewidth variations of the Pr3+ ground-state hyperfine levels for various positions within the 3H4(Γ1)–1D2(Γ1) inhomogeneous optical line and satellite transitions of Pr3+:LaF3. A linear increase in the broadening of the Pr3+ hyperfine transitions, without a shift of central frequency, is measured by the Stark modulated optical pumping hole-burning technique as the laser is tuned toward the wings of the inhomogeneous optical transition. The linear variation is attributed to electric quadrupole broadening caused by changes in the local density of point defects across the Stark-broadened optical transition. The optically detected NQR spectra of the satellite transitions associated with Pr ion pairs are shifted in frequency and for most satellites are narrower than the NQR spectra found in the wings of the main inhomogeneous optical line.
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.
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.