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Physical Review Letters

Observation of Laser-Induced Fluorescence Line Narrowing in Glass: Nd

L. A. Riseberg

Published Mar 27, 1972• 50 citations
Publisher

Abstract

Laser-induced fluorescence line narrowing has been observed for the first time in a nonresonantly excited rare-earth system. Excitation with the 4727-\AA{} ${A}^{+}$ line into the $^{4}G_{\frac{11}{2}}$ level of ${\mathrm{Nd}}^{3+}$ in glass results in narrowing of transitions from the $^{4}F_{\frac{3}{2}}$ to both the $^{4}I_{\frac{9}{2}}$ ground manifold and the $^{4}I_{\frac{11}{2}}$ excited manifold. The concentration dependence of the line narrowing provides information regarding resonant ion-ion energy transfer within the inhomogeneously broadened system.

DOI
10.1103/physrevlett.28.786

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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.
Fluorescence-line-narrowing and time-resolved studies have been conducted in ruby crystals and powders, in concentrations varying from 0.025 to 0.9 at.%. The resonance fluorescence component of the R1{R}_{1}R1​ line at low temperatures is observed to increase dramatically as the laser is tuned from line center toward the low-energy wing of the inhomogeneously broadened absorption. This is presumed to indicate the presence of weakly coupled pairs in the wings of the line. Intraline and interline (${R}_{1}\ensuremath{\rightarrow}{N}_{1,2}$) energy transfer have also been studied, and an elaboration of earlier work is given. Time-resolved selective-excitation scans have revealed numerous channels in the vicinity of the RRR lines by which the different pairs can be directly excited. These are assumed to be Cr ions near enough to a pair to be in a highly perturbed environment. Various experimental results are shown to be consistent with a model of rapid transfer between resonant Cr ions which feeds the pairs via a weak, nonresonant coupling to these perturbed ions. Macroscopic strain broadening is also shown to be favored over microscopic broadening, and the implications for Anderson localization in ruby are discussed.
Using resonance ruby-laser excitation, narrowing of the ruby R1{R}_{1}R1​ fluorescence line to width 0.002 ${\mathrm{cm}}^{\ensuremath{-}1}$ at 4.2\ifmmode^\circ\else\textdegree\fi{}K is observed. Absence of spectral diffusion indicates that a short-range interaction rather than earlier postulated multipolar interactions is responsible for energy transfer in concentrated ruby.
We have used time-resolved fluorescence line narrowing to study energy transfer among Yb3+{\mathrm{Yb}}^{3+}Yb3+ ions in a silicate glass as a function of energy mismatch between donors and acceptors and temperature from 4.2 to 51 K. The observed spectra are consistent with a one-phonon-assisted multipolar interaction between Yb3+{\mathrm{Yb}}^{3+}Yb3+ ions with a variation with site separation of ${r}^{\mathrm{\ensuremath{-}}13}$. These results are compared to that reported for other rare-earth-ion transitions in glasses and crystals.
We outline the results of an analysis of fluorescence line narrowing1 in dilute systems. We assume that a fraction, p, of the sites on a d-dimensional lattice are occupied at random by optically active ions and that the transfer of optical excitation can only take place between ions occupying nearest-neighbor sites. The normalized intensity of the sharp line fluorescence following excitation of an inhomogeneously broadened line by a monochromatic source is equal to exp [−γRt]<P(t)>, where γR is the radiative decay rate and <P(t)> is the probability that an ion excited at t=0 is also excited at time t.2