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Physical Review Letters

Laser-Induced Fluorescence-Line Narrowing in Ruby

Arthur G. Szabo

Published Oct 5, 1970• 241 citations
Publisher

Abstract

Using resonance ruby-laser excitation, narrowing of the ruby ${R}_{1}$ 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.

DOI
10.1103/physrevlett.25.924

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Using resonance ruby-laser excitation, narrowing of the ruby R1{R}_{1}R1​ fluorescence line to width 0.002 cm\ensuremath−1{\mathrm{cm}}^{\ensuremath{-}1}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.
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.
Laser-induced fluorescence line narrowing of the ruby R1{R}_{1}R1​ Zeeman spectra at 693.4 nm is reported using a continuous, stable, single-frequency ruby laser for resonant excitation. A resolution in excess of 107{10}^{7}107 corresponding to a linewidth of \ensuremath{\sim} 30 MHz has been achieved. The linewidths are anisotropic with respect to the relative magnetic-field-crystal-axis orientation and, at low Cr concentrations, are expected to be determined by Cr-Al superhyperfine interactions.
The first experimental evidence for distinct spectral and spatial energy transfer in ruby via nonradiative coupling is presented. Monochromatic laser excitation of the R1{R}_{1}R1​ line results in a rise of the inhomogeneous background on a millisecond time scale, consistent with a one-phonon---assisted process and contrary to recent theory. However, time-resolved studies of trap fluorescence suggest a rapid, coherent, spatial transfer within the R1{R}_{1}R1​ line which does not shift frequency.
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.