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Physical Review Letters

Nonradiative Spectral and Spatial Energy Transfer in Ruby

Peter M. Selzer, D. S. Hamilton, William M. Yen

Published Apr 11, 1977• 83 citations
Publisher

Abstract

The first experimental evidence for distinct spectral and spatial energy transfer in ruby via nonradiative coupling is presented. Monochromatic laser excitation of the ${R}_{1}$ 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 ${R}_{1}$ line which does not shift frequency.

DOI
10.1103/physrevlett.38.858

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Journal of Physics Condensed Matter•Jun 20, 1994•3 citations
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.
Measurements are reported of resonant nonradiative energy transfer in the R1{R}_{1}R1​ line of ruby at 5 K using a fast Stark shifting technique. The transfer rate for 0.8% ruby is found to be slow, \ensuremath{\sim} 1 ${\mathrm{msec}}^{\ensuremath{-}1}$, contrary to the much more rapid rates proposed earlier by several workers but in fair agreement with the results of Heber. Implications of the results for the occurrence of an Anderson transition in ruby are discussed.
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.
Systematic investigations of the effect of self-absorption on the dynamic and steady-state spectroscopic properties in ruby have been carried out at different temperatures (from approximately 130 to 500 K) using a long, pink laser rod. At about 140 K,the lengthening of decay times of the R lines reached a maximum and then decreased with increasing geometric trapping. Spectral diffusion as large as 10 cm -1 was observed in the complete-trapping regime. These observations suggest reexamination of the theoretical model for phonon-assisted radiative energy transfer in ruby.