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Physical review. B, Condensed matter

Fluorescence-line-narrowing and energy-transfer studies in ruby

Peter M. Selzer, David L. Huber, B. B. Barnett, William M. Yen

Published Jun 15, 1978• 91 citations
Publisher

Abstract

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 ${R}_{1}$ 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 $R$ 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.

DOI
10.1103/physrevb.17.4979

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Physical Review•Mar 10, 1967•64 citations
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 (R1\ensuremath→N1,2{R}_{1}\ensuremath{\rightarrow}{N}_{1,2}R1​\ensuremath→N1,2​) 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.
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.
The fluorescence intensities and lifetimes of various no-phonon lines in ruby samples with 2.1 and 0.94% Cr3+{\mathrm{Cr}}^{3+}Cr3+ were studied from 13 to 700\ifmmode^\circ\else\textdegree\fi{}K. The temperature dependences of the intensities of numerous lines were used to determine the energy levels of two pair systems. The relative intensities of the single-ion (RRR) lines and the pair (NNN) lines are proportional to Boltzmann factors ${e}^{\frac{\ensuremath{-}\ensuremath{\Delta}E}{\mathrm{kT}}}$, where $\ensuremath{\Delta}E$ is the difference in energy of the metastable states, at high temperatures but not at low temperatures. The deviation from this law is greater and occurs at higher temperatures in the less concentrated sample. The fluorescence decays of the RRR and NNN lines are pure exponentials in the temperature region where the NNN lines follow a Boltzmann law; at low temperatures the NNN lines have an initial rise in fluorescence and then a decay. These results are interpreted in terms of coupled fluorescence systems consisting of single ions and pairs. A phonon-assisted cross-relaxation coupling process is suggested which allows for thermalization of the systems at high temperatures and direct pumping of the pair systems by the single-ion system at low temperatures. Energy transfer from single-ion to multi-ion systems was also observed.