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Journal of Physics C Solid State Physics

Fluorescence line narrowing and spectral energy transfer in pair lines of ruby

André Monteil, Eugène Duval

Published Oct 20, 1984• 3 citations
Publisher

Abstract

The fluorescence line narrowing (FLN) of the N 1 and N 2 lines of pairs of Cr 3+ ions in concentrated ruby has been studied. The structure of the narrowed lines has been explained and measurements of the homogeneous width have been improved. By use of the FLN and time-resolved spectroscopy, spectral transfer within the N 1 line has been investigated. A two-phonon-assisted process has been found to be responsible for the transfer.

DOI
10.1088/0022-3719/17/29/021

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Physical review. B, Solid state•Sep 1, 1977•62 citations
The fluorescence line narrowing (FLN) of the N 1 and N 2 lines of pairs of Cr 3+ ions in concentrated ruby has been studied. The structure of the narrowed lines has been explained and measurements of the homogeneous width have been improved. By use of the FLN and time-resolved spectroscopy, spectral transfer within the N 1 line has been investigated. A two-phonon-assisted process has been found to be responsible for the transfer.
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.
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.
The transfer of energy from single chromium ions to closely coupled pairs of chromium ions in ruby has been investigated. Ruby samples whose concentrations ranged from 0.003 to 1.0% Cr2{\mathrm{Cr}}_{2}Cr2​O3{\mathrm{O}}_{3}O3​ were prepared and in each crystal the intensity of single-ion fluorescence and of pair fluorescence was accurately measured. Radiative-decay measurements were also made in an attempt to unravel the dynamics of the transfer process. The transfer from single ions to pairs is shown to occur nonradiatively, and its efficiency is enhanced by a fast energy transfer between individual single ions. The possibility is explored that an electric quadrupole-quadrupole interaction is responsible for this transfer process.
The transfer of energy from single chromium ions to closely coupled pairs of chromium ions in ruby has been investigated. Ruby samples whose concentrations ranged from 0.003 to 1.0% Cr2{\mathrm{Cr}}_{2}Cr2​O3{\mathrm{O}}_{3}O3​ were prepared and in each crystal the intensity of single-ion fluorescence and of pair fluorescence was accurately measured. Radiative-decay measurements were also made in an attempt to unravel the dynamics of the transfer process. The transfer from single ions to pairs is shown to occur nonradiatively, and its efficiency is enhanced by a fast energy transfer between individual single ions. The possibility is explored that an electric quadrupole-quadrupole interaction is responsible for this transfer process.
Time-resolved fluorescence line narrowing is used to study spectral energy transfer in PrF3{\mathrm{F}}_{3}F3​ and PrCl3{\mathrm{Cl}}_{3}Cl3​. The excitation spectrum of PrF3{\mathrm{F}}_{3}F3​ in the region of the ${(^{3}H_{4})}_{1}\ensuremath{\rightarrow}^{3}P_{0}$ absorption indicates that several strong satellite lines accompany the main transition, their origin being ascribed to different Pr3+{\mathrm{Pr}}^{3+}Pr3+ ions lying in strongly perturbed lattice sites. The spectral transfer within the inhomogeneously broadened main transiton is measured, where the energy mismatch is about 2 ${\mathrm{cm}}^{\ensuremath{-}1}$. This process is characterized by a strong ($\ensuremath{\sim}{T}^{4.3}$) dependence of the transfer probability on sample temperature. The growth of the full inhomogeneous emission profile accompanies a uniform decay of the donor line shape. A transfer process between the lowest-energy satellite ions is also measured. Here the energy mismatch is 32 ${\mathrm{cm}}^{\ensuremath{-}1}$ resulting in a weak temperature dependence for the transfer rate. Both the intraline and intersatellite transfer are characterized by simple exponential rate equations. Recent calculations of phonon-assisted transfer probabilities are compared to our measurements, with the intersatellite transfer ascribed to a "one-phonon direct" process whereas the transfer within the main transition occurs by a "one-phonon second-order" mechanism. In PrCl3{\mathrm{Cl}}_{3}Cl3​ the transfer times are faster than the 15-nsec response time of our detection system indicating a much stronger ion-ion coupling.