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physica status solidi (b)

Energy transfer and rate equations—application to ruby

Johann Heber

Published Jan 1, 1970• 13 citations
Publisher

Abstract

Abstract Atomistic rate equations are represented for the transfer of optical excitation energy between donor and acceptor ions in ionic crystals. The physical assumptions which are necessary to deduce the phenomenological collective rate equations from the atomistic ones are specified. Time resolved measurements of the energy transfer from isolated Cr3+ ions to Cr3+ pairs in ruby are discussed. It is shown that, contrary to the present ideas, the collective rate equations cannot be applied in this case.

DOI
10.1002/pssb.19700420204

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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 percent Cr2O3were 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.

IEEE Journal of Quantum Electronics•Sep 1, 1966•4 citations
Abstract Atomistic rate equations are represented for the transfer of optical excitation energy between donor and acceptor ions in ionic crystals. The physical assumptions which are necessary to deduce the phenomenological collective rate equations from the atomistic ones are specified. Time resolved measurements of the energy transfer from isolated Cr3+ ions to Cr3+ pairs in ruby are discussed. It is shown that, contrary to the present ideas, the collective rate equations cannot be applied in this case.
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.
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 optical energy transfer between Cr 3+ ions from cubic centres to tetragonal centres is measured. Transfer is observed only when the donor is very close to the acceptor and the measured transfer times are relatively short ( approximately 100 mu s). The tetragonal acceptors are Cr 3+ -ion pairs which form different triads with the donor. It is deduced that transfer to rhombic sites is also rapid only from very close cubic centres. The shortness of the transfer times explains why a spin memory is observed during the energy transfer from cubic to rhombic centres. The localisation of optical excitation in triads is due to the presence of charge-compensating Mg 2+ vacancies and the inefficiency of the dipole-dipole interaction.
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 percent Cr2O3were 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.