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Journal of Physics C Solid State Physics

Energy transfer in ruby under electric field

André Monteil, Eugène Duval, Aya Attar, G. Viliani

Published Jan 30, 1985• 2 citations
Publisher

Abstract

Spectral energy transfer in ruby is observed to be faster between Cr 3+ ions belonging to the same A sublattice than between Cr 3+ ions occupying different A and B sublattices which are separated by an electric field. The time evolution of the transfer rate is interpreted by selective occupation of sites in one sublattice at the micro-domain scale.

DOI
10.1088/0022-3719/18/3/018

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Spectral energy transfer in ruby is observed to be faster between Cr 3+ ions belonging to the same A sublattice than between Cr 3+ ions occupying different A and B sublattices which are separated by an electric field. The time evolution of the transfer rate is interpreted by selective occupation of sites in one sublattice at the micro-domain scale.
The energy transfer between single Cr 3+ ions and N 2 pairs in ruby is interpreted by energy diffusion on single ions. It is shown that the superexchange is responsible for this diffusion. The probability of transfer between single ions and the diffusion coefficient are evaluated. Experimental results on the transfers from fourth next-neighbour pairs to single ions and to third next-neighbour pairs are given. It appears that the diffusion is weak on the fourth NN pairs. The temperature dependence of the transfer probabilities are determined and interpreted.
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 optical spectrum due to the exchange coupled Cr 3+ ions in ruby has been studied theoretically. The effect of the lowering of the Cr 3+ site symmetry due to the formation of a pair was taken into account. For the 2nd neighbor pair, a good fitting of the excited state energies between theory and experiment was obtained. The effect of the higher order exchange is found to be very important for this pair. It is also found that the deviation of the Cr 3+ site symmetry from C 3 is rather large for this pair. For the 4th neighbor pair, the level diagram of the excited state was obtained and the absorption intensities were calculated. Most of the observed lines in this pair are explained by this theory. The lines so called N 1 and N 2 are found to be the transitions due to the exchange induced electric dipole.
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.