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Optics Letters

Radiative spectral transfer in ruby

Peter M. Selzer, William M. Yen

Published Sep 1, 1977• 25 citations
Publisher

Abstract

The first direct observation of radiative spectral transfer within an inhomogeneously broadened line (the R(1) line of ruby) is reported. As opposed to nonradiative transfer, the temperature dependence of the radiative process is consistent with exponential, in agreement with recent predictions. A temperature-independent, resonant process is also directly observed. The implication of these results for the concept of microscopic strain broadening is discussed.

DOI
10.1364/ol.1.000090

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Studies of the resonant interaction of radiation from a liquid-nitrogen-cooled ruby laser with a ruby crystal in the temperature range 4.2°–100°K are described. The interaction was measured by observation of the change which occurs in the Cr3+ ground state EPR absorption on laser irradiation. At low radiation intensities, the temperature dependence of this change is shown to be determined by the well-known thermal tuning behavior of the R lines. Precise measurement of the relative laser and ruby-sample absorption frequencies by this technique of double-resonance spectroscopy is described. Under optical saturation conditions, additional temperature-dependent pumping effects occur at low temperatures. In particular, as the ruby temperature is increased from 4.2° to 40°K, the laser-induced change in EPR absorption is observed to undergo a large increase. This increase cannot be explained by a relative thermal shift of the laser and absorption frequencies which is known to be very small in this temperature range. The phenomena are attributed in part to the temperature-dependent homogeneous linewidth which determines the widths of the holes burnt into the inhomogeneous strain-broadened R lines. Calculations indicate that the related temperature-dependent thermalization process which redistributes excited Cr3+ among the 2E levels quantitatively accounts for most of the increase.

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Phonon-assisted radiative transfer

Theodore D. Holstein, S. K. Lyo, R. Orbach

The radiative-transfer rate for inhomogeneously broadened optical lines is calculated. Photon emission and absorption is supplemented by one- and two-phonon processes to achieve energy conservation. These photon-assisted radiative transfer processes are shown to be effective at low concentrations, where electrostatic and exchange processes are weak, in the intermediate or strong radiative trapping regime. Specific application is made to the case of dilute ruby, and explicit transfer rates are calculated. The coherence factors, which undermine nonradiative single-phonon-assisted energy transfer for a small energy mismatch, are not important for radiative transfer, if the photon mean free path is longer than the wavelength of the energy matching phonon. The one-phonon process is found to vary linearly with temperature, and to be independent of the energy mismatch. However, the calculated rate for the case of ruby is found to be very slow. The two-phonon-assisted radiative-transfer process rates are calculated. They dominate the one-phonon-assisted rate for all reasonable temperatures. The results of an earlier paper are shown to be related to phonon-assisted radiative transfer if one replaces the exchange coupling between transfer sites $J$ by $\ensuremath{\sim}\frac{{\ensuremath{\tau}}_{R}^{\ensuremath{-}1}\ensuremath{\hbar}}{(\frac{{r}_{0}}{\ensuremath{\lambda}})}$. Here ${\ensuremath{\tau}}_{R}$ is the radiative lifetime, ${r}_{0}$ the distance between sites, and $\ensuremath{\lambda}$ the photon wavelength involved in the radiative transfer. This replacement results in a line center to wing transfer rate equal to 1.1 \ifmmode\times\else\texttimes\fi{} ${10}^{2}$ ${e}^{\ensuremath{-}\frac{42}{T}}$ ${\mathrm{sec}}^{\ensuremath{-}1}$ for ruby (independent of concentration for a photon mean free path smaller than the sample size).

Physical review. B, Solid state•Jul 15, 1977•37 citations
The first direct observation of radiative spectral transfer within an inhomogeneously broadened line (the R(1) line of ruby) is reported. As opposed to nonradiative transfer, the temperature dependence of the radiative process is consistent with exponential, in agreement with recent predictions. A temperature-independent, resonant process is also directly observed. The implication of these results for the concept of microscopic strain broadening is discussed.
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.
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.
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.
Studies of the resonant interaction of radiation from a liquid-nitrogen-cooled ruby laser with a ruby crystal in the temperature range 4.2°–100°K are described. The interaction was measured by observation of the change which occurs in the Cr3+ ground state EPR absorption on laser irradiation. At low radiation intensities, the temperature dependence of this change is shown to be determined by the well-known thermal tuning behavior of the R lines. Precise measurement of the relative laser and ruby-sample absorption frequencies by this technique of double-resonance spectroscopy is described. Under optical saturation conditions, additional temperature-dependent pumping effects occur at low temperatures. In particular, as the ruby temperature is increased from 4.2° to 40°K, the laser-induced change in EPR absorption is observed to undergo a large increase. This increase cannot be explained by a relative thermal shift of the laser and absorption frequencies which is known to be very small in this temperature range. The phenomena are attributed in part to the temperature-dependent homogeneous linewidth which determines the widths of the holes burnt into the inhomogeneous strain-broadened R lines. Calculations indicate that the related temperature-dependent thermalization process which redistributes excited Cr3+ among the 2E levels quantitatively accounts for most of the increase.
The radiative-transfer rate for inhomogeneously broadened optical lines is calculated. Photon emission and absorption is supplemented by one- and two-phonon processes to achieve energy conservation. These photon-assisted radiative transfer processes are shown to be effective at low concentrations, where electrostatic and exchange processes are weak, in the intermediate or strong radiative trapping regime. Specific application is made to the case of dilute ruby, and explicit transfer rates are calculated. The coherence factors, which undermine nonradiative single-phonon-assisted energy transfer for a small energy mismatch, are not important for radiative transfer, if the photon mean free path is longer than the wavelength of the energy matching phonon. The one-phonon process is found to vary linearly with temperature, and to be independent of the energy mismatch. However, the calculated rate for the case of ruby is found to be very slow. The two-phonon-assisted radiative-transfer process rates are calculated. They dominate the one-phonon-assisted rate for all reasonable temperatures. The results of an earlier paper are shown to be related to phonon-assisted radiative transfer if one replaces the exchange coupling between transfer sites JJJ by $\ensuremath{\sim}\frac{{\ensuremath{\tau}}_{R}^{\ensuremath{-}1}\ensuremath{\hbar}}{(\frac{{r}_{0}}{\ensuremath{\lambda}})}$. Here ${\ensuremath{\tau}}_{R}$ is the radiative lifetime, r0{r}_{0}r0​ the distance between sites, and $\ensuremath{\lambda}$ the photon wavelength involved in the radiative transfer. This replacement results in a line center to wing transfer rate equal to 1.1 \ifmmode\times\else\texttimes\fi{} 102{10}^{2}102 ${e}^{\ensuremath{-}\frac{42}{T}}$ ${\mathrm{sec}}^{\ensuremath{-}1}$ for ruby (independent of concentration for a photon mean free path smaller than the sample size).