Physical Review Letters

Resonant Optical Energy Transfer in Ruby

Paul E. Jessop, Arthur G. Szabo

Published Nov 24, 1980• 40 citations

Abstract

Measurements are reported of resonant nonradiative energy transfer in the ${R}_{1}$ 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.

DOI: 10.1103/physrevlett.45.1712

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Physical Review Letters

Resonant Optical Energy Transfer in Ruby

Paul E. Jessop, Arthur G. Szabo

Published Nov 24, 1980• 40 citations

Publisher

Abstract

Measurements are reported of resonant nonradiative energy transfer in the

{R}_{1}

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.

DOI: 10.1103/physrevlett.45.1712

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Nonradiative Spectral and Spatial Energy Transfer in Ruby

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The first experimental evidence for distinct spectral and spatial energy transfer in ruby via nonradiative coupling is presented. Monochromatic laser excitation of the ${R}_{1}$ 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 ${R}_{1}$ line which does not shift frequency.The first experimental evidence for distinct spectral and spatial energy transfer in ruby via nonradiative coupling is presented. Monochromatic laser excitation of the ${R}_{1}$ 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 ${R}_{1}$ line which does not shift frequency.

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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.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.

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Physical Review LettersOct 5, 1970241 citations

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Paul E. Jessop, T. Muramoto, A. Szabó

We report experimental and theoretical studies of optical hole burning in the inhomogeneous ${R}_{1}$ line of ruby at low temperatures. Both Stark-shifting and pump-probe techniques using narrow-band single-frequency lasers were employed. In addition to the observation of narrow holes, we have found that a large (up to 70%) decrease in absorption occurs outside the hole and that the relative size of this decrease is constant over the entire inhomogeneous line. This effect is ascribed to fast resonant cross-spin relaxation in the ground-state levels which drives all spins within the optically pumped volume to a common spin temperature. A theoretical model is formulated which describes the power-broadened hole shapes as well as the off-resonance decrease in the absorption coefficient. Fair agreement with experiment is obtained for the case of a magnetic field applied along the $c$ axis; however, sizable deviations from the theory are seen for zero field. We conclude that further studies are needed to elucidate the nature of the Al superhyperfine-broadening mechanism. An upper limit of 1200 nm is deduced for the size of macroscopically broadened regions in ruby.We report experimental and theoretical studies of optical hole burning in the inhomogeneous ${R}_{1}$ line of ruby at low temperatures. Both Stark-shifting and pump-probe techniques using narrow-band single-frequency lasers were employed. In addition to the observation of narrow holes, we have found that a large (up to 70%) decrease in absorption occurs outside the hole and that the relative size of this decrease is constant over the entire inhomogeneous line. This effect is ascribed to fast resonant cross-spin relaxation in the ground-state levels which drives all spins within the optically pumped volume to a common spin temperature. A theoretical model is formulated which describes the power-broadened hole shapes as well as the off-resonance decrease in the absorption coefficient. Fair agreement with experiment is obtained for the case of a magnetic field applied along the $c$ axis; however, sizable deviations from the theory are seen for zero field. We conclude that further studies are needed to elucidate the nature of the Al superhyperfine-broadening mechanism. An upper limit of 1200 nm is deduced for the size of macroscopically broadened regions in ruby.

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Energy transfer in ruby

G. F. Imbusch

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% ${\mathrm{Cr}}_{2}$ ${\mathrm{O}}_{3}$ 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% ${\mathrm{Cr}}_{2}$${\mathrm{O}}_{3}$ 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.

IEEE Journal of Quantum ElectronicsApr 1, 19660 citations

Measurements are reported of resonant nonradiative energy transfer in the

{R}_{1}

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}

The first experimental evidence for distinct spectral and spatial energy transfer in ruby via nonradiative coupling is presented. Monochromatic laser excitation of the

{R}_{1}

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

{R}_{1}

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

{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.

Using resonance ruby-laser excitation, narrowing of the ruby

{R}_{1}

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.

We report experimental and theoretical studies of optical hole burning in the inhomogeneous

{R}_{1}

line of ruby at low temperatures. Both Stark-shifting and pump-probe techniques using narrow-band single-frequency lasers were employed. In addition to the observation of narrow holes, we have found that a large (up to 70%) decrease in absorption occurs outside the hole and that the relative size of this decrease is constant over the entire inhomogeneous line. This effect is ascribed to fast resonant cross-spin relaxation in the ground-state levels which drives all spins within the optically pumped volume to a common spin temperature. A theoretical model is formulated which describes the power-broadened hole shapes as well as the off-resonance decrease in the absorption coefficient. Fair agreement with experiment is obtained for the case of a magnetic field applied along the

c

axis; however, sizable deviations from the theory are seen for zero field. We conclude that further studies are needed to elucidate the nature of the Al superhyperfine-broadening mechanism. An upper limit of 1200 nm is deduced for the size of macroscopically broadened regions in ruby.

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%

{\mathrm{Cr}}_{2}

{\mathrm{O}}_{3}

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.