Optics Letters

Temperature dependence of the Ē → 2Ā far-infrared absorption line of excited chromium ions in ruby

H. Lengfellner, J. Hummel, H. Netter, Karl Friedrich Renk

Published Apr 1, 1983• 6 citations

Abstract

By using far-infrared laser spectroscopy we have studied the temperature dependence of the absorption that is due to transitions between the E ((2)E) and 2A ((2)E) levels of excited Cr(3+) ions in ruby. From the temperature dependence of the linewidth we determined the inhomogeneous and the homogeneous contributions to line broadening. From the homogeneous width the lifetime of the 2A level was obtained. We found that, for emperatures up to 70 K, the lifetime is due mainly to one-phonon relaxation, whereas at higher temperatures another relaxation process, probably a two-phonon Raman process, becomes strong.

DOI: 10.1364/ol.8.000220

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Optics Letters

Temperature dependence of the Ē → 2Ā far-infrared absorption line of excited chromium ions in ruby

H. Lengfellner, J. Hummel, H. Netter, Karl Friedrich Renk

Published Apr 1, 1983• 6 citations

Publisher

Abstract

DOI: 10.1364/ol.8.000220

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Journal of Applied PhysicsOct 1, 19700 citations

Optical-Microwave Double-Resonance Studies of Ruby

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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.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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Fluorescence Studies of Energy Transfer between Single and Pair Cr3+ Systems in Al2 O3

Richard C. Powell, Baldassare Di Bartolo, Behzad Birang +1 more

The fluorescence intensities and lifetimes of various no-phonon lines in ruby samples with 2.1 and 0.94% ${\mathrm{Cr}}^{3+}$ 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 ( $R$ ) lines and the pair ( $N$ ) 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 $R$ and $N$ lines are pure exponentials in the temperature region where the $N$ lines follow a Boltzmann law; at low temperatures the $N$ 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 fluorescence intensities and lifetimes of various no-phonon lines in ruby samples with 2.1 and 0.94% ${\mathrm{Cr}}^{3+}$ 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 ($R$) lines and the pair ($N$) 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 $R$ and $N$ lines are pure exponentials in the temperature region where the $N$ lines follow a Boltzmann law; at low temperatures the $N$ 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.

Physical ReviewMar 10, 196764 citations

According to several recent studies, the width of the sharp zero-phonon lines in the electronic spectra of impurities in solids, such as the

R

lines of ruby, is due to Raman scattering of phonons by the impurity ions. The question whether such zero-phonon lines are homogeneously broadened is an important one, both for its own interest and for optical-maser applications. From a detailed study of the stimulated-emission spectra of a ruby laser operating in the traveling-wave modes, we obtain conclusive evidence that such zero-phonon lines are homogeneously broadened. Because the

{R}_{1}

line of ruby is essentially homogeneously broadened at room temperature, the traveling-wave laser oscillates for all practical purposes only in a single mode. The spectral width of the laser emission is extremely sharp. It is less than 0.005 ${\mathrm{cm}}^{\ensuremath{-}1}$ at room temperature as compared to a width of the order of 1 ${\mathrm{cm}}^{\ensuremath{-}1}$ for conventional ruby lasers of comparable intensity. In addition, the output intensity no longer shows random spikes but shows a predictable train of regularly spaced spikes which agree well with theory.

The fluorescence intensities and lifetimes of various no-phonon lines in ruby samples with 2.1 and 0.94%

{\mathrm{Cr}}^{3+}

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 (

R

) lines and the pair (

N

) 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

R

and

N

lines are pure exponentials in the temperature region where the

N

lines follow a Boltzmann law; at low temperatures the

N

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.