A high resolution study has been made of the R(1) doublet in the absorption spectrum of pink ruby, using a temperature-controlled ruby laser as a variable frequency monochromatic source. The source and sample crystals were oriented for measurement of the absorption of alpha-polarized radiation, and the measurements were made near liquid nitrogen temperature. The observed absorption coefficient was found to decrease as the intensity of the incident beam was increased, indicating that significant depletion of the ground state was effected by the resonant pumping action of the laser beam. The highest laser beam intensity employed was approximately 100 J/cm(2). At this intensity level a significant reduction in the spectral spacing of the R(1)(+/-3/2) and R(1)(+/-(1/2)) components of the absorption doublet was also observed. Time-resolved spectral measurements showed, moreover, that at similar intensity levels, temporally smooth incident beams at frequencies near the absorption line peaks emerged from the sample temporally structued. The observed reduction in the absorption coefficient agrees well with calculations based on a simple model for ground state depletion, but no detailed theoretical explanation of the other observed phenomena has yet been developed.
We report experimental and theoretical studies of optical hole burning in the inhomogeneous
R1 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 real and imaginary parts of the complex index of refraction have been measured in the R1 line of optically pumped ruby. The experiments, which employed a temperature-controlled, single-mode ruby laser as a variable-frequency monochromatic source, were performed near liquid-nitrogen temperature, where the R1 doublet structure is well resolved. R1 absorption profiles were measured for several optical-pumping conditions, ranging from zero up to a pump power that excited a population in the 2E state equal to about 60% of the population of the 4A2 ground state. For each pumping condition, the anomalous-dispersion curve was measured interferometrically. The spectral profiles of the absorption coefficient and the anomalous dispersion display a dependence on the optical-pumping conditions that is more complicated than simple saturation of the R1 transitions, but for given pumping conditions the two quantities are correlated as predicted by the Kramers–Kronig relations.
In this paper we report, for the first time, the observation of optical hole burning in a solid, ruby. In addition, we describe experimental results which show that optical saturation of the inhomogeneously broadened
R1 line in ruby at 4.2\ifmmode^\circ\else\textdegree\fi{}K occurs not only for ions in resonance with the saturating radiation but also for ions at frequencies up to about 50 MHz away from the radiation frequency. This result and others are consistent with a model in which cross relaxation occurs in the ground-state levels between ions in resonance with the laser beam and nonresonant ions.
Ruby lasers, when operated near threshold at 77°K with a low Q cavity (one end silvered for maximum reflectivity and the other end uncoated) oscillated at two frequencies. The frequency differences near threshold, measured with Fabry-Perot etalons, were in good agreement with the splitting of the R1 doublet, previously measured by microwave methods. As the power of the laser increased, the frequency difference between the oscillating components [2Ē → 4A2(±32, ±½)] decreased. These results are accounted for on the basis of saturation broadening of overlapping Lorentzian lines. The observed variations in the splitting are in good accord with the theory. The rise in temperature of the ruby rods produced a negligible change in the splitting of the R1 doublet. The same mechanism which produces the variation in the splitting should broaden the output spectrum of the laser.
We have measured the radiative efficiency (ratio of
R-line photons to the total number of photons emitted) and absorption cross sections for the
R lines of dilute ruby, as a function of polarization and temperature between 20 and 373\ifmmode^\circ\else\textdegree\fi{}K. We have also measured the fluorescent lifetime from 20 to 373\ifmmode^\circ\else\textdegree\fi{}K in optically thin crystals, and from 20 to 273\ifmmode^\circ\else\textdegree\fi{}K in optically thick crystals. The difference between the reciprocal lifetimes in thin and thick crystals is directly comparable (via the Einstein relations) with the integrated absorption in the
R lines. This comparison shows that for the
R lines at 20 and 77\ifmmode^\circ\else\textdegree\fi{}K detailed balance holds to well within the experimental error of 5%, a precision never to our knowledge previously approached in solids. An upper limit of 0.002 ${\mathrm{cm}}^{\ensuremath{-}1}$ was placed on any Stokes shift of the
R1 line, confirming that it is a no-phonon line. Comparison of $\ensuremath{\sigma}$ and $\ensuremath{\alpha}$ spectra confirms that the
R lines and their vibronic satellites are predominately electric-dipole in character. The radiative efficiency of the
R lines is strongly polarization dependent, a result which differs from that of previous workers. Its temperature dependence agrees well with that calculated from the observed vibronic spectrum at 77\ifmmode^\circ\else\textdegree\fi{}K. The integrated absorption in the
R lines increases by about 20% between 20 and 373\ifmmode^\circ\else\textdegree\fi{}K. The absorption in the vibronic satellites on the high-frequency side of the
R lines appears to be weaker than the corresponding emission on the low-frequency side. The temperature variation of the lifetime agrees well with that calculated from the absorption and radiative efficiency, but about 10% of the decay at 77\ifmmode^\circ\else\textdegree\fi{}K and 30% at 373\ifmmode^\circ\else\textdegree\fi{}K is either nonradiative or by emission at wavelengths outside the range of observation. The implications of our results for laser work are discussed.