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.
Small differences between the emission and absorption spectra of three-level maser centers can have a pronounced effect on maser operation. This paper considers the effects of a Stokes shift, the simplest and most probable difference. If there is a Stokes shift which is large compared to the linewidth, the operation of the maser will be essentially four level. If there is a small Stokes shift (some fraction of the linewidth) the operation will still be three level, but the Stokes shift will significantly affect the operation of the maser. The principal effects will be a shift of the maser line from the peak in the fluorescent emission line (away from the absorption peak) and a reduction in the upper level population required to reach the threshold of oscillation. The evidence is not conclusive as to whether there is a Stokes shift in the ruby R1 line, but if there is a shift it is at most a small fraction of the fluorescent linewidth at room temperature. Shifts of the ruby maser line to the red have been observed by D'Haenens and Asawa and have been attributed to large temperature changes. It is likely that the temperature shift, while important, will not explain the shift which has been observed. Gires and Mayer have found the lower state population of an operating ruby maser to be approximately 75% of the unexcited population rather than approximately 50% and have suggested a Stokes shift as a possible cause of the reduction in the upper state population at threshold. This paper considers the effect of such a small Stokes shift on the operation of an otherwise ideal three-level maser.
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 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.
Laser-induced fluorescence line narrowing of the ruby
R1 Zeeman spectra at 693.4 nm is reported using a continuous, stable, single-frequency ruby laser for resonant excitation. A resolution in excess of
107 corresponding to a linewidth of \ensuremath{\sim} 30 MHz has been achieved. The linewidths are anisotropic with respect to the relative magnetic-field-crystal-axis orientation and, at low Cr concentrations, are expected to be determined by Cr-Al superhyperfine interactions.