Absorption transitions between two excited optical states in ruby have been studied by comparing the absorption coefficients measured under optically pumped and unpumped conditions. The spectrum has been determined in the π-and σ-polarizations in the photon energy range from 5,500 to 45,000 cm -1 . Several absorption bands have been found which arise from the transitions from the excited states t 2g 3 2 E g and t 2g 3 2 T 1g of the Cr 3+ ion. From the locations and intensities of these bands, the terminal states of the observed transitions are assigned to the charge transfer state, the t 2g 3 2 T 2g state, and the doublet states belonging to the electron configuration t 2g 3 e g . Calculated energies between these states and the metastable states, t 2g 3 2 E g and t 2g 3 2 T 1g , are in good agreement with the peak energies of the observed absorption bands. The present experiment gives new information inaccessible by the ordinary ground state absorption measurement, such as the locations of several doublet states with the configuration t 2g 2 e g and the intensities of doublet-doublet transitions in ruby.
The absorption cross sections of the
Cr3+ ion in the metastable states
2E(Eand2A) of lightly doped ruby (\ensuremath{\sim}0.01%) have been measured as a function of polarization at temperatures of 30, 105, and 296\ifmmode^\circ\else\textdegree\fi{}K in the region from 2300 to 7000 \AA{}. The lifetime of these states was measured by observing the decay rate of the excited-state absorption, and agreed with the value of the measured fluorescence decay rate at various temperatures. The population of the excited states was measured by the change of the area under the first two vibronic sidebands at low temperatures. At room temperature the population was measured by the change of transmitted intensity of a ruby laser.
Absorption cross sections of Cr3+in the metastable2E states of pink ruby (0.05 percent Cr2O3) have been measured forE \perp Cbetween 4000 Å and 7000 Å at 297°K and 115°K. Both 0 degree and 90 degree ruby rods were measured in a flash absorption apparatus having a spectral resolution of 50 Å. The broad excited state absorption bands centered at 5600 Å appear to correlate with the positions of2T1(3T1) level, while the narrow band centered at 4540 Å correlates well with the predicted2A2(1E) level. The effect of excited state absorption on laser operation is discussed in this paper.
We consider ruby as a linear, uniaxial, maxwellian medium, which, in its absorbing state, has axially dependent material constants. It is made active by pumping with electric fields, in the region of shorter-wavelength absorption bands, which, by means of an energy transfer, induce source-type electric fields having constant amplitudes in the R1 and R2 regions, and make possible absorption, spontaneous emission, and stimulated emission. Experiments indicate that the absorption, fluorescence, and laser action are all maximum for electric fields perpendicular to the optic axis, and minimum when the electric field is parallel to the optic axis; the relative irradiances and shapes of the R1 and R2 bands in all cases depend upon the orientation of the plane of polarization of the emerging radiant flux relative to the optic axis. Attempts are made to compute the spectral distributions in the R1 and R2 bands for the ordinary and extraordinary waves, neglecting all boundary-value problems. Agreement was found to be possible only in the region below the threshold of laser action.
Systematic investigations of the effect of self-absorption on the dynamic and steady-state spectroscopic properties in ruby have been carried out at different temperatures (from approximately 130 to 500 K) using a long, pink laser rod. At about 140 K,the lengthening of decay times of the R lines reached a maximum and then decreased with increasing geometric trapping. Spectral diffusion as large as 10 cm -1 was observed in the complete-trapping regime. These observations suggest reexamination of the theoretical model for phonon-assisted radiative energy transfer in ruby.
The relaxation of resonant 29-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ phonons trapped in a laser-excited cylinder of submillimeter diameter is investigated under the conditions of modulated pumping in ruby of 130, 700, and 2500 at. ppm
Cr3+ at 1.5 K. The decay time
Teff of the 2\ifmmode \bar{A}\else \={A}\fi{}
(2E) population, which is a measure of the phonon relaxation time, appears to depend on the metastable population
N∗ and the cylinder diameter L as the product
N∗L only, establishing boundary-limited phonon decay. At
N∗L below 5\ifmmode\times\else\texttimes\fi{}
1015 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}2}$, pure spatial diffusion prevails.At higher
N∗L, where the measured
Teff levels off at about 1 \ensuremath{\mu}s, dependent on the ground-state concentration, the phonon relaxation is adequately accounted for by the assumption of enhancement by mediation of frequency-shifting Orbach processes at metastable
Cr3+ subject to diagonal exchange with ground-state
Cr3+. Shifts away from resonance to the extent that the phonons escape the zone by ballistic flight are considered active, which predominantly involve distant
Cr3+ neighbors.Furthermore, a random distribution of
Cr3+ is assumed, while the exchange is calibrated with reference to pair spectra. The spin-nonflip transitions of metastable
Cr3+ that are part of the pairs remain at resonance with the phonons because the exchange splittings of \ifmmode \bar{E}\else \={E}\fi{}
(2E) and 2\ifmmode \bar{A}\else \={A}\fi{}
(2E) are comparable. This is borne out by a separate calculation based on a perturbative molecular field. In addition, experiments have been performed as a function of an external magnetic field up to 4 T parallel to the c axis to disclose the effects of successive separation of the spin-flip and spin-nonflip transitions. The resultant complex development of
Teff with field as well as similar data on the
R2 luminescent intensity taken with continuous optical pumping are consistent with exchange-invoked relaxation and, further, yield effective spectral widths of the 29-${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$ transitions of the weakly coupled metastable
Cr3+ of order 1 ${\mathrm{cm}}^{\mathrm{\ensuremath{-}}1}$.