Selective pulsed optical excitation is used in 500-at.ppm ruby (Al 2 O 3 :Cr 3+ ) at 1.4 K to prepare complete population inversion of the Zeeman-split Ē( 2 E ) doublet in a zone of limited size. The inversion results in prolific stimulated emission of phonons resonant with the one-phonon transition connecting the doublet states. The phonons are detected via the R 1 luminescence. The angular and spectral distributions of the associated acoustic wave are measured using a geometry with inverted zones at either end of the crystal, one serving as generator and the other as detector. The divergence appears to be governed by the geometry of the zone, while the spectral distribution is, within errors, in keeping with the inhomogeneously broadened phonon transition.
Phonon avalanches resonant with the optically inverted Zeeman-split $\ifmmode \bar{E}\else \={E}\fi{}{(}^{2}E)$ doublet of
Cr3+ have been measured and analyzed in a single crystal of 500-at. ppm ruby
(Al2O3:Cr3+) with a geometry adapted to the study of coherence. A set of coherent Bloch equations governing the interacting acoustic wave and spin polarizations is found to provide an excellent description of the results, and to be far superior to incoherent rate equations for the phonon and level populations. The dephasing time conforms with the width of the inhomogeneously broadened transition connecting the $\ifmmode \bar{E}\else \={E}\fi{}{(}^{2}E)$ states, which indicates that dephasing primarily occurs by the spread in frequencies.
Spatial and, additionally, spectral diffusion of 29-${\mathrm{cm}}^{\ensuremath{-}1}$ phonons trapped in an excited cylindrical region with diameter \ensuremath{\sim}0.1 mm has been investigated under continuous optical pumping of ruby. For 130- and 700-ppm ruby, phonon decay strictly limited by spatial diffusion is reflected in a quadratic dependence of the bottlenecking factor $\ensuremath{\sigma}$ on the excited-state concentration
N∗ up to ${N}^{*}\ensuremath{\sim}3\ifmmode\times\else\texttimes\fi{}{10}^{17}/{\mathrm{cm}}^{3}$. At higher
N∗, attainable in 700- and 2500-ppm ruby, the observed reduction of $\ensuremath{\sigma}$ relative to the second-power dependence, as well as the increased width of the dependence of $\ensuremath{\sigma}$ on magnetic field, reveal that spectral diffusion from inhomogeneous packet to packet is operative. In the spatially diffusive regime, evidence for Zeeman-induced spectral diffusion is found in a characteristic narrowing of the magnetic-field dependence of the
R2 fluorescence upon raising $\ensuremath{\sigma}$. At full separation of the Zeeman transitions $2\overline{A}(^{2}E)\ensuremath{\leftrightarrow}\overline{E}(^{2}E)$, $\ensuremath{\sigma}$ is reduced to 15-40% relative to zero field, depending on
N∗ and ground-state concentration. Rate equations governing the
Cr3+ populations in the two-level scheme (
2A,
E) with inclusion of spatial diffusion and anharmonic decay of the phonons account for the second-power dependence. Diffusive phonon decay turns out to dominate from ${N}^{*}R\ensuremath{\sim}4\ifmmode\times\else\texttimes\fi{}{10}^{13}/{\mathrm{cm}}^{2}$ up to at least ${N}^{*}{R}^{2}\ensuremath{\sim}{10}^{14}/\mathrm{cm}$, with
R the characteristic dimension of the excited region. Spectral diffusion, treated as a perturbation, satisfactorily fits the data at higher $\ensuremath{\sigma}$, yielding a diffusive step of \ensuremath{\sim}2% of the linewidth. At low bottlenecking, the functional form of the magnetic field dependence of $\ensuremath{\sigma}$, including its width and level at full separation, is closely described by use of rate equations, taking the line shape to be Gaussian-type, and assuming the phonons associated with spin flip and those with non spin flip to belong to distinct classes.
Spectral hole burning in the 4A2–2E(2A) zero-phonon line for Cr3+ in Be3Al2(SiO3)6 is reported. Persistent holes with a linewidth of 0.5 GHz were observed when the crystal temperature was below 4 K. The burning is attributed to photoionization of Cr3+ from the 2E state and trapping of the released charge at other sites. The changes in the Coulomb field are the main factors contributing to the hole linewidth. High-resolution axial and transverse Zeeman measurements of the 4A2–2E(2A) transition performed by using the spectral hole are found to be consistent with the known g values.
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.