Optical hole burning and spectral diffusion in ruby.

Abstract

Frequency-domain optical hole burning of the ${\mathit{R}}_{1}$ line ${[}^{4}$${\mathit{A}}_{2}$(-1/2)\ensuremath{\leftrightarrows}E\ifmmode\bar\else\textasciimacron\fi{}(-1/2) transition] in dilute ruby is studied at 2 K and with a field of 3.6 kG applied along the c axis. A pump-probe (PP) technique is used with precise probe-frequency shifting obtained by an acousto-optic modulator. For sufficiently short PP pulses (50 \ensuremath{\mu}s), two holes (narrow and wide) are observed. The narrow (\ensuremath{\sim}20 kHz half width at half maximum at low power) hole-width dependence on Rabi frequency approximately agrees with that inferred from free-induction-decay measurements. For the present concentration (0.0034 wt. % ${\mathrm{Cr}}_{2}$${\mathrm{O}}_{3}$) and field, the narrow hole width is determined by fluctuating fields produced by Cr-Cr spin flips [A. Szabo, T. Muramoto, and R. Kaarli, Phys. Rev. B 42, 7769 (1990)]. When the PP delay time is varied, the amplitude of the narrow hole decays with a 1/e time constant of \ensuremath{\sim}300 \ensuremath{\mu}s compared to the E\ifmmode\bar\else\textasciimacron\fi{} fluorescence lifetime of 4 ms. The wide hole (\ensuremath{\sim}500 kHz half width at half maximum) is due to Al-Cr superhyperfine interactions and is created by a spectral diffusion mechanism driven by Al-spin flipping in the host lattice.