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physica status solidi (a)

Lifetimes of laser-induced population density gratings in ruby

Hans Joachim Eichler, Jürgen Eichler, J. Knof, Ch. Noack

Published Apr 16, 1979• 36 citations
Publisher

Abstract

A spatially periodic distribution of excited electronic states is produced in ruby which is placed into the interference region of two light beams derived from a pulsed laser (wavelength 530 nm). The spatially modulated population density acts like an optical grating and is detected by diffraction of a quasi-cw laser beam (488 nm). The lifetimes of the population density gratings are measured for ruby crystals with 0.05 to 5% Cr-doping and compared with the fluorescence lifetimes of the R-lines (694 nm). For the 0.05% ruby both lifetimes are nearly equal. At higher Cr-concentrations the grating decay is considerably faster than the fluorescent decay. The grating lifetimes are independent of the grating period A = 1 to 100 μm. From this observation an upper limit of the diffusion constant for energy transfer between excited electronic states in ruby is estimated.

DOI
10.1002/pssa.2210520216

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Annual Meeting Optical Society of America•Jan 1, 1988•0 citations
A spatially periodic distribution of excited electronic states is produced in ruby which is placed into the interference region of two light beams derived from a pulsed laser (wavelength 530 nm). The spatially modulated population density acts like an optical grating and is detected by diffraction of a quasi-cw laser beam (488 nm). The lifetimes of the population density gratings are measured for ruby crystals with 0.05 to 5% Cr-doping and compared with the fluorescence lifetimes of the R-lines (694 nm). For the 0.05% ruby both lifetimes are nearly equal. At higher Cr-concentrations the grating decay is considerably faster than the fluorescent decay. The grating lifetimes are independent of the grating period A = 1 to 100 μm. From this observation an upper limit of the diffusion constant for energy transfer between excited electronic states in ruby is estimated.
The unique optical properties of the ruby crystal that make it effective as a lasing medium were measured using a simple optical setup.Ruby's absorption of visible light was shown to be strongest at 420 and 550 nm, corresponding to its physical appearance as transparent pink.While the ruby crystal was illuminated with a 532 nm green laser, the R-line fluorescence peaked at 693.5 ± 1.1 nm.Finally, the fluorescence lifetime of ruby was measured by pulsing the laser with a signal generator and capturing the decaying fluorescence on a digital oscilloscope using a photodiode.An exponential decay time-constant of 3.6 ± 0.1 ms was obtained, corresponding to the fluorescence lifetime.
Direct measurements of the diffusion distance of E‾(2E)\overline{E}(^{2}E)E(2E) state excitation by time-resolved degenerate four-wave mixing in ruby are reported. Measurements are made on crystals with Cr3+{\mathrm{Cr}}^{3+}Cr3+ concentrations varying between 0.05 and 1.55 at.% at 10\ifmmode^\circ\else\textdegree\fi{}K. In all cases an upper limit of 30 nm is determined for the diffusion distance within the fluorescence lifetime.
Frequency-domain optical hole burning of the R1{\mathit{R}}_{1}R1​ line [4{[}^{4}[4A2{\mathit{A}}_{2}A2​(-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. % Cr2{\mathrm{Cr}}_{2}Cr2​O3{\mathrm{O}}_{3}O3​) 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.
Using resonance ruby-laser excitation, narrowing of the ruby R1{R}_{1}R1​ fluorescence line to width 0.002 ${\mathrm{cm}}^{\ensuremath{-}1}$ at 4.2\ifmmode^\circ\else\textdegree\fi{}K is observed. Absence of spectral diffusion indicates that a short-range interaction rather than earlier postulated multipolar interactions is responsible for energy transfer in concentrated ruby.
Laser-induced grating measurements were made as a function of laser power and write beam crossing angle for various temperatures between 10 and 300 K on Cr3+ ions in Gd3Ga5O12 (GGG), Gd3Sc2Ga3O12 (GSGG), and GGG mixed with Ca, Mg, and Zr ions. Population gratings were produced in the Cr3+ ions, and the diffusion coefficient describing energy migration among the Cr3+ ions was determined from the grating decay rate. The energy migration was found to increase as the temperature was raised for GGG and to decrease with decreasing temperature for GSGG. This difference is attributed to the differences in the crystal field splittings of the excited states in the two hosts. Enhanced energy diffusion was observed in the multiply doped GGG sample. Contributions to the laser-induced gratings from absorption and dispersion changes were determined, and this was used to provide information on radiationless relaxation and excited state absorption processes. For long writing times, long-lived changes in the refractive index were observed and attributed to optically induced color centers.