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Japanese Journal of Applied Physics

Determination of Ruby R-Lines Profile by Tunable Dye Laser

Yoshitoshi Noda

Published Feb 1, 1988• 1 citation
Publisher

Abstract

The R-line profile in a ruby of chromium concentration=0.065 wt% was determined by a nitrogen laser-pumped nile blue dye laser (spectral resolution=0.01 nm). This profile is much clearer than that obtained by the usual spectrometer method, and shows no splitting of the line in R1-line center (694.3 nm) at room temperature. The numerical value of the absorption coefficient α obtained by this method is compared with that of the other method.

DOI
10.1143/jjap.27.334

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The R-line profile in a ruby of chromium concentration=0.065 wt% was determined by a nitrogen laser-pumped nile blue dye laser (spectral resolution=0.01 nm). This profile is much clearer than that obtained by the usual spectrometer method, and shows no splitting of the line in R1-line center (694.3 nm) at room temperature. The numerical value of the absorption coefficient α obtained by this method is compared with that of the other method.
Virtually simultaneous measurements of the emission and absorption profiles of the ruby R1 line show that no significant Stokes' shift is present. Observations were made on rubies of 0.0055% and 0.0186% Cr by weight with both crystallographic orientations and both polarizations in the temperature range from 77° to 153°K. The position of the peaks in the absorption line matched those of the emission line to within 0.002 cm−1. Shifts of this size or smaller cause no significant change in the operating characteristics of a laser.
Laser-induced fluorescence line narrowing of the ruby R1{R}_{1}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{10}^{7}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.
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{R}_{1}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 RRR 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.
The real and imaginary parts of the complex index of refraction have been measured in the R1 line of optically pumped ruby. The experiments, which employed a temperature-controlled, single-mode ruby laser as a variable-frequency monochromatic source, were performed near liquid-nitrogen temperature, where the R1 doublet structure is well resolved. R1 absorption profiles were measured for several optical-pumping conditions, ranging from zero up to a pump power that excited a population in the 2E state equal to about 60% of the population of the 4A2 ground state. For each pumping condition, the anomalous-dispersion curve was measured interferometrically. The spectral profiles of the absorption coefficient and the anomalous dispersion display a dependence on the optical-pumping conditions that is more complicated than simple saturation of the R1 transitions, but for given pumping conditions the two quantities are correlated as predicted by the Kramers–Kronig relations.
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.
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.