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Journal of the Physical Society of Japan

Absorption Spectra of Cr3+ in Al2O3 Part B. Experimental Studies of the Zeeman Effect and Other Properties of the Line Spectra

Satoru Sugano, Ikuji Tsujikawa

Published Aug 1, 1958• 173 citations
Publisher

Abstract

The absorption intensities, widths and wave-numbers of R 1 , R 2 and B 1 B 2 lines of Cr 3+ in ruby for the polarized light E ⊥ C 3 and E // C 3 are experimentally studied at 20°K and 4.2°K. Zeeman effect is also studied, using a magnetic field H 0 =24,000 φ, for both R and B lines. The Zeeman effect has not been observed yet for the B lines, while Lehmann has already observed the Zeeman effect for R lines. In our results of R lines, the quantitative aspects of Lehmann's experiment are improved. The comparison is made with the theoretical results given in Part A and it is shown that nice agreements can be obtained when suitable assignments of the spectra are adopted and when fairly large g -shifts of the excited states are introduced.

DOI
10.1143/jpsj.13.899

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Physical Review B•May 17, 2011•3 citations
The absorption intensities, widths and wave-numbers of R 1 , R 2 and B 1 B 2 lines of Cr 3+ in ruby for the polarized light E ⊥ C 3 and E // C 3 are experimentally studied at 20°K and 4.2°K. Zeeman effect is also studied, using a magnetic field H 0 =24,000 φ, for both R and B lines. The Zeeman effect has not been observed yet for the B lines, while Lehmann has already observed the Zeeman effect for R lines. In our results of R lines, the quantitative aspects of Lehmann's experiment are improved. The comparison is made with the theoretical results given in Part A and it is shown that nice agreements can be obtained when suitable assignments of the spectra are adopted and when fairly large g -shifts of the excited states are introduced.
The Zeeman effect of the B and R absorption lines of ruby was observed photographically with strong pulsed magnetic fields up to 230 kOe at 77°K. This was achieved by flashing a Xe-lamp at the time when a magnetic field reached its peak. The duration of the pulsed field was made to be about 1 m sec which was much longer than that of the pulsed light, about 20 µ sec. The g -values of the excited states responsible for the B and R lines were measured and the comparison was made with those reported by other authors. For the Zeeman patterns of the R lines with magnetic fields perpendicular to the optic axis, the Paschen-Back effect was calculated and compared with the observed patterns.
The Zeeman effect of R-absorption lines in ruby was observed in a high pulsed magnetic field up to 520 kOe using an optical multichannel analyzer. The experiment was done under a thermal equilibrium condition ( T =130 K) and the Zeeman line intensity is satisfactorily explained. When a magnetic field is applied perpendicular to the C 3 -axis, the excited \barE and 2\barA states show a level mixing and the observed pattern indicates a clear Paschen-Back effect The observed g // -values of the excited states are -2.49±0.05 and 1.49±0.05 for \barE and 2\barA, respectively. g ⊥ -values for these levels were estimated to be smaller than 0.1 at 500 kOe.
The optical spectrum due to the exchange coupled Cr 3+ ions in ruby has been studied theoretically. The effect of the lowering of the Cr 3+ site symmetry due to the formation of a pair was taken into account. For the 2nd neighbor pair, a good fitting of the excited state energies between theory and experiment was obtained. The effect of the higher order exchange is found to be very important for this pair. It is also found that the deviation of the Cr 3+ site symmetry from C 3 is rather large for this pair. For the 4th neighbor pair, the level diagram of the excited state was obtained and the absorption intensities were calculated. Most of the observed lines in this pair are explained by this theory. The lines so called N 1 and N 2 are found to be the transitions due to the exchange induced electric dipole.
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.
The paramagnetic resonance properties of Cr+++ions in Al2O3(ruby) were investigated theoretically and experimentally in order to obtain information necessary for the application of this material as active material in a three-level solid-state maser (3LSSM). Numerically computed energy levels, together with their associated eigenvectors, are presented as a function of applied magnetic field for various orientations of the magnetic field with respect to the crystalline symmetry axis. A more detailed discussion is devoted to energy levels, eigenvectors and transition probabilities at angles O°, 54.74° and 90°, where certain simple relations and symmetries hold. Paramagnetic spectra for signal frequencies between 5 and 24 kmc are shown; agreement between computed and measured resonance fields is satisfactory.
Doubly resonant Raman electron paramagnetic transitions in ruby (Al2{}_{2}2​O3{}_{3}3​:Cr3+{}^{3+}3+) have been investigated using dye laser excitation tuned across the range of the Zeeman components of its well-known R1{R}_{1}R1​ emission line. With magnetic field B normal to c, the optic axis of ruby, it is seen that the Raman electron paramagnetic resonance (EPR) lines exhibit significant intensity enhancements due to the simultaneous occurrence of ``in resonance'' and ``out resonance,'' as visualized in the Kramers-Heisenberg formalism of inelastic light scattering. The specific Raman EPR features observed in the present study, together with their resonances, however, differ markedly from those observed in our previous investigation with $\mathbf{B}\ensuremath{\parallel}\mathbf{c}$. These differences can be traced to level mixing effects within the Zeeman multiplet of the 4A2{}^{4}{A}_{2}4A2​ (ground) state on the one hand, and the negligible value of ${g}_{\ensuremath{\perp}}$ for the $\mathrm{E\ifmmode \bar{}\else \={}\fi{}}$ (excited) state of the R1{R}_{1}R1​ emission line on the other. Furthermore, we note that with B\ensuremath{\perp}c and under resonant conditions, the experimentally observed \ensuremath{\Delta}mmm === \ifmmode\pm\else\textpm\fi{}1 pair of Stokes and anti-Stokes Raman lines are not connected by time-reversal symmetry.