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Physical review. B, Condensed matter

Optically generated pseudo-Stark effect in ruby

P. F. Liao, Alexander M. Glass, L. M. Humphrey

Published Sep 1, 1980• 36 citations
Publisher

Abstract

We report observations of an optically produced splitting of the luminescence lines of concentrated ruby samples for optical intensities of approximately 200 W/${\mathrm{cm}}^{2}$. This splitting is attributed to optical generation of a large, uniform electric field (${10}^{6}$ V/cm). At high intensities ($l>2$ kW/${\mathrm{cm}}^{2}$) high photoconductivity causes the splitting to decrease and disappear. It is suggested that the field-generation mechanism is directional charge transfer via two-step excitation of ${\mathrm{Cr}}^{3+}$ ion or ion clusters. The required electrical asymmetry is shown to be due to a growth-induced anisotropy of the ${\mathrm{Cr}}^{3+}$ ion distribution.

DOI
10.1103/physrevb.22.2276

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Physical review. B, Condensed matter•May 1, 1992•25 citations
We report observations of an optically produced splitting of the luminescence lines of concentrated ruby samples for optical intensities of approximately 200 W/cm2{\mathrm{cm}}^{2}cm2. This splitting is attributed to optical generation of a large, uniform electric field (106{10}^{6}106 V/cm). At high intensities (l>2l>2l>2 kW/cm2{\mathrm{cm}}^{2}cm2) high photoconductivity causes the splitting to decrease and disappear. It is suggested that the field-generation mechanism is directional charge transfer via two-step excitation of Cr3+{\mathrm{Cr}}^{3+}Cr3+ ion or ion clusters. The required electrical asymmetry is shown to be due to a growth-induced anisotropy of the Cr3+{\mathrm{Cr}}^{3+}Cr3+ ion distribution.
A pseudo-Stark splitting of the ${B}_{1}(20993 {\mathrm{cm}}^{\ensuremath{-}1})$ and the ${B}_{2}(21068 {\mathrm{cm}}^{\ensuremath{-}1})$ absorption lines in ruby has been observed at 2\ifmmode^\circ\else\textdegree\fi{}K. The splitting of each BBB line is 2.8\ifmmode\times\else\texttimes\fi{}${10}^{\ensuremath{-}5}$ ${\mathrm{cm}}^{\ensuremath{-}1}$/V/cm for an electric field parallel to the ccc axis. This is a factor 3.7 larger than the corresponding splitting of the RRR lines. There is no observable effect for fields perpendicular to the ccc axis. Crystal-field theory satisfactorily predicts these properties, which are determined by the symmetry of the Cr3+{\mathrm{Cr}}^{3+}Cr3+ site. The point-charge model does not correctly predict the absolute value of the observed electric splitting, nor the matrix elements of the BBB lines.
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.
The ruby R2{R}_{2}R2​-line intensity at 2.1 K is observed to be nearly quadratically depedent on the R1{R}_{1}R1​ intensity, indicative of strongly bottlenecked 29-${\mathrm{cm}}^{\ensuremath{-}1}$ phonons generated by the $2\overline{A}(^{2}E)\ensuremath{\rightarrow}\overline{E}(^{2}E)$ decay in the optical pumping cycle. The spectral width of the phonon excitation is probed by separating the degenerate phonon packets in a magnetic field and monitoring the decrease of the bottlenecking.
Absorption transitions between two excited optical states in ruby have been studied by comparing the absorption coefficients measured under optically pumped and unpumped conditions. The spectrum has been determined in the π-and σ-polarizations in the photon energy range from 5,500 to 45,000 cm -1 . Several absorption bands have been found which arise from the transitions from the excited states t 2g 3 2 E g and t 2g 3 2 T 1g of the Cr 3+ ion. From the locations and intensities of these bands, the terminal states of the observed transitions are assigned to the charge transfer state, the t 2g 3 2 T 2g state, and the doublet states belonging to the electron configuration t 2g 3 e g . Calculated energies between these states and the metastable states, t 2g 3 2 E g and t 2g 3 2 T 1g , are in good agreement with the peak energies of the observed absorption bands. The present experiment gives new information inaccessible by the ordinary ground state absorption measurement, such as the locations of several doublet states with the configuration t 2g 2 e g and the intensities of doublet-doublet transitions in ruby.
We have found that the amplitudes of the optical FID, two-pulse photon echoes and stimulated photon echoes in ruby measured as a function of applied magnetic field exhibit sharp increases at the magnetic fields where two Zeeman splittings in the ground state 4 A 2 or in the excited state \bar E ( 2 E ) are harmonically related. The phenomena are confirmed to be inherent in the Stark (or frequency) switching experiment where the sample is subjected to the cw irradiation, and the origin of the sharp increases be the change of the steady state population in 4 A 2 of the nonresonant Cr ions caused by a combined action of the cw optical pumping and the spin-spin cross relaxation. The mechanism involved is successfully explained by the analysis based on the rate equations.
We describe and demonstrate a method for performing ultrahigh-resolution optical spectroscopy in the time domain which utilizes modulations in the intensity of the two-pulse photon echo in the presence of a perturbation that splits the optical transition frequencies of two or more subgroups of ions. The method is applied to a measurement of the pseudo-Stark effect in alexandrite and YAlO3{\mathrm{YAlO}}_{3}YAlO3​:Er3+{\mathrm{Er}}^{3+}Er3+. Stark shifts of \ensuremath{\simeq}100 kHz are observed, but the technique is capable of resolutions 10 kHz in some systems.