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Journal de Physique Lettres

Interaction strength of weakly coupled pairs measured by a two laser spectroscopy technique

Jean‐Claude Vial, R. Buisson

Published Jan 1, 1982• 32 citations
Publisher

Abstract

When the coupling between two ions associated in pair exceeds a given value, the excitation of both ions of the pair is impossible when using a single narrow laser. This double excitation was obtained with two lasers of different wavelengths. A narrowing of the inhomogeneous broadened lines is observed which gives information on the strain field in the crystal. From the difference between the wavelengths, the order of magnitude of the coupling is deduced and compared with phonon assisted transfer rates.

DOI
10.1051/jphyslet:019820043010033900

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When the coupling between two ions associated in pair exceeds a given value, the excitation of both ions of the pair is impossible when using a single narrow laser. This double excitation was obtained with two lasers of different wavelengths. A narrowing of the inhomogeneous broadened lines is observed which gives information on the strain field in the crystal. From the difference between the wavelengths, the order of magnitude of the coupling is deduced and compared with phonon assisted transfer rates.
Using the energy level shift induced by a Nd3+ ion on a neighbour ion, the selective excitation of a class of (Nd, Nd) pairs is possible in weakly doped samples with a spectrally narrow laser. The observation of an anti-Stokes fluorescence shows that a pair can absorb two photons. From experiments with a magnetic field, it is shown that using a single laser, the double excitation of moderatly coupled pairs is essentially induced by a double quantum process by which two photons are simultaneously absorbed. The strongly coupled pairs, on the contrary, can only be doubly excited by two lasers of different frequencies. Orders of magnitude of the coupling strength between the two ions are deduced from the difference between these frequencies.
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 electron-phonon coupling for Cr 3+ in different oxide host lattices (MgO, α-Al 2 O 3 and LaAlO 3 ) was probed by performing temperature dependent line broadening measurements for zero-phonon emission lines of single ions and exchange coupled pairs. No differences in electron-phonon coupling were found comparing the results for pairs and single ions in α-Al 2 O 3 (3NN and 4NN pairs) and LaAlO 3 (NN pairs). In Cr 3+ doped MgO (Cr 3+ -V Mg -Cr 3+ pairs), it was found that the electron-phonon coupling strength parameter is larger for the pairs than for the isolated Cr 3+ ions. This is probably due to changes in the surroundings of Cr 3+ by local charge compensation by a magnesium vacancy, and not to interaction between the Cr 3+ ions.
Remarkably narrow optical homogeneous linewidths of the order of 1 kHz have now been observed in low temperature zero‐phonon transitions of dilute impurity ion crystals, such as Pr3+ in LaF3. Novel nonlinear optical resonance techniques have been devised for this purpose using ultrastable phase locked cw dye lasers where the measurements are performed either in the frequency domain (hole burning) or in the time domain (coherent optical transients). These studies effectively bring the Mossbauer effect into the optical region. Hence, the observed linewidths are no longer limited by inhomogeneous strain broadening (∼5 GHz) or even by static local fields due to neighboring spins (∼100 kHz). However, weak magnetic field fluctuations from local spins are readily detected. As an example, spin decoupling and line narrowing, which are well known in NMR, are observed in an optical transition of Pr3+:LaF3 at 2 K where the 19F– 19F dipolar interaction is quenched and the optical linewidth drops from 10 to 2 kHz, clearly demonstrating the spin broadening mechanism. Results will be discussed in terms of a Monte Carlo line broadening theory.
Abstract A history of the development of selective laser spectroscopy is presented, beginning with a pioneering work by Yu. V. Denisov and V. A. Kizel in 1967, who were the first to demonstrate the possibility of removing the inhomogeneous broadening of luminescence spectra of impurity ions in glasses upon monochromatic resonance excitation. Selective excitation of optical centers can be achieved due to existence of zero-phonon transitions corresponding to narrow homogeneous zero-phonon lines in the spectra of impurity centers in solids, which are hidden in broad inhomogeneous optical bands upon usual nonselective excitation. The fundamentals of zero-phonon transition spectroscopy are considered and the mechanism of removing the inhomogeneous broadening of optical spectra of ions and molecules in crystals and amorphous solids under selective laser excitation of luminescence and persistent hole burning in absorption spectra is presented in detail. Various applications of selective laser spectroscopy for fundamental and applied studies are discussed.