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Le Journal de Physique Colloques

EXCITED STATE ELECTRON SPIN RESONANCE USING NON-RESONANT FLUORESCENCE LINE NARROWING

D. J. Sox, Sara A. Majetich, John E. Rives, Richard S. Meltzer

Published Oct 1, 1985• 1 citation
Publisher

Abstract

Non-resonant fluorescence line narrowing (FLN) is used to examine resonances between excited states of ions. We discuss resonances between crystal field states in ruby, alexandrite and LaF3 : Pr3+ and between Zeeman sublevels in LaF3 : Er3+. We show that the latter is equivalent to excited state ESR, over which it can have many advantages.

DOI
10.1051/jphyscol:1985788

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Journal of the Physical Society of Japan•Jul 15, 1981•3 citations
Non-resonant fluorescence line narrowing (FLN) is used to examine resonances between excited states of ions. We discuss resonances between crystal field states in ruby, alexandrite and LaF3 : Pr3+ and between Zeeman sublevels in LaF3 : Er3+. We show that the latter is equivalent to excited state ESR, over which it can have many advantages.
A technique involving the laser-induced narrowing of a fluorescence line is used to obtain high-resolution spectra of Pr3+:LaCl3. The second-order effects caused by Zeeman and nuclear interactions are systematically investigated in the 3H4E2 to or from 1D2A1 transition. A non-zero perpendicular Zeeman splitting of the ground level, proportional to the square of the magnetic field, is measured and interpreted as being caused by the perturbation by the four upper Stark levels belonging to the 3H4 multiplet. The variation of the number and of the relative intensities of the hyperfine lines is demonstrated to be closely related to the angle between the external magnetic field direction and the crystal axis. It is unambiguously attributed to an angular dependence, with regard to the magnetic field direction, of the hyperfine states of the excited level. The importance of the effect, caused by a very distant perturbing level, is shown to be a result of the quasidegeneracy of the mu =0 excited level.
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.
A large number of small but sharp changes (increases and decreases) of the R 1 fluorescence in ruby are observed as a function of applied magnetic field between 2 K and 77 K. At liquid helium temperatures, these signals have linewidths much narrower than the inhomogeneous linewidth (∼0.1 cm -1 ) of the R 1 line. All of these signals appear at the fields where the Zeeman splittings in the excited state \bar E ( 2 E ) and the ground state 4 A 2 satisfy an energy-matching condition for simultaneous transitions of two or more ions. Two distinct mechanisms are found to be responsible for the signals: spin-spin cross-relaxation between \bar E ( 2 E ) and 4 A 2 , and resonant self-trapping of the R 1 line. From the temperature dependence of the linewidths of the signals, thermal broadening of \bar E ( 2 E ) is measured below 77 K. Similar signals are observed in the N lines due to energy transfer from isolated ions to pairs.