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Springer eBooks

Quantum Theory of Laser Field Effects on Impurity Ion Relaxation in Crystals: Applications to Transient Spectroscopy

Pavel A Apanasevich, S. Ya. Kilin, Alexander P. Nizovtsev, N. S. Onishchenko

Published Jan 1, 1991• 0 citations
Publisher
DOI
10.1007/978-1-4615-3726-7_53

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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.

Physica Scripta•Jan 11, 2018•0 citations
The frequency-field and orientation dependences of the electron paramagnetic resonance (EPR) spectra are measured for impurity Tm 3+ ions in yttrium orthosilicate (Y 2 SiO 5 ) single crystals by stationary EPR spectroscopy in the frequency range of 50–100 GHz at 4.2 K. The position of the impurity ion in the crystal lattice and its magnetic characteristics are determined. The temperature dependences of the spin–lattice and phase relaxation times are measured by pulse EPR methods in the temperature range of 5–15 K and the high efficiency of the direct single-phonon mechanism of spin–lattice relaxation is established. This greatly shortens the spin–lattice relaxation time at low temperatures and makes impurity Tm 3+ ions in Y 2 SiO 5 a promising basis for the implementation of high-speed quantum memory based on rare-earth ions in dielectric crystals.
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.