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Zero-Phonon Lines in the Spectroscopy and Photochemistry of Impurity-Doped Solid Matter

Estonian Ssr

Published Jan 1, 1988• 0 citations
OpenAlex

Abstract

A brief account of zero-phonon lines in the low-temperature spectra of impurity atoms and molecules in solid matrices - crystals, glasses, polymers - is given. Inhomoge­ neous broadening, its elimination and applications by photoburning of spectral holes are considered. Some remarks on the history and future of the topics are made. A va­ riety of physicists, chemists, biologists, applied spectroscopists and also data pro­ cessing specialists are considered as potential readers.

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A brief account of zero-phonon lines in the low-temperature spectra of impurity atoms and molecules in solid matrices - crystals, glasses, polymers - is given. Inhomoge­ neous broadening, its elimination and applications by photoburning of spectral holes are considered. Some remarks on the history and future of the topics are made. A va­ riety of physicists, chemists, biologists, applied spectroscopists and also data pro­ cessing specialists are considered as potential readers.
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.
The low temperature spectra of absorption and luminescence of a wide variety of impurity doped organic and inorganic solids comprise very narrow (io 1O cm1) and intense zero-phonon lines (zPL). They arise from the purely electronic transistions in the impurities i.e. from the changes of the electronic state not accompanied by creation or annihilation of the phonons of the host solid. (ZPL may be called the optical analog of the M5sbauer line), Because of their narrowness ZPL's are very sensitive to even very slight differences in the crystal fields at the 1oca tions of impurities and the ZPL spectruim of a body of impu.rities displays a large inhomogeneous broadening (formula available on paper).
Spectroscopies of matrix isolated species and impurity activated solids are close relatives. Both are among the well developing chapters of solid state spectroscopy and optics. In this paper I am trying to give very brief overview what has been achieved in science and applications of impurity activated solids based on zero-phonon lines (ZPLs) in optical data storage and processing. I would like to show that the latter comprises via persistent spectral hole burning time-and-space domain holography in a certain meaning also the "stopping of light". ZPLs are beginning to play a role in the approaches to optical quantum computing.
In this work, we study the relation between the widths of the zero-phonon lines (ZPL) of single impurity molecules (SM) in solid matrices with local effective values of the refractive index n. Since at ultralow temperatures the width of SM ZPL is determined mainly by the radiative lifetime T1, while the local-field effects produce the function T1(n), SM spectroscopy makes it possible to measure the distribution of n local values in solids. The approach proposed here for studying local fluctuations of n has been tested on the example of doped polymers and molecular crystals.
Zero-phonon lines in impurity optical spectra and their inhomogeneous broadening are discussed. Photoburning of persistent spectral holes is not only an effective method to eliminate the inhomogeneous broadening and perform high resolution spectroscopy, but it serves also as a powerful tool to control by means of illumination the absorption coefficient and refractive index of the matter. It opens new horizons for frequency-selective optical memories, data storage and data processing. Hole burning by picosecond pulses and the time-and space-domain holography based on it are discussed and the results of the experiments described.
The photoselection of impurity molecules caused by spectral hole burning produces a specific spectral angular distribution of the molecules in low-temperature amorphous matrices: All the molecules, whose zero-phonon absorption lines lie within a selected narrow spectral interval, have a specified distribution of their orientations relative to the laboratory coordinate system. In this paper, the possibility of application of known methods of hole burning in this spectral interval is studied and the outlook for combination of these methods with preliminary photoselection is demonstrated by the example of the Stark effect.