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Journal of Luminescence

Homogeneous line broadening of optical transitions of ions and molecules in glasses

R. M. Macfarlane, Robert M. Shelby

Published Jan 1, 1987• 240 citations
Publisher
DOI
10.1016/0022-2313(87)90194-3

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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.
The spectral diffusion theory developed for explaining the logarithmic temporal broadening of the optical line of an individual impurity center and based on spontaneous tunnel transitions in a polymer or glass is supplemented by taking into account the tunnel transitions occurring in the center itself upon the absorption of a photon. This light-induced additional tunneling leads to a sharp temporal broadening of the optical line from an individual impurity molecule occurring against the background of a slower logarithmic line broadening. It is shown that the inclusion of light-induced tunneling can explain the difference in the temporal line broadening of three individual Terylene molecules introduced in polyethylene, which was measured in experiments by the group headed by M. Orrit [A. M. Boiron et al. , Chem. Phys. 247 , 119 (1999)].
Numerous experimental investigations of homogeneous line broadening (Γh) of RE3+ ions in crystals and glasses in frequency and time domain [1] have shown that Γh for glasses exceed those for crystals by more than one order of magnitude at low temperatures (T) for the same ions and transitions. Discrepancies between theory and experimental results make it difficult to determine an influence of host disordering on the Γh in a wide temperature range. In this work we measured and compared Γh, values for ordered CaF2 and disordered CaF2-YF3 crystals doped with Nd3+ ions.