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Optics and Spectroscopy

Photoselection of impurity molecules with respect to the orientation of their stark moments induced by an amorphous matrix

G. M. Svishchev

Published Jan 1, 2003• 1 citation
Publisher

Abstract

A method of selective (relative to the magnitude of the linear Stark effect in zero-dipole impurity molecules) burning of holes in the spectra of amorphous matrices is studied. It is shown that this method makes it possible not only to select a subensemble of impurity molecules having both preset energy of the 0-0 transition and magnitude of the matrix-induced Stark moment, but also to divide this subensemble into two fractions whose Stark moments are predominantly oriented either along the transition moment or perpendicular to it. The possibility of experimental verification of the most popular hypothesis about the origin of induced Stark moments, which neglects a possible correlation between the direction of the Stark moment and that of the transition dipole moment, is considered. The method described also allows one to study experimentally the correlation of some other photophysical parameters of impurity molecules with the direction of local internal fields relative to the vector of the transition dipole moment.

DOI
10.1134/1.1540193

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Journal of the Optical Society of America B•Jun 1, 1992•2 citations
A method of selective (relative to the magnitude of the linear Stark effect in zero-dipole impurity molecules) burning of holes in the spectra of amorphous matrices is studied. It is shown that this method makes it possible not only to select a subensemble of impurity molecules having both preset energy of the 0-0 transition and magnitude of the matrix-induced Stark moment, but also to divide this subensemble into two fractions whose Stark moments are predominantly oriented either along the transition moment or perpendicular to it. The possibility of experimental verification of the most popular hypothesis about the origin of induced Stark moments, which neglects a possible correlation between the direction of the Stark moment and that of the transition dipole moment, is considered. The method described also allows one to study experimentally the correlation of some other photophysical parameters of impurity molecules with the direction of local internal fields relative to the vector of the transition dipole moment.
A method of selective (with respect to the Stark effect) burning of a spectral hole in the 0-0 absorption band of zero-dipole impurity molecules is suggested. It is shown that in combination with the Stark modulation of the optical density of a sample, this method makes it possible to determine that contribution to the total absorption and luminescence of the sample that the impurity molecules with a preset magnitude of the matrix-induced Stark moment (provided this magnitude exceeds the mean value for the entire ensemble) make. This allows one to experimentally study both the distribution of impurity molecules over the magnitude of the Stark moment and the correlation of the Stark moment with other parameters of impurity molecules.
The burning kinetics of closely spaced equidistant holes in impurity absorption spectra of glasses and polymers is theoretically studied in an alternating electric field (alternating in the magnitude, sign, and direction). The height of barriers between wells of the burnt multiwell spectral hole depends on the shape of the distribution of impurity molecules over the Stark dipole moments. Centrally symmetric impurity molecules are considered whose Stark moment is determined exclusively by the interaction with matrix molecules. Model calculations performed for different hypothetical distribution functions of Stark moments yield substantially different kinetics. Therefore, the method described allows one to verify experimentally various hypotheses about the nature of matrix-induced Stark moments.
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.
Burning of multiwell holes in impurity-absorption spectra of glasses and polymers in an alternating electric field was theoretically studied. A case of circularly polarized burning radiation with a spectrum consisting of a series of close equidistant lines that shift synchronously with the variation of the electric field across the sample was considered. It was shown that an electric field applied to the sample after hole burning changes the optical density in the hole center, and that this change depends on the orientation of the plane of polarization of the probing radiation. Centrosymmetric impurity molecules, whose Stark moments (with randomly distributed magnitudes and directions) are governed only by their interaction with matrix molecules, and molecules with small intrinsic permanent Stark moments were considered. It was shown that the measurements of electric dichroism of a multiwell spectral hole make it possible to study both the anisotropy of matrix-induced moments and additional moments that arise, for example, when a metal atom leaves the plane of a metalloporphyrin molecule. It was also shown that the sensitivity and selectivity of the suggested method exceed those of known methods.
The constructive interference between two Stark-effect-broadened holograms produced by spectral hole burning is discussed. The holograms are burned at the same frequency but at different external electric-field values. The phase difference is selected to be zero so that constructive interference between the waves diffracted by each grating occurs. Experimentally it is found that a dip in the hologram efficiency that is not predicted by previous theory occurs for all reconstruction external electric-field values in the region between the original burn values. This dip is interpreted as being due to the time nonlinearity of the hologram burn process. The dip corresponds to those molecules, oriented in a specific direction with respect to the electric field, for which no Stark shift occurs and that are therefore resonant with the laser during the production of both holograms. The width of the anomalous feature is close to that of the hologram when the hologram is reconstructed at the original burn external electric-field strength. Other molecular orientations may be selected by burning pairs of holographic gratings at other combinations of the frequency and the electric field.