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Optics and Spectroscopy

Determination of the distribution function of Stark dipole moments induced by a matrix in amorphous impurity systems

G. M. Svishchev

Published Aug 1, 2000• 4 citations
Publisher

Abstract

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.

DOI
10.1134/1.1307437

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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.

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The dependence of spectral holes of dye molecules in amorphous solids on the following parameters has been calculated: the electric field strength, the angles between the hole-burning and probing laser light fields and the external electric field, the electric dipole moment difference Δμm between the excited and ground state of the guest molecule, the contribution Δμ* of the host matrix to the electric dipole moment difference, and the angle γ, between Δμm and the transition dipole moment μge. When the molecular dipole moment difference Δμm dominates the spectral hole broadens or splits into two holes by the application of the electric field, depending on the angle γ and the directions of the laser light fields and the external field. With increasing values of the host-induced electric dipole moment difference Δμ* the spectral hole shape in the electric field changes significantly if appropriate directions of the light fields and the external field are chosen. The material parameters γ, Δμm, and Δμ* can be determined unequivocally by comparing the calculated holes both in the frequency dimension and the electric field dimension with experimental results.

The Journal of Chemical Physics•Jul 15, 1987•27 citations
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.
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.
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.
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.
Persistent spectral hole-burning (PSHB) is a versatile tool to study Stark effect in solids where impurity spectra is strongly inhomogeneously broadened. At liquid helium temperatures impurity homogeneous zero-phonon line widths are small (γhom~10–2-10–4cm–1) and narrow holes can be burnt in the inhomogeneous distribution by illumination with narrow band laser(Δνlaser < γhom) U1- Stark effect alters the shape of narrow spectral holes depending on the Stark shift (splitting) of impurity energy levels, orientation of the impurities, strength and orientation of the electric field, as well as on the properties of the matrix [2].
The dependence of spectral holes of dye molecules in amorphous solids on the following parameters has been calculated: the electric field strength, the angles between the hole-burning and probing laser light fields and the external electric field, the electric dipole moment difference Δμm between the excited and ground state of the guest molecule, the contribution Δμ* of the host matrix to the electric dipole moment difference, and the angle γ, between Δμm and the transition dipole moment μge. When the molecular dipole moment difference Δμm dominates the spectral hole broadens or splits into two holes by the application of the electric field, depending on the angle γ and the directions of the laser light fields and the external field. With increasing values of the host-induced electric dipole moment difference Δμ* the spectral hole shape in the electric field changes significantly if appropriate directions of the light fields and the external field are chosen. The material parameters γ, Δμm, and Δμ* can be determined unequivocally by comparing the calculated holes both in the frequency dimension and the electric field dimension with experimental results.