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Spectral Hole-Burning and Related Spectroscopies: Science and Applications

Stark Effect on Persistent Spectral Holes Measured by Electric Field Modulation Technique

Toshiyuki Shimada, Hiroyuki Suzuki

Published Jan 1, 1991• 0 citations
Publisher

Abstract

An external field applied to dye doped polymers which have inhomogeneous dispersion in their absorption spectra causes a shift in the absorption of the dye molecules. This, in turn, changes the line shapes of persistent spectral holes1). The Stark effect has been applied to optical storage2) and optical computing3). It has been also used as a powerful tool for investigating such physical profiles of materials as the difference between the effective molecular electric dipole moments in the host matrix in the ground and excited states which is related to hole burning4),5).

DOI
10.1364/pshb.1991.fe11

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Applied Physics Letters•Apr 15, 1991•1 citation
An external field applied to dye doped polymers which have inhomogeneous dispersion in their absorption spectra causes a shift in the absorption of the dye molecules. This, in turn, changes the line shapes of persistent spectral holes1). The Stark effect has been applied to optical storage2) and optical computing3). It has been also used as a powerful tool for investigating such physical profiles of materials as the difference between the effective molecular electric dipole moments in the host matrix in the ground and excited states which is related to hole burning4),5).
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.
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].
We study theoretically and experimentally the influence of a homogeneous static electric field on a photochemically accumulated stimulated photon echo in dye-doped polymers. The dependence of the time profile of the echo signal on the strength of the electric field is evaluated in the case of a linear Stark effect. Experiments using polymers doped with organic dye molecules are carried out at low temperature, and our new technique is applied to determine the difference of the permanent dipole moment in the ground and the first excited singlet electronic state of the impurity molecules.
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.