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The Journal of Chemical Physics

Calculations of electric field effects on persistent spectral holes in amorphous host–guest systems

P. Schätz, Max Maier

Published Jul 15, 1987• 27 citations

Abstract

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.

DOI: 10.1063/1.453288

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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).

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 possibility to investigate the influence of external electric and magnetic fields on complex molecules in amorphous solids is essentially limited by a large width of their spectral bands (Δν=102-103 cm−1 even at liquid helium temperature). Hole-burning opens up new excellent opportunities for using the Stark and Zeeman effects in spectroscopy of molecules and solids and their different applications [1]. Owing to the small hole width (Δν=10−1-10−2 cm−1 at 2-5 K) the sensitivity of measurements increases by several orders of magnitude.

The capacity of optical memories can be enhanced by using extra dimensions to store the signals besides the spatial dimension. We have investigated the photochemical persistent hole burning (PHB) reaction in a series of quinone derivatives as the guest molecules. In wavelength dimension, we showed that 600 ultra-high multiple spectral holes can be recorded in a double layered system. To increase the multiplicity of spectral holes, we intended to use electric field as another dimension. We have investigated the influence of electric field effect (Stark effect) in the PHB reaction characteristics. We observed for the first time with the quinone derivative systems that the burnt holes were broadened and then diminished when the applied electric field was changed, and that they reappeared when the applied electric field was changed again to the initial value. Multiple hole formation in the electric field dimension and optical modulation by electric field were also achieved.

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