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- W2133517445 abstract "We consider photochemical hole burning of an inhomogeneous and isotropic ensemble of chromophores through excitation with a narrow-bandwidth source of polarized light. We derive expressions for the depth and anisotropy of resonant and vibronic satellite spectral holes with increasing fluence. A fit of these saturation curves to experimental data yields the Debye-Waller factor of the system. A simple rate equation model predicts that the anisotropy of a spectral hole depends only on the angle between the transition dipoles of the burnt and the probed transitions. In experiments with pulsed lasers strong deviations from this ideal behavior are observed. An extended theory including saturation gives a satisfactory description of this phenomenon and provides a new method for the determination of photochemical quantum yields. A dilute solution of chromophores in a solid amorphous host such as a glass or polymer can be characterized by an inhomogeneous distribution of transition frequencies and an initially isotropic orientational distribution. Irradiation with a narrowbandwidth light source, e.g., a laser, excites only molecules which have their transition frequency within a homogeneous line width from the laser frequency. The excited subensemble is anisotropic since the probability of excitation depends on the angle 0 between the light polarization vector and the transition dipole. A fraction 3 of these excited molecules is removed from the ensemble through a photochemical reaction, leaving a narrow hole in the inhomogeneous distribution function. The orientational distribution of the remaining molecules at the frequencies of this spectral hole is anisotropic, and the measured depth of the hole depends on the polarization of the probe light. The degree of polarization p is frequently defined as" @default.
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- W2133517445 date "1994-03-01" @default.
- W2133517445 modified "2023-09-25" @default.
- W2133517445 title "Saturation of Depth and Polarization of Resonant and Satellite Spectral Holes Generated with Pulsed Laser Excitation" @default.
- W2133517445 doi "https://doi.org/10.1021/j100062a028" @default.
- W2133517445 hasPublicationYear "1994" @default.
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