This paper discusses the spectral properties and spatial orientation of the absorbing molecular components in layers of polymethine dyes on a glass substrate. Depending on the thickness of the layers, from one to four components that differ in spectra and in orientation angles are observed. One type of angular distribution of the components (the first) is observed in submonolayers, while two types (the first and second) are observed in multilayer coatings. Optical excitation of the layers converts the angular distribution of the second type into that of the first type. The relative yield of this process increases with increasing energy density per radiation pulse. It can be assumed that the reorientation is associated with an increase of the vibrational-energy content in the radiation-absorbing components and its transport to the nonabsorbing components of the layer. © 2004 Optical Society of America

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