Relationship between microscopic and macroscopic structures of organic thin films for SHG

The experiments described in this paper were undertaken in order to obtain information about the relationship between the structure and non-linear optical properties (second-harmonic generation) of organic thin films. For this purpose, two closely related dyes, diones and tetrones, were compared, both of which are shown to have large hyperpolarisabilities. Their microscopic properties are investigated by conformational analysis and electron diffraction. It could be shown that detailed knowledge about the structure and the adjacent neighbour packing can be obtained from conformational analysis and electron diffraction in order to understand the non-linear optical properties of the two dyes.