Abstract
The local structure of four amorphous organotin sulfide compounds exhibiting nonlinear optical (NLO) properties is investigated by low‐energy X‐ray absorption spectroscopy (XANES and EXAFS). The basic structural motif of a heteroadamantane cluster with different organic substituents is confirmed by the experiments and by comparison with computer simulations of the near‐edge structure. Essential information is obtained on a special role of the nonaromatic but electron‐rich cyclopentadienyl substituents, which are able to affect the structure of the heteroadamantane cluster core. The EXAFS fits also indicate a structural distinction between two groups within these compounds, which exhibit fundamentally different NLO responses: compounds that show a second harmonic generation can be described well using the single‐molecule approach, whereas the compounds exhibiting the generation of a supercontinuum manifest additional structural contributions.
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