Core hole-electron correlation in coherently coupled molecules

We study the core hole-electron correlation in coherently coupled molecules by energy dispersive near edge X-ray absorption fine-structure spectroscopy. In a transient phase, which exists during the transition between two bulk arrangements, 1,4,5,8-naphthalene-tetracarboxylicacid-dianhydride multilayer films exhibit peculiar changes of the line shape and energy position of the X-ray absorption signal at the C K-edge with respect to the bulk and gas phase spectra. By a comparison to a theoretical model based on a coupling of transition dipoles, which is established for optical absorption, we demonstrate that the observed spectroscopic differences can be explained by an intermolecular delocalized core hole-electron pair. By applying this model we can furthermore quantify the coherence length of the delocalized core-exciton.

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