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Functionalized adamantane molecular cluster materials show highly transientnonlinear optical properties of currently unclear structural origin. Severalinteraction mechanisms in compounds comprising molecular clusters, their inter-and intramolecular interactions as well as the interplay of their electronicsystems and vibrations of their backbone are viable concepts to explain thesenonlinear optical properties. We show that transient Coulomb forces also haveto be considered as they can lead to intramolecular structure transformationsand intermolecular rearrangements in the crystal. Both strongly influence thenonlinear optical properties. Moreover, selective bromine functionalization cantrigger a photochemical rearrangement of the molecules. The structure andchemical bonding within the compounds are investigated in dependence on thelaser irradiation at different stages of their nonlinear emission by electrondiffraction and electron energy loss spectroscopy. The transient structural andchemical states observed are benchmarked by similar observations duringelectron irradiation, which makes quantification of structural changes possibleand allows the correlation with first principles calculations. Thefunctionalization and its subsequent usage to exploit photochemical effects caneither enhance two-photon absorption or facilitate white-light emission ratherthan second-harmonic generation.

Adamantanes as white-light emitters: Controlling arrangement and functionality by external Coulomb forces