Dissociation of core excited polyatomic molecules: Sequential or concerted processes?

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Abstract
We show that molecular dissociation dynamics of free molecules, as induced by core excitation using synchrotron radiation and probed with 2D mass spectrometry, may be described either as sequential or instantaneous processes, depending on the size of the excited target. The studied molecules are the prototype molecules FeCO2NO2, N2O, and CO2 excited around the carbon and nitrogen K shell. Complex polyatomic molecules are shown to undergo fast internal energy conversion, followed by slower stepwise dissociation. In case of triatomics, on the contrary, fragmentation is very fast and we propose an impulsive model to describe the process, pointing out the breakdown of the Coulomb explosion picture.

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