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We explore time-resolved Coulomb explosion induced by intense, extremeultraviolet (XUV) femtosecond pulses from the FLASH free-electron laser as amethod to image photo-induced molecular dynamics in two molecules, iodomethaneand 2,6-difluoroiodobenzene. At an excitation wavelength of 267\,nm, thedominant reaction pathway in both molecules is neutral dissociation viacleavage of the carbon--iodine bond. This allows investigating the influence ofthe molecular environment on the absorption of an intense, femtosecond XUVpulse and the subsequent Coulomb explosion process. We find that the XUV probepulse induces local inner-shell ionization of atomic iodine in dissociatingiodomethane, in contrast to non-selective ionization of all photofragments indifluoroiodobenzene. The results reveal evidence of electron transfer frommethyl and phenyl moieties to a multiply charged iodine ion. In addition,indications for ultrafast charge rearrangement on the phenyl radical are found,suggesting that time-resolved Coulomb explosion imaging is sensitive to thelocalization of charge in extended molecules.

structural dynamics

Probing the UV-Induced Photodissociation of CH$_\text{3}$I and  C$_\text{6}$H$_\text{3}$F$_\text{2}$I with Femtosecond Time-Resolved Coulomb  Explosion Imaging at FLASH