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Abstract

Ultrashort x-ray pulses from free-electron lasers can efficiently charge up and trigger the full fragmentation of molecules. By coincident detection of up to five ions resulting from rapid Coulomb explosion of highly charged iodomethane, we show that the full three-dimensional equilibrium geometry of this prototypical polyatomic system can be determined from the measured ion momenta with the help of a charge buildup model. Supported by simulations of how the ion momenta would reflect specific changes in molecular bond lengths and angles, we demonstrate that Coulomb-explosion imaging with ultrashort x-ray pulses is a promising technique for recording movies of multidimensional nuclear wave packets, including hydrogen motions.