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000636675 1001_ $$0P:(DE-HGF)0$$aLi, Xiang$$b0$$eCorresponding author
000636675 245__ $$aImaging a light-induced molecular elimination reaction with an X-ray free-electron laser
000636675 260__ $$a[London]$$bSpringer Nature$$c2025
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000636675 520__ $$aTracking the motion of individual atoms during chemical reactions represents a severe experimental challenge, especially if several competing reaction pathways exist or if the reaction is governed by the correlated motion of more than two molecular constituents. Here we demonstrate how ultrashort X-ray pulses combined with coincident ion imaging can be used to trace molecular iodine elimination from laser-irradiated diiodomethane (CH2I2), a reaction channel of fundamental importance but small relative yield that involves the breaking of two molecular bonds and the formation of a new one. We map bending vibrations of the bound molecule, disentangle different dissociation pathways, image the correlated motion of the iodine atoms and the methylene group leading to molecular iodine ejection, and trace the vibrational motion of the formed product. Our results provide a quantitative mechanistic picture behind previously suggested reaction mechanisms and prove that a variety of geometries are involved in the molecular bond formation. 
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000636675 7001_ $$0P:(DE-H253)PIP1013728$$aMullins, Terence$$b17$$udesy
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000636675 7001_ $$0P:(DE-H253)PIP1006803$$aRudenko, Artem$$b28$$eCorresponding author
000636675 773__ $$0PERI:(DE-600)2553671-0$$a10.1038/s41467-025-62274-z$$gVol. 16, no. 1, p. 7006$$n1$$p7006$$tNature Communications$$v16$$x2041-1723$$y2025
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