Schnorr, KirstenAugustin, SvenSaalmann, UlfSchmid, GeorgRouzée, ArnaudObaid, RazibAl-Haddad, AndreBerrah, NoraBlaga, Cosmin I.Bostedt, ChristophCardosa-Gutierrez, ManuelCarini, GabriellaCoffee, RyanDiMauro, Louis F.Hart, PhilipIto, YutaKubicek, KatharinaKumagai, YoshiakiKüpper, JochenLai, Yu HangLindenblatt, HannesLivingstone, Ruth A.Meister, SeverinMoshammer, RobertMotomura, KojiMöller, ThomasNakahara, KazOsipov, TimurPandey, GauravRay, DipanwitaRemacle, FrançoiseRolles, DanielRost, Jan MichaelSchlichting, IlmeSchmidt, RüdigerTechert, SimoneTrost, FlorianUeda, KiyoshiUllrich, JoachimVrakking, Marc J. J.Zimmermann, JulianSchulz, Claus PeterPfeifer, Thomas2025-11-242025-11-242025-11-232025-11-2110.1126/sciadv.adz1900https://infoscience.epfl.ch/handle/20.500.14299/256236Laser-driven dynamics in polyatomic molecules poses a complex many-body problem. Understanding intense light-matter interaction is crucial for steering intramolecular quantum dynamical processes. Here, we record time-resolved x-ray diffraction images of C 60 molecules during and after their interaction with intense near-infrared fields, giving direct access to structural changes of the molecules and their fragmentation in real time. Tuning the intensity of the excitation pulses, we uncover a transition from a weak-field regime of excited but stable molecules to a high-field regime dominated by Coulomb explosion. In the transition region, the molecules expand by up to 50% of their initial size within just 140 fs, with major fragmentation only setting in afterward. This work demonstrates that x-ray diffractive imaging is capable of retrieving time-resolved structural information of large molecules reshaped by intense laser fields. Laser-driven fragmentation is a first step toward observing molecular processes modified by laser fields of increasing intensity.entext::journal::journal article::research article