X-ray laser–induced electron dynamics observed by femtosecond diffraction from nanocrystals of Buckminsterfullerene

Brian Abbey, Ruben A Dilanian, Connie Darmanin, Rebecca A Ryan, Corey T Putkunz, Andrew V Martin, David Wood, Victor Streltsov, Michael W M Jones, Naylyn Gaffney, Felix Hofmann, Garth J Williams, Sébastien Boutet, Marc Messerschmidt, M Marvin Seibert, Sophie Williams, Evan Curwood, Eugeniu Balaur, Andrew G Peele, Keith A Nugent, Harry M Quiney

X-ray free-electron lasers (XFELs) deliver x-ray pulses with a coherent flux that is approximately eight orders of magnitude greater than that available from a modern third-generation synchrotron source. The power density of an XFEL pulse may be so high that it can modify the electronic properties of a sample on a femtosecond time scale. Exploration of the interaction of intense coherent x-ray pulses and matter is both of intrinsic scientific interest and of critical importance to the interpretation of experiments that probe the structures of materials using high-brightness femtosecond XFEL pulses. We report observations of the diffraction of extremely intense 32-fs nanofocused x-ray pulses by a powder sample of crystalline C60. We find that the diffraction pattern at the highest available incident power significantly differs from the one obtained using either third-generation synchrotron sources or XFEL sources operating at low output power and does not correspond to the diffraction pattern expected from any known phase of crystalline C60. We interpret these data as evidence of a long-range, coherent dynamic electronic distortion that is driven by the interaction of the periodic array of C60 molecular targets with intense x-ray pulses of femtosecond duration.