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Abstract

For a fundamental understanding of ultra fast dynamics in chemistry, biology and materials science it has been a longstanding dream to record a molecular movie, where both the atomic trajectories and the chemical state of every atom in matter is followed in real time. Free-electron lasers (FEL) provide this perspective as they deliver brilliant femtosecond X-ray pulses spanning a wide photon energy range, which is necessary to gather element-specific and chemical-state-selective information with femtosecond time resolution. The key challenge lies in synchronizing the FEL with separate optical lasers. We exploit the peak brilliance of the FEL in Hamburg (FLASH) and establish X-ray pulse induced transient changes of the optical reflectivity in GaAs as a powerful tool for X-ray/optical cross-correlation. This constitutes a breakthrough en route to a molecular movie and – equally important – opens the novel field of femtosecond X-ray induced dynamics, only accessible with high brilliance X-ray free-electron lasers.