Fundamental Limits on Spatial Resolution in Ultrafast X-ray Diffraction

Adam Kirrander, Peter Weber

Research output: Contribution to journalArticlepeer-review

Abstract

X-ray Free-Electron Lasers have made it possible to record time-sequences of diffraction images to determine changes in molecular geometry during ultrafast photochemical processes. Using state-of-the-art simulations in three molecules (deuterium, ethylene, and 1,3-cyclohexadiene), we demonstrate that the nature of the nuclear wavepacket initially prepared by the pump laser, and its subsequent dispersion as it propagates along the reaction path, limits the spatial resolution attainable in a structural dynamics experiment. The delocalization of the wavepacket leads to a pronounced damping of the diffraction signal at large values of the momentum transfer vector q, an observation supported by a simple analytical model. This suggests that high-q measurements, beyond 10–15 Å −1 , provide scant experimental payback, and that it may be advantageous to prioritize the signal-to-noise ratio and the time-resolution of the experiment as determined by parameters such as the repetition-rate, the photon flux, and the pulse durations. We expect these considerations to influence future experimental designs, including source development and detection schemes.
Original languageEnglish
Pages (from-to)534
JournalApplied Sciences
Volume7
Issue number6
Early online date23 May 2017
DOIs
Publication statusE-pub ahead of print - 23 May 2017

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