NDLI: Fundamental Limits on Spatial Resolution in Ultrafast X-ray Diffraction

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Fundamental Limits on Spatial Resolution in Ultrafast X-ray Diffraction

Content Provider	MDPI
Author	Kirrander, Adam Weber, Peter
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.
File Size	11750400
File Format	PDF
e-ISSN	20763417
DOI	10.3390/app7060534
Journal	Applied Sciences
Issue Number	6
Volume Number	7
Language	English
Publisher Date	2017-05-23
Access Restriction	Open
Subject Keyword	X-ray free-electron lasers ultrafast dynamics diffraction spatial resolution pump-probe quantum dynamics wavepackets photochemistry
Content Type	Text
Resource Type	Article

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