Real-Space Inversion and Super-Resolution of Ultrafast Scattering

Ultrafast scattering using X-rays or electrons is an emerging method to obtain structure dynamics at the atomic length and time scales. However, directly resolving in real-space atomic motions is inherently limited by the finite detector range and the probe energy. As a result, the time-resolved signal interpretation is mostly done in reciprocal space and relies on modeling and simulations of specific structures and processes. Here, we introduce a model-free approach to directly resolve scattering signals in real space, surpassing the diffraction limit, using scattering kernels and signal priors that naturally arise from the measurement constraints. We demonstrate the approach on simulated and experimental data, recover multiple atomic motions at sub-\angstromngstrom resolutions, and discuss the recovery accuracy and resolution limits vs signal fidelity. The approach offers a robust path to obtain high-resolution real-space information of atomic-scale structure dynamics using current time-resolved X-ray or electron scattering sources

Supplement 1: Probing electron delays in above-threshold ionization

Originally published in Optica on 20 December 2014 (optica-1-6-361

phil-trans-data from On the limits of observing motion in time-resolved X-ray scattering

raw data for the processed Legendre decomposition of the x-ray scattering image