Model-free pattern separation of two-color ultrafast X-ray diffraction

Abstract

Two-color X-ray imaging with Free Electron Laser pulses offers a powerful approach for probing ultrafast structural dynamics in nanoscale systems, combining (near-)atomic spatial resolution with femtosecond temporal precision. The first X-ray pulse captures the object’s initial state, while the second, time-delayed pulse records its subsequent evolution. A key challenge lies in disentangling the two patterns simultaneously recorded by the same detector. We demonstrate the realization of this approach on structurally varying nanoscale particles using two X-ray pulses of different photon energies, 1 and 1.2 keV. Sub-micrometer helium nanodroplets generated in vacuum are irradiated by the two X-ray pulses separated in time by up to 750 femtoseconds. Taking advantage of the high photon-energy resolution of the imaging detector, we separate the overlapping diffraction signals by analyzing individual pixel counts and applying pattern recognition. The helium nanodroplets’ spherical shape allows us to cross-validate this approach by fitting the radial scattering profiles with Mie solutions for abichromatic field. The excellent agreement between the two methods, particularly in the sparsely illuminated outer regions of the diffraction patterns where high-resolution structural information is encoded, highlights the quality of this approach and its potential for future advanced X-ray movie techniques.