Abstract
Coherent diffractive imaging (CDI) has enabled the structural analysis of individual free nanoparticles in a single shot and offers the tracking of their light induced dynamics with unprecedented spatial and temporal resolution. The retrieval of structural information from scattering images in CDI experiments is so far mostly based on the assumption of classical scattering in linear response. For strong laser fields and in particular for resonant excitations, both the linear and the classical description may no longer be valid as population depletion and stimulated emission become important. Here we develop a density matrix-based scattering model in order to include such quantum effects in the local medium response and explore the transition from linear to non-linear CDI for the resonant scattering from Helium nanodroplets. We find substantial departures from the linear response case already for experimentally reachable pulse parameters and show that non-linear spatio-temporal excitation dynamics results in rich features in the scattering, leading to the proposal of quantum coherent diffractive imaging as a promising novel branch in strong-field XUV and x-ray physics.
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