Impact of hollow-atom formation on coherent x-ray scattering at high intensity

TL;DR

This paper investigates how hollow-atom formation affects coherent x-ray scattering at high intensities, demonstrating that ultrashort pulses can optimize scattering quality despite radiation damage, with implications for single-molecule imaging.

Contribution

Develops a theoretical toolkit to analyze ionization and scattering dynamics, revealing optimal pulse parameters for high-quality scattering from highly ionized atoms.

Findings

Scattering intensity saturates at a fluence of ~10^7 photons/Å^2 per pulse.

Ultrashort pulses shorter than relaxation times maximize scattering quality.

High-brightness attosecond x-ray FELs are ideal for single-molecule imaging.

Abstract

X-ray free-electron lasers (FELs) are promising tools for structural determination of macromolecules via coherent x-ray scattering. During ultrashort and ultraintense x-ray pulses with an atomic scale wavelength, samples are subject to radiation damage and possibly become highly ionized, which may influence the quality of x-ray scattering patterns. We develop a toolkit to treat detailed ionization, relaxation, and scattering dynamics for an atom within a consistent theoretical framework. The coherent x-ray scattering problem including radiation damage is investigated as a function of x-ray FEL parameters such as pulse length, fluence, and photon energy. We find that the x-ray scattering intensity saturates at a fluence of ~10^7 photons/{\AA}^2 per pulse, but can be maximized by using a pulse duration much shorter than the time scales involved in the relaxation of the inner-shell vacancy states created. Under these conditions, both inner-shell electrons in a carbon atom are removed, and the resulting hollow atom gives rise to a scattering pattern with little loss of quality for a spatial resolution > 1 {\AA}. Our numerical results predict that in order to scatter from a carbon atom 0.1 photons per x-ray pulse, within a spatial resolution of 1.7 {\AA}, a fluence of 10^7 photons/{\AA}^2 per pulse is required at a pulse length of 1 fs and a photon energy of 12 keV. By using a pulse length of a few hundred attoseconds, one can suppress even secondary ionization processes in extended systems. The present results suggest that high-brightness attosecond x-ray FELs would be ideal for single-shot imaging of individual macromolecules.