Awad Mohamed

We determine with high accuracy the energy of the inner-shell transition $1s^2 2s^2~{}^1\mathrm{S}_0 \rightarrow 1s~2s^2~2p_{3/2}~{}^1\mathrm{P}_1$ ${}^{16}\mathrm{O}_{Kα}^{4+}$ at $554.372(3)~\mathrm{eV}$ ($λ$ = $22.36480(12)~\unicode{x212B}$) as well as its small shift of $2.2 \pm 1.3~\mathrm{meV}$ ($Δλ$ = $0.089(52)~\mathrm{m}\unicode{x212B}$) for the ${}^{18}\mathrm{O}$ isotope. This transition blends with a $K_α$ line of $\mathrm{O}^{5+}$ used in astrophysical diagnostics, potentially affecting its reliability. In contrast to our experimental uncertainty of $\pm 3~\mathrm{meV}$, advanced electronic structure predictions for this four-electron system, including quantum electrodynamic (QED) corrections on the order of $100~\mathrm{meV}$, still scatter by more than $\pm 250~\mathrm{meV}$. Ions generated and stored in an electron beam ion trap were excited at the ELETTRA synchrotron facility with monochromatic soft x rays, with photon energies corrected by an additional spectrometer. Upon resonant excitation of $\mathrm{O}^{4+}$ and subsequent autoionization, we separate the photoions of each isotope by a time-of-flight measurement. This way, we resolve soft x-ray isotopic shifts of a few meV, obtain very accurate data on an essential astrophysical ion, and test calculations down to the level of QED contributions.

Ultraintense pulses from X-ray free-electron lasers can drive, within femtoseconds, multiple processes in the inner shells of atoms and molecules in all phases of matter. The ensuing complex ionization pathways of outer-shell electrons from the neutral to the final highly charged states make a comparison with theory enormously difficult. We resolve these pathways by preparing highly charged ions in an electron beam ion trap before exposing them to the pulsed radiation. This reveals how relativistic fine-structure effects shift electronic energies, largely compensate the core-screening potential, and enable the consecutive, resonant absorption of two quasi-monochromatic X-ray photons that would generally be unfeasible. This doubly-resonant channel enhances the efficiency of two-photon ionization by more than two orders of magnitude, dominating in this regime the nonlinear interaction of light and matter with possible application for future precision X-ray metrology.