The nonlinear process of laser-driven electron rescattering has enabled major breakthroughs such as the direct imaging and online tracking of ultrafast atomic and molecular processes. It is also at the heart of the generation of coherent light waves with atomic-scale wavelengths via high-order harmonic generation. While most studies in, for example, femtochemistry have focused on exploiting outer-shell electronic information, the possibility of accessing inner-shell excitations through laser-driven rescattering opens new horizons while posing new practical challenges.

In this work, Kelley and coauthors present a thorough theoretical investigation of the necessary conditions to be met by the laser sources so as to enable access to K and L_I-shell excitations (these belong to the innermost electronic shells). Surprisingly, it turns out that laser-driven electron rescattering can create inner-shell holes in any atom from lithium to uranium using intense laser sources with central wavelengths ranging from the far-infrared to the X-ray domain, i.e., from ~10 μm  to ~1 nm wavelength, and intensities up to the relativistic regime. These results may constitute a guide for future experiments aimed at gaining insight into the exotic ultrafast dynamics of inner-shell ionized atomic and molecular species.

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