Resonant two-photon absorption of extreme-ultraviolet free-electron-laser radiation in helium

Abstract

We have investigated the nonlinear response of helium to intense extreme-ultraviolet radiation from the free-electron laser in Hamburg (FLASH). We observe a spectral feature between 24 and $26\phantom{\rule{0.3em}{0ex}}\mathrm{eV}$ electron kinetic energy in photoemission which shows a quadratic fluence dependence. The feature is explained as a result of subsequent processes involving a resonant two-photon absorption process into doubly excited levels of even parity ($N=5$ and 6), radiative decay to the doubly excited states in the vicinity of the ${\mathrm{He}}^{+}$ $(N=2)$ ionization threshold and finally the photoionization of the inner electron by the radiation of the next microbunches. This observation suggests that even-parity states, which have been elusive to be measured with the low pulse energy of synchrotron radiation sources, can be investigated with the intense radiation of FLASH. This also demonstrates a first step to bring nonlinear spectroscopy into the xuv and soft-x-ray regime.