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

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 26eV 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 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.