Observation of two-XUV-photon ionization using harmonic generation from a short, intense laser pulse

We report the observation of a two-photon ionization process in the XUV wavelength regime. In a near-resonant 1 + 1 ionization scheme, Ar atoms are ionized absorbing the 15 eV third harmonic photons produced in a gas jet by the 0.5 ps intense laser pulses of a KrF excimer laser emitting at 248.6 nm. The present demonstration of a non-linear process in the XUV regime reveals feasibility of high-intensity applications utilizing the uniquely high peak power of non-conventional short wavelength radiation sources based on harmonic generation.

Realization of time-resolved two-vacuum-ultraviolet-photon ionization

International audience; Ultrafast dynamics of excited molecules is studied through time-resolved two-vacuum-ultraviolet (vuv)- photon ionization using a nonlinear volume autocorrelator unit. The two-vuv-photon process is induced by the intense fifth harmonic radiation of a femtosecond Ti:sapphire laser. In a proof-of-principle experiment, ultrafast dynamics of excited ethylene and oxygen molecules are investigated. Molecular decay times are deduced by comparing the experimental data with the results of a numerical model that accounts for the spatial and temporal characteristics of the harmonic field. The present experiments pave a convenient way for time domain investigations in the vuv-xuv s…

Laser-induced field-free alignment of the OCS molecule

We investigate the dynamical alignment of jet-cooled OCS molecules induced by a short laser pulse. The alignment is measured through the orientational contribution of the optical Kerr effect using a second weak laser pulse as a probe. Maximum alignment is observed at conditions close to saturation of ionization. The results are analysed with a quantum mechanical model solving for the rotational dynamics.

Tracking Autoionizing-Wave-Packet Dynamics at the 1-fs Temporal Scale

We present time-resolved studies and Fourier transform spectroscopy of inner-shell excited states undergoing Auger decay and doubly excited autoionizing states, utilizing coherent extreme-ultraviolet (XUV) radiation continua. Series of states spanning a range of ∼4  eV are excited simultaneously. An XUV probe pulse tracks the oscillatory and decaying evolution of the formed wave packet. The Fourier transform of the measured trace reproduces the spectrum of the series. The present work paves the way for ultrabroadband XUV spectroscopy and studies of ultrafast dynamics in all states of matter.

Controlling ionization products through laser-induced continuum structure