Two-electron dynamics in nonlinear double excitation of helium by intense ultrashort extreme-ultraviolet pulses

Abstract

We present a theoretical study for multiphoton double excitation of He atoms exposed to an intense ultrashort extreme-ultraviolet (EUV) pulse, where the photon energy coincides with the transition energy from the ground state to a Rydberg state, by solving the time-dependent Schr\odinger equation in the hyperspherical coordinates. Photoelectron spectra under the conditions comparable with a recent experiment [Hishikawa et al., Phys. Rev. Lett. 107, 243003 (2011)] are calculated and analyzed. We identify the mechanism of the enhanced three-photon absorption probability which is more than one order of magnitude larger than that for the two-photon process in accordance with the experiment. The enhancement is attributed to a propensity rule for double excitation in a two-step mechanism, in which a one-photon absorption by one electron to a Rydberg state is followed by a two-photon absorption by the other electron to an excited orbital, while the first electron remains at nearly the same principle quantum number. Based on the time-dependent perturbation theory, the three-photon absorption probability exhibits peculiar cubic dependence on the pulse duration due to the propensity rule, in contrast to the linear dependence of the two-photon absorption probability. Thus a crossover between the two- and three-photon absorption probabilities takes place for sufficiently intense and long pulses. We also study the time evolution of a doubly excited two-electron wave packet created by an intense ultrashort EUV pulse efficiently using the same enhancement scheme, opening up the possibility of visualizing the correlated motion of two electrons in the time domain.