The cross sections for single-electron photoionization in two-electron atoms show fluctuations which decrease in amplitude when approaching the double-ionization threshold. Based on semiclassical closed orbit theory, we show that the algebraic decay of the fluctuations can be characterized in terms of a threshold law sigma proportional to |E|(mu) as E --> 0(-) with exponent mu obtained as a combination of stability exponents of the triple-collision singularity. It differs from Wannier's exponent dominating double-ionization processes. The details of the fluctuations are linked to a set of infinitely unstable classical orbits starting and ending in the nonregularizable triple collision. The findings are compared with quantum calculations for a model system, namely, collinear helium.
The quantum regime of highly doubly excited states in two-electron atoms has, so far, been largely inaccessible both to numerical methods as well as to experiments. Recent advances in semiclassical closed orbit theory in combination with a quantum mapping approach have shown a new way into this region of high dynamical complexity. In particular, new scaling laws near the double-ionization threshold as well as the dominant semiclassical contributions to the total photoionization cross section can be identified. We will present this new approach here in all its detail. It is based on representing the photoionization cross section in terms of quantum maps. These quantum maps or quantum propagators are used as a starting point for developing an efficient numerical method for calculating cross sections. Furthermore, by writing the quantum operators in semiclassical approximations, it is possible to interpret the quantum results in terms of classical triple collision orbits and to derive threshold laws near the three-particle breakup point. Semiclassical and numerical quantum results show excellent agreement for a model system, namely collinear helium.
We investigate the classical motion of three charged particles with both attractive and repulsive interactions. The triple collision is a main source of chaos in such three-body Coulomb problems. By employing the McGehee scaling technique, we analyze here for the first time in detail the three-body dynamics near the triple collision in 3 degrees of freedom. We reveal surprisingly simple dynamical patterns in large parts of the chaotic phase space. The underlying degree of order in the form of approximate Markov partitions may help in understanding the global structures observed in quantum spectra of two-electron atoms.
Ultrafast atomic processes, such as excitation and ionization occurring on the femtosecond or shorter time scale, were explored by employing attosecond high-harmonic pulses. With the absorption of a suitable high-harmonic photon a He atom was ionized, or resonantly excited with further ionization by absorbing a number of infrared photons. The electron wave packets liberated by the two processes generated an interference containing the information on ultrafast atomic dynamics. The attosecond electron wave packet, including the phase, from the ground state was reconstructed first and, subsequently, that from the 1s3p state was retrieved by applying the holographic technique to the photoelectron spectra comprising the interference between the two ionization paths. The reconstructed electron wave packet revealed details of the ultrafast photoionization dynamics, such as the instantaneous two-photon ionization rate.
Experimental results on partial photo-ionisation cross sections of helium are analysed in the light of recent advances in the semiclassical theory of two-electron atoms. Byun et al [1] predict that the total photo-ionisation cross section below the double-ionisation threshold can, semiclassically, be described in terms of contributions associated with classical orbits starting and ending in the triple collision. The necessary modifications of the semiclassical theory for partial cross sections is developed here. It is argued that partial cross sections are also dominated by the triple collision dynamics. The expected semiclassical contributions can be identified in the Fourier transformation of the experimental data. This clearly demonstrates for the first time the validity of the basic assumptions made in [1]. Our findings explain furthermore in a natural way the self-similar structures observed in cross section signals for different channel numbers.
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