We publish three Roadmaps on photonic, electronic and atomic collision physics in order to celebrate the 60th anniversary of the ICPEAC conference. In Roadmap I, we focus on the light–matter interaction. In this area, studies of ultrafast electronic and molecular dynamics have been rapidly growing, with the advent of new light sources such as attosecond lasers and x-ray free electron lasers. In parallel, experiments with established synchrotron radiation sources and femtosecond lasers using cutting-edge detection schemes are revealing new scientific insights that have never been exploited. Relevant theories are also being rapidly developed. Target samples for photon-impact experiments are expanding from atoms and small molecules to complex systems such as biomolecules, fullerene, clusters and solids. This Roadmap aims to look back along the road, explaining the development of these fields, and look forward, collecting contributions from twenty leading groups from the field.

Quantum mechanically, photoionization can be fully described by the complex photoionization amplitudes that describe the transition between the ground state and the continuum state. Knowledge of the value of the phase of these amplitudes has been a central interest in photoionization studies and newly developing attosecond science, since the phase can reveal important information about phenomena such as electron correlation. We present a new attosecond-precision interferometric method of angle-resolved measurement for the phase of the photoionization amplitudes, using two phase-locked extreme ultraviolet pulses of frequency $\omega$ and $2\omega$, from a free-electron laser. Phase differences $\mathrm{\Delta }\tilde{\eta }$ between one- and two-photon ionization channels, averaged over multiple wave packets, are extracted for neon $2p$ electrons as a function of the emission angle at photoelectron energies 7.9, 10.2, and 16.6 eV. $\mathrm{\Delta }\tilde{\eta }$ is nearly constant for emission parallel to the electric vector but increases at 10.2 eV for emission perpendicular to the electric vector. We model our observations with both perturbation and ab initio theory and find excellent agreement. In the existing method for attosecond measurement, reconstruction of attosecond beating by interference of two-photon transitions (RABBITT), a phase difference between two-photon pathways involving absorption and emission of an infrared photon is extracted. Our method can be used for extraction of a phase difference between single-photon and two-photon pathways and provides a new tool for attosecond science, which is complementary to RABBITT.

The nature of transient electronic states created by photoabsorption critically determines the dynamics of the subsequently evolving system. Here, we investigate $K$-shell photoionized atomic neon by absorbing a second photon within the Auger-decay lifetime of 2.4 fs using the European XFEL, a unique high-repetition-rate, wavelength-tunable x-ray free-electron laser. By high-resolution electron spectroscopy, we map out the transient Rydberg resonances unraveling the details of the subsequent decay of the hollow atom. So far, ultra-short-lived electronic transients, which are often inaccessible by experiments, were mainly inferred from theory but are now addressed by nonlinear x-ray absorption. The successful characterization of these resonances with femtosecond lifetimes provides the basis for a novel class of site-specific, nonlinear, and time-resolved studies with strong impact for a wide range of topics in physics and chemistry.

The electron angular distribution after atomic photoionization by the fundamental frequency and its second harmonic is analyzed for a case when the frequency of the fundamental scans the region of an intermediate atomic state. The angular distribution and its left-right asymmetry, due to the two-pathway interference between nonresonant one-photon and resonant two-photon ionization, sharply change as a function of the photon energy. The phenomenon is exemplified by both solving the time-dependent Schrödinger equation on a numerical space-time grid and by applying perturbation theory for ionization of the hydrogen atom in the region of the $1s\text{−}2p$ transition for femtosecond pulses as well as an infinitely long exposure to the radiation. Parametrizations for the asymmetry and the anisotropy coefficients, obtained within perturbation theory, reveal general characteristics of observable quantities as functions of the parameters of the radiation beam.

Expressions for the angular distribution of photoelectrons produced in two-photon two-color atomic ionization are obtained within the statistical tensor formalism, taking into account a full multipole expansion of the radiation in electric and magnetic moments. The general expressions are reduced to a simpler form for a particular geometry used in experiments with XUV + optical radiation beams and analyzed within the first-order nondipole corrections for different polarization states of the photons. As a numerical example, the Ne $1s$ above-threshold ionization by two-color radiation is considered within the second-order perturbation theory. A large forward-backward asymmetry in the photoelectron angular distribution is predicted. DOI: http://dx.doi.org/10.1103/PhysRevA.89.043424 ©2014 American Physical Society