We supplement the theory of the inverse Faraday effect, which was developed in the 1960s, to the conditions used today in ultrafast magnetization experiments. We show that assumptions used to derive the effective Hamiltonian and magnetization are not valid under these conditions. We extended the approach to be applicable to describe magnetization dynamics at femtosecond time scales. We show that after the action of an ultrafast laser pulse the system is brought with a certain probability to a state, the magnetic signature of which is different from before the excitation.

We study theoretically the origin and mechanism of the ultrafast inverse Faraday effect, which is a magneto-optical effect, attracting much interest nowadays. Laser-induced subpicosecond spin dynamics in hydrogenlike systems and isolated many-electron atoms are investigated in order to get insight into this process. We show that the stimulated Raman scattering process leads to a change of the magnetic state of a system. We obtain the time evolution of the induced magnetization, its dependencies on laser properties, and the connection with the spin-orbit coupling of a system.

Time-resolved momentum microscopy provides insight into the ultrafast interplay between structural and electronic dynamics. Here we extend orbital tomography into the time domain in combination with time-resolved momentum microscopy at a free-electron laser (FEL) to follow transient photoelectron momentum maps of excited states of a bilayer pentacene film on Ag(110). We use optical pump and FEL probe pulses by keeping FEL source conditions to minimize space charge effects and radiation damage. From the momentum microscopy signal, we obtain time-dependent momentum maps of the excited-state dynamics of both pentacene layers separately. In a combined experimental and theoretical study, we interpret the observed signal for the bottom layer as resulting from the charge redistribution between the molecule and the substrate induced by excitation. We identify that the dynamics of the top pentacene layer resembles excited-state molecular dynamics.

We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a molecule by creating a valence electron hole. An ultrashort extreme ultraviolet probe pulse creates a second electron hole in the molecule. Information about the electron dynamics is accessed by analyzing angular distributions of photoemission probabilities at a fixed photoelectron energy. We demonstrate that a rigorous theoretical analysis, which takes into account the indistinguishability of transitions induced by the ultrashort, broadband probe pulse and electron hole correlation effects, is necessary for the interpretation of time- and angle-resolved photoelectron spectra. We show how a Fourier analysis of time- and angle-resolved photoelectron spectra from a molecule can be applied to follow its electron dynamics by considering photoelectron distributions from an indole molecular cation with coherent electron dynamics.

We describe, within the framework of quantum electrodynamics, an interaction between a nonresonant hard x-ray pulse and an electronic system in the presence of a temporally periodic laser field driving electron dynamics in this system. We apply Floquet theory to describe the laser-driven electronic system, and then obtain the scattering probability of an arbitrary nonresonant x-ray pulse from such a system employing the density-matrix formalism. We show that the scattering probability can be connected to the time-dependent electron density of the driven electronic system only under certain conditions, in particular, if the bandwidth of the probe x-ray pulse is sufficiently narrow to spectroscopically resolve transitions to different final states. A special focus is laid on application of the theory to laser-driven crystals in a strongly nonperturbative regime. We show how the time-dependent electron density of a crystal can be reconstructed from energy-resolved scattering patterns. This is illustrated by a calculation of a diffraction signal from a driven MgO crystal.