Ultrafast spectroscopy has in recent decades provided a more and more versatile means to follow the nuclear and electronic motion in molecular systems experimentally in real time. However, due to the intricate interplay between the large number of degrees of freedom in complex molecules, the measured signals often cannot be straightforwardly interpreted at the atomistic level. This gap between experimental observables and the underlying molecular mechanisms can only be filled by theoretical simulations. Based on our field-induced surface hopping approach for the simulation of light-driven coupled electron-nuclear dynamics, we have developed a methodology to compute time-resolved spectroscopic signals that can be directly confronted with experimental data. Specifically, we have devised an approach for the calculation of time-resolved photoelectron imaging spectra, which provide both the kinetic energy [1,2] and the angular distribution of the emitted photoelectrons . These time-resolved data can be utilized to extract valuable information on course and the time scales of molecular processes, such as vibratíonal motion or electronic relaxation [4,3,5,6,7].
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