Setting the photoelectron clock through molecular alignment

Nature Communications 11, 2546, (2020)

Setting the photoelectron clock through molecular alignment

Andrea Trabattoni, Joss Wiese, Umberto De Giovannini, Jean-François Olivieri, Terry Mullins, Jolijn Onvlee, Sang-Kil Son, Biagio Frusteri, Angel Rubio, Sebastian Trippel & Jochen Küpper

The interaction of strong laser fields with matter intrinsically provides a powerful tool for imaging transient dynamics with an extremely high spatiotemporal resolution. Here, we study strong-field ionisation of laser-aligned molecules, and show a full real-time picture of the photoelectron dynamics in the combined action of the laser field and the molecular interaction. We demonstrate that the molecule has a dramatic impact on the overall strong-field dynamics: it sets the clock for the emission of electrons with a given rescattering kinetic energy. This result represents a benchmark for the seminal statements of molecular-frame strong-field physics and has strong impact on the interpretation of self-diffraction experiments. Furthermore, the resulting encoding of the time-energy relation in molecular-frame photoelectron momentum distributions shows the way of probing the molecular potential in real-time, and accessing a deeper understanding of electron transport during strong-field interactions.

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This work has been supported by the Clusters of Excellence “Center for Ultrafast Imaging” (CUI, EXC 1074, ID 194651731) and “Advanced Imaging of Matter” (AIM, EXC 2056, ID 390715994) of the Deutsche Forschungsgemeinschaft (DFG), by the European Research Council under the European Union’s Seventh Framework Programme (FP7/ 2007–2013) through the Consolidator Grant COMOTION (ERC-Küpper-614507) and under the Horizon 2020 Research and Innovation Programme through the Advanced Grant QSpec-NewMat (ERC-Rubio-694097), and by the Helmholtz Association Initiative and Networking Fund. A.T. and J.O. gratefully acknowledge fellowships by the Alexander von Humboldt Foundation

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