Ultrafast nuclear dynamics of the acetylene cation C2H2+ and its impact on the infrared probe pulse induced C–H bond breaking efficiency
Literature Information
Nadja Hartmann, Swarnendu Bhattacharyya, Fabian Schlaepfer, Mikhail Volkov, Zeno Schumacher, Matteo Lucchini, Lukas Gallmann, Ursula Rothlisberger, Ursula Keller
The ultrafast nuclear dynamics of the acetylene cation C2H2+ following photoionization of the neutral molecule is investigated using an extreme-ultraviolet pump/infrared probe setup. The observed modulation of the C2H+ fragment ion yield with pump–probe delay is related to structural changes induced by the extreme-ultraviolet pump pulse taking place on the femtosecond timescale. High-level simulations suggest that the trans-bending and C–C bond stretching motion of the C2H2+ cation govern the observed interaction with the infrared pulse. Depending on the molecular configuration at arrival of the infrared pulse, it either transfers population to higher-lying states or to the C2H2+ ground state, thereby enhancing or lowering the C2H+ yield. Our ultrafast pump–probe scheme can thus be used to track excited state nuclear dynamics with a resolution of a few femtoseconds, leading the way to studying fast dynamics also in larger hydrocarbon molecules.
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Physical Chemistry Chemical Physics

Physical Chemistry Chemical Physics (PCCP) is an international journal co-owned by 19 physical chemistry and physics societies from around the world. This journal publishes original, cutting-edge research in physical chemistry, chemical physics and biophysical chemistry. To be suitable for publication in PCCP, articles must include significant innovation and/or insight into physical chemistry; this is the most important criterion that reviewers and Editors will judge against when evaluating submissions. The journal has a broad scope and welcomes contributions spanning experiment, theory, computation and data science. Topical coverage includes spectroscopy, dynamics, kinetics, statistical mechanics, thermodynamics, electrochemistry, catalysis, surface science, quantum mechanics, quantum computing and machine learning. Interdisciplinary research areas such as polymers and soft matter, materials, nanoscience, energy, surfaces/interfaces, and biophysical chemistry are welcomed if they demonstrate significant innovation and/or insight into physical chemistry. Joined experimental/theoretical studies are particularly appreciated when complementary and based on up-to-date approaches.










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