Probing the role of excited states in ionization of acetylene
文献信息
Daniel Dundas, Peter Mulholland, Abigail Wardlow, Alejandro de la Calle
Ionization of acetylene by linearly-polarized, vacuum ultraviolet (VUV) laser pulses is modelled using time-dependent density functional theory. Several laser wavelengths are considered including one that produces direct ionization to the first excited cationic state while another excites the molecules to a Rydberg series incorporating an autoionizing state. We show that for the wavelengths and intensities considered, ionization is greatest whenever the molecule is aligned along the laser polarization direction. By considering high harmonic generation we show that populating excited states can lead to a large enhancement in the harmonic yield. Lastly, angularly-resolved photoelectron spectra are calculated which show how the energy profile of the emitted electrons significantly changes in the presence of these excited states.
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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.




