2021, Malerz, Sebastian, Trinter, Florian, Hergenhahn, Uwe, Ghrist, Aaron, Ali, Hebatallah, Nicolas, Christophe, Saak, Clara-Magdalena, Richter, Clemens, Hartweg, Sebastian, Nahon, Laurent, Lee, Chin, Goy, Claudia, Neumark, Daniel M, Meijer, Gerard, Wilkinson, Iain, Winter, Bernd, Thürmer, Stephan

We report on the effects of electron collision and indirect ionization processes, occurring at photoexcitation and electron kinetic energies well below 30 eV, on the photoemission spectra of liquid water. We show that the nascent photoelectron spectrum and, hence, the inferred electron binding energy can only be accurately determined if electron energies are large enough that cross sections for quasi-elastic scattering processes, such as vibrational excitation, are negligible. Otherwise, quasi-elastic scattering leads to strong, down-to-few-meV kinetic energy scattering losses from the direct photoelectron features, which manifest in severely distorted intrinsic photoelectron peak shapes. The associated cross-over point from predominant (known) electronically inelastic to quasi-elastic scattering seems to arise at surprisingly large electron kinetic energies, of approximately 10–14 eV. Concomitantly, we present evidence for the onset of indirect, autoionization phenomena (occurring via superexcited states) within a few eV of the primary and secondary ionization thresholds. These processes are inferred to compete with the direct ionization channels and primarily produce low-energy photoelectrons at photon and electron impact excitation energies below ∼15 eV. Our results highlight that vibrational inelastic electron scattering processes and neutral photoexcitation and autoionization channels become increasingly important when photon and electron kinetic energies are decreased towards the ionization threshold. Correspondingly, we show that for neat water and aqueous solutions, great care must be taken when quantitatively analyzing photoelectron spectra measured too close to the ionization threshold. Such care is essential for the accurate determination of solvent and solute ionization energies as well as photoelectron branching ratios and peak magnitudes.

2019, Ueda, Kiyoshi, Sokell, Emma, Schippers, Stefan, Aumayr, Friedrich, Sadeghpour, Hossein, Burgdörfer, Joachim, Lemell, Christoph, Tong, Xiao-Min, Pfeifer, Thomas, Calegari, Francesca, Palacios, Alicia, Martin, Fernando, Corkum, Paul, Sansone, Giuseppe, Gryzlova, Elena V., Grum-Grzhimailo, Alexei N., Piancastelli, Maria Novella, Weber, Peter M., Steinle, Tobias, Amini, Kasra, Biegert, Jens, Berrah, Nora, Kukk, Edwin, Santra, Robin, Müller, Alfred, Dowek, Danielle, Lucchese, Robert R., McCurdy, C. William, Bolognesi, Paola, Avaldi, Lorenzo, Jahnke, Till, Schöffler, Markus S., Dörner, Reinhard, Mairesse, Yann, Nahon, Laurent, Smirnova, Olga, Schlathölter, Thomas, Campbell, Eleanor E.B., Rost, Jan-Michael, Meyer, Michael, Tanaka, Kazuo A.

We publish three Roadmaps on photonic, electronic and atomic collision physics in order to celebrate the 60th anniversary of the ICPEAC conference. In Roadmap I, we focus on the light-matter interaction. In this area, studies of ultrafast electronic and molecular dynamics have been rapidly growing, with the advent of new light sources such as attosecond lasers and x-ray free electron lasers. In parallel, experiments with established synchrotron radiation sources and femtosecond lasers using cutting-edge detection schemes are revealing new scientific insights that have never been exploited. Relevant theories are also being rapidly developed. Target samples for photon-impact experiments are expanding from atoms and small molecules to complex systems such as biomolecules, fullerene, clusters and solids. This Roadmap aims to look back along the road, explaining the development of these fields, and look forward, collecting contributions from twenty leading groups from the field. © 2019 IOP Publishing Ltd.