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- ItemEvolution of the charge carrier plasmon in the one-dimensional metal TTF-TCNQ as a function of temperature and momentum(Bristol : Institute of Physics Publishing, 2019) Kovbasa, N.; Graf, L.; Knupfer, M.We have investigated the charge carrier plasmon in the quasi one-dimensional metal TTF-TCNQ using electron energy-loss spectroscopy. Our data reveal a negative plasmon dispersion with a slope that is independent of temperature, which is in agreement to predictions from model calculations and previous room temperature data. A plasmon energy shift upon temperature is observed, and we discuss possible contributions to this shift. The spectral width of the plasmon is rather temperature independent, but increases clearly above a momentum value of about 0.3 Å-1.
- ItemAtomic and molecular suite of R-matrix codes for ultrafast dynamics in strong laser fields and electron/positron scattering(Bristol : IOP Publ., 2020) Wragg, J.; Benda, J.; Mašín, Z.; Armstrong, G.S.J.; Clarke, D.D.A.; Brown, A.C.; Ballance, C.; Harvey, A.G.; Houfek, K.; Sunderland, A.; Plummer, M.; Gorfinkiel, J.D.; Van Der Hart, H.We describe and illustrate a number of recent developments of the atomic and molecular ab initio R-matrix suites for both time-dependent calculations of ultrafast laser-induced dynamics and time-independentcalculations of photoionization and electron scattering. © 2019 Published under licence by IOP Publishing Ltd.
- ItemLow-energy constraints on photoelectron spectra measured from liquid water and aqueous solutions(Cambridge : RSC Publ., 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, StephanWe 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.
- ItemRecent developments in R-matrix applications to molecular processes(Bristol : IOP Publ., 2015) Mašín, Zdeněk; Harvey, Alex; Houfek, Karel; Brambila, Danilo S.; Morales, Felipe; Gorfinkiel, Jimena D.; Tennyson, Jonathan; Smirnova, OlgaWe report on recent developments of the UKRmol suite, an implementation of the molecular R- matrix method and present examples of the calculations (e.g. electron scattering, photoionization, high harmonic generation, etc.) it has enabled.
- ItemNonlocal dielectric function and nested dark excitons in MoS2(London : Nature Publishing Group, 2019) Koitzsch, A.; Pawlik, A.-S.; Habenicht, C.; Klaproth, T.; Schuster, R.; Büchner, B.; Knupfer, M.Their exceptional optical properties are a driving force for the persistent interest in atomically thin transition metal dichalcogenides such as MoS2. The optical response is dominated by excitons. Apart from the bright excitons, which directly couple to light, it has been realized that dark excitons, where photon absorption or emission is inhibited by the spin state or momentum mismatch, are decisive for many optical properties. However, in particular the momentum dependence is difficult to assess experimentally and often remains elusive or is investigated by indirect means. Here we study the momentum dependent electronic structure experimentally and theoretically. We use angle-resolved photoemission as a one-particle probe of the occupied valence band structure and electron energy loss spectroscopy as a two-particle probe of electronic transitions across the gap to benchmark a single-particle model of the dielectric function ϵ(q, ω) against momentum dependent experimental measurements. This ansatz captures key aspects of the data surprisingly well. In particular, the energy region where substantial nesting occurs, which is at the origin of the strong light–matter interaction of thin transition metal dichalcogenides and crucial for the prominent C-exciton, is described well and spans a more complex exciton landscape than previously anticipated. Its local maxima in (q≠0,ω) space can be considered as dark excitons and might be relevant for higher order optical processes. Our study may lead to a more complete understanding of the optical properties of atomically thin transition metal dichalcogenides.