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Enhanced reliability of drift-diffusion approximation for electrons in fluid models for nonthermal plasmas
Common fluid models used for the description of electron transport in nonthermal discharge plasmas are subject to substantial restrictions if the electron energy transport significantly influences the discharge behaviour. A drift-diffusion approach is presented which is based on a multiterm approximation of the electron velocity distribution function and overcomes some of these restrictions. It is validated using a benchmark model and applied for the analysis of argon discharge plasmas at low and atmospheric pressure. The results are compared to those of common drift-diffusion models as well as to experimental data. It is pointed out that fluid models are able to describe nonlocal phenomena caused by electron energy transport, if the energy transport is consistently described. Numerical difficulties that frequently occur when the conventional drift-diffusion model is consistently applied are avoided by the proposed method.
Low-energy constraints on photoelectron spectra measured from liquid water and aqueous solutions
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.
Unified description of low-order above-threshold ionization on and off axis
A recently developed unified description of low-order above-threshold ionization (Becker et al 2014 J. Phys. B: At. Mol. Opt. Phys. 47 204022; 2015 J. Phys. B: At. Mol. Opt. Phys. 48 151001) is revisited and extended. By considering the rescattering electron energies and angles at the classical cutoffs and the contributions of particular quantum-orbit solutions, it is shown that summing both the backward- and the forward-scattering contributions, within the low-frequency approximation, it is possible to reproduce the observed features of the ATI spectra both for low and high energies and both on and off the laser-polarization axis in the momentum plane.