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Low-energy constraints on photoelectron spectra measured from liquid water and aqueous solutions

Malerz, Sebastian (författare)
Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany.
Trinter, Florian (författare)
Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany.;Goethe Univ, Inst Kernphys, Max von Laue Str, D-60438 Frankfurt, Germany.
Hergenhahn, Uwe (författare)
Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany.;Leibniz Inst Surface Engn IOM, Dept Funct Surfaces, D-04318 Leipzig, Germany.
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Ghrist, Aaron (författare)
Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany.;Univ Southern Calif, Dept Chem, Los Angeles, CA 90089 USA.
Ali, Hebatallah (författare)
Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany.;Ain Shams Univ, Women Fac Art Sci & Educ, Dept Phys, Cairo 11757, Egypt.
Nicolas, Christophe (författare)
Synchrotron SOLEIL, BP 48, F-91192 Gif Sur Yvette, France.
Saak, Clara-Magdalena (författare)
Uppsala universitet,Kemisk och biomolekylär fysik
Richter, Clemens (författare)
Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany.;Leibniz Inst Surface Engn IOM, Dept Funct Surfaces, D-04318 Leipzig, Germany.
Hartweg, Sebastian (författare)
Synchrotron SOLEIL, BP 48, F-91192 Gif Sur Yvette, France.
Nahon, Laurent (författare)
Synchrotron SOLEIL, BP 48, F-91192 Gif Sur Yvette, France.
Lee, Chin (författare)
Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany.;Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA.;Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA.
Goy, Claudia (författare)
Deutsch Elektronen Synchrotron DESY, Photon Sci, Ctr Mol Waer Sci CMWS, Notkestr 85, D-22607 Hamburg, Germany.
Neumark, Daniel M. (författare)
Univ Calif Berkeley, Dept Chem, Berkeley, CA 94720 USA.;Lawrence Berkeley Natl Lab, Div Chem Sci, Berkeley, CA 94720 USA.
Meijer, Gerard (författare)
Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany.
Wilkinson, Iain (författare)
Helmholtz Zentrum Berlin Materialien & Energie, Dept Locally Sensit & Time Resolved Spect, Hahn Meitner Pl 1, D-14109 Berlin, Germany.
Winter, Bernd (författare)
Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany.
Thuermer, Stephan (författare)
Kyoto Univ, Grad Sch Sci, Dept Chem, Sakyo Ku, Kyoto 6068502, Japan.
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Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany Max Planck Gesell, Fritz Haber Inst, Dept Mol Phys, Faradayweg 4-6, D-14195 Berlin, Germany.;Goethe Univ, Inst Kernphys, Max von Laue Str, D-60438 Frankfurt, Germany. (creator_code:org_t)
2021
2021
Engelska.
Ingår i: Physical Chemistry, Chemical Physics - PCCP. - : Royal Society of Chemistry. - 1463-9076 .- 1463-9084. ; 23:14, s. 8246-8260
Relaterad länk:
https://doi.org/10.1...
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https://uu.diva-port... (primary) (Raw object)
https://pubs.rsc.org...
https://urn.kb.se/re...
https://doi.org/10.1...
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  • Tidskriftsartikel (refereegranskat)
Abstract Ämnesord
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  • We report on the effects of electron collision and indirect ionization processes, occurring at photo-excitation 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 crossover 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 similar to 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.

Ämnesord

NATURVETENSKAP  -- Kemi -- Fysikalisk kemi (hsv//swe)
NATURAL SCIENCES  -- Chemical Sciences -- Physical Chemistry (hsv//eng)
NATURVETENSKAP  -- Fysik -- Atom- och molekylfysik och optik (hsv//swe)
NATURAL SCIENCES  -- Physical Sciences -- Atom and Molecular Physics and Optics (hsv//eng)

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