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Resonant inelastic X-ray scattering of liquid water

Nilsson, Anders ; Tokushima, Takashi ; Horikawa, Yuka ; Harada, Yoshihisa ; Ljungberg, Mathias P. ; Shin, Shik ; Pettersson, Lars G.M.

Journal of electron spectroscopy and related phenomena, 2013-06, Vol.188, p.84-100 [Periódico revisado por pares]

Elsevier B.V

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  • Título:
    Resonant inelastic X-ray scattering of liquid water
  • Autor: Nilsson, Anders ; Tokushima, Takashi ; Horikawa, Yuka ; Harada, Yoshihisa ; Ljungberg, Mathias P. ; Shin, Shik ; Pettersson, Lars G.M.
  • Assuntos: Computer simulation ; Inelastic scattering ; Liquids ; Molecular dynamics ; Molecular structure ; Origins ; RIXS ; Water ; X-ray emission spectroscopy ; X-rays
  • É parte de: Journal of electron spectroscopy and related phenomena, 2013-06, Vol.188, p.84-100
  • Notas: ObjectType-Article-1
    SourceType-Scholarly Journals-1
    ObjectType-Feature-2
    content type line 23
  • Descrição: ► Two peaks are observed in the lone pair region of the XES spectrum of water assigned to tetrahedral and distorted hydrogen bonding configurations. ► The isotope effect observed as different relative peak heights is due to spectral line shape differences. ► The two different hydrogen bonding environments can be related to local structures mimicking either low density water or high density water. We review recent studies using resonant inelastic X-ray scattering (RIXS) or also here denoted X-ray emission spectroscopy (XES) on liquid water and the assignment of the two sharp peaks in the lone-pair region. Using the excitation energy dependence we connect the two peaks to specific features in the X-ray absorption (XAS) spectrum which have independently been assigned to molecules in tetrahedral or distorted configurations. The polarization dependence shows that both peaks are of 1b1 origin supporting an interpretation in terms of two structural species, tetrahedral or disordered, which is furthermore consistent with the temperature-dependence of the two peaks. We discuss effects of life-time vibrational interference and how this affects the two components differently and also leads to differences in the relative peak heights for H2O and D2O. We show furthermore that the inherent structure in molecular dynamics simulations contain the structural bimodality suggested by XES, but this is smeared out in the real structure when temperature is included. We present a discussion around alternative interpretations suggesting that the origin of the two peaks is related to ultrafast dissociation and show evidence that such a model is inconsistent with several experimental observations and theoretical concepts. We conclude that the peaks reflect a temperature-dependent balance in fluctuations between tetrahedral and disordered structures in the liquid. This is well-aligned with theories of water under supercooled conditions and higher pressures where water might exist as high- or low-density liquid with different possibilities for a transition between them. With the present work we provide a link between established models for supercooled water, where water's anomalies become extreme, and ambient water, where the anomalous contributions are weaker but still important.
  • Editor: Elsevier B.V
  • Idioma: Inglês;Francês;Alemão
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  • Realização: ABCD-USP USP   Logos de Redes Sociais: Freepik

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