Research ArticleChemistry

Binding energy of solvated electrons and retrieval of true UV photoelectron spectra of liquids

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Science Advances  30 Aug 2019:
Vol. 5, no. 8, eaaw6896
DOI: 10.1126/sciadv.aaw6896

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  • RE: Binding energy of solvated electrons and retrieval of true UV photoelectron spectra of liquids
    • Ruth Signorell, Professor, ETH Zurich, Department of Chemistry and Applied Biosciences

    In their recent article [1], Suzuki and coworkers propose a method for the analysis of time-dependent photoelectron spectra of liquids which they claim allows them to account for the effects of inelastic electron scattering and retrieve time-dependent genuine («true») photoelectron spectra, i.e. spectra corrected for distortions caused by electron transport in the liquid. In the following we demonstrate that the so-called «retrieval method» can in principle not afford this and that in essence it constitutes no more than a linear decomposition of time-dependent photoelectron spectra in terms of stationary reference spectra from which time-dependent vertical binding energies (as a result of time-dependent state populations) are inferred. While we do not question the validity of the kinetic analysis – within the approximations implied – we would like to clarify the following points:

    1) The retrieval of genuine spectra is only possible with independent quantitative information on the electron transport characteristics in the liquid, e.g. (double) differential scattering cross sections as shown in [2]. In contrast to what ref. [1] implies, genuine electron binding spectra and differential scattering cross sections cannot be retrieved simultaneously from the same measurements without further assumptions (see points below). Thus, the retrieval in ref. [1] cannot «examine the validity of theoretical analysis by Luckhaus et al.» [2] as claimed in the introduction of ref. [1]...

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    Competing Interests: None declared.

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