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Observation of electron-transfer-mediated decay in aqueous solution
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Molecular and Condensed Matter Physics. Helmholtz Zentrum Berlin Mat & Energie, Inst Methods Mat Dev, Albert Einstein Str 15, D-12489 Berlin, Germany.
Helmholtz Zentrum Berlin Mat & Energie, Inst Methods Mat Dev, Albert Einstein Str 15, D-12489 Berlin, Germany..
Helmholtz Zentrum Berlin Mat & Energie, Inst Methods Mat Dev, Albert Einstein Str 15, D-12489 Berlin, Germany.;Kyoto Univ, Dept Chem, Sakyo Ku, Kyoto 6068502, Japan..
Helmholtz Zentrum Berlin Mat & Energie, Inst Methods Mat Dev, Albert Einstein Str 15, D-12489 Berlin, Germany..
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2017 (English)In: Nature Chemistry, ISSN 1755-4330, E-ISSN 1755-4349, Vol. 9, no 7, 708-714 p.Article in journal (Refereed) Published
Abstract [en]

Photoionization is at the heart of X-ray photoelectron spectroscopy (XPS), which gives access to important information on a sample's local chemical environment. Local and non-local electronic decay after photoionization-in which the refilling of core holes results in electron emission from either the initially ionized species or a neighbour, respectively-have been well studied. However, electron-transfer-mediated decay (ETMD), which involves the refilling of a core hole by an electron from a neighbouring species, has not yet been observed in condensed phase. Here we report the experimental observation of ETMD in an aqueous LiCl solution by detecting characteristic secondary low-energy electrons using liquid-microjet soft XPS. Experimental results are interpreted using molecular dynamics and high-level ab initio calculations. We show that both solvent molecules and counterions participate in the ETMD processes, and different ion associations have distinctive spectral fingerprints. Furthermore, ETMD spectra are sensitive to coordination numbers, ion-solvent distances and solvent arrangement.

Place, publisher, year, edition, pages
NATURE PUBLISHING GROUP , 2017. Vol. 9, no 7, 708-714 p.
National Category
Chemical Sciences
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URN: urn:nbn:se:uu:diva-328978DOI: 10.1038/NCHEM.2727ISI: 000404056800019PubMedID: 28644468OAI: oai:DiVA.org:uu-328978DiVA: diva2:1140547
Funder
EU, European Research Council, 692657
Available from: 2017-09-12 Created: 2017-09-12 Last updated: 2017-09-12Bibliographically approved

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Unger, Isaak

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