Photoelectron spectra of alkali metal-ammonia microjets: From blue electrolyte to bronze metal.


Journal

Science (New York, N.Y.)
ISSN: 1095-9203
Titre abrégé: Science
Pays: United States
ID NLM: 0404511

Informations de publication

Date de publication:
05 06 2020
Historique:
received: 09 10 2019
revised: 25 02 2020
accepted: 03 04 2020
entrez: 6 6 2020
pubmed: 6 6 2020
medline: 6 6 2020
Statut: ppublish

Résumé

Experimental studies of the electronic structure of excess electrons in liquids-archetypal quantum solutes-have been largely restricted to very dilute electron concentrations. We overcame this limitation by applying soft x-ray photoelectron spectroscopy to characterize excess electrons originating from steadily increasing amounts of alkali metals dissolved in refrigerated liquid ammonia microjets. As concentration rises, a narrow peak at ~2 electron volts, corresponding to vertical photodetachment of localized solvated electrons and dielectrons, transforms continuously into a band with a sharp Fermi edge accompanied by a plasmon peak, characteristic of delocalized metallic electrons. Through our experimental approach combined with ab initio calculations of localized electrons and dielectrons, we obtain a clear picture of the energetics and density of states of the ammoniated electrons over the gradual transition from dilute blue electrolytes to concentrated bronze metallic solutions.

Identifiants

pubmed: 32499436
pii: 368/6495/1086
doi: 10.1126/science.aaz7607
doi:

Types de publication

Journal Article Research Support, Non-U.S. Gov't Research Support, U.S. Gov't, Non-P.H.S.

Langues

eng

Sous-ensembles de citation

IM

Pagination

1086-1091

Subventions

Organisme : Deutsche Forschungsgemeinschaft.
Pays : International

Commentaires et corrections

Type : CommentIn

Informations de copyright

Copyright © 2020 The Authors, some rights reserved; exclusive licensee American Association for the Advancement of Science. No claim to original U.S. Government Works.

Auteurs

Tillmann Buttersack (T)

Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences, Flemingovo nám. 2, 16610 Prague 6, Czech Republic.
Department of Chemistry, University of Southern California, Los Angeles, CA 90089-0482, USA.

Philip E Mason (PE)

Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences, Flemingovo nám. 2, 16610 Prague 6, Czech Republic.

Ryan S McMullen (RS)

Department of Chemistry, University of Southern California, Los Angeles, CA 90089-0482, USA.

H Christian Schewe (HC)

Molecular Physics, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin, Germany.

Tomas Martinek (T)

Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences, Flemingovo nám. 2, 16610 Prague 6, Czech Republic.

Krystof Brezina (K)

Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences, Flemingovo nám. 2, 16610 Prague 6, Czech Republic.
Charles University, Faculty of Mathematics and Physics, Ke Karlovu 3, 121 16 Prague 2, Czech Republic.

Martin Crhan (M)

Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences, Flemingovo nám. 2, 16610 Prague 6, Czech Republic.

Axel Gomez (A)

Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences, Flemingovo nám. 2, 16610 Prague 6, Czech Republic.
Département de Chimie, École Normale Supérieure, PSL University, 75005 Paris, France.

Dennis Hein (D)

Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Strasse 15, D-12489 Berlin, Germany.
Department of Chemistry, Humboldt-Universität zu Berlin, Brook-Taylor-Str. 2, D-12489 Berlin, Germany.

Garlef Wartner (G)

Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Strasse 15, D-12489 Berlin, Germany.
Department of Chemistry, Humboldt-Universität zu Berlin, Brook-Taylor-Str. 2, D-12489 Berlin, Germany.

Robert Seidel (R)

Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Strasse 15, D-12489 Berlin, Germany.
Department of Chemistry, Humboldt-Universität zu Berlin, Brook-Taylor-Str. 2, D-12489 Berlin, Germany.

Hebatallah Ali (H)

Molecular Physics, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin, Germany.

Stephan Thürmer (S)

Department of Chemistry, Graduate School of Science, Kyoto University, Kitashirakawa-Oiwakecho, Sakyo-Ku, Kyoto 606-8502, Japan.

Ondrej Marsalek (O)

Charles University, Faculty of Mathematics and Physics, Ke Karlovu 3, 121 16 Prague 2, Czech Republic. ondrej.marsalek@mff.cuni.cz winter@fhi-berlin.mpg.de stephen.bradforth@usc.edu pavel.jungwirth@uochb.cas.cz.

Bernd Winter (B)

Molecular Physics, Fritz-Haber-Institut der Max-Planck-Gesellschaft, Faradayweg 4-6, D-14195 Berlin, Germany. ondrej.marsalek@mff.cuni.cz winter@fhi-berlin.mpg.de stephen.bradforth@usc.edu pavel.jungwirth@uochb.cas.cz.

Stephen E Bradforth (SE)

Department of Chemistry, University of Southern California, Los Angeles, CA 90089-0482, USA. ondrej.marsalek@mff.cuni.cz winter@fhi-berlin.mpg.de stephen.bradforth@usc.edu pavel.jungwirth@uochb.cas.cz.

Pavel Jungwirth (P)

Institute of Organic Chemistry and Biochemistry, Czech Academy of Sciences, Flemingovo nám. 2, 16610 Prague 6, Czech Republic. ondrej.marsalek@mff.cuni.cz winter@fhi-berlin.mpg.de stephen.bradforth@usc.edu pavel.jungwirth@uochb.cas.cz.

Classifications MeSH