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          Institute: Fritz-Haber-Institut     Collection: Physical Chemistry     Display Documents



  history
ID: 403009.0, Fritz-Haber-Institut / Physical Chemistry
A Dynamic Landscape from Femtoseconds to Minutes for Excess Electrons at Ice-Metal Interfaces
Authors:Bovensiepen, Uwe; Gahl, Cornelius; Stähler, Julia; Bockstedte, Michel; Meyer, Michael; Baletto, Francesca; Scandolo, Sandro; Zhu, Xiaoyang; Rubio, Angel; Wolf, Martin
Language:English
Date of Publication (YYYY-MM-DD):2009-01-22
Title of Journal:Journal of Physical Chemistry C
Journal Abbrev.:J. Phys. Chem. C
Volume:113
Issue / Number:3
Start Page:979
End Page:988
Copyright:© 2009 The American Chemical Society
Review Status:Peer-review
Audience:Experts Only
Abstract / Description:Stabilization of excess electrons is studied at crystalline ice-metal interfaces by femtosecond time-resolved two-photon photoelectron spectroscopy and ab initio calculations. Following optical excitation into delocalized image potential states, electrons localize at pre-existing defects which are located at the ice-vacuum interface. Remarkably, the stabilization of these trapped electrons is monitored continuously from femtoseconds up to minutes.,By first principle calculations we identify defect structures, that support excess electrons in front of crystalline ice surfaces, and suggest that the stabilization proceeds through subsequent conformational substates. The excess electron wave functions are efficiently screened from the underlying bulk and explain the long residence times observed in the experiment. Thereby, we shed light on the collective character of the nuclear rearrangement that determines the energetics over all timescales.
Free Keywords:water-cluster anions; stretched-exponential relaxation; solvation; protein; diffusion; surface; localization; chemistry; transport; Ru(001)
External Publication Status:published
Document Type:Article
Communicated by:Gerhard Ertl
Affiliations:Fritz-Haber-Institut/Physical Chemistry
External Affiliations:Gahl C, Max Born Inst Nichtlineare Opt & Kurzzeitspektros, D-12489 Berlin, Germany; Bockstedte M, Rubio A, Univ Pais Vasco, ETSF, Dept Fis Mat, San Sebastian 20018, Spain; Bockstedte M, Univ Erlangen Nurnberg, Inst Theoret Festkorperphys, D-91058 Erlangen, Germany; Baletto F, Scandolo S, Abdus Salam Int Ctr Theoret Phys, I-34100 Trieste, Italy; Baletto F, Scandolo S, INFM, Democritos Natl Simulat Ctr, I-34100 Trieste, Italy; Zhu XY, Univ Minnesota, Dept Chem, Minneapolis, MN 55455 USA; Rubio A, UPV, EHU, CSIC, Ctr Mixto, San Sebastian 20018, Spain; Rubio A, DIPC, San Sebastian 20018, Spain; Bovensiepen U (uwe.bovensiepen@fu-berlin.de), Stähler J, Meyer M, Wolf M, Free Univ Berlin, Fachbereich Phys, D-14195 Berlin, Germany
Identifiers:URL:http://pubs.acs.org/doi/abs/10.1021/jp806997d [online 2008-12-31]
DOI:10.1021/jp806997d
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