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Perspectives of Attosecond Spectroscopy for the Understanding of Fundamental Electron Correlations.
Kraus, Peter M; Wörner, Hans Jakob.
Afiliação
  • Kraus PM; Department of Chemistry, University of California, Berkeley, California, 94720, USA.
  • Wörner HJ; Laboratorium für Physikalische Chemie, ETH Zürich, Vladimir-Prelog-Weg 2, 8093, Zürich, Switzerland.
Angew Chem Int Ed Engl ; 57(19): 5228-5247, 2018 05 04.
Article em En | MEDLINE | ID: mdl-29624808
The description of the electronic structure of molecules in terms of molecular orbitals is a highly successful concept in chemistry. However, it commonly fails if the electrons in a molecule are strongly correlated and cannot be treated as independent particles. Electron correlation is essential to understand inner-valence X-ray spectroscopies, it can drive ultrafast charge migration in molecules, and it is responsible for many exotic properties of strongly correlated materials. Time-resolved spectroscopy with attosecond resolution is generally capable of following electronic motion in real time and can thus provide experimental access to electron-correlation-driven phenomena. High-harmonic spectroscopy in particular uses the precisely timed laser-driven recollision of electrons to interrogate the electronic structure and dynamics of the investigated system on a sub-femtosecond timescale. In this Review, the capabilities of high-harmonic spectroscopy to follow electronic motion in molecules are discussed. Both qualitative and quantitative approaches to unraveling the detailed dynamical responses of molecular systems following ionization are presented. A new theoretical formalism for the reconstruction of correlation-driven charge migration is introduced. The importance of electron-ion entanglement and electronic coherence in the reconstruction of attosecond hole dynamics are discussed. These advances make high-harmonic spectroscopy a promising technique to decode fundamental electron correlations and to provide experimental data on the complex manifestations of multi-electron dynamics.
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Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Tipo de estudo: Qualitative_research Idioma: En Ano de publicação: 2018 Tipo de documento: Article

Texto completo: 1 Coleções: 01-internacional Base de dados: MEDLINE Tipo de estudo: Qualitative_research Idioma: En Ano de publicação: 2018 Tipo de documento: Article