Attosecond molecular dynamics: fact or fiction?

The emerging application of attosecond techniques to molecular systems allows the role of electronic coherence in the control of chemical reactions to be investigated. Prompt ionization of molecules by an attosecond pulse may induce charge migration across a molecular structure on attosecond to few-femtosecond timescales, thereby possibly determining the subsequent relaxation pathways that a molecule may take. We discuss how proposals for this 'charge-directed reactivity' fit within the current understanding of quantum control and review the current state of the art of attosecond molecular science. Specifically, we review the role of electronic coherence and coupling of the electronic and nuclear degrees of freedom in high-harmonic spectroscopy and in the first attosecond pump–probe experiments on molecular systems. Attosecond science allows the role of electronic coherence in the control of chemical reactions in molecular systems to be investigated. This article reviews recent activities in attosecond molecular science and identifies some promising directions for further development.

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