title: Charge oscillation controlled molecular excitation.
abstract: The direct manipulation of charge oscillations has emerged as a new perspective in chemical reaction control. Here, we demonstrate, in a joint experimental and theoretical study, that the electron dynamics of a molecule is efficiently steered by controlling the interplay of a driving femtosecond laser pulse with the photoinduced charge oscillation. These oscillations have a typical Bohr period of around 1 fs for valence electrons; therefore, control has to be exerted on a shorter time scale. Specifically, we show how precision pulse shaping is used to manipulate the coupled electron and nuclear dynamics in order to address different bound electronic target states in a molecule. We present a strong-field coherent control mechanism which is understood in terms of a simple classical picture and at the same time verified by solving the time-dependent Schrödinger equation. This mechanism is universally applicable and opens a wide spectrum of applications in the reaction control of complex systems.
authors.affiliation: Institut für Physik und CINSaT, Universität Kassel, Heinrich-Plett-Strasse 40, 34132 Kassel, Germany.
authors.forename: Tim
authors.initials: T
authors.lastname: Bayer
authors.affiliation: Institut für Physik und CINSaT, Universität Kassel, Heinrich-Plett-Strasse 40, 34132 Kassel, Germany.
authors.forename: Hendrike
authors.initials: H
authors.lastname: Braun
authors.affiliation: Institut für Physik und CINSaT, Universität Kassel, Heinrich-Plett-Strasse 40, 34132 Kassel, Germany.
authors.forename: Cristian
authors.initials: C
authors.lastname: Sarpe
authors.affiliation: Department Chemie, Ludwig-Maximilians-Universität München, Butenandt-Strasse 11, 81377 München, Germany.
authors.forename: Robert
authors.initials: R
authors.lastname: Siemering
authors.affiliation: Department Chemie, Ludwig-Maximilians-Universität München, Butenandt-Strasse 11, 81377 München, Germany.
authors.forename: Philipp
authors.initials: P
authors.lastname: von den Hoff
authors.affiliation: Department Chemie, Ludwig-Maximilians-Universität München, Butenandt-Strasse 11, 81377 München, Germany.
authors.forename: Regina
authors.initials: R
authors.lastname: de Vivie-Riedle
authors.affiliation: Institut für Physik und CINSaT, Universität Kassel, Heinrich-Plett-Strasse 40, 34132 Kassel, Germany.
authors.forename: Thomas
authors.initials: T
authors.lastname: Baumert
authors.affiliation: Institut für Physik und CINSaT, Universität Kassel, Heinrich-Plett-Strasse 40, 34132 Kassel, Germany.
authors.forename: Matthias
authors.initials: M
authors.lastname: Wollenhaupt