Charge oscillation controlled molecular excitation

• Published in: Physical review letters Vol. 110; no. 12; p. 123003
• Main Authors: Bayer, Tim, Braun, Hendrike, Sarpe, Cristian, Siemering, Robert, von den Hoff, Philipp, de Vivie-Riedle, Regina, Baumert, Thomas, Wollenhaupt, Matthias
• Format: Journal Article
• Language: English
• Published: United States 22.03.2013
• ISSN: 1079-7114
• DOI: 10.1103/physrevlett.110.123003

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.