Femtosecond quantum control of molecular dynamics in the condensed phase推荐.pdf

INVITED ARTICLE /pccp | Physical Chemistry Chemical Physics Femtosecond quantum control of molecular dynamics in the condensed phase Patrick Nuernberger, Gerhard Vogt, Tobias Brixner and Gustav Gerber* Received 22nd December 2006, Accepted 12th February 2007 First published as an Advance Article on the web 13th March 2007 DOI: 10.1039/b618760a We review the progress in controlling quantum dynamical processes in the condensed phase with femtosecond laser pulses. Due to its high particle density the condensed phase has both high relevance and appeal for chemical synthesis. Thus, in recent years different methods have been developed to manipulate the dynamics of condensed-phase systems by changing one or multiple laser pulse parameters. Single-parameter control is often achieved by variation of the excitation pulse’s wavelength, its linear chirp or its temporal subpulse separation in case of pulse sequences. Multiparameter control schemes are more flexible and provide a much larger parameter space for an optimal solution. This is realized in adaptive femtosecond quantum control, in which the optimal solution is iteratively obtained through the combination of an experimental feedback signal and an automated learning algorithm. Several experiments are presented that illustrate the different control concepts and highlight their broad applicability. These fascinating achievements show the continuous progress on the way towards the control of complex quantum reactions in the condensed phase. I. Introduction Unfortunately, in most cases the ultrafast intramolecular vibrational redistribution (IVR) of the deposited energy pre- Optical time-resolved spectroscopy and frequency-resolved vents the breaking