Vibrational wavepackets high in the electronic ground state

Summary form only given. Recently we have introduced a new method named (TD) CARS for the preparation and monitoring of arbitrarily high vibrational wavepackets in the ground state. We use two independent time delays between the three laser fields of the CARS process. Starting from the equilibrium ground state of a molecule we excite the molecule with a short-laser pulse to a higher electronic state (pump). Next, we allow the generated wavepacket to evolve to a state which is strongly coupled to the desired ground state, and induce this transition by a second laser pulse (Stokes).