Adiabatic climbing of vibrational ladders using Raman transitions with chirped pump lasers: effect of higher electronic surfaces and control of the shapes of vibrational wave packets

• DOI: 10.1002/jrs.1738
• Publication Date: 2007-04-11T19:33:30Z
• Authors: Deyana S. Tchitch...; Szczepan Chelkowski; André D. Bandrauk
• Keywords: 0103 physical sciences; 01 natural sciences; 7. Clean energy

Abstract Using numerical solutions of the time‐dependent Schrödinger equation for H 2 molecule in intense laser fields we calculate vibrational excitation induced by Raman chirped adiabatic process (RCAP). We show that adding several higher electronic surfaces to a simple two‐surface model improves efficiency ladder‐climbing at intensities below adiabaticity threshold. Furthermore, although using photon energies close one‐photon transition frequency allows use lower pump and Stokes intensities, general, this leads more population transfer upper accompanied loss selectivity on ground‐state surface. By contrast, considerable dissociation yields can be achieved when energy photons are used. also investigate structure time‐dependant wave packets prepared RCAP. find specific times packet is very well localised large inter‐nuclear separations which ionisation occurs with probability 3 orders magnitude larger than equilibrium separation. Copyright © 2007 John Wiley & Sons, Ltd.