Missing Rung Problem in Vibrational Ladder Climbing

Abstract

We observed vanishing of the transition dipole moment, interrupting vibrational ladder climbing (VLC) in molecular systems. We clarified the mechanism of this phenomenon and present a method to use an additional chirped pulse to preserve the VLC. To show the effectiveness of our method, we conducted wavepacket dynamics simulations for LiH dissociations with chirped pulses. The results indicate that the efficiency of LiH dissociation is significantly improved by our method compared to conventional methods. We also revealed the quantum interference effect behind the excitation process of VLC.