Missing Rung Problem in Vibrational Ladder Climbing

TL;DR

This paper investigates the missing rung problem in vibrational ladder climbing, identifies its mechanism, and proposes a chirped pulse method to enhance molecular dissociation efficiency, supported by wavepacket simulations.

Contribution

It introduces a novel chirped pulse technique to overcome the missing rung problem in VLC, improving dissociation efficiency in molecular systems.

Findings

Chirped pulses restore VLC in LiH dissociation.

Quantum interference influences VLC excitation.

Method significantly outperforms conventional approaches.

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.