Enhanced Total Vibrational Excitation Yield in a Slow Narrow-Pulsed Hydrogen Molecular Beam

High-efficiency excitation of a molecular beam is critical for investigating state-selected chemistry. However, achieving vibrational excitation of the entire beam for Raman-active molecules such as H₂ proves extremely challenging, primarily because laser pulses are much shorter than the molecular beam. In this study, we achieve a total excitation efficiency of over 20% by employing stimulated Raman pumping (SRP) in a slow, narrow-pulsed molecular beam. Through optimizing the intensity and spot shape of the SRP lasers, we attain saturated excitation within the laser crossing region. Furthermore, by reducing the beam velocity and narrowing the beam pulse using a cold valve and a fast chopper, we significantly enhance the total excitation yield. COMSOL simulation and a newly developed model reveal that a critical velocity allows the chopper to block unexcited molecules and reserve most of the excited ones from the beam, resulting in the highest overall excitation yield. This innovative setup opens new possibilities for state-selected experiments in surface science and ion–molecule reaction dynamics, particularly involving weak transitions and pulsed lasers.