High-precision molecular wave-packet interferometry with HgAr dimers

Molecular wave-packet (WP) interferometry has been demonstrated in the A electronic state of the HgAr van der Waals complex with two time-delayed UV fs pulses at 254 nm. The interferograms of three vibrational levels in the WP's display almost 100% fringe contrast as a function of the interpulse delay tau, which is tuned with sub-10 as stability and resolution. It is clearly observed that the three interferograms show their dephasing and rephasing within a single vibrational period, allowing us to prepare arbitrary relative populations of the three levels by adjusting a single parameter tau.