Imaging wavepacket interferences using Auger resonant Raman spectroscopy

Novel interference effects are observed in the Auger resonant Raman transitions of core-excited HF. Pronounced oscillations, controlled by detuning above the resonance maximum, appear in the spectator decay spectra of the dissociating molecule. Using predictions from the time-dependent theory of the resonant inelastic Raman scattering, these observations are explained by a favorable spatial localization of the nuclear wavepacket in the intermediate state during its creation. This phenomenon should occur whenever photoexcitation, electronic decay and nuclear dynamics have comparable time scales.