Interferometry of quantum revivals

J Chem Phys. 2022 Aug 7;157(5):054304. doi: 10.1063/5.0098056.

Abstract

It has recently been shown that an interferometric approach can be used to obtain Auger lifetimes in molecules in certain point groups. Here, we extend this concept to those molecular states for which Auger decay is energetically forbidden and which exhibit initial quasi-exponential decay followed by quantum revivals. We demonstrate that this allows us to extract the quasi-exponential decay rate and the revival timescale. We solve analytically a model containing a state coupled to the idealized Bixon-Jortner quasicontinuum, and we obtain an interferometric signature of revival, which can be easily generalized to realistic systems. Moreover, we analyze how this revival signature is influenced by the system parameters, and we suggest optimal conditions for its observation. We, therefore, show that our new approach allows population revivals of a molecular state to be detected interferometrically.