Collapses and revivals of polarization and radiation intensity induced by strong exciton-vibron coupling

Abstract: Recently, systems with strong coupling between electronic and vibrational degrees of freedom attract a great attention. In this work, we consider the transient dynamics of the system consisting of strongly coupled vibron and exciton driven by external monochromatic field. We show that under coherent pumping, polarization of exciton exhibits complex quantum dynamics which can be divided into three stages. At the first stage, exciton oscillations at its eigenfrequency relax due to the transition to set of shifted Fock states of vibrons. We demonstrate that these shifted Fock states play the role of an effective reservoir for the excited exciton state. The time of relaxation to this reservoir depends on exciton-vibron coupling. At the second stage, excitation, transferred to the reservoir of the vibronic shifted states at the first stage, returns into electronic degrees of freedom and revival of oscillations at exciton eigenfrequency appears. Thus, the dynamics of molecular polarization exhibit collapses and revivals. At the final stage, these collapses and revivals dissipate and polarization exhibits Rayleigh response at the frequency of the external field. Discovered collapses and revivals manifest in radiation spectrum as multiple splitting of the spectral line near the exciton transition frequency.