Modeling of quantum beats of the state populations of a molecule

Abstract

Analytical expressions for describing the dynamics of the populations of the states of a five-level model molecule during fluorescence reflecting the quantum beats of the populations of its two excited degenerate states coupled by dynamic interaction are derived. The cases of excitation of the molecule by a short light pulse in a state with an energy higher than the energy of the degenerate states and into one of the degenerate states are considered. The populations of states are determined by solving the Schrödinger equation for the amplitudes of probability of populating the states of the composite system comprised of the molecule and a quantized radiation field. It was found that the resulting expressions satisfy the optical Bloch equations for the considered dynamics of the populations of the molecule’s states. Significant distinctions of the present results on the simulation of quantum beats from the corresponding simulation results reported in some works, performed based on different approaches, are revealed. The reasons for these differences are discussed.