Quantum-phase and information-entropy dynamics of a molecular system interacting with a two-mode squeezed coherent field

Abstract

We investigate the quantum dynamics for a molecular-state-model system interacting with a resonant two-mode squeezed coherent field, in which each mode is initially correlated. As an example, we consider a three-state molecular model, which mimics the electronic excited states of trans-octatetraene obtained by a full-configuration-interaction calculation using the Pariser-Parr-Pople Hamiltonian, interacting with a two-mode squeezed coherent field. For comparison, we also perform parallel studies, in which the initial fields are prepared in uncorrelated two-mode states, i.e., a two-mode coherent state and a two-mode thermal state. It is well known that the case of two-mode coherent field leads to the usual collapse-revival phenomena of the Rabi oscillations, while the case of a two-mode thermal state leads to an irregular evolution of them. Although the two-mode squeezed coherent field exhibits similar collapse-revival behavior to that for the two-mode coherent field, some differences are detected in the amplitudes and periods of collapse-revival oscillations. Further, the dynamics of off-diagonal molecular density matrices between the ground and second excited states for these two fields are found to be distinctively different from each other. Such attractive behavior is found to be closely associated with the two-mode photon-phase dynamics obtained by the Pegg-Barnett phase operator and the initial quasiprobability (Q function) distribution of photons. These differences in phase properties are also shown to significantly affect the dynamics of the information entropy for a molecule, i.e., molecular entropy, which represents the degree of entanglement between the molecule and photons.