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Chemical Physics Letters

Quantum phase dynamics of an initially one-mode amplitude-squeezed field interacting with a two-state molecular system

Masayoshi Nakano, Kizashi Yamaguchi

Published Apr 1, 1999• 9 citations
Publisher
DOI
10.1016/s0009-2614(99)00322-x

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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.

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International Journal of Theoretical Physics•Sep 6, 2013•1 citation
From the viewpoints of photon-phase and information-entropy dynamics, we investigate the dynamical behavior of initially one-mode amplitude- and phase-squeezed photon fields interacting with a two-state molecular system. A peculiar behavior of these systems is known to be the collapses and revivals of Rabi oscillation of the molecular population. As shown in previous studies, significant differences are observed in the amplitude and the period of the collapse−revival behavior for these fields. These differences are found to be well-described by the dynamical behavior of the photon phase (the Pegg−Barnett phase and the quasiprobability ( Q function) distributions). The features of these photon-phase dynamics are also found to provide significant influence on the time evolution of the information entropy of the molecule, which characterizes the degree of the entanglement between the molecule and the field.
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.
We perform numerically exact calculations of quantum dynamics for a two-state molecular model system interacting with initially single-mode strongly amplitude- and strongly phase-squeezed fields (average photon number 〈n̂〉=8). The second-order correlation function for these fields are taken to be 2, which is equivalent to that for the chaotic field with the identical average photon number. Although the responses of the molecule for these two squeezed fields are relatively similar to those for the chaotic field as shown in a previous paper, there are found to be some significant differences among these fields in the dynamical behavior of quantum-phase distributions of photons, i.e., the Pegg–Barnett phase and the Q function distributions. These differences are also elucidated by the dynamics of the information entropy for the molecule, i.e., molecular entropy, which represents the degree of entanglement between the molecule and the photon field.