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Chemical Physics Letters

Intermolecular-interaction effects on quantum-phase and information-entropy dynamics of dimers interacting with a single-mode coherent field

Masayoshi Nakano, Kizashi Yamaguchi

Published Jul 1, 2000• 10 citations
Publisher
DOI
10.1016/s0009-2614(00)00594-7

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Abstract We develop a numerically exact approach to the quantum‐phase and information‐entropy dynamics of a molecular aggregate interacting with quantized fields. It is well known that a peculiar quantum nature, i.e., collapses and revivals, is observed in monomer and noninteracting aggregate models. In this article, we investigate the intermolecular interaction effects on the collapse‐revival behavior using several dimer models (composed of two‐state monomers with different intermolecular distances) interacting with a single‐mode coherent photon field. The intermolecular interaction is taken into account by using the dipole‐dipole interaction. Also, one‐ and two‐exciton dimer models are considered in order to elucidate the exciton contributions to collapse‐revival behavior. This quantum behavior is analyzed from the viewpoint of the dynamics of Pegg–Barnett photon‐phase and information‐entropy of dimers, which closely relate to the time evolution of quantum coherency between the ground and the excited dimer states and the degree of the entanglement between dimer and photon, respectively. It is found that the intermolecular interaction and the two‐exciton generation provide remarkable changes in the collapse‐revival behavior through their significant influence on the quantum‐phase dynamics and the photon‐dimer entanglement. From the dimer entropy dynamics, intermediate intermolecular interaction is found to cause the momentary decrease in the photon‐dimer correlation in the early time region. This feature leads to the enhancement of off‐diagonal density (quantum coherency) between two dimers. © 2001 John Wiley & Sons, Inc. Int J Quantum Chem, 2001

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Abstract We develop a numerically exact approach to the quantum‐phase and information‐entropy dynamics of a molecular aggregate interacting with quantized fields. It is well known that a peculiar quantum nature, i.e., collapses and revivals, is observed in monomer and noninteracting aggregate models. In this article, we investigate the intermolecular interaction effects on the collapse‐revival behavior using several dimer models (composed of two‐state monomers with different intermolecular distances) interacting with a single‐mode coherent photon field. The intermolecular interaction is taken into account by using the dipole‐dipole interaction. Also, one‐ and two‐exciton dimer models are considered in order to elucidate the exciton contributions to collapse‐revival behavior. This quantum behavior is analyzed from the viewpoint of the dynamics of Pegg–Barnett photon‐phase and information‐entropy of dimers, which closely relate to the time evolution of quantum coherency between the ground and the excited dimer states and the degree of the entanglement between dimer and photon, respectively. It is found that the intermolecular interaction and the two‐exciton generation provide remarkable changes in the collapse‐revival behavior through their significant influence on the quantum‐phase dynamics and the photon‐dimer entanglement. From the dimer entropy dynamics, intermediate intermolecular interaction is found to cause the momentary decrease in the photon‐dimer correlation in the early time region. This feature leads to the enhancement of off‐diagonal density (quantum coherency) between two dimers. © 2001 John Wiley & Sons, Inc. Int J Quantum Chem, 2001
We investigate the intermolecular-interaction (dipole–dipole interaction) effects on the quantum dynamics of dimer density matrices and photon-phase distributions using several dimer models with different intermolecular distances in the presence of a two-mode squeezed vacuum field. In this photon field, each mode is initially correlated and the reduced one-mode photon distribution is equivalent with that of a thermal field. For comparison, we perform parallel studies, in which the initial fields are two types of noncorrelated two-mode fields, i.e., a two-mode coherent field and a two-mode thermal field. It is found that although the two-mode squeezed vacuum field causes the random oscillations of dimer populations in the noninteracting dimer, the periodic oscillations like the collapse–revival behavior emerge as the intermolecular distance decreases (the intermolecular interaction increases). Similar and dissimilar features among quantum dynamics caused by these three types of fields are investigated by analyzing the dynamical behavior of two-mode Pegg–Barnett photon-phase distributions and off-diagonal dimer density matrices, which indicate the coherency between dimer states. In addition to the quantum statistical properties of initial photon field, the change in the degree of contribution between one- and two-photon processes caused by the intermolecular interaction is found to be important to determine these features.
It is well-known that the interaction among atoms/molecules and quantized electromagnetic fields with a small number of photons provides a peculiar quantum nature, i.e., collapses and revivals in the Rabi oscillations. In this study, we investigate the intermolecular interaction (dipole–dipole interaction) effect on the collapse-revival behavior using several dimer models (composed of two kinds of two-state monomers with slightly different excitation energies) with different intermolecular distances in the presence of a two-mode squeezed coherent field, in which each mode is initially correlated. It is found that although the collapse-revival behavior is fairly overlapped and indistinct in the case of a noninteracting dimer under the present two-mode squeezed coherent field, the decrease in the intermolecular distance (the increase in the intermolecular interaction) resurrects relatively distinct collapse-revival behavior with longer collapse and revival times. By analyzing the quantum behavior from the viewpoint of the dynamics of two-mode Pegg–Barnett photon-phase distributions and off-diagonal dimer density matrices, this feature is found to closely relate to a significant change in the degree of contribution between one- and two-photon processes caused by the variation in the intermolecular interaction.