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Synthetic Metals

Quantum-phase and information-entropy dynamics of molecular dimers and trimers interacting with quantized fields

Masayoshi Nakano, Kizashi Yamaguchi

Published Mar 1, 2001• 0 citations
Publisher
DOI
10.1016/s0379-6779(00)00902-4

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Quantum‐phase and information‐entropy dynamics of dimers interacting with a single‐mode coherent field: The difference between one‐ and two‐exciton models

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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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Ultracold molecules provide opportunities for exploring quantum matter, chemical dynamics and information processing thanks to their rich interactions, which can be controlled by external fields. Magnetic fields tune interactions through Feshbach resonances, enabling the formation of ultracold dimers and triatomic molecules from atom-dimer collisions. Here we demonstrate electric-field control of atom-molecule Feshbach resonances. In mixtures of ground-state sodium-potassium molecules and potassium atoms, electric fields shift resonance positions systematically, revealing specific trimer bound states and their electric-field dependent energies. The response differs markedly from isolated dimers, showing hindered rotation of the molecular constituent near an atom. Electric fields therefore add an independent knob for atom-molecule resonances, open spectroscopic access to triatomic quantum states, and advance controlled polyatomic quantum matter.

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Quantum-phase and information-entropy dynamics of a two-state molecular system interacting with strongly amplitude- and phase-squeezed fields

Masayoshi Nakano, Kizashi Yamaguchi

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.

The Journal of Chemical Physics•Feb 8, 2000•15 citations
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
Ultracold molecules provide opportunities for exploring quantum matter, chemical dynamics and information processing thanks to their rich interactions, which can be controlled by external fields. Magnetic fields tune interactions through Feshbach resonances, enabling the formation of ultracold dimers and triatomic molecules from atom-dimer collisions. Here we demonstrate electric-field control of atom-molecule Feshbach resonances. In mixtures of ground-state sodium-potassium molecules and potassium atoms, electric fields shift resonance positions systematically, revealing specific trimer bound states and their electric-field dependent energies. The response differs markedly from isolated dimers, showing hindered rotation of the molecular constituent near an atom. Electric fields therefore add an independent knob for atom-molecule resonances, open spectroscopic access to triatomic quantum states, and advance controlled polyatomic quantum matter.
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.