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Influence of a Phonon Bath on Electronic Correlations and Optical Response in Molecular Aggregates

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Nonlinear Optical Materials

Part of the book series: The IMA Volumes in Mathematics and its Applications ((IMA,volume 101))

Abstract

A generating function algorithm that allows the calculation of the optical response of coupled exciton-phonon systems is developed. For a model of assemblies of three-level molecules coupled via dipole interaction and interacting linearly with nuclear degrees of freedom, we derive a closed set of equations of motion for five generating functions representing the exact response to third order in the external field. These are equivalent to an infinite hierarchy of equations of motion for phonon-assisted variables. Starting with the equations for the generating functions, several reduction schemes are derived. By eliminating the phonon degrees of freedom in favor of self-energies, the Haken-Strobl model of relaxation is recovered as a limiting case. A set of time-local equations is presented extending the Haken-Strobl treatment by kee** the temperature dependence as well as the excitonic signatures of the phonon self-energies. Finally, we derive equations that interpolate between the coherent and incoherent limits of exciton propagation and properly include the two exciton dynamics.

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Authors and Affiliations

  1. Department of Chemistry, University of Rochester, Rochester, NY, 14627, USA

    Vollrath M. Axt & Shaul Mukamel

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  1. Vollrath M. Axt
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  2. Shaul Mukamel
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Editors and Affiliations

  1. Arizona Center for Mathematical Sciences Department of Mathematics, University of Arizona, Tuscon, AZ, 85721, USA

    Jerome V. Moloney

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© 1998 Springer Science+Business Media New York

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Axt, V.M., Mukamel, S. (1998). Influence of a Phonon Bath on Electronic Correlations and Optical Response in Molecular Aggregates. In: Moloney, J.V. (eds) Nonlinear Optical Materials. The IMA Volumes in Mathematics and its Applications, vol 101. Springer, New York, NY. https://doi.org/10.1007/978-1-4612-1714-5_1

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  • DOI: https://doi.org/10.1007/978-1-4612-1714-5_1

  • Publisher Name: Springer, New York, NY

  • Print ISBN: 978-1-4612-7253-3

  • Online ISBN: 978-1-4612-1714-5

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