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Influence of a phonon bath on electronic correlations and optical response in molecular aggregates

Title data

Axt, Vollrath M. ; Mukamel, Shaul:
Influence of a phonon bath on electronic correlations and optical response in molecular aggregates.
In: Moloney, Jerome V. (ed.): Nonlinear Optical Materials. - Berlin ; New York : Springer , 1998 . - pp. 1-32 . - (IMA Volumes in Mathematics and Its Applications ; 101 )
ISBN 0-387-98581-6
DOI: https://doi.org/10.1007/978-1-4612-1714-5_1

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Project information

Project financing: Deutsche Forschungsgemeinschaft
National Science Foundation and the US Air Force office of scientific research

Abstract in another language

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 keeping 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.

Further data

Item Type: Article in a book
Refereed: Yes
Keywords: generating functions; phonons; molecular aggregates; ultrafast dynamics; Frenkel-excitons; nonlinear optics
Institutions of the University: Faculties > Faculty of Mathematics, Physics und Computer Science > Department of Physics
Faculties > Faculty of Mathematics, Physics und Computer Science > Department of Physics > Chair Theoretical Physics III > Chair Theoretical Physics III - Univ.-Prof. Dr. Martin Axt
Faculties
Faculties > Faculty of Mathematics, Physics und Computer Science
Faculties > Faculty of Mathematics, Physics und Computer Science > Department of Physics > Chair Theoretical Physics III
Result of work at the UBT: No
DDC Subjects: 500 Science > 530 Physics
Date Deposited: 17 Oct 2017 08:18
Last Modified: 17 Oct 2017 08:18
URI: https://eref.uni-bayreuth.de/id/eprint/40024