Nature of polarized excitons

  • Ambjörnsson T
  • Apell S
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The electromagnetic interaction energy of a molecular aggregate consisting of pointlike molecules in the presence of an electromagnetic field is derived. The corresponding Hamiltonian consists of three parts; H0 describes the aggregate in the absence of the electromagnetic field, H1 describes the interaction of the molecules with the external field, and H2 corresponds to the induced interaction between the molecules. Based on this Hamiltonian we derive a self-consistent equation of motion for a quasiparticle, which we refer to as a polarized exciton. The equation has the same form as the one in classical dipole theory. The polarized exciton model is based on a time-dependent perturbative treatment and corresponds to the assumption H0@H11H2 . Our model is compared to standard exciton theory, which is based on the assumption H0@H2@H1 . In particular the differences and similarities are illustrated for a direct example, a finite linear chain. We advocate the use of polarized excitons to fully account for the physics in these systems. © 2001 American Institute of Physics. @DOI: 10.1063/1.1343873#

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  • T. Ambjörnsson

  • S. P. Apell

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