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Förster Coupling in Nanoparticle Excitonic Circuits

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2010

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American Chemical Society
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Rebentrost, Patrick, Michael Stopa, and Alán Aspuru-Guzik. 2010. Förster coupling in nanoparticle excitonic circuits. Nano Letters 10(8): 2849–2856.

Abstract

Exciton transport in semiconductor nanoparticles underlies recent experiments on electrically controlled nanostructures and proposals for new artificial light-harvesting systems. In this work, we develop a novel method for the numerical evaluation of the Förster matrix element, based on a three-dimensional real space grid and the self-consistent solution of the mesoscopic exciton in a macroscopic dielectric environment. This method enables the study of the role of the nanoparticle shape, spatially varying dielectric environments, and externally applied electric fields. Depending on the orientation of the transition dipole, the Förster coupling is shown to be either increased or decreased as a function of the nanoparticle shape and of the properties of the dielectric environment. In the presence of an electric field, we investigate the relation between excitonic binding and confinement effects. We also study a type II core−shell quantum dot where electron and hole are spatially separated due to a particular configuration of the bandstructure.

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dielectric effects, Förster theory, quantum dots, excitation energy transfer

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