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arXiv:quant-ph/0209078 · Physics Letters A

Resonant transfer of excitons and quantum computation

Brendon W. Lovett, John Henry Reina, Ahsan Nazir, Beeneet Kothari, G.Andrew D. Briggs

Published Jul 16, 2003• 36 citations
arXivHTMLPDF
DOI
10.1016/s0375-9601(03)00999-x

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The rates of exciton transfer within dyads of perylene diimide and terrylene diimide connected by oligophenylene bridge units have been shown to deviate significantly from those of Förster's resonance energy transfer theory, according to single molecule spectroscopy experiments. The present work provides a detailed computational and theoretical study investigating the source of such discrepancy. Electronic spectroscopy data are calculated by time-dependent density function theory and then compared with experimental results. Electronic couplings between exciton donor and acceptor are estimated based on both transition density cube method and transition dipole approximation. These results confirm that the delocalization of exciton to the bridge parts contribute to significant enhancement of donor-acceptor electronic coupling. Mechanistic details of exciton transfer are examined by estimating the contributions of the bridge electronic states, vibrational modes of the dyads commonly coupled to both donor and acceptor, inelastic resonance energy transfer mechanism, and dark exciton states. These analyses suggest that the contribution of common vibrational modes serves as the main source of deviation from Förster's spectral overlap expression.