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Examining Förster Energy Transfer for Semiconductor Nanocrystalline Quantum Dot Donors and Acceptors

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journal contribution
posted on 04.09.2008, 00:00 authored by Carles Curutchet, Alberto Franceschetti, Alex Zunger, Gregory D. Scholes
Excitation energy transfer involving semiconductor quantum dots (QDs) has received increased attention in recent years because their properties, such as high photostability and size-tunable optical properties, have made QDs attractive as Förster resonant energy transfer (FRET) probes or sensors. An intriguing question in FRET studies involving QDs has been whether the dipole approximation, commonly used to predict the electronic coupling, is sufficiently accurate. Accurate estimates of electronic couplings between two 3.9 nm CdSe QDs and between a QD and a chlorophyll molecule are reported. These calculations are based on transition densities obtained from atomistic semiempirical calculations and time-dependent density functional theory for the QD and the chlorophyll, respectively. In contrast to the case of donor−acceptor molecules, where the dipole approximation breaks down at length scales comparable to the molecular dimensions, we find that the dipole approximation works surprisingly well when donor and/or acceptor is a spherical QD, even at contact donor−acceptor separations. Our conclusions provide support for the use of QDs as FRET probes for accurate distance measurements.

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