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Langmuir 25, 5 (2009) 3232-9
Wrapping nanocrystals with an amphiphilic polymer preloaded with fixed amounts of fluorophore generates FRET-based nanoprobes with a controlled donor/acceptor ratio.
Aleksey V Yakovlev 1, Feng Zhang 2, Ali Zulqurnain, Abbasi Azhar-Zahoor, Camilla Luccardini 3, Stéphane Gaillard 4, Jean-Maurice Mallet 5, Patrick Tauc 6, Jean-Claude Brochon 6, Wolfgang J Parak, Anne Feltz 7, Martin Oheim 7
(2009-03-03)

Colloidal nanocrystal (NC) donors wrapped with a polymer coating including multiple organic acceptor molecules are promising scaffolds for fluorescence resonance energy transfer (FRET)-based nanobiosensors. Over other self-assembling donor-acceptor configurations, our preloaded polymers have the virtue of producing compact assemblies with a fixed donor/acceptor distance. This property, together with the possibility of stoichiometric polymer loading, allowed us to directly address how the FRET efficiency depended on the donor/acceptor. At the population level, nanoprobes based on commercial as well as custom CdSe/ZnS donors displayed the expected dose-dependent rise in transfer efficiency, saturating from about five ATTO dyes/NC. However, for a given acceptor concentration, both the intensity and lifetime of single-pair FRET data revealed a large dispersion of transfer efficiencies, highlighting an important heterogeneity among nominally identical FRET-based nanoprobes. Rigorous quality check during synthesis and shell assembly as well as postsynthesis sorting and purification are required to make hybrid semiconductor-organic nanoprobes a robust and viable alternative to organic or genetically encoded nanobiosensors.
1:  School of EECE
University of Newcastle upon Tyne
2:  Institute of Low Energy Nuclear Physics
Beijing Normal University / Beijing
3:  Laboratoire Kastler Brossel (LKB (Lhomond))
CNRS : UMR8552 – Université Pierre et Marie Curie [UPMC] - Paris VI – Ecole normale supérieure de Paris - ENS Paris
4:  Institut de Mathématiques de Bordeaux (IMB)
CNRS : UMR5251 – Université Sciences et Technologies - Bordeaux I – Université Victor Segalen - Bordeaux II
5:  BIOMOLÉCULES : SYNTHÈSE, STRUCTURE ET MODE D'ACTION (UMR CNRS 8642.)
Ecole Normale Suprieure,
6:  Laboratoire de Biotechnologie et Pharmacologie génétique Appliquée (LBPA)
CNRS : UMR8113 – École normale supérieure de Cachan - ENS Cachan
7:  Neurobiologie cellulaire et moléculaire (NCM)
CNRS : UMR8544 – Ecole normale supérieure de Paris - ENS Paris
Life Sciences/Biochemistry, Molecular Biology/Biophysics