Layer-by-Layer Biosensor Assembly Incorporating Functionalized Quantum Dots

Constantine, Celeste A.; Gattás‐Asfura, Kerim M.; Mello, Sarita V.; Crespo, Gema; Rastogi, Vipin K.; Cheng, Thomas K.; DeFrank, Joseph; Leblanc, Roger M.

doi:10.1021/la035237y

Cited by 123 publications

(87 citation statements)

References 34 publications

(51 reference statements)

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“…[9][10][11][12] Due to their unique optical properties colloidal semiconductor quantum dots (QDs)-or nanocrystals-have proven to be valuable building blocks for many different types of applications ranging from light emitting devices [13][14][15] to photovoltaics [16][17][18] and sensors. [19][20][21] The energy flow from donors to acceptors generated in FRET structures can also be optimized by the use of QDs as energy donors and/or acceptors due to their tuneable, narrow emission features. Broad absorption spectra, high photostability, and quantum yield present additional advantages for FRET applications such as light harvesting structures 22,23 and sensing devices.…”

Section: Introductionmentioning

confidence: 99%

Concentration dependence of Förster resonant energy transfer between donor and acceptor nanocrystal quantum dot layers: Effect of donor-donor interactions

et al. 2011

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The influences of donor and acceptor concentrations on Förster resonant energy transfer (FRET) in a separated donor-acceptor quantum dot bilayer structure have been investigated. Donor intra-ensemble energy transfer is shown to have an impact on the donor-acceptor FRET efficiency in the bilayer structure. At high donor concentrations the FRET distance dependence and the acceptor concentration dependence in the separated donor-acceptor layer structure agree well with theories developed for FRET between randomly distributed, homogeneous donor and acceptor ensembles. However, discrepancies between measurement and theory are found at low donor concentrations. A donor concentration study shows that the FRET efficiency decreases with increasing donor concentration even though a donor concentration-independent FRET efficiency is predicted by standard theory. The observed dependence of the FRET efficiency on the donor concentration can be explained within the FRET rate model, for a constant, donor concentration independent FRET rate, by taking into account the concentration dependent donor reference lifetime arising from intra-donor ensemble FRET. This shows that the decrease in the FRET efficiency with increasing donor concentration is not a signature of a change in the donor-acceptor FRET rate, but due to the competition of the donor-acceptor and donor-donor energy transfer for the higher energy donors. As the intra-donor ensemble FRET represents another decay mechanism, the donor quantum yield for the higher energy donors decreases with increasing donor quantum dot (QD) concentration, as can also be seen from the redshift of the donor emission spectrum. Using this concentration dependent donor quantum yield in the calculation of the Förster radius, the FRET theory for homogeneous donor and acceptor ensembles can be modified to include the effect of the donor intra-ensemble transfer and to correctly describe the trends and absolute values of the measured FRET efficiencies as a function of the donor and the acceptor concentrations. These results show that in QD systems where intra-donor ensemble FRET is as important as the radiative and nonradiative donor decay mechanisms, the FRET rate rather than the FRET efficiency more appropriately characterizes the donor-acceptor FRET. By fitting with the rate model, FRET rates as high as (1.2 ns) −1 have been determined for the structures presented here.

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Section: Introductionmentioning

confidence: 99%

Concentration dependence of Förster resonant energy transfer between donor and acceptor nanocrystal quantum dot layers: Effect of donor-donor interactions

et al. 2011

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“…[12][13][14][15] Thus, it is used for the preparation of many different types of structures and has, in particular, shown valuable results for the preparation of light emitting and guiding structures, [24][25][26][27] photovoltaic devices, [28][29][30] sensors, and detectors. [31][32][33] Artificially designed microparticles and nanoparticles with multiple functionality can be synthesized with the help of the LbL technique and have been proposed for applications in areas such as quantum-information processing, optoelectronics, or biotechnology. [34][35][36] As the LbL deposition allows for the positioning of layers in nanometer steps, it is also beneficial for the investigation of energy transfer processes 17,19,21,22 as well as the interaction of surface plasmons with QDs.…”

Section: Introductionmentioning

confidence: 99%

Influence of quantum dot concentration on Förster resonant energy transfer in monodispersed nanocrystal quantum dot monolayers

et al. 2010

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The quantum dot ͑QD͒ concentration dependence of the optical properties of QD monolayers is shown to be dominated by Förster resonant energy transfer ͑FRET͒ from smaller to larger QDs in the ensemble. With increasing QD concentration a redshift of the peak emission wavelength, a shortening of the photoluminescence lifetime of the QDs on the high-energy side of the ensemble emission spectrum as well as increased difference in the lifetimes on the high-and low-energy sides are observed in the layer-by-layer deposited QD monolayers. There is also evidence of an increased rise time in the time-resolved photoluminescence decays on the low-energy side of the QD emission for two of the three samples presented in most detail. A theory of FRET in two dimensions is applied to explain the lifetime decrease on the high-energy side of the ensemble emission and confirms that the impact of the QD concentration on the optical properties is primarily due to FRET from the smaller to larger QDs in the ensemble. The concentration effects are stronger in QD samples which have a broader emission peak compared to the Stokes shift. Based on good agreement with FRET theory, the QD concentration and the overlap of the QD emission and absorption peaks can both be used to control the efficiency of the FRET process in monodispersed QD layers.

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“…Additional treatment with dithiol created a multilayer structure for the QDs 63 . Layer-by-layer adsorption techniques 64 have also been used to create organized QD structures.…”

Section: Quantum Dots On Substratesmentioning

confidence: 99%

Optical Pulse Interactions in Nonlinear Excited State Materials

Potasek¹,

McLaughlin²,

Parilov³

2008

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Layer-by-Layer Biosensor Assembly Incorporating Functionalized Quantum Dots

Cited by 123 publications

References 34 publications

Concentration dependence of Förster resonant energy transfer between donor and acceptor nanocrystal quantum dot layers: Effect of donor-donor interactions

Concentration dependence of Förster resonant energy transfer between donor and acceptor nanocrystal quantum dot layers: Effect of donor-donor interactions

Influence of quantum dot concentration on Förster resonant energy transfer in monodispersed nanocrystal quantum dot monolayers

Optical Pulse Interactions in Nonlinear Excited State Materials

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