Quantum Dots as Templates for Self-Assembly of Photoswitchable Polymers: Small, Dual-Color Nanoparticles Capable of Facile Photomodulation

Dı́az, Sebastián A.; Giordano, Luciana; Azcárate, Julio C.; Jovin, Thomas M.; Jares‐Erijman, Elizabeth A.

doi:10.1021/ja3117813

Cited by 75 publications

(48 citation statements)

References 63 publications

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“…264 By integrating secondary dyes such as Alexa647 and Lucifer Yellow into these types of constructs, ratiometric probes with internal standards were also achieved. 613,614 Lastly, a novel strategy in exploiting photoswitchable QDs was developed in the Winter Lab. In this case, the irradiation of an azobenzene PC dye modulated the hybridization kinetics of two DNA strands.…”

Section: Aptamermentioning

confidence: 99%

Energy Transfer with Semiconductor Quantum Dot Bioconjugates: A Versatile Platform for Biosensing, Energy Harvesting, and Other Developing Applications

Spillmann²,

et al. 2016

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Luminescent semiconductor quantum dots (QDs) are one of the more popular nanomaterials currently utilized within biological applications. However, what is not widely appreciated is their growing role as versatile energy transfer (ET) donors and acceptors within a similar biological context. The progress made on integrating QDs and ET in biological configurations and applications is reviewed in detail here. The goal is to provide the reader with (1) an appreciation for what QDs are capable of in this context, (2) how this field has grown over a relatively short time span, and, in particular, (3) how QDs are steadily revolutionizing the development of new biosensors along with a myriad of other photonically active nanomaterial-based bioconjugates. An initial discussion of QD materials along with key concepts surrounding their preparation and bioconjugation is provided given the defining role these aspects play in the QDs ability to succeed in subsequent ET applications. The discussion is then divided around the specific roles that QDs provide as either Förster resonance energy transfer (FRET) or charge/electron transfer donor and/or acceptor. For each QD-ET mechanism, a working explanation of the appropriate background theory and formalism is articulated before examining their biosensing and related ET utility. Other configurations such as incorporation of QDs into multistep ET processes or use of initial chemical and bioluminescent excitation are treated similarly. ET processes that are still not fully understood such as QD interactions with gold and other metal nanoparticles along with carbon allotropes are also covered. Given their maturity, some specific applications ranging from in vitro sensing assays to cellular imaging are separated and discussed in more detail. Finally a perspective on how this field will continue to evolve is provided.

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Section: Aptamermentioning

confidence: 99%

Energy Transfer with Semiconductor Quantum Dot Bioconjugates: A Versatile Platform for Biosensing, Energy Harvesting, and Other Developing Applications

Spillmann²,

et al. 2016

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“…Similar equations have been derived for other QD systems with multiple FRET pathways. 38 To test this model, FRET efficiencies were calculated for the (M, 0) and (0, N) data sets (eq 1), and values of k QD −1 k QD-555 and k QD −1 k QD-A647 were subsequently determined by fitting the efficiencies for these two data sets with eq 6. For convenience, the k QD Figure 4B plots the QD quenching efficiencies predicted in this manner versus the measured QD a Estimated from TEM micrographs.…”

Section: ■ Experimental Sectionmentioning

confidence: 99%

Energy Transfer Pathways in a Quantum Dot-Based Concentric FRET Configuration

Massey

Petryayeva

et al. 2015

J. Phys. Chem. C

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The unique optical properties of semiconductor quantum dots (QDs) are highly advantageous for biological imaging and analysis, particularly when combined with Forster resonance energy transfer (FRET). A recent innovation in this area has been concentric FRET (cFRET), wherein QDs are assembled with multiple copies of two different types of fluorescent label. Although multifunctional biological probes have been developed utilizing cFRET, a detailed photophysical analysis of cFRET has not been undertaken, and energy transfer in these probes has been understood only qualitatively. Here, we characterize a prototypical QD-(A555) M -(A647) N cFRET configuration through photoluminescence (PL) intensity, decay, and photobleaching measurements. This cFRET configuration combines a central, green-emitting QD with Alexa Fluor 555 (A555) and Alexa Fluor 647 (A647) dyes that are assembled to QDs through peptide linkers, where M and N are the numbers of A555 and A647 per QD. Following initial photoexcitation of the QD, the energy transfer pathways are QD-to-A555 and QD-to-A647, which compete with one another, and A555-to-A647, which occurs subsequent to QD-to-A555 energy transfer. A rate analysis, calibrated to the conventional QD-(A555) M and QD-(A647) N FRET systems, accurately predicts quenching efficiencies and permits a first approximation of dye/ QD PL intensity ratios in the cFRET configurations. CdSe/CdS/ZnS QDs and CdSeS/ZnS QDs of different sizes but similar emission characteristics are used for these experiments, and they demonstrate the general applicability of the analysis. The interplay between the three FRET pathways and nonideal behavior within this system is discussed with directions for future research. Overall, this study provides a framework and predictive power for the rational design and optimization of novel cFRET probes and biosensors for biological applications. ■ INTRODUCTIONColloidal semiconductor nanocrystals, or "quantum dots" (QDs), are of great interest for biological imaging and analysis. 1−3 These materials are well-known for their bright, spectrally narrow photoluminescence (PL), which is also resistant to photobleaching. 4,5 As recent reviews attest, QDs have been widely utilized as labels for multicolor fluorescence measurements and imaging, single-particle tracking, and superresolution imaging, with applications spanning in vitro assays, cellular imaging, and in vivo imaging. 1,6−8 The chemistry associated with these materials is also well developed: methods for the synthesis of CdSe/ZnS and related core/shell nanocrystals are established, 9,10 several QD materials are available commercially, a variety of ligand and polymer coatings can be used to transfer QDs into aqueous media, 11−13 and numerous methods for bioconjugation have been reported. 11,14,15 The cumulative optical properties of QDs, which additionally include larger one-photon and two-photon absorption coefficients, spectrally broad absorption profiles, good quantum yields, and precise wavelength-tuning of PL through size and comp...

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“…[37][38][39] For these reasons, among others, they have been suggested as the active elements in many emitterbased systems. 37,[40][41][42][43][44][45][46][47][48][49][50] RESULTS AND DISCUSSIONS…”

mentioning

confidence: 99%

Plasmonic Control of Radiative Properties of Semiconductor Quantum Dots Coupled to Plasmonic Ring Cavities

2015

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(Word Style "BD_Abstract").In recent years, a lot of effort has been made to achieve controlled delivery of target particles to the hotspots of plasmonic nano-antennas, in order to probe and/or exploit the extremely large field enhancements produced by such structures. While in many cases such high fields are advantageous, there are instances where they should be avoided. In this work, we consider the implications of using the standard nanoantenna geometries when colloidal quantum dots are employed as target entities. We show that in this case, and for various reasons, dimer antennas are not the optimum choice. Plasmonic Ring Cavities are a better option despite low field enhancements, as they allow collective coupling of many quantum dots in a reproducible and

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Quantum Dots as Templates for Self-Assembly of Photoswitchable Polymers: Small, Dual-Color Nanoparticles Capable of Facile Photomodulation

Cited by 75 publications

References 63 publications

Energy Transfer with Semiconductor Quantum Dot Bioconjugates: A Versatile Platform for Biosensing, Energy Harvesting, and Other Developing Applications

Energy Transfer with Semiconductor Quantum Dot Bioconjugates: A Versatile Platform for Biosensing, Energy Harvesting, and Other Developing Applications

Energy Transfer Pathways in a Quantum Dot-Based Concentric FRET Configuration

Plasmonic Control of Radiative Properties of Semiconductor Quantum Dots Coupled to Plasmonic Ring Cavities

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