A Hybrid Quantum Dot−Antibody Fragment Fluorescence Resonance Energy Transfer-Based TNT Sensor

Goldman, Ellen R.; Medintz, Igor L.; Whitley, Jessica L.; Hayhurst, Andrew; Clapp, Aaron R.; Uyeda, H. Tetsuo; Deschamps, Jeffrey R.; Lassman, Michael E.; Mattoussi, Hedi

doi:10.1021/ja043677l

Cited by 552 publications

(457 citation statements)

References 32 publications

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“…In comparison with the other work on MIP@QDs for use in detection applications, [25][26][27][28]41,42 the developed DMIP@QDs showed excellent selectivity but low sensitivity. This problem of low sensitivity commonly exists for MIP@QDs-based systems.…”

Section: ■ Results and Discussionmentioning

confidence: 81%

Dummy Molecularly Imprinted Polymers-Capped CdTe Quantum Dots for the Fluorescent Sensing of 2,4,6-Trinitrotoluene

et al. 2013

ACS Appl. Mater. Interfaces

272

149

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Molecularly imprinted polymers (MIPs) with trinitrophenol (TNP) as a dummy template molecule capped with CdTe quantum dots (QDs) were prepared using 3-aminopropyltriethoxy silane (APTES) as the functional monomer and tetraethoxysilane (TEOS) as the cross linker through a seedgrowth method via a sol−gel process (i.e., DMIP@QDs) for the sensing of 2,4,6-trinitrotoluene (TNT) on the basis of electrontransfer-induced fluorescence quenching. With the presence and increase of TNT in sample solutions, a Meisenheimer complex was formed between TNT and the primary amino groups on the surface of the QDs. The energy of the QDs was transferred to the complex, resulting in the quenching of the QDs and thus decreasing the fluorescence intensity, which allowed the TNT to be sensed optically. DMIP@QDs generated a significantly reduced fluorescent intensity within less than 10 min upon binding TNT. The fluorescence-quenching fractions of the sensor presented a satisfactory linearity with TNT concentrations in the range of 0.8−30 μM, and its limit of detection could reach 0.28 μM. The sensor exhibited distinguished selectivity and a high binding affinity to TNT over its possibly competing molecules of 2,4-dinitrophenol (DNP), 4-nitrophenol (4-NP), phenol, and dinitrotoluene (DNT) because there are more nitro groups in TNT and therefore a stronger electron-withdrawing ability and because it has a high similarity in shape and volume to TNP. The sensor was successfully applied to determine the amount of TNT in soil samples, and the average recoveries of TNT at three spiking levels ranged from 90.3 to 97.8% with relative standard deviations below 5.12%. The results provided an effective way to develop sensors for the rapid recognition and determination of hazardous materials from complex matrices.

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Section: ■ Results and Discussionmentioning

confidence: 81%

Dummy Molecularly Imprinted Polymers-Capped CdTe Quantum Dots for the Fluorescent Sensing of 2,4,6-Trinitrotoluene

et al. 2013

ACS Appl. Mater. Interfaces

272

149

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“…Although a noncovalent conjugation strategy is used here, the ratio of His 6 peptide and thus acceptor DNA acceptor per QD is also easily controlled through the molar ratio added for self-assembly with the QD as repeatedly demonstrated in Refs. [1,2,6,7,11,13,14,21,23] and discussed in detail in references [13,21,23].…”

Section: Discussionmentioning

confidence: 99%

Improved peptidyl linkers for self-assembly of semiconductor quantum dot bioconjugates

Berti

D’Agostino²,

Boeneman

et al. 2009

Nano Res.

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We demonstrate improved peptide linkers which allow both conjugation to biomolecules such as DNA and self-assembly with luminescent semiconductor quantum dots. A hexahistidine peptidyl sequence was generated by standard solid phase peptide synthesis and modified with the succinimidyl ester of iodoacetamide to yield a thiol-reactive iodoacetyl polyhistidine linker. The reactive peptide was conjugated to dye-labeled thiolated DNA which was utilized as a model target biomolecule. Agarose gel electrophoresis and fl uorescence resonance energy transfer analysis confi rmed that the linker allowed the DNA to self-assemble with quantum dots via metal-affi nity driven coordination. In contrast to previous peptidyl linkers that were based on disulfi de exchange and were thus labile to reduction, the reactive haloacetyl chemistry demonstrated here results in a more stable thioether bond linking the DNA to the peptide which can withstand strongly reducing environments such as the intracellular cytoplasm. As thiol groups occur naturally in proteins, can be engineered into cloned proteins, inserted into nascent peptides or added to DNA during synthesis, the chemistry demonstrated here can provide a simple method for self-assembling a variety of stable quantum dot bioconjugates.

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“…In fact, clever assays for the recognition of various analytes are starting to be designed on the basis of energy transfer processes (18)(19)(20)(21)(22)(23)(24)(25)(26)(27)(28)(29)(30)(31)(32)(33)(34). Instead, mechanisms based on electron transfer still remain to be explored (35,36).…”

mentioning

confidence: 99%

A mechanism to signal receptor–substrate interactions with luminescent quantum dots

Yildiz

Tomasulo

Raymo

2006

Proc. Natl. Acad. Sci. U.S.A.

136

106

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Semiconductor quantum dots are becoming valuable analytical tools for biomedical applications. Indeed, their unique photophysical properties offer the opportunity to design luminescent probes for imaging and sensing with unprecedented performance. In this context, we have identified operating principles to transduce the supramolecular association of complementary receptor-substrate pairs into an enhancement in the luminescence of sensitive quantum dots. Our mechanism is based on the electrostatic adsorption of cationic quenchers on the surface of anionic quantum dots. The adsorbed quenchers suppress efficiently the emission character of the associated nanoparticles on the basis of photoinduced electron transfer. In the presence of target receptors able to bind the quenchers and prevent electron transfer, however, the luminescence of the quantum dots is restored. Thus, complementary receptor-substrate pairs can be identified with luminescence measurements relying on our design logic. In fact, we have demonstrated with a representative example that our protocol can be adapted to signal protein-ligand interactions.electron transfer ͉ luminescent chemosensors ͉ nanoparticles ͉ proteinligand interactions S emiconductor quantum dots are inorganic nanoparticles with remarkable photophysical properties (1-5). In particular, their one-and two-photon absorption cross-sections, luminescence lifetimes, and photobleaching resistances are significantly greater than those of conventional organic fluorophores. Furthermore, their broad absorption bands extend continuously from the UV to the visible region of the electromagnetic spectrum and, therefore, offer a vast selection of possible excitation wavelengths. Instead, their narrow emission bands can be positioned precisely within the visible and near-infrared regions with fine adjustments of their physical dimensions. In fact, pools of quantum dots with different diameters can be designed to emit in parallel at different wavelengths after excitation at a single wavelength, offering the opportunity to implement unprecedented multichannel assays.Organic dyes do not offer the unique collection of attractive photophysical properties associated with semiconductor quantum dots. Indeed, it is becoming apparent that these inorganic nanoparticles can complement, if not replace, their organic counterparts in a diversity of biomedical applications (6-12). Nonetheless, decades of intensive investigations on the structure and properties of organic chromophores have indicated valuable strategies to design sensitive fluorescent probes able to signal the presence of target analytes with changes in emission intensity (13-16). Their operating principles generally rely on the covalent connection of a fluorescent component to a receptor unit. The receptor is engineered to quench the emission of the fluorophore on the basis of either electron or energy transfer. The supramolecular association of the receptor with a complementary analyte, however, suppresses the quenching mechanism and leads to a si...

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A Hybrid Quantum Dot−Antibody Fragment Fluorescence Resonance Energy Transfer-Based TNT Sensor

Cited by 552 publications

References 32 publications

Dummy Molecularly Imprinted Polymers-Capped CdTe Quantum Dots for the Fluorescent Sensing of 2,4,6-Trinitrotoluene

Dummy Molecularly Imprinted Polymers-Capped CdTe Quantum Dots for the Fluorescent Sensing of 2,4,6-Trinitrotoluene

Improved peptidyl linkers for self-assembly of semiconductor quantum dot bioconjugates

A mechanism to signal receptor–substrate interactions with luminescent quantum dots

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