Artificial Light‐Harvesting System Based on Multifunctional Surface‐Cross‐Linked Micelles

Peng, Hui‐Qing; Chen, Yuzhe; Zhao, Yan; Yang, Qing‐Zheng; Wu, Li‐Zhu; Tung, Chen‐Ho; Zhang, Liping; Tong, Qing‐Xiao

doi:10.1002/ange.201107723

Cited by 44 publications

(20 citation statements)

References 53 publications

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“…A promising direction is to use the light-harvesting concept realized by Nature in photosynthetic centres,16 where multiple strongly communicating donors can efficiently collect and deliver the light energy to a single acceptor using Förster Resonance Energy Transfer (FRET) 17. Chemists developed highly efficient FRET systems that use conjugated polymers,18–20 dendrimers,21,22 multi-porphyrin arrays,23 micellar NPs,24–26 polymer NPs,27 dye assemblies,28,29 metal-organic frameworks,30 or nucleic acids 31. However, the obtained amplification of the acceptor has never reached 1,000 so far,32 being limited by self-quenching of donors at high local concentration and/or inefficient donor-donor coupling.…”

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confidence: 99%

Giant light-harvesting nanoantenna for single-molecule detection in ambient light

et al. 2017

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Here, we explore the enhancement of single molecule emission by polymeric nano-antenna that can harvest energy from thousands of donor dyes to a single acceptor. In this nano-antenna, the cationic dyes are brought together in very close proximity using bulky counterions, thus enabling ultrafast diffusion of excitation energy (≤30 fs) with minimal losses. Our 60-nm nanoparticles containing >10,000 rhodamine-based donor dyes can efficiently transfer energy to 1-2 acceptors resulting in an antenna effect of ~1,000. Therefore, single Cy5-based acceptors become 25-fold brighter than quantum dots QD655. This unprecedented amplification of the acceptor dye emission enables observation of single molecules at illumination powers (1-10 mW cm-2) that are >10,000-fold lower than typically required in single-molecule measurements. Finally, using a basic setup, which includes a 20X air objective and a sCMOS camera, we could detect single Cy5 molecules by simply shining divergent light on the sample at powers equivalent to sunlight.

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confidence: 99%

Giant light-harvesting nanoantenna for single-molecule detection in ambient light

et al. 2017

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“…50 We first cross-linked its micelle on the surface by the Cu(I)-catalyzed click reaction with diazide 6 . 51, 52 The surface-cross-linked micelle was further functionalized by the click reaction with monoazide 7 . The functionalization decorates the micelle with a layer of hydrophilic ligands to improve its water-solubility.…”

Section: Resultsmentioning

confidence: 99%

Selective Binding of Folic Acid and Derivatives by Imprinted Nanoparticle Receptors in Water

Duan

Zhao

2018

Bioconjugate Chem.

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Folate receptors are overexpressed on cancer cells and frequently used for targeted delivery. Creation of synthetic receptors to bind folic acid and its analogues in water, however, is challenging because of its complex hydrogen-bonding patterns and competition for hydrogen bonds from the solvent. Micellar imprinting within cross-linkable surfactants circumvented these problems because the nonpolar micellar environment strengthened the hydrogen bonds between the amide group in the surfactant and the template molecule. Incorporation of polymerizable thiouronium functional monomers further enhanced the binding through hydrogen-bond-reinforced ion pairs with the glutamate moiety of the template. The resulting imprinted micelles were able to bind folate and their analogues with submicromolar affinity and distinguish small changes in the hydrogen-bonding patterns as well as the number/position of carboxylic acids. The binding constant obtained was 2-3 orders of magnitude higher than those reported for small-molecule synthetic receptors. Our binding study also revealed interesting details in the binding. For example, the relative contributions of different segments of the molecule to the binding followed the order of carboxylates > pyrimidine ring > pyrazine ring.

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“…Eosin Y disodium salt (EY) is also employed as acceptor chromophore due to the overlap of its absorption with DPA emission. 29 As shown in Figure 3, DPA emits a fluorescence band between 400 and 500 nm with an excitation light at 375 nm. In addition, EY presents an emission band centered at 550 nm with an excitation wavelength at 490 nm.…”

Section: Resultsmentioning

confidence: 98%

Micelle-Induced Self-Assembling Protein Nanowires: Versatile Supramolecular Scaffolds for Designing the Light-Harvesting System

et al. 2015

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Organic nanoparticle induced self-assembly of proteins with periodic nanostructures is a promising and burgeoning strategy to develop functional biomimetic nanomaterials. Cricoid proteins afford monodispersed and well-defined hollow centers, and can be used to multivalently interact with geometrically symmetric nanoparticles to form one-dimensional protein nanoarrays. Herein, we report that core-cross-linked micelles can direct cricoid stable protein one (SP1) to self-assembling nanowires through multiple electrostatic interactions. One micelle can act as an organic nanoparticle to interact with two central concaves of SP1 in an opposite orientation to form a sandwich structure, further controlling the assembly direction to supramolecular protein nanowires. The reported versatile supramolecular scaffolds can be optionally manipulated to develop multifunctional integrated or synergistic biomimetic nanomaterials. Artificial light-harvesting nanowires are further developed to mimic the energy transfer process of photosynthetic bacteria for their structural similarity, by means of labeling donor and acceptor chromophores to SP1 rings and spherical micelles, respectively. The absorbing energy can be transferred within the adjacent donors around the ring and shuttling the collected energy to the nearby acceptor chromophore. The artificial light-harvesting nanowires are designed by mimicking the structural characteristic of natural LH-2 complex, which are meaningful in exploring the photosynthesis process in vitro.

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Artificial Light‐Harvesting System Based on Multifunctional Surface‐Cross‐Linked Micelles

Cited by 44 publications

References 53 publications

Giant light-harvesting nanoantenna for single-molecule detection in ambient light

Giant light-harvesting nanoantenna for single-molecule detection in ambient light

Selective Binding of Folic Acid and Derivatives by Imprinted Nanoparticle Receptors in Water

Micelle-Induced Self-Assembling Protein Nanowires: Versatile Supramolecular Scaffolds for Designing the Light-Harvesting System

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