Squeezing Fluorescent Dyes into Nanoscale Containers—The Supramolecular Approach to Radiative Decay Engineering

Nau, Werner M.; Hennig, Andréas; Koner, Apurba Lal

doi:10.1007/4243_2007_007

Cited by 24 publications

(19 citation statements)

References 103 publications

(189 reference statements)

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“…Radiative lifetime fluctuation arising from modulation of the refractive index and hyperpolarizability of the environment of the dye due to nanoconfinement could account for this observation and act as a second fluorescence contrast mechanism. 72 The very slow decay of the fluorescence polarization anisotropy of agonist-bound β 2 AR-TMR due to quasi-absence of TMR wobbling motion is consistent with nanoconfinement of the probe. This mechanism would also support the changes in radiative lifetime witnessed both in ensemble (Table 1) and in single-molecule (Figure 3) measurements, as neither changes in the orientation of the dipole moment of the probe nor spectral shifts can account for this observation in the solution phase.…”

Section: Discussionmentioning

confidence: 57%

Conformational Dynamics of Single G Protein-Coupled Receptors in Solution

et al. 2011

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G Protein-Coupled Receptors (GPCRs) comprise a large family of seven-helix transmembrane proteins which regulate cellular signaling by sensing light, ligands, and binding proteins. The GPCR activation process, however, is not a simple on-off switch; current models suggest a complex conformational landscape in which the active, signaling state includes multiple conformations with similar downstream activity. The present study probes the conformational dynamics of single β2-Adrenergic Receptors (β2ARs) in the solution phase by Anti-Brownian ELectrokinetic (ABEL) trapping. The ABEL trap uses fast electrokinetic feedback in a microfluidic configuration to allow direct observation of a single fluorescently-labeled β2AR for hundreds of milliseconds to seconds. By choosing a reporter dye and labeling site sensitive to ligand binding, we observe a diversity of discrete fluorescence intensity and lifetime levels in single β2ARs, indicating a varying radiative lifetime and a range of discrete conformational states with dwell times of hundreds of milliseconds. We find that binding of agonist increases the dwell times of these states, and furthermore, we observe millisecond fluctuations within states. The intensity autocorrelations of these faster fluctuations are well-described by stretched exponential functions with stretching exponent β ~ 0.5, suggesting protein dynamics over a range of timescales.

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Section: Discussionmentioning

confidence: 57%

Conformational Dynamics of Single G Protein-Coupled Receptors in Solution

et al. 2011

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“…The selectivity for the sidegroups of amino acids may be applied to recognition of peptides [57]. An inclusion complex of the electron acceptor 2,7-dimethyldiazapyrenium (34) with an equivalent of Q [8] provided effective recognition and detection of electron-donating guests (Scheme 12), particularly catechol (35) solution or on the surface of silica particles [58]. The Q[8]-induced assembly of polymers with viologen and naphthol terminal groups should be useful for predictable polymerization with applicable functionalization in electrochemistry and optics-mediated supramolecular strategy [59,60].…”

Section: Cucurbit[8]uril-induced Chemical Controlmentioning

confidence: 99%

“…The Q[7]-encapsulated alkyl diamino species with terminal ferrocene (11 and 12, Scheme 5) responded to electrochemical redox, and the guest species of alkylviologen substituted by carboxylic acid end group 13 displayed a change of UV-vis absorbance with change of pH in aqueous solution when the axles were joined by Q [6] and Q [7]. The simple inclusion complexes of 2,3-diazabicyclo[2.2.2]oct-2-ene [34] or protonated 2-aminoanthracene [35] with Q[7] exhibited analogous acidity-driven switch behaviour in fluorescent emission. It is likely that unique properties of the pseudorotaxanes with electrochemical or optical detection will lead to further investigation of the design and synthesis of novel functionalized supramolecular architectures involving cucurbiturils.…”

Section: Cucurbit[7]uril-induced Chemical Controlmentioning

confidence: 99%

Host-induced Chemical Control: Supramolecular Catalysis Based on the Host – Guest Interaction of Cucurbit[n]urils

Cong¹,

Tao

Xue³

et al. 2011

COC

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The controllable functional encapsulation of cucurbit[n]urils (Q[n]s) to form supramolecular catalysts is reviewed. The relationship of the supramolecular catalytic activity with the structure of included guests and cucurbit[n]urils is documented and discussed. The controllable functional encapsulation is attributed to overall interactions of hydrophobic, ion-dipole and size effects of the cucurbit[n]urils. The accelerated and stereochemical aspects of chemical reactions result from overcoming the hindrance of decreased entropy, the hydrophobic effect and the encapsulation model induced by hosts. The stability of drugs and chemical intermediates of the inclusion complexes depends on the environment within the hydrophobic cavity; the enhanced charge-transfer process of the included electron donor and acceptor guests depends on the compressed distance between guests, the electron donors, and acceptors within the limited space.

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“…The inclusion of the guest molecules into CB [8] is driven by the release of the pre-encapsulated high-energy water from the cavity (17). The encapsulation of dye molecules as guests inside the CB[n ] cavities exhibits well-known and often tuneable photophysical properties (18)(19)(20)(21)(22). Kaifer and co-workers have shown that CB [8] can form stable inclusion complexes with 2,7-dimethyldiazapyrenium with enhanced fluorescence when compared to the non-encapsulated dye (23).…”

Section: Introductionmentioning

confidence: 99%

A selective supramolecular photochemical sensor for dopamine

Kasera

Walsh

Barrio

et al. 2014

Supramolecular Chemistry

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Dopamine (DA) is an important biomarker for diseases and biological disorders. Existing techniques for DA detection suffer from drawbacks including low sensitivity and selectivity as well as interfering signals from non-target molecules. A simple and selective photochemical sensor for the determination of DA in a supramolecular manner is presented. This approach utilises the complexation properties of a highly fluorescent water-soluble complex of perylene bis(diimide) dye with the macrocyclic host cucurbit[8]uril. The method can be used for the determination of DA in aqueous media, with detection limits below 2 £ 10 25 M, even in the presence of known interferents including ascorbic acid and the catecholamines epinephrine and norepinepherine.

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Squeezing Fluorescent Dyes into Nanoscale Containers—The Supramolecular Approach to Radiative Decay Engineering

Cited by 24 publications

References 103 publications

Conformational Dynamics of Single G Protein-Coupled Receptors in Solution

Conformational Dynamics of Single G Protein-Coupled Receptors in Solution

Host-induced Chemical Control: Supramolecular Catalysis Based on the Host – Guest Interaction of Cucurbit[n]urils

A selective supramolecular photochemical sensor for dopamine

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