Dynamic supramolecular assemblies, driven by noncovalent interactions, pervade the biological realm. In synthetic domain, their counterparts, polymers, endowed with remarkable self-repair and adaptive traits, are often realized through bioinspired designs. Recently, controlled polymerization strategies have emerged, drawing inspiration from protein self-assembly. A burgeoning area of research involves mimicking liquid–liquid phase separation (LLPS) observed in proteins to create coacervate...

Study of the emission behavior all-inorganic perovskite nanocrystals CsPbBr3 and CsPbBr2I as a function excitation power employing fluorescence correlation spectroscopy conventional techniques reveals blinking in microsecond time scale photoinduced enhancement. The observation provides insight into radiative nonradiative deactivation pathways these promising substances. Because both photoactivation processes are intimately linked to charge separation efficiency dynamics nanocrystals, key...

The microscopic structure and dynamics of the room temperature ionic liquids (RTILs) that are responsible for some peculiar properties this class solvents continue to intrigue researchers stimulate new investigations. Herein, we use fluorescence correlation spectroscopy (FCS) technique study diffusion probe molecules in RTILs, results which, when combined with those obtained from lifetime studies, provide insights into structural details novel solvents. Experiments performed three charged...

Single-molecule Förster resonance energy transfer (smFRET) is widely used to monitor conformations and interaction dynamics at the molecular level. However, conventional smFRET measurements are ineffective donor–acceptor distances exceeding 10 nm, impeding studies on biomolecules of larger size. Here, we show that zero-mode waveguide (ZMW) apertures can be overcome nm barrier in smFRET. Using an optimized ZMW structure, demonstrate between standard commercial fluorophores up 13.6 distance...

Single molecule detection provides detailed information about molecular structures and functions but it generally requires the presence of a fluorescent marker which can interfere with activity target or complicate sample production. Detecting single protein its natural UV autofluorescence is an attractive approach to avoid all issues related fluorescence labeling. However, signal from extremely weak. Here, we use aluminum plasmonics enhance tryptophan emission proteins in range. Zero-mode...

Abstract Determining the structure of a protein and its transformation under different conditions is key to understanding activity. The structural stability activity proteins in aqueous–organic solvent mixtures, which an intriguing topic research biochemistry, dependent on nature properties medium. Herein, effect commonly used cosolvent, dimethyl sulfoxide (DMSO), conformational dynamics bovine serum albumin (BSA) studied by fluorescence correlation spectroscopy (FCS) measurements...

Self‐sorting of cellular components is essential for maintaining order and function in living systems, enabling complex processes to operate seamlessly. Emulating such self‐sorting synthetic self‐assembly, however, has conventionally relied on structural or chirality mismatches monomers yielding self‐sorted systems under thermodynamic conditions. In contrast, reaction‐coupled, kinetically‐controlled ubiquitous biological critical achieving spatiotemporal characteristics. Extending this...

Self‐sorting of cellular components is essential for maintaining order and function in living systems, enabling complex processes to operate seamlessly. Emulating such self‐sorting synthetic self‐assembly, however, has conventionally relied on structural or chirality mismatches monomers yielding self‐sorted systems under thermodynamic conditions. In contrast, reaction‐coupled, kinetically‐controlled ubiquitous biological critical achieving spatiotemporal characteristics. Extending this...

Abstract G-quadruplexes (GQs), a non-canonical form of DNA, are receiving huge interest as target sites for potential applications in antiviral and anticancer drug treatments. The biological functions GQs can be controlled by specifically binding proteins known proteins. Some the contain an arginine glycine-rich sequence RGG peptide. Despite important role RGG, GQs-RGG interaction remains poorly understood. By single molecule measurements, dynamics determined principle. However, RGG–GQs...

Supramolecular materials due to their ordered arrangement, and efficient charge transport, exhibit great potential in optoelectronic applications. Nonetheless, precise structural control over the length dispersity of supramolecular polymers is crucial for optimizing properties performance. Although recent advancements living polymerization (LSP) offer strategies this control, research so far has primarily focused on aspects, overlooking exploration functional implications. Moreover, studies...

We investigated the volumetric and kinetic profile of conformational landscape a poly dA loop DNA hairpin (Hp) in presence salts, osmolytes crowding media, mimicking intracellular milieu, using single-molecule FRET methodology. Pressure modulation was applied to explore hydrational characteristics free-energy Hp, but also because pressure is stress factor many organisms have cope with, e.g. deep sea where pressures even up kbar level are encountered. Urea synergistically destabilize closed...

Osmolyte mixtures from deep sea organisms are able to rescue nucleic acids pressure-induced unfolding.

Abstract Organisms are thriving in the deep sea at pressures up to 1 kbar level, which imposes severe stress on conformational dynamics and stability of their biomolecules. The impact osmolytes macromolecular crowders, mimicking intracellular conditions, effect pressure a human telomeric G‐quadruplex (G4) DNA is explored this study employing single‐molecule Förster resonance energy transfer (FRET) experiments. In neat buffer, pressurization favors parallel/hybrid state G4‐DNA over...

The understanding of the transport drugs and naturally occurring molecules in living cells tissues requires a thorough knowledge diffusion behaviour molecular systems these media. In this work, we studied translational three fluorescent molecules, electrically neutral coumarin 102 (C102), cationic rhodamine 6G (R6G) anionic fluorescein (FL) phosphate-buffered (pH 7) aqueous solutions bovine serum albumin (BSA) protein absence presence common salt urea using fluorescence correlation...

Abstract Fluorescence quenching of CdS quantum dots (QDs) by 4‐azetidinyl‐7‐nitrobenz‐2‐oxa‐1,3‐diazole (NBD), where the two partners satisfy spectral overlap criterion necessary for Förster resonance energy transfer (FRET), is studied steady‐state and time‐resolved fluorescence techniques. The QDs accompanied an enhancement acceptor a reduction average lifetime donor. Even though these observations are suggestive dynamic process, it shown that actually proceeds through static interaction...

Abstract The structural dynamics of a DNA hairpin (Hp) are studied in the absence and presence two natural osmolytes trimethylamine‐N‐oxide (TMAO) urea at ambient extreme environmental conditions, including high pressures temperatures, by using single‐molecule Förster resonance energy transfer fluorescence correlation spectroscopy. effect pressure on conformational Hp is investigated level, providing novel mechanistic insights into its conversions. Different from canonical duplex structures...

Abstract Zero mode waveguide (ZMW) nanoapertures efficiently confine the light down to nanometer scale and overcome diffraction limit in single molecule fluorescence analysis. However, unwanted adhesion of fluorescent molecules on ZMW surface can severely hamper experiments. Therefore a proper passivation is required for ZMWs, but information currently lacking both nature phenomenon optimization different protocols. Here we monitor influence dye (Alexa Fluor 546 647, Atto 550 647N)...

The influence of ligand and solvent on light-induced modulation the emission behavior quantum dots (QDs) has been studied for CdTe QDs capped with hexadecylamine (HDA), mercaptopropionic acid (MPA), 1-(1-undecanethiol)-3-methyl imidazolium bromide (SMIM) in CHCl3, H2O, [bmim][PF6] ionic liquid, respectively, using steady state time-resolved fluorescence correlation spectroscopy techniques. While an aqueous solution CdTe/MPA exhibits enhancement a small blue shift peak (λmaxem) early stages...

Aluminum can sustain plasmonic resonances down into the ultraviolet (UV) range to promote surface-enhanced spectroscopy and catalysis. Despite its natural alumina passivating layer, we find here that under 266 nm pulsed UV illumination, aluminum undergo a dramatic photocorrosion in water within few tens of seconds even at low average powers. This instability environments is critical limitation. We show related nonlinear absorption by leading production hydroxyl radicals. Different corrosion...

Nanoapertures milled in metallic films called zero-mode waveguides (ZMWs) overcome the limitations of classical confocal microscopes by enabling single molecule analysis at micromolar concentrations with improved fluorescence brightness. While ZMWs have found many applications studies, their shape has been mainly limited to be circular. Owing large parameter space explore and lack guidelines, earlier attempts using more elaborate shapes led unclear conclusions whether or not performance was...

Light-induced modulation of the fluorescence behavior mercaptopropionic acid (MPA) capped CdTe quantum dots (QDs) in aqueous solution is studied by a combination correlation spectroscopy (FCS) and steady-state time-resolved techniques. These investigations reveal dramatic variation properties QDs under exposure to light. In FCS measurement, large decrease amplitude change shape curves are observed with increasing excitation power. The curves, particularly at short lag time, e.g., faster...

Using pressure perturbation, conformational substates of CaM could be uncovered that conceivably facilitate target recognition by exposing the required binding surfaces.