The formation of a protein corona, where proteins spontaneously adhere to the surface nanomaterials in biological environments, leads changes their physicochemical properties and subsequently affects intended biomedical functionalities. Most current methods study corona are ensemble-averaging either require fluorescent labeling, washing steps, or only applicable specific types particles. Here we introduce real-time all-optical nanoparticle analysis by scattering microscopy (RONAS) track full...

Single-molecule fluorescence has revealed a wealth of biochemical processes but does not give access to submillisecond dynamics involved in transient interactions and molecular dynamics. Here we overcome this bottleneck demonstrate record-high photon count rates >10

The exchange of Ca2+ ions in hydroxyapatite (HAp) with Zn2+ into Zn-HAp is interest for applications ranging from bone tissue engineering to the use as a precursor subsequent ion-exchange reactions. Previous studies, using direct synthesis, showed that ~ 20 mol% can be incorporated HAp, before byproducts are observed. However, this realized at cost loss crystallinity and control over crystal size shape increasing amounts ion incorporation. In work simple post-synthetic strategy formation has...

Abstract Biofunctionalized nanoparticles are increasingly used in biomedical applications including sensing, targeted delivery, and hyperthermia. However, laser excitation associated heating of the nanomaterials may alter structure interactions conjugated biomolecules. Currently no method exists that directly monitors local temperature near material's interface where biomolecules are. Here, a nanothermometer is reported based on DNA‐mediated points accumulation for imaging nanoscale...

Structural characterization of gas-phase [M,C,2H]+ (M = Ta, Ir, Pt), formed by reacting laser ablation M+ with ethylene oxide (c-C2H4O) or methane under multiple collision conditions, is achieved using infrared multiple-photon dissociation (IR-MPD) spectroscopy the intracavity free-electron FELICE. After product formation, part distribution complexed Ar, allowing for simultaneous recording IR-MPD spectra both bare [M,C,2H]+, which dissociates via dehydrogenation, and [M,C,2H]+∙Ar, loses Ar....

Multivalency as an interaction principle is widely utilized in nature. It enables specific and strong binding by multiple weak interactions through enhanced avidity a core process immune recognition cellular signaling, which also current concept drug design. Here, we use the high signals from plasmon-enhanced fluorescence of nanoparticles to extract kinetics dynamics multivalent on single-molecule level real time. We study mono-, bi-, trivalent using DNA Holliday Junction model construct...

Abstract Multivalency as an interaction principle is widely utilized in nature. It enables specific and strong binding by multiple weak interactions through enhanced avidity a core process immune recognition cellular signaling current concept drug design. Rapid unbinding of monovalent constituent during multivalent creates dynamics that require single-molecule approach to be studied. Here, we use the high signals from plasmon fluorescence nanoparticles extract kinetics on level real-time. We...

IR multiple-photon dissociation (IRMPD) action spectroscopy is combined with quantum chemical calculations to examine the [M,C,2H]

Significant advances in synthesis and functionalization have provided state-of-the-art technology controlling the physico-chemical properties of nanomaterials. These are finding numerous applications including biomedical field whereby nanoparticles injected vivo for medical imaging, theranostics biosensing. However, interactions with proteins contained biological fluids lead to formation a shell on surface called "protein corona" (PC). PC plays detrimental role intended as it may modify...

Biomolecules exhibit dynamics on widely varying timescales, which are critical to their functioning in living systems. Particularly sub-millisecond dynamics, such as low-affinity ligand binding and interactions of individual sites within multivalent complexes, remain elusive. These typically probed real-time using single-molecule fluorescence, but photophysics limits it millisecond timescales. Here, we exploit optimize the strong plasmonic fluorescence enhancement provided by monocrystalline...

We have established a label-free plasmonic platform that monitors proteolytic activity in real-time. The sensor consists of random array gold nanorods are functionalized with design peptide is specifically cleaved by thrombin resulting blue-shift the longitudinal plasmon. By monitoring plasmon many individual we determined thrombin’s real-time and inferred relevant kinetic parameters. Furthermore, comparison to model revealed shift dictated competition between cleavage binding, which...

Significant advances in synthesis and functionalization have provided state-of-the-art technology controlling the physico-chemical properties of nanomaterials. These are finding numerous applications including biomedical field whereby nanoparticles injected vivo for medical imaging, theranostics biosensing. However, interactions with proteins contained biological fluids lead to formation a shell on surface called "protein corona" (PC). PC plays detrimental role intended as it may modify...

We have established a label-free plasmonic platform that monitors proteolytic activity in real time. The sensor consists of random array gold nanorods are functionalized with design peptide is specifically cleaved by thrombin, resulting blueshift the longitudinal plasmon. By monitoring plasmon many individual nanorods, we determined thrombin's time and inferred relevant kinetic parameters. Furthermore, comparison to model revealed shift dictated competition between cleavage thrombin binding,...