Modulating the optical response of fluorescent nanoparticles through rational modification of their surface chemistry can yield distinct optical signatures upon the interaction with structurally related molecules. Herein, we present a method for tuning the fluorescence response of single-walled carbon nanotubes (SWCNTs) toward dopamine (DA) and serotonin, two structurally related monoamine-hydroxylated aromatic neurotransmitters, by introducing oxygen defects into (6,5) chirality-enriched SWCNTs suspended by sodium cholate (SC). This modification facilitated opposite optical responses toward these neurotransmitters, where DA distinctly increased the fluorescence of the defect-induced emission of SWCNTs (D-SWCNTs) 6-fold, while serotonin notably decreased it.
View Article and Find Full Text PDFThe presence of multiple pesticide residues in vegetables has become an increasingly critical concern. Immunochromatography has garnered significant interest for its convenience, sensitivity and speed. However, conventional immunochromatography was typically limited to single-target detection, exhibiting restricted efficiency and high costs in on-site large-scale detection scenarios.
View Article and Find Full Text PDFIntegrating single-walled carbon nanotubes (SWCNTs) into supramolecular self-assemblies harnesses the distinctive mechanical, optical, and electronic properties of the nanoparticles alongside the structural and chemical properties of the assemblies. Organic molecules capable of forming supramolecular assemblies through hydrophobic, van der Waals, and π-π interactions have been demonstrated to be particularly effective in dispersing and functionalizing SWCNTs, as these same interactions facilitate the binding to the hydrophobic graphene-like surface of the SWCNTs. This review discusses a variety of self-assembling structures that were shown to integrate SWCNTs, ranging from simple micelles and ring structures to complex DNA origami and three-dimensional hydrogels formed by low-molecular-weight gelators.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2024
Biological processes are characterized by dynamic and elaborate temporal patterns driven by the interplay of genes, proteins, and cellular components that are crucial for adaptation to changing environments. This complexity spans from molecular to organismal scales, necessitating their real-time monitoring and tracking to unravel the active processes that fuel living systems and enable early disease detection, personalized medicine, and drug development. Single-walled carbon nanotubes (SWCNTs), with their unique physicochemical and optical properties, have emerged as promising tools for real-time tracking of such processes.
View Article and Find Full Text PDFJ Chem Theory Comput
October 2024
Inspired by biology and implemented using nanotechnology, the self-assembly of patchy particles has emerged as a pivotal mechanism for constructing complex structures that mimic natural systems with diverse functionalities. Here, we explore the dissipative self-assembly of patchy particles under nonequilibrium conditions, with the aim of overcoming the constraints imposed by equilibrium assembly. Utilizing extensive Monte Carlo (MC) and Molecular Dynamics (MD) simulations, we provide insight into the effects of external forces that mirror natural and chemical processes on the assembly rates and the stability of the resulting assemblies comprising 8, 10, and 13 patchy particles.
View Article and Find Full Text PDFACS Appl Mater Interfaces
October 2024
Insight into the behaviors of molecules in confined space is highly desired for the deep understanding of the mechanism of chemical reactions in a microenvironment. Yet the direct access of molecular evolutions at atomic resolution in nanoconfinements is still challenging. Among various guests, atomically precise clusters with well-defined structures are better suited for monitoring the chemical and physical processes in nanochannels because of their visibility under electron microscopy and identical structures that ensure homogeneous interactions.
View Article and Find Full Text PDFJ Chem Theory Comput
September 2024
Bridging biological complexity and synthetic material design, we investigate dissipative self-assembly in patchy particle systems. Utilizing Monte Carlo and Molecular Dynamics simulations, we demonstrate how external driving forces mitigate equilibrium trade-offs between assembly time and structural stability, traditionally encountered in self-assembly processes. Our findings also extend to biological-mimicking environments, where we explore the dynamics of patchy particles under crowded conditions.
View Article and Find Full Text PDFProtein folding is a critical process that determines the functional state of proteins. Proper folding is essential for proteins to acquire their functional three-dimensional structures and execute their biological role, whereas misfolded proteins can lead to various diseases, including neurodegenerative disorders like Alzheimer's and Parkinson's. Therefore, a deeper understanding of protein folding is vital for understanding disease mechanisms and developing therapeutic strategies.
View Article and Find Full Text PDFJ Colloid Interface Sci
September 2024
Hydrogels derived from fluorenylmethoxycarbonyl (Fmoc)-conjugated amino acids and peptides demonstrate remarkable potential in biomedical applications, including drug delivery, tissue regeneration, and tissue engineering. These hydrogels can be injectable, offering a minimally invasive approach to hydrogel implantation. Given their potential for prolonged application, there is a need for non-destructive evaluation of their properties over extended periods.
View Article and Find Full Text PDFEnzymes serve as pivotal biological catalysts that accelerate essential chemical reactions, thereby influencing a variety of physiological processes. Consequently, the monitoring of enzyme activity and inhibition not only yields crucial insights into health and disease conditions but also forms the basis of research in drug discovery, toxicology, and the understanding of disease mechanisms. In this context, near-infrared (NIR) fluorescent single-walled carbon nanotubes (SWCNTs) have emerged as effective tools for tracking enzyme activity and inhibition through diverse strategies.
View Article and Find Full Text PDFFunctionalized single-walled carbon nanotubes (SWCNTs) hold immense potential for diverse biomedical applications due to their biocompatibility and optical properties, including near-infrared fluorescence. Specifically, SWCNTs have been utilized to target cells as a vehicle for drug delivery and gene therapy, and as sensors for various intracellular biomarkers. While the main internalization route of SWCNTs into cells is endocytosis, methods for enhancing the cellular uptake of SWCNTs are of great importance.
View Article and Find Full Text PDFEnzymes play a pivotal role in regulating numerous bodily functions. Thus, there is a growing need for developing sensors enabling real-time monitoring of enzymatic activity and inhibition. The activity and inhibition of cholinesterase (CHE) enzymes in blood plasma are fluorometrically monitored using near-infrared (NIR) fluorescent single-walled carbon nanotubes (SWCNTs) as probes, strategically functionalized with myristoylcholine (MC)- the substrate of CHE.
View Article and Find Full Text PDFMicroRNAs (miRNAs) are single-stranded non-coding short ribonucleic acid sequences that take part in many cellular and biological processes. Recent studies have shown that altered expression of miRNAs is involved in pathological processes, and they can thus be considered biomarkers for the early detection of various diseases. Here, we demonstrate a selection and elimination process of fluorescent single-walled carbon nanotube (SWCNT) sensors for miRNA biomarkers based on RNA-DNA hybridization with a complementary DNA recognition unit bound to the SWCNT surface.
View Article and Find Full Text PDFMany biological systems rely on the ability to self-assemble target structures from different molecular building blocks using nonequilibrium drives, stemming, for example, from chemical potential gradients. The complex interactions between the different components give rise to a rugged energy landscape with a plethora of local minima on the dynamic pathway to the target assembly. Exploring a toy physical model of multicomponents nonequilibrium self-assembly, we demonstrate that a segmented description of the system dynamics can be used to provide predictions of the first assembly times.
View Article and Find Full Text PDFBlood coagulation is a critical defense mechanism against bleeding that results in the conversion of liquid blood into a solid clot through a complicated cascade, which involves multiple clotting factors. One of the final steps in the coagulation pathway is the conversion of fibrinogen to insoluble fibrin mediated by thrombin. Because coagulation disorders can be life-threatening, the development of novel methods for monitoring the coagulation cascade dynamics is of high importance.
View Article and Find Full Text PDFHydrogels formed via supramolecular self-assembly of fluorenylmethyloxycarbonyl (Fmoc)-conjugated amino acids provide excellent scaffolds for 3D cell culture, tissue engineering, and tissue recovery matrices. Such hydrogels are usually characterized by rheology or electron microscopy, which are invasive and cannot provide real-time information. Here, we incorporate near-infrared fluorescent single-walled carbon nanotubes (SWCNTs) into Fmoc-diphenylalanine hydrogels as fluorescent probes, reporting in real-time on the morphology and time-dependent structural changes of the self-assembled hydrogels in the transparency window of biological tissue.
View Article and Find Full Text PDFCholinesterase enzymes are involved in a wide range of bodily functions, and their disruption is linked to pathologies such as neurodegenerative diseases and cancer. While cholinesterase inhibitors are used as drug treatments for diseases such as Alzheimer and dementia at therapeutic doses, acute exposure to high doses, found in pesticides and nerve agents, can be lethal. Therefore, measuring cholinesterase activity is important for numerous applications ranging from the search for novel treatments for neurodegenerative disorders to the on-site detection of potential health hazards.
View Article and Find Full Text PDFPhys Chem Chem Phys
October 2022
The entropy production rate (EPR) measures time-irreversibility in systems operating far from equilibrium. The challenge in estimating the EPR for a continuous variable system is the finite spatiotemporal resolution and the limited accessibility to all of the nonequilibrium degrees of freedom. Here, we estimate the irreversibility in partially observed systems following oscillatory dynamics governed by coupled overdamped Langevin equations.
View Article and Find Full Text PDFFluorescent nanosensors hold the potential to revolutionize life sciences and medicine. However, their adaptation and translation into the in vivo environment is fundamentally hampered by unfavourable tissue scattering and intrinsic autofluorescence. Here we develop wavelength-induced frequency filtering (WIFF) whereby the fluorescence excitation wavelength is modulated across the absorption peak of a nanosensor, allowing the emission signal to be separated from the autofluorescence background, increasing the desired signal relative to noise, and internally referencing it to protect against artefacts.
View Article and Find Full Text PDFSuper resolution microscopy methods have been designed to overcome the physical barrier of the diffraction limit and push the resolution to nanometric scales. A recently developed super resolution technique, super-resolution radial fluctuations (SRRF) [Nature communications, 7, 12471 (2016)10.1038/ncomms12471], has been shown to super resolve images taken with standard microscope setups without fluorophore localization.
View Article and Find Full Text PDFNonequilibrium self-assembly can be found in various biological processes where chemical potential gradients are exploited to steer the system to a desired organized structure with a particular function. Microtubules, for example, are composed of two globular protein subunits, α-tubulin and β-tubulin, which bind together to form polar dimers that self-assemble a hollow cylinder structure in a process driven by GTPase activity. Inspired by this process, we define a generic self-assembly lattice model containing particles of two subunits, which is driven out-of-equilibrium by a dimer-favoring local driving force.
View Article and Find Full Text PDF( nematodes serve as a model organism for eukaryotes, especially due to their genetic similarity. Although they have many advantages like their small size and transparency, their autofluorescence in the entire visible wavelength range poses a challenge for imaging and tracking fluorescent proteins or dyes using standard fluorescence microscopy. Herein, near-infrared (NIR) fluorescent single-walled carbon nanotubes (SWCNTs) are utilized for imaging within the gastrointestinal track of .
View Article and Find Full Text PDF