Atomic Force Microscopy Measurements Research Articles

Localized compaction of collagen hydrogels using acoustic droplet vaporization promotes osteogenic differentiation of mesenchymal stem cells

The lineage specification of mesenchymal stem cells (MSCs) is dependent on matrix stiffness, with osteogenesis promoted on or within stiff microenvironments. Unlike native extracellular matrix, conventional hydrogels have relatively static and uniform mechanical properties, thereby limiting the study of how spatiotemporally controlled mechanical cues impact MSC behavior. Here, we spatiotemporally control MSC differentiation in 3D hydrogels by actively modulating matrix stiffness using acoustic droplet vaporization (ADV). An acoustically responsive scaffold (ARS) was generated by co-encapsulating MSCs and perfluorohexane-based emulsion (13 μm) within type I collagen. ADV was used to generate bubbles within the ARS. Bubble diameter and the width of the compacted matrix region increased over time following ADV. Atomic force microscopy measurements demonstrated that the hydrogel region proximal to the bubble was significantly stiffer than the distal regions. Significantly greater levels of Runx2 and osteocalcin expression were observed in MSCs proximal to bubbles compared to distal on days 7 and 14. Higher alkaline phosphatase activity also validated the above findings. The significant upregulation of these osteogenic biomarkers suggests ADV-induced, mechanical changes in ARSs were sufficient to enhance osteogenic differentiation of MSCs. This approach is a significant step towards controlling the 3D differentiation of MSCs in a spatially localized, non-invasive, and on-demand manner.

Topological Structure Realized in Cove-Edged Graphene Nanoribbons via Incorporation of Periodic Pentagon Rings.

Cove-edged zigzag graphene nanoribbons are predicted to show metallic, topological, or trivial semiconducting band structures, which are precisely determined by their cove offset positions at both edges as well as the ribbon width. However, due to the challenge of introducing coves into zigzag-edged graphene nanoribbons, only a few cove-edged graphene nanoribbons with trivial semiconducting bandgaps have been realized experimentally. Here, we report that the topological band structure can be realized in cove-edged graphene nanoribbons by embedding periodic pentagon rings on the cove edges through on-surface synthesis. Upon noncontact atomic force microscopy and scanning tunneling spectroscopy measurements, the chemical and electronic structures of cove-edged graphene nanoribbons with periodic pentagon rings have been characterized for different lengths. Combined with theoretical calculations, we find that upon inducing periodic pentagon rings the cove-edged graphene nanoribbons exhibit nontrivial topological structures. Our results provide insights for the design and understanding of the topological character in cove-edged graphene nanoribbons.

Avalanches and Extreme Value Statistics of a Mesoscale Moving Contact Line.

We report direct atomic force microscopy measurements of pinning-depinning dynamics of a circular moving contact line (CL) over the rough surface of a micron-sized vertical hanging glass fiber, which intersects a liquid-air interface. The measured capillary force acting on the CL exhibits sawtoothlike fluctuations, with a linear accumulation of force of slope k (stick) followed by a sharp release of force δf, which is proportional to the CL slip length. From a thorough analysis of a large volume of the stick-slip events, we find that the local maximal force F_{c} needed for CL depinning follows the extreme value statistics and the measured δf follows the avalanche dynamics with a power law distribution in good agreement with the Alessandro-Beatrice-Bertotti-Montorsi (ABBM) model. The experiment provides an accurate statistical description of the CL dynamics at mesoscale, which has important implications to a common class of problems involving stick-slip motion in a random defect or roughness landscape.

Atomic Defect Quantification by Lateral Force Microscopy.

Atomic defects in two-dimensional (2D) materials impact electronic and optoelectronic properties, such as doping and single photon emission. An understanding of defect-property relationships is essential for optimizing material performance. However, progress in understanding these critical relationships is hindered by a lack of straightforward approaches for accurate, precise, and reliable defect quantification on the nanoscale, especially for insulating materials. Here, we demonstrate that lateral force microscopy (LFM), a mechanical technique, can observe atomic defects in semiconducting and insulating 2D materials under ambient conditions. We first improve the sensitivity of LFM through consideration of cantilever mechanics. With the improved sensitivity, we use LFM to locate atomic-scale point defects on the surface of bulk MoSe2. By directly comparing LFM and conductive atomic force microscopy (CAFM) measurements on bulk MoSe2, we demonstrate that point defects observed with LFM are atomic defects in the crystal. As a mechanical technique, LFM does not require a conductive pathway, which allows defect characterization on insulating materials, such as hexagonal boron nitride (hBN). We demonstrate the ability to observe intrinsic defects in hBN and defects introduced by annealing. Our demonstration of LFM as a mechanical defect characterization technique applicable to both conductive and insulating 2D materials will enable routine defect-property determination and accelerate materials research.

Sulfate Doping Promotes Agglomeration of Calcium Fluoride Crystals.

Calcium salt precipitation is an effective solution to wastewater fluoride pollution. The purity and precipitation efficiency of calcium fluoride is critical for its removal and recovery. This study aimed to reveal the role of coexisting sulfates in the precipitation of calcium fluoride. A low sulfate concentration promoted calcium fluoride precipitation. The size of calcium fluoride-aggregated particle clusters increased from 750 to 2000 nm when the molar ratio of sulfate to fluoride was increased from 0 to 3:100. Sulfate doped in the calcium fluoride crystals neutralized the positive charge of the calcium fluoride. Online atomic force microscopy measurements showed that sulfate reduced the repulsive force between calcium fluoride crystals and increased the adhesion force from 1.62 to 2.46 nN, promoting the agglomeration of calcium fluoride crystals. Sulfate improved the precipitation efficiency of calcium fluoride by promoting agglomeration; however, the purity of calcium fluoride was reduced by doping. Sulfate reduced the induction time of calcium fluoride crystallization and improved the nucleation rate of calcium fluoride. Sulfate should be retained to improve the precipitation of calcium fluoride and to avoid its loss from the effluents. However, it is necessary to separate sulfate from fluoride to obtain high-purity calcium fluoride. Therefore, sulfate concentration regulation in high-fluoride wastewater is key to achieving the efficient removal and recovery of fluoride ions.

Gutless Helper-Dependent and First-Generation HAdV5 Vectors Have Similar Mechanical Properties and Common Transduction Mechanisms.

Delivering vectorized information into cells with the help of viruses has been of high interest to fundamental and applied science, and bears significant therapeutic promise. Human adenoviruses (HAdVs) have been at the forefront of gene delivery for many years, and the subject of intensive development resulting in several generations of agents, including replication-competent, -defective or retargeted vectors, and recently also helper-dependent (HD), so-called gutless vectors lacking any viral protein coding information. While it is possible to produce HD-AdVs in significant amounts, physical properties of these virus-like particles and their efficiency of transduction have not been addressed. Here, we used single-cell and single virus particle assays to probe the effect of genome length on HAdV-C5 vector transduction. Our results demonstrate that first-generation C5 vectors lacking the E1/E3 regions of the viral genome as well as HD-AdV-C5 particles with a wild type (wt) ∼36 kbp or an undersized double-strand DNA genome are similar to human adenovirus C5 (HAdV-C5) wt regarding attachment to human lung epithelial cells, endocytic uptake, endosome penetration and dependency on the E3 RING ubiquitin ligase Mind Bomb 1 for DNA uncoating at the nuclear pore complex. Atomic force microscopy measurements of single virus particles indicated that small changes in the genome length from 94% to 103% of HAdV-C5 have no major impact on physical and mechanical features of AdV vectors. In contrast, an HD-AdV-C5 with ∼30 kbp genome was slightly stiffer and less heat-resistant than the other particles, despite comparable entry and transduction efficiencies in tissue culture cell lines, including murine alveolar macrophage-like Max-Planck-Institute (MPI)-2 cells. Together, our in vitro studies reinforce the use of HD-AdV vectors for effective single round gene delivery. The results illustrate how physical properties and cell entry behavior of single virus particles can provide functional information for anticipated therapeutic vector applications.

Wavelet-based information theory in quantitative assessment of AFM images’ quality

The quantitative assessment of the image quality produced by atomic force microscopy (AFM) is an ongoing and challenging task. In our study, we demonstrate Shannon’s application of information theory for measuring image quality. Specifically, we propose quantifying the loss of image information due to the various distortion processes by exploring the relationship between image information based on the information channel capacity (ICC), spectral image representation, and visual quality. Since the ideal image is unavailable, the power and noise spectrum, the critical input information for the image quality evaluation, must be robustly estimated in the proposed method. The classical, most popular Welch method for spectral estimation uses an average of several windowed periodograms and can produce biased spectrum estimates. Therefore, in our work, we discuss an alternative technique based on the wavelet transform that can be applied to solve this challenging problem, specifically in the case of noisy, uncertain AFM measurements. Finally, we validate the performance of the enhanced ICC-wavelet-based algorithm with noisy measurement AFM data.

Boosted carbon electrocatalytic effect towards sensing and green energy applications by tailoring the catalyst-support interface on a nature-inspired solution

Carbon electrodes are widely accepted as very versatile platforms, with applications ranging from electrocatalysis to sensors and other devices, like fuel cells and water electrolyzers. However, there are still difficulties given that over time, at high potentials, the oxidation of carbon materials (as a catalyst and/or catalyst support) can play a detrimental role, undermining the efficiency and stability of the electrochemical processes and devices performance. In this paper, it is reported the research work followed by resourcing to electrochemical analytical techniques, like cyclic voltammetry (CV) and electrochemical impedance spectroscopy (EIS), along with complementary atomic force microscopy (AFM) and water contact angle (WCA) measurements. These techniques were used to characterise glass-type and paper-based carbon electrodes. On a nature-inspired solution, we took advantage of the different interfacial carbon-support hierarchical porous structures to boost the carbon electrocatalytic effect towards sensing the ferri/ferrocyanide redox couple ([Fe(CN)6]3-/4−) in aqueous solution. It is shown that the best results were achieved with carbon paper electrodes without wet proofing, given its hierarchical porous structure and absence of the insulating binder. This research endeavors to contribute to the ongoing advancements in the field of electrochemical green energy conversion by exploring innovative approaches and materials, with the ultimate aim of developing carbon substrates that not only enhance performance but also promote environmental sustainability.

The Effect of Deposition Temperature on Structural, Morphological, and Dielectric Properties of Yttria-Doped Zirconia Thin Films

The aim of this study was to investigate the effect of deposition temperature on the structural, optical, morphological, and dielectric properties of yttria-stabilised zirconia (YSZ) films prepared by sol-gel spin-coating method. X-ray diffraction (XRD) measurements of YSZ films showed that the peaks of the cubic phase were prominent and the peak intensities increased with deposition temperature. The crystallite size, dislocation density, and microstrain of the thin films were identified by XRD. It was observed that the crystal size of the YSZ thin films increased from 16 nm to 22 nm with the deposition temperature. The surface roughness of the thin films was found to have changed as revealed by Atomic Force Microscopy (AFM) measurements. The roughness increased from 7.72 nm to 11.92 nm with increasing temperature. The optical transmittance of the YSZ thin films was investigated in the wavelength range 200-900 nm and was found to increase slightly with increasing deposition temperature. Metal-Oxide-Semiconductor (MOS) devices were fabricated from these YSZ materials for dielectric characterization. The dielectric properties of the Ag/YSZ/n-Si MOS structure were investigated. It was found that the capacitance, conductivity and other dielectric parameters of these structures are strongly frequency dependent.

High pressure induced formation of carbon nanorods from tetracosane

Morphology control of carbon structures is essential for improving their performance in many applications. Direct pyrolysis of organic precursors, however, usually yields bulk amorphous carbon. Therefore, traditional methods for controlling the morphology of carbon structures involve multistep processes and complex precursor molecules. While various methods have been developed under ambient pressure, the impact of pressure on the morphology of the resulting carbon structures remains unexplored. Herein, we present the synthesis of carbon nanorods by direct pyrolysis of the low-cost aliphatic hydrocarbon tetracosane under high pressure conditions. The diameters of the carbon nanorods are adjusted by simply varying the synthetic pressures. High pressure allows controlling both the nanorod morphology as well as the degree of order, and local conductivity of the thus prepared nanorods has been confirmed by conductive atomic force microscopy measurements. Our method promises a convenient strategy to synthesize carbon structures with controlled morphology and high ordered chemical structure, which opens opportunities for potential electronic and electrochemical applications.

External electric field and UV-ozone treated Ti3C2T x -MXene nanosheets and their hole injection tailoring in UV organic light-emitting diodes

Solution-processed 2D nanosheets of Ti3C2T x -MXene have been facilely synthesized with ultrasonic-assisted liquid phase exfoliation. X-ray diffraction, scanning electron microscope, transmission electron microscope, atomic force microscopy and x-ray photoelectron spectroscopy measurements confirm that the Ti3C2T x -MXene nanosheets have been successfully synthesized, showing good film morphology and exceptional electronic properties. The comprehensive properties of Ti3C2T x -MXene nanosheets are systematically optimized by combination with appropriate sizes of Ti3C2T x -MXene nanosheets, external electric field and ultraviolet (UV)-ozone treatment. With Ti3C2T x -MXene nanosheets as hole injection layer and PBD as emissive molecule, UV organic light-emitting diodes (OLEDs) have been configurated and shown superior performance with maximum radiance of 1.47 mW cm−2, maximum external quantum efficiency of 1.084% and electroluminescent peak around 400 nm. The effects of external electric field and UV-ozone treatment on hole injection ability of Ti3C2T x -MXene nanosheets are investigated in details and further analyzed with impedance spectroscopy. Our experiments pave an alternative approach for advancing Ti3C2T x -MXene nanosheets and UV OLEDs.

Structure Discovery in Atomic Force Microscopy Imaging of Ice.

The interaction of water with surfaces is crucially important in a wide range of natural and technological settings. In particular, at low temperatures, unveiling the atomistic structure of adsorbed water clusters would provide valuable data for understanding the ice nucleation process. Using high-resolution atomic force microscopy (AFM) and scanning tunneling microscopy, several studies have demonstrated the presence of water pentamers, hexamers, and heptamers (and of their combinations) on a variety of metallic surfaces, as well as the initial stages of 2D ice growth on an insulating surface. However, in all of these cases, the observed structures were completely flat, providing a relatively straightforward path to interpretation. Here, we present high-resolution AFM measurements of several water clusters on Au(111) and Cu(111), whose understanding presents significant challenges due to both their highly 3D configuration and their large size. For each of them, we use a combination of machine learning, atomistic modeling with neural network potentials, and statistical sampling to propose an underlying atomic structure, finally comparing its AFM simulated images to the experimental ones. These results provide insights into the early phases of ice formation, which is a ubiquitous phenomenon ranging from biology to astrophysics.

Reconstruction of high-resolution atomic force microscopy measurements from fast-scan data using a Noise2Noise algorithm

The acquisition of large atomic-force-microscopy (AFM) scans at nanoscale resolutions can take hours and produce datasets with millions of pixels, which is time consuming and computationally expensive to analyze. In this paper, we present an approach to speedup this process by using a computer-vision algorithm, namely the Noise2Noise algorithm, to reconstruct high-resolution, low scan speed AFM data from high-speed, noisy, sparsely sampled AFM data. This algorithm is trained on various noise types to reproduce different sources of experimental noises encountered during the acquisition of AFM data. Our results demonstrate that a sparse, uniform AFM scan of 20 × 20 μm at 128 × 128 pixel resolution can be processed within seconds, and the output image is comparable to a higher quality raw AFM data scan which required 30 minutes or more to collect and process manually, reducing not only the acquisition and analysis time, but also the size of the data being collected.

A theoretical model relating intracellular forces to cell mechanics in atomic force microscopy measurements

A theoretical model relating intracellular forces to cell mechanics in atomic force microscopy measurements

Effect of methanol and photoinduced surface oxygen vacancies on the charge carrier dynamics in TiO2

The migration of holes in metal-oxide semiconductors such as TiO2 plays a vital role in (photo)catalytic applications. The dynamics of charge carriers under operation conditions can be influenced by both methanol addition and photoinduced surface oxygen vacancies (PI-SOVs). Nevertheless, the existing knowledge of the effect of methanol as a function of PI-SOVs solely concentrates on the chemical reduction process. For this reason, the fundamental understanding of the time-dependent charge carrier-vacancy interactions in the presence of methanol is impaired. Here, we conducted time-resolved atomic force microscopy measurements to quantitatively disclose the effect of methanol adsorption on the dynamics of hole migration in TiO2. Our results show that time constants associated with the migration of charge carriers significantly change due to methanol adsorption. Moreover, the energy landscape of the hole migration barrier was dominated and lowered by PI-SOVs. Our findings contribute to the physics of charge carrier dynamics by enabling the engineering of charge carrier-vacancy interactions.

Reproducibility of atomic force microscopy measurements on tau protein

Reproducibility of atomic force microscopy measurements on tau protein

Reexamination of Damping in Sliding Friction.

Friction is responsible for about one-third of the primary energy consumption in the world. So far, a thorough atomistic understanding of the frictional energy dissipation mechanisms is still lacking. The Amontons' law states that kinetic friction is independent of the sliding velocity while the Prandtl-Tomlinson model suggests that damping is proportional to the relative sliding velocity between two contacting objects. Through careful analysis of the energy dissipation process in atomic force microscopy measurements, here we propose that damping force is proportional to the tip oscillation speed induced by friction. It is shown that a physically well-founded damping term can better reproduce the multiple peaks in the velocity-dependent friction force observed in both experiments and molecular dynamics simulations. Importantly, the analysis gives a clear physical picture of the dynamics of energy dissipation in different friction phases, which provides insight into long-standing puzzles in sliding friction, such as velocity weakening and spring-stiffness-dependent friction.

Characterization of aTiO2 surfaces functionalized with CAP-p15 peptide.

Functionalization of Titanium implants using adequate organic molecules is a proposed method to accelerate the osteointegration process, which relates to topographical, chemical, mechanical, and physical features. This study aimed to assess thepotential of a peptide derived from cementum attachment protein (CAP-p15) adsorbed onto aTiO2 surfaces to promote the deposition of calcium phosphate (CaP) minerals and its impact on the adhesion and viability of human periodontal ligament cells (hPDLCs). aTiO2 surfaces were synthesized by magnetron sputtering technique. The CAP-p15 peptide was physically attached to aTiO2 surfaces and characterized by atomic force microscopy, fluorescence microscopy, and water contact angle measurement. We performed in vitro calcium phosphate nucleation assays using an artificial saliva solution (pH 7.4) to simulate the oral environment. morphological and chemical characterization of the deposits were evaluated by scanning electronic microscopy (SEM) and spectroscopy molecular techniques (Raman Spectroscopy, ATR-FTIR). The aTiO2 surfaces biofunctionalized with CAP-p15 were also analyzed for hPDLCs attachment, proliferation, and in vitro scratch-healing assay. The results let us see that the homogeneousamorphous titanium oxide coating was 70 nanometers thick. The CAP-p15 (1 μg/mL) displayed the ability to adsorb onto the aTiO2 surface, increasing the roughness and maintaining the hydrophilicity of the aTiO2 surfaces. The physical adsorption of CAP-p15 onto the aTiO2 surfaces promoted the precipitation of a uniform layer of crystals with a flake-like morphology and a Ca/P ratio of 1.79. According to spectroscopy molecular analysis, these crystalline deposits correspond to carbonated hydroxyapatite. Regarding cell behavior, the biofunctionalized aTiO2 surfaces improved the adhesion of hPDLCs after 24 h of cell culture, achieving 3.4-fold when compared to pristine surfaces. Moreover, there was an increase in cell proliferation and cell migration processes. Physical adsorption of CAP-p15 onto aTiO2 surfaces enhanced the formation of carbonate hydroxyapatite crystals and promoted the proliferation and migration of human periodontal ligament-derived cells in in vitro studies. This experimental model using the novel bioactive peptide CAP-p15 could be used as an alternative to increasing the osseointegration process of implants.

Understanding of the flocculating performance in varying salinity solutions of Chi-g-CPAM and CPAM

In this work, the adsorption performance of a novel chitosan-based flocculant (Chi-g-CPAM) and a cationic flocculant (CPAM) onto the kaolinite surface as well as the interaction mechanisms have been investigated by settling tests, atomic force microscopy (AFM) and quartz crystal microbalance with dissipation (QCM-D). When the KCl concentration of the solution altered from 1 mM to 100 mM, the settling rate of kaolinite suspension using CPAM deteriorated from 2.73 m/h to 1.97 m/h. However, the Chi-g-CPAM exhibited salt resistance as the settling rate changed slightly from 2.34 m/h to 2.44 m/h. From the QCM-D results, the Δf of CPAM onto silica sensor changed from − 3.6 Hz to − 33.6 Hz and -ΔD/Δf × 106 increased from 0.167 to 0.223, confirming that the CPAM layer adsorbed on the silica surface was thicker and more dissipative in 100 mM KCl solution. Meanwhile, the Δf of Chi-g-CPAM onto silica sensor changed from − 14.3 Hz to − 33.9 Hz. The conformation of Chi-g-CPAM layer changed slightly as the -ΔD/Δf × 106 increased from 0.174 to 0.186. From the AFM measurements in 1 mM and 100 mM KCl solution, the distance of adhesion forces between the silica probe and CPAM expanded from approximately 20 nm to around 50 nm, and the adhesion force changed from 1.9 nN± 0.1 nN to 21.3 nN± 0.1 nN. The interaction forces with a long range (∼100 nm) maintained at about 3 nN between the silica probe and Chi-g-CPAM. Such difference was mainly attributed to the steric hindrance effect originating from the shorter molecular chain of Chi-g-CPAM. In 100 mM KCl solution, the CPAM molecules with long chains had a more coiled conformation than Chi-g-CPAM, which resulted a train-like flat adsorption conformation and larger adhesion, and formed a loose and thick polymer layer of CPAM in high salinity. The insights into the flocculating performance in varying salinity solutions of CPAM and Chi-g-CPAM will contribute to the molecular design of chitosan-based flocculants for efficient wastewater treatment.

Towards quantification of doping in gallium arsenide nanostructures by low-energy scanning electron microscopy and conductive atomic force microscopy.

We calculate a universal shift in work function of 59.4 meV per decade of dopant concentration change that applies to all doped semiconductors and from this use Monte Carlo simulations to simulate the resulting change in secondary electron yield for doped GaAs. We then compare experimental images of doped GaAs layers from scanning electron microscopy and conductive atomic force microscopy. Kelvin probe force microscopy allows to directly measure and map local work function changes, but values measured are often smaller, typically only around half, of what theory predicts for perfectly clean surfaces.