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The native extracellular matrix (ECM) can exhibit heterogeneous nano-sequences periodically displaying ligands to regulate complex cell-material interactions in vivo. Herein, an ECM-emulating heterogeneous barcoding system, including ligand-bearing Au and ligand-free Fe nano-segments, is developed to independently present tunable frequency and sequences in nano-segments of cell-adhesive RGD ligand. Specifically, similar exposed surface areas of total Fe and Au nano-segments are designed. Fe segments are used for substrate coupling of nanobarcodes and as ligand-free nano-segments and Au segments for ligand coating while maintaining both nanoscale (local) and macroscale (total) ligand density constant in all groups. Low nano-ligand frequency in the same sequences and terminally sequenced nano-ligands at the same frequency independently facilitate focal adhesion and mechanosensing of stem cells, which are collectively effective both in vitro and in vivo, thereby inducing stem cell differentiation. The Fe/RGD-Au nanobarcode implants exhibit high stability and no local and systemic toxicity in various tissues and organs in vivo. This work sheds novel insight into designing biomaterials with heterogeneous nano-ligand sequences at terminal sides and/or low frequency to facilitate cellular adhesion. Tuning the electrodeposition conditions can allow synthesis of unlimited combinations of ligand nano-sequences and frequencies, magnetic elements, and bioactive ligands to remotely regulate numerous host cells in vivo., (© 2020 Wiley-VCH GmbH.)

With the advent of artificial intelligence (AI), memristors have received significant interest as a synaptic building block for neuromorphic systems, where each synaptic memristor should operate in an analog fashion, exhibiting multilevel accessible conductance states. Here, we demonstrate that the transition of the operation mode in poly(1,3,5-trivinyl-1,3,5-trimethyl cyclotrisiloxane) (pV3D3)-based flexible memristor from conventional binary to synaptic analog switching can be achieved simply by reducing the size of the formed filament. With the quantized conductance states observed in the flexible pV3D3 memristor, analog potentiation and depression characteristics of the memristive synapse are obtained through the growth of atomically thin Cu filament and lateral dissolution of the filament via dominant electric field effect, respectively. The face classification capability of our memristor is evaluated via simulation using an artificial neural network consisting of pV3D3 memristor synapses. These results will encourage the development of soft neuromorphic intelligent systems.

Elucidating chromatin structure in vitro requires resolution below 10 nm to visualize the mononucleosome has been an ongoing challenge. In this work, we achieve sub-10-nm imaging of nucleic acids via spectroscopic intrinsic-contrast photon-localization optical nanoscopy (SICLON) without the use of external labels. SICLON leverages two key innovations: using endogenous nucleotides as the emission source and a custom-made imaging system that can simultaneously record the position and optical spectra of emitting molecules. With a novel spectral regression algorithm that identifies the spectroscopic fingerprints of neighboring molecules that were previously indistinguishable, we demonstrate the utility of SICLON by visualizing unlabeled poly-nucleotides and linear single-stranded DNA fibers with a resolution of 6.2 nm.

In situ and cytocompatible nanoswitching by external stimuli is highly appealing for reversibly regulating cellular adhesion and functions in vivo. Here, a heterodimeric nanoswitch is designed to facilitate in situ switchable and combinatorial presentation of integrin-binding cell-adhesive moieties, such as Mg 2+ and Arg-Gly-Asp (RGD) ligand in nanostructures. In situ reversible nanoswitching is controlled by convertible coordination between bioactive Mg 2+ and bisphosphonate (BP) ligand. A BP-coated gold-nanoparticle monomer (BP-AuNP) on a substrate is prepared to allow in situ assembly of cell-adhesive Mg 2+ -active Mg-BP nanoparticles (NPs) on a BP-AuNP surface via Mg 2+ -BP coordination, yielding heterodimeric nanostructures (switching "ON"). Ethylenediaminetetraacetic acid (EDTA)-based Mg 2+ chelation allows in situ disassembly of Mg 2+ -BP NP, reverting to Mg 2+ -free monomer (switching "OFF"). This in situ reversible nanoswitching on and off of cell-adhesive Mg 2+ presentation allows reversible cell adhesion and release in vivo, respectively, and spatiotemporally controls cyclic cell adhesion. In situ heterodimeric assembly of dual RGD ligand- and Mg 2+ -active RGD-BP-Mg 2+ NP (switching "Dual ON") further tunes and promotes focal adhesion, spreading, and differentiation of stem cells. The modular nature of this in situ nanoswitch can accommodate various bioactive nanostructures via metal-ion-ligand coordination to regulate diverse cellular functions in vivo in reversible and compatible manner., (© 2018 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

Multiplexed surface encoding is achieved by positioning two different sizes of gold nanocubes on gold surfaces with precisely defined locations for each particle via template-confined, DNA-mediated nanoparticle assembly. As a proof-of-concept demonstration, cubes with 86 and 63 nm edge lengths are assembled into arrangements that physically and spectrally encrypt two sets of patterns in the same location. These patterns can be decrypted by mapping the absorption intensity of the substrate at λ = 773 and 687 nm, respectively. This multiplexed encoding platform dramatically increases the sophistication and density of codes that can be written using colloidal nanoparticles, which may enable high-security, high-resolution encoding applications.

Alloy nanoparticles are important in many fields, including catalysis, plasmonics, and electronics, due to the chemical and physical properties that arise from the interactions between their components. Typically, alloy nanoparticles are made by solution-based synthesis; however, scanning-probe-based methods offer the ability to make and position such structures on surfaces with nanometer-scale resolution. In particular, scanning probe block copolymer lithography (SPBCL), which combines elements of block copolymer lithography with scanning probe techniques, allows one to synthesize nanoparticles with control over particle diameter in the 2-50 nm range. Thus far, single-element structures have been studied in detail, but, in principle, one could make a wide variety of multicomponent systems by controlling the composition of the polymer ink, polymer feature size, and metal precursor concentrations. Indeed, it is possible to use this approach to synthesize alloy nanoparticles comprised of combinations of Au, Ag, Pd, Ni, Co, and Pt. Here, such structures have been made with diameters deliberately tailored in the 10-20 nm range and characterized by STEM and EDS for structural and elemental composition. The catalytic activity of one class of AuPd alloy nanoparticles made via this method was evaluated with respect to the reduction of 4-nitrophenol with NaBH4. In addition to being the first catalytic studies of particles made by SPBCL, these proof-of-concept experiments demonstrate the potential for SPBCL as a new method for studying the fundamental science and potential applications of alloy nanoparticles in areas such as heterogeneous catalysis.

A novel, apertureless, cantilever-free pen array can be used for dual scanning photochemical and molecular printing. Serial writing with light is enabled by combining self-focusing pyramidal pens with an opaque backing between pens. The elastomeric pens also afford force-tuned illumination and simultaneous delivery of materials and optical energy. These attributes make the technique a promising candidate for maskless high-resolution photopatterning and combinatorial chemistry., (© 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.)

The label-free detection of cholera toxin is demonstrated using microcantilevers functionalized with ganglioside nanodiscs. The cholera toxin molecules bind specifically to the active membrane protein encased in nanodiscs, nanoscale lipid bilayers surrounded by an amphipathic protein belt, immobilized on the cantilever surface. The specific molecular binding results in cantilever deflection via the formation of a surface stress-induced bending moment. The nanomechanical cantilever response is quantitatively monitored by optical interference. The consistent and reproducible nanomechanical detection of cholera toxin in nanomolar range concentrations is demonstrated. The results validated with such a model system suggest that the combination of a microcantilever platform with receptor nanodiscs is a promising approach for monitoring invasive pathogens and other types of biomolecular detection relevant to drug discovery.

Magnetic resonance imaging (MRI) has become a powerful technique in biological molecular imaging and clinical diagnosis. With the rapid progress in nanoscale science and technology, nanostructure-based MR contrast agents are undergoing rapid development. This is in part due to the tuneable magnetic and cellular uptake properties, large surface area for conjugation and favourable biodistribution. In this review, we describe our recent progress in the development of high-performance nanostructured MR contrast agents. Specifically, we report on Gd-enriched nanostructured probes that exhibit T(1) MR contrast and superparamagnetic Fe(3)O(4) and CoFe(2)O(4) nanostructures that display T(2) MR contrast enhancement. The effects of nanostructure size, shape, assembly and surface modification on relaxivity are described. The potential of these contrast agents for in vitro and in vivo MR imaging with respect to colloidal stability under physiological conditions, biocompatibility, and surface functionality are also evaluated.

Nanodisk arrays of technologically important magnetic (CoFe(2)O(4)) and ferroelectric (BaTiO(3)) oxides are fabricated on diverse substrates with well-defined size and separation using the soft-eBL approach. We demonstrate that below a certain pattern size, the as-deposited amorphous nanodisks can be readily converted into dense, single-crystal form that exhibit cube-on-cube heteroepitaxy with respect to the underlying single-crystal substrate. Such single-crystal disks show well-defined truncated-pyramid morphology that is consistent with Wulff construction. The mechanism of morphology development with the pattern size change is discussed. Localized characterization of the crystallinity, chemical composition, and magnetic behavior of the CFO nanodisk patterns are carried out using analytical transmission electron microscopy and magnetic force microscopy. Such solution-based epitaxial conversion of patterned arrays of multifunctional oxides has potential for viable cost-effective technological applications.

A versatile patterning approach based on electron-beam lithography (eBL) and solution deposition, termed soft-eBL, has been developed to fabricate radially stacked heterostructures of multifunctional oxides from their sol precursors. Well-defined nanorings of lead zirconate titanate (PZT) are fabricated on a variety of substrates such as noble metals (e.g., Au), semiconductors (e.g., Si), and oxide single crystals (e.g., SrTiO3), which were previously functionalized with appropriate self-assembled monolayers (SAMs). The undercut in the double-layer eBL resist and substrate functionalization with the SAM treatment play a vital role in the formation of the ring structures. The nanorings are then used as building block "containers" and ring-reservoirs are filled with a second sol (e.g., CoFe2O4) to form radially stacked composite ceramic heterostructures. The approach presented here does not require either feature alignment to realize heterostructures or the etching of ceramics, and is amenable to a variety of radially stacked composite heterostructures.

A nondestructive imaging method, scanning near-field ultrasound holography (SNFUH), has been developed that provides depth information as well as spatial resolution at the 10- to 100-nanometer scale. In SNFUH, the phase and amplitude of the scattered specimen ultrasound wave, reflected in perturbation to the surface acoustic standing wave, are mapped with a scanning probe microscopy platform to provide nanoscale-resolution images of the internal substructure of diverse materials. We have used SNFUH to image buried nanostructures, to perform subsurface metrology in microelectronic structures, and to image malaria parasites in red blood cells.

Although tremendous advances have been made in preparing porous crystals from molecular precursors1,2, there are no general ways of designing and making topologically diversified porous colloidal crystals over the 10-1,000 nm length scale. Control over porosity in this size range would enable the tailoring of molecular absorption and storage, separation, chemical sensing, catalytic and optical properties of such materials. Here, a universal approach for synthesizing metallic open-channel superlattices with pores of 10 to 1,000 nm from DNA-modified hollow colloidal nanoparticles (NPs) is reported. By tuning hollow NP geometry and DNA design, one can adjust crystal pore geometry (pore size and shape) and channel topology (the way in which pores are interconnected). The assembly of hollow NPs is driven by edge-to-edge rather than face-to-face DNA-DNA interactions. Two new design rules describing this assembly regime emerge from these studies and are then used to synthesize 12 open-channel superlattices with control over crystal symmetry, channel geometry and topology. The open channels can be selectively occupied by guests of the appropriate size and that are modified with complementary DNA (for example, Au NPs).

Aqueous phosphate pollution can dramatically impact ecosystems, introducing a variety of environmental, economic, and public health problems. While novel remediation tactics based on nanoparticle binding have shown considerable promise in nutrient recovery from water, they are challenging to deploy at scale. To bridge the gap between the laboratory-scale nature of these nanostructure solutions and the practical benchmarks for deploying an environmental remediation tool, we have developed a nanocomposite material. Here, an economical, readily available, porous substrate is dip coated using scalable, waterbased processes with a slurry of nanostructures. These nanomaterials have tailored affinity for specific adsorption of pollutants. Our Phosphate Elimination and Recovery Lightweight (PEARL) membrane can selectively sequester up to 99% of phosphate ions from polluted waters at environmentally relevant concentrations. Moreover, mild tuning of pH promotes at will adsorption and desorption of nutrients. This timed release allows for phosphate recovery and reuse of the PEARL membrane repeatedly for numerous cycles. We combine correlative microscopy and spectroscopy techniques to characterize the complex microstructure of the PEARL membrane and to unravel the mechanism of phosphate sorption. More broadly, through the example of phosphate pollution, this work describes a platform membrane approach based on nanostructures with specific affinity coated on a porous structure. Such a strategy can be tuned to address other environmental remediation challenges through the incorporation of other nanomaterials. [ABSTRACT FROM AUTHOR]

The article focuses on a research related to use of nanomechanical sensors to detect femtomolar concentrations of analytes underlying cantilever surface. It mentions role of passivation to limit the cantilevers through non-specific binding at the bottom surface. It also highlights limitations on detection of microcantilever bending that uses conventional lasers and photodiodes.

Abstract: The development of MRI contrast agents has experienced its version of the gilded age over the past decade, thanks largely to the rapid advances in nanotechnology. In addition to progress in single mode contrast agents, which ushered in unprecedented R1 or R2 sensitivities, there has also been a boon in the development of agents covering more than one mode of detection. These include T1–PET, T2–PET T1–optical, T2–optical, T1–T2 agents and many others. In this review, we describe four areas which we feel have experienced particular growth due to nanotechnology, specifically T2 magnetic nanostructure development, T1/T2–optical dual mode agents, and most recently the T1–T2 hybrid imaging systems. In each of these systems, we describe applications including in vitro, in vivo usage and assay development. In all, while the benefits and drawbacks of most MRI contrast agents depend on the application at hand, the recent development in multimodal nanohybrids may curtail the shortcomings of single mode agents in diagnostic and clinical settings by synergistically incorporating functionality. It is hoped that as nanotechnology advances over the next decade, it will produce agents with increased diagnostics and assay relevant capabilities in streamlined packages that can meaningfully improve patient care and prognostics. In this review article, we focus on T2 materials, its surface functionalization and coupling with optical and/or T1 agents. [Copyright &y& Elsevier]