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At least 253 records · Page 14Linked to original sources
PubMed2005

Nanofaceted platinum surfaces: a new model system for nanoparticle catalysts.

We present a novel model system for nanoparticle electrocatalysts. A surface consisting of alternating (100) and (111) facets, several nanometers across and nearly 1 microm long, were self-assembled by annealing Pt single crystal surfaces initially cut at the midpoint between [111] and [100] directions, i.e., Pt(1+ square root of 3 1 1). The formation of these self-assembled arrays of nanofacets was monitored by in-situ surface X-ray scattering. These surfaces were further characterized with scanning probe microscopy and cyclic voltammetry. We found that the Pt(1+ square root of 3 1 1) surface is flat with less than 1 nm rms roughness when it was annealed in argon/hydrogen atmosphere. Then the surface forms nanofacets when it is annealed in pure air. This nanofaceting transition was completely reversible and reproducible. We investigated effects of CO adsorption on the voltammetric characteristics of both hydrogen-annealed and air-annealed surfaces. We found that CO-adsorption/desorption cycles in CO containing electrolyte solution result in considerable modification of blank cyclic voltammograms for the both surfaces. We attributed these differences to the electrochemical annealing of surface defects due to the increased mobility during the cycles.

Journal Article↗
PubMed2006

Molecule-molecule versus molecule-substrate interactions in the assembly of oligothiophenes at surfaces.

In this paper we present a joint experimental and theoretical approach for the study of the assembly of end-substituted oligothiophenes at surfaces with different polarities (i.e., mica vs graphite). Scanning probe microscopy studies of (sub)monolayer deposits show various types of structures (one-dimensional fibrils, two-dimensional regular layers, and monolayers), depending on the nature of the end groups and the substrate. Using molecular modeling with an atomistic approach, we focus on the interplay between the molecule-molecule (and segment-segment) interactions and the molecule-substrate interactions and their influence on the observed morphologies and the stacking geometry. Such information is relevant for controlling the structural order in thin layers of thiophene oligomers for use in field-effect transistor applications, for example, by modifying the nature of dielectric material over which those compounds are deposited.

Journal Article↗
PubMed2006

Finite element simulations of tip-enhanced Raman and fluorescence spectroscopy.

Finite element electromagnetic simulations of scanning probe microscopy tips and substrates are presented. The enhancement of the scattered light intensity is found to be as high as 10(12) for a 20 nm radius gold tip, and tip-substrate separation of 1 nm. Molecular resolution imaging (< 1 nm) is achievable, even with a relatively large radius tip (20 nm). We also make predictions for imaging in aqueous environments, noting a sizable red shift of the spectral peaks. Finally, we discuss signal levels, and predict that high-speed Raman mapping should be possible with gold substrates and a small tip-substrate separation (< 4 nm).

Air↗
PubMed2004

Immobilization of the nanoparticle monolayer onto self-assembled monolayers by combined sterically enhanced hydrophobic and electrophoretic forces.

The immobilization of surface-derivatized gold nanoparticles onto methyl-terminated self-assembled monolayers (SAMs) on gold surface was achieved by the cooperation of hydrophobic and electrophoretic forces. Electrochemical and scanning probe microscopy techniques were utilized to explore the influence of the SAM's structure and properties of the nanoparticle/SAM/gold system. SAMs prepared from 1-decanethiol (DT) and 2-mercapto-3-n-octylthiophene (MOT) were used as hydrophobic substrates. The DT SAM is a closely packed and organized monolayer, which can effectively block the underlying gold and inhibit a variety of solution species including organic and inorganic molecules from penetrating, whereas the MOT monolayer is poorly packed or disorganized (because of a large difference in dimension between the thiophene head and the alkylchain tail) and permeable to many organic probes in aqueous solution but not to inorganic probes. Thus, the MOT monolayer provides a more energetically favorable hydrophobic surface for the penetration and adsorption of organic species than the DT monolayer. This hypothesis is supported by experiments in which the density of hydrophobically immobilized nanoparticles on the MOT SAM is much larger than that on the DT SAM. The results also suggest new approaches for modification of macroscopic surfaces with nanoscopic particles.

Electrochemistry↗
PubMed2004

Mixed polymer brushes by sequential polymer addition: anchoring layer effect.

Smart surfaces can be described as surfaces that have the ability to respond in a controllable fashion to specific environmental stimuli. A heterogeneous (mixed) polymer brush (HPB) can provide a synthetic route to designing smart polymer surfaces. In this research we study HPB comprised of end-grafted polystyrene (PS) and poly(2-vinyl pyridine) (P2VP). The synthesis of the HPB involves the use of an "intermolecular glue" acting as a binding/anchoring interlayer between the polymer brush and the substrate, a silicon wafer. We compare anchoring layers of epoxysilane (GPS), which forms a self-assembled monolayer with epoxy functionality, to poly(glycidyl methacrylate) (PGMA), which forms a macromolecular monolayer with epoxy functionality. The PS and P2VP were deposited onto the wafers in a sequential fashion to chemically graft PS in a first step and subsequently graft P2VP. Rinsing the HPB in selective solvents and observing the change in water contact angle as a function of the HPB composition studied the switching nature of the HPB. Scanning probe microscopy was used to probe the topography and phase imagery of the HPB. The nature of the anchoring layer significantly affected the wettability and morphology of the mixed brushes.

Journal Article↗
PubMed2005

Structure and bonding issues at the interface between gold and self-assembled conjugated dithiol monolayers.

Organic thiols have received extensive attention recently because of their relative stability and ease of examination compared to other potential molecular electronic materials. In this work, scanning probe microscopy (SPM) is used to study (i) the structural properties of self-assembled monolayers (SAMs) containing conjugated dithiols and (ii) the formation of the upper molecule-metal interface on dithiol SAMs. The top gold film is deposited either by thermal evaporation or by nano-transfer printing (nTP). Generally, the utility of thermal evaporation is limited because of Au diffusion through the SAMs. However, several dithiol SAMs are identified in this work that bond well to Au overlayers and act as satisfactory diffusion barriers. Coassembly of conjugated dithiols and alkanemonothiols is suggested as a route to obtain dithiols that are denser packed and more vertical (than is obtained from pure dithiol routes). High-yield nTP is demonstrated on coassembled SAMs. Advantages and limitations of different Au deposition and transfer techniques are compared on a variety of length scales.

Gold↗
PubMed2005

High-resolution submicron patterning of self-assembled monolayers using a molecular fluorine laser at 157 nm.

Using a molecular fluorine laser at 157 nm wavelength, submicron patterning of organosilane self-assembled monolayers (SAMs) is demonstrated utilizing mask-contact photolithography. An organosilane, namely, octadecyltrimethoxysilane [ODS, CH(3)(CH(2))(17)Si(OCH(3))(3)], SAM is chemisorbed onto Si substrates covered with a 2 nm thick oxide layer and subsequently patterned using the laser. The optical path of the laser beam and the photomask-sample space are evacuated and then backfilled and purged with nitrogen during laser firing. The resulting pattern is investigated using various measurement techniques. The scanning probe microscopy images show that patterns are transferred to the SAM-covered Si substrates and that 500 nm features are successfully photoprinted in this way.

Journal Article↗
PubMed2006

Electrochemically nanopatterned conducting coronas of a conjugated polymer precursor: SPM parameters and polymer composition.

Here we describe the formation of precisely controlled corona-type nanopatterns on electroactive polymer precursor films using scanning probe microscopy (SPM) methods. The binary composition of electroactive groups in the polymer triggers the formation of corona-type nanopatterns at particular voltages and tip writing speeds through the electrooxidation of the polymer precursor film. Various parameters such as tip speed and applied bias were explored in the nanopatterning process, and the formation of a conductive nanopattern was investigated using conducting atomic force microscopy (C-AFM). The formation of the nanopattern was attributed to the flow of electrons from the AFM tip to the polymer film in a controlled electric field distribution. We also report a new method to distinguish the polymer composition and distribution of a polymer blend film by characterizing biasing differences in the patterning of a polymer film.

Journal Article↗
PubMed2005

Enzyme-assisted nanolithography.

We have chemically immobilized alkaline phosphatase molecules onto the apex of a tip of an atomic force microscope. When the substrate BCIP is dephosphorylated by alkaline phosphatase, it will precipitate in the presence of NBT. By bringing the tip in the vicinity of a suitable sample, we could locally deposit this complex on the sample. Thus we combined the activity of an enzyme with the accuracy in positioning a tip in scanning probe microscopy to demonstrate a novel technique referred to as enzyme-assisted nanolithography. By use of other enzymes, this method will open the possibility to chemically modify surfaces on a nanometer scale.

Alkaline Phosphatase↗
PubMed2004

Semi-synthetic DNA-protein conjugates: novel tools in analytics and nanobiotechnology.

This article reports on the syntheses, characterization and applications of semi-synthetic conjugates composed of nucleic acids, proteins and inorganic nanoparticles. For example, self-assembled oligomeric networks consisting of streptavidin and double-stranded DNA are applicable as reagents in immunoassays, model systems for ion-switchable nanoparticle networks as well as nanometer-scaled 'soft material' standards for scanning probe microscopy. Covalent conjugates of single-stranded DNA and streptavidin are utilized as biomolecular adapters for the immobilization of biotinylated macromolecules at solid substrates via nucleic acid hybridization. This 'DNA-directed immobilization' allows for reversible and site-selective functionalization of solid substrates with metal and semiconductor nanoparticles or, vice versa, for the DNA-directed functionalization of gold nanoparticles with proteins, such as immunoglobulins and enzymes. This approach is applicable for the detection of chip-immobilized antigens. Moreover, covalent DNA-protein conjugates allow for their selective positioning along single-stranded nucleic acids, and thus for the construction of nanometre-scale assemblies composed of proteins and/or nanoclusters. Examples include the fabrication of functional biometallic nanostructures from gold nanoparticles and antibodies, applicable as diagnostic tools in bioanalytics.

Biotechnology↗
PubMed1999

Flat-bed scanning as a tool for quantitative neuroimaging.

The aim of this study was to compare three different imaging techniques which are used to provide data on the laminar structure of the human cerebral cortex. Region V1 of Brodmann's area 17 stained with cresyl violet was investigated, and a conventional semi-automatic morphometric evaluation, the videomicroscropic procedure and a new transparent flat-bed scanning technique were compared. The results of each digitizing method were converted into normalized profiles which allow the laminae in the striate cortex to be displayed. It was found that major laminar patterns can be detected by the scanning technique, but that subsidiary laminations are more clearly displayed by morphometry and videomicroscopy. For magnifications up to x 400 a high resolution transparent flat-bed scanner may be used in place of the videomicroscopy technique.

Aged↗
PubMed2003

Isolation and biophysical studies of natural eumelanins: applications of imaging technologies and ultrafast spectroscopy.

The major pigments found in the skin, hair, and eyes of humans and other animals are melanins. Despite significant research efforts, the current understanding of the molecular structure of melanins, the assembly of the pigment within its organelle, and the structural consequences of the association of melanins with protein and metal cations is limited. Likewise, a detailed understanding of the photochemical and photophysical properties of melanins has remained elusive. Many types of melanins have been studied to date, including natural and synthetic model pigments. Such studies are often contradictory and to some extent the diversity of systems studied may have detracted from the development of a basic understanding of the structure and function of the natural pigment. Advances in the understanding of the structure and function of melanins require careful characterization of the pigments examined so as to assure the data obtained may be relevant to the properties of the pigment in vivo. To address this issue, herein the influence of isolation procedures on the resulting structure of the pigment is examined. Sections describing the applications of new technologies to the study of melanins follow this. Advanced imaging technologies such as scanning probe microscopies are providing new insights into the morphology of the pigment assembly. Recent photochemical studies on photoreduction of cytochrome c by different mass fraction of sonicated natural melanins reveal that the photogeneration of reactive oxygen species (ROS) depends upon aggregation of melanin. Specifically, aggregation mitigates ROS photoproduction by UV-excitation, suggesting the integrity of melanosomes in tissue may play an important role in the balance between the photoprotective and photodamaging behaviors attributed to melanins. Ultrafast laser spectroscopy studies of melanins are providing insights into the time scales and mechanisms by which melanin dissipates absorbed light energy.

Animals↗
PubMed2004

Marking of specific sequences in double-stranded DNA molecules--SNP detection and direct observation.

In this study, we describe a simple method to mark specific sequences in double-stranded DNA molecules. For the marking, we used two specifically designed oligonucleotides, one of which is complementary to the sequence to be marked and the other, serving as a splint, to make the marking stable and detectable by subsequent various analytical means. In the presence of the two deoxyoligonucleotides, whereas RecA protein-mediated reaction converts the sequence to be marked to a regional triple-stranded structure with the complementary (probing) oligonucleotide, DNA ligase transforms it to a stable multi- (possibly quintuple) stranded structure with the splint oligonucleotide. The whole marking process is simple and completed in a single reaction mixture. Because RecA protein makes the marking to proceed with high fidelity, we were able to mark (detect) SNPs in complex genomes like human's. Furthermore, the structure of the marked sequence is stable and quite distinct enough to be readily detectable by biochemical means or direct observation by scanning probe microscopy.

Blotting, Southern↗
PubMed2000

Structure analysis of regenerated cellulose hydrogels by small-angle and ultra-small-angle x-ray scattering.

Absolute intensities Deltai(q) of small-angle x-ray scattering (SAXS) and ultra-small-angle x-ray scattering (USAXS) were measured in a wide range of scattering vector q from 2x10(-4) to 0.5 A(-1) for transparent (VI-P) and translucent (VI-L) cellulose hydrogels prepared by coagulation and regeneration of viscose in acid solutions with and without acetone, respectively. We obtained the scattering intensities at very small q conveniently by desmearing the combined data measured by SAXS and USAXS. The plot of Deltai(q)q(2) versus log(10) q showed a peak at -2.5<log(10) q<-1.0. By assuming a two-phase model with the high-density phase (phase 1) composed of only cellulose and with the low-density phase (phase 2) composed of cellulose dispersed in water, volume fractions of phase 1 in VI-P and VI-L were determined to be 0.18 and 0.09, respectively, from the mean-square fluctuation of electron density determined as integral of (Deltai(q)q(2)dq). By fitting the observed scattering profile with the theoretical particle scattering functions of spheres, the average diameter of the high-density region including crystallite was determined to be 120 A for VI-P and 80 A for VI-L. Similar analyses were applied also to freeze-dried VI-P. These results were consistent with those obtained by the wide-angle x-ray-diffraction measurement and also with the observation by scanning probe microscopy.

Cellulose↗
PubMed2002

Fractal analysis of sampled profiles: systematic study.

A quantitative evaluation of the influence of sampling on the numerical fractal analysis of experimental profiles is of critical importance. Although this aspect has been widely recognized, a systematic analysis of the sampling influence is still lacking. Here we present the results of a systematic analysis of synthetic self-affine profiles in order to clarify the consequences of the application of a poor sampling (up to 1000 points) typical of scanning probe microscopy for the characterization of real interfaces and surfaces. We interpret our results in terms of a deviation and a dispersion of the measured exponent with respect to the "true" one. Both the deviation and the dispersion have always been disregarded in the experimental literature, and this can be very misleading if results obtained from poorly sampled images are presented. We provide reasonable arguments to assess the universality of these effects and propose an empirical method to take them into account. We show that it is possible to correct the deviation of the measured Hurst exponent from the "true" one and give a reasonable estimate of the dispersion error. The last estimate is particularly important in the experimental results since it is an intrinsic error that depends only on the number of sampling points and can easily overwhelm the statistical error. Finally, we test our empirical method calculating the Hurst exponent for the well-known 1+1 dimensional directed percolation profiles, with a 512-point sampling.

Journal Article↗
PubMed2003

Uniform semiclassical wave function for coherent two-dimensional electron flow.

We find a uniform semiclassical (SC) wave function describing coherent branched flow through a two-dimensional electron gas (2DEG), a phenomenon recently discovered by direct imaging of the current using scanned probed microscopy [M.A. Topinka, B.J. LeRoy, S.E.J. Shaw, E.J. Heller, R.M. Westervelt, K.D. Maranowski, and A.C. Gossard, Science 289, 2323 (2000)]. The formation of branches has been explained by classical arguments [M.A. Topinka, B.J. LeRoy, R.M. Westervelt, S.E.J. Shaw, R. Fleischmann, E.J. Heller, K.D. Maranowski, and A.C. Gossard, Nature (London) 410, 183 (2001)], but the SC simulations necessary to account for the coherence are made difficult by the proliferation of catastrophes in the phase space. In this paper, expansion in terms of "replacement manifolds" is used to find a uniform SC wave function for a cusp singularity. The method is then generalized and applied to calculate uniform wave functions for a quantum-map model of coherent flow through a 2DEG. Finally, the quantum-map approximation is dropped and the method is shown to work for a continuous-time model as well.

Journal Article↗
PubMed2000

Nanotomography

Scanning probe microscopy (SPM) can be expanded to volume imaging. As an example, the core of a dislocation within the three-dimensional (3D) spatial microdomain structure of poly(styrene-block-butadiene-block-styrene) was imaged with approximately 10 nm resolution. The specimen was eroded step by step and its chemical composition in layers beneath the original surface was imaged with SPM. Similar to computed tomography, the 3D distribution of polystyrene and polybutadiene was reconstructed from a series of images. This approach might provide a simple means for real-space volume imaging with nanometer and even atomic resolution of various materials and physical properties.

Journal Article↗
PubMed2001

Electronic structure of carbon nanocones.

Topology related changes in the local density of states near the apex of carbon nanocones are investigated using both tight-binding and ab initio calculations. Sharp resonant states are found to dominate the electronic structure in the region close to the Fermi energy. The strength and the position of these states with respect to the Fermi level depend sensitively on the number and the relative positions of the pentagons constituting the conical tip. Carbon nanocones are thus proposed as good candidates for nanoprobes in scanning probe microscopy.

Journal Article↗