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At least 829 records · Page 46Linked to original sources
PubMed2006

First-principles theoretical analysis of silyl radical diffusion on silicon surfaces.

We report results from a detailed analysis of the fundamental radical precursor diffusion processes on silicon surfaces and discuss their implications for the surface smoothness of hydrogenated amorphous silicon (a-Si:H) thin films. The analysis is based on a synergistic combination of first-principles density functional theory (DFT) calculations of SiH(3) radical migration on the hydrogen-terminated Si(001)-(2 x 1) surface with molecular-dynamics (MD) simulations of SiH(3) radical precursor migration on surfaces of a-Si:H films. Our DFT calculations yield activation energies for SiH(3) migration that range from 0.18 to 0.89 eV depending on the local electronic environment on the Si(001)-(2 x 1):H surface. In particular, when no substantial surface relaxation (Si-Si bond breaking or formation) accompanies the hopping of the SiH(3) radical the activation barriers are highest, whereas hopping between nearest-neighbor overcoordinated surface Si atoms results in the lowest radical diffusion barrier of 0.18 eV; this low barrier is consistent with the activation barrier for SiH(3) migration through overcoordinated sites on the a-Si:H surface. Specifically, the analysis of the MD simulations of SiH(3) radical migration on a-Si:H surfaces yields an effective diffusion barrier of 0.16 eV, allowing for the rapid migration of the SiH(3) radical prior to its incorporation in surface valleys; rapid migration and subsequent incorporation constitute the two-step mechanism responsible for the smoothness of plasma deposited a-Si:H thin films.

Chemical Phenomena↗
PubMed2006

Chemoresponsive monolayer transistors.

This work details a method to make efficacious field-effect transistors from monolayers of polycyclic aromatic hydrocarbons that are able to sense and respond to their chemical environment. The molecules used in this study are functionalized so that they assemble laterally into columns and attach themselves to the silicon oxide surface of a silicon wafer. To measure the electrical properties of these monolayers, we use ultrasmall point contacts that are separated by only a few nanometers as the source and drain electrodes. These contacts are formed through an oxidative cutting of an individual metallic single-walled carbon nanotube that is held between macroscopic metal leads. The molecules assemble in the gap and form transistors with large current modulation and high gate efficiency. Because these devices are formed from an individual stack of molecules, their electrical properties change significantly when exposed to electron-deficient molecules such as tetracyanoquinodimethane (TCNQ), forming the basis for new types of environmental and molecular sensors.

Biosensing Techniques↗
PubMed2002

Colloidal assemblies on patterned silane layers.

The site-selective assembly of colloidal polymer particles onto laterally patterned silane layers was studied as a model system for the object assembly process at mesoscale dimensions. The structured silane monolayers on silicon oxide substrates were fabricated by a combination of liquid- and gas-phase deposition of different trialkoxysilanes with a photolithographic patterning technique. By using this method various types of surface functionalizations such as regions with amino functions next to areas of the bare silica surface or positively charged regions of a quaternary ammonium silane surrounded by a hydrophobic octadecylsilane film could be obtained. Furthermore, a triethoxysilane with a photoprotected amino group was synthesized, which allowed direct photopatterning after monolayer preparation, leading to free NH(2) groups at the irradiated regions. The different silane monolayer patterns were used to study the surface assembly behavior of carboxylated methacrylate particles by optical and scanning electron microscopy. In dependence of the assembly conditions (different surface functionalizations, pH, and drying conditions), a selective preference of the particles for a specific surface type versus others was found. Site-specific colloid adsorption could be observed also on the photosensitive silane layers after local deprotection with light. From the photosensitive silane and positively charged ammonium silane, molecularly mixed monolayers were prepared, which allowed particle adsorption and photoactivation within the same monolayer as shown by fluorescence labeling.

Carboxylic Acids↗
PubMed2001

Origin of nanomechanical cantilever motion generated from biomolecular interactions.

Generation of nanomechanical cantilever motion from biomolecular interactions can have wide applications, ranging from high-throughput biomolecular detection to bioactuation. Although it has been suggested that such motion is caused by changes in surface stress of a cantilever beam, the origin of the surface-stress change has so far not been elucidated. By using DNA hybridization experiments, we show that the origin of motion lies in the interplay between changes in configurational entropy and intermolecular energetics induced by specific biomolecular interactions. By controlling entropy change during DNA hybridization, the direction of cantilever motion can be manipulated. These thermodynamic principles were also used to explain the origin of motion generated from protein-ligand binding.

DNA, Single-Stranded↗
PubMed2004

Mineralization of dentin induced by treatment with bioactive glass S53P4 in vitro.

Dentin hypersensitivity can be managed to occlude dentin tubules, but none of the agents used are components of natural dentin. Using a calcium phosphate precipitation (CPP) method, dentin tubules can be occluded with a calcium phosphate (CaP) layer similar to the major inorganic component of dentin. The CPP method utilizes acidic pH conditions, such as etching of dentin, over the course of several dental treatments. A gentler method can be used to produce a CaP layer on the surface of dentin. By treating with bioactive glass S53P4 (BAG), or regular commercial glass (CG), mineralization occurs in physiologically neutral solutions such as simulated body fluid (SBF) and remineralization solution (RMS). After a short period of immersion, silica is dissolved from both types of glass, but the amount of silica released is much greater from BAG than from CG. The dissolved silica is adsorbed on the surface of dentin during the pretreatment procedure and enhances the mineralization of dentin in SBF. After 14 days' mineralization the dentin is fully covered by the CaP layer, but after 14 days' immersion in RMS decalcification of the dentin occurs. Pretreatment with BAG decreases the degree of decalcification of dentin during the mineralization process. These findings suggest that bioactive glass S53P4 can be used as a therapeutic material for mineralization of dentin and its tubules in a physiological environment.

Adsorption↗
PubMed2001

Determination of permeation parameters of experimental PET films coated with SiOx to ethyl acetate, oxygen and water vapour.

The permeation parameters of conventional PET films, films coated with SiOx and SiOx-coated films laminated to LDPE were determined for ethyl acetate using the permeation cell/gas chromatography method. Permeation to O2 and water vapour was also determined to monitor overall changes in the barrier properties of the experimental films. Coating of the PET film was achieved by a 'directed evaporation' method that increased the yield of the coating process from 30-35 to > 70%. It was shown that the SiOx coating increased the film barrier to ethyl acetate by approximately 20-30 times. Permeation values showed low reproducibility, indicating the need for further development and standardization of the 'directed evaporation' web-coating process. The barrier to oxygen and water vapour increased by 20-25 and 12-14 times respectively after coating. The web-coating speed did not seem to influence the barrier properties of the films. Permeation coefficients, diffusion coefficients and solubility coefficients were calculated for all samples.

Acetates↗
PubMed1999

Rapid screening for organochlorine and organophosphorus pesticides in milk using C18 and graphitized carbon black solid phase extraction cleanup.

A rapid, multiresidue, solid phase extraction (SPE) technique for the isolation and gas chromatographic determination of organochlorine and moderately polar organophosphorus pesticide residues in milk is described. Milk is sonicated with an acetonitrile-acetone-methanol mixture and centrifuged. The supernatant is subjected to a cleanup using both C18 and graphitized carbon black SPE columns. The pesticide residues are determined by gas chromatography with electron capture and flame photometric detection. The method required minimal volumes of solvent and resulted in the production of minimal volumes of hazardous waste.

Animals↗
PubMed2003

Structure-property relationships of silicone biofouling-release coatings: effect of silicone network architecture on pseudobarnacle attachment strengths.

Model silicone foul-release coatings with controlled molecular architecture were evaluated to determine the effect of compositional variables such as filler loading and crosslink density on pseudobarnacle attachment strength. Pseudobarnacle adhesion values correlated with filler loadings in both condensation and hydrosilylation-cured silicones. Variation of crosslink density of hydrosilylation-cured silicones had an insignificant effect on attachment strength. X-ray photoelectron spectroscopy (XPS) indicated that the mode of failure upon detachment of the pseudobarnacle was dependent upon the crosslink density; samples with high crosslink density failed cohesively within the silicone.

Adhesiveness↗
PubMedDate not supplied

Using an extractive Fourier transform infrared spectrometer for improving cleanroom air quality in a semiconductor manufacturing plant.

A mobile extractive Fourier transform infrared (FTIR) spectrometer was successfully used to locate, identify, and quantify the "odor" sources inside the cleanroom of a semiconductor manufacturing plant. It was found that ozone (O(3)) gas with a peak concentration of 120 ppm was unexpectedly releasing from a headspace of a drain for transporting used ozonized water and that silicon tetrafluoride (SiF(4)) with a peak concentration of 3 ppm was off-gassed from silicon wafers after dry-etching processing. When the sources of the odors was pinpointed by the FTIR, engineering control measures were applied. For O(3) control, a water-sealed pipeline was added to prevent the O(3) gas (emitting from the ozonized water) from entering the mixing unit. A ventilation system also was applied to the mixing unit in case of O(3) release. For SiF(4) mitigation, before the wafer-out chamber was opened, N(2) gas with a flow rate of 150 L/min was used for 100 sec to purge the wafer-out chamber, and a vacuum system was simultaneously activated to pump away the purging N(2). The effectiveness of the control measures was assured by using the FTIR. In addition, the FTIR was used to monitor the potential hazardous gas emissions during preventative maintenance of the semiconductor manufacturing equipment.

Air Pollution, Indoor↗
PubMed2004

Organic carbon and ammonium nitrogen removal in a laboratory sand percolation filter.

The on-site treatment of wastewaters from single dwellings requires simple, low maintenance systems that reduce the chemical and biochemical oxygen demand (COD and BOD respectively), ammonium-nitrogen (NH4-N), orthophosphate (PO4-P), phosphorus (P), and microorganisms to acceptable concentrations. Sand filters have the potential to achieve these reductions. In this study, a sand tank model of a percolation trench and filter was constructed in the laboratory, loaded with wastewater, and monitored for a period of 293 days. The silty sand filter was seeded for 153 days with effluent from an aerobic biofilm treatment unit. The filter was then loaded with synthetic wastewater of domestic strength for 193 days, when the average organic and hydraulic loading rates on the percolation trench were 13.33 g BOD/m2 d and 75 L/m2 d respectively. Removal rates of 90% for total COD, 99.3% for BOD5, >99% for total NH4-N, 89% for total PO4-P, and 96% for total suspended solids (TSS) were recorded during the study. No excessive clogging of the sand filter was observed. During the study very good dispersion of the wastewater over the sand filter by the percolation trench was recorded. The sand filter was simple to construct and operate and achieved excellent results.

Biofilms↗
PubMedDate not supplied

MDPSCL2: a new protecting group for chemoselective synthesis of 2'-O-alkylated guanosines.

An improved strategy for the synthesis of 2'-O-methyl-guanosine (6) and 2'-MOE-guanosine (8) is reported. The regioselectivity of the alkylation was attained using a novel silicon-based protecting group, methylene-bis (diisopropyl-silylchloride) (MDPSCl2, 2). The alkylation proceeded in a chemoselective manner using NaHMDS as the base and MeCl or MOE-Br as the appropriate electrophiles.

Alkylation↗
PubMed1988

SiS in Orion-KL: evidence for "outflow" chemistry.

SiS has been conclusively detected toward Orion-KL via its J = 6-5 and J = 5-4 rotational transitions at 91 and 109 GHz. Line profiles indicate that the species is present at an LSR velocity of 7.5 km s-1 with a half-width at zero power of 36 km s-1. Such characteristics associate SiS with the moderate velocity outflow (V approximately 18 km s-1) centered on IRc2 and observed in thermal SiO, the NH3 "plateau," and OH, H2O, and SiO masers. The column density estimated for SiS in this region is Ntot = 4 x 10(15) cm-2, corresponding to a fractional abundance of f approximately 4 x 10(-9). Such an abundance implies an SiO/SiS ratio of approximately 60 in the outflow material, remarkably close to the cosmic O/S ratio of approximately 40 and contrasting with the SiO/SiS value of > approximately 10(3) predicted by ion-molecule models. This difference is probably a result of the high temperatures and densities present in the outflow, which favor thermal equilibrium abundances similar to those observed in the circumstellar shells of late-type stars rather than "ion-molecule"-type concentrations. In addition to SiS, some twenty new unidentified lines near 91 and 109 GHz were detected toward KL, as well as transitions arising from HC5N, HC13CCN, HCC13CN, O13CS, and, possibly, CH3CH2OH, CH3CHO, and CH3OD.

Astronomical Phenomena↗
PubMed1989

Shock chemistry in the molecular clouds associated with SNR IC 443.

Several interstellar molecules have been detected toward the highly perturbed B and G clouds associated with the supernova remnant IC 443 via their 3 mm transitions, including N2H+, SiO, SO, CN, HNC, and H13CO+. The (J, K) = (1, 1) and (2, 2) inversion lines of metastable ammonia have also been observed, as well as the J = 3-2 transition of HCO+ at 1.2 mm. Analysis of the (1, 1) and (2, 2) inversion lines of NH3 indicates minimum gas kinetic temperatures of TK = 70 K toward cloud B, and TK = 33 K in cloud G. Modeling of the J = 1-0 and J = 3-2 transitions of HCO+ implies densities greater than 10(5) cm-3 toward both positions. These data clearly show that hot and dense material is present in IC 443, and they suggest the presence of shocks in both regions. A careful analysis of the HCO+ lines indicates that the HCO+ abundance is at most enhanced by factors of a few over that found in cold, quiescent gas. This conclusion contradicts past claims of HCO+ abundance enhancements of several orders of magnitude in the perturbed regions. The N2H+ abundance was also found to be similar to that in cold gas, suggesting that there is no increase in ionization in the clouds. The abundances of SO and CS, as well as CN and NH3, do not appear to differ significantly from those found in cold dark clouds, although chemistry models predict sulfur-containing species to undergo high-temperature enhancements. SiO, however, is found to have an abundance in the perturbed gas 100 times larger than the upper limits observed in the dark cloud TMC 1, a result in agreement with high temperature chemistry models. In addition, the HNC/HCN ratio in both IC 443 B and G was found to be approximately 0.1--far from the ratio of 1 predicted by low-temperature ion-molecule chemistry, but similar to the values observed in clouds where elevated temperatures are present.

Ammonia↗
PubMed1989

Interstellar SiO as a tracer of high-temperature chemistry.

The J = 2-1 transition of SiO has been searched for toward both hot and cold molecular gas. SiO was not detected toward the dark clouds TMC-1, L134 N, and B335, down to column density upper limits of N < 2-4 x 10(10) cm-2. The species, however, has been observed toward all sources with a kinetic temperature greater than or equal to 30 K, with the largest column densities (N approximately 10(13)-10(17) cm-2) measured in the warmest (TK > or = 100 K) material. The abundance of SiO, relative to HCN, is found to be approximately 0.1-1 in the massive star-forming regions toward Orion and NGC 7538; toward the dark clouds, the upper limits to this ratio is less than 0.0002-0.004. A similar enhancement in the warmer regions is reflected in the SiO/H2 ratio as well. A linear relation was found between the natural log of the SiO concentration and 1/TK, suggesting that the species' formation involves a chemically specific process that contains an activation barrier of approximately 90 K. SiO was also found to be underabundant with respect to SO in cold clouds, with SiO/SO < 1/1000, versus SiO/SO > or =, measured in Orion-KL. The formation of SiO is therefore linked closely to the local gas kinetic temperature, rather than the oxygen abundance, and its synthesis is likely to involve high-temperature gas-phase reactions. The species thus may serve as an unambiguous indicator of high-temperature or "shock" chemistry.

Astronomical Phenomena↗
PubMed1994

The circumstellar environment of IRAS 05338-0624.

Millimeter continuum and spectral line observations with 10", 30", and 60" resolution are used to characterize the structure and chemistry of the gas around the young, embedded star, IRAS 05338-0624. On arcminute scales, emission from dense gas tracers outline an isolated condensation centered on the IRAS source position. The condensation is characterized by a size of approximately 60", a density of 2 x 10(5) cm-3, and a virial mass of 40 M solar. Interferometric CS J = 2-1 observations show two peaks, one toward the continuum peak and the other toward a position 14" west and 8" south. Single-dish maps of SO, CH3OH, and SiO show pronounced wing emission to the west of the IRAS source, which interferometer observations reveal to be a compact region of outflow activity. CS emission as redshifted and blueshifted velocities reveals a bipolar outflow oriented with a position angle of 45 degrees, while SiO emission appears to be tracing a fast shock interaction region at the CS red-lobe peak, 14" west and 8" south of the IRAS source. Finally, H13CO+ emission traces clumps of quiescent gas toward the IRAS source and adjacent to the blue lobe of the outflow. Column densities and molecular fractional abundances are derived to explore the interaction between the surrounding condensation and the young stellar object. We find evidence for gas phase depletions within the overall condensation in several gas tracers (CO, CS, HCN, SO) but not in the region immediately around the young stellar object. Enhanced abundances of SO, CH3OH, and SiO (by factors of 4, >100, >1000, respectively) are observed in the shocked gas; these enhancements may be explained in terms of a nondissociative shock liberating mantle materials that contain some amount of refractory materials, a moderate velocity dissociative shock in which only minor sputtering of Si occurs, or a shock that impacts surrounding material with a range of speeds.

Astronomy↗
PubMed1994

The molecular emission-line spectrum of IRC +10216 between 330 and 358 GHz.

We have conducted a spectral line survey of IRC +10216 using the Caltech Submillimeter Observatory to an average sensitivity of < or approximately 95 mK. A deconvolution algorithm has been used to derive the continuous single-sideband spectrum from 330.2 to 358.1 GHz. A total of 56 spectral lines were detected of which 54 have been identified with 8 molecules and a total of 18 isotopomers. The observed lines are used to derive column densities and relative abundances for the detected species. Within this frequency range the spectral lines detected contribute the majority of the total flux emitted by IRC +10216. We use the derived column densities and excitation temperatures to simulate the molecular line emission (assuming LTE) at frequencies up to 1000 GHz. The observed and simulated flux from line emission is compared to broadband total flux measurements and to dust emission assuming a power-law variation of the dust emissivity. We conclude that significant corrections for the line flux must be made to broadband flux measurements of IRC +10216 at wavelengths longer than approximately 750 micrometers.

Algorithms↗
PubMed1997

A line survey of Orion KL from 325 to 360 GHz.

We present a high-sensitivity spectral line survey of the high-mass star-forming region Orion KL in the 325-360 GHz frequency band. The survey was conducted at the Caltech Submillimeter Observatory on Mauna Kea, Hawaii. The sensitivity achieved is typically 0.1-0.5 K and is limited mostly by the sideband separation method utilized. We find 717 resolvable features consisting of 1004 lines, among which 60 are unidentified. The identified lines are due to 34 species and various isotopomers. Most of the unidentified lines are weak, and many of them most likely due to isotopomers or vibrationally or torsionally excited states of known species with unknown line frequencies, but a few reach the 2-5 K level. No new species have been identified, but we were able to strengthen evidence for the identification of ethanol in Orion and found the first nitrogen sulfide line in this source. The molecule dominating the integrated line emission is S02, which emits twice the intensity of CO, followed by SO, which is only slightly stronger than CO. In contrast, the largest number of lines is emitted from heavy organic rotors like HCOOCH3, CH3CH2CN, and CH3OCH3, but their contribution to the total flux is unimportant. CH3OH is also very prominent, both in the number of lines and in integrated flux. An interesting detail of this survey is the first detection of vibrationally excited HCN in the v2 = 2 state, 2000 K above ground. Clearly this is a glimpse into the very inner part of the Orion hot core.

Astronomy↗