Showing papers on "Particle published in 2004"

Electromagnetic fields around silver nanoparticles and dimers.

Abstract: We use the discrete dipole approximation to investigate the electromagnetic fields induced by optical excitation of localized surface plasmon resonances of silver nanoparticles, including monomers and dimers, with emphasis on what size, shape, and arrangement leads to the largest local electric field (E-field) enhancement near the particle surfaces. The results are used to determine what conditions are most favorable for producing enhancements large enough to observe single molecule surface enhanced Raman spectroscopy. Most of the calculations refer to triangular prisms, which exhibit distinct dipole and quadrupole resonances that can easily be controlled by varying particle size. In addition, for the dimer calculations we study the influence of dimer separation and orientation, especially for dimers that are separated by a few nanometers. We find that the largest /E/2 values for dimers are about a factor of 10 larger than those for all the monomers examined. For all particles and particle orientations, the plasmon resonances which lead to the largest E-fields are those with the longest wavelength dipolar excitation. The spacing of the particles in the dimer plays a crucial role, and we find that the spacing needed to achieve a given /E/2 is proportional to nanoparticle size for particles below 100 nm in size. Particle shape and curvature are of lesser importance, with a head to tail configuration of two triangles giving enhanced fields comparable to head to head, or rounded head to tail. The largest /E/2 values we have calculated for spacings of 2 nm or more is approximately 10(5).

A new thermal conductivity model for nanofluids

Abstract: In a quiescent suspension, nanoparticles move randomly and thereby carry relatively large volumes of surrounding liquid with them. This micro-scale interaction may occur between hot and cold regions, resulting in a lower local temperature gradient for a given heat flux compared with the pure liquid case. Thus, as a result of Brownian motion, the effective thermal conductivity, keff, which is composed of the particles’ conventional static part and the Brownian motion part, increases to result in a lower temperature gradient for a given heat flux. To capture these transport phenomena, a new thermal conductivity model for nanofluids has been developed, which takes the effects of particle size, particle volume fraction and temperature dependence as well as properties of base liquid and particle phase into consideration by considering surrounding liquid traveling with randomly moving nanoparticles.

Particle Morphology and Density Characterization by Combined Mobility and Aerodynamic Diameter Measurements. Part 1: Theory

Abstract: Different on-line submicron particle sizing techniques report different “equivalent diameters.” For example, differential mobility analyzers (DMAs) report electrical mobility diameter (dm ), while a number of recently developed instruments (such as the Aerodyne aerosol mass spectrometer, or AMS) measure vacuum aerodynamic diameter (dva ). Particle density and physical morphology (shape) have important effects on diameter measurements. Here a framework is presented for combining the information content of different equivalent diameter measurements into a single coherent mathematical description of the particles. We first present a review of the mathematical formulations used in the literature and their relationships. We then show that combining dm and dva measurements for the same particle population allows the placing of constraints on particle density, dynamic shape factor (x), and fraction of internal void space. The amount of information that can be deduced from the combination of dm and dm measurement...

Self-Assembly of Patchy Particles.

Abstract: Molecular simulations are performed to study the self-assembly of particles with discrete, attractive interaction sites − “patches” − at prescribed locations on the particle surface. Chains, sheets, rings, icosahedra, square pyramids, tetrahedra, and twisted and staircase structures are obtained through suitable design of the surface pattern of patches. Our simulations predict that the spontaneous formation of two-dimensional sheets and icosahedra occurs via a first-order transition while the formation of chains occurs via a continuous disorder-to-order transition as in equilibrium polymerization. Our results show how precise arrangements of patches combined with patch “recognition” or selectivity may be used to control the relative position of particles and the overall structure of particle assemblies. In this context, patchy particles represent a new class of building block for the fabrication of precise structures.

Hierarchically mesostructured doped CeO2 with potential for solar-cell use.

Abstract: Many properties provided by supramolecular chemistry, nanotechnology and catalysis only appear in solids exhibiting large surface areas and regular porosity at the nanometre scale In nanometre-sized particles, the ratio of the number of atoms in the surface to the number in the bulk is much larger than for micrometre-sized materials, and this can lead to novel properties Here we report the preparation of a hierarchically structured mesoporous material from nanoparticles of CeO(2) of strictly uniform size The synthesis involves self-assembly of these 5-nm CeO(2) pre-treated nanoparticles in the presence of a structure directing agent (poly(alkylene oxide) block polymer) The walls of this hexagonal structured CeO(2) material are formed from the primary nanoparticles The material possesses large pore volumes, high surface areas, and marked thermal stability, allowing it to be easily doped after synthesis whilst maintaining textural and mechanical integrity It also exhibits a photovoltaic response, which is directly derived from the nanometric particle size-normal CeO(2) does not show this response We have constructed operational organic-dye-free solar cells using nanometric ceria particles (in both mesostructured or amorphous forms) as the active component, and find efficiencies that depend on the illuminating power

Discharge Model for the Lithium Iron-Phosphate Electrode

Abstract: This paper develops a mathematical model for lithium intercalation and phase change in an iron phosphate-based lithium-ion cell in order to understand the cause for the low power capability of the material. The juxtaposition of the two phases is assumed to be in the form of a shrinking core, where a shell of one phase covers a core of the second phase. Diffusion of lithium through the shell and the movement of the phase interface are described and incorporated into a porous electrode model consisting of two different particle sizes. Open-circuit measurements are used to estimate the composition ranges of the single-phase region. Model-experimental comparisons under constant current show that ohmic drops in the matrix phase, contact resistances between the current collector and the porous matrix, and transport limitations in the iron phosphate particle limit the power capability of the cells. Various design options, consisting of decreasing the ohmic drops, using smaller particles, and substituting the liquid electrolyte by a gel are explored, and their relative importance discussed. The model developed in this paper can be used as a means of optimizing the cell design to suit a particular application.

Solid-phase diffusion mechanism for GaAs nanowire growth

Abstract: Controllable production of nanometre-sized structures is an important field of research, and synthesis of one-dimensional objects, such as nanowires, is a rapidly expanding area with numerous applications, for example, in electronics, photonics, biology and medicine Nanoscale electronic devices created inside nanowires, such as p-n junctions, were reported ten years ago More recently, hetero-structure devices with clear quantum-mechanical behaviour have been reported, for example the double-barrier resonant tunnelling diode and the single-electron transistor The generally accepted theory of semiconductor nanowire growth is the vapour-liquid-solid (VLS) growth mechanism, based on growth from a liquid metal seed particle In this letter we suggest the existence of a growth regime quite different from VLS We show that this new growth regime is based on a solid-phase diffusion mechanism of a single component through a gold seed particle, as shown by in situ heating experiments of GaAs nanowires in a transmission electron microscope, and supported by highly resolved chemical analysis and finite element calculations of the mass transport and composition profiles

Synthesis of Fe Oxide Core/Au Shell Nanoparticles by Iterative Hydroxylamine Seeding

Abstract: Water-soluble, Au-coated magnetic Fe oxide nanoparticles with diameters ∼60 nm were synthesized by the reduction of Au3+ onto the surfaces of ∼9 nm diameter particles consisting of either γ-Fe2O3 or partially oxidized Fe3O4 via iterative hydroxylamine seeding. The morphology and optical properties of the core/shell particles are dependent on the quantity of deposited Au, while the magnetic properties remain largely independent of Au addition. The Au-coated particles exhibit a surface plasmon resonance peak that blue-shifts from 570 to 525 nm with increasing Au deposition. SQUID magnetometry reveals that particle magnetic properties are not affected by the overlayer of a moderately thick Au shell.

Single virus particle mass detection using microresonators with nanoscale thickness

Abstract: In this letter, we present the microfabrication and application of arrays of silicon cantilever beams as microresonator sensors with nanoscale thickness to detect the mass of individual virus particles. The dimensions of the fabricated cantilever beams were in the range of 4–5 μm in length, 1–2 μm in width and 20–30 nm in thickness. The virus particles we used in the study were vaccinia virus, which is a member of the Poxviridae family and forms the basis of the smallpox vaccine. The frequency spectra of the cantilever beams, due to thermal and ambient noise, were measured using a laser Doppler vibrometer under ambient conditions. The change in resonant frequency as a function of the virus particle mass binding on the cantilever beam surface forms the basis of the detection scheme. We have demonstrated the detection of a single vaccinia virus particle with an average mass of 9.5 fg. These devices can be very useful as components of biosensors for the detection of airborne virus particles.

Controlled, Rapid Deposition of Structured Coatings from Micro- and Nanoparticle Suspensions

Abstract: The objective of the study was to develop the operational basis for rapid and controlled deposition of crystal coatings from particles of a wide size range. We deposited such structured coatings by dragging with constant velocity a small volume of liquid confined in a meniscus between two plates. Two types of structured coatings were characterized: latex colloidal crystals and thin layers from metallic nanoparticles. The crystal deposition was sped up by use of preconcentrated suspensions. Crystal coatings larger than a few square centimeters were deposited in minutes from aqueous suspension volumes of approximately 10 μL. The governing mechanism of crystal deposition is convective assembly at high volume fractions. The two major process parameters that allow control over the coating thickness and structure were the deposition speed and particle volume fraction. The evaporation rate was not found to affect the process to a large extent. A volumetric flux balance was used to relate the deposition paramete...

Small-angle neutron scattering study of structural changes in temperature sensitive microgel colloids

Abstract: The structure of temperature-sensitive poly(N-isopropylacrylamide) microgels in dilute suspension was investigated by means of small-angle neutron scattering. A direct modeling expression for the scattering intensity distribution was derived which describes very well the experimental data at all temperatures over an extensive q range. The overall particle form as well as the internal structure of the microgel network is described by the model. The influence of temperature, cross-linking density, and particle size on the structure was revealed by radial density profiles and clearly showed that the segment density in the swollen state is not homogeneous, but gradually decays at the surface. The density profile reveals a box profile only when the particles are collapsed at elevated temperatures. An increase of the cross-linking density resulted in both an increase of the polymer volume fraction in the inner region of the particle and a reduction of the smearing of the surface. The polymer volume fraction inside the colloid decreased with increasing particle size. The structural changes are in good agreement with the kinetics of the emulsion copolymerization used to prepare the microgel colloids.

The particle finite element method: a powerful tool to solve incompressible flows with free-surfaces and breaking waves

Abstract: SUMMARY Particle Methods are those in which the problem is represented by a discrete number of particles. Each particle moves accordingly with its own mass and the external/internal forces applied to it. Particle Methods may be used for both, discrete and continuous problems. In this paper, a Particle Method is used to solve the continuous fluid mechanics equations. To evaluate the external applied forces on each particle, the incompressible Navier–Stokes equations using a Lagrangian formulation are solved at each time step. The interpolation functions are those used in the Meshless Finite Element Method and the time integration is introduced by an implicit fractional-step method. In this manner classical stabilization terms used in the momentum equations are unnecessary due to lack of convective terms in the Lagrangian formulation. Once the forces are evaluated, the particles move independently of the mesh. All the information is transmitted by the particles. Fluid–structure interaction problems including free-fluid-surfaces, breaking waves and fluid particle separation may be easily solved with this methodology. Copyright 2004 John Wiley & Sons, Ltd.

The particle finite element method. An overview

Abstract: We present a general formulation for the analysis of fluid-structure interaction problems using the particle finite element method (PFEM). The key feature of the PFEM is the use of a Lagrangian description to model the motion of nodes (particles) in both the fluid and the structure domains. Nodes are thus viewed as particles which can freely move and even separate from the main analysis domain representing, for instance, the effect of water drops. A mesh connects the nodes defining the discretized domain where the governing equations, expressed in an integral form, are solved as in the standard FEM. The necessary stabilization for dealing with the incompressibility condition in the fluid is introduced via the finite calculus (FIC) method. A fractional step scheme for the transient coupled fluid-structure solution is described. Examples of application of the PFEM method to solve a number of fluid-structure interaction problems involving large motions of the free surface and splashing of waves are presented.

Rheology of active-particle suspensions.

Abstract: We study the interplay of activity, order, and flow through a set of coarse-grained equations governing the hydrodynamic velocity, concentration, and stress fields in a suspension of active, energy-dissipating particles. We make several predictions for the rheology of such systems, which can be tested on bacterial suspensions, cell extracts with motors and filaments, or artificial machines in a fluid. The phenomena of cytoplasmic streaming, elastotaxis, and active mechanosensing find natural explanations within our model.

Knowledge concerning splat formation : An invited review

Abstract: This paper summarizes our knowledge at the beginning of 2003 about splat formation. First, the analytical and numerical models related to the impact and flattening of single particles on smooth or rough substrates with different tilting are recalled. Then, the different diagnostic methods, including imaging, are briefly described. The last part of the paper is devoted to the results and their discussion. Studies are related to the effect of various parameters on particle flattening. They include the characteristics of particles prior to impact: normal impact velocity, temperature, molten state, oxidation state, etc.; the parameters related to the substrate: tilting angle, roughness, oxide layer composition, thickness and crystallinity, desorption of adsorbates and condensates, wetting properties between impacting particle and substrate, etc.; and, finally, the parameters related to the heat exchange between the flattening particle and the substrate. They depend on previous parameters and control the propagation of the solidification front within the flattening particle, eventually modifying its liquid flow. It is obvious from this review that, if our understanding of the involved phenomena has been drastically improved during the last years, many points have still to be clarified. This is of primary importance because all the coating properties are linked to the particle flattening, splat formation, and layering.

Synthesis and utilization of monodisperse hollow polymeric particles in photonic crystals.

Abstract: We developed a process to fabricate 150-700 nm monodisperse polymer particles with 100-500 nm hollow cores. These hollow particles were fabricated via dispersion polymerization to synthesize a polymer shell around monodisperse SiO(2) particles. The SiO(2) cores were then removed by HF etching to produce monodisperse hollow polymeric particle shells. The hollow core size and the polymer shell thickness, can be easily varied over significant size ranges. These hollow polymeric particles are sufficiently monodisperse that upon centrifugation from ethanol they form well-ordered close-packed colloidal crystals that diffract light. After the surfaces are functionalized with sulfonates, these particles self-assemble into crystalline colloidal arrays in deionized water. This synthetic method can also be used to create monodisperse particles with complex and unusual morphologies. For example, we synthesized hollow particles containing two concentric-independent, spherical polymer shells, and hollow silica particles which contain a central spherical silica core. In addition, these hollow spheres can be used as template microreactors. For example, we were able to fabricate monodisperse polymer spheres containing high concentrations of magnetic nanospheres formed by direct precipitation within the hollow cores.

Size distributions and mixtures of dust and black carbon aerosol in Asian outflow: Physiochemistry and optical properties

Abstract: [1] During Transport and Chemical Evolution over the Pacific (TRACE-P) and Asian Aerosol Characterization Experiment (ACE-Asia) we measured the dry size distribution of Asian aerosols, their state of mixing, and the optical properties of dust, black carbon (BC) and other aerosol constituents in combustion and/or dust plumes. Optical particle sizing in association with thermal heating extracted volatile components and resolved sizes for dust and refractory soot that usually dominated light absorption. BC was internally mixed with volatile aerosol in � 85% of accumulation mode particles and constituted � 5–15% of their mass. These optically effective sizes constrained the soot and dust size distributions and the imaginary part of the dust refractive index, k, to 0.0006 ± 0.0001. This implies a single-scatter albedo, v (550 nm), for dust ranging from 0.99+ for Dp <1 m mt o� 0.90 at Dp =1 0mm and a size-integrated campaign average near 0.97 ± 0.01. The typical mass scattering efficiency for the dust was � 0.3 m 2 g � 1 , and the mass absorption efficiency (MAE) was 0.009 m 2 g � 1 . Less dust south of 25� N and stronger biomass burning signatures resulted in lower values for v of � 0.82 in plumes aloft. Chemically inferred elemental carbon was moderately correlated with BC light absorption (R 2 = 0.40), while refractory soot volume between 0.1 and 0.5 mm was highly correlated (R 2 = 0.79) with absorption. However, both approaches yield an MAE for BC mixtures of � 7±2m 2 g � 1 and higher than calculated MAE values for BC of 5 m 2 g � 1 . The increase in the mass fraction of soot and BC in pollution aerosol in the presence of elevated dust appears to be due to uptake of the volatile components onto the coarse dust. This predictably lowered v for the accumulation mode from 0.84 in typical pollution to � 0.74 in high-dust events. A chemical transport model revealed good agreement between model and observed BC absorption for most of SE Asia and in biomass plumes but underestimated BC for combustion sources north of 25� N by a factor of � 3. INDEX TERMS: 0305 Atmospheric Composition and Structure: Aerosols and particles (0345, 4801); 0350 Atmospheric Composition and Structure: Pressure, density, and temperature; 0360 Atmospheric Composition and Structure: Transmission and scattering of radiation; 0365 Atmospheric Composition and Structure: Troposphere—composition and chemistry; 0368 Atmospheric Composition and Structure: Troposphere— constituent transport and chemistry; KEYWORDS: dust, black carbon, absorption, single scatter albedo

Deviation from the classical colloid filtration theory in the presence of repulsive DLVO interactions.

Abstract: A growing body of experimental evidence suggests that the deposition behavior of microbial particles (e.g., bacteria and viruses) is inconsistent with the classical colloid filtration theory (CFT). Well-controlled laboratory-scale column deposition experiments were conducted with uniform model particles and collectors to obtain insight into the mechanisms that give rise to the diverging deposition behavior of microorganisms. Both the fluid-phase effluent particle concentration and the profile of retained particles were systematically measured over a broad range of physicochemical conditions. The results indicate that, in the presence of repulsive Derjaguin-Landau-Verwey-Overbeek (DLVO) interactions, the concurrent existence of both favorable and unfavorable colloidal interactions causes significant deviation from the CFT. A dual deposition mode model is presented which considers the combined influence of "fast" and "slow" particle deposition. This model is shown to adequately describe both the spatial distribution of particles in the packed bed and the suspended particle concentration at the column effluent.

Microfluidic synthesis of colloidal silica.

Abstract: We demonstrate the design, fabrication, and operation of microfluidic chemical reactors for the synthesis of colloidal silica particles. Two reactor configurations are examined: laminar flow reactors and segmented flow reactors. We analyze particle sizes and size distributions and examine their change with varying linear flow velocity and mean residence time. Laminar flow reactors are affected by axial dispersion at high linear velocities, thus leading to wide particle size distributions under these conditions. Gas is used to create a segmented flow, consisting liquid plugs separated by inert gas bubbles. The internal recirculation created in the liquid plugs generates mixing, which eliminates the axial dispersion effects associated with laminar flow reactors and produces a narrow size distribution of silica nanoparticles.

Van der Waals versus dipolar forces controlling mesoscopic organizations of magnetic nanocrystals

Abstract: The structure, thermodynamics and dynamics in many physical and chemical systems are determined by interplay of short-range isotropic and long-range anisotropic forces. Magnetic nanoparticles dispersed in solution are ideal model systems to study this interplay, as they are subjected to both isotropic van der Waals and anisotropic dipolar forces. Here we show from experiment an abrupt transition of maghemite nanocrystal organization from chain-like to random structures when nanoparticle solutions are evaporated under a magnetic field. This is explained by brownian dynamics simulations in terms of a variation of the strength of van der Waals interactions with the particle contact distance, which is tuned by the length of the molecules coating the particles. The weak dipole-dipole interactions between the maghemite particles are usually not sufficient to result in the chain formation observed here. However, due to the van der Waals interactions, when the nanocrystal contact distance is short enough, clusters of nanocrystals are formed during the evaporation process. These clusters exhibit large dipole moments compared with a single particle, which explains the formation of chain-like structures. Conversely, when the nanocrystal contact distance is too long, no nanocrystal aggregation occurs, and a random distribution of maghemite nanocrystals is obtained.

Particle phase acidity and oligomer formation in secondary organic aerosol.

Abstract: A series of controlled laboratory experiments are carried out in dual Teflon chambers to examine the presence of oligomers in secondary organic aerosols (SOA) from hydrocarbon ozonolysis as well as to explore the effect of particle phase acidity on SOA formation. In all seven hydrocarbon systems studied (i.e., α-pinene, cyclohexene, 1-methyl cyclopentene, cycloheptene, 1-methyl cyclohexene, cyclooctene, and terpinolene), oligomers with MW from 250 to 1600 are present in the SOA formed, both in the absence and presence of seed particles and regardless of the seed particle acidity. These oligomers are comparable to, and in some cases, exceed the low molecular weight species (MW < 250) in ion intensities in the ion trap mass spectra, suggesting they may comprise a substantial fraction of the total aerosol mass. It is possible that oligomers are widely present in atmospheric organic aerosols, formed through acid- or base-catalyzed heterogeneous reactions. In addition, as the seed particle acidity increases, larger oligomers are formed more abundantly in the SOA; consequently, the overall SOA yield also increases. This explicit effect of particle phase acidity on the composition and yield of SOA may have important climatic consequences and need to be considered in relevant models.

Shape-controlled synthesis and shape-induced texture of MnFe2O4 nanoparticles.

Abstract: Monodisperse MnFe2O4 nanoparticles with cubelike and polyhedron shapes were synthesized by reaction of Fe(acac)3 and Mn(acac)2 with 1,2-hexadecanediol, oleic acid, and oleylamine. Controlled evaporation of the particle dispersion led to nanoparticle superlattices. The crystal orientation of the particle in the assembly depends on the shape of the particles, with particles in a cubelike shape showing (100) texture and those in the polyhedron shape exhibiting (110) texture.