Evaluation of Influence of Multiple Scattering Effect in Light-Scattering-Based Applications

The extinction cross sections of a system containing two particles are calculated by the T-matrix method, and the results are compared with those of two single particles with single-scattering approximation. The necessity of the correction of the refractive indices of water and polystyrene for different incident wavelengths is particularly addressed in the calculation. By this means, the volume fractions allowed for certain accuracy requirements of single-scattering approximation in the light scattering experiment can be evaluated. The volume fractions calculated with corrected refractive indices are compared with those obtained with fixed refractive indices which have been rather commonly used, showing that fixed refractive indices may cause significant error in evaluating multiple scattering effect. The results also give a simple criterion for selecting the incident wavelength and particle size to avoid the ＇blind zone＇ in the turbidity measurement, where the turbidity change is insensitive to aggregation of two particles.     

Local fields close to the surface of nanoparticles and aggregates of nanoparticles

A refined discussion of the near-field scattering of spherical nanoparticles and the electromagnetic fields close to the particle surface is given. New results for the dependence on the distance from the surface and the angular distribution of the scattered light in the near-field are given. It will be shown that the radial component of the electric field leads to striking differences in the phase functions in the near-field and the far-field. Exemplary computations are presented for Ag and Au particles with different size. In a second part the discussion is extended to assemblies of spherical Ag and Au nanoparticles. It will be shown that large near-fields at wavelengths commonly used in SERS experiments are obtained for aggregates. In the near-field scattering intensity “hot spots” mark regions between particles in the aggregate where the near-field is particularly high. Received: 4 May 2001 / Revised version: 20 July 2001 / Published online: 19 September 2001     

Effect of counterions on the swelling of spherical polyelectrolyte brushes

We investigate the swelling of colloidal spherical polyelectrolyte brushes in the presence of different counterions. The colloidal particles consist of a solid poly(styrene) core of ca. 100 nm diameter onto which linear polyelectrolyte chains are chemically grafted. Two types of polyelectrolyte chains have been used here: The cationic polyelectrolyte poly(2-(acryloyl)ethyltrimethylammonium chloride)) (PATAC) and the anionic poly(styrenesulfonate) (PSS). Both systems are dispersed in water and the degree of swelling of the surface layer is studied by dynamic light scattering. Adding more and more salt leads to a strong shrinking of the surface layer as expected for polyelectrolyte brushes. It is shown that data obtained at low ionic strength can be collapsed on suitable master curves for monovalent and divalent counterions, respectively. For some ions, however, high salt concentrations may lead to a re-swelling of the brush layer in case of the cationic systems. This points to specific interactions of the counterions with the PATAC chains. This strong specific interaction between the counterions and the attached polyelectrolyte may even lead to flocculation of the particles at intermediate salt concentration. Surprisingly, for iodide and magnesium counterions the solubility increases again if the salt concentration is raised to 1 mol/l. Hence, specific interaction leads to salting-out effects as well as to salting-in effects for these colloidal particles. All specific effects seen at high concentrations of added salt can be explained by the increase of the reduced excluded-volume parameter which is due to the adsorption of salt ions.     

High-energy probes

We review some results on energetic particle production in heavy-ion collisions below roughly 100A·MeV, both theoretically and experimentally. We discuss the possible mechanisms of particle production, as well as the possibility to gather information on the nuclear equation of state (EOS) from data. Results on subthreshold pions, energetic photons, nucleons and light charged particles (Z ⩽ 2) are discussed and contrasted to microscopic models. Important information about the first stages of the reaction are obtained by such probes. At present, we can conclude that we have at least a qualitative understanding of the processes involved when such particles are produced. However, a quantitative determination of relevant EOS parameters is still missing. The production mechanism close to the kinematical threshold (incoherent, cooperative or statistical) is not completely elucidated either. This calls for new data using more modern detector systems and comparison to more refined microscopic models.     

Manipulation of Particles with Counter-Propagating Evanescent Waves

Two counter-propagating evanescent beams are used to align and manipulate polystyrene particles on a prism surface. Since the radiation pressure transferred laterally from the evanescent wave is negated on both sides, particles can be stably aligned. By projecting a circular and a linear beam spot onto the interface, both multiple and single arrays of particles are achieved. Arrays of particles trapped on the interface can be easily moved adjusting the intensity of incident beams on either side. We also simulate electromagnetic distribution of scattering light that is converted from the evanescent wave using the FDTD method. The results show that scattering light converts from an evanescent wave propagating through a particle array and has a distance longer than that propagating from a normal evanescent wave.     

Light scattering with swollen hexagonal phases

We investigate, using quasi-elastic light scattering, some features of the long-wavelength, low-frequency modes of the hexagonal phase often encountered in the study of lyotropic (surfactant-solvent) systems. The hexagonal phase is swollen by an oil-based ferrofluid, allowing magnetically aligned samples to be prepared. We show experimentally the anisotropy of the two lowest-frequency modes. We develop a model which predicts that these slow modes are associated to particle diffusion and tube motion. With the help of microscopic as well as phenomenological analyses, we suggest that the latter presumably corresponds to a peristaltic mode. Confinement effects on the one-dimensional, Brownian diffusion of the colloids along the tube axis together with the coupling between the two modes are studied experimentally, varying the tube diameter to particle size ratio. Received 7 July 1999     

球形雾霾粒子的紫外光散射偏振特性研究

在我国经济社会快速发展的同时,雾霾天气成为了突出的环境问题,雾霾粒子的测量非常重要。偏振紫外光与大气雾霾粒子发生散射后,散射光偏振状态(Stokes矢量以及偏振度)的改变能反映雾霾粒子的相关物理特性(粒径、复杂折射率等)。基于Mie散射理论建立了紫外光雾霾球形粒子直视和非直视单次散射模型,研究了单个球形粒子和链状结构球形粒子物理特性的改变对散射光偏振状态的影响,并用蒙特卡洛仿真分析已知粒径分布的雾霾粒子浓度对散射光偏振状态的影响。结果表明：针对单个球形粒子,随着粒子粒径的增大Stokes矢量中散射光光强(I_s)随之增强,粒子复折射率虚部为先增大后较小,偏振度也是在不断增大,且复折射率虚部较小时,偏振度增加趋势快;对于粒径分布不变的雾霾粒子,随着粒子的浓度增加,雾霾粒子的散射系数、消光系数和吸收系数均呈线性增加,但是I_s先增大后减小。针对链状球形粒子,随着粒子个数的增加,I_s均呈现增大的趋势,且偏振度可用于区分链状球形粒子是否由相同球形粒子组成; 相同球形粒子组成链状结构中,I_s随着粒子数量的增加而线性增大,偏振度不改变;不同球形粒子组成的链状结构,I_s以及偏振度的变化趋势可以区分粒子物理特性。     

Existence, stability and structure of a hexagonal phase doped with nanoparticles

We describe and study by small-angle X-ray scattering (SAXS) a new type of hybrid system. It is composed of a swollen lyotropic hexagonal phase into the cylinders of which solid magnetic particles of nanometric size have been incorporated. It has been found to be stable for volume fractions of particles up to 2% provided the cylinders are sufficiently large. A unidimensionnal magnetic liquid is thus realized. The structural properties of this colloidal assembly have been investigated by SAXS, and the specific features of the scattering spectra are analysed and interpreted. One of the remarkable results is the evidence of depletion interactions between the particles and the inner walls of the cylinders inside which particles are located. Received: 4 September 1997 / Revised: 14 October 1997 / Accepted: 19 November 1997     

Scattering and absorption by spherical multilayer particles

We present a recursion formalism for the scattering coefficients of multilayered spherical particles which is more treatable for computer programs than the matrixformalism of Bhandari [1]. We computed explicitely the extinction and scattering cross section spectra of different metal coated spheres. Comparison with experimental results is done for gold-silver heterosystems. The spectra are in very good agreement with the experimental data.     

Teleportation of an Arbitrary Multipartite GHZ-Class State by One EPR Pair

We present a scheme for perfectly teleporting an arbitrary and unknown N-particle GHZ-class state from a sender to a receiver. We just need one quantum channel composed of two or three particles in the maximally entangled state. The sender performs one Bell-state measurement on two of her particles and N - 1 Hadamard operations and N - 1 yon Neumann measurements on the rest N - 1 particles. The receiver adopts one corresponding unitary transformation on his particles shared with the sender. After that, the receiver can obtain the original N-particle GHZ-class state by introducing N - 1 ancillary particles and carrying out N - 1 controlled-NOT operations. We also generalize the scheme to the case of controlled teleportation.     

Light scattering by Gaussian particles with internal inclusions and roughened surfaces using ray optics

We study light scattering by Gaussian-random-sphere particles that are large compared to the wavelength of the incident light using ray optics that, in addition to Fresnellian reflection and refraction, accounts for diffuse scattering. We consider two types of diffusely scattering media. One type of media constitutes a uniform medium inside the particle, i.e. a diffuse internal medium. The second type of media constitutes a layer on the surface of the particle that is thin compared to the particle dimensions and acts as a diffuse external medium mimicking the particle surface roughness. We illustrate the effects of the diffuse media on the scattering characteristics for both cases and show that incorporating diffuse scatterers allows us to explain the scattering matrices measured experimentally for Saharan sand particles large compared to the wavelength.     

Dynamic and static light scattering study of the formation of cross-linked PMMA gels

Free radical co-polymerization of methyl methacrylate (MMA) and ethyl glycol dimethyl metacrylate (EGDMA) was investigated in solution at different molar ratios R = [EGDMA]/[MMA] between 0 and 0.05. Initially mainly linear PMMA was formed with weight average molar mass 7.5 g/mol independent of R. At larger reaction extents branched polymers were formed and the systems gelled. The scattering intensity rose initially with the reaction extent, but reached a plateau value at larger reaction extents. The plateau value increased strongly with R. Dynamic light scattering showed the appearance of a slow relaxation not observed in linear PMMA solutions. The data can be interpreted by assuming that the excess scattering originates from the branching points and relaxes through self diffusion of the branched particles. The results agree with predictions of the percolation model for gelation and Rouse dynamics. Viscosity measurements corroborate this interpretation. Measurements on a progressively diluted sample quenched close to the gel point again showed quantitative agreement with the percolation model for gelation. Received 11 May 1998 and Received in final form 22 October 1998     

Soft Dynamics simulation. 1. Normal approach of two deformable particles in a viscous fluid and optimal-approach strategy

Discrete simulation methods are efficient tools to investigate the behaviors of complex fluids such as dry granular materials or dilute suspensions of hard particles. By contrast, materials made of soft and/or concentrated units (emulsions, foams, vesicles, dense suspensions) can exhibit both significant elastic particle deflections (Hertz-like response) and strong viscous forces (squeezed liquid). We point out that the gap between two particles is then not determined solely by the positions of their centers, but rather exhibits its own dynamics. We provide the first ingredients of a new discrete numerical method, named Soft Dynamics, to simulate the combined dynamics of particles and contacts. As an illustration, we present the results for the approach of two particles. We recover the scaling behaviors expected in three limits: the Stokes limit for very large gaps, the Poiseuille-lubricated limit for small gaps and even smaller surface deflections, and the Hertz limit for significant surface deflections. We find that for each gap value, an optimal force achieves the fastest approach velocity. The principle of larger-scale simulations with this new method is provided. They will consitute a promising tool for investigating the collective behaviors of many complex materials.     

Phase control algorithms for focusing light through turbid media

Light propagation in materials with microscopic inhomogeneities is affected by scattering. In scattering materials, such as powders, disordered metamaterials or biological tissue, multiple scattering on sub-wavelength particles makes light diffuse. Recently, we showed that it is possible to construct a wavefront that focuses through a solid, strongly scattering object. The focusing wavefront uniquely matches a certain configuration of the particles in the medium. To focus light through a turbid liquid or living tissue, it is necessary to dynamically adjust the wavefront as the particles in the medium move. Here we present three algorithms for constructing a wavefront that focuses through a scattering medium. We analyze the dynamic behavior of these algorithms and compare their sensitivity to measurement noise. The algorithms are compared both experimentally and using numerical simulations. The results are in good agreement with an intuitive model, which may be used to develop dynamic diffusion compensators with applications in, for example, light delivery in human tissue.     

Light scattering by slightly nonspherical particles on surfaces

We investigate the shape dependence of the scattering by dielectric and metallic particles on surfaces by considering particles whose free-space scattering properties are nearly identical. The scattering by metallic particles is strongly dependent on the shape of the particle in the region near where the particle touches the surface. The scattering by dielectric particles displays a weaker, but nonetheless significant, dependence on particle shape. These results have a significant effect on the use of light scattering to size and identify particles on surfaces.     

Conformation and aggregation of poly-L-proline in solution

Although a large number of physical techniques have been successfully used to investigate many of the properties of poly-L-proline, the work reported here has used a combination of osmometry, light scattering, viscometry, and sedimentation studies to reveal a new aspect of this model biopolymer. Experiments were made both on solutions (propionic acid) of poly-L-proline Form I and Form II and on solutions (propionic acid with a threefold dilution of n-propanol) in which Form II was in the process of converting to Form I. The results indicate that an increase in the measured molecular weight accompanies known optical activity and intrinsic viscosity changes which occur as Form II becomes Form I. It appears that the molecular weight determined at infinite dilution for poly-L-proline I is approximately twice that found for poly-L-proline II, and evidence for concentration-promoted aggregation beyond the level of a dimer has been noted in these Form I solutions. Based on these facts and on the information obtained about the particle shapes, it is proposed that this association occurs by a side-to-side binding of two macro-molecules. Discussion is directed toward how these experimental findings can be incorporated into the established concept of the Form I conformation. Light, scattering experiments were also performed on solutions (propionic acid 3 M in LiBr) in which the high-salt, or collapsed, form of poly-L-proline had been generated from either Form II or Form I material. These results showed that the dissolved particles are composed of single chains and are significantly smaller in size than found in solutions of either form and it appears possible that in the collapsed form poly-L-proline might be represented by rodlike macromolecules possessing trans-peptide bonds and a conformation with a relatively small helical pitch.     

Structural and dynamical properties of aqueous suspensions of NaPSS (HPSS) at very low ionic strength

Results on the structural and dynamical properties of aqueous solutions of NaPSS (HPSS) are reported. Most samples of previous measurements, including our own, are contaminated by the presence of (temporal) aggregates. The emphasis of this paper lies on investigations of well purified samples at very low ionic strength where interacting effects are maximum. As previously reported, this can be achieved by pumping the suspension through ion exchange resin by means of a tube-pump, using filters of pore size. Information has been extracted from static and dynamic light scattering and viscosity measurements. A second maximum is observed in the scattering curves versus wavenumber for the first time. It is discussed on the basis of two current models describing the structure of charged macromolecules. The short time dynamics reflects the measured intensity. Detailed viscosity data in comparison of those of rodlike (TMV), slightly flexible so-called fd virus particles (length 880 nm) are used to confirm the interpretation of the light scattering results. The recently observed maximum in the reduced viscosity could be confirmed. Received: 5 May 1997 / Revised: 1 September 1997 / Accepted: 10 November 1997     

Rheology of nanosized hairy grain suspensions

Suspensions of nanosized hairy grains have been prepared by grafting long polydimethylsiloxane chains (molecular weight ) onto silica particles (radius ), dispersed into a good solvent of PDMS. Depending on the particle volume fraction, different rheological behaviors are observed. In the very dilute regime, the suspensions are perfectly stable and the particles behave almost as hard spheres: flow penetration inside the corona is then very weak. When the particle volume fraction goes to the close packing volume fraction, the suspension viscosity does not diverge as for hard spheres due to the increase of flow penetration inside the corona and to corona entanglements. The particles have then the same behavior as polymer stars having an intermediate number of arms (). Finally, in the concentrated regime (), the suspensions form irreversible gels. We shown that this unexpected gelation phenomenon is related to the presence of the silica cores: grafted PDMS chains can adsorb onto different particles and form irreversible bonds between the cores. The viscosity and elastic modulus evolutions during gelation are well described by the scalar percolation model of sol-gel transition. Received 23 March 1998     

Plasmon coupling in binary metal core–satellite assemblies

Controlled plasmon coupling is observed in nanoparticle assemblies composed of 20 nm silver ‘satellite’ nanoparticles tethered by reconfigurable duplex DNA linkers to a 50 nm gold ‘core’ particle. The assemblies incorporate silver nanoparticle–oligonucleotide conjugates prepared using a new conjugation method in which the recognition strand is anchored by a 10 base pair, double strand spacer that presents adjacent 3’- and 5’-thiols to the silver surface. Reconfiguration of the DNA linkers from a compact to an extended state results in decreased core–satellite coupling and a blue-shift in the gold core plasmon resonance. The structural basis for the observed resonance modulation is investigated through simulation of the scattering spectra of binary assemblies with various core–satellite separations. Additional simulations of core–satellite assemblies composed of gold satellite particles bound to silver cores and of assemblies composed entirely of silver particles are used to clarify the dependence of the coupling response on the composition of the components and their distribution within the assembly. Electronic Supplementary Material  The online version of this article () contains supplementary material, which is available to authorized users.     

Counting of particles in aqueous solutions by laser-induced photoacoustic breakdown detection

Laser-induced photoacoustic breakdown detection is applied for the determination of particles in aqueous dispersion. Polystyrene (latex), alumina and thoriasol particles of different sizes are investigated for demonstration. Laser pulses at 500 nm with 28 ns pulse width (FWHM), generated by an excimer ( = 308 nm) pumped dye laser, are focused into aqueous particle dispersions to produce breakdown. The dye laser pulse energy is fixed at a value lower than the breakdown threshold of pure water to initiate a dielectric breakdown only when particles are present in a given focus volume. Focus volume parameters and particle size dependent breakdown thresholds are calculated and the results are compared with data from literature. Dependence of breakdown threshold values on the chemical composition of the particles is determined for polystyrene, alumina and thoriasol particles.