Mie scattering efficiency of a large spherical particle embedded in an absorbing medium

The Mie scattering calculations are usually performed for non-absorbing spherical particles embedded in a non-absorbing medium. We consider a case of an absorbing sphere placed in an absorbing medium. We find, by numerical calculation for large size parameter of the order of 10⁴, that the scattering efficiency of a spherical particle in an absorbing medium approaches the reflectance of a plane surface at perpendicular incidence.     

Lorenz-Mie Theory for Spheres Immersed in an absorbing host medium

Light scattering by particles is often used to determine velocities or concentrations of particles in gaseous or liquid streams. Within the Lorenz-Mie theory, light scattering is well understood both for a single compact spherical particle and a single multilayered particle in a non-absorbing surrounding medium. However, in some cases of practical importance the Lorenz-Mie theory in its present form may fail to describe the scattering because the host medium is absorbing (e.g. water droplets in oil). In this case, a new treatment of the scattering theory is required. In previous work, solutions were obtained in the far-field of the scattering sphere. In this paper, a rigorous solution is derived from the calculation of the total absorption rate of the particle in the host medium, which is valid for all distances from the surface of the encapsulated particle. It is shown that it is necessary to consider finite sizes R of the integrating sphere when dealing with absorbing host media. Cross-sections are defined which are characteristic quantities not only for the particle, depending on the size of a conceptual sphere around the scatterer and the imaginary part of the refractive index of the host medium. The results obtained are discussed for the case of non-absorbing host media and in the far-field approximation. Some numerical examples are given which are also related to experimental results.     

Optical extinction of an assembly of spherical particles in an absorbing medium: Application to silver clusters in absorbing organic materials

The theory presented by Gerardy and Ausloos for the calculation of the linear optical response of aggregates of spherical particles is analytically continued for absorbing embedding media. The method is based on the calculation of the extinction rate by a single particle embedded in an absorbing matrix. Explicit expressions for the extinction and scattering cross-sections are given. The method is applied to calculate the energy losses in several organic matrices with embedded silver clusters. Comparison with experimental data shows a very good agreement. Received: 21 December 1998     

Radiative properties of densely packed spheres in semitransparent media: A new geometric optics approach

This contribution presents a new Ray-tracing method for calculating effective radiative properties of densely packed spheres in non-absorbing or semitransparent host medium. The method is restricted to the geometric optic objects and neglects the wave effects. The effective radiative properties such as the absorption and scattering coefficients, and phase function are retrieved from the calculation of mean-free paths of scattering and absorption, and the angular scattering probability of radiation propagating in the dispersed medium. The model accounts for the two geometric effects called here as non-point scattering and ray transportation effects. The successful comparison of the current model with data of radiative properties and transmittances of particle beds in a non-absorbing medium reported in the literature confirm its suitability. It is shown that: (i) for opaque or absorbing particles (not systematically opaque), the non-point scattering is the dominant geometric effects whereas both non-point scattering and ray transportation effects occur for weakly absorbing and transparent particles. In the later cases, these two geometric effects oppose and may cancel out. This may explain why the Independent scattering theory works well for packed of quasi-transparent particles; (ii) the non-point scattering and ray transportation effects can be captured through the scattering and absorption coefficients while using the classical form of phase function. This enables using the standard radiative transfer equation (RTE); (iii) the surrounding medium absorption can be accounted for without any homogenization rule. It contributes to increasing the effective absorption coefficient of the composite medium as expected but, at the same time, it reduces the particle extinction; and (iv) the current transfer calculation predicts remarkably the results of direct Monte Carlo (MC) simulation. This study tends therefore to confirm that the RTE can be applied to densely packed media by using effective radiative properties.     

The influence of surface forces on shear-induced tracer diffusion in mono and bidisperse suspensions

The shear-induced self-diffusivity of tracer particles of radius a _t = λa in a suspension of particles having a radius, a , is calculated by Stokesian dynamics for different values of the size ratio, λ , both in 2 and 3 dimensions in the binary-collision regime. The self-diffusion is found to decrease strongly when the size ratio becomes quite different from unity. On the other hand, for the same average distance of contact between two spheres, the presence of a soft force always increases greatly the diffusion compared to the effect of a hard shell which is used to model the roughness. This is particularly true for tracer particles smaller than the bath particles, where the shear-induced diffusion can be increased by many order of magnitudes in the presence of a soft force. For suspensions of monodisperse particles we show that, for low volume fraction, the diffusion coefficient is much smaller than the one predicted by the binary collision model, due to the existence of a layered structure. On the contrary at higher volume fraction, many-body collisions strongly enhance the diffusion and it appears that the value of the diffusion is quite sensitive to the presence of clusters of particles which are themselves determined by the range of interparticle forces.     

Diffusion of adsorbates on random alloy surfaces

In this work the diffusion of non-interacting adsorbates on a random AB alloy surface is considered. For this purpose a simple cubic (sc), body-centered cubic (bcc) or face-centered cubic (fcc) auxiliary metal lattice is introduced. The auxiliary lattice is truncated parallel to its (100) plane in such a way that the fourfold hollow positions of the metal surface form a regular net of adsorption sites with square symmetry. The adsorption energy of each adsorption site is determined by its own environment, i.e. by the numbers of direct A or B neighbors. The Monte-Carlo method has been utilized to simulate surface diffusion of adsorbates on such energetically heterogeneous alloy surfaces and to calculate the tracer, jump and chemical diffusion coefficients. The chemical diffusion coefficient was calculated via two different approaches: the fluctuation and the Kubo-Green method. The influence of energetical heterogeneities on the surface diffusion is largely pronounced at low temperatures and low surface coverages, where most of the adatoms are trapped by deep adsorption sites. It was found that at low temperatures the sequential occupation of the different types of adsorption sites can be observed. Received: 24 October 1997 / Accepted: 17 December 1997     

Ground states versus low-temperature equilibria in random field Ising chains

Random walk arguments and exact numerical computations are used to study one-dimensional random field chains. The ground state structure is described with absorbing and non-absorbing random walk excursions. At low temperatures, the local magnetization follows the ground state except at regions where a local random field fluctuation makes thermal excitations easier. This is explained by the random walk picture, implying that the magnetization lengthscale is a product of the domain size and the thermal excitation scale. Received 16 October 2000 and Received in final form 7 June 2001     

X-ray dichroism in biaxial gyrotropic media: Differential absorption and fluorescence excitation spectra

The differential absorption and the differential change in the polarization state of an X-ray beam propagating inside a gyrotropic crystal are described using a Müller matrix, the 16 elements of which are related to the anisotropic components of the multipolar polarizability tensors at the absorbing site. Analytical expressions are given up to third order for X-ray linear and circular dichroism, X-ray optical rotation and X-ray circular polarimetry in transmission. The same formalism is extended to discuss Fluorescence detected dichroism spectra with or without polarization analysis of the fluorescence. Fluorescence detected dichroism is strictly proportional to dichroism measured in the transmission geometry only for uniaxial crystals. In biaxial crystals, the tiny effects of X-ray gyrotropy are swamped by large linear dichroism signals due to the imperfect polarization transfer function of Bragg monochromators. Second order effects should also be taken into consideration. Our general formulation of linear and circular dichroism includes terms of odd parity with respect to the action of the time reversal operator: such terms cannot contribute to natural dichroism but can be activated by a magnetic field. The terms responsible for X-ray magnetic circular dichroism are well known but non-reciprocal X-ray gyrotropy effects are also predicted in magnetic crystals of appropriate symmetry. Received 3 March 1999     

Optical properties of gold metal clusters: A time-dependent local-density-approximation investigation

The optical response of free and matrix-embedded gold metal clusters Au_N is investigated in the framework of the time-dependent local-density-approximation (TDLDA). The characteristics of the surface plasmon resonance are carefully analyzed as a function of the model parameters and the particle radius. The strong influence of the frequency-dependence of the 5d core-electron dielectric function in the vicinity of the interband threshold is emphasized. The size evolution of the Mie-frequency in free gold clusters exhibits a noticeable blue-shift trend as the particle size decreases, much stronger than in silver clusters. The width and shape of the resonance, essentially ruled by the decay via the interband transitions, are found closely correlated to the imaginary component of the core-electron dielectric function. In presence of a surrounding matrix the blue-shift trend is largely rubbed out. Agreement with recent experimental results on size-selected gold clusters embedded in an alumina matrix may be achieved by taking into account the porosity effects at the metal/matrix interface. The comparison with the predictions of classical models is also provided. Received: 9 March 1998 / Revised: 5 June 1998 / Accepted: 3 July 1998     

Scattering from solutions of star polymers

We study the scattering intensity of dilute and semi-dilute solutions of star polymers. The star conformation is described by a model introduced by Daoud and Cotton. In this model, a single star is regarded as a spherical region of a semi-dilute polymer solution with a local, position dependent screening length. For high enough concentrations, the outer sections of the arms overlap and build a semi-dilute solution (a sea of blobs) where the inner parts of the actual stars are embedded. The scattering function is evaluated following a method introduced by Auvray and de Gennes. In the dilute regime there are three regions in the scattering function: the Guinier region (low wave vectors, ) from where the radius of the star can be extracted; the intermediate region () that carries the signature of the form factor of a star with f arms: ; and a high wavevector zone () where the local swollen structure of the polymers gives rise to the usual q ^-5/3 decay. In the semi-dilute regime the different stars interact strongly, and the scattered intensity acquires two new features: a liquid peak that develops at a reciprocal position corresponding to the star-star distances; and a new large wavevector contribution of the form q ^-5/3 originating from the sea of blobs. Received: 3 September 1997 / Revised: 13 January 1988 / Accepted: 31 March 1998     

Exact propagator of the Fokker-Planck equation with a space-dependent diffusion coefficient and a time-dependent mean-reverting force

We have investigated the algebraic structure of the Fokker-Planck equation with a variable diffusion coefficient and a time-dependent mean-reverting force. Such a model could be useful to study the general problem of a Brownian walker with a space-dependent diffusion coefficient. We also show that this model is related to the Fokker-Planck equation with a constant diffusion coefficient and a time-dependent anharmonic potential of the form V(x, t) = ?a(t)x ² + b ln x, which has been widely applied to model different physical and biological phenomena, e.g. the study of neuron models and stochastic resonance in monostable nonlinear oscillators. Using the Lie algebraic approach we have derived the exact diffusion propagators for the Fokker-Planck equations associated with different boundary conditions, namely (i) the case of a single absorbing barrier, and (ii) the case of two absorbing barriers. These exact diffusion propagators enable us to study the time evolution of the corresponding stochastic systems. Received 23 October 2001 and Received in final form 24 December 2001     

Structure and size distribution of percolating clusters. Comparison with gelling systems

Dynamic properties of Brownian particles immersed in a periodic potential with two barriers V₁ and V₂ (symmetric bistable potential) are studied by using the Fokker-Planck equation which we solve numerically by the matrix continued fraction method. This study will therefore serve to demonstrate the influence of this form of potential, which is of great interest for superionic conductors and for many other solid systems, on the diffusion process. Thus, we have calculated the full width at half maximum (FWHM) ) of the quasi-elastic line of the dynamic structure factor, for a large range of values of the wave-vectors q. Our results show clearly that, by varying the ratio of the barriers strictly between and 1, the Fokker-Planck equation describes a diffusive process which has some characteristic of jump and liquid-like regimes. While in the limit cases, i.e. when tends to or 1, the diffusion process can be described only by a simple jump motion. However, the jump-lengths corresponding to each limit case are not equal. In general the change of the ratio is found to have a significant effect on the character of the diffusive motion. We have also performed Fokker-Planck dynamics calculations of the diffusion coefficient in a bistable potential. We have found a good agreement between numerical calculations and analytical approximation results obtained in the high friction limit. Received 25 May 1998 and Received in final form 15 November 1998     

Field Effects in Condensed Media on Polarized Absorption

The existence of anisotropic local field perturbation on electronic absorption is proved by non-zero linear dichroism of isotropic chromophores (Mo(CO)₆) in anisotropic environment. Two sources of such effects are possible: a) perturbation of the electronic energy levels in the chromophore by the static electric solvent field (= Stark effect) or, in case of anisotropic polarizable or dipolar molecules, similar effects involving molecular orientation, and b) dielectric effects on the effective radiation field. The latter effect was considered by various models: The Lorentz field model predicts an effect with wrong sign, it also yields too large a magitude if the anisotropy of the field is considered. If no local field correction is made and the anisotropy only operates in the radiation intensity a result more in agreement with experiment is obtained. By using the Onsager-Böttcher model one may take into account specific properties of the absorbing molecule, like anisotropy in α/r³ where α is its polarizability and r its Onsager radius.     

Localisation and damping in resonators with complex geometry

Based on numerical studies, we show that localisation is a common phenomenon in resonators exhibiting some kind of geometrical complexity. In two-dimensional (2d) shallow cavities of irregular shape, localisation effects are due to spatial decoherence in a major fraction of the volume. In 2d shallow cavities of regular geometry with embedded absorbing material of irregular shape, one observes the appearance of eigenmodes localised in both, the absorbing and the non-absorbing media. Those modes are thought to be responsible for increased dissipation. These results may be a hint to understand why natural or practical systems absorbing wave energy are found, or built, with complex geometry.     

Models of environmental effects on anion polarizability

This paper deals with three different approaches to the representation of environmental effects on anion polarizability in cubic crystals of the stoichiometry MX, where M is an alkali metal and X is a halogen. Ab initio embedded cluster calculations of the variation in anion polarizability with pressure in a fixed crystal type are presented and compared with experiment. The results are then used in a scaled ab initio model used to predict further values for the pressure dependence of the in-crystal anion polarizability. This scaled model is compared with a fully empirical ‘universal’ model due to Batana et al. based on polarizability change with ionic radius [1997, Molec. Phys., 92, 1029]. The assumptions of the two models differ substantially and the central purpose of this paper is to contrast these differences and highlight their consequences for prediction. Although the empirical model typically overestimates the experimental pressure derivatives, and the ab initio calculations somewhat underestimate them, it is shown that the assumption of incompressible cations in the scaled ab initio-derived model has a firmer physical basis than the empirical picture in which all ions are compressible.     

Some calculations of temperature profiles in thin films with laser heating

We present some calculations of heat flow in an absorbing film deposited on a non-absorbing substrate. The energy source is a Gaussian laser beam. We analyse the effects of film thickness, thermal conductivity, spot radius and forced cooling on the temperature profile and, in a special case, the time evolution of that profile. The emphasis is on applications in optical bistability.     

Single layer homogeneous model for surface roughness by polarized light scattering

In this paper a homogeneous single layer model for surface roughness by polarized light has been developed. It has been shown that the reflectance change in non-absorbing layer is directly proportional to the refractive index of the ambient and substrate media for s polarization but inversely proportional to the p polarization and it is directly proportional to the square of the thickness of the layer for both the polarization. In an absorbing layer, it has been shown that the thickness of the layer is equal to the twice of surface roughness of the single layer identical system for s polarization but it is ratio of twice of surface roughness to the square of refractive index of thin film for p polarization. The extinction coefficient of the layer is directly proportional to the thickness of that layer for both the polarization. The consequence of the scattered light on the specular reflectance and transmittance for oblique incidence shows that there is reduction in reflectance (in both non-absorbing and absorbing cases) and transmittance (in the absorbing case for p polarization only), due to roughness on the surface under the Drude effective-medium approximation. Thus such an absorbing layer provides a valid model for the effect of scatter on the transmittance for p polarization only.     

Effect of shear on an onion texture

Lamellar systems are self-assemblies of surfactant molecules forming planar bilayers separated by layers of solvent. At sufficiently high shear rates, they are known to form spherical objects often referred to as onions. In this paper, we are concerned with the effect of shear on those multi-lamellar vesicles. We measure solvent diffusion by nuclear magnetic resonance (NMR) using a method which is sensitive to the time dependence of mean-squared displacements. This method, combined with NMR velocimetry, allows us to infer onion structure as a function of shear rate, identifying different regimes in which local viscosity is related to the onion size. The role of slip is examined and the stress dependence of wall slip velocities is determined.     

Metastable states of spin glasses on random thin graphs

In this paper we calculate the mean number of metastable states for spin glasses on so called random thin graphs with couplings taken from a symmetric binary distribution . Thin graphs are graphs where the local connectivity of each site is fixed to some value c. As in totally connected mean field models we find that the number of metastable states increases exponentially with the system size. Furthermore we find that the average number of metastable states decreases as c in agreement with previous studies showing that finite connectivity corrections of order 1/c increase the number of metastable states with respect to the totally connected mean field limit. We also prove that the average number of metastable states in the limit is finite and converges to the average number of metastable states in the Sherrington-Kirkpatrick model. An annealed calculation for the number of metastable states of energy E is also carried out giving a lower bound on the ground state energy of these spin glasses. For small c one may obtain analytic expressions for . Received 14 October 1999 and Received in final form 14 December 1999