Developing Scattering Morphology Resolved Total Internal Reflection Microscopy (SMR-TIRM) for Orientation Detection of Colloidal Ellipsoids.

Micrometer scale colloidal particles experiencing ∼kT scale interactions and suspended in a fluid are relevant to a broad spectrum of applications. Often, colloidal particles are anisotropic, either by design or by nature. Yet, there are few techniques by which ∼kT scale interactions of anisotropic particles can be measured. Herein, we present the initial development of scattering morphology resolved total internal reflection microscopy (SMR-TIRM). The hypothesis of this work is that the morphology of light scattered by an anisotropic particle from an evanescent wave is a sensitive function of particle orientation. This hypothesis was tested with experiments and simulations mapping the scattered light from colloidal ellipsoids at systemically varied orientations. Scattering morphologies were first fitted with a two-dimensional (2D) Gaussian surface. The fitted morphology was parameterized by the morphology's orientation angle Mϕ and aspect ratio MAR. Data from both experiments and simulations show Mϕ to be a function of the particle azimuthal angle, while MAR was a sensitive function of the polar angle. This analysis shows that both azimuthal and polar angles of a colloidal ellipsoid could be resolved from scattering morphology as well or better than using bright-field microscopy. The integrated scattering intensity, which will be used for determining the separation distance, was also found to be a sensitive function of particle orientation. A procedure for interpreting these confounding effects was developed that in principle would uniquely determine the separation distance, the azimuthal angle, and the polar angle. Tracking these three quantities is necessary for calculating the potential energy landscape sampled by a colloidal ellipsoid.

Numerical method for analyzing the near-field enhancement of nonspherical dielectric-core metallic-shell particles accounting for the nonlocal dispersion.

Over the last few decades, dielectric core and metallic plasmonic shell (Die@Me) nanoparticles have found a wide variety of applications. The trend to reduce the thickness of the metallic coating requires to account for the influence of the nonlocal dispersion on the spectral response of such nanoparticles. In this paper, we use the discrete sources method and the generalized nonlocal optical response model to describe the nonlocality within the plasmonic metal shell. We found that the variation of the plasmonic shell thickness and the elongation of the nonspherical core-shell particle can enlarge the near-field enhancement and the absorption cross section by an order of magnitude. Besides, we show that the nonlocal dispersion can decrease the field enhancement in the wavelength domain up to 2.5 times with a small blue-shift of about 5 nm.

Electromagnetic scattering by discrete random media. IV: Coherent backscattering.

The problem of backscattering of light by a discrete random medium illuminated by an obliquely incident plane electromagnetic wave is considered. The analysis is performed in a linear-polarization basis and includes (i) a complete derivation of the cross reflection matrix for a layer with densely and sparsely distributed particles, (ii) the design of an approximate method for computing the ladder and cross reflection matrices in the case of a semi-infinite medium with a sparse distribution of particles, (iii) the derivation of the relations between the elements of the ladder and cross reflection matrices in the exact backscattering direction for dense and sparse media, and (iv) the development of practical algorithms for solving the underlying integral equations by the method of Picard iterations and the discrete ordinate method. Simulation results for particles with large size parameters are also presented.

An overview of methods for deriving the radiative transfer theory from the Maxwell equations. II: Approach based on the Dyson and Bethe-Salpeter equations.

In this paper, the vector radiative transfer equation is derived by means of the vector integral Foldy equations describing the electromagnetic scattering by a group of particles. By Assuming that in a discrete random medium the positions of the particles are statistically independent and by applying the Twersky approximation to the order-of-scattering expansion of the total field, we derive the Dyson equation for the coherent field and the ladder approximated Bethe-Salpeter equation for the dyadic correlation function. Then, under the far-field assumption for sparsely distributed particles, the Dyson equation is reduced to the Foldy integral equation for the coherent field, while the iterated solution of the Bethe-Salpeter equation ultimately yields the vector radiative transfer equation.

Electromagnetic scattering by discrete random media. II: The coherent field.

The computation of the coherent field in the case of a plane electromagnetic wave obliquely incident on a discrete random layer with non-scattering boundaries is addressed. For dense media, the analysis is based on a special-form solution for the conditional configuration-averaged exciting field coefficients, and is restricted to the computation of the so-called zeroth-order fields without a special treatment of the boundary regions. In this setting, we calculate the coherent fields reflected and transmitted by the layer, and the coherent field inside the layer. We found that these fields are analytically equivalent to plane electromagnetic waves, and investigated the fulfillment of the boundary conditions for the electric fields at the layer interfaces. The results are then particularized to the cases of normal incidence and a semi-infinite discrete random medium. For sparsely distributed particles, we present a self-consistent derivation of the coherent field and discuss the Twersky and Foldy approximations.

Radiative transfer in a discrete random medium adjacent to a half-space with a rough interface.

For a macroscopically plane-parallel discrete random medium, the boundary conditions for the specific coherency dyadic at a rough interface are derived. The derivation is based on a modification of the Twersky approximation for a scattering system consisting of a group of particles and the rough surface, and reduces to the solution of the scattering problem for a rough surface illuminated by a plane electromagnetic wave propagating in a discrete random medium with non-scattering boundaries. In a matrix-form setting, the boundary conditions for the specific coherency dyadic imply the boundary conditions for specific intensity column vectors which in turn, yield the expressions for the reflection and transmission matrices. The derived expressions are shown to be identical to those obtained by applying a phenomenological approach based on a facet model to the solution of the scattering problem for a rough surface illuminated by a plane electromagnetic wave.