Fractal and Polarization Properties of Light Scattering Using Microcrystalline Pharmaceutical Aggregates.

Fractal and polarization analysis of diffusively scattered light is applied to determine the complex relationship between fractal dimension of structural morphology and concentration of chemically active ingredients in two pharmaceutical mixture systems including a series of binary mixtures of acetaminophen in lactose and three multicomponent blends with a proprietary active ingredient. A robust approach is proposed to identify and filter out multiple- and single-scattering components of scattering indicatrix. The fractal dimension extracted from scattering field reveals complex structural details of the sample, showing strong dependence on low-dose drug concentration in the blend. Low-angle diffraction shows optical "halo" patterns near the angle of specular reflection caused by light refraction in microcrystalline aggregates. Angular measurements of diffuse reflection demonstrate noticeable dependence of Brewster's angle on drug concentration. It is shown that the acetaminophen microcrystals produce scattered light depolarization due to their optical birefringence. The light scattering measurement protocol developed for diffusively scattered light by microcrystalline pharmaceutical compositions provides a novel approach for the pattern recognition, analysis and classification of materials with a low concentration of active chemical ingredients.

Large non-thermal contribution to picosecond strain pulse generation using the photo-induced phase transition in VO2.

Picosecond strain pulses are a versatile tool for investigation of mechanical properties of meso- and nano-scale objects with high temporal and spatial resolutions. Generation of such pulses is traditionally realized via ultrafast laser excitation of a light-to-strain transducer involving thermoelastic, deformation potential, or inverse piezoelectric effects. These approaches unavoidably lead to heat dissipation and a temperature rise, which can modify delicate specimens, like biological tissues, and ultimately destroy the transducer itself limiting the amplitude of generated picosecond strain. Here we propose a non-thermal mechanism for generating picosecond strain pulses via ultrafast photo-induced first-order phase transitions (PIPTs). We perform experiments on vanadium dioxide VO2 films, which exhibit a first-order PIPT accompanied by a lattice change. We demonstrate that during femtosecond optical excitation of VO2 the PIPT alone contributes to ultrafast expansion of this material as large as 0.45%, which is not accompanied by heat dissipation, and, for excitation density of 8 mJ cm-2, exceeds the contribution from thermoelastic effect by a factor of five.

Photoinduced surface plasmon switching at VO2/Au interface.

Angle-resolved reflection, light scattering and ultrafast pump-probe spectroscopy combined with a surface plasmon-polariton (SPP) resonance technique in attenuated total reflection geometry was used to investigate the light-induced plasmonic switching in a photorefractive VO2/Au hybrid structure. Measurements of SPP scattering and reflection shows that the optically-induced formation of metallic state in a vanadium dioxide layer deposited on a gold film significantly alters the electromagnetic field enhancement and SPP propagation length at the VO2/Au interface. The ultrafast optical manipulation of SPP resonance is shown on a picosecond timescale. Obtained results demonstrate high potential of photorefractive vanadium oxides as efficient plasmonic modulating materials for ultrafast optoelectronic devices.

Ultrafast Excited-State Dynamics of V_{3}O_{5} as a Signature of a Photoinduced Insulator-Metal Phase Transition.

The ultrafast elastic light scattering technique is applied to reveal the strong nonlinearity of V_{3}O_{5} associated with a photoinduced insulator-metal phase transition. Observation of time-domain relaxation dynamics suggests several stages of structural transition. We discuss the nonequilibrium processes in V_{3}O_{5} in terms of photoinduced melting of a polaronic Wigner crystal, coalescence of V-O octahedra, and photogeneration of acoustical phonons in the low-T and high-T phases of V_{3}O_{5}. A molecular dynamics computation supports experimentally observed stages of V_{3}O_{5} relaxation dynamics.

Super-resolution in diffractive imaging from hemispherical elastic light scattering data.

Angle-resolved hemispherical elastic light scattering techniques have been used to reconstruct the surface profile of two-dimensional photonic crystals with submicron resolution and metrological precision. Iterative algorithms permit subsequent calculation of a surface autocorrelation function with additional numerical approximation of the power spectrum and then yield final reconstruction of the surface shape. The proposed method enables filtering out unwanted scattering background, precluding the convergence of phase-retrieval algorithms. The estimation of higher harmonics in the power spectrum provides the reconstruction of a realistic surface achieving subwavelength resolution.

Effect of Shear Applied During a Pharmaceutical Process on Near Infrared Spectra.

This study describes changes observed in the near-infrared (NIR) diffuse reflectance (DR) spectra of pharmaceutical tablets after these tablets were subjected to different levels of strain (exposure to shear) during the mixing process. Powder shearing is important in the mixing of powders that are cohesive. Shear stress is created in a system by moving one surface over another causing displacements in the direction of the moving surface and is part of the mixing dynamics of particulates in many industries including the pharmaceutical industry. In continuous mixing, shear strain is developed within the process when powder particles are in constant movement and can affect the quality attributes of the final product such as dissolution. These changes in the NIR spectra could affect results obtained from NIR calibration models. The aim of the study was to understand changes in the NIR diffuse reflectance spectra that can be associated with different levels of strain developed during blend shearing of laboratory samples. Shear was applied using a Couette cell and tablets were produced using a tablet press emulator. Tablets with different shear levels were measured using NIR spectroscopy in the diffuse reflectance mode. The NIR spectra were baseline corrected to maintain the scattering effect associated with the physical properties of the tablet surface. Principal component analysis was used to establish the principal sources of variation within the samples. The angular dependence of elastic light scattering shows that the shear treatment reduces the size of particles and produces their uniform and highly isotropic distribution. Tablet compaction further reduces the diffuse component of scattering due to realignment of particles.

Photoinduced insulator-to-metal transition and surface statistics of VO2 monitored by elastic light scattering.

Measurements of ultrafast light scattering within a hemisphere are performed for statistical analysis of nonequilibrium processes in VO2 epitaxial film. A Gerchberg-Saxton error reduction algorithm is applied for accurate calculation of a surface autocorrelation function from light scattering data and for partial reconstruction of a power spectral density function. Upon ultrafast photoinduced phase transition of VO2, the elastic light scattering reveals anisotropic grain-size-dependent dynamics. It was found that the transition rate depends on the optical absorption and orientation of VO2 grains with respect to polarization of the pump pulse. An observed stepwise evolution of surface autocorrelation length and transient anisotropy of the scattering field presumably originates from complex multistage transformation of VO2 lattice on a subpicosecond time scale.