Frank Scheffold

Strong magnetic response of submicron Silicon particles in the infrared

High-permittivity dielectric particles with resonant magnetic properties are being explored as constitutive elements of new metamaterials and devices. Magnetic properties of low-loss dielectric nanoparticles in the visible or infrared are not expected due to intrinsic low refractive index of optical media in these regimes. Here we analyze the dipolar electric and magnetic response of lossless dielectric spheres made of moderate permittivity materials. For low material refractive index (<∼3) there are no sharp resonances due to strong overlapping between different multipole contributions. However, we find that Silicon particles with index of refraction∼3.5 and radius∼200 nm present strong electric and magnetic dipolar resonances in telecom and near-infrared frequencies, (i.e. at wavelengths≈1.2-2 mm) without spectral overlap with quadrupolar and higher order resonances. The light scattered by these Si particles can then be perfectly described by dipolar electric and magnetic fields.

Localization or classical diffusion of light

Wiersma et al. have reported near-infrared optical transmission and coherent backscattering data from strongly scattering slabs of micrometre-sized semiconductor particles. Their optical transmission was much weaker, and the angular shape of their coherent backscattering more rounded, than would be expected for classical diffusive light propagation without absorption. The authors interpret this as evidence for the onset of strong localization of light, but we find that their data can be explained by classical diffusion combined with reasonable amounts of absorption. Moreover, the turbidities of their samples are much lower than those given in ref. 1 and are comparable to samples with classical transport properties. We therefore question whether their samples are in fact close to the proposed localization transition.

Dynamic laser speckle imaging of cerebral blood flow

Laser speckle imaging (LSI) based on the speckle contrast analysis is a simple and robust technique for imaging of heterogeneous dynamics. LSI finds frequent application for dynamical mapping of cerebral blood flow, as it features high spatial and temporal resolution. However, the quantitative interpretation of the acquired data is not straightforward for the common case of a speckle field formed by both by moving and localized scatterers such as blood cells and bone or tissue. Here we present a novel processing scheme, we call dynamic laser speckle imaging (dLSI), that can be used to correctly extract the temporal correlation parameters from the speckle contrast measured in the presence of a static or slow-evolving background. The static light contribution is derived from the measurements by cross-correlating sequential speckle images. In-vivo speckle imaging experiments performed in the rodent brain demonstrate that dLSI leads to improved results. The cerebral hemodynamic response observed through the thinned and intact skull are more pronounced in the dLSI images as compared to the standard speckle contrast analysis. The proposed method also yields benefits with respect to the quality of the speckle images by suppressing contributions of non-uniformly distributed specular reflections.

Depolarization of backscattered linearly polarized light

We formulate a quantitative description of backscattered linearly polarized light with an extended photon diffusion formalism taking explicitly into account the scattering anisotropy parameter g of the medium. From diffusing wave spectroscopy measurements, the characteristic depolarization length for linearly polarized light, lp , is deduced. We investigate the dependence of this length on the scattering anisotropy parameter g spanning an extended range from -1 (backscattering) to 1 (forward scattering). Good agreement is found with Monte Carlo simulations of multiply scattered light.

Optical imaging of the spatiotemporal dynamics of cerebral blood flow and oxidative metabolism in the rat barrel cortex

Oxidative metabolism and cerebral blood flow (CBF) are two of the most important measures in neuroimaging. However, results from concurrent imaging of the two with high spatial and temporal resolution have never been published. We used flavoprotein autofluorescence (AF) and laser speckle imaging (LSI) in the anaesthetized rat to map oxidative metabolism and CBF in response to single vibrissa stimulation. Autofluorescence responses reflecting oxidative metabolism demonstrated a fast increase with a delay of 0.1 s. The sign‐reversed speckle contrast reflecting CBF started to rise with a delay of 0.6 s and reached its maximum 1.4 s after the stimulation offset. The fractional signal changes were 2.0% in AF and 9.7% in LSI. Pixelwise modelling revealed that CBF maps spread over an area up to 2.5‐times larger than metabolic maps. The results provide evidence that the increase in cerebral oxidative metabolism in response to sensory stimulation is considerably faster and more localized than the CBF response. This suggests that future developments in functional imaging concentrating on the metabolic response promise an increased spatial resolution.

Quantitative modeling of laser speckle imaging

We have analyzed the image formation and dynamic properties in laser speckle imaging (LSI) both experimentally and with Monte Carlo simulation. We show for the case of a liquid inclusion that the spatial resolution and the signal itself are both significantly affected by scattering from the turbid environment. Multiple scattering leads to blurring of the dynamic inhomogeneity as detected by LSI. The presence of a nonfluctuating component of scattered light results in the significant increase in the measured image contrast and complicates the estimation of the relaxation time. We present a refined processing scheme that allows a correct estimation of the relaxation time from LSI data.

Linear-to-Branched Micelles Transition: A Rheometry and Diffusing Wave Spectroscopy (DWS) Study

The frequency-dependent shear modulus of aqueous wormlike micellar solutions of cetylpyridinium chloride (CPyCl) and sodium salicylate (NaSal) has been measured over a broad frequency range from 10(-2) to 10(6) rad/s using diffusing wave spectroscopy (DWS) based tracer microrheology as well as mechanical techniques including rotational rheometry and oscillatory squeeze flow. Good agreement between mechanical and optical techniques is found in the frequency range from 10(-1) to 10(5) rad/s (Willenbacher, N.; Oelschlaeger, C.; Schopferer, M.; Fischer, P.; Cardinaux, F.; Scheffold, F. Phys. Rev. Lett. 2007, 99 (6), 068302). At intermediate frequencies between 10 and 10(4) rad/s, squeeze flow provides most accurate data and is used to determine the plateau modulus G(0), which is related to the cross-link density or mesh size of the entanglement network, as well as the scission energy E(sciss), which is deduced from the temperature dependence of the shear moduli in the plateau zone. In the frequency range above 10(4) rad/s, DWS including a new inertia correction is most reliable and is used to determine the persistence length l(p). The system CPyCl/NaSal is known to exhibit two maxima in zero-shear viscosity and terminal relaxation time as the salt/surfactant ratio R is varied (Rehage, H.; Hoffman, H. J. Phys. Chem. 1988, 92 (16), 4712-4719). The first maximum is attributed to a transition from linear to branched micelles (Lequeux, F. Europhys. Lett. 1992, 19 (8), 675-681), and the second one is accompanied by a charge reversal due to strongly binding counterions. Here, we discuss the variation of G(0), E(sciss), and l(p) with salt/surfactant ratio R at constant surfactant concentration of 100 mM CPyCl. G(0) increases at the linear-to-branched micelles transition, and this is attributed to the additional contribution of branching points to the cross-link density. E(sciss) exhibits two maxima analogous to the zero-shear viscosity, which can be understood in terms of the variation of micellar length and variation of the amount of branched micelles and contour length between branching points consistent with the results of a comprehensive cryo-transmission electron microscopy (TEM) study (Abezgauz, L.; Ramon, O.; Danino, D. Department of Biotechnology and Food Engineering, Technion, Haifa, Israel. European Colloid and Interface Society, Geneva, 2007). The persistence length decreases with increasing R. This decrease is stronger than expected from the decrease of Debye length according to the Odijk-Skolnick-Fixman (OSF) theory and is attributed to the penetration of salicylate ions into the micelles; the linear-to-branched transition obviously does not have an effect on l(p).

Laser speckle imaging with an active noise reduction scheme

We present an optical scheme to actively suppress statistical noise in Laser Speckle Imaging (LSI). This is achieved by illuminating the object surface through a diffuser. Slow rotation of the diffuser leads to statistically independent surface speckles on time scales that can be selected by the rotation speed. Active suppression of statistical noise is achieved by accumulating data over time. We present experimental data on speckle contrast and noise for a dynamically homogenous and a heterogeneous object made from Teflon. We show experimentally that for our scheme spatial and temporal averaging provide the same statistical weight to reduce the noise in LSI: The standard deviation of the speckle contrast value scales with the effective number N of independent speckle as 1/ radicalN.

Brushlike interactions between thermoresponsive microgel particles.

Using a simplified microstructural picture we show that interactions between thermosensitive microgel particles can be described by a polymer brushlike corona decorating the dense core. The softness of the potential is set by the relative thickness L0 of the compliant corona with respect to the overall size of the swollen particle R. The elastic modulus in quenched solid phases derived from the potential is found to be in excellent agreement with diffusing wave spectroscopy data and mechanical rheometry. Our model thus provides design rules for the microgel architecture and opens a route to tailor rheological properties of pasty materials.

Thermoresponsive hybrid microgel particles with intrinsic optical and magnetic anisotropy

We describe the synthesis of thermoresponsive, magnetic, optically anisotropic and orientable colloidal particles based on poly(N-isopropylacrylamide) hybrid microgels (PNIPAMs) with an embedded ellipsoidal hematite (α-Fe2O3) core. Our ability to orient the particles with a magnetic field is demonstrated by small angle X-ray scattering and by optical polarization microscopy.