Ignatz M. de Schepper

Real-space interpretation of spin-echo small-angle neutron scattering

Spin-echo small-angle neutron scattering (SESANS) is a novel real-space scattering technique. SESANS measures a correlation-like function G(Z), the meaning of which was unknown until now. Here a direct real-space interpretation of G(Z) through the particle scattering density and pair correlation function is given. One-dimensional and two-dimensional SESANS are compared. The case of non-interacting particles is considered in detail with an explicit geometrical interpretation. General methods for the calculation of structural parameters, such as the total scattering length and the radius of gyration, are developed. Analytical expressions of G(Z) for non-interacting solid spheres, hollow spheres and Gaussian coils are derived. The case of solid spheres is compared with experimental data.

Analysis of spin‐echo small‐angle neutron scattering measurements

Spin-echo small-angle neutron scattering (SESANS) is, in contrast to conventional small-angle neutron scattering (SANS), a real-space technique. SESANS measures the projection of the density–density correlation function of a sample, rather than, as in SANS, its Fourier transform. This paper introduces a toolkit for interpretion and analysis of a SESANS measurement. Models that are used in SANS are discussed and translated into a SESANS formalism. These models can be used to analyse and fit the data obtained by SESANS. Dilute, concentrated, random, fractal and anisotropic density distributions are considered. Numerical methods used to calculate the projection from numerical data are presented, either by using Fourier transformation or via the real-space pair correlation function.

Cage diffusion in liquid mercury

We present inelastic neutron scattering measurements on liquid mercury at room temperature for wave numbers q in the range 0.3 <q<7.0 A(-1). We find that the energy half width of the incoherent part of the dynamic structure factor S(q,E) is determined by a self-diffusion process. The half width of the coherent part of S(q,E) shows the characteristic behavior expected for a cage diffusion process. We also show that the response function at small wave numbers exhibits a quasielastic mode with a time scale characteristic of cage diffusion, however, its intensity is larger by an order of magnitude than what would be expected for cage diffusion. We speculate on a scenario in which the intensity of the cage diffusion mode at small wave numbers is amplified through a valence fluctuation mechanism.

Angular and time resolution of neutron time of flight spectrometers

Abstract We show that the angular resolution Δφ and time resolution Δt of neutron time-of-flight spectrometers can be determined accurately by measuring the scattering spectrum of superfluid 4He at low temperature. The method is used to determine Δφ and Δt of the IRIS spectrometer at ISIS (UK), yielding the values (FWHM) Δφ=0.118 rad (6.8°) and Δt=212 μs, and to reinterpret the results of Blagoveshchenskii et al., showing that their measured linewidths for superfluid 4He can be ascribed solely to the effect of the angular resolution of their time-of-flight spectrometer.

Milk gelation studied with small angle neutron scattering techniques and Monte Carlo simulations.

The sol-gel transition of fat-free milk by acidification was studied with neutron scattering experiments and Monte Carlo simulations. Spin-echo small angle neutron scattering (SESANS) and ultrasmall angle neutron scattering (USANS) experiments were performed to measure the static structure of milk and yogurt, as well as the aggregation kinetics. Colloidal gelation was simulated from a reaction limited domain (RLCA) to the diffusion limited regime (DLCA) as cluster-cluster aggregation of adhesive, hard spheres on a three-dimensional lattice. Comparisons were drawn between experimental and numerical correlation functions. Milk was modeled as a suspension of casein micelles in water, and its structure was described with a dilute system of solid spheres with a log-normal distribution of sizes. The structure and formation of yogurt were described with a self-affine model, used for systems containing heterogeneities with a wide range of sizes. Simulation speed was increased by 1 order-of-magnitude using a new algorithm to eliminate dead time. Observations by SESANS and USANS of milk particle sizes and yogurt length scales were consistent and agreed well with literature. Kinetic USANS data yielded reliable information about the growth of typical length scale during aggregation. The simulation model predicted the measurement data qualitatively best staying close to the RLCA regime until large structures had formed. Correlation lengths were in good quantitative agreement, but longest simulated length scales were a of factor 2(1)/(2) below experimental findings. We conclude that small, mobile aggregates are formed during the first 3 h, mostly influencing the dimensionality of the system and that large, inert structures are formed from 2 up to 8 h, which determine the typical length scale.

Structural slowing down and depolarized light spectra in dense noble gas fluids

We argue that the narrowing at increasing densities of the light spectra obtained for Ar and Kr by An et al.(J. Chem. Phys., 1979, 70, 4626) using depolarized interaction-induced light scattering techniques is due to the slowing down of structural relaxation in dense fluids which is observed in neutron scattering experiments on He, Kr, Ar and Rb.

Spin-Echo Small Angle Neutron Scattering analysis of liposomes and bacteria

Two types of liposomes, commonly used in drug delivery studies, and E. coli bacteria, all prepared in H2O, were resuspended in D2O and measured with Small Angle Spin-Echo Neutron Scattering (SESANS). Modeling was performed using correlation functions for solid spheres and hollow spheres. The signal strength and curve shape were more indicative of hollow particles, indicating that the H2O-D2O exchange occurred too fast to be observed with the available time resolution. Fitting the particle diameter and membrane thickness of the hollow sphere model to the data, gave results which were in good agreement with Dynamic Light Scattering (DLS) data and literature, showing as a proof-of-principle that SESANS is able to investigate such systems. SESANS may become a good alternative to conventional tritium studies or a tool with which to study intracellular vesicle transport phenomena, with possible in vivo applications. Calculations show that a substantial change in numbers of a mixed system of small and large biological particles should be observable. A possible application is the destruction by external means of great numbers of liposomes in the presence of tumor cells for triggered drug release in cancer treatment. Since SESANS is both non-invasive and non-destructive and can handle relatively thick samples, it could be a useful addition to more conventional techniques.

Spin-echo small-angle neutron scattering (SESANS) measurements of needle-like crystallites of gelator compounds

From dibenzoyl cystine, a low molecular weight gelator, we have prepared needle shaped crystals at relatively high concentrations. For the first time SESANS measurements are performed on objects with this geometry. From the measurements the average diameter can be seen directly. From a more careful analysis the width distribution is determined. The gel phase itself prepared at lower concentrations did not show any signal, in contrast to what one observes with conventional SANS. This shows the complementarity of SESANS and SANS.