Dorthe Posselt

Analytical treatment of the resolution function for small-angle scattering

Analytical expression for the resolution function for small-angle scattering in pinhole geometry are derived. The contributions to the resolution function due to wavelength spread, finite collimation and detector resolution are determined separately using Gaussian functions to approximate the contributions. A general resolution function is derived which is the result of the combined effect of the three contributions. An azimuthal-integrated resolution function, which can be applied to scattering from a material with a circular symmetric scattering cross section, is calculated. This resolution function contains in addition a contribution from the averaging procedure itself. The analytical results are compared with the results of computer simulations. The comparison shows that Gaussian functions give a good description of the resolution function and that the widths agree with those calculated by the analytical expressions. The resolution function is applied in the analysis of two experimental examples: neutron scattering from latex particles [Wignall, Christen & Ramakrishnan (1988). J. Appl. Cryst. 21, 438–451] and neutron scattering from lamellar structures of bilayer lipid membranes (Mortensen, Pfeiffer, Sackmann & Knoll, unpublished). The analytical expressions for the resolution function allow a least-squares analysis to be performed and excellent agreement between experimental and theoretical scattering patterns are obtained.

Grazing-incidence small-angle X-ray scattering from thin polymer films with lamellar structures – the scattering cross section in the distorted-wave Born approximation

Grazing-incidence small-angle X-ray or neutron scattering of thin polymer films reveals information about the ordering and preferential orientations of the phase-separated microdomains within the films. The grazing-incidence geometry enhances the surface sensitivity; however, the scattering has to be treated within the framework of the distorted-wave Born approximation. In this work, the case of thin films with lamellar mesostructure is studied, where the orientation of the lamellae is either perpendicular or parallel to the film interfaces. For perpendicular lamellae, Bragg rods are found, which are extended along the film normal, whereas for parallel lamellae, peaks along the film normal appear. The positions of the maxima present in the latter case are explained by accounting for refraction at the film surface and reflection at the film–substrate interface. The results are relevant for thin films of lamellar diblock copolymers.

Calcium addition in straw gasification

Abstract The present work focuses on the influence of calcium addition in gasification. The inorganic–organic element interaction as well as the detailed inorganic–inorganic elements interaction has been studied. The effect of calcium addition as calcium sugar/molasses solutions to straw significantly affected the ash chemistry and the ash sintering tendency but much less the char reactivity. Thermo balance test are made and high-temperature X-ray diffraction measurements are performed, the experimental results indicate that with calcium addition major inorganic–inorganic reactions take place very late in the char conversion process. Comprehensive global equilibrium calculations predicted important characteristics of the inorganic ash residue. Equilibrium calculations predict the formation of liquid salt if sufficient amounts of Ca are added and according to experiments as well as calculations calcium binds silicon primarily as calcium silicates and less as potassium calcium silicates.

Characterization of Polymer Thin Films with Small-Angle X-ray Scattering under Grazing Incidence (GISAXS)

Polymer thin films have numerous technical applications as functional coatings, the most prominent example being PMMA coatings for lithography of integrated circuits and micromechanical devices. Polymer blends and block copolymers can be tailored for specific mechanical, optical, electric, and chemical properties. For instance, functional surfaces have been created by means of polymer blend and diblock copolymer films which may serve as templates for nanolithography [1] or as antireflection coatings [2]. In the rapidly developing field of molecular electronics, opto-electronical properties of polymer films have been exploited and first devices have appeared on the market [3].

Structural Instabilities in Lamellar Diblock Copolymer Thin Films During Solvent Vapor Uptake

We have studied the structural rearrangements in a lamellae-forming poly(styrene-b-butadiene) film during exposure to toluene vapor. Real-time, in situ grazing-incidence small-angle X-ray scattering allowed us to identify distinct kinetic regimes: First, the lamellae swell linearly, and the blocks stretch uniaxially. Then, the blocks relax to a more globular molecular conformation, and the lamellar thickness abruptly shrinks again. The increased interfacial area culminates in a dramatic instability causing a major rearrangement of the lamellar stack and the formation of new lamellae. Finally, the lamellar thickness levels off, and the interfaces flatten again.

Reversible membrane reorganizations during photosynthesis in vivo: Revealed by small-angle neutron scattering

In the present study, we determined characteristic repeat distances of the photosynthetic membranes in living cyanobacterial and eukaryotic algal cells, and in intact thylakoid membranes isolated from higher plants with time-resolved small-angle neutron scattering. This non-invasive technique reveals light-induced reversible reorganizations in the seconds-to-minutes time scale, which appear to be associated with functional changes in vivo.

A SANS investigation on absolute scale of a homologous series of base-catalysed silica aerogels

Small angle neutron scattering data for a homologous series of base-catalysed silica aerogels are presented. The data are brought on an absolute scale by normalisation with water. Both oxidised and untreated samples are investigated, and it is found that oxidation does not alter the overall aerogel structure, the only effect of oxidation being the removal of surface groups. It is concluded that the samples are best described as consisting of elemental building blocks with a radial size of 20 A, aggregated into clusters with a density dependent radius, 5–10 times larger than the building block size. The monolithic aerogel is formed by connection of these clusters. The existence of clusters in the aerogel structure is manifested in the data by the presence of cluster-cluster correlation effects. These effects are not observed in SANS spectra reported in the literature for neutrally reacted aerogels.

The ultrastructure and flexibility of thylakoid membranes in leaves and isolated chloroplasts as revealed by small-angle neutron scattering ☆ ☆☆

We studied the periodicity of the multilamellar membrane system of granal chloroplasts in different isolated plant thylakoid membranes, using different suspension media, as well as on different detached leaves and isolated protoplasts-using small-angle neutron scattering. Freshly isolated thylakoid membranes suspended in isotonic or hypertonic media, containing sorbitol supplemented with cations, displayed Bragg peaks typically between 0.019 and 0.023Å(-1), corresponding to spatially and statistically averaged repeat distance values of about 275-330 Å⁻¹. Similar data obtained earlier led us in previous work to propose an origin from the periodicity of stroma thylakoid membranes. However, detached leaves, of eleven different species, infiltrated with or soaked in D2O in dim laboratory light or transpired with D2O prior to measurements, exhibited considerably smaller repeat distances, typically between 210 and 230 Å⁻¹, ruling out a stromal membrane origin. Similar values were obtained on isolated tobacco and spinach protoplasts. When NaCl was used as osmoticum, the Bragg peaks of isolated thylakoid membranes almost coincided with those in the same batch of leaves and the repeat distances were very close to the electron microscopically determined values in the grana. Although neutron scattering and electron microscopy yield somewhat different values, which is not fully understood, we can conclude that small-angle neutron scattering is a suitable technique to study the periodic organization of granal thylakoid membranes in intact leaves under physiological conditions and with a time resolution of minutes or shorter. We also show here, for the first time on leaves, that the periodicity of thylakoid membranes in situ responds dynamically to moderately strong illumination. This article is part of a special issue entitled: photosynthesis research for sustainability: keys to produce clean energy.

Structural Evolution of Perpendicular Lamellae in Diblock Copolymer Thin Films during Solvent Vapor Treatment Investigated by Grazing-Incidence Small-Angle X-Ray Scattering

The structural evolution in poly(styrene-b-butadiene) (P(S-b-B)) diblock copolymer thin films during solvent vapor treatment is investigated in situ using time-resolved grazing-incidence small-angle X-ray scattering (GISAXS). Using incident angles above and below the polymer critical angle, structural changes near the film surface and in the entire film are distinguished. The swelling of the film is one-dimensional along the normal of the substrate. During swelling, the initially perpendicular lamellae tilt within the film to be able to shrink. In contrast, at the film surface, the lamellae stay perpendicular, and eventually vanish at the expense of a thin PB wetting layer. During the subsequent drying, the perpendicular lamellae reappear at the surface, and finally, PS blocks protrude. By modeling, the time-dependent height of the protrusions can be quantitatively extracted.

Kinetics of structural reorganizations in multilamellar photosynthetic membranes monitored by small angle neutron scattering

We demonstrate the power of time-resolved small-angle neutron scattering experiments for the investigation of the structure and structural reorganizations of multilamellar photosynthetic membranes. In addition to briefly summarizing our results on thylakoid membranes isolated from higher plants and in unicellular organisms, we discuss the advantages and technical and methodological limitations of time-resolved SANS. We present a detailed and more systematical investigation of the kinetics of light-induced structural reorganizations in isolated spinach thylakoid membranes, which show how changes in the repeat distance and in the long-range order of the multilamellar membranes can be followed with a time resolution of seconds. We also present data from comparative measurements performed on thylakoid membranes isolated from tobacco.Graphical abstract