| 1. |
- Adlmann, Franz Alois
(författare)
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Opportunities and challenges of surface scattering at next generation neutron sources
- 2018
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Doktorsavhandling (övrigt vetenskapligt/konstnärligt)abstract
- Complex fluids and soft matter are ubiquitously found in the world and all contacts in life are made over surfaces. To describe the mechanical behavior of such substances, rheological methods are used. Flow instabilities are a big challenge in rheology since they will be reflected in the macroscopic variables probed, like e. g. the viscosity. Many such discontinuities may actually originate at the surface. Investigating the properties of liquids in contact with the surface under mechanical load is the main course of the thesis. Neutron reflectometry and GISANS are perfect tools in this context to access the solid liquid interfaces, since they can penetrate many engineering materials and show a comparably large scattering potential at deuterated samples. In this thesis shear was applied on a model solution and neutron scattering techniques were used to investigate the structure under load. The focus was set on the development of the measurement methods themselves to enable new scientific insights in the future. First, by stroboscopic measurements the flux limitations are overcome for oscillatory rheology. By reintegration in the post processing it is shown that kinetic measurements with neutrons are possible with a time resolution below one millisecond. Second, the transformation of grazing incidence data from the laboratory system into q-space is strongly non-linear resulting in a need for re-binning. In this thesis a universal tool has been developed for this purpose. Finally, there is an ongoing discussion on depth sensitive neutron scattering experiments from solid-liquid boundaries. By using emission densities we show that such experiments face severe limitations due to the low absorption cross section of the neutron.
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| 2. |
- Adlmann, Franz A., et al.
(författare)
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Towards neutron scattering experiments with sub-millisecond time resolution
- 2015
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Ingår i: Journal of applied crystallography. - 0021-8898 .- 1600-5767. ; 48, s. 220-226
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Tidskriftsartikel (refereegranskat)abstract
- Neutron scattering techniques offer several unique opportunities in materials research. However, most neutron scattering experiments suffer from the limited flux available at current facilities. This limitation becomes even more severe if time-resolved or kinetic experiments are performed. A new method has been developed which overcomes these limitations when a reversible process is studied, without any compromise on resolution or beam intensity. It is demonstrated that, by recording in absolute time the neutron detector events linked to an excitation, information can be resolved on sub-millisecond timescales. Specifically, the concept of the method is demonstrated by neutron reflectivity measurements in time-of-flight mode at the Liquids Reflectometer located at the Spallation Neutron Source, Oak Ridge National Laboratory, Tennessee, USA, combined with in situ rheometry. The opportunities and limitations of this new technique are evaluated by investigations of a micellar polymer solution offering excellent scattering contrast combined with high sensitivity to shear.
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| 3. |
- Adlmann, Franz A., et al.
(författare)
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Överlåtaren : a fast way to transfer and orthogonalize two-dimensional off-specular reflectivity data
- 2016
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Ingår i: Journal of applied crystallography. - 0021-8898 .- 1600-5767. ; 49, s. 2091-2099
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Tidskriftsartikel (refereegranskat)abstract
- Reflectivity measurements offer unique opportunities for the study of surfaces and interfaces, and specular reflectometry has become a standard tool in materials science to resolve structures normal to the surface of a thin film. Off-specular scattering, which probes lateral structures, is more difficult to analyse, because the Fourier space being probed is highly anisotropic and the scattering pattern is truncated by the interface. As a result, scattering patterns collected with (especially time-of-flight) neutron reflectometers are difficult to transform into reciprocal space for comparison with model calculations. A program package is presented for a generic two-dimensional transformation of reflectometry data into q space and back. The data are represented on an orthogonal grid, allowing cuts along directions relevant for theoretical modelling. This treatment includes background subtraction as well as a full characterization of the resolution function. The method is optimized for computational performance using repeatable operations and standardized instrument settings.
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| 4. |
- Adlmann, Franz, et al.
(författare)
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Depth resolved grazing incidence neutron scattering experiments from semi-infinite interfaces : a statistical analysis of the scattering contributions
- 2018
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Ingår i: Journal of Physics. - : Institute of Physics Publishing (IOPP). - 0953-8984 .- 1361-648X. ; 30
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Tidskriftsartikel (refereegranskat)abstract
- Grazing incidence neutron scattering experiments offer surface sensitivity by reflecting from an interface at momentum transfers close to total external reflection. Under these conditions the penetration depth is strongly non-linear and may change by many orders of magnitude. This fact imposes severe challenges for depth resolved experiments, since the brilliance of neutron beams is relatively low in comparison to e.g. synchrotron radiation. In this article we use probability density functions to calculate the contribution of scattering at different distances from an interface to the intensities registered on the detector. Our method has the particular advantage that the depth sensitivity is directly extracted from the scattering pattern itself. Hence for perfectly known samples exact resolution functions can be calculated and visa versa. We show that any tails in the resolution function, e.g. Gaussian shaped, hinders depth resolved experiments. More importantly we provide means for a descriptive statistical analysis of detector images with respect to the scattering contributions and show that even for perfect resolution near surface scattering is hardly accessible.
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| 5. |
- Adlmann, Franz, et al.
(författare)
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Normalization of stroboscopic neutron scattering experiments
- 2018
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Ingår i: Nuclear Instruments and Methods in Physics Research Section B. - : Elsevier BV. - 0168-583X .- 1872-9584. ; 434, s. 61-65
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Tidskriftsartikel (refereegranskat)abstract
- Neutron scattering studies of kinetic processes are often flux limited. For processes which can be repeated many times, this can be mitigated by stroboscopic reintegration. The recorded scattering events are assigned to different time slices of the process and corresponding slices from all repetitions are summed up. The normalization of such data with respect to the incident beam spectrum can be challenging since the incident neutron flux may not necessarily be evenly distributed over all time slices. In this paper, we discuss how this can result in misleading information and we expand on a technique to amend these issues.
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| 6. |
- Forooqi Motlaq, Vahid, et al.
(författare)
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Dissolution mechanism of supported phospholipid bilayer in the presence of amphiphilic drug investigated by neutron reflectometry and quartz crystal microbalance with dissipation monitoring
- 2022
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Ingår i: Biochimica et Biophysica Acta - Biomembranes. - : Elsevier. - 0005-2736 .- 1879-2642. ; 1864:10
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Tidskriftsartikel (refereegranskat)abstract
- The influence and interaction of the ionizable amphiphilic drug amitriptyline hydrochloride (AMT) on a 1,2-dioleoyl-sn-glycero-3-phosphocholine (DOPC) phospholipid bilayer supported on a silica surface have been investigated using a combination of neutron reflectometry and quartz crystal microbalance with dissipation monitoring. Adding AMT solutions with concentrations 3, 12, and 50 mM leaves the lipid bilayer mainly intact and we observe most of the AMT molecules attached to the head-group region of the outer bilayer leaflet. Virtually no AMT penetrates into the hydrophilic head-group region of the inner leaflet close to the silica surface. By adding 200 mM AMT solution, the lipid bilayer dissolved entirely, indicating a threshold concentration for the solubilization of the bilayer by AMT. The observed threshold concentration is consistent with the observation that various bilayer structures abruptly transform into mixed AMT-DOPC micelles beyond a certain AMT-DOPC composition. Based on our experimental observations, we suggest that the penetration of drug into the phospholipid bilayer, and subsequent solubilization of the membrane, follows a two-step mechanism with the outer leaflet being removed prior to the inner leaflet.
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| 7. |
- Kawecki, Maciej, et al.
(författare)
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Direct measurement of topological interactions in polymers under shear using neutron spin echo spectroscopy
- 2019
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Ingår i: Scientific Reports. - : NATURE PUBLISHING GROUP. - 2045-2322. ; 9
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Tidskriftsartikel (refereegranskat)abstract
- We present in-situ neutron spin echo measurements on an entangled polydimethylsiloxane melt under shear and demonstrate the ability to monitor nano-scale dynamics in flowing liquids. We report no changes in the topological interactions of the chains for shear rates approaching the inverse longest relaxation time. Further experiments following along this line will allow to systematically test the predictions of theories, like e.g. convective constraint release.
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| 8. |
- Kawecki, Maciej, et al.
(författare)
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Probing the dynamics of high-viscosity entangled polymers under shear using Neutron Spin Echo spectroscopy
- 2016
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Ingår i: VI European Conference On Neutron Scattering (ECNS2015). - : IOP Publishing.
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Konferensbidrag (refereegranskat)abstract
- Neutron Spin Echo spectroscopy provides unique insight into molecular and submolecular dynamics as well as intra-and inter-molecular interactions in soft matter. These dynamics may change drastically under shear flow. In particular in polymer physics a stress plateau is observed, which might be explained by an entanglement-disentanglement transition. However, such a transition is difficult to identify directly by experiments. Neutron Spin Echo has been proven to provide information about entanglement length and degree by probing the local dynamics of the polymer chains. Combining shear experiments and neutron spin echo is challenging since, first the beam polarisation has to be preserved during scattering and second, Doppler scattered neutrons may cause inelastic scattering. In this paper we present a new shear device adapted for these needs. We demonstrate that a high beam polarisation can be preserved and present first data on an entangled polymer solution under shear. To complement the experiments on the dynamics we present novel SANS data revealing shear-induced conformational changes in highly entangled polymers.
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| 9. |
- Korolkovas, Airidas, et al.
(författare)
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Polymer Brush Collapse under Shear Flow
- 2017
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Ingår i: Macromolecules. - : American Chemical Society (ACS). - 0024-9297 .- 1520-5835. ; 50:3, s. 1215-1224
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Tidskriftsartikel (refereegranskat)abstract
- Shear responsive surfaces offer potential advances in a number of applications. Surface functionalization using polymer brushes is one route to such properties, particularly in the case of entangled polymers. We report on neutron reflectometry measurements of polymer brushes in entangled polymer solutions performed under controlled shear as well as coarse-grained computer simulations corresponding to these interfaces. Here we show a reversible and reproducible collapse of the brushes, increasing with the shear rate. Using two brushes of greatly different chain lengths and grafting densities, we demonstrate that the dynamics responsible for the structural change of the brush are governed by the free chains in solution rather than the brush itself, within the range of parameters examined. The phenomenon of the brush collapse could find applications in the tailoring of nanosensors and as a way to dynamically control surface friction and adhesion.
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| 10. |
- Korolkovas, Airidas, et al.
(författare)
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Shear deformation of low-density polymer brushes in a good solvent
- 2018
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Ingår i: Physical review. E. - : AMER PHYSICAL SOC. - 2470-0045 .- 2470-0053. ; 98:3
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Tidskriftsartikel (refereegranskat)abstract
- Self-consistent field approach is used to model a single end-tethered polymer chain on a substrate subject to various forces in three dimensions. Starting from a continuous Gaussian chain model, the following perturbations are considered: (i) hydrodynamic interaction with an externally imposed shear flow for which an alternative theoretical framework is formulated; (ii) excluded volume effect in a good solvent, treated in a mean field approximation; (iii) monomer-substrate repulsion. While the chain stretches along the flow, the change of the density profile perpendicular to the substrate is negligible for any reasonable simulation parameters. This null effect is in agreement with multiple neutron scattering studies.
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