Quasielastic Neutron Scattering Research Articles

Short-range magnetic order within the multiferroic erythrosiderite mineral(NH4)2FeCl5·H2O

Molecular multiferroics are receiving a large amount of interest, in part due to the ease of synthesis and their potential for tuneability. An important compound within this field is ammonium pentachloroaquaferrate(III), ${({\mathrm{NH}}_{4})}_{2}{\mathrm{FeCl}}_{5}\ifmmode\cdot\else\textperiodcentered\fi{}{\mathrm{H}}_{2}\mathrm{O}$, which has received a lot of attention due to it having both magnetic and ferroelectric transitions at 7.3 and 6.9 K, respectively. The magnetic structure is complex, with many different exchange pathways; however, to date there has been no consideration of magnetic interactions above the critical temperature. Our paper utilizes muon spin spectroscopy, inelastic neutron scattering and quasielastic neutron scattering (QENS) to show that, as one might expect for these complex magnetic systems, there is indeed evidence for short-range order above 7.3 K and this persists up to $\ensuremath{\sim}15$ K. We also highlight the sensitivity of the QENS technique to the magnetic transition and any localized fluctuations.

Rotation of complex ions with ninefold hydrogen coordination studied by quasielastic neutron scattering and first-principles molecular dynamics calculations

Quasielastic neutron scattering (QENS) and neutron powder diffraction of the complex transition metal hydrides ${\mathrm{Li}}_{5}{\mathrm{MoH}}_{11}$ and ${\mathrm{Li}}_{6}{\mathrm{NbH}}_{11}$ were measured in a temperature range of 10--300 K to study their structures and dynamics, especially the dynamics of the hydrogen atoms. These hydrides contain unusual ninefold H-coordinated complex ions (${\mathrm{MoH}}_{9}^{3\ensuremath{-}}$ or ${\mathrm{NbH}}_{9}^{4\ensuremath{-}}$) and hydride ions $({\mathrm{H}}^{\ensuremath{-}})$. A QENS signal appeared >150 K due to the relaxation of H atoms. The intermediate scattering functions derived from the QENS spectra are well fitted by a stretched exponential function called the Kohlrausch-Williams-Watts functions with a small stretching exponent \ensuremath{\beta} \ensuremath{\approx} 0.3--0.4, suggesting a wide relaxation time distribution. The $Q$ dependence of the elastic incoherent structure factor is reproduced by the rotational diffusion of $M{\mathrm{H}}_{9}$ ($M=\mathrm{Mo}$ or Nb) anions. The results are well supported by a van Hove analysis for the motion of H atoms obtained using first-principles molecular dynamics calculations. We conclude that the wide relaxation time distribution of the $M{\mathrm{H}}_{9}$ rotation is due to the positional disorder of the surrounding Li ions and a unique rotation with $M{\mathrm{H}}_{9}$ anion deformation (pseudorotation).

A Molecular Description of Hydrogel Forming Polymers for Cement-Based Printing Paste Applications

This research endeavors to link the physical and chemical characteristics of select polymer hydrogels to differences in printability when used as printing aids in cement-based printing pastes. A variety of experimental probes including differential scanning calorimetry (DSC), NMR-diffusion ordered spectroscopy (DOSY), quasi-elastic neutron scattering (QENS) using neutron backscattering spectroscopy, and X-ray powder diffraction (XRD), along with molecular dynamic simulations, were used. Conjectures based on objective measures of printability and physical and chemical-molecular characteristics of the polymer gels are emerging that should help target printing aid selection and design, and mix formulation. Molecular simulations were shown to link higher hydrogen bond probability and larger radius of gyration to higher viscosity gels. Furthermore, the higher viscosity gels also produced higher elastic properties, as measured by neutron backscattering spectroscopy.

Structure and dynamics of supercooled water in the hydration layer of poly(ethylene glycol).

The statics and dynamics of supercooled water in the hydration layer of poly(ethylene glycol) (PEG) were studied by a combination of quasi-elastic neutron scattering (QENS) and molecular dynamics (MD) simulations. Two samples, that is, hydrogenated PEG/deuterated water (h-PEG/D2O) and fully deuterated PEG/hydrogenated water (d-PEG/H2O) with the same molar ratio of ethylene glycol (EG) monomer to water, 1:1, are compared. The QENS data of h-PEG/D2O show the dynamics of PEG, and that of d-PEG/H2O reveals the motion of water. The temperature-dependent elastic scattering intensity of both samples has shown transitions at supercooled temperature, and these transition temperatures depend on the energy resolution of the instruments. Therefore, neither one is a phase transition, but undergoes dynamic process. The dynamic of water can be described as an Arrhenius to super-Arrhenius transition, and it reveals the hydrogen bonding network relaxation of hydration water around PEG at supercooled temperature. Since the PEG-water hydrogen bond structural relaxation time from MD is in good agreement with the average relaxation time from QENS (d-PEG/H2O), MD may further reveal the atomic pictures of the supercooled hydration water. It shows that hydration water molecules form a series of pools around the hydrophilic oxygen atom of PEG. At supercooled temperature, they have a more bond ordered structure than bulk water, proceed a trapping sites diffusion on the PEG surface, and facilitate the structural relaxation of PEG backbone.

Exceptionally Fast Ion Diffusion in Block Copolymer-Based Porous Carbon Fibers.

Confined ionic liquids in hydrophilic porous media have disrupted lattices and can be divided into two layers: An immobile ion layer adheres to the pore surfaces, and an inner layer exhibits faster mobility than the bulk. In this work, we report the first study of ionic liquids confined in block copolymer-based porous carbon fibers (PCFs) synthesized from polyacrylonitrile-block-polymethyl methacrylate (PAN-b-PMMA). The PCFs contain a network of unimodal mesopores of 13.6 nm in diameter and contain more hydrophilic surface functional groups than previously studied porous carbon. Elastic neutron scattering shows no freezing point for 1-butyl-3-methylimidazolium tetrafluoroborate ([BMIM]BF4) confined in PCFs down to 20 K. Quasi-elastic neutron scattering (QENS) is used to measure the diffusion of [BMIM]BF4 confined in PCFs, which, surprisingly, is 7-fold faster than in the bulk. The unprecedentedly high ion diffusion remarks that PCFs hold exceptional potential for use in electrochemical catalysis, energy conversion, and storage.

Microscopic diffusion in cationic vesicles across different phases

Understanding the phase behavior and microscopic diffusion mechanism of cationic vesicles is crucial for controlled-release kinetics in gene/DNA transfection. Here, we report our findings on the structure, phase behavior, and microscopic dynamics of a vesicle based on a cationic double-chained surfactant, dihexadecyldimethylammonium bromide (DHDAB), which is a promising candidate for a nonviral gene/DNA carrier. Small-angle neutron-scattering measurements reveal that DHDAB aggregates are in the form of unilamellar vesicles. Calorimetric studies show a strong thermal hysteresis in the heating and cooling cycles following different pathways. Two first-order transitions are observed at 303 and 318 K in the heating cycle. Fourier transform infrared spectroscopy reveals that the first transition (at 303 K) is associated with a polymorphic (solid-solid) transition from coagel to an intermediate crystalline (IC) phase, and subsequently the second transition (at 318 K) is an order-disorder transition from IC to the fluid phase. Interestingly, it is found that in the cooling cycle, the fluid phase directly transforms back into the coagel phase without passing through the IC phase. This is also confirmed by an elastic fixed window scan (EFWS) using incoherent neutron scattering. The phase behavior of DHDAB is in strong contrast to that of its longer-chain counterpart, dioctadecyldimethylammonium bromide (DODAB), where the intermediate gel phase was observed during the cooling cycle. Moreover, no polymorphic transition was observed in the heating cycle of DODAB, in which the coagel phase directly converts to the fluid phase. These sharply contrasting phase behaviors for DHDAB and DODAB suggest the strong dependence of membrane phase behavior to the alkyl chain length. EFWS measurements reveal that the phase transitions observed in the DHDAB membrane are associated with strong changes in the DHDAB dynamics. The changes in conformational entropy of DHDAB molecules estimated from EFWS confirm that the coagel-fluid and IC-fluid phase transitions are accompanied by strong changes in the conformations of the alkyl chains. The microscopic dynamics of DHDAB molecules in each of these phases is investigated by employing quasielastic neutron-scattering (QENS). In the ordered phases (coagel and IC), only localized internal dynamics of the DHDAB is observed in the QENS spectra. However, in the fluid phase, the presence of a long-range lateral diffusion is detected in addition to the localized internal dynamics of the alkyl chain. The lateral motion is found to follow Fickian diffusion. The internal dynamics of DHDAB depends on the phase state of the bilayer. In the ordered phase, the internal dynamics is described by a fractional uniaxial rotational diffusion model. However, in the fluid phase, where alkyl tails are disordered with significant gauche defects, the internal dynamics is described using localized translation within confined spheres. This study highlights the rich phase behavior of the DHDAB membrane and the surfactant dynamics across these phases.

The Impact of Surface Charges of Carboxylated Cellulose Nanofibrils on the Water Motions in Hydrated Films.

Cellulose nanofibrils (CNFs) with carboxylated surface ligands are a class of materials with tunable surface functionality, good mechanical properties, and bio-/environmental friendliness. They have been used in many applications as scaffold, reinforcing, or functional materials, where the interaction between adsorbed moisture and the CNF could lead to different properties and structures and become critical to the performance of the materials. In this work, we exploited multiple experimental methods to study the water movement in hydrated films made of carboxylated CNFs prepared by TEMPO oxidation with two different surface charges of 600 and 1550 μmol·g–1. A combination of quartz crystal microbalance with dissipation (QCM-D) and small-angle X-ray scattering (SAXS) shows that both the surface charge of a single fibril and the films’ network structure contribute to the moisture uptake. The films with 1550 μmol·g–1 surface charges take up twice the amount of moisture per unit mass, leading to the formation of nanostructures with an average radius of gyration of 2.1 nm. Via the nondestructive quasi-elastic neutron scattering (QENS), a faster motion is explained as a localized movement of water molecules inside confined spheres, and a slow diffusive motion is found with the diffusion coefficient close to bulk water at room temperature via a random jump diffusion model and regardless of the surface charge in films made from CNFs.

Uncovering the Dynamics of Confined Water Using Neutron Scattering: Perspectives

The main characteristic of liquid water is the formation of dynamic hydrogen bond networks that occur over a broad range of time scales from tens of femtoseconds to picoseconds and are responsible for water’s unique properties. However, in many important processes water does not exist in its bulk form, but in confined nanometer scale environments. The investigation of this confined water dynamics is challenging since the intermediate strength of the hydrogen bonds makes it possible to alter the structure and dynamics of this constrained water. Even if no single experimental technique can give a full picture of such intricate dynamics, it is well established that quasielastic neutron scattering (QENS) is a powerful tool to study the modification of hydrogen bonds in confinement in various materials. This is possible because neutrons tell us where the atoms are and what they are doing, can detect hydrogen, are penetrative and non-destructive. Furthermore, QENS is the only spectroscopic technique that provides information on the dynamics and atomic-motion amplitudes over a predetermined length scale. However scientific value of these data is hardly exploited and never to its full potential. This perspective highlights how new developments on instrumentation and data analysis will lead to appreciable progress in our understanding of the dynamics of complex systems, ranging from biological organisms to cloud formation.

Highly Efficient Proton Conduction in the Metal-Organic Framework Material MFM-300(Cr)·SO4(H3O)2.

The development of materials showing rapid proton conduction with a low activation energy and stable performance over a wide temperature range is an important and challenging line of research. Here, we report confinement of sulfuric acid within porous MFM-300(Cr) to give MFM-300(Cr)·SO4(H3O)2, which exhibits a record-low activation energy of 0.04 eV, resulting in stable proton conductivity between 25 and 80 °C of >10–2 S cm–1. In situ synchrotron X-ray powder diffraction (SXPD), neutron powder diffraction (NPD), quasielastic neutron scattering (QENS), and molecular dynamics (MD) simulation reveal the pathways of proton transport and the molecular mechanism of proton diffusion within the pores. Confined sulfuric acid species together with adsorbed water molecules play a critical role in promoting the proton transfer through this robust network to afford a material in which proton conductivity is almost temperature-independent.

Diffusive Dynamic Modes of Recombinant Squid Ring Teeth Proteins by Neutron Spectroscopy.

Stimuli-responsive structural proteins are emerging as promising biocompatible materials for a wide range of biological and nonbiological applications. To understand the physical properties of structural proteins and to replicate their performance in biosynthetic systems, there is a need to understand the molecular mechanisms and relationships that regulate their structure, dynamics, and properties. Here, we study the dynamics of a recombinant squid-inspired protein from Loligo vulgaris (Lv18) by elastic and quasielastic neutron scattering (QENS) to understand the connection between nanostructure, chain dynamics, and mechanical properties. Lv18 is a semicrystalline structural protein, which is plasticized by water above its glass transition temperature at 35 °C. Elastic scans revealed an increased protein chain mobility upon hydration, superimposed dynamic processes, and a decrease in dynamic transition temperatures. Further analysis by QENS revealed that while dry Lv18 protein dynamics are dominated by localized methyl group rotations, hydrated Lv18 dynamics are dominated by the confined diffusion of flexible chains within a β-sheet nanocrystalline network (8 Å of confinement radius). Our findings establish a relationship between the segment block architecture of Lv18, the diffusive motions within the protein structure, and the mechanical properties of recombinant squid proteins, which will advance the molecular design of novel high-performance protein-inspired materials with tailored dynamics and mechanical properties.

Understanding the Impacts of Support-Polymer Interactions on the Dynamics of Poly(ethyleneimine) Confined in Mesoporous SBA-15.

Supported amines are a promising class of CO2 sorbents offering large uptake capacities and fast uptake rates. Among supported amines, poly(ethyleneimine) (PEI) physically impregnated in the mesopores of SBA-15 silica is widely used. Within these composite materials, the chain dynamics and morphologies of PEI strongly influence the CO2 capture performance, yet little is known about chain and macromolecule mobility in confined pores. Here, we probe the impact of the support-PEI interactions on the dynamics and structures of PEI at the support interface and the corresponding impact on CO2 uptake performance, which yields critical structure-property relationships. The pore walls of the support are grafted with organosilanes with different chemical end groups to differentiate interaction modes (spanning from strong attraction to repulsion) between the pore surface and PEI. Combinations of techniques, such as quasi-elastic neutron scattering (QENS), 1H T1-T2 relaxation correlation solid-state NMR, and molecular dynamics (MD) simulations, are used to comprehensively assess the physical properties of confined PEI. We hypothesized that PEI would have faster dynamics when subjected to less attractive or repulsive interactions. However, we discover that complex interfacial interactions resulted in complex structure-property relationships. Indeed, both the chain conformation of the surface-grafted chains and of the PEI around the surface influenced the chain mobility and CO2 uptake performance. By coupling knowledge of the dynamics and distributions of PEI with CO2 sorption performance and other characteristics, we determine that the macroscopic structures of the hybrid materials dictate the first rapid CO2 uptake, and the rate of CO2 sorption during the subsequent gradual uptake stage is determined by PEI chain motions that promote diffusive jumps of CO2 through PEI-packed domains.

Dynamical Behavior of Disordered Regions in Disease-Related Proteins Revealed by Quasielastic Neutron Scattering.

Background and Objectives: Intrinsically disordered proteins (IDPs) and proteins containing intrinsically disordered regions (IDRs) are known to be involved in various human diseases. Since the IDPs/IDRs are fluctuating between many structural substrates, the dynamical behavior of the disease-related IDPs/IDRs needs to be characterized to elucidate the mechanisms of the pathogenesis of the diseases. As protein motions have a hierarchy ranging from local side-chain motions, through segmental motions of loops or disordered regions, to diffusive motions of entire molecules, segmental motions, as well as local motions, need to be characterized. Materials and Methods: Combined analysis of quasielastic neutron scattering (QENS) spectra with the structural data provides information on both the segmental motions and the local motions of the IDPs/IDRs. Here, this method is applied to re-analyze the QENS spectra of the troponin core domain (Tn-CD), various mutants of which cause the pathogenesis of familial cardiomyopathy (FCM), and α-synuclein (αSyn), amyloid fibril formation of which is closely related to the pathogenesis of Parkinson’s disease, collected in the previous studies. The dynamical behavior of wild-type Tn-CD, FCM-related mutant Tn-CD, and αSyn in the different propensity states for fibril formation is characterized. Results: In the Tn-CD, the behavior of the segmental motions is shown to be different between the wild type and the mutant. This difference is likely to arise from changes in the intramolecular interactions, which are suggested to be related to the functional aberration of the mutant Tn-CD. In αSyn, concerted enhancement of the segmental motions and the local motions is observed with an increased propensity for fibril formation, suggesting the importance of these motions in fibril formation. Conclusions: Characterization of the segmental motions as well as the local motions is thus useful for discussing how the changes in dynamical behavior caused by the disease-related mutations and/or environmental changes could be related to the functional and/or behavioral aberrations of these proteins.

Study of the water dynamics near hydrophilic, nanostructured CuO surfaces by quasielastic and inelastic neutron scattering

We have used quasielastic and inelastic neutron scattering to investigate the structure, dynamics, and phase transitions of water interacting with superhydrophilic CuO surfaces that not only possess a strong affinity for water but also a “grass-like” topography that is rough on both micro- and nanoscales. Here, we report quasielastic neutron scattering (QENS) measurements on two samples differing in water content at five temperatures below 280 K. The QENS spectra show water undergoing two different types of diffusive motion near the CuO surfaces: a “slow” translational diffusion occurring on a nanosecond time scale and a faster rotational motion. Further from the surfaces, there is “fast” translational diffusion comparable in rate to that of bulk supercooled water and the rotational motion occurring in the interfacial water. Analysis of the QENS spectra supports wetting of water to the CuO blades as seen in electron microscopy images. In addition, we observe an anomalous temperature dependence of the QENS spectra on cooling from 270 to 230 K with features consistent with a liquid–liquid phase transition. We suggest that the solvent-like properties of the coexisting bulk-like water in our CuO samples are a significant factor in determining the temperature dependence of the interfacial water’s dynamics. Our results are compared with those obtained from two well-studied substrate classes: (1) silicas that contain ordered cylindrical nanopores but have weaker hydrophilicity and (2) nanoparticles of other transition-metal oxides, such as TiO2, which share the strong hydrophilicity of our samples but lack their porosity.

Water Dynamics in Cancer Cells: Lessons from Quasielastic Neutron Scattering.

The severity of the cancer statistics around the globe and the complexity involving the behavior of cancer cells inevitably calls for contributions from multidisciplinary areas of research. As such, materials science became a powerful asset to support biological research in comprehending the macro and microscopic behavior of cancer cells and untangling factors that may contribute to their progression or remission. The contributions of cellular water dynamics in this process have always been debated and, in recent years, experimental works performed with Quasielastic neutron scattering (QENS) brought new perspectives to these discussions. In this review, we address these works and highlight the value of QENS in comprehending the role played by water molecules in tumor cells and their response to external agents, particularly chemotherapy drugs. In addition, this paper provides an overview of QENS intended for scientists with different backgrounds and comments on the possibilities to be explored with the next-generation spectrometers under construction.

Neutrons in Softmatter

Neutron scattering is a powerful method to investigate hierarchical structure and dynamics of soft matter. In this article, several experimental results of surfactant systems, binary liquid mixtures with antagonistic salt, lipid membrane and hydration water by means of Small-Angle Neutron Scattering, Neutron Spin Echo and Quasi-Elastic Neutron Scattering were introduced.

Data Collection for Dilute Protein Solutions via a Neutron Backscattering Spectrometer

Understanding protein functions requires not only static but also dynamic structural information. Incoherent quasi-elastic neutron scattering (QENS), which utilizes the highly incoherent scattering ability of hydrogen, is a powerful technique for revealing the dynamics of proteins in deuterium oxide (D2O) buffer solutions. The background scattering of sample cells suitable for aqueous protein solution samples, conducted with a neutron backscattering spectrometer, was evaluated. It was found that the scattering intensity of an aluminum sample cell coated with boehmite using D2O was lower than that of a sample cell coated with regular water (H2O). The D2O-Boehmite coated cell was used for the QENS measurement of a 0.8 wt.% aqueous solution of an intrinsically disordered protein in an intrinsically disordered region of a helicase-associated endonuclease for a fork-structured type of DNA. The cell was inert against aqueous samples at 283–363 K. In addition, meticulous attention to cells with small individual weight differences and the positional reproducibility of the sample cell relative to the spectrometer neutron beam position enabled the accurate subtraction of the scattering profiles of the D2O buffer and the sample container. Consequently, high-quality information on protein dynamics could be extracted from dilute protein solutions.

The dynamical Matryoshka model: 3. Diffusive nature of the atomic motions contained in a new dynamical model for deciphering local lipid dynamics

In accompanying papers [Bicout et al., BioRxiv https://doi.org/10.1101/2021.09.21.461198 (2021); Cissé et al., BioRxiv https://doi.org/10.1101/2022.03.30.486370 (2022)], a new model called Matryoshka model has been proposed to describe the geometry of atomic motions in phospholipid molecules in bilayers and multilamellar vesicles based on their quasielastic neutron scattering (QENS) spectra. Here, in order to characterize the relaxational aspects of this model, the energy widths of the QENS spectra of the samples were analyzed first in a model-free way. The spectra were decomposed into three Lorentzian functions, which are classified as slow, intermediate, and fast motions depending on their widths. The analysis provides the diffusion coefficients, residence times, and geometrical parameters for the three classes of motions. The results corroborate the parameter values such as the amplitudes and the mobile fractions of atomic motions obtained by the application of the Matryoshka model to the same samples. Since the current analysis was carried out independently of the development of the Matryoshka model, the present results enhance the validity of the model. The model will serve as a powerful tool to decipher the dynamics of lipid molecules not only in model systems, but also in more complex systems such as mixtures of different kinds of lipids or natural cell membranes.

The dynamical Matryoshka model: 1. Incoherent neutron scattering functions for lipid dynamics in bilayers

Fluid lipid bilayers are the building blocks of biological membranes. Although there is a large amount of experimental data using incoherent quasi-elastic neutron scattering (QENS) techniques to study membranes, very little theoretical works have been developed to study the local dynamics of membranes. The main objective of this work is to build a theoretical framework to study and describe the local dynamics of lipids and derive analytical expressions of intermediate scattering functions (ISF) for QENS. As results, we developed the dynamical Matryoshka model which describes the local dynamics of lipid molecules in membrane layers as a nested hierarchical convolution of three motional processes: (i) individual motions described by the vibrational motions of H-atoms; (ii) internal motions including movements of the lipid backbone, head groups and tails, and (iii) molecule movements of the lipid molecule as a whole. The analytical expressions of the ISF associated with these movements are all derived. For use in analyzing the QENS experimental data, we also derived an analytical expression for the aggregate ISF of the Matryoshka model which involves an elastic term plus three inelastic terms of well-separated time scales and whose amplitudes and rates are functions of the lipid motions. And as an illustrative application, we used the aggregated ISF to analyze the experimental QENS data on a lipid sample of multilamellar bilayers of DMPC (1,2-dimyristoyl-sn-glycero-3-phosphocholine). It is clear from this analysis that the dynamical Matryoshka model describes very well the experimental data and allow extracting the dynamical parameters of the studied system.

Nanoscale Structure and Dynamics of Model Membrane Lipid Raft Systems, Studied by Neutron Scattering Methods

Quasi-elastic neutron scattering (QENS) and small angle neutron scattering (SANS), in combination with isotopic contrast variation, have been used to determine the structure and dynamics of three-component lipid membranes, in the form of vesicles, comprising an unsaturated [palmitoyl-oleoyl-phosphatidylcholine (POPC) or dioleoyl-phosphatidylcholine (DOPC)], a saturated phospholipid (dipalmitoyl-phosphatidylcholine (DPPC)), and cholesterol, as a function temperature and composition. SANS studies showed vesicle membranes composed of a 1:1:1 molar ratio of DPPC:DOPC:cholesterol and a 2:2:1 molar ratio of DPPC:POPC:cholesterol phase separated, forming lipid rafts of ∼18 and ∼7 nm diameter respectively, when decreasing temperature from 308 to 297 K. Phase separation was reversible upon increasing temperature. The larger rafts observed in systems containing DOPC are attributed to the greater mis-match in lipid alkyl chains between DOPC and DPPC, than for POPC and DPPC. QENS studies, over the temperature range 283–323K, showed that the resulting data were best modelled by two Lorentzian functions: a narrow component, describing the “in-plane” lipid diffusion, and a broader component, describing the lipid alkyl chain segmental relaxation. The overall “in-plane” diffusion was found to show a significant reduction upon increasing temperature due to the vesicle membranes transitioning from one containing rafts to one where the component lipids are homogeneously mixed. The use of different isotopic combinations allowed the measured overall reduction of in-plane diffusion to be understood in terms of an increase in diffusion of the saturated DPPC lipid and a corresponding decrease in diffusion of the unsaturated DOPC/POPC lipid. As the rafts are considered to be composed principally of saturated lipid and cholesterol, the breakdown of rafts decreases the exposure of the DPPC to cholesterol whilst increasing the exposure of cholesterol to unsaturated lipid. These results show the sensitivity of lipid diffusion to local cholesterol concentration, and the importance of considering the local, rather that the global composition of a membrane when understanding the diffusion processes of lipids within the membrane. The novel combination of SANS and QENS allows a non-intrusive approach to characterize the structure and dynamics occurring in phase-separated model membranes which are designed to mimic the lateral heterogeneity of lipids seen in cellular membranes–a heterogeneity that can have pathological consequences.

Development of a hybrid piston cylinder cell for quasielastic neutron scattering experiments up to 1 GPa

ABSTRACT We have developed a hybrid piston cylinder cell for quasielastic neutron scattering (QENS) experiments up to about 1 GPa. It consists of a fretted cylinder made of the high tensile steel (SNCM439) liner and the Al alloy (NA700) jacket. Performance tests revealed that the cell can withstand a pressure of 0.8 GPa without irreversible damage and has 4.4 times larger neutron transmission at 3.14 meV (5.10 Å in wavelength) than that of a conventional CuBe monobloc cylinder. Combined with the sample assembly devised for suppressing multiple scattering, high quality QENS spectra of water were obtained up to 0.8 GPa. This study illustrates the efficacy of the hybrid cylinders not only for increasing maximum available pressure but also manipulating the available pressure and the signal intensity, depending on the purpose of the experiments.