Neutron Spin Research Articles

Phase correction method in a wide detector plane for MIEZE spectroscopy with pulsed neutron beams

In this study, we propose a phase correction method for a type of neutron spin echo spectroscopy, known as modulation of intensity with zero effort using a time-of-flight method (TOF-MIEZE). The phase of the MIEZE signal sensitively varies with the neutron flight path lengths. The geometrical lengths from the sample position to the flat detector plane differ depending on the positions on the detector plane. Integrating the phase-shifted signals may decrease the signal contrast solely through the geometrical path-length deviations. To measure the decrement of contrast accurately, which corresponds to the intermediate scattering function, the position-dependent phase shifts must be corrected. The data correction is performed by shifting the MIEZE signal in time depending on path-length deviations, the MIEZE frequency, and neutron wavelengths. In the calculation of path-length deviations, the sample is assumed to be a point scatterer while a detector inclination is taken into account. We also discuss the relation between the frequency shift of TOF-MIEZE signal and path-length deviation, which is helpful to quantify phase shifts larger than 2π. The presented phase correction method is demonstrated with a 32 × 32 cm2 area detector for a 200 kHz TOF-MIEZE signal scattered from an elastic sample.

Stiffening Effect of the [Bmim][Cl] Ionic Liquid on the Bending Dynamics of DMPC Lipid Vesicles

The elastic properties of the cellular lipid membrane play a crucial role for life. Their alteration can lead to cell malfunction, and in turn, being able to control them holds the promise of effective therapeutic and diagnostic approaches. In this context, due to their proven strong interaction with lipid bilayers, ionic liquids (ILs)—a vast class of organic electrolytes—may play an important role. This work focuses on the effect of the model imidazolium-IL [bmim][Cl] on the bending modulus of DMPC lipid vesicles, a basic model of cellular lipid membranes. Here, by combining small-angle neutron scattering and neutron spin–echo spectroscopy, we show that the IL, dispersed at low concentrations at the bilayer–water interface, (i) diffuses into the lipid region, accounting for five IL-cations for every 11 lipids, and (ii) causes an increase of the lipid bilayer bending modulus, up to 60% compared to the neat lipid bilayer at 40 °C.

Structure and dynamics of large ring polymers

We report a comprehensive study on the molecular conformation and dynamics of very large poly(ethylene oxide) rings in the melt: (i) for all rings, independent of the ring size, by small angle neutron scattering we observe a crossover from a strong Q-dependence at intermediate Q to a Q−2 dependence at higher Q. Constructing a generic model including a crossover from Gaussian statistics at short distances to more compact structures at larger distances, we find the crossover at a distance along the ring of Ne,0=45±2.5 monomers close to the entanglement distance in the linear counterpart. This finding is clear evidence for the predicted elementary loops building the ring conformation. (ii) The radius of gyration Rg(N) follows quantitatively the result of numerous simulations. However, other than claimed, the crossover to mass fractal statistics does occur around N≅10Ne,0, but up to N≅44Ne,0, the relation Rg(N)∼N0.39 holds. The self-similar ring dynamics was accessed by pulsed field gradient-NMR and neutron spin echo spectroscopy: we find three dynamic regimes for center of mass diffusion starting (i) with a strong subdiffusive domain ⟨rcom2(t)⟩∼tα(0.4≤α≤0.65), (ii) a second subdiffusive region ⟨rcom2(t)⟩∼t0.75 that (iii) finally, crosses over to Fickian diffusion. The internal dynamics at scales below the elementary loop size is well described by the ring Rouse motion. At larger scales, the dynamics is self-similar and follows very well the predictions of scaling models with a preference for the fractal loopy globule model. Finally, we note that the key results were previously published in the form of two letters [Kruteva et al., ACS Macro Lett. 9, 507–511 (2020) and Kruteva et al., Phys. Rev. Lett. 125, 238004 (2020)].

New design of a magnetic device for wide-angle XYZ polarization analysis PASTIS-3, from the concept to first tests with thermal neutrons

We present the new concept and neutron test results of the third generation PASTIS device for XYZ wide-angle polarization analysis for thermal neutrons. PASTIS-3 uses two polarized 3He Neutron Spin filter Cells (NSF) for polarizing and analyzing neutrons spins, flipping the incident neutron beam polarization by reversing the 3He spin state of the polarizing entrance cell. We detail a new coil design for high spatial homogeneity of the magnetic field in any field direction, and the calculation method employed to optimize the geometry and to characterize the field gradients. Various components of the apparatus are described with particular attention to their performance and impact on the relaxation time of the NSF cells. Finally, we present test results of the new device tested on the thermal triple-axis spectrometer IN20 at the ILL.

A large beam high efficiency radio frequency neutron spin flipper.

A design for a radio frequency (RF) neutron spin flipper obtained from magneto-static and neutron spin transport simulations is presented. The RF flipper constructed from this design provides a flipping probability of 0.999 or better for a beam size 6cm wide and 15cm high and a wavelength band between 0.4 and 0.6nm. Three permanent magnet guide field sections with air gaps provide a linear field gradient along the beam propagation direction over a large cross-sectional area. An RF oscillator based on coupling the resonant coil of a Hartley oscillator to the excitation coil was developed, which provides a higher current and, thereby, a larger RF amplitude, as compared to a conventional RF power amplifier. Two opaque He3 neutron spin filters were employed to measure the flipping probability of the flipper with very high precision. A spatially uniform flipping probability of 0.9995(2) or higher was measured over the large cross-sectional area neutron guide. This RF neutron spin flipper will be employed in a polychromatic beam reflectometer at the National Institute of Standards and Technology Center for Neutron Research. This design can be applied to other polarized neutron instruments or applications requiring a very high continuous flipping probability of the neutron spin for a large cross-sectional area beam.

Measurement of the generalized spin polarizabilities of the neutron in the low-Q2 region

Understanding the nucleon spin structure in the regime where the strong interaction becomes truly strong poses a challenge to both experiment and theory. At energy scales below the nucleon mass of about 1 GeV, the intense interaction among the quarks and gluons inside the nucleon makes them highly correlated. Their coherent behaviour causes the emergence of effective degrees of freedom, requiring the application of non-perturbative techniques, such as chiral effective field theory. Here, we present measurements of the neutron's generalized spin-polarizabilities that quantify the neutron's spin precession under electromagnetic fields at very low energy-momentum transfer squared down to 0.035 GeV$^2$. In this regime, chiral effective field theory calculations are expected to be applicable. Our data, however, show a strong discrepancy with these predictions, presenting a challenge to the current description of the neutron's spin properties.

Double-focusing geometry for phase correction in neutron resonance spin-echo spectroscopy

Neutron spin phase correction is an essential technique for achieving a high energy resolution in neutron spin-echo experiments. We propose a double-focusing geometry in which two identical ellipsoidal mirrors are arranged in series. This arrangement enables us to correct the path length differences for large divergent beams using a complete ellipsoidal focusing mirror. In this study, we evaluated the effectiveness of this geometry both analytically and numerically. A Fourier time of 1 μs is achievable using this geometry.

Herriott-cavity-assisted closed-loop Xe isotope comagnetometer

We present in this paper a Herriott-cavity-assisted closed-loop Xe isotope gas comagnetometer. In this system, $^{129}$Xe and $^{131}$Xe atoms are pumped and probed by polarized Rb atoms, and continuously driven by oscillating magnetic fields, whose frequencies are kept on resonance by phase-locked loops (PLLs). Different from other schemes, we use a Herriott cavity to improve the Rb magnetometer sensitivity instead of the parametric modulation method, and this passive method is aimed to improve the system stability while maintaining the sensitivity. This system has demonstrated an angle random walk (ARW) of 0.06 $^\circ$/h$^{1/2}$, and a bias instability of 0.2 $^\circ$/h (0.15 $\mu$Hz) with a bandwidth of 1.5 Hz. By adding a closed-loop Rb isotope comagnetometer, we can extend this system to dual simultaneously working comagnetometers sharing the same cell. This extended system has wide applications in precision measurements, where we can simultaneously and independently measure the coupling of anomalous fields with proton spin and neutron spin.

Neutron Spin Echo Spectroscopy as a Unique Probe for Lipid Membrane Dynamics and Membrane-Protein Interactions

This paper describes the protocols for sample preparation, data reduction, and data analysis in neutron spin echo (NSE) studies of lipid membranes. Judicious deuterium labeling of lipids enables access to different membrane dynamics on mesoscopic length and time scales, over which vital biological processes occur.

Neutron Spin Echo Spectroscopy as a Unique Probe for Lipid Membrane Dynamics and Membrane-Protein Interactions.

Lipid bilayers form the main matrix of cell membranes and are the primary platform for nutrient exchange, protein-membraneinteractions, and viral budding, among other vital cellular processes. For efficient biological activity, cell membranes should be rigid enough to maintain the integrity of the cell and its compartments yet fluid enough to allow membrane components, such as proteins and functional domains, to diffuse and interact. This delicate balance of elastic and fluid membrane properties, and their impact on biological function, necessitate a better understanding of collective membrane dynamics over mesoscopic length and time scales of key biological processes, e.g., membrane deformations and protein binding events. Among the techniques that can effectively probe this dynamic range is neutron spin echo (NSE) spectroscopy. Combined with deuterium labeling, NSE can be used to directly access bending and thickness fluctuations as well as mesoscopic dynamics of select membrane features. This paper provides a brief description of the NSE technique and outlines the procedures for performing NSE experiments on liposomal membranes, including details of sample preparation and deuteration schemes, along with instructions for data collection and reduction. The paper also introduces data analysis methods used to extract key membrane parameters, such as the bending rigidity modulus, area compressibility modulus, and in-plane viscosity. To illustrate the biological importance of NSE studies, select examples of membrane phenomena probed by NSE are discussed, namely, the effect of additives on membrane bending rigidity, the impact of domain formation on membrane fluctuations, and the dynamic signature of membrane-protein interactions.

Neutron Radiography and Computed Tomography of Biological Systems at the Oak Ridge National Laboratory's High Flux Isotope Reactor.

Neutrons have historically been used for a broad range of biological applications employing techniques such as small-angle neutron scattering, neutron spin echo, diffraction, and inelastic scattering. Unlike neutron scattering techniques that obtain information in reciprocal space, attenuation-based neutron imaging measures a signal in real space that is resolved on the order of tens of micrometers. The principle of neutron imaging follows the Beer-Lambert law and is based on the measurement of the bulk neutron attenuation through a sample. Greater attenuation is exhibited by some light elements (most notably, hydrogen), which are major components of biological samples. Contrast agents such as deuterium, gadolinium, or lithium compounds can be used to enhance contrast in a similar fashion as it is done in medical imaging, including techniques such as optical imaging, magnetic resonance imaging, X-ray, and positron emission tomography. For biological systems, neutron radiography and computed tomography have increasingly been used to investigate the complexity of the underground plant root network, its interaction with soils, and the dynamics of water flux in situ. Moreover, efforts to understand contrast details in animal samples, such as soft tissues and bones, have been explored. This manuscript focuses on the advances in neutron bioimaging such as sample preparation, instrumentation, data acquisition strategy, and data analysis using the High Flux Isotope Reactor CG-1D neutron imaging beamline. The aforementioned capabilities will be illustrated using a selection of examples in plant physiology(herbaceous plant/root/soil system)and biomedical applications(rat femur and mouse lung).

Cooperative Chain Dynamics of Tracer Chains in Highly Entangled Polyethylene Melts.

By neutron spin echo spectroscopy, we have studied the center of mass motion of short tracer chains on the molecular length scale within a highly entangled polymer matrix. The center of mass mean square displacements of the tracers independent of their molecular weight is subdiffusive at short times until it has reached the size of the tube d; then, a crossover to Fickian diffusion takes place. This observation cannot be understood within the tube model of reptation, but is rationalized as a result of important interchain couplings that lead to cooperative chain motion within the entanglement volume ∼d^{3}. Thus, the cooperative tracer chain motions are limited by the tube size d. If the center of mass displacement exceeds this size, uncorrelated Fickian diffusion takes over. Compared to the prediction of the Rouse model we observe a significantly reduced contribution of the tracer's internal modes to the spectra corroborating the finding of cooperative rather than Rouse dynamics within d^{3}.

Development of a 3He Gas Filling Station at the China Spallation Neutron SourceSupported by the National Key Research and Development Program of China (Grant No. 2020YFA0406000), the Scientific Instrument Development Project of the Chinese Academy of Sciences (Grant No. 284(2018)), and the National Natural Science Foundation of China (Grant No. 11875265).

At the China Spallation Neutron Source (CSNS), we have developed a custom gas-filling station, a glassblowing workshop, and a spin-exchange optical pumping (SEOP) system for producing high-quality 3He-based neutron spin filter (NSF) cells. The gas-filling station is capable of routinely filling 3He cells made from GE180 glass of various dimensions, to be used as neutron polarizers and analyzers on beamlines at the CSNS. Performance tests on cells fabricated at our gas-filling station are conducted via neutron transmission and nuclear-magnetic-resonance measurements, revealing nominal filling pressures, and a saturated 3He polarization in the region of 80%, with a lifetime of approximately 240 hours. These results demonstrate our ability to produce competitive NSF cells to meet the ever-increasing research needs of the polarized neutron research community.

Biomembrane Structure and Material Properties Studied With Neutron Scattering.

Cell membranes and their associated structures are dynamical supramolecular structures where different physiological processes take place. Detailed knowledge of their static and dynamic structures is therefore needed, to better understand membrane biology. The structure–function relationship is a basic tenet in biology and has been pursued using a range of different experimental approaches. In this review, we will discuss one approach, namely the use of neutron scattering techniques as applied, primarily, to model membrane systems composed of lipid bilayers. An advantage of neutron scattering, compared to other scattering techniques, is the differential sensitivity of neutrons to isotopes of hydrogen and, as a result, the relative ease of altering sample contrast by substituting protium for deuterium. This property makes neutrons an ideal probe for the study of hydrogen-rich materials, such as biomembranes. In this review article, we describe isotopic labeling studies of model and viable membranes, and discuss novel applications of neutron contrast variation in order to gain unique insights into the structure, dynamics, and molecular interactions of biological membranes. We specifically focus on how small-angle neutron scattering data is modeled using different contrast data and molecular dynamics simulations. We also briefly discuss neutron reflectometry and present a few recent advances that have taken place in neutron spin echo spectroscopy studies and the unique membrane mechanical data that can be derived from them, primarily due to new models used to fit the data.

Chain Dynamics of Ultrahigh Molecular Weight Polyethylene Composites with Graphene Oxide Nanosheets.

We investigate the melt chain dynamics of ultrahigh molecular weight polyethylene (UHMWPE) and its composites with graphene oxide (GO) nanosheets by means of neutron spin echo spectroscopy. For the GO concentrations explored, we observe hindered chain dynamics with respect to the pure UHMWPE. We propose a model where a fraction of the polymer is immobilized on top and at the bottom of GO sheets. This model enables us to provide a microscopic measurement of the adsorbed and free polymer fractions, as well as the thickness of the adsorbed layer. Our experiments provide experimental nanoscopic evidence of GO hindering entanglement formation in a polymer melt, a phenomenon that had been observed at the macroscale before via rheological measurements.

Why the Brillouin Light Scattering Relaxation Times of Molten Zinc Chloride Are Shorter and Weaker in Temperature Dependence than the Structural Relaxation Times from Depolarized Light and Neutron Spin Echo Spectroscopy

A longstanding problem in the Brillouin light scattering (BLS) study of polymers is the relaxation times τBLS(T) being more than an order of magnitude shorter than the α-relaxation times τα(T) determined by dielectric, depolarized light scattering (DLS), and molecular dynamics simulations. In tackling the problem, τBLS(T) was identified with the relaxation time τ0(T) of the primitive relaxation in the coupling model, which can be calculated from τα(T) and the stretch exponent βK of the Kohlrausch correlation function for the α-relaxation.. The problem was solved by finding that indeed τ0(T) is in good agreement with τBLS(T). A recent work performed the neutron spin echo study of the structural α-relaxation of the network ionic liquid ZnCl2 and found the same anomaly as polymers. The α-relaxation time τNSE(T) from neutron spin echo (NSE) as well as the α-relaxation time τDLS(T) from DLS of ZnCl2 are much longer than τBLS(T) from BLS obtained before by several research groups. The finding of the same anomaly in ZnCl2 and polymers with very different chemical and physical structures offers an opportunity to critically test the explanation given before. The test was carried out by calculating the primitive relaxation times τ0,DLS(T) and τ0,NSE(T) from τDLS(T) and τNSE(T), respectively, in zinc chloride. Good agreements of τBLS(T) from BLS with τ0,DLS(T) and τ0,NSE(T) were found and thus the explanation given for polymers remains valid for ZnCl2. The test was extended to glycerol by comparing τBLS(T) with τ0,ICNS(T) and τ0,CNS(T) calculated from the α-relaxation time τICNS(T) and τCNS(T) from incoherent and coherent neutron scattering, respectively. There is good agreement between τBLS(T) and τ0,ICNS(T) in glycerol. There is also semiquantitative agreement of τBLS(T) with τ0,DS(T) from dielectric spectroscopy as well as τ0,CNS(T). Thus, the explanation for polymers is verified in the two very different glass formers, ZnCl2 and glycerol, and it is an advancement in the application of BLS to study the dynamics of glass formers.

Activated nanoscale actin-binding domain motion in the catenin–cadherin complex revealed by neutron spin echo spectroscopy

As the core component of the adherens junction in cell-cell adhesion, the cadherin-catenin complex transduces mechanical tension between neighboring cells. Structural studies have shown that the cadherin-catenin complex exists as an ensemble of flexible conformations, with the actin-binding domain (ABD) of α-catenin adopting a variety of configurations. Here, we have determined the nanoscale protein domain dynamics of the cadherin-catenin complex using neutron spin echo spectroscopy (NSE), selective deuteration, and theoretical physics analyses. NSE reveals that, in the cadherin-catenin complex, the motion of the entire ABD becomes activated on nanosecond to submicrosecond timescales. By contrast, in the α-catenin homodimer, only the smaller disordered C-terminal tail of ABD is moving. Molecular dynamics (MD) simulations also show increased mobility of ABD in the cadherin-catenin complex, compared to the α-catenin homodimer. Biased MD simulations further reveal that the applied external forces promote the transition of ABD in the cadherin-catenin complex from an ensemble of diverse conformational states to specific states that resemble the actin-bound structure. The activated motion and an ensemble of flexible configurations of the mechanosensory ABD suggest the formation of an entropic trap in the cadherin-catenin complex, serving as negative allosteric regulation that impedes the complex from binding to actin under zero force. Mechanical tension facilitates the reduction in dynamics and narrows the conformational ensemble of ABD to specific configurations that are well suited to bind F-actin. Our results provide a protein dynamics and entropic explanation for the observed force-sensitive binding behavior of a mechanosensitive protein complex.

Intermediate scattering functions of a rigid body monoclonal antibody protein in solution studied by dissipative particle dynamic simulation.

In the past decade, there was increased research interest in studying internal motions of flexible proteins in solution using Neutron Spin Echo (NSE) as NSE can simultaneously probe the dynamics at the length and time scales comparable to protein domain motions. However, the collective intermediate scattering function (ISF) measured by NSE has the contributions from translational, rotational, and internal motions, which are rather complicated to be separated. Widely used NSE theories to interpret experimental data usually assume that the translational and rotational motions of a rigid particle are decoupled and independent to each other. To evaluate the accuracy of this approximation for monoclonal antibody (mAb) proteins in solution, dissipative particle dynamic computer simulation is used here to simulate a rigid-body mAb for up to about 200 ns. The total ISF together with the ISFs due to only the translational and rotational motions as well as their corresponding effective diffusion coefficients is calculated. The aforementioned approximation introduces appreciable errors to the calculated effective diffusion coefficients and the ISFs. For the effective diffusion coefficient, the error introduced by this approximation can be as large as about 10% even though the overall agreement is considered reasonable. Thus, we need to be cautious when interpreting the data with a small signal change. In addition, the accuracy of the calculated ISFs due to the finite computer simulation time is also discussed.

Pluronic-based lamellar phases: influence of polymer architecture on bilayer bending elasticity

ABSTRACT In this study, we investigate the influence of the block copolymer architecture on the bending elasticity of polymer-rich lamellar phases. In detail, we study the polymer-rich system water/o-xylene/Pluronic triblock copolymer/CTAB and change the polymer while keeping the mass ratios constant. We use neutron spin echo measurements (NSE) to determine κ. With the measurements we determine the relaxation rate of the bilayer bending mode and subsequently calculate the bilayer bending modulus κ using the Zilman-Granek approach [Zilman et al., Phys. Rev. Lett. 77, 4788–4791 (1996)]. Moreover, we have investigated the lamellar phases via small-angle X-ray scattering (SAXS) and have analysed the data with the modified Caillé theory to obtain the Caillé parameter η. Based on κ the bulk compression modulus can be calculated. Increasing values of κ are found with increasing EO and PO block size in the range of 3.8 to 13.4 T. The computed values of are in the range of 10 to 10 Pa.

Decomposing Magnetic Dark-Field Contrast in Spin Analyzed Talbot-Lau Interferometry: A Stern-Gerlach Experiment without Spatial Beam Splitting.

We have recently shown how a polarized beam in Talbot-Lau interferometric imaging can be used to analyze strong magnetic fields through the spin dependent differential phase effect at field gradients. While in that case an adiabatic spin coupling with the sample field is required, here we investigate a nonadiabatic coupling causing a spatial splitting of the neutron spin states with respect to the external magnetic field. This subsequently leads to no phase contrast signal but a loss of interferometer visibility referred to as dark-field contrast. We demonstrate how the implementation of spin analysis to the Talbot-Lau interferometer setup enables one to recover the differential phase induced to a single spin state. Thus, we show that the dark-field contrast is a measure of the quantum mechanical spin split analogous to the Stern-Gerlach experiment without, however, spatial beam separation. In addition, the spin analyzed dark-field contrast imaging introduced here bears the potential to probe polarization dependent small-angle scattering and thus magnetic microstructures.