Reflective, polarizing, and magnetically soft amorphous neutron optics with 11B-enriched B4C.

The utilization of polarized neutrons is of great importance in scientific disciplines spanning materials science, physics, biology, and chemistry. However, state-of-the-art multilayer polarizing neutron optics have limitations, particularly low specular reflectivity and polarization at higher scattering vectors/angles, and the requirement of high external magnetic fields to saturate the polarizer magnetization. Here, we show that, by incorporating 11B4C into Fe/Si multilayers, amorphization and smooth interfaces can be achieved, yielding higher neutron reflectivity, less diffuse scattering, and higher polarization. Magnetic coercivity is eliminated, and magnetic saturation can be reached at low external fields (>2 militesla). This approach offers prospects for substantial improvement in polarizing neutron optics with nonintrusive positioning of the polarizer, enhanced flux, increased data accuracy, and further polarizing/analyzing methods at neutron scattering facilities.

M-STAR: Magnetism second target advanced reflectometer at the Spallation Neutron Source.

M-STAR is a next generation polarized neutron reflectometer with advanced capabilities. A new focusing guide concept is optimized for samples with dimensions down to a millimeter range. A proposed hybrid pulse-skipping chopper will enable experiments at constant geometry at one incident angle in a broad range of wavevector transfer Q up to 0.3 A-1 for specular, off-specular, and GISANS measurements. M-STAR will empower nanoscience and spintronics studies routinely on small samples (∼2 × 2 mm2) and of atomic-scale thickness using versatile experimental conditions of magnetic and/or electric fields, light, and temperature applied in situ to novel complex device-like nanosystems with multiple buried interfaces. M-STAR will enable improved grazing incidence diffraction measurements, as a surface-sensitive depth-resolved probe of, e.g., the out-of-plane component of atomic magnetic moments in ferromagnetic, antiferromagnetic, and more complex structures as well as in-plane atomic-scale structures inaccessible with contemporary diffractometry and reflectometry. New horizons will be opened by the development of an option to probe near-surface dynamics with inelastic grazing incidence scattering in the time-of-flight mode. These novel options in combination with ideally matched parameters of the second target station will place M-STAR in the world's leading position for high resolution polarized reflectometry.

GenX 3: the latest generation of an established tool.

Since its publication more than 15 years ago the GenX software has been continuously developed and has established itself as a standard package for analyzing X-ray and neutron reflectometry data. The evolution of the software during the last two major revisions is reported here. This includes a simplified model builder for beginners, simple samples, additional sample models, statistical error analysis and the use of just-in-time compilation modules for the reflectometry kernel to achieve higher performance. In addition, the influence of experimental errors on the reflectivity curve is discussed, and new features are described that allow the user to include these in the error statistics to improve the fitting and uncertainty estimation.

Low temperature aging in a molecular glass: the case of cis-methyl formate.

Glassy films of cis-methyl formate show spontaneous dipole orientation on deposition from the vacuum, the so-called 'spontelectric effect', creating surface potentials and electric fields within the films. We follow the decay of these fields, and their accompanying dipole orientation, on the hours timescale at deposition temperatures between 40 K and 55 K. Our data trace the low temperature 'secondary decay' mechanism, at tens of degrees below the glass transition temperature of 90 K. We show that secondary decay is due to molecular rotation, with associated activation energies lying between 0.1 and 0.2 eV. Diffusion is absent, as established from published neutron reflectivity data. Using an analytical model for the spontelectric effect, data are placed on a quantitative footing, showing that angular motion in excess of 50° reproduces the observed values of activation energies. Exploitation of the spontelectric effect is new in the study of glass aging and is shown here to give insight into the elusive processes which take place far from the molecular glass transition temperature.

A mechanism for ageing in a deeply supercooled molecular glass.

Measurements of the decay of electric fields, formed spontaneously within vapour-deposited films of cis-methyl formate, provide the first direct assessment of the energy barrier to secondary relaxation in a molecular glass. At temperatures far below the glass transition temperature, the mechanism of relaxation is shown to be through hindered molecular rotation. Magnetically-polarised neutron scattering experiments exclude diffusion, which is demonstrated to take place only close to the glass transition temperature.

Direct observation of spin correlations in an artificial triangular lattice Ising spin system with grazing-incidence small-angle neutron scattering.

The triangular lattice with Ising magnetic moments is an archetypical example of geometric frustration. In the case of dipolar-coupled out-of-plane moments, the geometric frustration results in a disordered classical spin-liquid state at higher temperatures while the system is predicted to transition to an anti-ferromagnetic stripe ground state at low temperatures. In this work we fabricate artificial triangular Ising spin systems without and with uniaxial in-plane compression to tune the nature and temperature of the correlations. We probe the energy scale and nature of magnetic correlations by grazing-incidence small-angle neutron scattering. In particular, we apply a newly-developed empirical structure-factor model to describe the measured short-range correlated spin-liquid state, and find good agreement with theoretical predictions. We demonstrate that grazing-incidence neutron scattering on our high-quality samples, in conjunction with detailed modeling of the scattering using the Distorted Wave Born Approximation, can be used to experimentally quantify the spin-liquid-like correlations in highly-frustrated artificial spin systems.

Soliton-Mediated Magnetic Reversal in an All-Oxide-Based Synthetic Antiferromagnetic Superlattice.

All-oxide-based synthetic antiferromagnets (SAFs) are attracting intense research interest due to their superior tunability and great potentials for antiferromagnetic spintronic devices. In this work, using the La2/3Ca1/3MnO3/CaRu1/2Ti1/2O3 (LCMO/CRTO) superlattice as a model SAF, we investigated the layer-resolved magnetic reversal mechanism by polarized neutron reflectivity. We found that the reversal of LCMO layer moments is mediated by nucleation, expansion, and shrinkage of a magnetic soliton. This unique magnetic reversal process creates a reversed magnetic configuration of the SAF after a simple field cycling. Therefore, it can enable vertical data transfer from the bottom to the top of the superlattice. The physical origin of this intriguing magnetic reversal process could be attributed to the cooperation of the surface spin-flop effect and enhanced uniaxial magnetic anisotropy of the bottom LCMO layer. This work may pave a way to utilize all-oxide-based SAFs for three-dimensional spintronic devices with vertical data transfer and high-density data storage.

Strong size selectivity in the self-assembly of rounded nanocubes into 3D mesocrystals.

The self-assembly of nanoparticles into highly ordered crystals is largely influenced by variations in the size and shape of the constituent particles, with crystallization generally not observed if their polydispersity is too large. Here, we report on size selectivity in the self-assembly of rounded cubic maghemite nanoparticles into three-dimensional mesocrystals. Different X-ray scattering techniques are used to study and compare a nanoparticle dispersion that is used later for self-assembly, an ensemble of mesocrystals grown on a substrate, as well as an individual mesocrystal. The individual µm-sized mesocrystal is isolated using a focused-ion-beam-based technique and investigated by the diffraction of a micro-focused X-ray beam. Structural analysis reveals that individual mesocrystals have a drastically smaller size dispersity of nanoparticles than that in the initial dispersion, implying very strong size selectivity during self-assembly. The small size dispersity of the nanoparticles within individual mesocrystals is accompanied by a very narrow lattice parameter distribution. In contrast, the lattice parameter distribution within all mesocrystals of an ensemble is about four times wider than that of individual mesocrystals, indicating significant size fractionalization between mesocrystals during self-assembly. The small size dispersity within each mesocrystal has important implications for their physical properties.

Spin Solid versus Magnetic Charge Ordered State in Artificial Honeycomb Lattice of Connected Elements.

The nature of magnetic correlation at low temperature in two-dimensional artificial magnetic honeycomb lattice is a strongly debated issue. While theoretical researches suggest that the system will develop a novel zero entropy spin solid state as T → 0 K, a confirmation to this effect in artificial honeycomb lattice of connected elements is lacking. This study reports on the investigation of magnetic correlation in newly designed artificial permalloy honeycomb lattice of ultrasmall elements, with a typical length of ≈12 nm, using neutron scattering measurements and temperature-dependent micromagnetic simulations. Numerical modeling of the polarized neutron reflectometry data elucidates the temperature-dependent evolution of spin correlation in this system. As temperature reduces to ≈7 K, the system tends to develop novel spin solid state, manifested by the alternating distribution of magnetic vortex loops of opposite chiralities. Experimental results are complemented by temperature-dependent micromagnetic simulations that confirm the dominance of spin solid state over local magnetic charge ordered state in the artificial honeycomb lattice with connected elements. These results enable a direct investigation of novel spin solid correlation in the connected honeycomb geometry of 2D artificial structure.

HEKATE-A novel grazing incidence neutron scattering concept for the European Spallation Source.

Structure and magnetism at surfaces and buried interfaces on the nanoscale can only be accessed by few techniques, one of which is grazing incidence neutron scattering. While the technique has its strongest limitation in a low signal and large background, due to the low scattering probability and need for high resolution, it can be expected that the high intensity of the European Spallation Source in Lund, Sweden, will make many more such studies possible, warranting a dedicated beamline for this technique. We present an instrument concept, Highly Extended K range And Tunable Experiment (HEKATE), for surface scattering that combines the advantages of two Selene neutron guides with unique capabilities of spatially separated distinct wavelength frames. With this combination, it is not only possible to measure large specular reflectometry ranges, even on free liquid surfaces, but also to use two independent incident beams with tunable sizes and resolutions that can be optimized for the specifics of the investigated samples. Further the instrument guide geometry is tuned for reduction of high energy particle background and only uses low to moderate supermirror coatings for high reliability and affordable cost.

Superlattice growth and rearrangement during evaporation-induced nanoparticle self-assembly.

Understanding the assembly of nanoparticles into superlattices with well-defined morphology and structure is technologically important but challenging as it requires novel combinations of in-situ methods with suitable spatial and temporal resolution. In this study, we have followed evaporation-induced assembly during drop casting of superparamagnetic, oleate-capped γ-Fe2O3 nanospheres dispersed in toluene in real time with Grazing Incidence Small Angle X-ray Scattering (GISAXS) in combination with droplet height measurements and direct observation of the dispersion. The scattering data was evaluated with a novel method that yielded time-dependent information of the relative ratio of ordered (coherent) and disordered particles (incoherent scattering intensities), superlattice tilt angles, lattice constants, and lattice constant distributions. We find that the onset of superlattice growth in the drying drop is associated with the movement of a drying front across the surface of the droplet. We couple the rapid formation of large, highly ordered superlattices to the capillary-induced fluid flow. Further evaporation of interstitital solvent results in a slow contraction of the superlattice. The distribution of lattice parameters and tilt angles was significantly larger for superlattices prepared by fast evaporation compared to slow evaporation of the solvent.

High-quality EuO thin films the easy way via topotactic transformation.

Epitaxy is widely employed to create highly oriented crystalline films. A less appreciated, but nonetheless powerful means of creating such films is via topotactic transformation, in which a chemical reaction transforms a single crystal of one phase into a single crystal of a different phase, which inherits its orientation from the original crystal. Topotactic reactions may be applied to epitactic films to substitute, add or remove ions to yield epitactic films of different phases. Here we exploit a topotactic reduction reaction to provide a non-ultra-high vacuum (UHV) means of growing highly oriented single crystalline thin films of the easily over-oxidized half-metallic semiconductor europium monoxide (EuO) with a perfection rivalling that of the best films of the same material grown by molecular-beam epitaxy or UHV pulsed-laser deposition. As the technique only requires high-vacuum deposition equipment, it has the potential to drastically improve the accessibility of high-quality single crystalline films of EuO as well as other difficult-to-synthesize compounds.