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SignificanceThe exactly solvable Kitaev model of bond-dependent near-neighbor interactions has drawn attention to quantum spins on the honeycomb lattice. But exotic quantum magnetism may also arise from competing interactions beyond nearest neighbors. Combining state-of- the-art theory and neutron scattering, we show that ferromagnetic nearest-neighbor interactions between effective spin-1/2 Co2+ spins in BaCo2(AsO4)2 are frustrated by antiferromagnetic third neighbor interactions. While an in-plane field suppresses the resulting incommensurate order, a ĉ−oriented field enhances quantum fluctuations. The spin Hamiltonian that we obtain will inform the search for quantum spin liquid physics in BaCo2(AsO4)2 subjected to tilted fields. Recently, Co-based honeycomb magnets have been proposed as promising candidate materials to host the Kitaev spin liquid (KSL) state. One of the front-runners is BaCo2(AsO4)2 (BCAO), where it was suggested that the exchange processes between Co2+ ions via the surrounding edge-sharing oxygen octahedra could give rise to bond-dependent Kitaev interactions. In this work, we present and analyze a comprehensive inelastic neutron scattering (INS) study of BCAO with fields in the honeycomb plane. Combining the constraints from the magnon excitations in the high-field polarized state and the inelastic spin structure factor measured in zero magnetic field, we examine two leading theoretical models: the Kitaev-type JKΓΓ′ model and the XXZ-J1-J3model. We show that the existing experimental data can be consistently accounted for by the XXZ-J1-J3model but not by the JKΓΓ′ model, and we discuss the implications of these results for the realization of a spin liquid phase in BCAO and more generally for the realization of the Kitaev model in cobaltates.

Advanced batteries require advanced characterization techniques, and neutron scattering is one of the most powerful experimental methods available for studying next-generation battery materials. Neutron scattering offers a non-destructive method to probe the complex structural and chemical processes occurring in batteries during operation in truly in situ/in operando measurements with a high sensitivity to battery-relevant elements such as lithium. Neutrons have energies comparable to the energies of excitations in materials and wavelengths comparable to atomic distances in the solid state, thus giving access to study structural and dynamical properties of materials on an atomic scale. In this review, a broad overview of selected neutron scattering techniques is presented to illustrate how neutron scattering can be used to gain invaluable information of solid-state battery materials, with a focus on in situ/in operando methods. These techniques span multiple decades of length and time scales to uncover the complex processes taking place fundamentally on the atomic scale and to determine how these processes impact the macroscale properties and performance of functional battery systems. This review serves the solid-state battery research community by examining how the unique capabilities of neutron scattering can be applied to answer critical and unresolved questions of materials research in this field. A thorough and broad perspective is provided with numerous practical examples showing these techniques in action for battery research.

Despite the widespread use of silicon in modern technology, its peculiar thermal expansion is not well understood. Adapting harmonic phonons to the specific volume at temperature, the quasiharmonic approximation, has become accepted for simulating the thermal expansion, but has given ambiguous interpretations for microscopic mechanisms. To test atomistic mechanisms, we performed inelastic neutron scattering experiments from 100 K to 1,500 K on a single crystal of silicon to measure the changes in phonon frequencies. Our state-of-the-art ab initio calculations, which fully account for phonon anharmonicity and nuclear quantum effects, reproduced the measured shifts of individual phonons with temperature, whereas quasiharmonic shifts were mostly of the wrong sign. Surprisingly, the accepted quasiharmonic model was found to predict the thermal expansion owing to a large cancellation of contributions from individual phonons.

The development of qualitatively new measurement capabilities is often a prerequisite for critical scientific and technological advances. Here we introduce an unconventional quantum probe, an entangled neutron beam, where individual neutrons can be entangled in spin, trajectory and energy. The spatial separation of trajectories from nanometers to microns and energy differences from peV to neV will enable investigations of microscopic magnetic correlations in systems with strongly entangled phases, such as those believed to emerge in unconventional superconductors. We develop an interferometer to prove entanglement of these distinguishable properties of the neutron beam by observing clear violations of both Clauser-Horne-Shimony-Holt and Mermin contextuality inequalities in the same experimental setup. Our work opens a pathway to a future of entangled neutron scattering in matter. Exploring correlations in strongly entangled quantum materials is of interest. Here the authors generate a tunable spin-, trajectory-, and energy-entangled neutron beam using a neutron spin-echo interferometer and show violations of Clauser-Horne-Shimony-Holt and Mermin contextuality inequalities with micron-scale trajectory separation.

Understanding the nature and origin of collective excitations in materials is of fundamental importance for unraveling the underlying physics of a many-body system. Excitation spectra are usually obtained by measuring the dynamical structure factor, S ( Q ,  ω ), using inelastic neutron or x-ray scattering techniques and are analyzed by comparing the experimental results against calculated predictions. We introduce a data-driven analysis tool which leverages ‘neural implicit representations’ that are specifically tailored for handling spectrographic measurements and are able to efficiently obtain unknown parameters from experimental data via automatic differentiation. In this work, we employ linear spin wave theory simulations to train a machine learning platform, enabling precise exchange parameter extraction from inelastic neutron scattering data on the square-lattice spin-1 antiferromagnet La 2 NiO 4 , showcasing a viable pathway towards automatic refinement of advanced models for ordered magnetic systems. Analysis of experimental data in condensed matter is often challenging due to system complexity and slow character of physical simulations. The authors propose a framework that combines machine learning with theoretical calculations to enable real-time analysis for electron, neutron, and x-ray spectroscopies.

Uncharged bottlebrush polymer melts and highly charged polyelectrolytes in solution exhibit correlation peaks in scattering measurements and simulations. Given the striking superficial similarities of these scattering features, there may be a deeper structural interrelationship in these chemically different classes of materials. Correspondingly, we constructed a library of isotopically labeled bottlebrush molecules and measured the bottlebrush correlation peak position q* = 2π/ξ by neutron scattering and in simulations. We find that the correlation length scales with the backbone concentration, ξ ∼ c B B − 0.47 , in striking accord with the scaling of ξ with polymer concentration cP in semidilute polyelectrolyte solutions ( ξ ∼ c P − 1 / 2 ). The bottlebrush correlation peak broadens with decreasing grafting density, similar to increasing salt concentration in polyelectrolyte solutions. ξ also scales with sidechain length to a power in the range of 0.35–0.44, suggesting that the sidechains are relatively collapsed in comparison to the bristlelike configurations often imagined for bottlebrush polymers.

Hydrogen-containing materials are of fundamental as well as technological interest. An outstanding question for both is the amount of hydrogen that can be incorporated in such materials, because that determines dramatically their physical properties such as electronic and crystalline structure. The number of hydrogen atoms in a metal is controlled by the interaction of hydrogens with the metal and by the hydrogen–hydrogen interactions. It is well established that the minimal possible hydrogen–hydrogen distances in conventional metal hydrides are around 2.1 Å under ambient conditions, although closer H–H distances are possible for materials under high pressure. We present inelastic neutron scattering measurements on hydrogen in ZrV₂Hₓ showing nonexpected scattering at low-energy transfer. The analysis of the spectra reveals that these spectral features in part originate from hydrogen vibrations confined by neighboring hydrogen at distances as short as 1.6 Å. These distances are much smaller than those found in related hydrides, thereby violating the so-called Switendick criterion. The results have implications for the design and creation of hydrides with additional properties and applications.

The physics of mutual interaction of phonon quasiparticles with electronic spin degrees of freedom, leading to unusual transport phenomena of spin and heat, has been a subject of continuing interests for decades. Despite its pivotal role in transport processes, the effect of spin-phonon coupling on the phonon system, especially acoustic phonon properties, has so far been elusive. By means of inelastic neutron scattering and first-principles calculations, anomalous scattering spectral intensity from acoustic phonons was identified in the exemplary collinear antiferromagnetic nickel (II) oxide, unveiling strong spin-lattice correlations that renormalize the polarization of acoustic phonon. In particular, a clear magnetic scattering signature of the measured neutron scattering intensity from acoustic phonons is demonstrated by its momentum transfer and temperature dependences. The anomalous scattering intensity is successfully modeled with a modified magneto-vibrational scattering cross-section, suggesting the presence of spin precession driven by phonon. The renormalization of phonon eigenvector is indicated by the observed “geometry-forbidden” neutron scattering intensity from transverse acoustic phonon. Importantly, the eigenvector renormalization cannot be explained by magnetostriction but instead, it could result from the coupling between phonon and local magnetization of ions.

Aluminum-based adjuvants are widely used in vaccine formulations due to their immunostimulatory properties and strong safety profile. Despite their effectiveness and safety, the exact mechanisms by which they enhance vaccine efficacy remain unclear. One proposed mechanism is that aluminum adjuvants form a depot that gradually releases antigens, thereby improving antigen uptake by antigen-presenting cells. This study investigates the porous structures of two commonly used aluminum adjuvants, aluminum hydroxide (AH) and aluminum phosphate (AP), using small-angle X-ray scattering (SAXS) and small-angle neutron scattering (SANS). Our measurements reveal that AH nanoparticles, with their needle-like morphology, form smaller, interconnected pores within the aggregated architecture. In contrast, AP nanoparticles, with a plate-like shape, form more discrete, isolated porous structures. Both adjuvants have pore sizes within the range of commonly used vaccine antigens, supporting the depot theory. Our findings also reveal that antigen retention is prolonged when the antigen size is comparable to the average pore size of the adjuvant. This study highlights the utility of SAXS and SANS for in-situ characterization of adjuvant porosity and provides insights into how nanoparticle morphology affects antigen retention and release. By elucidating these structural details, our research underscores the importance of porous structure in adjuvant function and offers potential pathways for improving vaccine formulations through tailored adjuvant design.

Polarisation analysis for neutron scattering experiments is a powerful tool suitable for a wide variety of studies, including soft-matter samples which have no bulk magnetic behaviour and/or a significant hydrogen content. Here, we describe a method to leverage the versatility and spin-polarisation capabilities of a cold triple-axis spectrometer to perform a measurement to separate coherent and incoherent neutron scattering for a non-magnetic sample in the quasielastic neutron scattering (QENS) regime. Such measurements are complementary to unpolarised QENS measurements, which may typically be performed on a backscattering or time-of-flight spectrometer instrument where polarisation analysis can be significantly more difficult to achieve, and utilise the strengths of each type of instrument.