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A large body of knowledge about magnetism is attained from models of interacting spins, which usually reside on magnetic ions. Proposals beyond the ionic picture are uncommon and seldom verified by direct observations in conjunction with microscopic theory. Here, using inelastic neutron scattering to study the itinerant near-ferromagnet MnSi, we find that the system's fundamental magnetic units are interconnected, extended molecular orbitals consisting of three Mn atoms each, rather than individual Mn atoms. This result is further corroborated by magnetic Wannier orbitals obtained by ab initio calculations. It contrasts the ionic picture with a concrete example, and presents a novel regime of the spin waves where the wavelength is comparable to the spatial extent of the molecular orbitals. Our discovery brings important insights into not only the magnetism of MnSi, but also a broad range of magnetic quantum materials where structural symmetry, electron itinerancy and correlations act in concert., Comment: 27 pages, 27 figures including supplemental; comments are welcome

Competition among exchange interactions is able to induce novel spin correlations on a bipartite lattice without geometrical frustration. A prototype example is the spiral spin liquid, which is a correlated paramagnetic state characterized by sub-dimensional degenerate propagation vectors. Here, using spectral graph theory, we show that spiral spin liquids on a bipartite lattice can be approximated by a further-neighbor model on the corresponding line-graph lattice that is non-bipartite, thus broadening the space of candidate materials that may support the spiral spin liquid phases. As illustrations, we examine neutron scattering experiments performed on two spinel compounds, ZnCr$_2$Se$_4$ and CuInCr$_4$Se$_8$, to demonstrate the feasibility of this new approach and expose its possible limitations in experimental realizations., Comment: 20 pages, 18 figures

Spiral spin-liquids are correlated paramagnetic states with degenerate propagation vectors forming a continuous ring or surface in reciprocal space. On the honeycomb lattice, spiral spin-liquids present a novel route to realize emergent fracton excitations, quantum spin liquids, and topological spin textures, yet experimental realizations remain elusive. Here, using neutron scattering, we show that a spiral spin-liquid is realized in the van der Waals honeycomb magnet FeCl$_3$. A continuous ring of scattering is directly observed, which indicates the emergence of an approximate U(1) symmetry in momentum space. Our work demonstrates that spiral spin-liquids can be achieved in two-dimensional systems and provides a promising platform to study the fracton physics in spiral spin-liquids., Comment: 16 pages, 14 figures

Classical hydrodynamics is a remarkably versatile description of the coarse-grained behavior of many-particle systems once local equilibrium has been established. The form of the hydrodynamical equations is determined primarily by the conserved quantities present in a system. Some quantum spin chains are known to possess, even in the simplest cases, a greatly expanded set of conservation laws, and recent work suggests that these laws strongly modify collective spin dynamics even at high temperature. Here, by probing the dynamical exponent of the one-dimensional Heisenberg antiferromagnet KCuF$_3$ with neutron scattering, we find evidence that the spin dynamics are well described by the dynamical exponent $z=3/2$, which is consistent with the recent theoretical conjecture that the dynamics of this quantum system are described by the Kardar-Parisi-Zhang universality class. This observation shows that low-energy inelastic neutron scattering at moderate temperatures can reveal the details of emergent quantum fluid properties like those arising in non-Fermi liquids in higher dimensions., 12 pages and 4 figures. Includes 1 pages of methods and >> 1 pages Supplementary Information

In quantum magnets, magnetic moments fluctuate heavily and are strongly entangled with each other, a fundamental distinction from classical magnetism. Here, with inelastic neutron scattering measurements, we probe the spin correlations of the honeycomb lattice quantum magnet YbCl3. A linear spin wave theory with a single Heisenberg interaction on the honeycomb lattice, including both transverse and longitudinal channels of the neutron response, reproduces all of the key features in the spectrum. In particular, we identify a Van Hove singularity, a clearly observable sharp feature within a continuum response. The demonstration of such a Van Hove singularity in a two-magnon continuum is important as a confirmation of broadly held notions of continua in quantum magnetism and additionally because analogous features in two-spinon continua could be used to distinguish quantum spin liquids from merely disordered systems. These results establish YbCl3 as a benchmark material for quantum magnetism on the honeycomb lattice., Honeycomb lattices with interacting spins can host rich magnetic behaviour; however, typically features are complicated by additional interactions. Here, the authors perform neutron scattering on YbCl3, which exhibits near perfect two-dimensional magnetism, providing a benchmark for other materials.

The kagome lattice is a fertile platform to explore topological excitations with both Fermi-Dirac and Bose-Einstein statistics. While relativistic Dirac Fermions and flat-bands have been discovered in the electronic structure of kagome metals, the spin excitations have received less attention. Here we report inelastic neutron scattering studies of the prototypical kagome magnetic metal FeSn. The spectra display well-defined spin waves extending up to 120 meV. Above this energy, the spin waves become progressively broadened, reflecting interactions with the Stoner continuum. Using linear spin wave theory, we determine an effective spin Hamiltonian that reproduces the measured dispersion. This analysis indicates that the Dirac magnon at the K-point remarkably occurs on the brink of a region where well-defined spin waves become unobservable. Our results emphasize the influential role of itinerant carriers on the topological spin excitations of metallic kagome magnets., 6 pages, 4 figures

For topological magnon spectra, determining and explaining the presence of a gap at a magnon crossing point is a key to characterize the topological properties of the system. An inelastic neutron scattering study of a single crystal is a powerful experimental technique that is widely employed to probe the magnetic excitation spectra of topological materials. Here, we show that when the scattering intensity rapidly disperses in the vicinity of a crossing point, such as a Dirac point, the apparent topological gap size is extremely sensitive to experimental conditions including sample mosaic, resolution, and momentum integration range. We demonstrate these effects using comprehensive neutron-scattering measurements of CrCl$_3$. Our measurements confirm the gapless nature of the Dirac magnon in CrCl$_3$, but also reveal an artificial, i.e. extrinsic, magnon gap unless the momentum integration range is carefully controlled. Our study provides an explanation of the apparent discrepancies between spectroscopic and first-principles estimates of Dirac magnon gap sizes, and provides guidelines for accurate spectroscopic measurement of topological magnon gaps., 6 pages and 4 figures

The thermally activated dynamics of methyl groups are important for biochemical activity as they allow for a more efficient sampling of the energy landscape. Here, we compare methyl rotations in the dry and variously hydrated states of three primary drugs under consideration to treat the recent coronavirus disease (COVID-19), namely, hydroxychloroquine and its sulfate, dexamethasone and its sodium diphosphate, and remdesivir. We find that the main driving force behind the considerable reduction in the activation energy for methyl rotations in the hydrated state is the hydration-induced disorder in the methyl group local environments. Furthermore, the activation energy for methyl rotations in the hydration-induced disordered state is much lower than that in an isolated drug molecule, indicating that neither isolated molecules nor periodic crystalline structures can be used to analyze the potential landscape governing the side group dynamics in drug molecules. Instead, only the explicitly considered disordered structures can provide insight.

Research examining radiation damage and its effects in graphite began in the 1940’s during the development of moderated nuclear reactors. Interest in this topic is expanding because of emerging applications associated with fullerenes and carbon nanostructures as well as its long-standing use as a fission moderator. In this work, we report the measurements of the full phonon density of states of irradiated nuclear graphite using inelastic neutron scattering experiments at room temperature. The samples were previously exposed to different levels of neutron doses and irradiation temperatures. The phonon density of states of perfect and defected graphite supercells including different configurations of vacancies and interstitials were calculated using first-principles direct method. Despite high neutron irradiation doses, the scattering measurements show that the induced damage is localized, and the layered structure is preserved. A comparison of the measured phonon densities of states of irradiated samples with those calculated of defected supercells indicates that the main changes observed are mainly attributed to formation of vacancies.

We report the static and dynamic magnetic properties of LaSrCrO$_4$, a seemingly canonical spin-3/2 square-lattice antiferromagnet that exhibits frustration between magnetic layers -- owing to their AB stacking -- and offers a rare testbed to investigate accidental-degeneracy lifting in magnetism. Neutron diffraction experiments on single-crystal samples uncover a remarkable anticollinear magnetic order below $T_N$ = 170 K characterized by a N\'eel arrangement of the spins within each layer and an orthogonal arrangement between adjacent layers. To understand the origin of this unusual magnetic structure, we analyze the spin-wave excitation spectrum by means of inelastic neutron scattering and bulk measurements. A spectral gap of 0.5 meV, along with a spin-flop transition at 3.2\, T, reflect the energy scale associated with the degeneracy-lifting. A minimal model to explain these observations requires both a positive biquadratic interlayer exchange and dipolar interactions, both of which are on the order of 10$^{-4}$ meV, only a few parts per million of the dominant exchange interaction $J_1 \approx 11$ meV. These results provide direct evidence for the selection of a non-collinear magnetic structure by the combined effect of two distinct degeneracy lifting interactions., Comment: 6 pages of main tex with 16 pages of supplemental material

Inelastic neutron scattering (INS) is a powerful technique to study vibrational dynamics of materials with several unique advantages. However, analysis and interpretation of INS spectra often require advanced modeling that needs specialized computing resources and relevant expertise. This difficulty is compounded by the limited experimental resources available to perform INS measurements. In this work, we develop a machine-learning based predictive framework which is capable of directly predicting both one-dimensional INS spectra and two-dimensional INS spectra with additional momentum resolution. By integrating symmetry-aware neural networks with autoencoders, and using a large scale synthetic INS database, high-dimensional spectral data are compressed into a latent-space representation, and a high-quality spectra prediction is achieved by using only atomic coordinates as input. Our work offers an efficient approach to predict complex multi-dimensional neutron spectra directly from simple input; it allows for improved efficiency in using the limited INS measurement resources, and sheds light on building structure-property relationships in a variety of on-the-fly experimental data analysis scenarios.

With the rise of interest in thermal neutron scattering data for advanced reactor, criticality safety, and shielding applications, new experimental data are required for evaluation of new materials or for re-evaluation (or validations) of previously evaluated materials. New experimental data are evaluated in a three-step process: (1) computing the phonon characteristics, (2) computing the dynamic structure factor (DSF) from the data, and (3) using the experimental setup to simulate the experimental data. All three steps have challenges, ranging from the need for a suffciently general material simulation code—a processing code that can compute the corresponding DSF—to having a detailed layout of the instrument/beamline/facility where the data were measured. Whereas phonon characteristics of materials can be computed using various methods (molecular dynamics, density functional theory, etc.), a high-fidelity computation of the DSF and the simulation of the experiment based on the DSF is vital to the accuracy of the evaluation. The latter two steps can be achieved by using the two corresponding code systems developed by instrument scientists at the Spallation Neutron Source (SNS) at Oak Ridge National Laboratory: (1) OCLIMAX, a program that calculates the dynamic structure factor from DFT and MD simulation results, and (2) MCViNE, a Monte Carlo neutron ray-tracing program designed to simulate neutron scattering experiments. Recently, polyethylene and yttrium hydride were measured at the Wide Angular-Range Chopper (ARCS) and SEQUOIA instrument stations of the SNS. These experiments are simulated using the density functional theory code, the Cambridge Serial Total Energy Package (CASTEP), to compute its phonon characteristics (eigenvalues/vectors and PDOS), which is then processed using OCLIMAX to yield the DSF, and finally the data at each instrument station are simulated by the MCViNE for comparison to the measured data for evaluation. For comparison to conventional evaluation methods, the scattering data processed from OCLIMAX are compared against those processed from the LEAPR module of NJOY, and the results from MCViNE simulations are compared against previously used simplified beamline models implemented in the Monte Carlo N-Particle (MCNP) code.

Swedenborgite Ca${}_{0.5}$Y${}_{0.5}$BaCo${}_{4}$O${}_{7}$, with geometrically frustrated kagome and triangular lattices, exhibits a disordered ground state in spite of strong antiferromagnetic coupling between the Co spins. Here, the authors perform single-crystal diffuse neutron scattering experiments to fully characterize the short-range spin correlations in this compound and determine that long-range incommensurate spin correlations are suppressed by exchange disorder. This result reveals a general correspondence between unequal interactions and incommensurate spin correlations on the swedenborgite lattice.

Spin and lattice are two fundamental degrees of freedom in a solid, and their fluctuations about the equilibrium values in a magnetic ordered crystalline lattice form quasiparticles termed magnons (spin waves) and phonons (lattice waves), respectively. In most materials with strong spin-lattice coupling (SLC), the interaction of spin and lattice induces energy gaps in the spin wave dispersion at the nominal intersections of magnon and phonon modes. Here we use neutron scattering to show that in the two-dimensional (2D) van der Waals honeycomb lattice ferromagnetic CrGeTe

Understanding magnetism and its possible correlations to topological properties has emerged to the forefront as a difficult topic in studying magnetic Weyl semimetals. ${\mathrm{Co}}_{3}{\mathrm{Sn}}_{2}{\mathrm{S}}_{2}$ is a newly discovered magnetic Weyl semimetal with a kagome lattice of cobalt ions and has triggered intense interest for rich fantastic phenomena. Here, we report the magnetic exchange couplings of ${\mathrm{Co}}_{3}{\mathrm{Sn}}_{2}{\mathrm{S}}_{2}$ using inelastic neutron scattering and two density functional theory (DFT) based methods: constrained magnetism and multiple-scattering Green's function methods. ${\mathrm{Co}}_{3}{\mathrm{Sn}}_{2}{\mathrm{S}}_{2}$ exhibits highly anisotropic magnon dispersions and linewidths below ${T}_{C}$, and paramagnetic excitations above ${T}_{C}$. The spin-wave spectra in the ferromagnetic ground state is well described by the dominant third-neighbor ``across-hexagon'' ${J}_{d}$ model. Our density functional theory calculations reveal that both the symmetry-allowed 120\ifmmode^\circ\else\textdegree\fi{} antiferromagnetic orders support Weyl points in the intermediate temperature region, with distinct numbers and the locations of Weyl points. Our study highlights the important role ${\mathrm{Co}}_{3}{\mathrm{Sn}}_{2}{\mathrm{S}}_{2}$ can play in advancing our understanding of kagome physics and exploring the interplay between magnetism and band topology.

Magnetic frustration, arising from the competition of exchange interactions, has received great attention because of its relevance to exotic quantum phenomena in materials. In the current work, we report an unusual checkerboard-shaped scattering anomaly in $\rm FeGe_2$, far from the known incommensurate magnetic satellite peaks, for the first time by inelastic neutron scattering. More surprisingly, such phenomenon appears as spin dynamics at low temperature, but it becomes prominent above N\'eel transition as elastic scattering. A new model Hamiltonian that includes an intraplane next-nearest neighbor was proposed and attributes such anomaly to the near-perfect magnetic frustration and the emergence of unexpected two-dimensional magnetic order in the quasi-one-dimensional $\rm FeGe_2$., Comment: 24 pages, 10 figures

The search for topological spin excitations in recently discovered two-dimensional (2D) van der Waals (vdW) magnetic materials is important because of their potential applications in dissipationless spintronics. In the 2D vdW ferromagnetic (FM) honeycomb lattice CrI_{3} (T_{C}=61 K), acoustic and optical spin waves are found to be separated by a gap at the Dirac points. The presence of such a gap is a signature of topological spin excitations if it arises from the next-nearest-neighbor (NNN) Dzyaloshinskii-Moriya (DM) or bond-angle-dependent Kitaev interactions within the Cr honeycomb lattice. Alternatively, the gap is suggested to arise from an electron correlation effect not associated with topological spin excitations. Here, we use inelastic neutron scattering to conclusively demonstrate that the Kitaev interactions and electron correlation effects cannot describe spin waves, Dirac gaps, and their in-plane magnetic field dependence. Our results support the idea that the DM interactions are the microscopic origin of the observed Dirac gap. Moreover, we find that the nearest-neighbor (NN) magnetic exchange interactions along the c axis are antiferromagnetic (AF), and the NNN interactions are FM. Therefore, our results unveil the origin of the observed c-axis AF order in thin layers of CrI_{3}, firmly determine the microscopic spin interactions in bulk CrI_{3}, and provide a new understanding of topology-driven spin excitations in 2D vdW magnets.

Nd-based pyrochlore oxides have garnered significant interest owing to the moment-fragmentation physics observed in Nd${}_{2}$Zr${}_{2}$O${}_{7}$ and speculated in Nd${}_{2}$Hf${}_{2}$O${}_{7}$. Notably, this phenomenon is absent in Nd${}_{2}$Sn${}_{2}$O${}_{7}$, which features a smaller $B$-site ionic radius. Here, bulk characterization and neutron scattering measurements reveal a similar absence of moment fragmentation in Nd${}_{2}$GaSbO${}_{7}$, which is characterized by significant $B$-site disorder and an extremely small average ionic radius on the $B$ site. These results may indicate that chemical pressure (and not necessarily the $B$-site disorder) plays a key role in the presence or absence of this exotic phenomenon.

Single crystals of the underscreened Kondo ferromagnet Yb14MnSb11 were investigated using polarised neutron diffraction and magnetisation measurements. The magnitude and direction of the ma...

The SEQUOIA direct geometry chopper spectrometer at the Spallation Neutron Source is considering acquisition of a radial collimator. We present here Monte-Carlo calculations examining the proposed collimator's performance. Through comparison of calculations with and without sample environments in place, one can determine appropriate parameters to use in the collimator design. The numerical results provide enough detail to determine the angular collimation for the radial collimator.

Spin liquid ground states are predicted to arise within several distinct scenarios in condensed matter physics. The observation of these disordered magnetic states is particularly pervasive amongst a class of materials known as frustrated magnets, in which the competition between various magnetic exchange interactions prevents the system from adopting long-range magnetic order at low temperatures. Spin liquids continue to be of great interest due to their exotic nature and the possibility that they may support fractionalised excitations, such as Majorana fermions. Systems that allow for such phenomena are not only fascinating from a fundamental perspective but may also be practically significant in future technologies based on quantum computation. Here we show that the underlying antiferromagnetic sublattice in TbInO$_3$ undergoes a crystal field induced triangular-to-honeycomb dilution at low temperatures. The absence of a conventional magnetic ordering transition at the lowest measurable temperatures indicates that another critical mechanism must govern in the ground state selection of TbInO$_3$. We propose that anisotropic exchange interactions, mediated through strong spin-orbit coupling on the emergent honeycomb lattice of TbInO$_3$, give rise to a highly frustrated spin liquid., Comment: 23 pages, 5 figures, supporting information

Low temperature powder inelastic neutron scattering measurements were performed on three different powder samples; parent BaMn 2 As 2 ,12.5% K-doped Ba 0.875 K 0.125 Mn 2 As 2 and 25% K-doped Ba ( 0.75 ) K 0.25 Mn 2 As 2 . The Heisenberg Model involving J 1 ‐ J 2 ‐ J z coupling constants were compared to the data by a powder integration routine using Monte Carlo integration methods. The best magnetic parameters were selected using a chi-square test where model intensities were compared to the full (q,E) dependence of magnetic scattering. A key step to this analysis is the characterization of the background which is formed mostly by phonon scattering intensities along with other sources including the magnetic impurity scattering events. The calculated powder magnetic intensities added to the estimated background obtained from the non-magnetic high momentum transfer region. The agreement between the simulated and the raw data enabled us to perform quantitative analysis of the unreacted MnO impurities. Overall, this is another confirmation along with earlier studies using this technique, that magnetic exchange constants can be calculated within an acceptable range with a very quick inelastic neutron powder experiment without need for a single crystal sample.

The magnetic ground state of the pyrochlore Yb2GaSbO7 has not been established. The persistent spin fluctuations observed by muon spin-relaxation measurements at low temperatures have not been adequately explained for this material using existing theories for quantum magnetism. Here we report on the synthesis and characterisation of Yb2GaSbO7 to revisit the nature of the magnetic ground state. Through DC and AC magnetic susceptibility, heat capacity, and neutron scattering experiments, we observe evidence for a dynamical ground state that makes Yb2GaSbO7 a promising candidate for disorder-induced spin-liquid or spin-singlet behaviour. This state is quite fragile, being tuned to a splayed ferromagnet in a modest magnetic field μ0Hc ~ 1.5 T.

The authors describe a method to analyze crystal field excitation spectra using adjustable effective point-charges and apply to two families of materials.

In two-dimensional (2D) metallic kagome lattice materials, destructive interference of electronic hopping pathways around the kagome bracket can produce nearly localized electrons, and thus electronic bands that are flat in momentum space. When ferromagnetic order breaks the degeneracy of the electronic bands and splits them into the spin-up majority and spin-down minority electronic bands, quasiparticle excitations between the spin-up and spin-down flat bands should form a narrow localized spin-excitation Stoner continuum coexisting with well-defined spin waves in the long wavelengths. Here we report inelastic neutron scattering studies of spin excitations in 2D metallic kagome lattice antiferromagnetic FeSn and paramagnetic CoSn, where angle resolved photoemission spectroscopy experiments found spin-polarized and nonpolarized flat bands, respectively, below the Fermi level. Our measurements on FeSn and CoSn reveal well-defined spin waves extending above 140 meV and correlated paramagnetic scattering around Γ point below 90 meV, respectively. In addition, we observed non-dispersive excitations at ~170 meV and ~360 meV arising mostly from hydrocarbon scattering of the CYTOP-M used to glue the samples to aluminum holder. Therefore, our results established the evolution of spin excitations in FeSn and CoSn, and identified anomalous flat modes overlooked by the neutron scattering community for many years. By exploiting the geometric frustration of a kagome crystal lattice, it is possible to enhance electron localisation and engineer exotic electronic structures such as electronic flat bands. Here, the authors use inelastic neutron scattering to investigate the evolution of spin excitations modes for FeSn and CoSn, finding that an anomalous flat mode actually arises from the material used to fix the sample to the aluminium holder for analysis instead of the expected magnetic flat bands.