A New Spin on Material Properties: Local Magnetic Structure in Functional and Quantum Materials.

The past few decades have made clear that the properties and performances of emerging functional and quantum materials can depend strongly on their local atomic and/or magnetic structure, particularly when details of the local structure deviate from the long-range structure averaged over space and time. Traditional methods of structural refinement (e.g.

Transformations to the aluminum coordination environment and network polymerization in amorphous aluminosilicates under pressure.

The structure of calcium aluminosilicate glasses (CaO)x(Al2O3)y(SiO2)1-x-y with the near tectosilicate compositions x ≃ 0.19 and 1 - x - y ≃ 0.61 or x ≃ 0.

Pressure dependent structure of amorphous magnesium aluminosilicates: The effect of replacing magnesia by alumina at the enstatite composition.

The effect of replacing magnesia by alumina on the pressure-dependent structure of amorphous enstatite was investigated by applying in situ high-pressure neutron diffraction with magnesium isotope substitution to glassy (MgO)0.375(Al2O3)0.125(SiO2)0.

Structure of amorphous materials in the NASICON system Na1+xTiSiP3-xO.

The structure of glasses in the sodium (Na) super-ionic conductor (NASICON) system Na1+xTiSiP3-xOwith= 0.8 and= 1.0 was explored by combining neutron and high-energy x-ray diffraction withSi,P andNa solid-state nuclear magnetic resonance (NMR) spectroscopy.

Effect of antifluorite layer on the magnetic order in Eu-based 1111 compounds, EuTAsF (T = Zn, Mn, and Fe).

The 1111 compounds with an alternating sequence of fluorite and antifluorite layers serve as structural hosts for the vast family of Fe-based superconductors. Here, we use neutron powder diffraction and density-functional-theory (DFT) band-structure calculations to study magnetic order of Eu in the [EuF] fluorite layers depending on the nature of the [TAs] antifluorite layer that can be non-magnetic semiconducting (T = Zn), magnetic semiconducting (T = Mn), or magnetic metallic (T = Fe). Antiferromagnetic transitions at ∼ 2.

Temperature-dependent anisotropy in the bond lengths of UOas a result of phonon-induced atomic correlations.

Previous experiments on cubic UOhave suggested that the temperature dependences of the nearest-neighbour U-O and U-U distances are. We have acquired total-scattering neutron diffraction patterns out to = 23.5 Åfor50 View Article and Find Full Text PDF

Structure of diopside, enstatite, and magnesium aluminosilicate glasses: A joint approach using neutron and x-ray diffraction and solid-state NMR.

Neutron diffraction with magnesium isotope substitution, high energy x-ray diffraction, and Si, Al, and Mg solid-state nuclear magnetic resonance (NMR) spectroscopy were used to measure the structure of glassy diopside (CaMgSiO), enstatite (MgSiO), and four (MgO)(AlO)(SiO) glasses, with x = 0.375 or 0.25 along the 50 mol.

Structure and dynamics of aqueous NaCl solutions at high temperatures and pressures.

The structure of a concentrated solution of NaCl in DO was investigated by in situ high-pressure neutron diffraction with chlorine isotope substitution to give site-specific information on the coordination environment of the chloride ion. A broad range of densities was explored by first increasing the temperature from 323 to 423 K at 0.1 kbar and then increasing the pressure from 0.

From SmOF to SmHOF: H/F Substitution in Oxide Fluorides as a Synthesis Route to Heteroanionic Compounds.

Mixed anionic hydrides of the rare earths are a fascinating class of compounds as potential functional materials, especially in luminescence, as photochromic thin films and for ion conduction. For exploratory studies, the effectiveness of various synthesis methods must be investigated, which is done here for metathesis reactions. The reaction of SmO with PTFE yields SmOF (2/, = 5.

Molecular Dynamics and Neutron Scattering Studies of Potassium Chloride in Aqueous Solution.

Neutron diffraction with isotopic substitution (NDIS) experiments were done on both natural abundance potassium and isotopically labeled KCl heavy water solutions to characterize the solvent structuring around the potassium ion in water. Preliminary measurements suggested that the literature value for the coherent neutron scattering length (2.69 fm) for K was significantly in error.

Femtosecond x-ray diffraction reveals a liquid-liquid phase transition in phase-change materials.

In phase-change memory devices, a material is cycled between glassy and crystalline states. The highly temperature-dependent kinetics of its crystallization process enables application in memory technology, but the transition has not been resolved on an atomic scale. Using femtosecond x-ray diffraction and ab initio computer simulations, we determined the time-dependent pair-correlation function of phase-change materials throughout the melt-quenching and crystallization process.

Adjustable Magnetic Phase Transition Inducing Unusual Zero Thermal Expansion in Cubic RCo-Based Intermetallic Compounds (R = Rare Earth).

Metallic materials that exhibit negligible thermal expansion or zero thermal expansion (ZTE) have great merit for practical applications, but these materials are rare and their thermal expansions are difficult to control. Here, we successfully tailored the thermal expansion behaviors from strongly but abruptly negative to zero over wide temperature ranges in a series of (Gd,R)(Co,Fe) (R = Dy, Ho, Er) intermetallic compounds by tuning the composition to bring the first-order magnetic phase transition to second-order. Interestingly, an unusual isotropic ZTE property with a coefficient of thermal expansion of α = 0.

Structure and dynamics of high-temperature strontium aluminosilicate melts.

We report the study of high-temperature melts (1600-2300 °C) and related glasses in the SrO-Al2O3-SiO2 phase diagram considering three series: (i) depolymerized ([SrO]/[Al2O3] = 3); (ii) fully polymerized ([SrO]/[Al2O3] = 1); and (iii) per-aluminous ([SrO]/[Al2O3] < 1). By considering the results from high-temperature 27Al NMR and high-temperature neutron diffraction, we demonstrate that the structure of the polymerized melts is controlled by a close-to-random distribution of Al and Si in the tetrahedral sites, while the depolymerized melts show smaller rings with a possible loss of non-bridging oxygens on AlO4 units during cooling for high-silica compositions. A few five-fold coordinated VAl sites are present in all compositions, except per-aluminous ones where high amounts of high-coordinated aluminium are found in glasses and melts with complex temperature dependence.

Structure of Strontium Aluminosilicate Glasses from Molecular Dynamics Simulation, Neutron Diffraction, and Nuclear Magnetic Resonance Studies.

The structure of strontium glasses with the composition (SiO)(AlO) (SrO) ( R = [SrO]/[AlO] = 1) and (SiO)(AlO) (SrO) ( R = 3) has been explored experimentally over both short- and intermediate-length scales using neutron diffraction, Al and Si nuclear magnetic resonance, and classical molecular dynamics simulations in model systems containing around 10 000 atoms. We aim at understanding the structural role of aluminum and strontium as a function of the chemical composition of these glasses. The short- and medium-range structure such as aluminum coordination, bond angle distribution, Q distribution, and oxygen speciation have been systematically studied.

Calcium ions in aqueous solutions: Accurate force field description aided by ab initio molecular dynamics and neutron scattering.

We present a combination of force field and ab initio molecular dynamics simulations together with neutron scattering experiments with isotopic substitution that aim at characterizing ion hydration and pairing in aqueous calcium chloride and formate/acetate solutions. Benchmarking against neutron scattering data on concentrated solutions together with ion pairing free energy profiles from ab initio molecular dynamics allows us to develop an accurate calcium force field which accounts in a mean-field way for electronic polarization effects via charge rescaling. This refined calcium parameterization is directly usable for standard molecular dynamics simulations of processes involving this key biological signaling ion.

Characterization of Oxygen Defect Clusters in UO Using Neutron Scattering and PDF Analysis.

In hyper-stoichiometric uranium oxide, both neutron diffraction work and, more recently, theoretical analyses report the existence of clusters such as the 2:2:2 cluster, comprising two anion vacancies and two types of anion interstitials. However, little is known about whether there exists a region of low deviation-from-stoichiometry in which defects remain isolated, or indeed whether at high deviation-from-stoichiometry defect clusters prevail that contain more excess oxygen atoms than the di-interstitial cluster. In this study, we report pair distribution function (PDF) analyses of UO and UO ( x ≈ 0.

Structure of semiconducting versus fast-ion conducting glasses in the Ag-Ge-Se system.

The transition from a semiconductor to a fast-ion conductor with increasing silver content along the Ag (GeSe) tie line (0≤≤25) was investigated on multiple length scales by employing a combination of electric force microscopy, X-ray diffraction, and neutron diffraction. The microscopy results show separation into silver-rich and silver-poor phases, where the Ag-rich phase percolates at the onset of fast-ion conductivity. The method of neutron diffraction with Ag isotope substitution was applied to the =5 and =25 compositions, and the results indicate an evolution in structure of the Ag-rich phase with change of composition.

Hydration and Ion Pairing in Aqueous Mg and Zn Solutions: Force-Field Description Aided by Neutron Scattering Experiments and Ab Initio Molecular Dynamics Simulations.

Magnesium and zinc dications possess the same charge and have an almost identical size, yet they behave very differently in aqueous solutions and play distinct biological roles. It is thus crucial to identify the origins of such different behaviors and to assess to what extent they can be captured by force-field molecular dynamics simulations. In this work, we combine neutron scattering experiments in a specific mixture of HO and DO (the so-called null water) with ab initio molecular dynamics simulations to probe the difference in the hydration structure and ion-pairing properties of chloride solutions of the two cations.

From atomic structure to excess entropy: a neutron diffraction and density functional theory study of CaO-Al₂O₃-SiO₂ melts.

Calcium aluminosilicate CaO-Al2O3-SiO2 (CAS) melts with compositions (CaO-SiO2)(x)(Al2O3)(1-x) for x  <  0.5 and (Al2O3)(x)(SiO2)(1-x) for x ≥ 0.5 are studied using neutron diffraction with aerodynamic levitation and density functional theory molecular dynamics modelling.

High-pressure transformation of SiO₂ glass from a tetrahedral to an octahedral network: a joint approach using neutron diffraction and molecular dynamics.

A combination of in situ high-pressure neutron diffraction at pressures up to 17.5(5) GPa and molecular dynamics simulations employing a many-body interatomic potential model is used to investigate the structure of cold-compressed silica glass. The simulations give a good account of the neutron diffraction results and of existing x-ray diffraction results at pressures up to ~60  GPa.

Magnetic structure of the metallic triangular antiferromagnet Ag2NiO2.

The magnetic structure of the metallic antiferromagnet Ag2NiO2 with the Néel temperature TN = 56 K has been investigated by means of a neutron diffraction technique using a powder sample in the temperature range between 5 and 65 K. The antiferromagnetic (AF) diffraction peaks are clearly observed below TN and can be indexed with the propagation vector [Formula: see text]. Based on the results of both a representational analysis and a Rietveld refinement of the magnetic peaks, the AF spin structure is determined as an A-type AF structure with ml = m0cos(2πk ⋅l), where ml is the moment at the lth Ni(3+) site and m0 = (0.