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At least 127 records · Page 7
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Frustrated Ising charge correlations in the kagome metal ScV 6 Sn 6

Here we resolve the real-space nature of the high-temperature, short-range charge correlations in the kagome metal ScV 6 Sn 6 . Diffuse scattering appears along a frustrated wave vector q H = ($\frac{1}{3}, \frac{1}{3}, \frac{1}{2}$) at temperatures far exceeding the charge order T CO = 92 K, preempting long-range charge order with wave vectors along q$_{\bar{K}}$ = ($\frac{1}{3}, \frac{1}{3}, \frac{1}{3}$). Using a combination of real space and reciprocal space analysis, we resolve the nature of the interactions between the primary out-of-plane Sc-Sn chain instability and the secondary strain-mediated distortion of the in-plane V kagome network. Finally, a minimal model of the diffuse scattering data reveals a high-temperature, short-ranged "zig-zag" phase of in-plane correlations that maps to a frustrated triangular lattice Ising model with antiferromagnetic interactions and provides a real-space understanding of the origin frustrated charge order in this material.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Observation of photo-induced plasmon–phonon coupling in PbTe via ultrafast x-ray scattering

We report the observation of photo-induced plasmon–phonon coupled modes in the group IV–VI semiconductor PbTe using ultrafast x-ray diffuse scattering at the Linac Coherent Light Source. We measure the near-zone-center excited-state dispersion of the heavily screened longitudinal optical (LO) phonon branch as extracted from differential changes in x-ray diffuse scattering intensity following above bandgap photoexcitation. We suggest that upon photoexcitation, the LO phonon-plasmon coupled (LOPC) modes themselves become coupled to longitudinal acoustic modes that drive electron band shifts via acoustic deformation potentials and possibly to low-energy single-particle excitations within the plasma and that these couplings give rise to displacement-correlations that oscillate in time with a period given effectively by the heavily screened LOPC frequency.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Emergence of liquid following laser melting of gold thin films

X-ray structural science is undergoing a revolution driven by the emergence of X-ray Free-electron Laser (XFEL) facilities. The structures of crystalline solids can now be studied on the picosecond time scale relevant to phonons, atomic vibrations which travel at acoustic velocities. In the work presented here, X-ray diffuse scattering is employed to characterize the time dependence of the liquid phase emerging from femtosecond laser-induced melting of polycrystalline gold thin films using an XFEL. In a previous analysis of Bragg peak profiles, we showed the supersonic disappearance of the solid phase and presented a model of pumped hot electrons carrying energy from the gold surface to scatter at internal grain boundaries. This generates melt fronts propagating relatively slowly into the crystal grains. By conversion of diffuse scattering to a partial X-ray pair distribution function, we demonstrate that it has the characteristic shape obtained by Fourier transformation of the measured F ( Q ). The diffuse signal fraction increases with a characteristic rise-time of 13 ps, roughly independent of the incident pump fluence and consequent final liquid fraction. This suggests the role of further melt-front nucleation processes beyond grain boundaries.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Turbulent pitch-angle scattering and diffusive transport of hard X-ray-producing electrons in flaring coronal loops

Recent observations from RHESSI have revealed that the number of non-thermal electrons in the coronal part of a flaring loop can exceed the number of electrons required to explain the hard X-ray-emitting footpoints of the same flaring loop. Such sources cannot, therefore, be interpreted on the basis of the standard collisional transport model, in which electrons stream along the loop while losing their energy through collisions with the ambient plasma; additional physical processes, to either trap or scatter the energetic electrons, are required. Motivated by this and other observations that suggest that high-energy electrons are confined to the coronal region of the source, we consider turbulent pitch-angle scattering of fast electrons off low-frequency magnetic fluctuations as a confinement mechanism, modeled as a spatial diffusion parallel to the mean magnetic field. In general, turbulent scattering leads to a reduction of the collisional stopping distance of non-thermal electrons along the loop, and hence to an enhancement of the coronal hard X-ray source relative to the footpoints. The variation of source size L with electron energy E becomes weaker than the quadratic behavior pertinent to collisional transport, with the slope of L(E) depending directly on the mean free path λ associated with the non-collisional scattering mechanism. Comparing the predictions of the model with observations, we find that λ ∼ (10{sup 8}-10{sup 9}) cm for ∼30 keV, less than the length of a typical flaring loop and smaller than, or comparable to, the size of the electron acceleration region.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2018

Long-wavelength correlations in ferromagnetic titanate pyrochlores as revealed by small-angle neutron scattering

Here, we have carried out small angle neutron scattering measurements on single crystals of two members of the family of cubic rare-earth titanate pyrochlores that display ferromagnetic Curie-Weiss susceptibilities, Yb 2 Ti 2 O 7 and Ho 2 Ti 2 O 7 . Ho 2 Ti 2 O 7 is established as displaying a prototypical classical dipolar spin ice ground state, while Yb 2 Ti 2 O 7 has been purported as a candidate for a quantum spin ice ground state. While both materials have been well studied with neutron scattering techniques, neither has been previously explored in single crystal form with small angle neutron scattering (SANS). Our results for Yb 2 Ti 2 O 7 show distinct SANS features below its Θ CW ~0.50K, with rods of diffuse scattering extending along < 111 > directions in reciprocal space, off-rod scattering which peaks in temperature near Θ CW , and quasi-Bragg scattering at very small angles which correlates well with T C ~0.26K. The quasi-Bragg scattering corresponds to finite extent ferromagnetic domains ~140Å across, at the lowest temperatures. We interpret the < 111 > rods of diffuse scattering as arising from domain boundaries between the finite-extent ferromagnetic domains. In contrast the SANS signal in Ho 2 Ti 2 O 7 is isotropic within the (HHL) plane around Q = 0, consistent with the expectations of the dipolar spin ice model. However the strength of this overall SANS signal has a temperature dependence resembling that of the magnetic heat capacity, with a peak near 3 K. Below the break between the field-cooled and the zero-field cooled susceptibility in Ho 2 Ti 2 O 7 at ~0.60K, the SANS signal is very low, approaching zero.

36 MATERIALS SCIENCE↗
DOE OSTI2022

X-ray nano-imaging of defects in thin film catalysts via cluster analysis

Functional properties of transition-metal oxides strongly depend on crystallographic defects; crystallographic lattice deviations can affect ionic diffusion and adsorbate binding energies. Scanning x-ray nanodiffraction enables imaging of local structural distortions across an extended spatial region of thin samples. Yet, localized lattice distortions remain challenging to detect and localize using nanodiffraction, due to their weak diffuse scattering. Here, in this study, we apply an unsupervised machine learning clustering algorithm to isolate the low-intensity diffuse scattering in as-grown and alkaline-treated thin epitaxially strained SrIrO 3 films. We pinpoint the defect locations, find additional strain variation in the morphology of electrochemically cycled SrIrO 3 , and interpret the defect type by analyzing the diffraction profile through clustering. Our findings demonstrate the use of a machine learning clustering algorithm for identifying and characterizing hard-to-find crystallographic defects in thin films of electrocatalysts and highlight the potential to study electrochemical reactions at defect sites in operando experiments.

42 ENGINEERING↗
DOE OSTI2019

Emergence of topologically protected states in the MoTe 2 Weyl semimetal with layer-stacking order

Electronic tunability in crystals with weakly bound layers can be achieved through layer stacking order. One such example is MoTe 2 , where the low-temperature orthorhombic T d phase is topological and host to Weyl quasiparticles. The transition mechanism to the nontrivial topology is elucidated by single-crystal neutron diffraction. Upon cooling from the monoclinic 1 T' to the T d phase, diffuse scattering accompanies the transition, arising from random, in-plane layer displacements, and dissipates upon entering the T d phase. Here, diffuse scattering is observed only in the H0L plane due to irreversible layer shifts along the c axis that break the centrosymmetry of the monoclinic lattice.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Short-range magnetic correlations in quasicrystalline i -Tb-Cd

Here, we report on elastic and inelastic neutron scattering from single-grain isotopically enriched samples to elucidate the local magnetic correlations between Tb 3+ moments in quasicrystalline i -Tb-Cd. The inelastic neutron scattering measurements of the crystalline electric field excitations demonstrated that the Tb 3+ moments are directed primarily along the local fivefold axes of the Tsai-type cluster as was found for the TbCd 6 approximant phase. Based on the inelastic measurements, we consider a simple Ising-type model for the moment configurations on a single Tb 3+ icosahedron and enumerate the lowest energy moment configurations. We then calculate the diffuse scattering from these configurations and compare with the experimental magnetic diffuse scattering measurements to identify the most likely single cluster moment configurations and find reasonable agreement between the broad features observed in our scattering simulations. We further use a heuristic glass model as well as large-scale Monte-Carlo simulations of a multicluster model to consider the role of higher-order (longer-range) intercluster correlations for magnetic frustration and the magnetic scattering.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2019

Ultrafast time-resolved x-ray scattering reveals diffusive charge order dynamics in La 2-x Ba x CuO 4

Charge order is universal among high-T c cuprates but its relation to super-conductivity is unclear. While static order competes with superconductivity,dynamic order may be favorable and even contribute to Cooper pairing. Using time-resolved resonant soft x-ray scattering at a free electron laser, we show that the charge order in prototypical La 2–x Ba x CuO 4 exhibits transverse fluctuations at ps timescales. These sub-meV excitations propagate by Brownian-like diffusion and have an energy scale remarkably close to the superconducting T c . At sub-meV energy scales, the dynamics are governed by universal scaling laws defined by propagation of topological defects. Our results show that charge order in La 2–x Ba x CuO 4 exhibits dynamics favorable to the in-plane superconducting tunneling, and establish time-resolved x-rays as a means to study excitations at energy scales inaccessible to conventional scattering techniques.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Detailed Characterization of a Nanosecond-Lived Excited State: X-ray and Theoretical Investigation of the Quintet State in Photoexcited [Fe(terpy) 2 ] 2+

Theoretical predictions show that depending on the populations of the Fe 3dxy, 3dxz, and 3dyz orbitals two possible quintet states can exist for the high-spin state of the photoswitchable model system [Fe(terpy)2]2+. The differences in the structure and molecular properties of these 5B2 and 5E quintets are very small and pose a substantial challenge for experiments to resolve them. Yet for a better understanding of the physics of this system, which can lead to the design of novel molecules with enhanced photoswitching performance, it is vital to determine which high-spin state is reached in the transitions that follow the light excitation. The quintet state can be prepared with a short laser pulse and can be studied with cutting-edge time-resolved X-ray techniques. Here we report on the application of an extended set of X-ray spectroscopy and scattering techniques applied to investigate the quintet state of [Fe(terpy)2]2+ 80 ps after light excitation. High-quality X-ray absorption, nonresonant emission, and resonant emission spectra as well as X-ray diffuse scattering data clearly reflect the formation of the high-spin state of the [Fe(terpy)2]2+ molecule; moreover, extended X-ray absorption fine structure spectroscopy resolves the Fe-ligand bond-length variations with unprecedented bondlength accuracy in time-resolved experiments. With ab initio calculations we determine why, in contrast to most related systems, one configurational mode is insufficient for the description of the low-spin (LS)-high-spin (HS) transition. We identify the electronic structure origin of the differences between the two possible quintet modes, and finally, we unambiguously identify the formed quintet state as 5E, in agreement with our theoretical expectations.

Vankó, György↗
DOE OSTI2018

A suite-level review of the neutron single-crystal diffraction instruments at Oak Ridge National Laboratory

The nascent suite of single-crystal neutron diffractometers at the Oak Ridge National Laboratory has no equal at any other neutron scattering facility worldwide and offers the potential to re-assert single-crystal diffraction using neutrons as a significant tool to study nuclear and magnetic structures of small unit cell crystals, nuclear structures of macromolecules, and diffuse scattering. Signature applications and features of single-crystal neutron diffraction are high resolution nuclear structure analysis, magnetic structure and spin density determinations, contrast variation (particularly D 2 O/H 2 O) for nuclear structural studies, lack of radiation damage when using crystals of biological molecules such as proteins, and the fidelity to measure nuclear and magnetic diffuse scattering with elastic discrimination.

47 OTHER INSTRUMENTATION↗
DOE OSTI2018

Correlated local dipoles in PbTe

We present a combined single-crystal x-ray diffuse scattering and ab-initio molecular dynamics study of lead telluride, PbTe. Well-known for its thermoelectric and narrow-gap semiconducting properties, PbTe recently achieved further notoriety following the report of an unusual off-centering of the lead atoms, accompanied by a local symmetry breaking, on heating. This observation, which was named emphanisis, ignited considerable controversy regarding the details of the underlying local structure and the appropriate interpretation of the total scattering experiments. In this study, we identify an unusual correlated local dipole formation extending over several unit cells with an associated local reduction of the cubic symmetry in both our x-ray diffuse scattering measurements and our molecular dynamics simulations. Importantly, when averaged spatially or temporally, the most probable positions for the ions are at the centers of their coordination polyhedra. Our results therefore clarify the nature of the local symmetry breaking, and reveal the source of the earlier controversy regarding the existence or absence of off-centering. Finally, we provide an interpretation of the behavior in terms of coupled soft optical and acoustic modes, which is linked also to the high thermoelectric performance of PbTe.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2015

Phonon coupling to dynamic short-range polar order in a relaxor ferroelectric near the morphotropic phase boundary

We report neutron inelastic scattering experiments on single-crystal PbMg 1/3 Nb 2/3 O 3 doped with 32% PbTiO 3 , a relaxor ferroelectric that lies close to the morphotropic phase boundary. When cooled under an electric field E∥ [001] into tetragonal and monoclinic phases, the scattering cross section from transverse acoustic (TA) phonons polarized parallel to E weakens and shifts to higher energy relative to that under zero-field-cooled conditions. Likewise, the scattering cross section from transverse optic (TO) phonons polarized parallel to E weakens for energy transfers 4 ≤ ℏω ≤ 9 meV. However, TA and TO phonons polarized perpendicular to E show no change. This anisotropic field response is similar to that of the diffuse scattering cross section, which, as previously reported, is suppressed when polarized parallel to E but not when polarized perpendicular to E. Lastly, our findings suggest that the lattice dynamics and dynamic short-range polar correlations that give rise to the diffuse scattering are coupled.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2012

Ferroelectric and octahedral tilt twin disorder and the lead-free piezoelectric, sodium potassium niobate system

Using electron diffraction, trends in the local structural behaviour of the K{sub x}Na{sub 1-x}NbO{sub 3} (KNN x) 'solid solution' system are investigated and interpreted using an order/disorder based theoretical framework. At room temperature, electron diffraction shows a single plane of transverse polarised, diffuse intensity perpendicular to [0 1 0]{sub p} Low-Asterisk (p for parent sub-structure) across the entire phase diagram, indicative of ferroelectric disorder along the [0 1 0]{sub p} direction co-existing with long range ferroelectric order along the orthogonal [1 0 0]{sub p} and [0 0 1]{sub p} directions. An additional characteristic pattern of diffuse scattering is also observed, involving rods of diffuse intensity running along the [1 0 0]{sub p}* and [0 0 1]{sub p}* directions of the perovskite sub-structure and indicative of octahedral tilt disorder about the [1 0 0]{sub p} and [0 0 1]{sub p} axes co-existing with long range ordered octahedral tilting around the [0 1 0]{sub p} direction. A possible crystal chemical explanation for the existence of this latter octahedral tilt disorder is explored through bond valence sum calculations. The possible influence of both types of disorder on the previously refined, room temperature space group/s and average crystal structure/s is examined. - Graphical abstract: [-3,0.-1]p zone axis EDP of K{sub 0.46}Na{sub 0.54}NbO{sub 3} indexed according to both the relevant Pcm21 space groups (no subscripts) and the parent perovskite subcell (denoted by a subscript p). Highlights: Black-Right-Pointing-Pointer Characterises ferroelectric and octahedral tilt disorder in the KNN solid solution. Black-Right-Pointing-Pointer Discusses the possible driving forces for this disorder. Black-Right-Pointing-Pointer Discusses the implications of this disorder for physical properties. Black-Right-Pointing-Pointer Discusses the effects of this disorder on powder diffraction data.

36 MATERIALS SCIENCE↗
DOE OSTI2015

Bi{sub 1−x}Nb{sub x}O{sub 1.5+x} (x=0.0625, 0.12) fast ion conductors: Structures, stability and oxide ion migration pathways

A combined experimental and computational study of Bi{sub 1−x}Nb{sub x}O{sub 1.5+x} (x=0.0625 and 0.12) has been carried out using laboratory X-ray, neutron and electron diffraction, impedance measurements and ab-initio molecular dynamics. We demonstrate that Bi{sub 0.9375}Nb{sub 0.0625}O{sub 1.5625}, previously reported to adopt a cubic fluorite-type superstructure, can form two different polymorphs depending on the synthetic method: a metastable cubic phase is produced by quenching; while slower cooling yields a stable material with a tetragonal √2×√2×1 superstructure, which undergoes a reversible phase transition into the cubic form at ~680 °C on subsequent reheating. Neutron diffraction reveals that the tetragonal superstructure arises mainly from ordering in the oxygen sublattice, with Bi and Nb remaining disordered, although structured diffuse scattering observed in the electron diffraction patterns suggests a degree of short-range ordering. Both materials are oxide ion conductors. On thermal cycling, Bi{sub 0.88}Nb{sub 0.12}O{sub 1.62} exhibits a decrease in conductivity of approximately an order of magnitude due to partial transformation into the tetragonal phase, but still exhibits conductivity comparable to yttria-stabilised zirconia (YSZ). Ab-initio molecular dynamics simulations performed on Bi{sub 0.9375}Nb{sub 0.0625}O{sub 1.5625} show that oxide ion diffusion occurs by O{sup 2−} jumps between edge- and corner-sharing OM{sub 4} groups (M=Bi, Nb) via tetrahedral □M{sub 4} and octahedral □M{sub 6} vacancies. - Graphical abstract: Oxide ion migration in tetragonal Bi{sub 0.9375}Nb{sub 0.0625}O{sub 1.5625} occurs by O{sup 2−} jumps between edge- and corner-sharing OM{sub 4} groups (M=Bi, Nb) via tetrahedral M{sub 4} and octahedral M{sub 6} vacancies. - Highlights: • Bi{sub 0.9375}Nb{sub 0.0625}O{sub 1.5625} adopts a tetragonal √2×√2×1 fluorite superstructure. • Superstructure is due to ordering in the O-sublattice, with Bi/Nb disordered. • Bi{sub 0.9375}Nb{sub 0.0625}O{sub 1.5625} is a good oxide ion conductor. • O{sup 2−} jump between OM{sub 4} groups (M=Bi, Nb) via tetrahedral and octahedral vacancies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

The nature of photoinduced phase transition and metastable states in vanadium dioxide

Photoinduced threshold switching processes that lead to bistability and the formation of metastable phases in photoinduced phase transition of VO 2 are elucidated through ultrafast electron diffraction and diffusive scattering techniques with varying excitation wavelengths. We uncover two distinct regimes of the dynamical phase change: a nearly instantaneous crossover into an intermediate state and its decay led by lattice instabilities over 10 ps timescales. The structure of this intermediate state is identified to be monoclinic, but more akin to M 2 rather than M1 based on structure refinements. The extinction of all major monoclinic features within just a few picoseconds at the above-threshold-level (~20%) photoexcitations and the distinct dynamics in diffusive scattering that represents medium-range atomic fluctuations at two photon wavelengths strongly suggest a density-driven and nonthermal pathway for the initial process of the photoinduced phase transition. These results highlight the critical roles of electron correlations and lattice instabilities in driving and controlling phase transformations far from equilibrium.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗