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DOE OSTI2024

Nanoscale structural correlations in a model cuprate superconductor

Understanding the extent and role of inhomogeneity is a pivotal challenge in the physics of cuprate superconductors. While it is known that structural and electronic inhomogeneity is prevalent in the cuprates, it has proven difficult to disentangle compound-specific features from universally relevant effects. Here, in this study, we combine advanced neutron and x-ray diffuse scattering with numerical modeling to obtain insight into bulk structural correlations in HgBa 2 ⁢ CuO 4+δ . This cuprate exhibits a high optimal transition temperature of nearly 100 K, pristine charge-transport behavior, and a simple average crystal structure without long-range structural instabilities, and is therefore uniquely suited for investigations of intrinsic inhomogeneity. We uncover diffuse reciprocal-space patterns that correspond to prominent nanoscale correlations of atomic displacements perpendicular to the CuO 2 planes. The real-space nature of the correlations is revealed through three-dimensional pair distribution function analysis and complementary numerical refinement. We find that relative displacements of ionic and CuO 2 layers play a crucial role, and that the structural inhomogeneity is not directly caused by the presence of conventional point defects. The observed correlations are therefore intrinsic to HgBa 2 ⁢ CuO 4+δ , and thus likely important for the physics of cuprates more broadly. It is possible that the structural correlations are closely related to the unusual superconducting fluctuations and Mott-localization in these complex oxides. As advances in scattering techniques yield increasingly comprehensive data, the experimental and analysis tools developed here for large volumes of diffuse scattering data can be expected to aid future investigations of a wide range of materials.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

Mixed gain detector configurations for time-resolved X-ray solution scattering

X-ray detection at X-ray free-electron lasers is challenging in part due to the XFEL's extremely short and intense X-ray pulses. Experimental measurements are further complicated by the large fluctuations inherent to the self-amplified spontaneous emission process producing the X-rays. At the Linac Coherent Light Source the ePix10ka2M detector offers multiple gain modes, and auto-ranging between these, to increase the dynamic range while retaining low noise. For diffuse scattering techniques, such as time-resolved X-ray solution scattering, where the shape of the scattering pattern largely does not change between exposures, a fixed mix of different gain modes offers many of the same advantages as auto-ranging. We find that configuring individual ASICs in separate gain modes does not impact the intensity linearity of the gain response and has a limited effect on the effective dynamic range in regions with different gain mode settings while avoiding the complexities of auto-ranging. Small (<5%) non-linear gain contributions arise when pixels on the same ASIC are configured in different gain modes. We present a configuration scheme that is designed to select the optimal mixed gain configuration to minimize effects of saturation in the high-/medium-gain region, while maximizing the number of pixels with higher gain to improve the signal-to-noise ratio.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

DOE OSTI2025

Emergent topological polarization textures in relaxor ferroelectrics

Relaxor ferroelectrics underpin high-performance actuators and sensors, yet the nature of polar heterogeneities driving their broadband dielectric response remains debated. Using a unified, multimodal structural refinement framework— simultaneously fitting complementary X-ray and neutron total scattering, X-ray absorption spectra, and diffuse scattering—we reconstruct 3D mesoscale polarization maps in the classic relaxor system PbMg 1/3 Nb 2/3 O 3 –PbTiO 3 . We uncover self-organized swirling polarization textures with half-skyrmion (meron) vortices, challenging models of independent polar nanoregions. These textures, characterized by smooth changes in the polarization direction, originate from overlapping volumes in which the projections of locally correlated polarization vectors onto each volume’s long axis share the same sign. Vortex cores correlate strongly with local charge and strain gradients imposed by compositional heterogeneities. In this work, our results suggest that chemical disorder, acting via depolarizing and strain fields, stabilizes topological vortex textures of the polarization field, offering a route for engineering new dielectric and ferroelectric functionalities.

Eremenko, Maksim [National Institute of Standards ↗

NASA NTRS2013

A New Approach for Spectroradiometric Calibration Consistency on the Ground and in Space

A Space-based Calibration Transfer Spectroradiometer (SCATS) is combined with a ground calibration spectral albedo radiometric standard which consists of an opaque quartz glass Mie scattering diffuser (MSD) which has very good Lambertian scattering properties in both reflectance and transmittance modes. This system provides the capability for determining long term changes in the spectral albedo calibrations which operate in the solar reflective wavelength region. The spectral albedo calibration would be traceable to the SIRCUS and STARR NIST calibration facilities. The on-orbit radiometric standard is the Sun. The NIST traceable ground spectral albedo calibration is invariant between the ground and on-orbit over the instrument lifetime due to the use of a field of view defining mechanical baffle to differentiate between radiance and irradiance.

Heath, Donald F.↗

DOE OSTI2026

Symmetry-protected topological polarons

Emergent quasiparticles in solids often exhibit unique topological properties as a result of the complex interplay between charge, orbital, spin, and lattice degrees of freedom. Among these quasiparticles, the polaron occupies a special place as the first known manifestation of the interaction between a fermion and a boson field. While polarons have been investigated for almost a century, whether these quasiparticles exhibit topological properties and why remain open questions. Here, we establish the universal symmetry principles governing the topology of polar textures in large polarons. Using a group-theoretic analysis, we identify four distinct classes of polar textures in time-reversal-invariant systems, and we show that they carry integer topological charges. We validate this classification by performing state-of-the-art first-principles calculations of materials representative of each class. For these materials, we compute the fingerprints of polaron topology in Huang diffuse scattering and propose ultrafast electron and X-ray scattering experiments to detect these quasiparticles.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2024

Nanometer-Scale Acoustic Wave Packets Generated by Stochastic Core-Level Photoionization Events

We demonstrate that the absorption of femtosecond hard x-ray pulses excites quasispherical, high-amplitude, and high-wave-vector coherent acoustic phonon wave packets using an all hard-x-ray pump-probe scattering experiment. The time- and momentum-resolved diffuse scattering signal is consistent with an ensemble of 3D strain wave packets induced by the rapid electron cascade dynamics following photoionization at uncorrelated excitation centers. We quantify key parameters of this process, including the localization size of the stress field and the photon energy conversion efficiency into elastic energy. The parameters are determined by the photoelectron and Auger electron cascade dynamics, as well as the electron-phonon interaction. In particular, we obtain the localization size of the observed strain wave packet to be 1.5 and 2.5 nm for bulk SrTiO 3 and KTaO 3 single crystals, respectively. The results provide crucial information on the mechanism of x-ray energy deposition into matter and shed light on the shortest collective length scales accessible to coherent acoustic phonon generation using x-ray excitation. Published by the American Physical Society 2024

36 MATERIALS SCIENCE↗

NASA NTRS1992

Physics of pitch angle scattering and velocity diffusion. I - Theory

A general theory for the pitch angle scattering and velocity diffusion of particles in the field of a spectrum of waves in a magnetized plasma is presented. The test particle theory is used to analyze the particle motion. The form of diffusion surfaces is examined, and analytical expressions are given for the resonance width and bounce frequency. The resonance widths are found to vary strongly as a function of harmonic number. The resulting diffusion can be quite asymmetric with respect to pitch angle of 90 deg. The conditions for the onset of pitch angle scattering and energy diffusion are explained in detail. Some of the known shortcomings of the standard quasi-linear theory are also addressed, and ways to overcome them are shown. In particular, the often stated quasi-linear gap at 90 deg is found to exist only under very special cases. For instance, oblique wave propagation can easily remove the gap. The conditions for the existence of the gap are described in great detail. A new diffusion equation which takes into account the finite resonance widths is also discussed. The differences between this new theory and the standard resonance broadening theory is explained.

Karimabadi, H.↗

NASA NTRS1991

Instabilities of line-driven stellar winds. V - Effect of an optically thick continuum

Earlier analyses of the linear instability of line-driven stellar winds are extended to the case, relevant to Wolf-Rayet stars, in which the continuum remains optically thick well above the sonic point. It is found that an optically thick flow driven by pure scattering lines is stabilized by the drag effect of the diffuse, scattered radiation. However, even a relatively small photon destruction probability can cause a flow with continuum optical thickness much greater than 1 to remain unstable, with a given growth rate. The implications of these results for the variability characteristics of winds from Wolf-Rayet stars are briefly discussed.

Owocki, Stanley P.↗

NASA NTRS1995

Terrain classification using circular polarimetric features

Conventional representations of polarization response are referred to a horizontally and vertically polarized basis. Recent studies by Freeman and Durden, van Zyl, and others suggest that alternative polarimetric features which more easily resolve the contributions of simple scattering mechanisms such as odd-bounce, even-bounce, and diffuse scattering could offer several advantages in terrain classification. The circular polarization covariance matrix is a potential source of such features. In this paper, we derive its relationship to the Stokes matrix, describe some of its properties, and compare the utility of linear and circular polarimetric features in classifying an AIRSAR scene containing urban, park, and ocean terrain.

Michelson, David G.↗

NASA NTRS2013

Updated Model of Radar Backscatter for Rough Lunar Craters

We reexamined our radar scattering model for young, rough craters [1] based on unpublished data from the 1980's [2]. Our model for scattering from the lunar surface is a mixing model consisting of varying amounts of diffuse and specular components as shown in Figure 1. The specular component, which consists of only opposite-sense circular (OC) echoes, results from the mirror-like surface and sub-surface layers that are smooth to a tenth of a radar wavelength for large (>10 wavelengths) areas oriented perpendicular to the radar's line-ofsight. The diffuse component, which has both OC and same sense (SC) circular echoes, is associated with either surface roughness (wavelength-sized rocks) or ice, and is assumed to be uniformly bright, with backscatter being proportional to the cosine of the incidence angle. Only diffuse scattering contributes to the SC echoes.

Moon↗

NASA NTRS1990

Applicability of steady models for hot-star winds

Non-Sobolev models of radiatively driven stellar winds based on a pure-absorption approximation do not have a well-defined steady state. Here the implications of this for flow time-dependence are examined, showing that, under such circumstances, instabilities in the flow attain an absolute character that leads to intrinsic variability. In this case, steady solutions are inherently inapplicable because they do not represent physically realizable states. However, for actual hot-star winds, driving is principally by scattering, not pure absorption. In practice, the relatively weak force associated with slight asymmetries in the diffuse, scattered radiation field may play a crucial role in breaking the solution degeneracy and reducing the instability from an absolute to an advective character.

Owocki, Stanley P.↗

DOE OSTI2025

Resolving the dynamic correlated disorder in KTa 1- x Nb x O 3

Understanding the complex temporal and spatial correlations of ions in disordered perovskite oxides is critical to rationalize their functional properties. Here, in this study, we provide new insights into the longstanding controversy regarding the off-centering of transition metal ions in the archetypal ferroelectric alloy KTa 1-x Nb x O 3 (KTN). By mapping the full energy (E) and wavevector (Q) dependence of the dynamical structure factor S(Q, E) using neutron scattering, and rationalizing our observations with atomistic simulations leveraging machine learning, we fully resolve the static vs dynamic nature of diffuse scattering sheets, as well as their composition (x) and temperature dependence. Our first-principles simulations, extended with machine-learning molecular dynamics, reproduce both inelastic neutron spectra and diffuse features, and establish how dynamically-correlated transition metal off-centerings couple to phonons, unifying local and collective viewpoints. This study sheds new light into an exemplary ferroelectric systems and shows the importance of mapping the full S(Q, E) to reveal critical spatio-temporal correlations of atomic disorder from which functional properties emerge.

42 ENGINEERING↗

NASA NTRS1973

Dual-frequency bistatic-radar investigations of the moon with Apollos 14 and 15.

Simultaneous 13- and 116-cm wavelength radio transmissions from the Apollo 14 and 15 spacecraft were received on the earth after reflection from the lunar surface. The received data were processed to obtain complete polarization and power spectra of the echo signal; the ellipticity, orientation, and magnitude of the deterministically polarized part were obtained as a function of frequency. The polarized parts of the echo spectra were then reduced according to the theory of quasi-specular scattering from a gently undulating surface. The unpolarized portions of the echo spectra were associated with a diffuse scattering mechanism. Within Mare Serenitatis and Oceanus Procellarum, the 13-cm data follow a classical Fresnel reflection curve corresponding to relative dielectric constant epsilon = 3.1 plus or minus 0.1. Over most of these same areas, the 116-cm data are consistent with this value of relative dielectric constant. In some areas, however, notably between Reiner and Hevelius, there are marked deviations from the reflectivities predicted for epsilon = 3.1. These results cannot be explained on the basis of simple models employing contiguous, semiinfinite, dielectric interfaces.

Tyler, G. L.↗

NASA NTRS1974

Scattering of helium nozzle beams from LiF/001/ and NaCl/001/ crystal surfaces. I - Elastic and inelastic transitions

Nozzle-type atomic beams and time-of-flight detection methods are employed in studies of the scattering of thermal-energy He-4 atoms from LiF (001) and NaCl (001) surfaces under conditions where diffraction is observed and where substantial inelastic scattering occurs. Intensity and speed-distribution measurements are obtained for the portion of the scattering within the plane of incidence. For these measurements, incident-beam orientation with respect to target (polar angle and azimuth), incident-beam de Broglie wavelength (0.38-0.60 A), and crystal temperature (300-1000 K) are varied. For LiF, the measured intensity distributions exhibit sharp peaks comprised essentially of elastically scattered atoms and corresponding to up to third-order diffraction, inelastic scattering in the form of local dispersion about each of the elastic peaks, and a component of nominally diffuse scattering distributed below and between the peaks. For NaCl, the same general types of scattering are observed, with elastic scattering less prevalent, intensity peaks not as sharp, and dispersions of inelastic scattering harder to resolve.

Bledsoe, J. R.↗

NASA NTRS1981

Visible light scatter measurements of the Advanced X-ray Astronomical Facility /AXAF/ mirror samples

NASA is studying the properties of mirror surfaces for X-ray telescopes, the data of which will be used to develop the telescope system for the Advanced X-ray Astronomical Facility. Visible light scatter measurements, using a computer controlled scanner, are made of various mirror samples to determine surface roughness. Total diffuse scatter is calculated using numerical integration techniques and used to estimate the rms surface roughness. The data measurements are then compared with X-ray scatter measurements of the same samples. A summary of the data generated is presented, along with graphs showing changes in scatter on samples before and after cleaning. Results show that very smooth surfaces can be polished on the common substrate materials (from 2 to 10 Angstroms), and nickel appears to give the lowest visible light scatter.

Griner, D. B.↗

NASA NTRS1984

Theory and measure of certain image norms in SAR

The principal properties of synthetic aperture radar SAR imagery of point and distributed objects are summarized. Against this background, the response of a SAR (Synthetic Aperture Radar) to the moving surface of the sea is considered. Certain conclusions are drawn as to the mechanism of interaction between microwaves and the sea surface. Focus and speckle spectral tests may be used on selected SAR imagery for areas of the ocean. The fine structure of the sea imagery is sensitive to processor focus and adjustment. The ocean reflectivity mechanism must include point like scatterers of sufficient radar cross section to dominate the return from certain individual resolution elements. Both specular and diffuse scattering mechanisms are observed together, to varying degree. The effect is sea state dependent. Several experiments are proposed based on imaging theory that could assist in the investigation of reflectivity mechanisms.

Raney, R. K.↗

DOE OSTI2026

Disorder-induced proximate quantum spin ice phase in Pr2Sn2O7

We report a comprehensive bulk characterization and neutron scattering investigation of single-crystalline Pr2Sn2O7, a magnetic pyrochlore synthesized via a flux-growth method. Unpolarized neutron diffuse scattering reveals the emergence of spin-ice correlations below T ∼ 1 K, evidenced by the development of anisotropic pinch-point features that are consistent with quantum-spin-ice (QSI) behavior. A.C. susceptibility measurements indicate a progressive slowing of spin dynamics in this regime, culminating in complete spin freezing below Tf ≈ 0.15 K. Inelastic neutron scattering at T = 0.5 K reveals a broad spectrum of quasi-elastic magnetic excitations, with intensity in the low-energy range [0, 0.2] meV significantly suppressed below Tf. Meanwhile, an incipient (100)-type magnetic order begins to nucleate, and a gapped excitation centered at ℏω = 0.23 meV persists. We further identify two distinct dynamical timescales above Tf , a slow component τ_slow ∼ 10^−5 s and a fast component τ_fast ∼ 10^−10 s, in quantitative agreement with theoretical predictions for QSI systems. Taken together, these results indicate that Pr2Sn2O7 enters a disorder-induced spin-frozen phase below Tf , lying in close proximity to a U(1) quantum spin liquid

Luo, Yi [ORNL] (ORCID:000900048710428X)↗

DOE OSTI2024

Absence of magnetoelastic deformation in the spin-chain compound CuBr 2

Here, we investigate a spin-$\frac{1}{2}$ antiferromagnet, CuBr 2 , which has quasi-one-dimensional structural motifs. The system has previously been observed to exhibit unusual Raman modes possibly due to a locally deformed crystal structure driven by the low-dimensional magnetism. Using hard x-ray scattering and neutron total scattering, here we aim to verify a specific form of tetramerizing deformation proposed in the previous study. Apart from diffuse scattering signals, which we can reproduce by performing a thorough modeling of the lattice's thermal vibrations, we do not observe evidence for a tetramerized lattice structure within our detection sensitivity. Consequently, we consider it unlikely that the unusual Raman modes in CuBr 2 arise from quantum spin-singlet-driven lattice deformations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗