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At least 1,621 records · Page 90

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DOE OSTI2024

AI-NERD: Elucidation of relaxation dynamics beyond equilibrium through AI-informed X-ray photon correlation spectroscopy

Abstract Understanding and interpreting dynamics of functional materials in situ is a grand challenge in physics and materials science due to the difficulty of experimentally probing materials at varied length and time scales. X-ray photon correlation spectroscopy (XPCS) is uniquely well-suited for characterizing materials dynamics over wide-ranging time scales. However, spatial and temporal heterogeneity in material behavior can make interpretation of experimental XPCS data difficult. In this work, we have developed an unsupervised deep learning (DL) framework for automated classification of relaxation dynamics from experimental data without requiring any prior physical knowledge of the system. We demonstrate how this method can be used to accelerate exploration of large datasets to identify samples of interest, and we apply this approach to directly correlate microscopic dynamics with macroscopic properties of a model system. Importantly, this DL framework is material and process agnostic, marking a concrete step towards autonomous materials discovery.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Direct observation of ultrafast cluster dynamics in supercritical carbon dioxide using X-ray Photon Correlation Spectroscopy

Supercritical fluids exhibit distinct thermodynamic and transport properties, making them of particular interest for a wide range of scientific and engineering applications. These anomalous properties emerge from structural heterogeneities due to the formation of molecular clusters at conditions above the critical point. While the static behavior of these clusters and their effects on the thermodynamic response functions have been recognized, the relation between the ultrafast cluster dynamics and transport properties remains elusive. By measuring the intermediate scattering function in carbon dioxide at conditions near the critical point with X-ray photon correlation spectroscopy, we directly capture the cross-over dynamics between 4 and 13 picoseconds, revealing the transition between ballistic and diffusive motion. Complementary analysis using large-scale molecular dynamics simulations reveals that this behavior arises from collisions between unbound molecules and clusters. This study provides direct evidence of the ultrafast momentum exchange between clusters, which has significant impact on transport properties, solvation processes, and reaction kinetics in supercritical fluids.

carbon capture and storage↗

DOE OSTI2025

Non-equilibrium anti-Stokes Raman spectroscopy for investigating Higgs modes in superconductors

Abstract Even before its role in electroweak symmetry breaking, the Anderson-Higgs mechanism was introduced to explain the Meissner effect in superconductors. Spontaneous symmetry-breaking yields massless phase modes representing the low-energy excitations of the Mexican-Hat potential. Only in superconductors the phase mode is shifted towards higher energies owing to the gauge field of the charged condensate. This results in a low-energy excitation spectrum governed by the Higgs mode. Consequently, the Bardeen-Cooper-Schrieffer-like Meissner effect signifies a macroscopic quantum condensate in which a photon acquires mass, representing a one-to-one analogy to high-energy physics. We report on an innovative spectroscopic technique to study symmetries and energies of the Higgs modes in the high-temperature superconductor Bi 2 Sr 2 CaCu 2 O 8 after a soft quench of the Mexican-Hat potential. Population inversion induced by an initial laser pulse leads to an additional anti-Stokes Raman-scattering signal, which is consistent with polarization-dependent Higgs modes. Within Ginzburg-Landau theory, the Higgs-mode energy is connected to the Cooper-pair coherence length. Within a Bardeen-Cooper-Schrieffer weak-coupling model we develop a quantitative and coherent description of single-particle and two-particle channels. This opens the avenue for Higgs Spectroscopy in quantum condensates and provides a unique pathway to control and explore Higgs physics.

Science & Technology - Other Topics↗

DOE OSTI2020

Tensor factorization for elucidating mechanisms of piezoresponse relaxation via dynamic Piezoresponse Force Spectroscopy

Spatially resolved time and voltage-dependent polarization dynamics in PbTiO 3 thin films is explored using dynamic piezoresponse force microscopy (D-PFM) in conjunction with interferometric displacement sensing. This approach gives rise to 4D data sets containing information on bias-dependent relaxation dynamics at each spatial location without long-range electrostatic artifacts. To interpret these data sets in the absence of defined physical models, we employ a non-negative tensor factorization method which clearly presents the data as a product of simple behaviors allowing for direct physics interpretation. Correspondingly, we perform phase-field modeling finding the existence of ‘hard’ and ‘soft’ domain wall edges. This approach can be extended to other multidimensional spectroscopies for which even exploratory data analysis leads to unsatisfactory results due to many components in the decomposition.

36 MATERIALS SCIENCE↗

DOE OSTI2021

Gaussian process analysis of electron energy loss spectroscopy data: multivariate reconstruction and kernel control

Abstract Advances in hyperspectral imaging including electron energy loss spectroscopy bring forth the challenges of exploratory and physics-based analysis of multidimensional data sets. The multivariate linear unmixing methods generally explore similarities in the energy dimension, but ignore correlations in the spatial domain. At the same time, Gaussian process (GP) explicitly incorporate spatial correlations in the form of kernel functions but is computationally intensive. Here, we implement a GP method operating on the full spatial domain and reduced representations in the energy domain. In this multivariate GP, the information between the components is shared via a common spatial kernel structure, while allowing for variability in the relative noise magnitude or image morphology. We explore the role of kernel constraints on the quality of the reconstruction, and suggest an approach for estimating them from the experimental data. We further show that spatial information contained in higher-order components can be reconstructed and spatially localized.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Forecasting of in situ electron energy loss spectroscopy

Abstract Forecasting models are a central part of many control systems, where high-consequence decisions must be made on long latency control variables. These models are particularly relevant for emerging artificial intelligence (AI)-guided instrumentation, in which prescriptive knowledge is needed to guide autonomous decision-making. Here we describe the implementation of a long short-term memory model (LSTM) for forecasting in situ electron energy loss spectroscopy (EELS) data, one of the richest analytical probes of materials and chemical systems. We describe key considerations for data collection, preprocessing, training, validation, and benchmarking, showing how this approach can yield powerful predictive insight into order-disorder phase transitions. Finally, we comment on how such a model may integrate with emerging AI-guided instrumentation for powerful high-speed experimentation.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Ramification of complex magnetism in Nd 2 Ir 2 O 7 observed by Raman scattering spectroscopy

Using Raman scattering spectroscopy, we uncover a complex magnetic behavior of Nd2Ir2O7, which stands out among magnetic pyrochlores by the lowest temperature of the all-in-all-out (AIAO) Ir moments ordering (${T}_{{\rm{Ir}}}^{{\rm{N}}} = 33$ K) and the highest temperature at which AIAO order of rare-earth Nd ions is detected (${T}_{{\rm{Nd}}}^{{\rm{* }}}$ = 15 K). Detected magnetic Raman scattering and calculations of expected response allow us to demonstrate that the ordering of Ir magnetic moments is accompanied by an appearance of one-magnon Raman modes at 26.3 and 29.6 meV compatible with the AIAO order and allowing to estimate the energies of Ir-Ir interactions. An additional two-magnon excitation of the AIAO Nd order at around 33 meV appears in the spectra below the ordering temperature of Nd moments ${T}_{{\rm{Nd}}}^{{\rm{* }}}$ = 15 K. In the temperature range between 15 K and 33 K we observe a broad mode, which demonstrates strong temperature dependence and shifts on cooling below 20 K from 14 meV to higher frequencies, and disappears at 5 K, when two-magnon excitation of Nd moments becomes prominent. We suggest an interpretation of this excitation in terms of continuum arising from collective fluctuations of Nd moments above the transition. This complex behavior emerges from the interplay of strong spin-orbit coupling, electronic correlations, and geometric frustration on two magnetic pyrochlore sublattices of Nd and Ir ions.

magnetic properties and materials↗

DOE OSTI2022

Observation of light-driven band structure via multiband high-harmonic spectroscopy

Intense light–matter interactions have revolutionized our ability to probe and manipulate quantum systems at sub-femtosecond timescales, opening routes to the all-optical control of electronic currents in solids at petahertz rates. Such control typically requires electric-field amplitudes in the range of almost volts per angstrom, when the voltage drop across a lattice site becomes comparable to the characteristic bandgap energies. In this regime, intense light–matter interaction induces notable modifications to the electronic and optical properties, dramatically modifying the crystal band structure. Yet, identifying and characterizing such modifications remain an outstanding problem. As the oscillating electric field changes within the driving field’s cycle, does the band structure follow and how can it be defined? Here we address this fundamental question, proposing all-optical spectroscopy to probe the laser-induced closing of the bandgap between adjacent conduction bands. Our work reveals the link between nonlinear light–matter interactions in strongly driven crystals and the sub-cycle modifications in their effective band structure.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2024

Probing inhomogeneous cuprate superconductivity by terahertz Josephson echo spectroscopy

Abstract Inhomogeneities crucially influence the properties of quantum materials, yet methods that can measure them remain limited and can access only a fraction of relevant observables. For example, local probes such as scanning tunnelling microscopy have documented that the electronic properties of cuprate superconductors are inhomogeneous over nanometre length scales. However, complementary techniques that can resolve higher-order correlations are needed to elucidate the nature of these inhomogeneities. Furthermore, local tunnelling probes are often effective only far below the critical temperature. Here we develop a two-dimensional terahertz spectroscopy method to measure Josephson plasmon echoes from an interlayer superconducting tunnelling resonance in a near-optimally doped cuprate. The technique allows us to study the multidimensional optical response of the interlayer Josephson coupling in the material and disentangle intrinsic lifetime broadening from extrinsic inhomogeneous broadening for interlayer superconducting tunnelling. We find that inhomogeneous broadening persists up to a substantial fraction of the critical temperature, above which this is overcome by the thermally increased lifetime broadening.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2022

Attosecond spectroscopy of size-resolved water clusters

Electron dynamics in water are of fundamental importance for a broad range of phenomena, but their real-time study faces numerous conceptual and methodological challenges. Here, in this paper, we introduce attosecond size-resolved cluster spectroscopy and build up a molecular-level understanding of the attosecond electron dynamics in water. We measure the effect that the addition of single water molecules has on the photoionization time delays of water clusters. We find a continuous increase of the delay for clusters containing up to four to five molecules and little change towards larger clusters. We show that these delays are proportional to the spatial extension of the created electron hole, which first increases with cluster size and then partially localizes through the onset of structural disorder that is characteristic of large clusters and bulk liquid water. These results indicate a previously unknown sensitivity of photoionization delays to electron-hole delocalization and indicate a direct link between electronic structure and attosecond photoionization dynamics. Our results offer new perspectives for studying electron-hole delocalization and its attosecond dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Spectroscopy of the fractal Hofstadter energy spectrum

Hofstadter’s butterfly, the predicted energy spectrum for non-interacting electrons confined to a two-dimensional lattice in a magnetic field, is one of the most remarkable fractal structures in nature. At rational ratios of magnetic flux quanta per lattice unit cell, this spectrum shows self-similar distributions of energy levels that reflect its recursive construction. For most materials, Hofstadter’s butterfly is predicted under experimental conditions that are unachievable using laboratory-scale magnetic fields. More recently, electrical transport studies have provided evidence for Hofstadter’s butterfly in materials engineered to have artificially large lattice constants, such as those with moiré superlattices. Yet, so far, direct spectroscopy of the fractal energy spectrum predicted by Hofstadter nearly 50 years ago has remained out of reach. Here, in this work, we use high-resolution scanning tunnelling microscopy/spectroscopy (STM/STS) to investigate the flat electronic bands in twisted bilayer graphene (TBG) near the predicted second magic angle, an ideal setting for spectroscopic studies of Hofstadter’s spectrum. Our study shows the fractionalization of flat moiré bands into discrete Hofstadter subbands and discerns experimental signatures of self-similarity of this spectrum. Moreover, our measurements uncover a spectrum that evolves dynamically with electron density, showing phenomena beyond that of Hofstadter’s original model owing to the combined effects of strong correlations, Coulomb interactions and the quantum degeneracy of electrons in TBG.

electronic properties and materials↗

DOE OSTI2025

Superconducting gap of H 3 S measured by tunnelling spectroscopy

Several hydrogen-rich superconductors have been found to show unprecedentedly high critical temperatures, stimulating investigations into the nature of the superconductivity in these materials. Although their macroscopic superconducting properties are established, microscopic insights into the pairing mechanism remains unclear. Here we characterize the superconducting gap structure in the high-temperature superconductor H 3 S and its deuterium counterpart D 3 S by performing tunnelling spectroscopy measurements. The tunnelling spectra reveal that H 3 S and D 3 S both have a fully gapped structure, which could be well described by a single s-wave Dynes model, with gap values 2Δ of approximately 60 meV and 44 meV, respectively. Furthermore, we observed gap features of another likely H-depleted H x S superconducting phase in a poorly synthesized hydrogen sulfide sample. Our work offers direct experimental evidence for superconductivity in the hydrogen-rich superconductor H 3 S from a microscopic perspective. It validates the phonon-mediated mechanism of superconducting pairing and provides a foundation for further understanding the origins of high-temperature superconductivity in hydrogen-rich compounds.

36 MATERIALS SCIENCE↗

DOE OSTI2025

Magnon spectroscopy in the electron microscope

Abstract The miniaturization of transistors is approaching its limits owing to challenges in heat management and information transfer speed 1 . To overcome these obstacles, emerging technologies such as spintronics 2 are being developed, which make use of the electron’s spin as well as its charge. Local phenomena at interfaces or structural defects will greatly influence the efficiency of spin-based devices, making the ability to study spin-wave propagation at the nanoscale and atomic scale a key challenge 3,4 . The development of high-spatial-resolution tools to investigate spin waves, also called magnons, at relevant length scales is thus essential to understand how their properties are affected by local features. Here we detect bulk THz magnons at the nanoscale using scanning transmission electron microscopy (STEM). By using high-resolution electron energy-loss spectroscopy with hybrid-pixel electron detectors, we overcome the challenges posed by weak signals to map THz magnon excitations in a thin NiO nanocrystal. Advanced inelastic electron scattering simulations corroborate our findings. These results open new avenues for detecting magnons and exploring their dispersions and their modifications arising from nanoscale structural or chemical defects. This marks a milestone in magnonics and presents exciting opportunities for the development of spintronic devices.

Science & Technology - Other Topics↗

DOE OSTI2026

Symmetry, microscopy and spectroscopy signatures of altermagnetism

The recent discovery of altermagnetism was in part motivated by the research of compensated magnets towards highly scalable spintronic technologies. Simultaneously, altermagnetism shares the anisotropic higher-partial-wave nature of ordering with unconventional superfluid phases, which have been at the forefront of research for the past several decades. These examples illustrate the interest in altermagnetism from a broad range of science and technology perspectives. Here we review the symmetry, microscopy and spectroscopy signatures of altermagnetism. We describe the spontaneously broken and retained symmetries that delineate altermagnetism as a distinct phase of matter with d-, g- or i-wave compensated collinear spin ordering. In materials ranging from weakly interacting metals to strongly correlated insulators, the microscopic crystal-structure realizations of the altermagnetic symmetries feature a characteristic ferroic order of anisotropic higher-partial-wave components of atomic-scale spin densities. These symmetry and microscopy signatures of altermagnetism are directly reflected in spin-dependent electronic spectra and responses. Here, we review salient band-structure features originating from the altermagnetic ordering, and from its interplay with spin–orbit coupling and topological phenomena. Throughout, we compare altermagnetism with traditional ferromagnetism and Néel antiferromagnetism, and with magnetic phases with symmetry-protected compensated non-collinear spin orders. We accompany the theoretical discussions with references to relevant experiments.

Jungwirth, Tomas [Czech Academy of Sciences, Pragu↗

DOE OSTI2023

Simulated sulfur K-edge X-ray absorption spectroscopy database of lithium thiophosphate solid electrolytes

X-ray absorption spectroscopy (XAS) is a premier technique for materials characterization, providing key information about the local chemical environment of the absorber atom. In this work, we develop a database of sulfur K-edge XAS spectra of crystalline and amorphous lithium thiophosphate materials based on the atomic structures reported in Chem. Mater., 34, 6702 (2022). The XAS database is based on simulations using the excited electron and core-hole pseudopotential approach implemented in the Vienna Ab initio Simulation Package. Our database contains 2681 S K-edge XAS spectra for 66 crystalline and glassy structure models, making it the largest collection of first-principles computational XAS spectra for glass/ceramic lithium thiophosphates to date. This database can be used to correlate S spectral features with distinct S species based on their local coordination and short-range ordering in sulfide-based solid electrolytes. The data is openly distributed via the Materials Cloud, allowing researchers to access it for free and use it for further analysis, such as spectral fingerprinting, matching with experiments, and developing machine learning models.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Single crystal structure, vibrational spectroscopy, gas sorption and antimicrobial properties of a new inorganic acidic diphosphates material (NH 4 ) 2 Mg(H 2 P 2 O 7 ) 2 • 2 H 2 O

We report on the successful synthesis of diammonium magnesium dihydrogendiphosphate (V) dihydrate compound (NH 4 ) 2 Mg(H 2 P 2 O 7 ) 2 •2H 2 O using a wet chemical route. Single crystal X-ray diffraction analysis and micro Raman spectroscopy are employed to characterize the compound. We demonstrate, using a multidisciplinary approach, that this compound is ideal for carbon dioxide (CO 2 ) capture in addition to other anthropogenic gasses. We show here -from both an experimental as well as from a density functional theory (DFT) calculations routes- the potential for adopting this compound into domestic air-conditioning units (ACUs). From these experiments, the resistance to bacterial growth is also investigated, which is critical for the adoption of this compound in ACUs. Our compound exhibits a higher methane (CH 4 ) sorptivity as compared to CO 2 at 25 °C and 45 °C under pressures up to 50 bars. Furthermore, DFT electronic structure calculations are used to compute the main structural and electronic properties of the compound, taking into consideration the characteristics of the identified pores as a function of the progressive CO 2 vs. CH 4 loadings. Finally, the antibacterial assay reveals a strong antibacterial activity against the tested Gram-positive and Gram-negative bacteria, with a large zone of inhibition against the tested E. Coli, S. Aureus and K. Pneumonia

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Near field excited state imaging via stimulated electron energy gain spectroscopy of localized surface plasmon resonances in plasmonic nanorod antennas

Continuous wave (cw) photon stimulated electron energy loss and gain spectroscopy (sEELS and sEEGS) is used to image the near field of optically stimulated localized surface plasmon resonance (LSPR) modes in nanorod antennas. An optical delivery system equipped with a nanomanipulator and a fiber-coupled laser diode is used to simultaneously irradiate plasmonic nanostructures in a (scanning) transmission electron microscope. The nanorod length is varied such that the m = 1, 2, and 3 LSPR modes are resonant with the laser energy and the optically stimulated near field spectra and images of these modes are measured. Various nanorod orientations are also investigated to explore retardation effects. Optical and electron beam simulations are used to rationalize the observed patterns. As expected, the odd modes are optically bright and result in observed sEEG responses. The m = 2 dark mode does not produce a sEEG response, however, when tilted such that retardation effects are operative, the sEEG signal emerges. Thus, we demonstrate that cw sEEGS is an effective tool in imaging the near field of the full set of nanorod plasmon modes of either parity.

36 MATERIALS SCIENCE↗

DOE OSTI2020

Spatially resolved fibre cavity ring down spectroscopy

Abstract This paper presents a fibre cavity ring down spectroscopy probed by Rayleigh scattering optical frequency domain reflectometry (OFDR), which provides spatial location of stimuli and improved signal to noise ratio for distributed sensing measurements. A section of optical fibre was integrated into an active fibre ring cavity with optical gain and interrogated by the OFDR system for 11 cycles with a single laser scan. Through the cavity ring down configuration, root-mean-squared (RMS) noise of distributed temperature and strain measurements was reduced to 6.9 mK and less than 0.1 με, respectively for 1-cm spatially resolved measurements. Our work shows that the active fibre cavity configuration can be combined with distributed fibre sensing schemes to achieve both high spatial resolution and high sensitivity measurements.

97 MATHEMATICS AND COMPUTING↗