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DOE OSTI2024

Out-of-equilibrium charge redistribution in a copper-oxide based superconductor by time-resolved X-ray photoelectron spectroscopy

Charge-transfer excitations are of paramount importance for understanding the electronic structure of copper-oxide based high-temperature superconductors. In this study, we investigate the response of a Bi 2 Sr 2 CaCu 2 O 8+δ crystal to the charge redistribution induced by an infrared ultrashort pulse. Element-selective time-resolved core-level photoelectron spectroscopy with a high energy resolution allows disentangling the dynamics of oxygen ions with different coordination and bonds thanks to their different chemical shifts. Our experiment shows that the O 1s component arising from the Cu–O planes is significantly perturbed by the infrared light pulse. Conversely, the apical oxygen, also coordinated with Sr ions in the Sr-O planes, remains unaffected. This result highlights the peculiar behavior of the electronic structure of the Cu–O planes. It also unlocks the way to study the out-of-equilibrium electronic structure of copper-oxide-based high-temperature superconductors by identifying the O 1s core-level emission originating from the oxygen ions in the Cu–O planes. This ability could be critical to gain information about the strongly-correlated electron ultrafast dynamical mechanisms in the Cu–O plane in the normal and superconducting phases.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

DOE OSTI2025

A Representation Fusion Framework for Decoupling Diagnostic Information in Multimodal Learning

Modern medicine increasingly relies on multimodal data, ranging from clinical notes to imaging and genomics, to guide diagnosis and treatment. However, integrating these heterogeneous data sources in a principled and interpretable manner remains a major challenge. We present MODES (Multi-mOdal Disentangled Embedding Space), a representation fusion framework that explicitly separates shared and modality-specific factors of variation, offering a structured latent space for multimodal information that improves both prediction and interpretability. By leveraging pre-trained unimodal foundation models, MODES mitigates the dependency on extensive paired datasets, crucial in data-scarce clinical settings. We introduce a masking strategy that optimizes representation dimensionality by eliminating low-information dimensions, to achieve compact, information-rich representations. Our framework demonstrates superior performance in predicting diagnoses and phenotypes compared to unimodal and conventional fusion models. MODES also enables robust diagnostic inference in missing data scenarios, offering an opportunity toward interpretable and efficient multimodal diagnostics in personalized healthcare.

60 APPLIED LIFE SCIENCES↗

DOE OSTI2022

A localized view on molecular dissociation via electron-ion partial covariance

Inner-shell photoelectron spectroscopy provides an element-specific probe of molecular structure, as core-electron binding energies are sensitive to the chemical environment. Short-wavelength femtosecond light sources, such as Free-Electron Lasers (FELs), even enable time-resolved site-specific investigations of molecular photochemistry. Here, we study the ultraviolet photodissociation of the prototypical chiral molecule 1-iodo-2-methylbutane, probed by extreme-ultraviolet (XUV) pulses from the Free-electron LASer in Hamburg (FLASH) through the ultrafast evolution of the iodine 4d binding energy. Methodologically, we employ electron-ion partial covariance imaging as a technique to isolate otherwise elusive features in a two-dimensional photoelectron spectrum arising from different photofragmentation pathways. The experimental and theoretical results for the time-resolved electron spectra of the 4d 3/2 and 4d 5/2 atomic and molecular levels that are disentangled by this method provide a key step towards studying structural and chemical changes from a specific spectator site.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2020

Time-reversal of an unknown quantum state

For decades, researchers have sought to understand how the irreversibility of the surrounding world emerges from the seemingly time-symmetric, fundamental laws of physics. Quantum mechanics conjectured a clue that final irreversibility is set by the measurement procedure and that the time-reversal requires complex conjugation of the wave function, which is overly complex to spontaneously appear in nature. Building on this Landau-Wigner conjecture, it became possible to demonstrate that time-reversal is exponentially improbable in a virgin nature and to design an algorithm artificially reversing a time arrow for a given quantum state on the IBM quantum computer. However, the implemented arrow-of-time reversal embraced only the known states initially disentangled from the thermodynamic reservoir. Here we develop a procedure for reversing the temporal evolution of an arbitrary unknown quantum state. This opens the route for general universal algorithms sending temporal evolution of an arbitrary system backward in time.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2023

Competing incommensurate spin fluctuations and magnetic excitations in infinite-layer nickelate superconductors

The recently discovered infinite-layer nickelates show great promise in helping to disentangle the various cooperative mechanisms responsible for high-temperature superconductivity. However, lack of antiferromagnetic order in the pristine nickelates presents a challenge for connecting the physics of the cuprates and nickelates. Here, by using a quantum many-body Green’s function-based approach to treat the electronic and magnetic structures, we unveil the presence of many two- and three-dimensional magnetic stripe instabilities that are shown to persist across the phase diagram of LaNiO 2 . Our analysis indicates that the magnetic properties of the infinite-layer nickelates are closer to those of the doped cuprates, which host a stripe ground state, rather than the undoped cuprates. The computed longitudinal-spin, transverse-spin, and charge spectra of LaNiO 2 are found to contain an admixture of contributions from localized and itinerant carriers. Theoretically obtained dispersion of magnetic excitations (spin-flip) is found to be in good accord with the results of recent resonant inelastic X-ray scattering experiments. Our study gives insight into the origin of strong magnetic competition in the infinite-layer nickelates and their relationship with the cuprates.

36 MATERIALS SCIENCE↗

DOE OSTI2026

Terahertz 2D coherent spectroscopy for probing and controlling multicorrelations in quantum matter

Terahertz 2D coherent spectroscopy (THz-2DCS) is an emerging technique that brings multidimensional resolution to the ultrafast spectral–temporal dynamics of non-equilibrium quantum phases of matter, enabling new capabilities for precise coherent control in many-body dynamics and multiorder correlations. Here, by mapping and disentangling complex excitation and detection pathways across distinct time and frequency dimensions, THz-2DCS provides a form of coherence tomography of light-induced quantum matter — revealing multiquantum coherences, separating nonlinear response functions and capturing collective modes and quantum kinetics on ultrafast THz timescales. This Perspective discusses the technical capabilities of THz-2DCS, provides a comparison to other multidimensional and coherent transient spectroscopies and looks ahead towards opportunities for advancing THz-2DCS instrumentation and experimental strategies towards new frontier discoveries.

Huang, Chuankun [Ames Laboratory (AMES), Ames, IA ↗

DOE OSTI2022

AtomAI framework for deep learning analysis of image and spectroscopy data in electron and scanning probe microscopy

Over the past several decades, electron and scanning probe microscopes have become critical components of condensed matter physics, materials science and chemistry research. At the same time, the infrastructure for establishing a connection between microscopy observations and materials behaviour over a broader parameter space is lacking. In this work, we introduce AtomAI, an open-source software package bridging instrument-specific Python libraries, deep learning and simulation tools into a single ecosystem. AtomAI allows direct applications of deep neural networks for atomic and mesoscopic image segmentation converting image and spectroscopy data into class-based local descriptors for downstream tasks such as statistical and graph analysis. For atomically resolved imaging data, the output is types and positions of atomic species, with an option for subsequent refinement. AtomAI further allows the implementation of a broad range of image and spectrum analysis functions, including invariant variational autoencoders for disentangling structural factors of variation and im2spec type of encoder–decoder models for mapping structure–property relationships. Finally, our framework allows seamless connection to the first principles modelling with a Python interface on the inferred atomic positions.

36 MATERIALS SCIENCE↗

DOE OSTI2022

TbasCO: trait-based comparative ‘omics identifies ecosystem-level and niche-differentiating adaptations of an engineered microbiome

A grand challenge in microbial ecology is disentangling the traits of individual populations within complex communities. Various cultivation-independent approaches have been used to infer traits based on the presence of marker genes. However, marker genes are not linked to traits with complete fidelity, nor do they capture important attributes, such as the timing of gene expression or coordination among traits. To address this, we present an approach for assessing the trait landscape of microbial communities by statistically defining a trait attribute as a shared transcriptional pattern across multiple organisms. Leveraging the KEGG pathway database as a trait library and the Enhanced Biological Phosphorus Removal (EBPR) model microbial ecosystem, we demonstrate that a majority (65%) of traits present in 10 or more genomes have niche-differentiating expression attributes. For example, while many genomes containing high-affinity phosphorus transporter pstABCS display a canonical attribute (e.g. up-regulation under phosphorus starvation), we identified another attribute shared by many genomes where transcription was highest under high phosphorus conditions. Taken together, we provide a novel framework for unravelling the functional dynamics of uncultivated microorganisms by assigning trait-attributes through genome-resolved time-series metatranscriptomics.

59 BASIC BIOLOGICAL SCIENCES↗

DOE OSTI2024

Ultrafast dynamics of fluorene initiated by highly intense laser fields

Here, we present an investigation of the ultrafast dynamics of the polycyclic aromatic hydrocarbon fluorene initiated by an intense femtosecond near-infrared laser pulse (810 nm) and probed by a weak visible pulse (405 nm). Using a multichannel detection scheme (mass spectra, electron and ion velocity-map imaging), we provide a full disentanglement of the complex dynamics of the vibronically excited parent molecule, its excited ionic states, and fragments. We observed various channels resulting from the strong-field ionization regime. In particular, we observed the formation of the unstable tetracation of fluorene, above-threshold ionization features in the photoelectron spectra, and evidence of ubiquitous secondary fragmentation. We produced a global fit of all observed time-dependent photoelectron and photoion channels. This global fit includes four parent ions extracted from the mass spectra, 15 kinetic-energy-resolved ionic fragments extracted from ion velocity map imaging, and five photoelectron channels obtained from electron velocity map imaging. The fit allowed for the extraction of 60 lifetimes of various metastable photoinduced intermediates.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2023

Observation of parallel intersystem crossing and charge transfer-state dynamics in [Fe(bpy) 3 ] 2+ from ultrafast 2D electronic spectroscopy

Transition metal-based charge-transfer complexes represent a broad class of inorganic compounds with diverse photochemical applications. Charge-transfer complexes based on earth-abundant elements have been of increasing interest, particularly the canonical [Fe(bpy) 3 ] 2+ . Photoexcitation into the singlet metal–ligand charge transfer ( 1 MLCT) state is followed by relaxation first to the ligand-field manifold and then to the ground state. While these dynamics have been well-studied, processes within the MLCT manifold that facilitate and/or compete with relaxation have been more elusive. We applied ultrafast two-dimensional electronic spectroscopy (2DES) to disentangle the dynamics immediately following MLCT excitation of this compound. First, dynamics ascribed to relaxation out of the initially formed 1 MLCT state was found to correlate with the inertial response time of the solvent. Second, the additional dimension of the 2D spectra revealed a peak consistent with a ~20 fs 1 MLCT → 3 MLCT intersystem crossing process. These two observations indicate that the complex simultaneously undergoes intersystem crossing and direct conversion to ligand-field state(s). Resolution of these parallel pathways in this prototypical earth-abundant complex highlights the ability of 2DES to deconvolve the otherwise obscured excited-state dynamics of charge-transfer complexes.

2-dimensional electronic spectroscopy↗

DOE OSTI2024

Metal–support interactions in metal oxide-supported atomic, cluster, and nanoparticle catalysis

Supported metal catalysts are essential to a plethora of processes in the chemical industry. The overall performance of these catalysts depends strongly on the interaction of adsorbates at the atomic level, which can be manipulated and controlled by the different constituents of the active material (i.e., support and active metal). The description of catalyst activity and the relationship between active constituent and the support, or metal–support interactions (MSI), in heterogeneous (thermo)catalysts is a complex phenomenon with multivariate (dependent and independent) contributions that are difficult to disentangle, both experimentally and theoretically. So-called “strong metal–support interactions” have been reported for several decades and summarized in excellent review articles. However, in recent years, there has been a proliferation of new findings related to atomically dispersed metal sites, metal oxide defects, and, for example, the generation and evolution of MSI under reaction conditions, which has led to the designation of (sub)classifications of MSI deserving to be critically and systematically evaluated. These include dynamic restructuring under alternating redox and reaction conditions, adsorbate-induced MSI, and evidence of strong interactions in oxide-supported metal oxide catalysts. Here, we review recent literature on MSI in oxide-supported metal particles to provide an up-to-date understanding of the underlying physicochemical principles that dominate the observed effects in supported metal atomic, cluster, and nanoparticle catalysts. Critical evaluation of different subclassifications of MSI is provided, along with discussions on the formation mechanisms, theoretical and characterization advances, and tuning strategies to manipulate catalytic reaction performance. We also provide a perspective on the future of the field, and we discuss the analysis of different MSI effects on catalysis quantitatively.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Oxygen redox activities governing high-voltage charging reversibility of Ni-rich layered cathodes

A schematic illustration indicative of the improved structural reversibility through stabilizing oxidized oxygen by Al doping. The chemical reactions and phase transitions at high voltages are generally considered to determine the electrochemical properties of high-voltage layered cathodes such as Ni-rich rhombohedral oxides. Even if significantly higher SOCs (states-of-charge) are utilized above the capability of transition metal redox (primarily Ni and Co), the effect of oxygen redox on Ni-rich rhombohedral oxides still looks mysterious thereby necessitating research that can clarify the relationship between redox reactions and phase transitions. Here, we performed a comprehensive and comparative study of the cationic and anionic redox reactions, as well as the structural evolution of a series of commercial Ni-rich layered oxides with and without Al doping. We combined the results from X-ray spectroscopy, operando electrochemical mass spectrometry, and neutron diffraction with electrochemical properties and thereby revealed the different oxygen redox activities associated with structural and electrochemical degradations. We reveal that Al doping suppresses the irreversible oxygen release but enhances the lattice oxygen oxidization. With this modulated oxygen redox activity, the Ni-rich layered oxides’ notorious H2–H3 structural phase transition becomes highly reversible. Our findings disentangle the different oxygen redox activities during high-voltage cycling and clarify the role of dopants in the Ni-rich layered oxides in terms of structural and electrochemical stability, shedding light on the future direction of optimizing layered cathode materials for safer high energy-density secondary batteries.

Lee, Gi-Hyeok↗

DOE OSTI2024

Decoupling first-cycle capacity loss mechanisms in sulfide solid-state batteries

Solid-state batteries (SSBs) promise more energy-dense storage than liquid electrolyte lithium-ion batteries (LIBs). However, first-cycle capacity loss is higher in SSBs than in LIBs due to interfacial reactions. The chemical evolution of key interfaces in SSBs has been extensively characterized. Electrochemically, however, we lack a versatile strategy for quantifying the reversibility of solid electrolyte (SE) redox for established and next-generation SSB electrolytes. In this work, we perform tailored electrochemical tests and operando X-ray diffraction to disentangle reversible and irreversible sources of capacity loss in positive electrodes composed of Li 6 PS 5 Cl SE, Li(Ni 0.5 Mn 0.3 Co 0.2 )O 2 (NMC), and carbon conductive additives. We leverage an atypically low voltage cutoff (2.0 V vs. Li/Li + ) to quantify the reversibility of SE redox. Using slow (5.5 mA g NMC −1 ) cycling paired with >100 h low-voltage holds, our cells achieve a surprising 96.2% first-cycle coulombic efficiency, which is higher than previously reported (mean: 72%, maximum: 91.6% across surveyed literature). We clarify that sluggish NMC relithiation kinetics have been historically mistaken for permanently irreversible capacity loss. In conclusion, through systematic decoupling of loss mechanisms, we uncover the unexpected reversibility of SE redox and isolate the major contributors to capacity loss, outlining a strategy for accurate assessment of next-generation SE materials and interface modifications.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2025

Electrolytic gold plating, stripping, and ion transport dynamics through a solid-state iodide perovskite

The pronounced electrochemical reactivity between halide perovskites and metal electrodes can introduce mobile extrinsic metal ions which can cause device instability or enable novel functionalities. Here we systematically investigate the kinetics of gold cation (Au + ) migration in indium tin oxide (ITO)/methylammonium lead triiodide (MAPbI 3 )/Au model devices under long-term potentiostatic biasing. Scanning electron microscopy (SEM), X-ray photoelectron spectroscopy (XPS), and density functional theory (DFT) analyses reveal that Au + ions, electrochemically generated at the Au anode, traverse the perovskite layer with diffusion coefficients on the order of 10 −11 to 10 −10 cm 2 s −1 and are subsequently reduced at the cathode as Au 0 clusters, resembling metal plating behavior in electrolytic cells and solid-state batteries during charging. Furthermore, reversing the applied bias strips the plated Au 0 , revealing reversibility suitable for bipolar resistive switching devices and providing direct evidence of the electrochemical and ionic nature of Au transport within the perovskite matrix. Quantitatively determining diffusion coefficients and ion concentrations provides foundational inputs for future drift-diffusion modelling opportunities and allows us to relate our findings to implications on long term operation of devices like photovoltaic modules. These results clearly demonstrate the solid-state electrochemical nature of perovskite devices, highlight methods to be more quantitative about ion transport properties, provide and emphasize the importance of disentangling electro-, photo-, photoelectrochemical processes for understanding device performance and unlocking new functionalities.

14 SOLAR ENERGY↗

DOE OSTI2020

Simultaneous observations of the blazar PKS 2155-304 from ultra-violet to TeV energies

Here we report the results of the first ever contemporaneous multi-wavelength observation campaign on the BL Lac object PKS 2155−304 involving Swift , NuSTAR , Fermi -LAT, and H.E.S.S. The use of these instruments allows us to cover a broad energy range, which is important for disentangling the different radiative mechanisms. The source, observed from June 2013 to October 2013, was found in a low flux state with respect to previous observations but exhibited highly significant flux variability in the X-rays. The high-energy end of the synchrotron spectrum can be traced up to 40 keV without significant contamination by high-energy emission. A one-zone synchrotron self-Compton model was used to reproduce the broadband flux of the source for all the observations presented here but failed for previous observations made in April 2013. A lepto-hadronic solution was then explored to explain these earlier observational results.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2021

Looking through the photoionisation wake: Vela X-1 at φ orb ≈ 0.75 with Chandra /HETG

In this work, we detect and identify five narrow radiative recombination continua (Mg XI-XII, Ne IX-X, O VIII) and several emission lines from Fe, S, Si, Mg, Ne, Al, and Na, including four He-like triplets (S XV, Si XIII, Mg XI, and Ne IX). Photoionisation models reproduce the overall spectrum well, except for the near-neutral fluorescence lines of Fe, S, and Si. We conclude that the plasma is mainly photoionised, but more than one component is most likely present, which is consistent with a multi-phase plasma scenario, where denser and colder clumps of matter are embedded in the hot, photoionised wind of the companion star. Simulations with the future X-ray satellites Athena and XRISM show that a few hundred seconds of exposure is sufficient to disentangle the lines of the Fe Kα doublet and the He-like Fe XXV, improving, in general, the determination of the plasma parameters.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2024

Cepheids with giant companions: II. Spectroscopic confirmation of nine new double-lined binary systems composed of two Cepheids

Context.Binary Cepheids with giant companions are crucial for studying the physical properties of Cepheid variables, in particular providing the best means to measure their masses. Systems composed of two Cepheids are even more important, but to date, only one such system has been identified, in the Large Magellanic Cloud (LMC). Aims.Our current aim is to increase the number of these systems known tenfold and to provide their basic characteristics. The final goal is to obtain the physical properties of the component Cepheids, including their masses and radii, and to learn about their evolution in the multiple systems, also revealing their origin. Methods.We started a spectroscopic monitoring campaign of nine unresolved pairs of Cepheids from the OGLE catalog to check if they are gravitationally bound. Two of these so-called double Cepheids are located in the LMC, five are in the Small Magellanic Cloud (SMC), and two are in the Milky Way (MW). Results.We report a spectroscopic detection of the binarity of all nine of these double Cepheids with orbital periods ranging from 2 to 18 years. This increases the number of known binary double (BIND) Cepheids from 1 to 10 and triples the number of all confirmed double-lined binary (SB2) Cepheids. For five BIND Cepheids, the disentangled pulsational light curves of the components show anti-correlated phase shifts due to orbital motion. We show the first empirical evidence that typical period–luminosity relations (PLRs) are rather binary Cepheid PLRs, as they include light of the companion. Conclusions.The statistics of pulsation period ratios of BIND Cepheids do not agree with those expected for pairs of Cepheids of the same age. These ratios together with the determined mass ratios far from unity suggest a merger origin of at least one component for about half of the systems. The SMC and MW objects are the first found in SB2 systems composed of giants in their host galaxies. The Milky Way BIND Cepheids are also the closest such systems, being located at about 11 and 26 kpc.

Astronomy & Astrophysics↗

DOE OSTI2023

How can a diverse set of integral and semi-integral measurements inform identification of discrepant nuclear data?

Nuclear data are used for a variety of applications, including criticality safety, reactor performance, and material safeguards. Despite the breadth of use-cases, the effective neutron multiplication factor, keff, of ICSBEP critical assemblies are primarily used for nuclear data validation; these are sensitive to specific energy regions and nuclides and are unable to uniquely constrain nuclear data. As a consequence, general-purpose nuclear data libraries, such as ENDF/B-VIII.0, may have deficiencies that, while not apparent in criticality applications, negatively impact other applications, such as non-destructive analysis of special nuclear material and neutron diagnosed subcritical experiments. Recent work by the Experiments Underpinned by Computational Learning for Improvements in Nuclear Data (EUCLID) project developed a machine learning tool, RAFIEKI, which uses random forests and the SHAP metric to determine which nuclear data contribute most to predicted bias between measured and simulated responses (e.g. keff). This paper contrasts RAFIEKI analysis applied to keff only against RAFIEKI analysis with keff paired with either LLNL pulsed sphere measurements or subcritical benchmarks. Two examples show that a) including pulsed sphere measurements substantially increases 9Be nuclear data importance to bias between 2 and 15 MeV, and b) including subcritical benchmarks has the potential for disentangling compensating errors between 240Pu (n,el) and (n,il) cross-sections between 0.1 and 10 MeV. These results show that RAFIEKI analysis applied to response sets that include, but go beyond, keff can aid nuclear data evaluators in identifying issues in nuclear data.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗