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Search indexed NASA NTRS and DOE OSTI research on propulsion, heat transfer, battery materials and energy systems. Follow report and document links to the original sources.

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At least 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Table-Top High Photon Energy Sources for Chemical Dynamics Investigations

Time-resolved spectroscopies using high-energy photons in the vacuum ultraviolet (VUV) to the X-ray region of the electromagnetic spectrum, have proven to be powerful probes of chemical dynamics. These high-energy photons can access valence and core orbitals of molecules and materials, providing key information on molecular and electronic structure and their time evolution. This report details the development of table-top sources of extreme ultraviolet (XUV) and VUV pulses at Sandia National Laboratories for use in studies of gas phase chemical dynamics. Femtosecond duration XUV pulses are produced using laser-driven high harmonic generation and their detected range span ~40-140 eV photon energies. These pulses are used in conjunction with ultraviolet pulses in a pump-probe scheme to study excited state dynamics of gas phase molecules. VUV pulses at 7.75 eV are generated using a four-wave-mixing scheme driven by 800 nm and 266 nm pulses in an argon-filled hollow-core fiber.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Time-resolved X-ray Spectroscopy from the Atomic Orbital Ground State Up

X-ray spectroscopy has been a key method to determine ground and excited state properties of quantum materials with atomic specificity. Now, new x-ray facilities are opening the door to the study of pump-probe x-ray spectroscopy - specifically time-resolved x-ray absorption (trXAS) and time-resolved resonant inelastic x-ray scattering (trRIXS). In this paper we will present simulations of each of these spectroscopies using a time-domain full atomic multiplet, charge transfer Hamiltonian, adapted to study the properties of a generalized cluster model including a central transition metal ion caged by ligand atoms in a planar geometry. The numerically evaluated trXAS and trRIXS cross-sections for representative electron configurations 3d9 and 3d8 demonstrate the insights that can be obtained from charge transfer pumping, and how this nonequilibrium process affects ground and excited state properties. The straightforward characterization of the excitations in these systems, based on our analysis of the simulations, can serve as a benchmark for future experiments, as access to these time-resolved spectroscopic techniques becomes more widely available.

Jost, Daniel↗
DOE OSTI2022

Ultrafast infrared nano-imaging of far-from-equilibrium carrier and vibrational dynamics

Ultrafast infrared nano-imaging has demonstrated access to ultrafast carrier dynamics on the nanoscale in semiconductor, correlated-electron, or polaritonic materials. However, mostly limited to short-lived transient states, the contrast obtained has remained insufficient to probe important long-lived excitations, which arise from many-body interactions induced by strong perturbation among carriers, lattice phonons, or molecular vibrations. Here, we demonstrate ultrafast infrared nano-imaging based on excitation modulation and sideband detection to characterize electron and vibration dynamics with nano- to micro-second lifetimes. As an exemplary application to quantum materials, in phase-resolved ultrafast nano-imaging of the photoinduced insulator-to-metal transition in vanadium dioxide, a distinct transient nano-domain behavior is quantified. In another application to lead halide perovskites, transient vibrational nano-FTIR spatially resolves the excited-state polaron-cation coupling underlying the photovoltaic response. These examples show how heterodyne pump-probe nano-spectroscopy with low-repetition excitation extends ultrafast infrared nano-imaging to probe elementary processes in quantum and molecular materials in space and time.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

Orbital-selective time-domain signature of nematicity dynamics in the charge-density-wave phase of La 1.65 Eu 0.2 Sr 0.15 CuO 4

Understanding the interplay between charge, nematic, and structural ordering tendencies in cuprate superconductors is critical to unraveling their complex phase diagram. Using pump–probe time-resolved resonant X-ray scattering on the (0 0 1) Bragg peak at the Cu L 3 and O K resonances, we investigate nonequilibrium dynamics of Q a = Q b = 0 nematic order and its association with both charge density wave (CDW) order and lattice dynamics in La 1.65 Eu 0.2 Sr 0.15 CuO 4 . The orbital selectivity of the resonant X-ray scattering cross-section allows nematicity dynamics associated with the planar O 2 p and Cu 3 d states to be distinguished from the response of anisotropic lattice distortions. A direct time-domain comparison of CDW translational-symmetry breaking and nematic rotational-symmetry breaking reveals that these broken symmetries remain closely linked in the photoexcited state, consistent with the stability of CDW topological defects in the investigated pump fluence regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2021

Toward witnessing molecular exciton entanglement from spectroscopy

Entanglement is a defining feature of quantum mechanics that can be a resource in engineered and natural systems, but measuring entanglement in experiment remains elusive especially for large chemical systems. Most practical approaches require determining and measuring a suitable entanglement witness which provides some level of information about the entanglement structure of the probed state. A fundamental quantity of quantum metrology is the quantum Fisher information (QFI), which is a rigorous witness of multipartite entanglement that can be evaluated from linear response functions for certain states. Here, in this paper, we explore measuring the QFI of molecular exciton states of the first-excitation subspace from spectroscopy. In particular, we utilize the fact that the linear response of a pure state subject to a weak electric field over all possible driving frequencies encodes the variance of the collective dipole moment in the probed state, which is a valid measure for QFI. The systems that are investigated include the molecular dimer, N-site linear aggregate with nearest-neighbor coupling, and N-site circular aggregate, all modeled as a collection of interacting qubits. Our theoretical analysis shows that the variance of the collective dipole moment in the brightest dipole-allowed eigenstate is the maximum QFI. The optical response of a thermally equilibrated state in the first-excitation subspace is also a valid QFI. Theoretical predictions of the measured QFI for realistic linear dye aggregates as a function of temperature and energetic disorder due to static variations of the host matrix show that two- to three-partite entanglement is realizable. This paper lays some groundwork and inspires measurement of multipartite entanglement of molecular excitons with ultrafast pump-probe experiments.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

An accurate and efficient Ehrenfest dynamics approach for calculating linear and nonlinear electronic spectra

Linear and nonlinear electronic spectra provide an important tool to probe the absorption and transfer of electronic energy. Here, we introduce a pure state Ehrenfest approach to obtain accurate linear and nonlinear spectra that is applicable to systems with large numbers of excited states and complex chemical environments. We achieve this by representing the initial conditions as sums of pure states and unfolding multi-time correlation functions into the Schrödinger picture. By doing this, we show that one can obtain significant improvements in accuracy over the previously used projected Ehrenfest approach and that these benefits are particularly pronounced in cases where the initial condition is a coherence between excited states. While such initial conditions do not arise when calculating linear electronic spectra, they play a vital role in capturing multidimensional spectroscopies. We demonstrate the performance of our method by showing that it is able to quantitatively capture the exact linear, 2D electronic spectroscopy, and pump–probe spectra for a Frenkel exciton model in slow bath regimes and is even able to reproduce the main spectral features in fast bath regimes.

Chemistry↗
DOE OSTI2022

Transient superconductivity at nano- and meso-scales

High-T c superconductivity is surpassed by few, if any, other unsolved problems in contemporary physics in terms of its richness, complexity, impact on other fields, and potential technological importance in energy applications. Recent discoveries reveal that the highest transition temperatures emerge under extraordinary experimental conditions such as the strong perturbation of a single atomic layer material by the underlying substrate, application of ~200 GPa pressure or ~MV/cm static electric fields, or irradiation by intense femtosecond optical fields. Research in superconductivity under extreme experimental conditions is challenging and requires the development of novel experimental methods and new theoretical tools suitable to tackle the problem. Our team has approached the challenges of transient superconductivity under intense optical fields by rethinking the types of experimental observables that are best suited to elucidate the physics of light-induced effects. This exercise has identified the need for: i) ultra-fast spatio-temporal probes enabling access to plasmonic properties and also nano-scale inhomogeneities that are ubiquitous in unconventional superconductors; ii) meso-scale structures and hybrid meta-surfaces imperative for strong enhancement of optical fields and iii) theoretical approaches suitable to explain and predict the response of superconductors under ultra-fast photo-excitation. Co-PIs have already made major advances with developing capabilities i)-iii). Therefore, our team is poised to make significant progress in transient superconductivity by exploring novel spatio-temporal effects that currently remain unattainable. Co-investigators will search for light-induced superconductivity in the high-T c cuprates to build upon spectacular recent results still lacking independent confirmations. Novel data acquisition methods combined with nano-plasmonic imaging will allow our team to test the hypothesis of photo-induced superconducting pairing. Spatio-temporal experiments will provide insights into the interplay between superconductivity and competing orders in the cuprates. Co-PIs will also investigate strong light-matter interaction and superconductivity in FeSe monolayers. Finally, we will study spatio-temporal electrodynamics of planar Josephson junctions. This latter direction will allow our team to thoroughly characterize one of the most fundamental examples of inhomogeneity in all of unconventional superconductivity. The proposed experiments in combination with theoretical analysis will provide information that is difficult to obtain using alternative methods. Basov and Averitt will carry out pump-probe spectroscopy and nano-imaging experiments. Averitt and Hone will design and fabricate state-of-the-art meta-surfaces. Theoretical and computational studies of ultrafast transient phenomena will be carried out by Millis and Fogler. Modeling of time-resolved nano-optical effects will be done by Fogler. The bulk of the requested budget will be used to support graduate students at Columbia & UCSD that will be co-supervised by co-PIs. The proposed program is transformative, since it will enable an entire suite of experiments previously either impossible or technically implausible. It will deliver critically important insights not only into mechanisms of unconventional superconductivity but also to many other correlated quantum materials.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Transient Terahertz Oscillations During Photoinduced Polarization Topology Reconfiguration in Ferroelectric Superlattices

Terahertz resonances embedded in crystalline heterostructures could close a spectral gap between conventional electronics and photonics while opening new windows on non-equilibrium lattice dynamics. We show that femtosecond optical screening of the depolarization field in epitaxial PbTiO3/SrTiO3 superlattices launches a collective polar mode that oscillates near 1 THz and coherently spans the entire mini-Brillouin zone. Wave-vector-resolved pump–probe X-ray diffraction resolves a nearly dispersion-less oscillation at 0.87 THz and 0.94 THz at the zone boundary and zone center, respectively, persisting for ~2.5 ps, corresponding to a weakly damped resonance. Dynamical phase-field simulations reveal the origin of the mode to mesoscopic rotation of closure-domain textures during the photo-excited transition from an unscreened to a screened electrostatic state. Varying the PbTiO3 and SrTiO3 ratio tunes the mode frequency continuously from 0.9 to 1.4 THz, providing a quantitative design rule for frequency-selectable THz oscillators in ferroelectric heterostructures. By coupling nanoscale polarization reconfiguration to long-wavelength coherent dynamics, this work establishes depolarization-field engineering to topology-driven THz functionality and expanding the landscape of collective lattice dynamics.

Sri Gyan, Deepankar [Univ. of Wisconsin, Madison, ↗
DOE OSTI2023

Photoexcitation of Fe 3 O Nodes in MOF Drives Water Oxidation at pH=1 When Ru Catalyst Is Present

Abstract Artificial photosynthesis strives to convert the energy of sunlight into sustainable, eco‐friendly solar fuels. However, systems with light‐driven water oxidation reaction (WOR) at pH=1 are rare. Broadly used [Ru(bpy) 3 ] 2+ (bpy=2,2’‐bipyridine) photosensitizer has a fixed +1.23 V potential which is insufficient to drive most water oxidation catalysts (WOCs) in acid, while Fe 2 O 3 , featuring the highly oxidizing holes, is not stable at low pH. Here, the key examples of Fe‐based metal–organic framework (MOF) water oxidation photoelectrocatalysts active at pH=1 are presented. Fe‐MIL‐126 and Fe MOF‐dcbpy structures were formed with 4,4’‐biphenyl dicarboxylate (bpdc), 2,2’‐bipyridine‐5,5’‐dicarboxylate (dcbpy) linkers and their mixtures. Presence of dcbpy linkers allows integration of metal‐based catalysts via coordination to 2,2’‐bipyridine fragments. Fe‐based MOFs were doped with Ru‐based precursors to achieve highly active MOFs bearing [Ru(bpy)(dcbpy)(H 2 O) 2 ] 2+ WOC. Materials were analyzed with X‐ray diffraction (XRD), scanning electron microscopy (SEM), Fourier transform infra‐red (FTIR) spectroscopy, resonance Raman, X‐ray absorption spectroscopy, fs optical pump‐probe, electron paramagnetic resonance (EPR), diffuse reflectance and electric conductivity measurements and were modeled by band structure calculations. It is shown that under reaction conditions, Fe III and Ru III oxidation states are present, indicating rate‐limiting electron transfer in MOF. Fe 3 O nodes emerge as photosensitizers able to drive prolonged O 2 evolution in acid. Further developments are possible via MOF's linker modification for enhanced light absorption, electrical conductivity, reduced MOF solubility in acid, Ru‐WOC modification for faster WOC catalysis, or Ru‐WOC substitution to 3d metal‐based systems. The findings give further insight for development of light‐driven water splitting systems based on Earth‐abundant metals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2024

Time-resolved photoelectron spectroscopy via trajectory surface hopping

Time-resolved photoelectron spectroscopy is a powerful pump-probe technique which can probe nonadiabatic dynamics in molecules. Interpretation of the experimental signals however requires input from theoretical simulations. Advances in electronic structure theory, nonadiabatic dynamics, and theory to calculate the ionization yields, have enabled accurate simulation of time-resolved photoelectron spectra leading to successful applications of the technique. Here, we review the basic theory and steps involved in calculating time-resolved photoelectron spectra, and highlight successful applications.

Chakraborty, Pratip↗
DOE OSTI2022

A Square Pulse Thermoreflectance Technique for the Measurement of Thermal Properties

We report on a laser-based square pulse thermoreflectance (SPTR) technique for the measurement of thermal properties for a wide range of materials. SPTR adopts the pump-probe thermoreflectance principle to monitor the evolution of local temperature after square pulse excitation. The technique features a compact setup, high spatial resolution, and fast data collection. By comparing the acquired SPTR signals with a continuum heat transfer model, material thermal properties can be obtained. Taking advantage of various spot sizes and modulation frequencies, SPTR can measure both the thermal diffusivity and thermal conductivity of poorly to moderately conductive materials and the thermal conductivity of conductive materials with satisfactory accuracy, with potential to be applied to more conductive materials. The technique was validated on three materials: fused silica, single crystal CaF2 and single crystal nickel (with conductivities ranging from 1 W·m -1 ·K -1 to 100 W·m -1 ·K -1 ) with typical measurement errors of 5 % to 20 %. The leading sources of error have been identified by Monte Carlo simulations, and the primary limitations of SPTR are discussed. The compact, fiberized platform we describe here will allow instruments based on this methodology to be deployed in complex, multi-analytical environments for the type of high-throughput correlative analyses that are key to materials design and discovery.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2025

Electronic Melting of Silicon in Nanostructures using X-ray Forbidden Bragg Reflections

Abstract We carried out a short beamtime at the Pohang Accelerator Laboratory x-ray Free Electron Laser to perform a pump-probe (PP) laser excitation diffraction experiment on the silicon (222) forbidden Bragg peak. To limit the x-ray penetration, we used a “device layer” silicon film wafer bonded to a silicon substrate. The sample, specially fabricated by MEMC Electronic Materials, had a Si(100) substrate bonded to a 170 nm Si(100) film rotated at 45° for crystallographic isolation. A second sample was reactive-ion-etched down to 52 nm thickness. In the silicon lattice, the covalent bonds are seen exclusively at the 222 reflection. Upon laser excitation, these electrons are expected to be excited to the valence band on femtosecond electronic time scales. The Si(222) reflection is therefore expected to be extinguished on this fast time scale, while the electron–phonon coupled acoustic response is determined by the lattice dynamics. The latter is determined by the speed of sound over the device thickness, which is in the mid-picosecond range.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2024

Exploring the relationship between deposition method, microstructure, and performance of Nb/Si-based superconducting coplanar waveguide resonators

Superconducting quantum circuits (SQC) are one of the most promising hardware platforms for quantum computing, yet their performance is currently limited by the presence of various structural defects inside the circuit's structure. Despite impressive progress in the past decade, a precise understanding of the origin of these defects from various fabrication processes and their impact on coherence is still lacking. Here, in this study, we performed a comprehensive investigation on the microstructure, superconductivity, and resonator quality factor of Nb films deposited by high-power impulse magnetron sputtering (HiPIMS) and direct current (DC) magnetron sputtering. A suite of characterization techniques, including electron microscopy with spectroscopy, secondary ion mass spectrometry, magneto-optical microscopy, and pump-probe reflectivity spectroscopy is used. We reveal that niobium (Nb) resonators fabricated using HiPIMS exhibit a smaller average grain size, thicker surface oxide with larger thickness variations (rougher surface), and a thicker amorphous Nb/Si interface layer compared to samples deposited by DC sputtering. We identified that the amorphous Nb oxides (mainly located at the Nb surface and along the grain boundaries) and Nb-Si amorphous layers (at the Nb/Si interface) are major and potential sources of two-level system (TLS), while off-stochiometric oxides and suboxides of Nb close to the surface, crystalline defects (i.e., dislocations at grain boundary, point defects introduced during deposition) are main contributors of non-TLS sources. Our findings clarify the relationship between different defects and coherence loss mechanisms, highlighting the importance of material microstructure control on performance optimization in SQC.

36 MATERIALS SCIENCE↗
DOE OSTI2020

NESSi : The N on- E quilibrium S ystems S imulation package

The nonequilibrium dynamics of correlated many-particle systems is of interest in connection with pump–probe experiments on molecular systems and solids, as well as theoretical investigations of transport properties and relaxation processes. Nonequilibrium Green’s functions are a powerful tool to study interaction effects in quantum many-particle systems out of equilibrium, and to extract physically relevant information for the interpretation of experiments. Here, we present the open-source software package NESSi (The Non-Equilibrium Systems Simulation package) which allows to perform many-body dynamics simulations based on Green’s functions on the L-shaped Kadanoff–Baym contour. NESSi contains the library libcntr which implements tools for basic operations on these nonequilibrium Green’s functions, for constructing Feynman diagrams, and for the solution of integral and integro-differential equations involving contour Green’s functions. The library employs a discretization of the Kadanoff–Baym contour into time points and a high-order implementation of integration routines. The total integrated error scales up to $\mathcal{O}(N^{-7})$, which is important since the numerical effort increases at least cubically with the simulation time. A distributed-memory parallelization over reciprocal space allows large-scale simulations of lattice systems. We provide a collection of example programs ranging from dynamics in simple two-level systems to problems relevant in contemporary condensed matter physics, including Hubbard clusters and Hubbard or Holstein lattice models. The libcntr library is the basis of a follow-up software package for nonequilibrium dynamical mean-field theory calculations based on strong-coupling perturbative impurity solvers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Photometric sensing of heavy metal ions using a naphthoquinodimethyl- bis -thioamide dye: Selectivity & photophysics of the metal organic complexes

As Mother Nature is experiencing catastrophic environmental pollutions from both natural sources and anthropogenic activities, many scientists have been working around the clock to develop environmentally benign and cost-effective, yet sensitive, detection techniques for pollutants, especially heavy metal species (e.g. lead, cadmium, mercury, among others) that are deleterious to human health. Herein, we report a novel sulfur-containing small organic dye/sensor naphthoquinodimethyl-bis-thioamide (QDM), which was found to be particularly selective toward mercury ion (Hg 2+ ). Using a combination of UV-vis absorption, photoluminescence, and time-resolved pump-probe techniques, we established that QDM and Hg 2+ can form stable complex(es) due to the strong affinity of sulfur toward mercury. In this investigation, while a higher ratio of QDM:Hg 2+ was necessary to fully quench the fluorescence emission of QDM, only 1 equiv of the Hg 2+ ion was necessary to observe the sensing effect on the excited state photo-behavior(s) of QDM. Furthermore, the present results highlight a synergy between molecular sensors' selectivity/sensitivity and sensor-analytes dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Unsupervised anomaly detection in MeV ultrafast electron diffraction

MeV ultrafast electron diffraction (MUED) is a pump-probe technique used to study the dynamic structural evolution of materials. An ultrashort laser pulse triggers structural changes, which are then probed by an ultrashort relativistic electron beam. To overcome low signal-to-noise ratios, diffraction patterns are averaged over thousands of shots. However, shot-to-shot instabilities in the electron beam can distort individual patterns, introducing uncertainty. Improving MUED accuracy requires detecting and removing these anomalous patterns from large datasets. In this work, we developed a fully unsupervised methodology for the detection of anomalous diffraction patterns. Using a convolutional autoencoder, we calculate the reconstruction mean squared error of the diffraction patterns. Based on the statistical analysis of this error, we provide the user an estimation of the probability that the pattern is normal, which also allows a posterior visual inspection of the images that are difficult to classify. This method has been trained with only 100 diffraction patterns and tested on 1521 patterns, resulting in a false positive rate between 0.2% and 0.4%, with a training time of 10 s per image and a test time of about 1 s per image. Here, the proposed methodology can also be applied to other diffraction techniques in which large datasets are collected that include faulty images due to instrumental instabilities.

43 PARTICLE ACCELERATORS↗
DOE OSTI2023

Measurement of optically-pumped electron spin polarization in n-GaAs at high external electric fields

We use the technique of time-resolved Kerr rotation (TRKR) to measure the electron spin polarization generated by optical spin pumping in an n-type gallium arsenide (GaAs) epilayer when an external electric field is simultaneously applied on the sample. The drift of the electron spins under the influence of the external electric field is captured with spatial scans of the pump–probe separation. A significant decay in the magnitude of electron spin polarization with electric field is observed and is attributed to the increased inhomogeneous broadening caused by the field-induced drift and the hot electron effects. Here, we extend the electric field range to as high as the Gunn threshold field in the measurement and we do not observe a spin amplification effect due to the spin Gunn effect under our experimental scheme.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Magnetic field driven emergent phenomena: Insights from magneto-optics and nanoscopy

This review explores magnetic field-driven emergent phenomena across various material systems, emphasizing the pivotal roles of magneto-optical and nanoscopy techniques. We examine fundamental aspects of Landau electrodynamics in both 2D and 3D systems, including quantum Hall and topological magnetoelectric effects in graphene and topological insulators. Particularly attention is given to magnetic excitations and magnetopolaritons, such as surface magnon polaritons, magnetoplasmons, and magnetoexcitons in novel quantum materials, including quantum magnets and hybrid heterostructures. Advanced imaging techniques, such as scattering-type scanning near-field optical microscopy (SNOM) and microwave impedance microscopy, are showcased for their capability to resolve these phenomena with microscopic and nanoscopic resolution. These insights are complemented by discussions of advanced experimental approaches, including cryogenic environments, ultrafast pump-probe techniques, and the integration of magnetic fields into near-field optical methodologies. We further investigate the potential of these imaging techniques for unraveling complex magnetic orders, quantum phases, and correlated electronic behaviors. Finally, we offer perspectives on future research directions and highlight emerging opportunities in the evolving field of optical magneto-nanoscopy.

36 MATERIALS SCIENCE↗