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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 919 records · Page 51
All sourcesNASA NTRSDOE OSTI
DOE OSTI2021

Photocarrier Dynamics in MoTe 2 Nanofilms with 2 H and Distorted 1 T Lattice Structures

Molybdenum telluride (MoTe 2 ), an emerging layered two-dimensional (2D) material, possesses excellent phase-changing properties. Previous studies revealed its reversible transition between 2H and 1T' phases with a transition energy as small as 35 meV. Since 1T'-MoTe 2 is metallic, it can serve as an electrical contact for semiconducting 2H-MoTe 2 -based optoelectronic devices. Here, the photocarrier dynamics in MoTe 2 nanofilms synthesized by a one-step method and with coexisting multiple phases are investigated by transient absorption measurements. Both the energy relaxation time and the recombination lifetime of the excitons are shorter in the 1T'-MoTe 2 compared to its 2H phase. Furthermore, these results provide information on the different photocarrier dynamical properties of these two phases, which is important for future 2D optoelectronic and phase-change electronic devices based on MoTe 2 .

36 MATERIALS SCIENCE↗
DOE OSTI2023

Temperature dependence of resistivity of carbon micro/nanostructures: Microscale spatial distribution with mixed metallic and semiconductive behaviors

The temperature coefficient of resistivity (θ T ) of carbon-based materials is a critical property that directly determines their electrical response upon thermal impulses. It could have metal- (positive) or semiconductor-like (negative) behavior, depending on the combined temperature dependence of electron density and electron scattering. Its distribution in space is very difficult to measure and is rarely studied. Here, for the first time, we report that carbon-based micro/nanoscale structures have a strong non-uniform spatial distribution of θ T . This distribution is probed by measuring the transient electro-thermal response of the material under extremely localized step laser heating and scanning, which magnifies the local θ T effect in the measured transient voltage evolution. For carbon microfibers (CMFs), after electrical current annealing, θ T varies from negative to positive from the sample end to the center with a magnitude change of >130% over <1 mm. This θ T sign change is confirmed by directly testing smaller segments from different regions of an annealed CMF. For micro-thick carbon nanotube bundles, θ T is found to have a relative change of >125% within a length of ~2 mm, uncovering strong metallic to semiconductive behavior change in space. In conclusion, our θ T scanning technique can be readily extended to nm-thick samples with μm scanning resolution to explore the distribution of θ T and provide a deep insight into the local electron conduction.

36 MATERIALS SCIENCE↗
DOE OSTI2020

A chemical dynamics study on the gas-phase formation of triplet and singlet C 5 H 2 carbenes

Significance Carbenes represent key reactive intermediates in molecular mass growth processes leading to carbonaceous nanostructures in the interstellar medium and in combustion systems. However, due to their short lifetimes and tendency for dimerization, carbenes represent one of the foremost obscured classes of reactive intermediates, with the preparation of carbenes in the gas phase remaining largely elusive. By merging molecular beams with electronic structure and quasi-classical trajectory calculations and exploiting triplet pentadiynylidene (HCCCCCH) and singlet ethynylcyclopropenylidene (c-C 5 H 2 ) carbene as benchmarks, we present a versatile protocol to unravel the dynamics leading to exotic carbenes under single-collision conditions. These elementary mechanisms are of significance to our understanding of the fundamental processes leading to unsaturated organic transients in extreme, hydrocarbon-rich environments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Process-Structure-Property Relations for As-Deposited Solid-State Additively Manufactured High-Strength Aluminum Alloy

Solid-state additive manufacturing methods provide innovative solutions to circumvent problems associated with materials susceptible to hot cracking by avoiding liquid solid phase transformations. In this work, the process parameter influence on microstructural evolution and mechanical response of a fully dense aluminum alloy 7050 (AA7050) component manufactured via a rapid, solid-state additive manufacturing process known as Additive Friction Stir Deposition (AFS-D) was quantified for the first time. Three sections (starting dwell, transient, crossover of roads) of the deposition that exhibit differing thermomechanical processing histories were evaluated for the resulting microstructure and mechanical response. The microstructural characterization was performed on the as-deposited AA7050 via Electron Backscatter Diffraction (EBSD), TEM, optical microscopy, and Scanning Electron Microscopy (SEM). The microstructural characterization revealed refined constituent particles and grains throughout the as-deposited AA7050 microstructure. Furthermore, quasi-static tensile experiments were conducted in both the build and transverse directions, in order to quantify the orientation influence on tensile properties of the as-deposited AA7050 build. Spatially dependent tensile properties were observed in the material due to heat input variation coarsening of secondary phases towards the initial layers of the AFS-D build. Post-mortem analysis revealed that voids nucleated and coalesced from the overgrowth of the strengthening precipitates present in the material, resulting in fracture.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Effect of Anisotropic Confinement on Electronic Structure and Dynamics of Band Edge Excitons in Inorganic Perovskite Nanowires

Inorganic lead halide perovskite nanostructures show promise as the active layers in photovoltaics, light emitting diodes, and other optoelectronic devices. They are robust in the presence of oxygen and water, and the electronic structure and dynamics of these nanostructures can be tuned through quantum confinement. Here we create aligned bundles of CsPbBr3 nanowires with widths resulting in quantum confinement of the electronic wave functions and subject them to ultrafast microscopy. We directly image rapid one-dimensional exciton diffusion along the nanowires, and we measure an exciton trap density of roughly one per nanowire. Using transient absorption microscopy, we observe a polarization-dependent splitting of the band edge exciton line, and from the polarized fluorescence of nanowires in solution, we determine that the exciton transition dipole moments are anisotropic in strength. Furthermore, our observations are consistent with a model in which splitting is driven by shape anisotropy in conjunction with long-range exchange.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2020

Simultaneous Observation of Carrier-Specific Redistribution and Coherent Lattice Dynamics in 2H-MoTe 2 with Femtosecond Core-Level Spectroscopy

In this study, we employ few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy to reveal simultaneously the intra- and interband carrier relaxation and the light-induced structural dynamics in nanoscale thin films of layered 2H-MoTe 2 semiconductor. By interrogating the valence electronic structure via localized Te 4 d (39-46 eV) and Mo 4 p (35-38 eV) core levels, the relaxation of the photoexcited hole distribution is directly observed in real time. We obtain hole thermalization and cooling times of 15 ± 5 fs and 380 ± 90 fs, respectively, and an electron-hole recombination time of 1.5 ± 0.1 ps. Furthermore, excitations of coherent out-of-plane A 1g (5.1 THz) and in-plane E 1g (3.7 THz) lattice vibrations are visualized through oscillations in the XUV absorption spectra. By comparison to Bethe-Salpeter equation simulations, the spectral changes are mapped to real-space excited-state displacements of the lattice along the dominant A 1g coordinate. By directly and simultaneously probing the excited carrier distribution dynamics and accompanying femtosecond lattice displacement in 2H-MoTe 2 within a single experiment, our work provides a benchmark for understanding the interplay between electronic and structural dynamics in photoexcited nanomaterials.

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

Photodriven Ammonia Synthesis from Manganese Nitrides: Photophysics and Mechanistic Investigations

Ammonia synthesis from N,N,O,O-supported manganese(V) nitrides and 9,10-dihydroacridine using proton-coupled electron transfer and visible light irradiation in the absence of precious metal photocatalysts is described. While the reactivity of the nitride correlated with increased absorption of blue light, excited-state lifetimes determined by transient absorption were on the order of picoseconds. Furthermore, this eliminated excited-state manganese nitrides as responsible for bimolecular N–H bond formation. Spectroscopic measurements on the hydrogen source, dihydroacridine, demonstrated that photooxidation of 9,10-dihydroacridine was necessary for productive ammonia synthesis. Transient absorption and pulse radiolysis data for dihydroacridine provided evidence for the presence of intermediates with weak E–H bonds, including the dihydroacridinium radical cation and both isomers of the monohydroacridine radical, but notably these intermediates were unreactive toward hydrogen atom transfer and net N–H bond formation. Additional optimization of the reaction conditions using higher photon flux resulted in higher rates of the ammonia production from the manganese(V) nitrides due to increased activation of the dihydroacridine.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

RapidEELS: machine learning for denoising and classification in rapid acquisition electron energy loss spectroscopy

Recent advances in detectors for imaging and spectroscopy have afforded in situ, rapid acquisition of hyperspectral data. While electron energy loss spectroscopy (EELS) data acquisition speeds with electron counting are regularly reaching 400 frames per second with near-zero read noise, signal to noise ratio (SNR) remains a challenge owing to fundamental counting statistics. In order to advance understanding of transient materials phenomena during rapid acquisition EELS, trustworthy analysis of noisy spectra must be demonstrated. In this study, we applied machine learning techniques to denoise high frame rate spectra, benchmarking with slower frame rate “ground truths”. The results provide a foundation for reliable use of low SNR data acquired in rapid, in-situ spectroscopy experiments. Such a tool-set is a first step toward both automation in microscopy as well as use of these methods to interrogate otherwise poorly understood transformations.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Ghost-imaging-enhanced noninvasive spectral characterization of stochastic x-ray free-electron-laser pulses

Abstract High-intensity ultrashort X-ray free-electron laser (XFEL) pulses are revolutionizing the study of fundamental nonlinear x-ray matter interactions and coupled electronic and nuclear dynamics. To fully exploit the potential of this powerful tool for advanced x-ray spectroscopies, a noninvasive spectral characterization of incident stochastic XFEL pulses with high resolution is a key requirement. Here we present a methodology that combines high-acceptance angle-resolved photoelectron time-of-flight spectroscopy and ghost imaging to enhance the quality of spectral characterization of x-ray free-electron laser pulses. Implementation of this noninvasive high-resolution x-ray diagnostic can greatly benefit the ultrafast x-ray spectroscopy community by functioning as a transparent beamsplitter for applications such as transient absorption spectroscopy in averaging mode as well as covariance-based x-ray nonlinear spectroscopies in single-shot mode where the shot-to-shot fluctuations inherent to a self-amplified spontaneous emission (SASE) XFEL pulse are a powerful asset.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Pump-induced motion of an interface between competing orders

In this work, we study the motion of an interface separating two regions with different electronic orders following a short-duration pump that drives the system out of equilibrium. Using a generalized Ginzburg-Landau approach and assuming that the main effect of the nonequilibrium drive is to transiently heat the system we address the question of the direction of interface motion—in other words, which ordered region expands and which contracts after the pump. Our analysis includes the effects of differences in free-energy landscape and in order parameter dynamics and identifies circumstances in which the drive may act to increase the volume associated with the subdominant order, for example when the subdominant order has a second-order free-energy landscape while the dominant order has a first-order one.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Dynamical Scaling Reveals Topological Defects and Anomalous Evolution of a Photoinduced Phase Transition

Nonequilibrium states of quantum materials can exhibit exotic properties and enable unprecedented functionality and applications. These transient states are inherently inhomogeneous, characterized by the formation of topologically protected structures, requiring nanometer spatial resolution on femtosecond timescales to resolve their evolution. Using ultrafast total x-ray scattering at a free electron laser and a sophisticated scaling analysis, we gain unique access to the dynamics on the relevant mesoscopic length scales. Our results provide direct evidence that ultrafast excitation of LaTe 3 leads to formation of topological vortex strings of the charge density wave. These dislocations of the charge density wave exhibit anomalous, subdiffusive dynamics, slowing the equilibration process, providing rare insight into the nonequilibrium mesoscopic response in a quantum material. Our findings establish a general framework to investigate properties of topological defects, which are expected to be ubiquitous in nonequilibrium phase transitions and may arrest equilibration and enhance competing orders.

Orenstein, Gal [SLAC National Accelerator Laborato↗
DOE OSTI2023

Optical anisotropy of CsPbBr3 perovskite nanoplatelets

Abstract The two-dimensional CsPbBr 3 nanoplatelets have a quantum well electronic structure with a band gap tunable with sample thicknesses in discreet steps based upon the number of monolayers. The polarized optical properties of CsPbBr 3 nanoplatelets are studied using fluorescence anisotropy and polarized transient absorption spectroscopies. Polarized spectroscopy shows that they have absorption and emission transitions which are strongly plane-polarized. In particular, photoluminescence excitation and transient absorption measurements reveal a band-edge polarization approaching 0.1, the limit of isotropic two-dimensional ensembles. The degree of anisotropy is found to depend on the thickness of the nanoplatelets: multiple measurements show a progressive decrease in optical anisotropy from 2 to 5 monolayer thick nanoplatelets. In turn, larger cuboidal CsPbBr 3 nanocrystals, are found to have consistently positive anisotropy which may be attributed to symmetry breaking from ideal perovskite cubes. Optical measurements of anisotropy are described with respect to the theoretical framework developed to describe exciton fine structure in these materials. The observed planar absorption and emission are close to predicted values at thinner nanoplatelet sizes and follow the predicted trend in anisotropy with thickness, but with larger anisotropy than theoretical predictions. Dominant planar emission, albeit confined to the thinnest nanoplatelets, is a valuable attribute for enhanced efficiency of light-emitting devices.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Dynamical Scaling Reveals Topological Defects and Anomalous Evolution of a Photoinduced Phase Transition

Nonequilibrium states of quantum materials can exhibit exotic properties and enable unprecedented functionality and applications. These transient states are inherently inhomogeneous, characterized by the formation of topologically protected structures, requiring nanometer spatial resolution on femtosecond timescales to resolve their evolution. Using ultrafast total x-ray scattering at a free electron laser and a sophisticated scaling analysis, we gain unique access to the dynamics on the relevant mesoscopic lengthscales. Our results provide direct evidence that ultrafast excitation of LaTe$_3$ leads to formation of topological vortex strings of the charge density wave. These dislocations of the charge density wave exhibit anomalous, subdiffusive dynamics, slowing the equilibration process, providing rare insight into the nonequilibrium mesoscopic response in a quantum material. Our findings establish a general framework to investigate properties of topological defects, which are expected to be ubiquitous in nonequilibrium phase transitions and may arrest equilibration and enhance competing orders.

FOS: Physical sciences↗
NASA NTRS1991

Transient particle acceleration in strongly magnetized neutron stars

Although several reasonable physical processes have been proposed to account for the initial energy release in transient events on strongly magnetized neutron stars, and although the manifestation of this activity as a burst of X- or gamma-radiation evidently results from the Compton upscattering of soft photons by relativistic electrons, a self-consistent picture for the particle acceleration itself is lacking. Here, a detailed model is developed in which sheared Alfven waves generated by the energized stellar crust (e.g., due to a starquake) accelerate the changes to large Lorentz factors. For canonical stellar parameters and a burst energy of about 10 to the 37th ergs, the maximum attainable Lorentz factor is gamma(max) 50m, where m (of about 2-3/cm) characterizes the shear of the magnetic perturbation. This value of gamma(max) is consistent with the particle energy required to produce the most energetic gamma-rays (of about 10-100 MeV) observed in gamma-ray bursts.

Melia, Fulvio↗
DOE OSTI2021

Probing Microstructure-induced Swelling & Thermal Property Changes in Ion-Irradiated Oxide Fuels using Laser-generated Surface Acoustic Waves

Radiation of fuel rods with neutrons during a fission reaction in a nuclear reactor is known to affect the material microstructure of the fuel as a result of fission fragment damage, and lead to the formation of atomic-level defects such as voids, dislocation loops, and lattice swelling from fission-gas release. A consequence of the radiation-induced damage in nuclear fuels is the drastic alteration of material properties, in particular, the reduction of the thermal conductivity – a key parameter that governs the transport of thermal energy released from fissile fuel atoms to the surrounding coolant. Swelling can induce high stresses and ultimate failure of the cladding. A fundamental understanding of the role of radiation-induced damage on the thermal transport and mechanical properties of nuclear fuels is therefore critical for efficient, reliable and safe operation of a nuclear power plant. As opposed to conventional post-irradiation examination techniques that are often time-consuming and require significant sample preparation, laser-based characterization methods have emerged as promising non-contact, non-destructive tools to measure the evolution of microstructure-induced material property changes. Moreover, laser methods offer the promise of in-situ characterization while the material is being irradiated. This project aims to develop an improved understanding of the impact of radiation-induced changes to material microstructure on the thermal and elastic properties of nuclear materials. A laser ultrasonic technique, known as the transient grating (TG) spectroscopy method, is used to simultaneously measure thermal diffusivity and elastic properties in unirradiated and ion-irradiated oxide nuclear fuel samples. The results will complement on-going investigations on electron- and phonon-mediated thermal transport in nuclear materials and will provide foundational work for incorporating the influence of defects in fuel performance codes.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2021

Ir(III)-Naphthoquinone complex as a platform for photocatalytic activity

Inspired by the primary events that take place in Photosystem II (PSII), we designed and synthesized a heteroleptic Ir(III) complex featuring an attached naphthoquinone (NQ) as an electron transfer (ET) auxiliary reminiscent of the plastoquinone electron acceptor in PSII. In this design, NQ is covalently attached to the 2,2'-bipyridyl (bpy) ligand of [Ir(dF(CF 3 )ppy) 2 (bpy)][PF 6 ], (dF(CF 3 )ppy = 2-(2,4-difluorophenyl)-5-(trifluoromethyl)pyridine). Following excitation of the photocatalyst ([Ir(dF(CF 3 )ppy) 2 (bpy-NQ)][PF 6 ]), reduced NQ (NQ •– ) was observed in transient absorption spectroscopy. Here, this novel catalyst has potential applications in oxidative and reductive photocatalytic processes.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2024

Advances in in situ/operando techniques for catalysis research: enhancing insights and discoveries

Abstract Catalysis research has witnessed remarkable progress with the advent of in situ and operando techniques. These methods enable the study of catalysts under actual operating conditions, providing unprecedented insights into catalytic mechanisms and dynamic catalyst behavior. This review discusses key in situ techniques and their applications in catalysis research. Advances in in situ electron microscopy allow direct visualization of catalysts at the atomic scale under reaction conditions. In situ spectroscopy techniques like X-ray absorption spectroscopy and nuclear magnetic resonance spectroscopy can track chemical states and reveal transient intermediates. Synchrotron-based techniques offer enhanced capabilities for in situ studies. The integration of in situ methods with machine learning and computational modeling provides a powerful approach to accelerate catalyst optimization. However, challenges remain regarding radiation damage, instrumentation limitations, and data interpretation. Overall, continued development of multi-modal in situ techniques is pivotal for addressing emerging challenges and opportunities in catalysis research and technology.

Chen, Linfeng↗
DOE OSTI2020

Thermally induced cracking on the massive concrete structure of the NSLS II synchrotron and its engineering remediation

Synchrotron accelerator facilities such as the NSLS II require extreme stability, both transient (short-term) and quasi-static (long-term) to achieve the desired resolution performance. Consequently, even μm-level movements, particularly differential movements between locations in the concrete structure supporting the accelerator electron beam lattice (storage ring) or high sensitivity experiments (experimental floor) will lead to serious degradation of its performance. Differential settlement in the overall structure or structural movement exceeding anticipated levels will inevitably degrade the performance and will require intervention. Presented in this paper are the design philosophy of the NSLS II ring structure favoring a monolithic ring, the observed cracking behavior of the young NSLS II concrete following casting and in combination with extreme ambient temperature fluctuation, the results of a non-linear, high-fidelity numerical analysis used to emulate the observed cracking and establish the driving mechanism, the numerical analysis-based identification of the crack-arresting solution and finally the implementation of the remediation solution and the long-term performance of the adopted engineering solution. The multi-stage process revealed that computational methods such as non-linear finite element methods have the potential of providing engineering guidance even when complex structures and in combination with non-linear materials, such as steel reinforcement and concrete are involved.

42 ENGINEERING↗