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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 1,027 records · Page 57
All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

High sensitivity pump–probe measurements of magnetic, thermal, and acoustic phenomena with a spectrally tunable oscillator

We describe an optical pump/probe system for sensitive measurements of time-resolved optical measurements of material dynamics. The instrument design is optimized for time-resolved magneto-optic Kerr effect (TR-MOKE) measurements of dynamics in magnetic materials. The system also allows for time-domain thermoreflectance (TDTR) measurements of thermal transport properties and picosecond acoustic measurements of film thickness and/or elastic constants. The system has several advantages over the conventional designs for TRMOKE and/or TDTR systems. Measurements of pump-induced changes to the probe beam intensity are shot-noise limited. The system’s design allows for MOKE and/or thermoreflectance measurements of both sides of a sample. Pumping and probing the sample on opposite sides allows nanoscale flash diffusivity measurements of transport properties. The wavelengths of the pump and probe beams are straightforward to tune between 350–525 nm and 690–1050 nm. A tunable wavelength allows for optical resonances in a wide array of materials to be excited and/or probed. Finally, the setup is calibrated to allow for the real and imaginary components of Kerr signals to be separately quantified.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

A multi-wavelength streaked optical pyrometer for dynamic shock compression measurements above 2500 K

This work presents a concept and implementation of a calibrated streaked spectral pyrometer (SSP) temperature diagnostic used in dynamically driven shock experiments on a two-stage gas gun. This system relies upon measuring the total system response using a tunable monochromator, a NIST-traceable calibrated power meter, and a SSP. The diagnostic performance is validated against previously measured temperatures of shock driven z-cut quartz at 99 GPa and 93 GPa. The results are found to agree with the literature to within 5% and are discussed in this manuscript. The experimental setup utilizes measurements from multiple SSP systems per sample, providing several independent measurements and substantially increasing confidence in the extrapolated shock driven sample temperature.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

An in situ shearing x-ray measurement system for exploring structures and dynamics at the solid–liquid interface

Revealing interfacial structure and dynamics has been one of the essential thematic topics in material science and condensed matter physics. Synchrotron-based x-ray scattering techniques can deliver unique and insightful probing of interfacial structures and dynamics, in particular, in reflection geometries with higher surface and interfacial sensitivity than transmission geometries. We demonstrate the design and implementation of an in situ shearing x-ray measurement system, equipped with both inline parallel-plate and cone-and-plate shearing setups and operated at the advanced photon source at Argonne National Laboratory, to investigate the structures and dynamics of end-tethered polymers at the solid-liquid interface. With a precise lifting motor, a micrometer-scale gap can be produced by aligning two surfaces of a rotating upper shaft and a lower sample substrate. A torsional shear flow forms in the gap and applies tangential shear forces on the sample surface. The technical combination with nanoscale rheology and the utilization of in situ x-ray scattering allow us to gain fundamental insights into the complex dynamics in soft interfaces under shearing. In this work, we demonstrate the technical scope and experimental capability of the in situ shearing x-ray system through the measurements of charged polymers at both flat and curved interfaces upon shearing. Furthermore, through the in situ shearing x-ray scattering experiments integrated with theoretical simulations, we aim to develop a detailed understanding of the short-range molecular structure and mesoscale ionic aggregate morphology, as well as ion transport and dynamics in soft interfaces, thereby providing fundamental insight into a long-standing challenge in ionic polymer brushes with a significant technological impact.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Design and implementation of a J -coupled spectrometer for multidimensional structure and relaxation detection at low magnetic fields

In recent years, it has been realized that low and ultra-low field (mT-nT magnetic field range) nuclear magnetic resonance (NMR) spectroscopy can be used for molecular structural analysis. However, spectra are often hindered by lengthy acquisition times or require large sample volumes and high concentrations. Here, we report a low field (50 µT) instrument that employs a linear actuator to shuttle samples between a 1 T prepolarization field and a solenoid detector in a laboratory setting. The current experimental setup is benchmarked using water and 13 C-methanol with a single scan detection limit of 2x10 20 spins (3 μL, 55 M H 2 O) and detection of 2.9x10 19 (200 μL, 617 mM 13 C-methanol) spins with signal averaging. The system has a dynamic range of >3 orders of magnitude. Investigations of room-temperature relaxation dynamics of 13Cmethanol show that sample dilution can be used in lieu of sample heating to acquire spectra with linewidths comparable to high-temperature spectra. These results indicate that the T 1 and T 2 mechanisms are governed by both the proton exchange rate and the dissolved oxygen in the sample. Finally, a 2D correlation spectroscopy (COSY) experiment is reported, performed in the strong coupling regime that resolves the multiple resonances associated with the heteronuclear Jcoupling. The spectrum was collected using 10 times less sample and in less than half the time from previous reports in the strong coupling limit.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Excited-state electronic structure of molecules using many-body Green’s functions: Quasiparticles and electron–hole excitations with VOTCA-XTP

Here, we present the open-source VOTCA-XTP software for the calculation of the excited-state electronic structure of molecules using many-body Green’s function theory in the GW approximation with the Bethe–Salpeter equation (BSE). This work provides a summary of the underlying theory and discusses the details of its implementation based on Gaussian orbitals, including resolution-of-identity techniques and different approaches to the frequency integration of the self-energy or acceleration by offloading compute-intensive matrix operations using graphics processing units in a hybrid OpenMP/Cuda scheme. A distinctive feature of VOTCA–XTP is the capability to couple the calculation of electronic excitations to a classical polarizable environment on an atomistic level in a coupled quantum- and molecular-mechanics (QM/MM) scheme, where a complex morphology can be imported from Molecular Dynamics simulations. The capabilities and limitations of the GW–BSE implementation are illustrated with two examples. First, we study the dependence of optically active electron–hole excitations in a series of diketopyrrolopyrrole-based oligomers on molecular-architecture modifications and the number of repeat units. Second, we use the GW–BSE/MM setup to investigate the effect of polarization on localized and intermolecular charge-transfer excited states in morphologies of low-donor content rubrene–fullerene mixtures. These showcases demonstrate that our implementation currently allows us to treat systems with up to 2500 basis functions on regular shared-memory workstations, providing accurate descriptions of quasiparticle and coupled electron–hole excited states of various characters on an equal footing.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Real-time interfacial electron dynamics revealed through temporal correlations in x-ray photoelectron spectroscopy

We present a novel technique to monitor dynamics in interfacial systems through temporal correlations in x-ray photoelectron spectroscopy (XPS) signals. To date, the vast majority of time-resolved x-ray spectroscopy techniques rely on pump–probe schemes, in which the sample is excited out of equilibrium by a pump pulse, and the subsequent dynamics are monitored by probe pulses arriving at a series of well-defined delays relative to the excitation. By definition, this approach is restricted to processes that can either directly or indirectly be initiated by light. It cannot access spontaneous dynamics or the microscopic fluctuations of ensembles in chemical or thermal equilibrium. Enabling this capability requires measurements to be performed in real (laboratory) time with high temporal resolution and, ultimately, without the need for a well-defined trigger event. The time-correlation XPS technique presented here is a first step toward this goal. The correlation-based technique is implemented by extending an existing optical-laser pump/multiple x-ray probe setup by the capability to record the kinetic energy and absolute time of arrival of every detected photoelectron. The method is benchmarked by monitoring energy-dependent, periodic signal modulations in a prototypical time-resolved XPS experiment on photoinduced surface-photovoltage dynamics in silicon, using both conventional pump–probe data acquisition, and the new technique based on laboratory time. The two measurements lead to the same result. The findings provide a critical milestone toward the overarching goal of studying equilibrium dynamics at surfaces and interfaces through time correlation-based XPS measurements.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2023

Relativistic ultrafast electron diffraction at high repetition rates

The ability to resolve the dynamics of matter on its native temporal and spatial scales constitutes a key challenge and convergent theme across chemistry, biology, and materials science. The last couple of decades have witnessed ultrafast electron diffraction (UED) emerge as one of the forefront techniques with the sensitivity to resolve atomic motions. Increasingly sophisticated UED instruments are being developed that are aimed at increasing the beam brightness in order to observe structural signatures, but so far they have been limited to low average current beams. Here, we present the technical design and capabilities of the HiRES (High Repetition-rate Electron Scattering) instrument, which blends relativistic electrons and high repetition rates to achieve orders of magnitude improvement in average beam current compared to the existing state-of-the-art instruments. The setup utilizes a novel electron source to deliver femtosecond duration electron pulses at up to MHz repetition rates for UED experiments. Instrument response function of sub-500 fs is demonstrated with < 100 fs time resolution targeted in future. We provide example cases of diffraction measurements on solid-state and gas-phase samples, including both micro- and nanodiffraction (featuring 100 nm beam size) modes, which showcase the potential of the instrument for novel UED experiments.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2020

Ultrashort XUV pulse absorption spectroscopy of partially oxidized cobalt nanoparticles

High-order harmonic generation (HHG) based transient extreme ultraviolet (XUV) absorption spectroscopy is an emerging technique to trace photoinduced charge carrier dynamics in condensed phase materials with femtosecond and even attosecond temporal resolution and elemental specificity. However, its application to nanoparticulate samples that are relevant, for example, for novel photocatalytic light harvesting concepts, has been limited. This is in part due to the challenge to produce residual-free samples on ultrathin, XUV-transparent substrates as well as a widespread understanding that sparsely distributed nanoparticles do not provide sufficient contrast for XUV absorption measurements. Here, we present static XUV absorption spectra of partially oxidized Co nanowire-structures with diameters of approximately 4.5 nm and lengths between 10 and 40 nm, recorded with an ultrashort pulse HHG light source. Nanoparticles are synthesized by the agglomeration of Co atoms inside superfluid helium droplets, followed by surface deposition and oxidation in ambient air. The method is uniquely suited for residual-free synthesis of transition metal nanowires and their deposition on ultrathin substrates. Analysis by high-resolution transmission electron microscopy reveals the formation of CoO nanowires with regions of unoxidized Co in their interior. The nanoparticle samples are investigated in an HHG-driven ultrafast XUV absorption setup. Despite the low surface coverage of only 23%, the recorded spectrum exhibits a distinct absorption feature at the Co M 2,3 (2p) edge near 60 eV with a peak height of about 40 mOD. Finally, the results support the feasibility of table-top ultrafast transient XUV absorption studies of photoinduced dynamics in transition metal oxide nanoparticles with sub-monolayer surface coverage.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

A compact, high resolution energy, and emittance diagnostic for electron beams using active plasma lenses

High-resolution (sub-%), single-shot energy distribution, and emittance measurements of GeV-class electron beams generated by laser plasma accelerators (LPAs) have been enabled through the use of an active plasma lens combined with relatively short dipole magnets. This setup, with only 60 cm between the LPA source and the final diagnostic screen, was facilitated through the use of a replenishable ∼20–40 nm thick liquid crystal plasma mirror to separate remnant laser radiation from the electron beam without emittance degradation. As LPAs capable of generating GeV-class electron beams at cm-scale distances become increasingly ubiquitous, there is a need to supplement these compact accelerators with equally compact diagnostics.

Barber, S. K. (ORCID:0000000172518755)↗
DOE OSTI2020

Measurement and modeling of the radio frequency sheath impedance in a large magnetized plasma

The DC and RF properties of radio frequency (RF) driven sheaths were studied in the Large Plasma Device (LAPD) at the University of California, Los Angeles. The experiments diagnosed RF sheaths on field lines connected to a grounded plate at one end and an ion cyclotron range of frequencies (ICRF) antenna at the other end. The experimental setup permitted measurement of the RF sheath impedance at the plate as a function of DC sheath voltage, with the latter controlled by varying the RF current applied to the antenna. Here, the DC current-voltage characteristics of these sheaths and the RF sheath impedance measurements were compared with modeling. Hot electrons, present in the LAPD plasma, were inferred to contribute significantly to both the DC and RF currents and hence the RF impedance. It was postulated that at very low power hot electrons could not access the region of the plasma subject to RF waves, resulting in an increased RF impedance. Within some experimental limitations and significant assumptions, an RF sheath impedance model was verified by the experimental data.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Experimental demonstration of externally driven millimeter-wave particle accelerator structure

We report the experimental demonstration of a mm-wave electron accelerating structure powered by a high-power rf source. We demonstrate reliable coupling of an unprecedented rf power—up to 575kW into the mm-wave accelerator structure using a quasi-optical setup. This standing wave accelerating structure consists of a single-cell copper cavity and a Gaussian to TM 01 mode converter. The accelerator structure is powered by 110 GHz, 10-ns long rf pulses. These pulses are chopped from 3 microsecond pulses from a gyrotron oscillator using a laser-driven silicon switch. We show an unprecedented high gradient up to 230MV/m that corresponds to a peak surface electric field of more than 520 MV/m. We have achieved these results after conditioning the cavity with more than 100,000 pulses. We also report preliminary measurements of rf breakdown rates, which are important for understanding rf breakdown physics in the millimeter-wave regime. Furthermore, these results open up many frontiers for applications not only limited to the next generation particle accelerators but also x-ray generation, probing material dynamics, and nonlinear light-matter interactions at mm-wave frequency.

43 PARTICLE ACCELERATORS↗
DOE OSTI2020

Piezoresponse amplitude and phase quantified for electromechanical characterization

Piezoresponse force microscopy (PFM) is a powerful characterization technique to readily image and manipulate the ferroelectric domains. PFM gives an insight into the strength of local piezoelectric coupling and polarization direction through PFM amplitude and phase, respectively. Converting measured arbitrary units into units of effective piezoelectric constant remains a challenge, and insufficient methods are often used. While most quantification efforts have been spent on quantifying the PFM amplitude signal, little attention has been given to the PFM phase, which is often arbitrarily adjusted to fit expectations. This is problematic when investigating materials with unknown or negative sign of the probed effective electrostrictive coefficient or strong frequency dispersion of electromechanical responses, because assumptions about the PFM phase cannot be reliably made. The PFM phase can, however, provide important information on the polarization orientation and the sign of the effective electrostrictive coefficient probed by PFM. Most notably, the orientation of the PFM hysteresis loop is determined by the PFM phase. Moreover, when presenting PFM data as a combined signal, the resulting response can be artificially lowered or asymmetric if the phase data have not been correctly processed. Here, we explain the PFM amplitude quantification process and demonstrate a path to identify the phase offset required to extract correct meaning from the PFM phase data. We explore different sources of phase offsets including the experimental setup, instrumental contributions, and data analysis. We discuss the physical working principles of PFM and develop a strategy to extract physical meaning from the PFM amplitude and phase.

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

Mechanical detwinning device for anisotropic resistivity measurements in samples requiring dismounting for particle irradiation

Uniaxial stress is used to detwin samples of orthorhombic iron based superconductors to study their intrinsic electronic anisotropy. Here we describe the development of a new detwinning setup enabling variable-load stress-detwinning with easy sample mounting/dismounting without the need to re-solder the contacts. It enables the systematic study of the anisotropy evolution as a function of an external parameter when the sample is modified between the measurements. In our case, the external parameter is the dose of 2.5 MeV electron irradiation at low temperature. We illustrate the approach by studying resistivity anisotropy in single crystals of Ba 1-x K x Fe 2 As 2 at x =0.25 where the much discussed unusual re-entrance of tetragonal C 4 phase, C 4 → C 2 → C 4 , is observed on cooling. With the described technique we found a significant anisotropy increase in C 2 phase after electron irradiation with dose of 2.35 C/cm 2 .

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Measurement of gas-concentration-driven permeation for the examination of permeability, solubility, and diffusivity in varying materials

This manuscript describes the development and operation of an apparatus for the measurement of steady-state and transient gas permeation through different types of solid materials with varying geometries. It is capable of operation from 293 K to 673 K and could theoretically be used with any non-corrosive gas or a mix of gases, although only hydrogen isotopes are used in the current study. A quadrupole mass spectrometer is used to measure permeation fluxes as low as 1011 molecules/s. This unique test setup allows for the simultaneous measurement of diffusivity, solubility, and permeability. Furthermore, varying the pressure in the fore-sample volume allows for tests of Sievert’s law and can give information on surface effects.

Young, Katherine T. (ORCID:0000000285845576)↗
DOE OSTI2020

Determination of acoustic nonlinearity parameters using thermal modulation of ultrasonic waves

This study presents a test method and its theoretical framework to determine the acoustic nonlinearity parameters (α, β, δ) of material using thermal modulation of ultrasonic waves. Temperature change-induced thermal strain excites the nonlinear response of the material and modulates the ultrasonic wave propagating in it. Experimental results showed a strong correlation between the relative wave velocity change and the temperature change. With a quadratic polynomial model, the acoustic nonlinearity parameters were obtained from the polynomial coefficients by curve fitting the experimental data. Their effects on thermal-induced velocity change were discussed. The parameters α, β, and δ govern the hysteretic gap, average slope, and curvature of the correlation curve, respectively. The proposed theory was validated on aluminum, steel, intact and damaged concrete samples. The obtained nonlinear parameters show reasonable agreement with values reported in the literature. Compared to other nonlinear acoustic methods using vibration or acoustic excitation, the thermal modulation method generates more uniform, slow changing, and larger strain field in the test sample. Employing the thermal effect as the driving force for nonlinearity instead of an undesired influencing factor, this method can measure the absolute values of α, β, and δ with good accuracy using a simple ultrasonic test setup.

Physics↗
DOE OSTI2020

Materials loss measurements using superconducting microwave resonators

The performance of superconducting circuits for quantum computing is limited by materials losses. In particular, coherence times are typically bounded by two-level system (TLS) losses at single photon powers and millikelvin temperatures. The identification of low loss fabrication techniques, materials, and thin film dielectrics is critical to achieving scalable architectures for superconducting quantum computing. Superconducting microwave resonators provide a convenient qubit proxy for assessing performance and studying TLS loss and other mechanisms relevant to superconducting circuits such as non-equilibrium quasiparticles and magnetic flux vortices. In this review article, we provide an overview of considerations for designing accurate resonator experiments to characterize loss, including applicable types of losses, cryogenic setup, device design, and methods for extracting material and interface losses, summarizing techniques that have been evolving for over two decades. Results from measurements of a wide variety of materials and processes are also summarized. Finally, we present recommendations for the reporting of loss data from superconducting microwave resonators to facilitate materials comparisons across the field.

47 OTHER INSTRUMENTATION↗
DOE OSTI2020

Looking at the bigger picture: Identifying the photoproducts of pyruvic acid at 193 nm

Here, photodissociation of pyruvic acid (PA) was studied in the gas-phase at 193 nm using two complementary techniques. The time-sliced velocity map imaging arrangement was used to determine kinetic energy release distributions of fragments and estimate dissociation timescales. The multiplexed photoionization mass spectrometer setup was used to identify and quantify photoproducts, including isomers and free radicals, by their mass-to-charge ratios, photoionization spectra, and kinetic time profiles. Using these two techniques, it is possible to observe the major dissociation products of PA photodissociation: CO 2 , CO, H, OH, HCO, CH 2 CO, CH 3 CO, and CH 3 . Acetaldehyde and vinyl alcohol are minor primary photoproducts at 193 nm, but products that are known to arise from their unimolecular dissociation, such as HCO, H 2 CO, and CH 4 , are identified and quantified. A multivariate analysis that takes into account the yields of the observed products and assumes a set of feasible primary dissociation reactions provides a reasonable description of the photoinitiated chemistry of PA despite the necessary simplifications caused by the complexity of the dissociation. These experiments offer the first comprehensive description of the dissociation pathways of PA initiated on the S 3 excited state. Most of the observed products and yields are rationalized on the basis of three reaction mechanisms: (i) decarboxylation terminating in CO 2 + other primary products (~50%); (ii) Norrish type I dissociation typical of carbonyls (~30%); and (iii) O—H and C—H bond fission reactions generating the H atom (~10%). The analysis shows that most of the dissociation reactions create more than two products. This observation is not surprising considering the high excitation energy (~51 800 cm –1 ) and fairly low energy required for dissociation of PA. We find that two-body fragmentation processes yielding CO 2 are minor, and the expected, unstable primary co-fragment, methylhydroxycarbene, is not observed because it probably undergoes fast secondary dissociation and/or isomerization. Norrish type I dissociation pathways generate OH and only small yields of CH 3 CO and HOCO, which have low dissociation energies and further decompose via three-body fragmentation processes. Experiments with d 1 -PA (CH 3 COCOOD) support the interpretations. The dissociation on S 3 is fast, as indicated by the products’ recoil angular anisotropy, but the roles of internal conversion and intersystem crossing to lower states are yet to be determined.

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

Target normal sheath acceleration with a large laser focal diameter

In this work, the dependence of the laser-driven ion acceleration from thin titanium foils in the Target Normal Sheath Acceleration (TNSA) regime on target and laser parameters is explored using two dimensional particle-in-cell simulations. The oblique incidence (θ L = 45°) and large focal spot size (w 0 = 40μm) are chosen to take an advantage of quasi one-dimensional geometry of sheath fields and effective electron heating. This interaction setup also reveals low and achromatic angular divergence of a proton beam. It is shown that the hot electron temperature deviates from the ponderomotive scaling for short laser pulses and small pre-plasmas. This deviation is mainly due to the laser sweeping, as the short duration laser pulse each moment in time effectively heats only a fraction of a focal spot on the foil. This instantaneous partial heating results in an electron temperature deviation from the ponderomotive scaling and, thus, lower maximum proton energies than it could have been expected from the TNSA theory.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗