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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 1,657 records · Page 92
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Time-resolved momentum imaging of UV photodynamics in structural isomers of iodopropane probed by site-selective XUV ionization

The photodynamics of 1- and 2-iodopropane (1 and 2-IP) were studied in a time-resolved scheme incorporating ultraviolet (UV) excitation and extreme ultraviolet (XUV) probing, which initiates photoionization selectively from the I 4d core orbital. UV absorption in the A-band of both isomers leads to prompt C–I bond fission, with significant disposal of internal energy into the propyl radical product. Site-selective ionization enables a range of charge transfer (CT) processes between the nascent highly charged iodine ions and neutral propyl radicals, dependent on the interfragment distance at the instant of ionization. Subtle differences in the dynamics of these CT processes between the two isomers are observed. In 1-IP, the kinetic energies of iodine ions produced by UV photodissociation and subsequent XUV multiple ionization increased notably over the first few hundred femtoseconds, which could be understood in terms of differing gradients along the photodissociation coordinates of the neutral and polycationic states involved in the pump and probe steps, respectively. Led by a recent report of HI elimination in UV photoexcited 2-IP [Todt et al., Phys. Chem. Chem. Phys., 22(46), 27338 (2020)], we also model the most likely signatures of this process in the present experiment, and can identify signal in the 2-IP data (that is absent or significantly weaker in the data from the unbranched 1-IP isomer) that is consistent with such a process occurring on ultrafast timescales.

Allum, Felix [Deutsches Elektronen-Synchrotron (DE↗
DOE OSTI2025

Probing the proton exchange kinetics of BaZr 0.1 Ce 0.7 Y 0.1 Yb 0.1 O 3− δ ceramic electrolyte by operando diffuse reflectance infrared Fourier transform spectroscopy

Proton exchange kinetics plays an important role in governing the performance of intermediate-temperature protonic ceramic electrolysis cells (PCECs) for hydrogen production. Our understanding of the nature of the surface hydration reaction at the single-cell level, however, remains very limited, hampering further efficiency improvements. Here, in this study, we developed a custom operando diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) platform that operates under high temperature and steam conditions with applied bias. Quantitative investigations of surface H 2 O/D 2 O isotope exchange in a BaZr 0.1 Ce 0.7 Y 0.1 Yb 0.1 O 3−δ (BZCYYb1711) protonic electrolyte-based single cell were conducted under different applied voltages using this DRIFTS platform, to gain molecular-level insight into hydration kinetics. The findings show that the application of an external voltage significantly enhances the surface proton exchange rate, decreasing the apparent activation energy from 29.1 kJ mol −1 at open-circuit voltage (OCV) to 6.8 kJ mol −1 at 1.3 V. In addition, distinct voltage-induced spectral shifts in O–D vibrations point to dynamic changes in surface hydration. These findings demonstrate a sensitive spectroscopic platform for probing interfacial proton processes and reveal strong electrochemical control over surface proton kinetics, offering new opportunities for probing electrolyte hydration behavior in PCECs.

36 - MATERIALS SCIENCE↗
DOE OSTI2025

Probing circular polarization and magnetic field structure in active galactic nuclei

The composition and magnetic field morphology of relativistic jets can be studied using circular polarization (CP) measurement. Recent three-dimensional relativistic magnetohydrodynamic (3D RMHD) simulations coupled with radiative transfer (RT) calculations make strong predictions about the level (and morphology) of the jet’s CP emission. These simulations show that the sign of CP and the electric vector position angle (EVPA) are both sensitive to the jet’s magnetic field morphology within the radio core. We probe this theory by exploring whether the jet’s radio core EVPA orientation is consistent with the observed sign of the core CP in deep full-track polarimetric observations. Based on a selection of sources from earlier MOJAVE observations, we aim to probe the nature of linear polarization (LP) and CP in the innermost regions of jets from a small sample of nine blazars. This sample includes sources that have exhibited: (i) positive CP; (ii) negative CP; or (iii) positive and negative CP simultaneously in the radio core region. By coupling deep polarimetric observations of a carefully selected sample of blazars with state-of-the-art RMHD and RT calculations, we hope to gain a deeper understanding of the physics of blazar jets.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2013

Atom probe tomography evaporation behavior of C-axis GaN nanowires: Crystallographic, stoichiometric, and detection efficiency aspects

The field evaporation behavior of c-axis GaN nanowires was explored in two different laser-pulsed atom probe tomography (APT) instruments. Transmission electron microscopy imaging before and after atom probe tomography analysis was used to assist in reconstructing the data and assess the observed evaporation behavior. It was found that the ionic species exhibited preferential locations for evaporation related to the underlying crystal structure of the GaN and that the species which evaporated from these locations was dependent on the pulsed laser energy. Additionally, the overall stoichiometry measured by APT was significantly correlated with the energy of the laser pulses. At the lowest laser energies, the apparent composition was nitrogen-rich, while higher laser energies resulted in measurements of predominantly gallium compositions. The percent of ions detected (detection efficiency) for these specimens was found to be considerably below that shown for other materials, even for laser energies which produced the expected Ga:N ratio. The apparent stoichiometry variation and low detection efficiency appear to be a result of evaporation of Ga ions between laser pulses at the lowest laser energies and evaporation of neutral N{sub 2} species at higher laser energies. All of these behaviors are tied to the formation of nitrogen-nitrogen bonds on the tip surface, which occurred under all analysis conditions. Similar field evaporation behaviors are therefore expected for other materials where the anionic species readily form a strong diatomic bond.

36 MATERIALS SCIENCE↗
DOE OSTI2014

Adsorption of probe molecules in pillared interlayered clays: Experiment and computer simulation

In this paper we investigate the adsorption of various probe molecules in order to characterize the porous structure of a series of pillared interlayered clays (PILC). To that aim, volumetric and microcalorimetric adsorption experiments were performed on various Zr PILC samples using nitrogen, toluene, and mesitylene as probe molecules. For one of the samples, neutron scattering experiments were also performed using toluene as adsorbate. Various structural models are proposed and tested by means of a comprehensive computer simulation study, using both geometric and percolation analysis in combination with Grand Canonical Monte Carlo simulations in order to model the volumetric and microcalorimetric isotherms. On the basis of this analysis, we propose a series of structural models that aim at accounting for the adsorption experimental behavior, and make possible a microscopic interpretation of the role played by the different interactions and steric effects in the adsorption processes in these rather complex disordered microporous systems.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Investigation of electronically excited indole relaxation dynamics via photoionization and fragmentation pump-probe spectroscopy

The studies herein investigate the involvement of the low-lying {sup 1}L{sub a} and {sup 1}L{sub b} states with {sup 1}ππ{sup *} character and the {sup 1}πσ{sup *} state in the deactivation process of indole following photoexcitation at 201 nm. Three gas-phase, pump-probe spectroscopic techniques are employed: (1) Time-resolved photoelectron spectroscopy (TR-PES), (2) hydrogen atom (H-atom) time-resolved kinetic energy release (TR-KER), and (3) time-resolved ion yield (TR-IY). Each technique provides complementary information specific to the photophysical processes in the indole molecule. In conjunction, a thorough examination of the electronically excited states in the relaxation process, with particular focus on the involvement of the {sup 1}πσ{sup *} state, is afforded. Through an extensive analysis of the TR-PES data presented here, it is deduced that the initial excitation of the {sup 1}B{sub b} state decays to the {sup 1}L{sub a} state on a timescale beyond the resolution of the current experimental setup. Relaxation proceeds on the {sup 1}L{sub a} state with an ultrafast decay constant (<100 femtoseconds (fs)) to the lower-lying {sup 1}L{sub b} state, which is found to possess a relatively long lifetime of 23 ± 5 picoseconds (ps) before regressing to the ground state. These studies also manifest an additional component with a relaxation time of 405 ± 76 fs, which is correlated with activity along the {sup 1}πσ{sup *} state. TR-KER and TR-IY experiments, both specifically probing {sup 1}πσ{sup *} dynamics, exhibit similar decay constants, further validating these observations.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Probing channel temperature profiles in Al{sub x}Ga{sub 1−x}N/GaN high electron mobility transistors on 200 mm diameter Si(111) by optical spectroscopy

Using micro-Raman and photoluminescence (PL) techniques, the channel temperature profile is probed in Al{sub x}Ga{sub 1-x}N/GaN high electron mobility transistors (HEMTs) fabricated on a 200 mm diameter Si(111) substrate. In particular, RuO{sub x}-based gate is used due to the semitransparent nature to the optical excitation wavelengths, thus allowing much accurate thermal investigations underneath the gate. To determine the channel temperature profile in devices subjected to different electrical bias voltages, the GaN band-edge PL peak shift calibration with respect to temperature is used. PL analyses show a maximum channel temperature up to 435 K underneath the gate edge between gate and drain, where the estimated thermal resistance in such a HEMT structure is about 13.7 KmmW{sup −1} at a power dissipation of ∼10 W/mm. The temperature profiles from micro-Raman measurements are also addressed from the E{sub 2}-high optical phonon peak shift of GaN, and this method also probes the temperature-induced peak shifts of optical phonon from Si thus showing the nature of thermal characteristics at the AlN/Si substrate interface.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Atom probe tomography studies of Al₂O₃ gate dielectrics on GaN

Atom probe tomography was used to achieve three-dimensional characterization of in situ Al₂O₃/GaN structures grown by metal organic chemical vapor deposition (MOCVD). Al₂O₃ dielectrics grown at three different temperatures of 700, 900, and 1000 °C were analyzed and compared. A low temperature GaN cap layer grown atop Al₂O₃ enabled a high success rate in the atom probe experiments. The Al₂O₃/GaN interfaces were found to be intermixed with Ga, N, and O over the distance of a few nm. Impurity measurements data showed that the 1000 °C sample contains higher amounts of C (4 × 10¹⁹/cm³) and lower amounts of H (7 × 10¹⁹/cm³), whereas the 700 °C sample exhibits lower C impurities (<10¹⁷/cm³) and higher H incorporation (2.2 × 10²⁰/cm³). On comparing with Al₂O₃ grown by atomic layer deposition (ALD), it was found that the MOCVD Al₂O₃/GaN interface is comparatively abrupt. Scanning transmission electron microscopy data showed that the 900 °C and 1000 °C MOCVD films exhibit polycrystalline nature, while the ALD films were found to be amorphous.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Calculating time-resolved differential absorbance spectra for ultrafast pump-probe experiments with surface hopping trajectories

We report a surface hopping approach for modeling the full time- and frequency-resolved differential absorbance spectra (beyond the inhomogenous limit) obtained in ultrafast pump-probe experiments. In our approach, we combine dynamical information obtained from ensembles of classical trajectories propagated on the ground and on the excited potential energy surfaces to directly calculate optical response functions and hence spectral lineshapes. We demonstrate that our method is exact for the model problem of two shifted harmonic potentials with identical harmonic frequencies in the absence of electronic relaxation. We then consider a model three state system with electronic relaxation and show that our method is able to capture the effects of nonadiabatic excited state dynamics on the time-dependent differential absorbance spectra. Furthermore, by comparing our spectra against those spectra calculated with either an (1) inhomogenous expression, (2) ground-state Kubo theory, or (3) excited-state Kubo theory, we show that including dynamical information from both the ground and excited potential energy surfaces significantly improves the reliability of the semiclassical approximations. As such, our surface hopping method should find immediate use in modeling the time-dependent differential abosrbance spectra of ultrafast pump-probe experiments.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Invited Article: SUBGLACIOR: An optical analyzer embedded in an Antarctic ice probe for exploring the past climate

This article describes the advances made in the development of a specific optical spectrometer based on the Optical Feedback-Cavity Enhanced Absorption Spectroscopy technique for exploring past climate by probing the original composition of the atmosphere stored in the ice sheet of a glacier. Based on significant technological progresses and unconventional approaches, SUBGLACIOR will be a revolutionary tool for ice-core research: the optical spectrometer, directly embedded in the drilling probe, will provide in situ real-time measurements of deuterium isotopic variations (δ{sup 2}H ) and CH{sub 4} concentrations down to 3500 m of ice depth within a single Antarctic season. The instrument will provide simultaneous and real-time vertical profiles of these two key climate signatures in order to evaluate if a target site can offer ice cores as old as 1.5 million years by providing direct insight into past temperatures and climate cycles. The spectrometer has a noise equivalent absorption coefficient of 2.8 × 10{sup −10} cm{sup −1} Hz{sup −1/2}, corresponding to a detection limit of 0.2 ppbv for CH{sub 4} and a precision of 0.2‰ on the δ{sup 2}H of H{sub 2}O within 1 min acquisition time.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2015

Optoelectronically probing the density of nanowire surface trap states to the single state limit

Surface trap states play a dominant role in the optoelectronic properties of nanoscale devices. Understanding the surface trap states allows us to properly engineer the device surfaces for better performance. But characterization of surface trap states at nanoscale has been a formidable challenge using the traditional capacitive techniques. Here, we demonstrate a simple but powerful optoelectronic method to probe the density of nanowire surface trap states to the single state limit. In this method, we choose to tune the quasi-Fermi level across the bandgap of a silicon nanowire photoconductor, allowing for capture and emission of photogenerated charge carriers by surface trap states. The experimental data show that the energy density of nanowire surface trap states is in a range from 10{sup 9 }cm{sup −2}/eV at deep levels to 10{sup 12 }cm{sup −2}/eV near the conduction band edge. This optoelectronic method allows us to conveniently probe trap states of ultra-scaled nano/quantum devices at extremely high precision.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Investigating vibrational relaxation in cyanide-bridged transition metal mixed-valence complexes using two-dimensional infrared and infrared pump-probe spectroscopies

Using polarization-selective two-dimensional infrared (2D IR) and infrared pumpprobe spectroscopies, we study vibrational relaxation of the four cyanide stretching (CN) vibrations found in [(NH3)5RuIIINCFeII(CN)5] (FeRu) dissolved in D2O or formamide and [(NC)5FeIICNPtIV(NH3)4NCFeII(CN)5] 4 (FePtFe) dissolved in D2O. These cyanide-bridged transition metal complexes serve as models for understanding the role high frequency vibrational modes play in metal-to-metal charge transfers over a bridging ligand. However, there is currently little information about vibrational relaxation and dephasing dynamics of the anharmonically coupled CN modes in the electronic ground state of these complexes. IR pump-probe experiments reveal that the vibrational lifetimes of the CN modes are 2 times faster when FeRu is dissolved in D2O versus formamide. They also reveal that the vibrational lifetimes of the CN modes of FePtFe in D2O are almost four times as long as for FeRu in D2O. Combined with mode-specific relaxation dynamics measured from the 2D IR experiments, the IR pump-probe experiments also reveal that intramolecular vibrational relaxation is occurring in all three systems on 1 ps timescale. Center line slope dynamics, which have been shown to be a measure of the frequency-frequency correlation function, reveal that the radial, axial, and trans CN modes exhibit a 3 ps timescale for frequency fluctuations. This timescale is attributed to the forming and breaking of hydrogen bonds between each mode and the solvent. The results presented here along with our previous work on FeRu and FePtFe reveal a picture of coupled anharmonic CN modes where the spectral diffusion and vibrational relaxation dynamics depend on the spatial localization of the mode on the molecular complex and its specific interaction with the solvent.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2016

Optical method for distance and displacement measurements of the probe-sample separation in a scanning near-field optical microscope

In this work, we present an alternative optical method to determine the probe-sample separation distance in a scanning near-field optical microscope. The experimental method is based in a Lloyd’s mirror interferometer and offers a measurement precision deviation of ∼100 nm using digital image processing and numerical analysis. The technique can also be strategically combined with the characterization of piezoelectric actuators and stability evaluation of the optical system. It also opens the possibility for the development of an automatic approximation control system valid for probe-sample distances from 5 to 500 μm.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2016

Permeability studies of redox-sensitive nitroxyl spin probes in corn oil using an L-band ESR spectrometer

Electron spin resonance (ESR) studies were carried out for 2mM {sup 14}N labeled {sup 2}H enriched 3-methoxycarbonyl-2,2,5,5-tetramethyl-pyrrolidine-1-oxyl (MC-PROXYL) and 3–carboxy-2,2,5,5,-tetramethyl-1-pyrrolidinyloxy (carboxy-PROXYL) in pure water and various concentrations of corn oil. The ESR parameters, such as the line width, hyperfine coupling constant, g-factor, rotational correlation time, partition parameter and permeability were reported for the samples. The line width broadening was observed for both nitroxyl radicals in corn oil solutions. The partition parameter for permeable MC-PROXYL in corn oil increases with increasing concentration of corn oil, which reveals that the nitroxyl spin probe permeates into the oil phase. From the results, the corn oil concentration was optimized as 50 % for phantom studies. The rotational correlation time also increases with increasing concentration of corn oil. The permeable and impermeable nature of nitroxyl spin probes was demonstrated. These results will be useful for the development of ESR/OMR imaging modalities in in vivo and in vitro studies.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2016

Examination of biogenic selenium-containing nanosystems based on polyelectrolyte complexes by atomic force, Kelvin probe force and electron microscopy methods

The morphology and electrical properties of biogenic selenium-containing nanosystems based on polyelectrolyte complexes (PECs) were examined using AFM, Kelvin Probe Force and electron microscopy methods. It has been found, that prepared nanostructures significantly differed in their morphological types and parameters. In particular, multilayers capsules can be produced via varying synthesis conditions, especially, the selenium–PEC mass ratio ν. At the “special point” (ν = 0.1), filled and hollow nano- and microcapsules are formed in the system. The multilayer character of the capsules walls is visible in the phase images. Kelvin Probe Force images showed the inhomogeneity of potential distribution in capsules and outside them.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2017

Nuclear magnetic resonance probe head design for precision strain control

Here, we present the design and construction of an NMR probe to investigate single crystals under strain at cryogenic temperatures. The probe head incorporates a piezoelectric-based apparatus from Razorbill Instruments that enables both compressive and tensile strain tuning up to strain values on the order of 0.3% with a precision of 0.001%. 75 As NMR in BaFe 2 As 2 reveals large changes to the electric field gradient and indicates that the strain is homogeneous to within 16% over the volume of the NMR coil.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2017

Time and space resolved current density mapping in three dimensions using magnetic field probe array in a high voltage coaxial gap

We present an experimental analysis of the symmetry of current density in a coaxial geometry, diagnosed using a magnetic field probe array and calculations of the Fowler-Nordheim enhancement factor. Data were collected on the coaxial gap breakdown device (240 A, 25 kV, 150 ns, ~0.1 Hz), and data from experiments using 2 different gap sizes and different penetration depths are compared over runs comprising 50 shots for each case. The magnetic field probe array quantifies the distribution of current density at three axial locations, on either sides of a vacuum breakdown, and tracks the evolution with time and space. The results show asymmetries in current density, which can be influenced by changes in the gap size and the penetration depth (of the center electrode into the outer electrode). For smaller gap sizes (400 μm), symmetric current profiles were not observed, and the change in the penetration depth changes both the symmetric behavior of the current density and the enhancement factor. For larger gaps (900 μm), current densities were typically more uniform and less influenced by the penetration depth, which is reflected in the enhancement factor values. Furthermore it is possible that the change in inductance caused by the localization of current densities plays a role in the observed behavior.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2018

Development of a multi-channel capacitive probe for electric field measurements with fine spatial and high time resolution

A capacitive probe is one of a few diagnostics that is directly sensitive to the plasma potential. Using this diagnostic technique, a Multi-channel Linear Capacitive Probe (MLCP) is developed herein for turbulence measurements. The MLCP has 10 spatial channels and provides 9 points of radial electric field measurements simultaneously with a spatial step of 7 mm. A new readout circuit and a correction technique for low frequency attenuation are also developed to achieve the required spatial and time resolution. A performance test of the MLCP using a reversed field pinch plasma confirms that the MLCP resolves sub-centimeter structures of the equilibrium radial electric field profile and fluctuations up to 680 kHz.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗