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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 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Compact high repetition rate Thomson parabola ion spectrometer

Here, we present the development of a compact Thomson parabola ion spectrometer capable of characterizing the energy spectra of various ion species of multi-MeV ion beams from >10 20 W/cm 2 laser produced plasmas at rates commensurate with the highest available from any of the current and near-future PW-class laser facilities. This diagnostic makes use of a polyvinyl toluene based fast plastic scintillator (EJ-260), and the emitted light is collected using an optical imaging system coupled to a thermoelectrically cooled scientific complementary metal–oxide–semiconductor camera. This offers a robust solution for data acquisition at a high repetition rate, while avoiding the added complications and nonlinearities of micro-channel plate based systems. Different ion energy ranges can be probed using a modular magnet setup, a variable electric field, and a varying drift-distance. We have demonstrated operation and data collection with this system at up to 0.2 Hz from plasmas created by irradiating a solid target, limited only by the targeting system. With the appropriate software, on-the-fly ion spectral analysis will be possible, enabling real-time experimental control at multi-Hz repetition rates.

47 OTHER INSTRUMENTATION↗
DOE OSTI2021

Ultraviolet photodissociation of gas-phase iron pentacarbonyl probed with ultrafast infrared spectroscopy

It is well known that ultraviolet photoexcitation of iron pentacarbonyl results in rapid loss of carbonyl ligands leading to the formation of coordinatively unsaturated iron carbonyl compounds. Here we employ ultrafast mid-infrared transient absorption spectroscopy to probe the photodissociation dynamics of gas-phase iron pentacarbonyl following ultraviolet excitation at 265 and 199 nm. After photoexcitation at 265 nm, our results show evidence for sequential dissociation of iron pentacarbonyl to form iron tricarbonyl via a short-lived iron tetracarbonyl intermediate. Photodissociation at 199 nm results in the prompt production of Fe(CO) 3 within 0.25 ps via several energetically accessible pathways. An additional 15 ps time constant extracted from the data is tentatively assigned to intersystem crossing to the triplet manifold of iron tricarbonyl or iron dicarbonyl. Mechanisms for formation of iron tetracarbonyl, iron tricarbonyl, and iron dicarbonyl are proposed and theoretically validated with one-dimensional cuts through the potential energy surface as well as bond dissociation energies. Ground state calculations are computed at the CCSD(T) level of theory and excited states are computed with EOM-EE-CCSD(dT).

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

Insights into Sustainable Nitrogen Fixation by Gas-phase Spectroscopic Measurements and Global Modeling of Reaction Intermediates in Humid Nitrogen Plasma

In this article, there is growing interest in reacting molecular nitrogen and water to sustainably synthesize fixed forms of nitrogen such as ammonia. In particular, low-temperature plasmas can activate these relatively inert feedstocks at or near room temperature without a catalyst. However, because of the enhanced reactivity and nonequilibrium chemistry, a diverse range of products is formed, and the underlying reaction mechanisms are exceedingly complex. In this work, we studied a simplified reactor consisting of a gaseous plasma containing controlled mixtures of nitrogen gas and water vapor. Densities of key chemical species such as N, H, OH, NH, and NO were measured by emission and laser-based spectroscopy as a function of the relative humidity. A global model was constructed and the reaction network was validated by comparing calculated species densities with experiments. We discover that N, a key initial intermediate for ammonia, strongly decreases in the presence of water vapor, and as a result, ammonia formation becomes limited at high relative humidity. This decrease is surprisingly not because N itself reacts, but because one of its main sources, an excited molecular nitrogen state, is reacted away. In addition, oxidation pathways for nitrogen, which lead to NO and related products, are found to be favored over reduction pathways because the corresponding reverse reactions are less significant. Together, this understanding helps explain previously reported observations of selectivity toward nitrogen oxides over ammonia, particularly at higher relative humidities.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Attosecond Optical Orientation

Circularly polarized light offers opportunities to probe symmetry-dependent properties of matter such as chirality and spin. Circular-dichroic measurements typically require further intrinsic or extrinsic breaking of symmetry by, e.g., enantiomeric excess, orientation, magnetic fields, or direction-sensitive detectors. Here we introduce circular-dichroic attosecond transient absorption spectroscopy by leveraging the angular momentum of two circularly polarized pulses, both pump and probe, in an isotropic medium, optically orienting the angular momentum of excited states on an attosecond timescale. We investigate a circular-dichroic measurement of the attosecond transient absorption of He Rydberg states. By limiting the allowed pathways via dipole selection rules for co- and counterrotating circularly polarized near-infrared and extreme ultraviolet (XUV) pulses, different spectral reshapings of the XUV transient absorption due to the AC Stark effect are observed. Furthermore, paired with time-dependent Schrödinger equation calculations, the results show the role of selection and propensity rules and open up new opportunities to study coupling pathways of excited states as well as spin-dependent dynamics in atoms and beyond via attosecond optical orientation.

Angular momentum of light↗
DOE OSTI2026

Proton beam enhancements from ultrafast laser interactions with compound parabolic concentrators

Target normal sheath acceleration (TNSA) is among the most widely studied laser–plasma ion acceleration mechanisms. In this Letter, we report on studies of proton acceleration from flat Cu targets with cone-like focusing structures called compound parabolic concentrators (CPCs) coupled to their front surface. The CPC acts as a non-imaging focusing optic that enhances the laser intensity at the target's front surface by ∼2×, from 9 × 10 18 to 2 × 10 19 W/cm 2 . This effect drives a reduction in the particle source size from the typical laser spot size of 120 μm to the CPC tip size of 65 μm and significant enhancements in the peak energy and temperature (2.6 × increase) of the resulting TNSA proton beam. We also observe increased opening angle of the beam. 2D PIC simulations have been conducted and replicate the experimental behavior. These increases have implications for long focal length facilities that require higher energy proton beams, which now can be achieved without significant infrastructure changes.

3D printing↗
DOE OSTI2021

Coupled valence carrier and core-exciton dynamics in WS 2 probed by few-femtosecond extreme ultraviolet transient absorption spectroscopy

Few-femtosecond extreme ultraviolet (XUV) transient absorption spectroscopy, performed with optical 500-1000 nm supercontinuum and broadband XUV pulses (30-50 eV), simultaneously probes dynamics of photoexcited carriers in WS$_{2}$ at the W O$_3$ edge (37-45 eV) and carrier-induced modifications of core-exciton absorption at the W N$_{6,7}$ edge (32-37 eV). Access to continuous core-to-conduction band absorption features and discrete core-exciton transitions in the same XUV spectral region in a semiconductor provides a novel means to investigate the effect of carrier excitation on core-exciton dynamics. The core-level transient absorption spectra, measured with either pulse arriving first to explore both core-level and valence carrier dynamics, reveal that core-exciton transitions are strongly influenced by the photoexcited carriers. A $1.2\pm0.3$ ps hole-phonon relaxation time and a $3.1\pm0.4$ ps carrier recombination time are extracted from the XUV transient absorption spectra from the core-to-conduction band transitions at the W O$_{3}$ edge. Global fitting of the transient absorption signal at the W N$_{6,7}$ edge yields $\sim 10$ fs coherence lifetimes of core-exciton states and reveals that the photoexcited carriers, which alter the electronic screening and band filling, are the dominant contributor to the spectral modifications of core-excitons and direct field-induced changes play a minor role. This work provides a first look at the modulations of core-exciton states by photoexcited carriers and advances our understanding of carrier dynamics in metal dichalcogenides.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Generation of radioisotopes for medical applications using high-repetition, high-intensity lasers

We used the PW high-repetition laser facility VEGA-3 at Centro de Láseres Pulsados in Salamanca, with the goal of studying the generation of radioisotopes using laser-driven proton beams. Various types of targets have been irradiated, including in particular several targets containing boron to generate α-particles through the hydrogen–boron fusion reaction. We have successfully identified γ-ray lines from several radioisotopes created by irradiation using laser-generated α-particles or protons including 43 Sc, 44 Sc, 48 Sc, 7 Be, 11 C and 18 F. We show that radioisotope generation can be used as a diagnostic tool to evaluate α-particle generation in laser-driven proton–boron fusion experiments. We also show the production of 11 C radioisotopes, ≈ 6 × 10 6 , and of 44 Sc radioisotopes, ≈ 5 × 10 4 per laser shot. This result can open the way to develop laser-driven radiation sources of radioisotopes for medical applications.

gamma ray spectroscopy↗
DOE OSTI2025

Electromagnetic moments of 215,217 Bi: Probing shell evolution beyond N = 126

The nuclear properties of bismuth isotopes (Z = 83) , with just one valence proton above the closed spherical shell at (Z = 82) , are expected to be governed by a single unpaired proton. However, already in semimagic 209 Bi (Z = 83, N = 126) , , the magnetic moment (μ) strongly deviates from the single-particle Schmidt value. A near linear decrease in μ with the increase of N after the N = 126 magic number was observed up to N = 130 . In order to test whether this trend is kept at N > 130 and to reveal the underlying mechanisms, an investigation of 215,217 Bi (N = 132, 134) has been undertaken. The magnetic dipole and electric quadrupole moments of the I π = 9/2 - nuclear ground states in these isotopes have been measured for the first time using the in-source resonance-ionization spectroscopy technique at ISOLDE (CERN). It has been shown that the linearly decreasing trend of μ( 209,211,213 Bi g ) is broken in 215,217 Bi with a nearly constant value of μ observed. Experimental data have been compared to calculations in the framework of the configuration-interaction shell model with the monopole-based universal V MU +LS interaction. The peculiarities in the behavior of μ(Bi, 9/2 - ) with increasing neutron number are explained as being due to the shell evolution, change of the neutron orbitals occupancies and strong configuration mixing beyond N = 130 . Also, the difference in the μ trends for bismuth (Z = 83) and astatine (Z = 85) isotopes with N > 126 are reproduced by the shell-model calculations. It is shown that monopole interaction plays noticeable role in the description of the peculiarities of the μ behaviour. Additionally, the extension of the application of the V MU interaction to the μ isotopic trends for heavy nuclei is important for further study of the capabilities of this promising version of the shell-model calculations.

Dipole magnetic moments↗
DOE OSTI2025

Charge radii and electromagnetic moments of 214−218 Bi : Exploring the “southern” border of the 𝑍 > 82 octupole-deformation region

The changes in the mean-squared charge radii relative to 209 Bi 126 (𝛿⁢⟨𝑟 2 ⟩ 𝑁,126 ) and the magnetic dipole and electric quadrupole moments in 214−218 Bi have been measured using the in-source resonance-ionization spectroscopy technique at ISOLDE (CERN). Magnetic moments of odd-odd bismuth nuclei have been analyzed by the additivity relation. Previous tentative spin-parity and configuration assignments based on the 𝛽-decay feeding patterns have been supported. A normal odd-even staggering in charge radii of bismuth isotopes with 𝑁>126 has been observed. The new data for the 𝛿⁡⟨𝑟 2 ⟩ of bismuth isotopes allow a study of the isotonic dependencies in the charge radii, revealing jumps in 𝛿⁢⟨𝑟 2 ⟩ 132,126 and 𝛿⁢⟨𝑟 2 ⟩ 134,126 at 𝑍 = 84. This pattern could be explained by a sudden onset of octupole deformation at 𝑁 = 132 and 134 when going from polonium (𝑍 = 84) to astatine (𝑍 = 85).

fundamental symmetries↗
DOE OSTI2020

What can we learn from N 2 O isotope data? – Analytics, processes and modelling

The isotopic composition of nitrous oxide (N 2 O) provides useful information for evaluating N 2 O sources and budgets. Due to the co–occurrence of multiple N 2 O transformation pathways, it is, however, challenging to use isotopic information to quantify the contribution of distinct processes across variable spatiotemporal scales. Here, we present an overview of recent progress in N 2 O isotopic studies and provide suggestions for future research, mainly focusing on: analytical techniques; production and consumption processes; and interpretation and modelling approaches. Comparing isotope–ratio mass spectrometry (IRMS) with laser absorption spectroscopy (LAS), we conclude that IRMS is a precise technique for laboratory analysis of N 2 O isotopes, while LAS is more suitable for in situ/inline studies and offers advantages for site–specific analyses. When reviewing the link between the N 2 O isotopic composition and underlying mechanisms/processes, we find that, at the molecular scale, the specific enzymes and mechanisms involved determine isotopic fractionation effects. In contrast, at plot–to–global scales, mixing of N 2 O derived from different processes and their isotopic variability must be considered. We also find that dual isotope plots are effective for semi–quantitative attribution of co–occurring N 2 O production and reduction processes. More recently, process–based N 2 O isotopic models have been developed for natural abundance and 15 N–tracing studies, and have been shown to be effective, particularly for data with adequate temporal resolution. Here, despite the significant progress made over the last decade, there is still great need and potential for future work, including development of analytical techniques, reference materials and inter–laboratory comparisons, further exploration of N 2 O formation and destruction mechanisms, more observations across scales, and design and validation of interpretation and modelling approaches. Synthesizing all these efforts, we are confident that the N 2 O isotope community will continue to advance our understanding of N 2 O transformation processes in all spheres of the Earth, and in turn to gain improved constraints on regional and global budgets.

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

Large-scale atomistic model construction of subbituminous and bituminous coals for solvent extraction simulations with reactive molecular dynamics

Large-scale atomistic models for complex polycyclic aromatic hydrocarbon systems help understand the chemical properties and behaviors of complex feedstocks such as coal or petroleum. However, the development and utilization of large-scale models remain limited due to the difficulty in achieving the varied structural characteristics necessary to capture stochastic nature of these feedstocks. Here we demonstrate a systematic workflow to construct stochastic molecular systems from a broad analytical suite: high-resolution transmission electron microscopy (HRTEM), carbon-13 nuclear magnetic resonance spectroscopy ( 13 C NMR), laser desorption ionization mass spectroscopy (LDI-MS), and elemental analysis. We present a model construction and analysis utility of a new Python-based module. We selected one subbituminous and three high-volatile bituminous coals to construct large-scale models (~40,000 atoms). The constructed models were utilized to examine the affinity for solvent extraction (naphthalene or tetralin) and the effect of structural properties (e.g., aromatic cluster size, functional groups, and cross-linking) in reactive molecular dynamics simulations. Complex chemical reactions were monitored with bond order transitions, intermediates formation, and mass distributions. Reactive molecular dynamics simulations suggest a plausible chemical extraction process and products for the complex fossil feedstocks. The results indicated that radical formations with bond breaking of bridging oxygens and carbons were required at high temperatures to facilitate hydrogeneration and extraction of gas molecules from radical-free molecules. We observed that aliphatic chains of tetralin were easily decomposed and combined with radicals to form small size of molecules with aryl bonding, mainly increasing molecules in the 500–1000 Da, while naphthalene had little impact on chemical extraction process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2025

Methane pyrolysis by Joule heating for graphitic carbon and hydrogen production

The global energy transition toward sustainability requires technologies that can decarbonize energy carriers and fuels while producing valuable materials. Methane, a primary component of natural gas, is both a high-energy-density fuel and a significant greenhouse gas. This study reports an approach for methane pyrolysis utilizing Joule heating within the deposition substrate to drive the endothermic reaction. With electric current passing through a resistive porous carbon cloth, heat is generated to break C-H bonds of methane molecules. Here, the decomposition of methane as it flows through the cloth results in hydrogen production and the formation of conformally layered graphite around the carbon fibers. The effects of input power, chamber pressure, feedstock flow rate, and process duration on hydrogen and graphite production are characterized via in situ mass spectrometry and laser absorption spectroscopy, resulting in methane conversion rates up to 88%, with hydrogen and carbon yields of 82% and 72%, respectively. Material characterization verifies uniform high-quality graphite deposition, with a Raman I D /I G ratio of 0.1 and 3.38 Å d-spacing. This Joule heating method for catalyst-free methane pyrolysis offers the potential for advancing hydrogen production technology by simultaneously producing valuable materials such as solid graphite, thus enhancing the economic viability of the fuel decarbonization process.

Energy Resources↗
DOE OSTI2020

The 1.66 μm spectrum of the ethynyl radical, CCH

Frequency-modulated diode laser transient absorption spectra of the ethynyl radical have been recorded at wavelengths close to 1.66 μm. The observed spectrum includes strong, regular, line patterns. The two main bands observed originate in the ground $\tilde{χ}$ 2 Σ + state and its first excited bending vibrational level of 2 $Π$ symmetry. The upper states, of 2 Σ + symmetry at 6055.6 cm -1 and 2 $Π$ symmetry at 6413.5 cm -1 , respectively, had not previously been observed and the data were analyzed in terms of an effective Hamiltonian representing their rotational and fine structure levels to derive parameters which can be used to calculate rotational levels up to J = 37/2 for the 2 $Π$ level and J = 29/2 for the 2 Σ one. Additionally, a weaker series of lines have been assigned to absorption from the second excited bending, (0 2 0), level of 2 Σ symmetry, to a previously observed state of 2 $Π$ symmetry near 6819 cm -1 . These strong absorption bands at convenient near-IR laser wavelengths will be useful for monitoring CCH radicals in chemical systems.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Spectroscopic study and lifetime measurement of the 6d7p 3 F 2 o state of radium

We report a method for the precision measurement of the oscillator strengths and the branching fractions of the decay channels of the 6d7p 3 F 2 o state in 226 Ra. Here, this method exploits a set of metastable states present in Ra, allowing a measurement of the oscillator strengths that does not require knowledge of the number of atoms in the atomic beam. We measure the oscillator strengths and the branching fractions for decays from the 6d7p 3 F 2 o state to the 7s6d 3 D 1 , 7s6d 3 D 2 , and 7s6d 1 D 2 states and constrain the branching fraction to the 7s6d 3 D 3 state to be less than 0.4% (68% confidence limit). The lifetime of the 3 F 2 o state is determined to be 15 ± 4 ns.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2020

Surface Enhanced Raman Scattering Selectivity in Proteins Arises from Electron Capture and Resonant Enhancement of Radical Species

Plasmon-enhanced Raman scattering is a powerful approach to detecting and characterizing proteins in live and dynamic biological systems. However, the selective detection/enhancement of specific residues as well as spectral diffusion and fluctuations have complicated the interpretation of enhanced Raman spectra and images of biological matter. In this paper, we therefore demonstrate that the amino acid tryptophan (Trp) can capture an electron from an excited plasmon, which generates a radical anion that is resonantly enhanced: a visible excited electronic state slides into resonance upon charging. This surface enhanced resonance Raman scattering (SERRS) mechanism explains the persistence of Trp signatures in the SERS and TERS spectra of proteins. Evidence for this picture includes the observation of visible resonances in the UV-Vis extinction spectrum, changes in the ground state vibrational spectrum, and plasmon-resonance dependent behavior. DFT calculations support the experimental observations. The behavior observed from the free Trp molecule is shown to explain the SERS spectrum of the Trp-cage protein. In effect, resonant Raman scattering from radicals formed through plasmonic excitation represents an under-investigated mechanism that may be exploited for chemical sensing applications. This work was supported by the National Institutes of Health Award R01-GM109988. The authors thank Hannah Shafaat for helpful discussions and providing an azurin sample for comparison. The authors also thank Joel Harris for providing constructive comments on our manuscript.

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

EPR of Photoexcited Triplet-State Acceptor Porphyrins

The photoexcited triplet states of porphyrin architectures are of significant interest in a wide range of fields including molecular wires, nonlinear optics, and molecular spintronics. Electron paramagnetic resonance (EPR) is a key spectroscopic tool in the characterization of these transient paramagnetic states singularly well suited to quantify spin delocalization. Previous work proposed a means of extracting the absolute signs of the zero-field splitting (ZFS) parameters, D and E, and triplet sublevel populations by transient continuous wave, hyperfine measurements, and magnetophotoselection. Here, we present challenges of this methodology for a series of mesoperfluoroalkyl-substituted zinc porphyrin monomers with orthorhombic symmetries, where interpretation of experimental data must proceed with caution and the validity of the assumptions used in the analysis must be scrutinized. The EPR data are discussed alongside quantum chemical calculations, employing both DFT and CASSCF methodologies. Despite some success of the latter in quantifying the magnitude of the ZFS interaction, the results clearly provide motivation to develop improved methods for ZFS calculations of highly delocalized organic triplet states.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2022

Super-Resolution Airy Disk Microscopy of Individual Color Centers in Diamond

Super-resolution imaging techniques enable nanoscale microscopy in fields such as physics, biology, and chemistry. However, many super-resolution techniques require specialized optical components, such as a helical-phase mask. In this work, we present a novel technique, super-resolution Airy disk microscopy, that can be used in a standard confocal microscope without any specialized optics. We demonstrate this technique, in combination with ground state depletion, to image and control nitrogen-vacancy (NV) centers in bulk diamond below the diffraction limit. A greater than 14-fold improvement in resolution compared to the diffraction limit is achieved, corresponding to a spatial resolution of 16.9(8) nm for a 1.3 NA microscope with 589 nm light. We make use of our enhanced spatial resolution to control the spins states of individual NV centers separated from each other by less than the diffraction limit, including pairs sharing the same orientation that are indistinguishable with a conventional electron spin resonance measurement.

36 MATERIALS SCIENCE↗