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At least 1,009 records · Page 56
All sourcesNASA NTRSDOE OSTI
DOE OSTI2022

Sequential Bond Dissociation Energies of Th + (CO) x , x = 3–6: Guided Ion Beam Collision-Induced Dissociation and Quantum Computational Studies

Collision-induced dissociation (CID) of [Th,xC,xO] + , x = 3–6, with Xe is performed using a guided ion beam tandem mass spectrometer (GIBMS). Products are formed exclusively by the loss of CO ligands. Analyses of the kinetic energy-dependent CID product cross sections yield bond dissociation energies (BDEs) of (CO) x–1 Th + –CO at 0 K as 1.09 ± 0.05, 0.82 ± 0.07, 0.63 ± 0.05, and 0.70 ± 0.05 eV, respectively. Different structures of [Th,xC,xO] + were explored using various electronic structure methods, and BDEs for CO ligand loss from precursor [Th,xC,xO] + complexes were computed. Both experimental and theoretical results corroborate that the structures of [Th,xC,xO] + , x = 3–6, formed experimentally are homoleptic thorium cation carbonyl complexes, Th + (CO) x . The nonmonotonic trend in experimental BDEs is reproduced theoretically, although ambiguities in the spin states of the x = 4–6 complexes (doublet or quartet) remain. BDEs calculated at the coupled cluster with single, double, and perturbative triple excitations (CCSD(T))/cc-pVXZ//B3LYP/cc-PVXZ (X = T and Q) level and a complete basis set (CBS) extrapolation agree reasonably well with the experimental values for all complexes. Thorium oxide ketenylidene carbonyl cations, OTh + CCO(CO) y , y = 1–4, were calculated to be the most stable structures of [Th,xC,xO] + , x = 3–6, respectively; however, these are not observed in our experiment. Potential energy profiles (PEPs) having either quartet or doublet spin calculated at the B3LYP/cc-pVQZ level suggest that the failure to observe OTh + CCO(CO) y , y = 1–4, is the result of a barrier corresponding to the C–C bond formation, making the formation of OTh + CCO(CO) y inaccessible kinetically under the present experimental conditions.

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

Controlled Spalling of 4H Silicon Carbide with Investigated Spin Coherence for Quantum Engineering Integration

We detail scientific and engineering advances which enable the controlled spalling and layer transfer of single crystal 4H silicon carbide (4H-SiC) from bulk substrates. 4HSiC’s properties, including high thermal conductivity and a wide bandgap, make it an ideal semiconductor for power electronics. Moreover, 4H-SiC is an excellent host of solid-state atomic defect qubits for quantum computing and quantum networking. Because 4H-SiC substrates are expensive (due to long growth times and limited yield), techniques for removal and transfer of bulk-quality films are desirable for substrate reuse and integration of the separated films. In this work, we utilize updated approaches for stressor layer thickness control and spalling crack initiation to demonstrate controlled spalling of 4H-SiC, the highest fracture toughness crystal spalled to date. We achieve coherent spin control of neutral divacancy (VV 0 ) qubit ensembles and measure a quasi-bulk spin T 2 of 79.7 μs in the spalled films.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Direct Conversion of Methane to Ethylene and Acetylene over an Iron-Based Metal–Organic Framework

Conversion of methane (CH 4 ) to ethylene (C 2 H 4 ) and/or acetylene (C 2 H 2 ) enables routes to a wide range of products directly from natural gas. However, high reaction temperatures and pressures are often required to activate and convert CH 4 controllably, and separating C 2+ products from unreacted CH 4 can be challenging. Here, we report the direct conversion of CH 4 to C 2 H 4 and C 2 H 2 driven by non-thermal plasma under ambient (25 °C and 1 atm) and flow conditions over a metal–organic framework material, MFM-300(Fe). The selectivity for the formation of C 2 H 4 and C 2 H 2 reaches 96% with a high time yield of 334 μmol g cat –1 h –1 . At a conversion of 10%, the selectivity to C 2+ hydrocarbons and time yield exceed 98% and 2056 μmol g cat –1 h –1 , respectively, representing a new benchmark for conversion of CH 4 . In situ neutron powder diffraction, inelastic neutron scattering and solid-state nuclear magnetic resonance, electron paramagnetic resonance (EPR), and diffuse reflectance infrared Fourier transform spectroscopies, coupled with modeling studies, reveal the crucial role of Fe–O(H)–Fe sites in activating CH 4 and stabilizing reaction intermediates via the formation of an Fe–O(CH 3 )–Fe adduct. In addition, a cascade fixed-bed system has been developed to achieve online separation of C 2 H 4 and C 2 H 2 from unreacted CH 4 for direct use. Integrating the processes of CH 4 activation, conversion, and product separation within one system opens a new avenue for natural gas utility, bridging the gap between fundamental studies and practical applications in this area.

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

Many-body enhancement of high-harmonic generation in monolayer MoS2

Abstract Many-body effects play an important role in enhancing and modifying optical absorption and other excited-state properties of solids in the perturbative regime, but their role in high harmonic generation (HHG) and other nonlinear response beyond the perturbative regime is not well-understood. We develop here an ab initio many-body method to study nonperturbative HHG based on the real-time propagation of the non-equilibrium Green’s function with the GW self energy. We calculate the HHG of monolayer MoS 2 and obtain good agreement with experiment, including the reproduction of characteristic patterns of monotonic and nonmonotonic harmonic yield in the parallel and perpendicular responses, respectively. Here, we show that many-body effects are especially important to accurately reproduce the spectral features in the perpendicular response, which reflect a complex interplay of electron-hole interactions (or exciton effects) in tandem with the many-body renormalization and Berry curvature of the independent quasiparticle bandstructure.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Cluster defects in gibbsite nanoplates grown at acidic to neutral pH

Gibbsite [α-Al(OH) 3 ] is the solubility limiting phase for aluminum across a wide pH range, and it is a common mineral phase with many industrial applications. The growth mechanism of this layered-structure material, however, remains incompletely understood. Synthesis of gibbsite at low to circumneutral pH yields nanoplates with substantial interlayer disorder. Here we examine defects in this material in detail, and the effects of recrystallization in highly alkaline sodium hydroxide solution at 80 °C. We employed a multimodal approach, including scanning electron microscopy, magic-angle spinning nuclear magnetic resonance (MAS-NMR), Raman and infrared spectroscopies, X-ray diffraction (XRD), and X-ray total scattering pair distribution function (XPDF) analysis to characterize the ageing of the nanoplates over several days. Additionally, XRD and XPDF indicate that gibbsite nanoplates precipitated at circumneutral pH contain dense, truncated sheets imparting a local difference in interlayer distance. These interlayer defects appear well described by flat Al 13 aluminum hydroxide nanoclusters nearly isostructural with gibbsite sheets present under synthesis conditions and trapped as interlayer inclusions during growth. Ageing at elevated temperature in alkaline solutions gradually improves crystallinity, showing a gradual increase in H-bonding between interlayer OH groups. Between 7 to 8 vol% of the initial gibbsite nanoparticles exhibit this defect, with the majority of differences disappearing after 2–4 hours of recrystallization in alkaline solution. The results not only identify the source of disorder in gibbsite formed under acidic/neutral conditions but also point to a possible cluster-mediated growth mechanism evident through inclusion of relict oligomers with gibbsite-like topology trapped in the interlayer spaces.

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

Towards constraining cosmological parameters with SPT-3G observations of 25% of the sky

The South Pole Telescope (SPT), using its third-generation camera, SPT-3G, is conducting observations of the cosmic microwave background (CMB) in temperature and polarization across approximately 10 000 deg$^2$ of the sky at 95, 150, and 220 GHz. This comprehensive dataset should yield stringent constraints on cosmological parameters. In this work, we explore its potential to address the Hubble tension by forecasting constraints from temperature, polarization, and CMB lensing on early dark energy (EDE) and the variation in electron mass in spatially flat and curved universes. For this purpose, we investigate first whether analyzing the distinct SPT-3G observation fields independently, as opposed to as a single, unified region, results in a loss of information relevant to cosmological parameter estimation. We develop a realistic temperature and polarization likelihood pipeline capable of analyzing these fields in these two ways, and subsequently forecast constraints on cosmological parameters. Our findings indicate that any loss of constraining power from analyzing the fields separately is primarily concentrated at low multipoles ($\ell$ < 50) and the overall impact on the relative uncertainty on standard $Λ$ cold dark matter parameters is minimal (< 3%). Our forecasts suggest that SPT-3G data should improve by more than a factor of 90 and 190 the figure of merit of the EDE and the varying electron mass models, respectively, when combined with Planck data. The likelihood pipeline developed and used in this work is made publicly available online.

Vitrier, A. [Paris, Inst. Astrophys.]↗
DOE OSTI2024

Determination of Vibrational Motions Driving Photoinduced Electron Transfer Reactions in Molecular Crystals and Organic Thin Films

The objective of this research is to develop an understanding of how nuclear motions can be used to drive and control photo-induced charge transfer and singlet fission reactions in molecular crystals and thin films. By following the structural evolution of reacting molecules and nanostructures on the timescale of their nuclear motion, we will determine what interplay of nuclear coordinates is most efficient in driving electron transfers, a necessary first step in most photovoltaic and photocatalytic processes. We will identify which nuclear coordinates effectively promote desirable electron transfer processes, or ineffectively dissipate photon energy into unwanted thermal energy, thus guiding the design and implementation of molecular systems tailored for high efficiency processes. Specifically, we aim to identify which nuclear coordinates are responsible for driving electron transfer and singlet fission reactions at different points along the reaction coordinate, particularly in regimes which deviate from Marcus theory predictions. We will do so by investigating systems with electron transfer and singlet fission occurring from non-thermalized states due to strong donor-acceptor electronic coupling. First, we will prove that specific vibrational modes are responsible for charge transfer processes in molecular crystals. Secondly, we will investigate how vibrational coherences and specific nuclear motions can be used to drive high yield singlet fission processes. Finally, we will determine how complex film morphology affects long-range charge transport, a key limiting factor in our ability to make gains in efficiency.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2022

Conformer-Specific Dissociation Dynamics in Dimethyl Methylphosphonate Radical Cation

The dynamics of the dimethyl methylphosphonate (DMMP) radical cation after production by strong field adiabatic ionization have been investigated. Pump-probe experiments using strong field 1300 nm pulses to adiabatically ionize DMMP and a 800 nm non-ionizing probe induce coherent oscillations of the parent ion yield with a period of about 45 fs. The yields of two fragments, PO 2 C 2 H 7 + and PO 2 CH 4 + , oscillate approximately out of phase with the parent ion, but with a slight phase shift relative to each other. We use electronic structure theory and nonadiabatic surface hopping dynamics to understand the underlying dynamics. The results show that while the cation oscillates on the ground state along the P=O bond stretch coordinate, the probe excites population to higher electronic states that can lead to fragments PO 2 C 2 H 7 + and PO 2 CH 4 + . The computational results combined with the experimental observations indicate that the two conformers of DMMP that are populated under experimental conditions exhibit different dynamics after being excited to the higher electronic states of the cation leading to different dissociation products. These results highlight the potential usefulness of these pump-probe measurements as a tool to study conformer-specific dynamics in molecules of biological interest.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2022

Cyanobacterial photosystem II reaction center design in tobacco chloroplasts increases biomass in low light

Abstract The D1 polypeptide of the photosystem II (PSII) reaction center complex contains domains that regulate primary photochemical yield and charge recombination rate. Many prokaryotic oxygenic phototrophs express two or more D1 isoforms differentially in response to environmental light needs, a capability absent in flowering plants and algae. We report that tobacco (Nicotiana tabacum) plants carrying the Synechococcus (Synechococcus elongatus PCC 7942) low-light mutation (LL-E130Q) in the D1 polypeptide (NtLL) acquire the cyanobacterial photochemical phenotype: faster photodamage in high light and significantly more charge separations in productive linear electron flow in low light. This flux increase produces 16.5% more (dry) biomass under continuous low-light illumination (100 μE m−2 s−1, 24 h). This gain is offset by the predicted lower photoprotection at high light. By contrast, the introduction of the Synechococcus high-light mutation (HL-A152S) into tobacco D1 (NtHL) has slightly increased photoprotection, achieved by photochemical quenching, but no apparent impact on biomass yield compared to wild type under the tested conditions. The universal design principle of all PSII reaction centers trades off energy conversion for photoprotection in different proportions across all phototrophs and provides a useful guidance for testing in crop plants. The observed biomass advantage under continuous low light can be transferred between evolutionarily isolated lineages to benefit growth under artificial lighting conditions. However, removal of the selective marker gene was essential to observe the growth phenotype, indicating growth penalty imposed by use of the particular spectinomycin-resistance gene.

Zhang, Yuan (ORCID:0000000291785207)↗
DOE OSTI2021

Parabolic oxidation kinetics of a plutonium alloy at room temperature

Auger electron spectroscopy (AES) was used to characterize the oxide scale formed on an ~0.5 wt. % Ga plutonium metal alloy. Analysis of changes to the characteristic Auger transitions for Pu and O during sputter depth profiles were used in combination with previously measured sputter yields to determine the thickness of the oxide scale and provide insight into its chemistry. From this data, the parabolic kinetics for the Pu-Ga alloy were determined as a function of relative humidity, RH = 14–92%, and oxygen partial pressure, p(O 2 ) = 31–157 Torr, at 25°C. For each relative humidity investigated, the parabolic rate constant was found to be independent of oxygen partial pressure. Furthermore, power-law fits to the relative humidity effect on the rate constant was found to have a power of n = 1.265, indicating the diffusion species which rate-limits the reaction isn’t molecular water, which subsequent dissociates at the oxide-metal interface, or hydroxyl from dissociation at the gas-surface interface.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Modeling electron beam irradiation of methane

We built a chemical kinetic model for the electron beam irradiation of methane and report simulation results with dose rates ranging from 2 to 200 kGy s -1 at 298 K and 1 atm pressure. The model contains 92 species and 778 gas-phase reactions. We report the time evolution of concentrations of stable products (including H 2 , C 2 H 6 , C 3 H 8 , C 2 H 4 , C 3 H 6 , C 4 H 10 , C 2 H 2 , and C 3 H 4 ) as well as some radicals and ions. Here we discuss how yields of products depend on dose rate and how they change during the course of irradiation. To understand the processes controlling product formation, we quantify the extent to which various reactions produce and destroy major products and the key radicals and ions. Normalized sensitivity coefficients are computed for the production of stable products to gain further insight into factors controlling product yields. We were able to reduce the mechanism to 63 species and 331 reactions while incurring less than 5% error in the final concentrations of stable products.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Delocalization and Universality of the Fractional Quantum Hall Plateau-to-Plateau Transitions

Disorder and electron-electron interaction play essential roles in the physics of electron systems in condensed matter. In two-dimensional, quantum Hall systems, extensive studies of disorder-induced localization have led to the emergence of a scaling picture with a single extended state, characterized by a power-law divergence of the localization length in the zero-temperature limit. Experimentally, scaling has been investigated via measuring the temperature dependence of plateau-to-plateau transitions between the integer quantum Hall states (IQHSs), yielding a critical exponent κ ≃ 0.42. Here, in this study, we report scaling measurements in the fractional quantum Hall state (FQHS) regime where interaction plays a dominant role. Our Letter is partly motivated by recent calculations, based on the composite fermion theory, that suggest identical critical exponents in both IQHS and FQHS cases to the extent that the interaction between composite fermions is negligible. The samples used in our experiments are two-dimensional electron systems confined to GaAs quantum wells of exceptionally high quality. We find that κ varies for transitions between different FQHSs observed on the flanks of Landau level filling factor v = 1/2 and has a value close to that reported for the IQHS transitions only for a limited number of transitions between high-order FQHSs with intermediate strength. We discuss possible origins of the nonuniversal κ observed in our experiments.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2025

Lepton flavor asymmetries: from the early Universe to BBN

Large primordial lepton flavor asymmetries with almost vanishing total baryon-minus-lepton number can evade the usual BBN and CMB constraints if neutrino oscillations lead to perfect flavor equilibration. Solving the momentum averaged quantum kinetic equations (QKEs) describing neutrino oscillations and interactions, we perform the first systematic investigation of this scenario, uncovering a rich flavor structure in stark contradiction to the assumption of simple flavor equilibration. We find (i) a particular direction in flavor space, ∆ne ≃ – 2/3 (– 1)∆n μ for normal (inverted) neutrino mass hierarchy, in which the flavor equilibration is efficient and primordial asymmetries are essentially unconstrained, (ii) a minimal washout factor, ∆$n_{e}^{2}$| BBN ≤ 0.03 (0.016) ∑ α ∆$n_{α}^{2}$| ini yielding a conservative estimate for the allowed primordial asymmetries in a generic flavor direction, and (iii) particularly strong or weak washout if one of the initial flavor asymmetries vanishes due to non-adiabatic muon- or electron-driven MSW transitions. These results open up the possibility of a first-order QCD phase transition facilitated by large lepton asymmetries as well as baryogenesis from large and compensated ∆n e = ∆n μ asymmetries. Our systematic approach of deriving momentum averaged QKEs includes collision terms beyond the damping approximation, energy transfer between the neutrino and electron-photon plasma, and provides a fast and reliable way to investigate the impact of primordial lepton asymmetries at the time of BBN. We publicly release the Mathematica code COFLASY-M on https://github.com/mariofnavarro/COFLASY which solves the QKEs numerically.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2026

Oligoether-Functionalized PEDOT: Combining an EDOT Backbone with Polar Side Chains for Solution Processability and High Electrical Conductivity

Conjugated polymers functionalized with oligoether (OE)-based side chains are a key class of materials for various organic electronic applications, including transparent electrodes, thermoelectrics, electrochromic displays, and electrochemical transistors. Herein, we report a highly soluble OE-functionalized poly(3,4-ethylenedioxythiophene) (PEDOT) homopolymer, prepared by direct (hetero)arylation polymerization, which allows solution processing to yield films with comparable redox properties to oxidatively polymerized PEDOT. This polymer, PEDOT(OE3), when optimally oxidatively doped, reaches among the highest electrical conductivities of any OE-functionalized polymer and is comparable to more synthetically complex OE-functionalized polymers. X-ray scattering and spectroscopy were utilized to rationalize the transport properties resulting from varying the doping level. Comparison of PEDOT(OE3) to a series of OE-functionalized dioxythiophenes with varying amounts of 3,4-ethylenedioxythiophene units allows for a deeper understanding of structure–property relationships through charge-transport models. Ultimately, PEDOT(OE3) is shown to be a material with exceptional charge-transport properties and is promising for various applications.

36 MATERIALS SCIENCE↗
DOE OSTI2026

Expanding the Zinc Precursor Toolbox: A Comparative Study of Precursors for Thermal ALD of ZnO Thin Films

Atomic layer deposition (ALD) of zinc oxide (ZnO) has been widely researched using diethyl zinc (DEZ)-based methods. The significant importance of thin films of ZnO as transparent conductive oxides (TCO) in optoelectronic devices and photovoltaics warrants examining alternative Zn precursors for ZnO ALD as potential replacements for the pyrophoric DEZ. In this study, we investigated three alternative Zn precursors: Zn(EEKI)2, Zn(DMP)2, ZnEt(HMDS), in the process development for high-quality ZnO thin films and compared them to DEZ. The ALD processes were studied using in situ spectroscopic ellipsometry. The properties of the ALD ZnO films were characterized using ex situ X-ray photoelectron spectroscopy (XPS), Rutherford backscattering spectrometry and nuclear reaction analysis (RBS/NRA), X-ray diffraction (XRD), atomic force microscopy (AFM), transmission electron microscopy (TEM), and ultraviolet-visible (UV/Vis) spectrophotometry. These measurements confirmed the formation of pure, stoichiometric, and polycrystalline ZnO films using all four Zn precursors. Although the selected precursors are chemically diverse Zn compounds, they all yielded saturating ALD processes and high-quality ZnO thin films at 200 °C. This study highlights the potential benefits of alternative zinc precursors in designing ALD processes for ZnO thin films.

Obenlüneschloß, Jorit↗
DOE OSTI2025

Automated tabletop exfoliation and identification of monolayer graphene flakes

Over the past two decades, graphene has been intensively studied because of its remarkable mechanical, optical, and electronic properties. Initial studies were enabled by manual “Scotch Tape” exfoliation; nearly two decades later, this method is still widely used to obtain chemically pristine flakes of graphene and other 2D van der Waals materials. Unfortunately, the yield of large, pristine flakes with uniform thickness is inconsistent. Thus, significant time and effort are required to exfoliate and locate flakes suitable for fabricating multilayer van der Waals heterostructures. Here, we describe a relatively affordable tabletop device (the “eXfoliator”) that can reproducibly control key parameters and largely automate the exfoliation process. In a typical exfoliation run, the eXfoliator produces 3 or more large (≥ 400 μm 2 ) high-quality graphene monolayer flakes, allowing new users to produce such flakes at a rate comparable to manual exfoliation by an experienced user. Furthermore, we use an automated mapping system and a computer vision algorithm to locate candidate flakes. Our results provide a starting point for future research efforts to identify more precisely which parameters matter for the success of exfoliation and to optimize them.

47 OTHER INSTRUMENTATION↗
DOE OSTI2023

Validating the simulation of beam-ion charge exchange in MAST Upgrade

Abstract Simulation of the impact of charge-exchange (CX) reactions on beam ions in the Mega Amp Spherical Tokamak (MAST) Upgrade was compared to measurements carried out with a fission chamber (neutron fluxes) and a fast ion deuterium-alpha (FIDA) diagnostic. A simple model was developed to reconstruct the outer-midplane neutral density based on measurements of deuterium-alpha emission from edge neutrals, and on Thomson scattering measurements of electron density and temperature. The main computational tools used were the ASCOT orbit-following code and the FIDASIM code for producing synthetic FIDA signals. The neutral density reconstruction agrees qualitatively with SOLPS-ITER modelling and yields a synthetic passive FIDA signal that is consistent with measurement. When CX losses of beam ions are accounted for, predicted neutron emission rates are quantitatively more consistent with measurement. It was necessary to account for CX losses of beam ions in simulations to reproduce the measured passive FIDA signal quantitatively and qualitatively. The results suggest that the neutral density reconstruction is a good approximation, that CX with edge neutrals causes significant beam-ion losses in MAST Upgrade, typically 20% of beam power, and that the ASCOT fast-ion CX model can be used to accurately predict the redistribution and loss of beam ions due to CX.

Physics↗
DOE OSTI2021

Structured large-pore foams improve thermal performance of LiMIT-style liquid lithium PFC

As magnetically confined fusion devices improve, the conditions at the walls become increasingly intense. Plasma facing components (PFCs) must withstand these extreme heat and particle loads without damage or degradation. Liquid lithium PFCs are known to be quite resilient, and the presence of lithium also serves to improve plasma properties. The liquid metal infused trench (LiMIT) concept is an open surface liquid lithium PFC design that has been tested extensively at the University of Illinois and in fusion devices around the world. LiMIT utilizes thermoelectric magnetohydrodynamics (TEMHD) to passively drive liquid lithium flow. This work demonstrates an extension of the LiMIT trench geometry to three dimensions. Additively manufactured large pore metallic foams maintain TEMHD drive while drastically improving heat flux handling and resistance to lithium dryout, a phenomenon where locally high TEMHD forces depresses the lithium level and exposes underlying solid structure. COMSOL multiphysics modeling of the system yields insight into the forces at play in dryout development, and shows the 3D structures can eliminate dryout. Here, low heat proof-of-concept experimental testing of the system matches computational results, and high heat flux electron beam tests more than double the proven operational range of a LiMIT-style PFC, to 6.8 MW m –2 , with no indications of dryout or impending damage.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗