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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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DOE OSTI2022

Abundance of Major Cell Wall Components in Natural Variants and Pedigrees of Populus trichocarpa

The rapid analysis of biopolymers including lignin and sugars in lignocellulosic biomass cell walls is essential for the analysis of the large sample populations needed for identifying heritable genetic variation in biomass feedstocks for biofuels and bioproducts. In this study, we reported the analysis of cell wall lignin content, syringyl/guaiacyl (S/G) ratio, as well as glucose and xylose content by high-throughput pyrolysis-molecular beam mass spectrometry (py-MBMS) for >3,600 samples derived from hundreds of accessions of Populus trichocarpa from natural populations, as well as pedigrees constructed from 14 parents (7 × 7). Partial Least Squares (PLS) regression models were built from the samples of known sugar composition previously determined by hydrolysis followed by nuclear magnetic resonance (NMR) analysis. Key spectral features positively correlated with glucose content consisted of m/z 126, 98, and 69, among others, deriving from pyrolyzates such as hydroxymethylfurfural, maltol, and other sugar-derived species. Xylose content positively correlated primarily with many lignin-derived ions and to a lesser degree with m/z 114, deriving from a lactone produced from xylose pyrolysis. Models were capable of predicting glucose and xylose contents with an average error of less than 4%, and accuracy was significantly improved over previously used methods. The differences in the models constructed from the two sample sets varied in training sample number, but the genetic and compositional uniformity of the pedigree set could be a potential driver in the slightly better performance of that model in comparison with the natural variants. Broad-sense heritability of glucose and xylose composition using these data was 0.32 and 0.34, respectively. In summary, we have demonstrated the use of a single high-throughput method to predict sugar and lignin composition in thousands of poplar samples to estimate the heritability and phenotypic plasticity of traits necessary to develop optimized feedstocks for bioenergy applications.

09 BIOMASS FUELS↗
DOE OSTI2023

Azimuthal Correlations within Exclusive Dijets with Large Momentum Transfer in Photon-Lead Collisions

The structure of nucleons is multidimensional and depends on the transverse momenta, spatial geometry, and polarization of the constituent partons. Such a structure can be studied using high-energy photons produced in ultraperipheral heavy-ion collisions. The first measurement of the azimuthal angular correlations of exclusively produced events with two jets in photon-lead interactions at large momentum transfer is presented, a process that is considered to be sensitive to the underlying nuclear gluon polarization. This study uses a data sample of ultraperipheral lead-lead collisions at s NN = 5.02 TeV , corresponding to an integrated luminosity of 0.38 nb - 1 , collected with the CMS experiment at the LHC. The measured second harmonic of the correlation between the sum and difference of the two jet transverse momentum vectors is found to be positive, and rising, as the dijet transverse momentum increases. A well-tuned model that has been successful at describing a wide range of proton scattering data from the HERA experiments fails to describe the observed correlations, suggesting the presence of gluon polarization effects.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2020

Correlation of Spatiotemporal Dynamics of Polarization and Charge Transport in Blended Hybrid Organic–Inorganic Perovskites on Macro- and Nanoscales

Progress in flexible organic electronics necessitates a full understanding of how local inhomogeneities impact electronic and ionic conduction pathways and underlie macroscopic device characteristics. In this work, we used frequency- and time-resolved macro- and nanoprobe measurements to study spatiotemporal characteristics of multiscale charge transport dynamics in a series of ternary-blended hybrid organic inorganic perovskites (HOIPs) (MA 0.95– x FA x Cs 0.05 PbI 3 ). We show that A-site cation composition defines charge transport mechanisms across broad temporal (10 2 –10 –6 s) and spatial (millimeters–picometers) scales. Ab initio molecular dynamic simulations suggest that insertion of FA results in a dynamic lattice, improved ion transport, and dipole screening. We demonstrate that correlations between macro- and nanoscale measurements provide a pathway for accessing distribution of relaxation in nanoscale polarization and charge transport dynamics of ionically conductive functional perovskites.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Thermodynamic and Kinetic Modulation of Methylammonium Lead Bromide Crystallization Revealed by In Situ Monitoring

Hybrid organic–inorganic perovskite (HOIP) crystals are promising optoelectronic materials, but little is known about either the thermodynamic and kinetic controls on crystal growth or the underlying growth mechanism(s). Herein, we use fluid cell atomic force microscopy (AFM) and solution nuclear magnetic resonance (NMR) spectroscopy to investigate growth of the model HOIP crystal CH 3 NH 3 PbBr 3 (MAPbBr 3 ) and to determine how formic acid (HCOOH) modulates the thermodynamics and kinetics of growth. The results show that growth of MAPbBr 3 in dimethylformamide (DMF) proceeds through the classical pathway by the spreading of atomic crystal steps generated at screw dislocations on the {100} surface. Temperature dependent step velocity measurements demonstrate that with increasing concentration, HCOOH decreases both the solubility of MAPbBr 3 and the kinetic coefficient (b) of step movement. 1 H-NMR measurements indicate that HCOOH increases the lifetime of the methylammonium (MA + ) ions and promotes the association of MAPbBr 3 , thus tuning the solubility of the perovskite. HCOOH also alters the molecular tumbling motion and bulk diffusion of the MA + ions, possibly via H-bonding. Further, our findings establish a direct correlation between the mesoscale crystal growth kinetics and the molecular-scale interactions between organic additives and constituent ions, providing unprecedented insights for developing predictive syntheses of HOIP crystals with defined size, crystal habit and shape, and defect distribution.

36 MATERIALS SCIENCE↗
DOE OSTI2020

Thermodynamics of Metal Carbonates and Bicarbonates and Their Hydrates for Mg, Ca, Fe, and Cd Relevant to Mineral Energetics

The heats of formation of carbonate, bicarbonate and bicarbonate/hydroxide metal complexes and hydrated versions these complexes of Mg 2+ , Ca 2+ , Fe 2+ , and Cd 2+ are predicted from atomization energies using correlated molecular orbital theory at the CCSD(T) level extrapolated to the complete basis set limit following the Feller-Peterson-Dixon (FPD) approach. Using the calculated gas phase values and the available experimental solid state values, the cohesive energies of selected minerals were calculated. The gas phase decomposition energies into MO, CO 2 and H 2 O follow the order Mg ~ Ca > Cd ~ Fe, and correlate with the hardness of the metal +2 ions. Gas phase hydration energies show that the order is Mg > Fe > Ca ~ Cd. There are a number of bulk hydrated Mg and Ca complexes that occur as minerals but there are few if any for Fe and Cd, suggesting that a number of factors are important in determining the stability of the bulk mineral hydrates. The FPD heats of formation were used to benchmark a range of density functional theory exchange-correlation functionals, including those commonly used in solid state mineral calculations. None of the functionals provided chemical accuracy agreement (± 1 kcal/mol) with the FPD results The best functionals are ωB97X and ωB97X-D with mean average unsigned errors of 10 kcal/mol.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2026

Four-Dimensional Quasielastic Neutron Scattering (4D-QENS) Analysis of Correlated Ionic Conduction in Sr⁢Cl2

Methods of elucidating the mechanisms of fast-ion conduction in solid-state materials are pivotal for advancements in energy technologies such as batteries, fuel cells, sensors, and supercapacitors. In this study, we examine the ionic conduction pathways in single crystal Sr⁢Cl2, which is a fast-ion conductor above 900 K, using four-dimensional quasielastic neutron scattering (4D-QENS). We explore both coherent and incoherent neutron scattering at temperatures above the transition temperature into the superionic phase to explore the correlated motion of hopping anions. Refinements of the incoherent QENS yield residence times and jump probabilities between lattice sites in good agreement with previous studies, confirming that ionic hopping along nearest-neighbor directions is the most probable conduction pathway. However, the coherent QENS reveals evidence of de Gennes narrowing, indicating the importance of ionic correlations in the conduction mechanism. This highlights the need for improvements both in the theory of ionic transport in fluorite compounds and the modeling of coherent 4D-QENS in single crystals.

Coles, Jared [Materials Science Division, Argonne ↗
DOE OSTI2020

Angle-resolved nonresonant two-photon single ionization of argon using 9.3-eV photons produced via high-order harmonic generation

Here we present an experimental study on the photoionization dynamics of nonresonant one-color two-photon single valence ionization of neutral argon atoms. Using 9.3-eV photons produced via high harmonic generation and a three-dimensional momentum imaging spectrometer, we detect the photoelectrons and ions produced from nonresonant two-photon ionization in coincidence. Photoionization from the $3p$ orbital produces a photoelectron scattering wave function with $p$- and $f$-partial-wave components, which interfere and result in a photoelectron angular distribution with peak amplitude perpendicular to the vacuum ultraviolet polarization. The comparison between the present results and the two previous sets of theoretical calculations [Phys. Rev. A 44, 324 (1991), and J. Phys. B: At. Mol. Phys. 16, 2737 (1983)] indicates that electron-electron correlation contributes appreciably to the two-photon ionization dynamics.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

How threshold effects in spectroscopic factors influence heavy-ion knockout reactions

A two-decade-old puzzle in heavy-ion one-nucleon knockout reactions is the strong correlation between the reduction factor R S = σ exp /σ t h and the Fermi surface asymmetry ΔS. Theoretical cross sections typically rely on spectroscopic factors (SFs) from shell model (SM) calculations, which neglect continuum coupling effects. Here, we employ the Gamow shell model (GSM), which explicitly incorporates continuum coupling, to compute SFs for p-shell nuclei and predict corresponding theoretical cross sections. Systematic calculations demonstrate that using GSM-derived SFs substantially reduces discrepancies between theoretical and experimental results. This improvement is particularly significant for deeply bound nucleon knockout in nuclei near the dripline, where traditional SM-based calculations fall short. As a result, using GSM SFs, the ratio R s exhibits no pronounced dependence on ΔS. Furthermore, both the ratio of GSM SFs to SM SFs and their corresponding reaction cross sections ratios exhibit a strong ΔS dependence. We have also compared GSM SFs and cross sections with those from the no-core shell model calculations, giving a similar pronounced sensitivity to ΔS. Detailed analysis attributes these correlations to threshold effects for SFs in weakly bound systems. Overall, incorporating continuum coupling via GSM enhances the reliability of SF predictions for exotic, weakly bound nuclei and provides key insights toward resolving the enduring puzzle in heavy-ion knockout reactions from a nuclear structure perspective.

Gamow shell model↗
DOE OSTI2023

Rapid screening of secondary aromatic metabolites in Populus trichocarpa leaves

Abstract Background High-throughput metabolomics analytical methodology is needed for population-scale studies of bioenergy-relevant feedstocks such as poplar ( Populus sp.). Here, the authors report the relative abundance of extractable aromatic metabolites in Populus trichocarpa leaves rapidly estimated using pyrolysis-molecular beam mass spectrometry (py-MBMS). Poplar leaves were analyzed in conjunction with and validated by GC/MS analysis of extracts to determine key spectral features used to build PLS models to predict the relative composition of extractable aromatic metabolites in whole poplar leaves. Results The Pearson correlation coefficient for the relative abundance of extractable aromatic metabolites based on ranking between GC/MS analysis and py-MBMS analysis of the Boardman leaf set was 0.86 with R 2 = 0.76 using a simplified prediction approach from select ions in MBMS spectra. Metabolites most influential to py-MBMS spectral features in the Clatskanie set included the following compounds: catechol, salicortin, salicyloyl-coumaroyl-glucoside conjugates, α-salicyloylsalicin, tremulacin, as well as other salicylates, trichocarpin, salicylic acid, and various tremuloidin conjugates. Ions in py-MBMS spectra with the highest correlation to the abundance of extractable aromatic metabolites as determined by GC/MS analysis of extracts, included m/z 68, 71, 77, 91, 94, 105, 107, 108, and 122, and were used to develop the simplified prediction approach without PLS models or a priori measurements. Conclusions The simplified py-MBMS method is capable of rapidly screening leaf tissue for relative abundance of extractable aromatic secondary metabolites to enable prioritization of samples in large populations requiring comprehensive metabolomics that will ultimately inform plant systems biology models and advance the development of optimized biomass feedstocks for renewable fuels and chemicals.

09 BIOMASS FUELS↗
DOE OSTI2025

Expanding Configurational Complexity through Dipole Dilution in Pseudohalide Argyrodite Ion Conductors

The advantageous properties of (pseudo)halide argyrodite ion conductors of the formula Li 6 PS 5 X (X = Cl – , Br – , I – , CN – ) have motivated extensive studies of their structure-transport relationships, particularly as they pertain to the role of atomic site disorder. The argyrodite structure can accommodate additional configurational complexity to promote ion transport via extended three-anion site mixing and the potential for orientational disorder of molecular anions. In this work, we explore a ternary anion system including the cyanide anion, expanding site disorder and introducing dipolar orientations as an additional degree of freedom. We prepared the series Li 6 PS 5 (CN) 1–x Br x , in which the dipolar cyanide anions are systematically diluted with bromide. We find that anion disorder, as determined by synchrotron and neutron diffraction and quantified by configurational entropy (S config ), is correlated with lowered activation barriers and increased lithium ion conductivity. We propose that S config describes the electrostatic heterogeneity of the Li environments, flattening the energetic landscape for ion transport. While anion substitution strongly impacts the activation barrier for transport, the temperature-independent Arrhenius prefactor does not follow the same trend. Through heat-capacity measurements of attempt frequency and deconvolution of terms within the prefactor, we rationalize the apparent decoupling of activation energy and prefactor to strong cyanide-lithium interactions that increase the entropy of migration. Together, these results expand the structure–property relationships in the argyrodite family to encompass multiple facets of disorder and the subsequent impact on lithium ion transport.

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

Influence of aluminum incorporation and aqueous conditions on metal ion release of high-Ni transition metal oxide nanomaterials

Developing a materials perspective of how to control the degradation and negative impact of complex metal oxides requires an integrated understanding of how these nanomaterials transform in the environment and interact with biological systems. Doping with aluminum is known to stabilize oxide materials, but has not been assessed cohesively from synthesis to environmental fate and biological impact. In the present study, the influence of aluminum doping on metal ion release from transition metal oxides was investigated by comparing aqueous transformations of lithium nickel cobalt aluminum oxide (LiNi 0.82 Co 0.15 Al 0.03 O 2 ; NCA) and lithium nickel cobalt oxide (LiNi 0.80 Co 0.20 O 2 ; NC) nanoparticles and by calculating the energetics of metal release using a density functional theory (DFT) and thermodynamics method. Two model environmental organisms were used to assess biological impact, and metal ion release was compared for NCA and NC nanoparticles incubated in their respective growth media: moderately hard reconstituted water (MHRW) for the freshwater invertebrate Daphnia magna (D. magna) and minimal growth medium for the Gram-negative bacterium Shewanella oneidensis MR-1 (S. oneidensis). Further, the amount of metal ions released was reduced for NCA compared to NC in MHRW, which correlated to changes in the modeled energetics of release upon Al substitution in the lattice. In minimal medium, metal ion release was approximately an order of magnitude higher compared to MHRW and was similar to the stoichiometry of the bulk nanoparticles for both NCA and NC. Interpretation of the release profiles and modeling indicated that the increase in total metal ion release and the reduced influence of Al doping arises from lactate complexation of metal ions in solution. The relative biological impacts of NC and NCA exposure for both S. oneidensis and D. magna were consistent with the metal release trends observed for minimal medium and MHRW, respectively. Together, these results demonstrate how a combined experimental and computational approach provides valuable insight into the aqueous transformations and biological impacts of complex metal oxide nanoparticles.

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

RF antenna helicity dependent particle heating in a helicon source

Experiments have demonstrated that ion phenomena, such as the lower hybrid resonance, play an important role in helicon source operation. Damping of the slow branch of the bounded whistler wave at the edge of a helicon source (i.e. the Trivelpiece-Gould mode) has been correlated with the creation of energetic electrons, heating of ions at the plasma edge, and anisotropic ion heating. Here we present ion velocity distribution function measurements, electron density and temperature measurements, and magnetic fluctuation measurements on both sides of an m = |1| helical antenna in a helicon source as a function of the driving frequency, magnetic field strength, and magnetic field orientation relative to the antenna helicity. Significant electron and ion heating (up to two times larger) occurs on the side of the antenna consistent with the launch of the m = +1 mode. The electron and ion heating occurs within one electron skin depth of the plasma edge, where slow wave damping is expected. The source parameters for enhanced particle heating are also consistent with lower hybrid resonance effects, which can only occur for Trivelpiece-Gould wave excitation.

wave modes↗
DOE OSTI2025

Acceptance dependence of factorial cumulants, long-range correlations, and the antiproton puzzle

We analyze joint factorial cumulants of protons and antiprotons in relativistic heavy-ion collisions and point out that they obey the scaling Ĉnmp,p¯∝〈Np〉n〈Np¯〉m as a function of acceptance when only long-range correlations are present in the system, such as global baryon conservation and volume fluctuations. This hypothesis can be directly tested experimentally without the need for corrections for volume fluctuations. We show that if correlations among protons and antiprotons are driven by global baryon conservation and volume fluctuations only, the equality Ĉ2p/〈Np〉2=Ĉ2p¯/〈Np¯〉2 holds for large systems created in central collisions. We point out that the experimental data of the STAR Collaboration from phase I of the Relativistic Heavy Ion Collider (RHIC) beam energy scan (BES) are approximately consistent with the scaling Ĉnmp,p¯∝〈Np〉n〈Np¯〉m, but the normalized antiproton correlations are stronger than those of protons, −Ĉ2p¯/〈Np¯〉2>−Ĉ2p/〈Np〉2. Existing theoretical baselines, based on global baryon conservation and volume fluctuations, cannot explain the data, which we refer to as the antiproton puzzle. We also discuss high-order factorial cumulants which can be measured with sufficient precision within phase II of RHIC-BES.

Bzdak, Adam↗
DOE OSTI2021

Bulk properties and multi-particle correlations in large and small systems

Charged particle production is calculated in a hybrid framework consisting of the IP-Glasma initial state, Music viscous relativistic fluid dynamics, and the UrQMD microscopic hadronic cascade. Using one set of parameters, we compute observables for a large variety of collision systems. Furthermore, we compare to experimental data in p+p, p+Pb, Xe+Xe, Au+Au and Pb+Pb collisions at various energies, and make predictions for potential O+O runs at RHIC and LHC.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2024

Linear Boltzmann transport for jet propagation in the quark-gluon plasma: Inelastic processes and jet modification

A linear Boltzmann transport (LBT) Monte Carlo model has been developed to describe jet propagation and interaction with the quark-gluon plasma (QGP) in relativistic heavy-ion collisions. A complete set of elastic-scattering processes and medium-induced gluon emissions based on the higher-twist formalism are incorporated for both jet shower and medium recoil partons. It has been employed to describe experimental data on large transverse momentum hadron and jet spectra, correlation and jet substructures in high-energy heavy-ion collisions. Here, we document in detail the structure of the model and validation of the Monte Carlo implementations of the physics processes in LBT, in particular, the inelastic process of medium-induced gluon radiation. We carry out a comprehensive examination of the jet-medium interaction as implemented in LBT through energy loss and momentum broadening of a single hard parton, the energy and transverse momentum transfer from leading partons to medium-induced gluons and jet-induced medium excitation, and medium modification of reconstructed jets in a static and uniform medium. With realistic and event-by-event hydrodynamic medium in heavy-ion collisions, we compute and compare with experimental data on the jet cone-size dependence of the single inclusive jet suppression at both the BNL Relativistic Heavy-Ion Collider (RHIC) and the CERN Large Hadron Collider (LHC), the dijet asymmetry at the LHC and γ-jet correlation at RHIC. Effects of medium-induced gluon emissions and jet-induced medium excitation on jet observables are systematically examined. Rescatterings of the radiated gluons and recoil partons with the QGP are found essential to account for the enhancement of soft particle yield toward the edge of the jet cone.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2021

QCD thermalization: Ab initio approaches and interdisciplinary connections

Heavy-ion collisions at BNL's Relativistic Heavy Ion Collider and CERN's Large Hadron Collider provide strong evidence for the formation of a quark-gluon plasma, with temperatures extracted from relativistic viscous hydrodynamic simulations shown to be well above the transition temperature from hadron matter. Outstanding problems in QCD include how the strongly correlated quark gluon matter forms in a heavy-ion collision, its properties off-equilibrium, and the thermalization process in the plasma. In this work, we review the theoretical progress in this field in weak coupling QCD effective field theories and in strong coupling holographic approaches based on gauge-gravity duality. We outline the interdisciplinary connections of different stages of the thermalization process to non equilibrium dynamics in other systems across energy scales ranging from inflationary cosmology, to strong field QED, to ultracold atomic gases, with emphasis on the universal dynamics of non-thermal and hydrodynamic attractors. We survey measurements in heavy-ion collisions that are sensitive to the early non-equilibrium stages of the collision and discuss the potential for future measurements. We summarize the current state-of-the art in thermalization studies and identify promising avenues for further progress.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

Photoelectron–residual-ion interaction in angle-resolved streaked shake-up ionization of helium

Streaked photoelectron emission spectra access the correlated dynamics of photoelectrons and residual target electrons with attosecond temporal resolution. Here, we calculated ab initio single-ionization spectra for photoemission from helium atoms by colinearly polarized ultrashort XUV and assisting few-femtosecond IR pulses. Distinguishing direct and shake-up ionization resulting in ground-state and excited (𝑛 = 2, 3) He + residual ions, respectively, we examined the effects of the correlated photoemission dynamics on the photoelectron phase accumulation as a function of the observable photoelectron detection direction and kinetic energy and XUV–IR pulse delay. We tracked the dynamical evolution of the residual ion in relative streaked photo- emission delays and found dominant contributions for shake-up emission from the residual-ion–photoelectron interaction. These are in very good and fair agreement, respectively, for 𝑛 = 2 and 𝑛 = 3 shake-up photoemission along the pulse-polarization directions, with previous experimental and theoretical investigations [Ossiander et al ., Nat. Phys. 13, 280 (2017)] and reveal a strong photoemission-direction dependence for shake-up ionization due to the coupling between the photoelectron and evolving residual-ion charge distribution in the IR-laser field.

Stark effect↗
DOE OSTI2020

The electronic structure of the actinide oxides and their singly and doubly charged cations: A ligand field approach

Abstract Ligand field theory (LFT) calculations of energy levels were performed for the neutral actinide monooxides ( An O) and their singly and doubly ionized cations ( An O + and An O 2+ ) by treating the molecular electronic states as An m+ free‐ion energy levels (where An ∈ Th through Lr and m = 1, 2, 3, or 4) perturbed by the electric field of O 2− or O − . LFT parameters obtained from fits to the energy levels of ThO, ThO + , UO, and UO + were used to compute molecular energy levels for the lowest energy (maximum S c , maximum L c ) 5 f ‐core states of An 4+ , An 3+ , An 2+ , and An + for the majority of the An 4+ O 2− , An 3+ O − , An 3+ O 2− , An 2+ O − , An 2+ O 2− , and An + O − electronic configurations. Simple linear relationships enabled predictions of the dissociation energies for An O, An O + and An O 2+ (where An ∈ Bk through Lr) and ionization energies for An O and An O + (where An ∈ Bk through Lr), mainly based on recent accurate experimental data for the ionization energies of An atoms (where An ∈ Fm, Md, No, and Lr) and correlations with the energetics of the atoms and ions.

Kaledin, Leonid A.↗