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At least 1,207 records · Page 67
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Influence of elevated temperature and oxygen on the capture of radioactive iodine by silver functionalized silica aerogel

Reprocessing is considered a competent strategy for spent nuclear fuel management, yet radioiodine ( 129 I) is emitted in reprocessing off-gas as a hazardous byproduct. Silver functionalized silica aerogel (Ag 0 -aerogel), a promising iodine capture material, experiences a reduction in its capacity after prolonged exposure to off-gas components at elevated temperatures, a phenomenon termed as aging. To fully understand this process, we isolated the contribution of each aging factor, exposing Ag 0 -aerogel samples to N 2 and dry air gas streams, respectively, at 150 °C for different time periods. Aged samples were loaded with I 2 to examine the capacity change and comprehensively characterized to investigate the evolution of their properties. Results show that temperature alone did not alter Ag 0 -aerogel's capacity but triggered Ag 0 nanoparticles sintering and generated organic sulfur species. The presence of O 2 reduced the capacity by ~20 %, causing (i) formation of silver sulfide (Ag 2 S) crystals and (ii) oxidation of Ag-thiolate (Ag-S-r) to Ag sulfonate (Ag-SO 3 -r). Given that Ag 2 S readily adsorbs I 2 , the formation of Ag-SO 3 -r is the major inhibitor for iodine adsorption. This hypothesis was supported by density functional theory (DFT) simulations. These findings unraveled key mechanisms of Ag 0 -aerogel aging, which are useful in the development of materials that withstand realistic spent-nuclear-fuel-reprocessing off-gas conditions.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2026

Measurements of excitation functions and photoneutron cross sections of 96,98,99,104 Ru and 100 Mo

Photoneutron cross sections were extracted for isotopes of ruthenium and molybdenum on natural abundance targets via a reduced chi-squared analysis on excitation functions, or activation yields, as function of electron beam energy. Bremsstrahlung photons were produced via an electron linear accelerator and a tungsten radiator at the Idaho Accelerator Center. A total of 16 irradiations were performed with electron beam energies ranging from approximately 8 MeV to 23 MeV. Induced radioactivity was measured using a high purity germanium detector. The cross sections were extracted assuming a three parameter Lorentzian fit with a smooth truncated rise at reaction threshold.

07 - ISOTOPES AND RADIATION SOURCES↗
DOE OSTI2020

Jet shapes and fragmentation functions in Au+Au collisions at s NN = 200 GeV in STAR

The STAR Collaboration reports measurements of differential jet shapes and semi-inclusive jet fragmentation functions in Au+Au collisions at with the STAR detector at RHIC. Additionally, jet shapes, which represent the radial distribution of momentum carried by constituents, are measured differentially for (1) the charged particles transverse momentum and (2) the jet azimuthal angle relative to the second-order event plane. Based on the semi-inclusive population of jets recoiling from a high transverse momentum trigger hadron, jet fragmentation functions in 40-60% central heavy-ion collisions are measured, and compared to those in PYTHIA simulations for pp collisions.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2020

A parallel strategy for density functional theory computations on accelerated nodes

Using the Löwdin orthonormalization of tall-skinny matrices as a proxy-app for wavefunction-based Density Functional Theory solvers, we investigate a distributed memory parallel strategy focusing on Graphics Processing Unit (GPU)-accelerated nodes as available on some of the top ranked supercomputers at the present time. Here we present numerical results in the strong limit regime, as it is particularly relevant for First-Principles Molecular Dynamics. We also examine how matrix product-based iterative solvers provide a competitive alternative to dense eigensolvers on GPUs, allowing to push the strong scaling limit of these computations to a larger number of distributed tasks. Our strategy, which relies on replicated Gram matrices and efficient collective communications using the NCCL library, leads to a time-to-solution under 0.5 s for the Löwdin orthonormalization of a tall-skinny matrix of 3000 columns on Summit at Oak Ridge Leadership Facility (OLCF). Given the similarity in computational operations between one iteration of a DFT solver and this proxy-app, this shows the possibility of solving accurately the DFT equations well under a minute for 3000 electronic wave functions, and thus perform First-Principles molecular dynamics of physical systems much larger than traditionally solved on CPU systems.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2021

Reweighting the Sivers function with jet data from STAR

The reweighting procedure that using Bayesian statistics incorporates the information contained in a new data set, without the need of re-fitting, is applied to the quark Sivers function extracted from Semi-Inclusive Deep Inelastic Scattering (SIDIS) data. We exploit the recently published single spin asymmetry data for the inclusive jet production in polarized pp collisions from the STAR Collaboration at RHIC, which cover a much wider x region compared to SIDIS measurements. The reweighting method is extended to the case of asymmetric errors and the results show a remarkable improvement of the knowledge of the quark Sivers function.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2022

Spectral function of fermions in a highly occupied non-Abelian plasma

We develop a method to obtain fermion spectral functions non-perturbatively in a non-Abelian gauge theory with high occupation numbers of gauge fields. After recovering the free field case, we extract the spectral function of fermions in a highly occupied non-Abelian plasma close to its non-thermal fixed point, i.e., in a self-similar regime of the non-equilibrium dynamics. We find good agreement with hard loop perturbation theory for medium-induced masses, dispersion relations and quasiparticle residues. We also extract the full momentum dependence of the damping rate of the collective excitations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2025

Collins function for pion-in-jet production in polarized pp collisions: a test of universality and factorization

We present an updated study of the Collins azimuthal asymmetries for pion-in-jet production in polarized pp collisions. To this aim, we employ a recent extraction of the transversity and Collins fragmentation functions from semi-inclusive deep inelastic scattering and e + e - annihilation into hadron pairs processes, obtained within a simplified transverse momentum dependent (TMD) approach at leading order in the strong coupling constant α s . In the present case we adopt a collinear configuration for the initial state, keeping transverse momentum effects only in the fragmentation mechanism. Our theoretical estimates, when compared against 200 GeV and 510 GeV data from the STAR Collaboration, show a generally good agreement for the distributions in the transverse momentum of the jet, the pion longitudinal momentum fraction and its transverse momentum with respect to the jet direction. While not being a proof, due the assumptions and limitations behind the entire approach, these findings corroborate the hypothesis of TMD factorization for such processes as well as of the universality of the Collins function and, once again, of a reduced impact of the proper TMD evolution on azimuthal asymmetries. We will also present predictions based on an extraction of the Collins and transversity distributions where information from data on single spin asymmetry for inclusive pion production in p ↑ p collisions is included through a Bayesian reweighting procedure.

Azimuthal asymmetries↗
DOE OSTI2023

Small bimetallic clusters Agn-1M (M = Au, Co, Cu, Ni, Pd, Pt; n = 3, 9, 15): Density functional theory and genetic algorithm

We investigated the effect of size and composition on the properties of bimetallic nanoclusters. The geometric structures, stabilities, and electronic properties of size-selected Ag n-1 M (M = Au, Co, Cu, Ni, Pd, Pt; n = 3, 9, 15) bimetallic nanoclusters are systematically analyzed using spin-polarized density functional theory (DFT) within the generalized gradient approximation (GGA). We determine the most stable geometries for these clusters using a genetic algorithm (GA) in combination with DFT. Our results show that doping pure silver clusters with an M atom (transition metal), referred to as a “guest atom”, increases the stability as compared to pure Ag n (n = 3, 9, 15) clusters. The results for various properties including formation energy per atom, electronic structure, magnetic moments, and vibrational density of states (VDOS) are evaluated as a function of both size and composition of the system. The adsorption of selected bimetallic clusters on hydroxylated alumina substrate shows weak binding and minor changes in geometric properties except for Ag 8 Pt.

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

Understanding How Ligand Functionalization Influences CO2 and N2 Adsorption in a Sodalite Metal–Organic Framework

In this work, a detailed study is conducted to understand how ligand substitution influences the CO2 and N2 adsorption properties of two highly crystalline sodalite metal–organic frameworks (MOFs) known as Cu–BTT (BTT–3 = 1,3,5-benzenetristetrazolate) and Cu–BTTri (BTTri–3 = 1,3,5-benzenetristriazolate). The enthalpy of adsorption and observed adsorption capacities at a given pressure are significantly lower for Cu–BTTri compared to its tetrazole counterpart, Cu–BTT. In situ X-ray and neutron diffraction, which allow visualization of the CO2 and N2 binding sites on the internal surface of Cu–BTTri, provide insights into understanding the subtle differences. As expected, slightly elongated distances between the open Cu2+ sites and surface-bound CO2 in Cu–BTTri can be explained by the fact that the triazolate ligand is a better electron donor than the tetrazolate. The more pronounced Jahn–Teller effect in Cu–BTTri leads to weaker guest binding. The results of the aforementioned structural analysis were complemented by the prediction of the binding energies at each CO2 and N2 adsorption site by density functional theory calculations. In addition, variable temperature in situ diffraction measurements shed light on the fine structural changes of the framework and CO2 occupancies at different adsorption sites as a function of temperature. Finally, simulated breakthrough curves obtained for both sodalite MOFs demonstrate the materials’ potential performance in dry postcombustion CO2 capture. The simulation, which considers both framework uptake capacity and selectivity, predicts better separation performance for Cu–BTT. The information obtained in this work highlights how ligand substitution can influence adsorption properties and hence provides further insights into the material optimization for important separations.

adsorption capacities↗
DOE OSTI2021

Probing the Chemical Kinetics of Minimalist Functional Group Gasoline Surrogates

We report surrogate mixtures are routinely used for understanding gasoline fuel combustion in engine simulations. The general trend in surrogate formulation has been to increase the number of fuel components in a mixture to better emulate real fuel properties. Recently, a new surrogate design strategy based on functional group analysis of real gasolines was proposed using a minimal number of species [minimalist functional group (MFG)-approach]. MFG surrogates (having just one or two components) could experimentally capture the ignition delay time (IDT), threshold sooting index, and smoke point of different gasoline fuels with hundreds of components. However, other combustion characteristics were not explored, and kinetic modeling of MFG surrogates was not reported. These aspects are addressed in this paper, where the combustion behavior of MFG surrogates for various gasolines was assessed by simulating IDT, jet-stirred reactor oxidation, and premixed laminar flame speeds using chemical kinetic modeling. MFG simulations were compared with experimental data of the real gasolines as well as with the more complex multicomponent (five to nine species) surrogates. This study reveals that binary MFG surrogate mixtures are capable of accurately simulating the combustion behavior of more complex gasoline fuels with hundreds of components.

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

Unmasking Static Correlation Error in Hybrid Kohn–Sham Density Functional Theory

To uncover the way Hartree–Fock exchange brings static correlation error into hybrid Kohn–Sham density functional theory, we compare the potential energy curves of four diatomic molecules, namely, H 2 , F 2 , HF, and NaF, using both restricted and unrestricted Kohn–Sham theory. Here, we find that increasing the percentage of Hartree–Fock exchange significantly increases the static correlation error because Hartree–Fock exchange replaces the ability of local exchange in density functionals to account for the localization effects associated with static correlation.

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

Semi-Automated Creation of Density Functional Tight Binding Models through Leveraging Chebyshev Polynomial-Based Force Fields

Density functional tight binding (DFTB) is an attractive method for accelerated quantum simulations of condensed matter due to its enhanced computational efficiency over standard density functional theory (DFT) approaches. However, DFTB models can be challenging to determine for individual systems of interest, especially for metallic and interfacial systems where different bonding arrangements can lead to significant changes in electronic states. In this regard, we have created a rapid-screening approach for determining systematically improvable DFTB interaction potentials that can yield transferable models for a variety of conditions. Our method leverages a recent reactive molecular dynamics force field where many-body interactions are represented by linear combinations of Chebyshev polynomials. This allows for the efficient creation of multi-center representations with relative ease, requiring only a small investment in initial DFT calculations. Here, we have focused our workflow on TiH 2 as a model system and show that a relatively small training set based on unit-cell-sized calculations yields a model accurate for both bulk and surface properties. Our approach is easy to implement and can yield reliable DFTB models over a broad range of thermodynamic conditions, where physical and chemical properties can be difficult to interrogate directly and there is historically a significant reliance on theoretical approaches for interpretation and validation of experimental results.

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

GronOR: Scalable and Accelerated Nonorthogonal Configuration Interaction for Molecular Fragment Wave Functions

GronOR is a program package for nonorthogonal configuration interaction calculations. Electronic wave functions are constructed in terms of antisymmetrized products of multiconfiguration molecular fragment wave functions. The computational complexity of the nonorthogonal methodologies implemented in GronOR applied to large molecular assemblies requires a design that takes full advantage of massively parallel supercomputer architectures and accelerator technologies. This work describes the implementation strategy and resulting performance characteristics. In addition to parallelization and acceleration, the software development strategy includes aspects of fault resiliency and heterogeneous computing. The program was designed for large-scale supercomputers but also runs effectively on small clusters and workstations for small molecular systems. GronOR is available as open source to the scientific community.

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

Density Functional Tight-Binding Models for Band Structures of Transition-Metal Alloys and Surfaces across the d -Block

First-principles electronic structure simulations are an invaluable tool for understanding chemical bonding and reactions. While machine-learning models such as interatomic potentials significantly accelerate the exploration of potential energy surfaces, electronic structure information is generally lost. Particularly in the field of heterogeneous catalysis, simulated electron band structures provide fundamental insights into catalytic reactivity. This ab initio knowledge is preserved in semiempirical methods such as density functional tight binding (DFTB), which extend the accessible computational length and time scales beyond first-principles approaches. In this paper here we present Shell-Optimized Atomic Confinement (SOAC) DFTB electronic-part-only parametrizations for bulk and surface band structures of all d-block transition metals that enable efficient predictions of electronic descriptors for large structures or high-throughput studies on complex systems outside the computational reach of density functional theory.

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

An Accurate, Affordable Density Functional Tight-Binding Model for Excited State Hydrocarbon Polymer Molecular Dynamics

We have developed a density functional tight-binding model for hydrocarbon excited state dynamics by referencing to high-level electronic structure theory and incorporating a many-body repulsive energy. We then validate our model against n-octane geometry optimizations, bond dissociation scans, and vibrational frequencies. Our model is approximately 10 3 times more efficient than hybrid time-dependent density functional theory calculations with comparable accuracy. In conclusion, our efforts enable longer timescale excited state simulations of photochemistry and scattering of incident radiation.

Chemical calculations↗
DOE OSTI2023

Graphically Contracted Function Construction with the Recursive Pairwise Merge Algorithm

A new implementation of a recursive pairwise merge algorithm to construct a GCF from a list of CSF expansion coefficients is presented. The essential new feature is the preallocation of some work arrays used within the intermediate steps of the merge procedure. This results in roughly an order of magnitude improvement in overall efficiency and also approximately eliminates a factor of n, the molecular orbital dimension, from the original implementation. Initial application of this merge procedure to a series of H m molecules shows that the GCF wave functions can be represented well both with delocalized canonical Hartree-Fock orbitals and with localized molecular orbitals. Finally, for a given wave function complexity, as measured by the average facet count, $\bar{\text {f}}$, the delocalized Hartree-Fock orbitals show smaller errors for small $\bar{\text {f}}$ values, while the localized orbitals show smaller errors for larger $\bar{\text {f}}$ values.

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

Adsorbate Partition Functions via Phase Space Integration: Quantifying the Effect of Translational Anharmonicity on Thermodynamic Properties

A new method for computing anharmonic thermophysical properties for adsorbates on metal surfaces is presented. Classical Monte Carlo phase space integration is performed to calculate the partition function for the motion of a hydrogen atom on Cu(111). Here, a minima-preserving neural network potential energy surface is used within the integration routine. Two different sampling schema for generating the training data are presented, and two different density functionals are used. The results are benchmarked against direct state counting results by using discrete variable representation. The phase space integration results are in excellent quantitative agreement with the benchmark results. Additionally, both the discrete variable representation and the phase space integration results confirm that the motion of H on Cu(111) is highly anharmonic. The results were applied to calculate the free energy of dissociative adsorption of H 2 and the resulting Langmuir isotherms at 400, 800, and 1200 K in a partial pressure range of 0–1 bar. It shows that the anharmonic effects lead to significantly higher predicted surface site fractions of hydrogen.

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

Leveraging Sequential Doping of Semiconducting Polymers to Enable Functionally Graded Materials for Organic Thermoelectrics

With the ability to modulate electronic properties through molecular doping coupled with ease in processability, semiconducting polymers are at the forefront in enabling organic thermoelectric devices for thermal energy management. In contrast to uniform thermoelectric material properties, an alternative route focuses on functionally graded materials (FGMs) where one spatially controls and optimizes transport properties across the length of a thermoelectric material. While primarily studied in the context of inorganic materials, the concept of FGMs for organic thermoelectrics has not been explored. Herein, we introduce how molecular doping of semiconducting polymers enables spatial compositional control of thin-film FGMs. Specifically, we utilize sequential vapor doping of poly[2,5-bis(3-tetradecylthiophen-2-yl) thieno [3,2-b]thiophene] (PBTTT) with the small molecule acceptor 2,3,5,6-tetrafluoro-7,7,8,8-tetracyanoquinodimethane (F4TCNQ) to fabricate the simplest form of FGMs – double- segmented thin films. The two thin-film segments are of equal length (7.5 mm), but each set to different doping levels. Our study focuses on understanding the thermoelectric properties (Seebeck coefficient, α, and electronic conductivity, σ) and structural properties (through X-ray scattering, UV-vis-NIR spectroscopy, and Raman spectroscopy) within and across the two segments. We observe the presence of a small diffuse interfacial region of 0.5 – 1 mm between the two segments where the doping level and transport properties vary continuously. Despite the diffuse interface, the measured effective Seebeck coefficient (αeff) across the two segments is simply the average of α within each segment. Importantly, this experimental result is consistent with reported mathematical models describing αeff in graded thermoelectric materials. Finally, our results demonstrate the facile fabrication and characterization of functionally graded organic thermoelectric materials, providing guidelines for further development on more complex FGMs.

36 MATERIALS SCIENCE↗