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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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All sourcesNASA NTRSDOE OSTI
DOE OSTI2020

Three-Dimensional Patterning of Nanoparticles by Molecular Stamping

Directing the formation of nanoscale architectures from nanoparticles is one of the key challenges in designing nanomaterials with prescribed functions. Atomic systems, given their ability to form molecules and crystals via directional chemical bonds, provide an inspiration for establishing approaches where nanoparticles with designed anisotropic binding modalities can be assembled into nanoscale architectures. However, fabricating such nanoparticles has been challenging due to their small dimensions and limited ways for site-specific control of their surface. To this end, we present a Molecular Stamping (MOST) approach to pattern DNA-coated nanoparticles with molecules at the predefined positions on a nanoparticle surface. This patterning is realized by use of a rigid and coordinative DNA frame as a molecular stamping apparatus (MOST App). The MOST App transfers multiple types of molecular “inks”, DNA sequences, onto nanoparticle surface and fixes these molecular inks into place to form a designed pattern. After a nanoparticle release from MOST App, it possesses single-molecule patches that can provide anisotropic bonds with distinctive affinities. We further use these stamped nanoparticles to assemble prescribed clusters, whose structure is determined by the locations of patches. Using electron microscopy and tomographic methods, we investigate the efficiency of cluster formation and the resulting spatial arrangements of nanoparticles. The presented approach provides a single-molecule and spatiallydetermined control over nanoparticle functionalization for creating nanoparticles with designed placement of different molecules and for realizing a rational fabrication of nanomaterial architectures.

77 NANOSCIENCE AND NANOTECHNOLOGY↗
DOE OSTI2023

Causal interaction in high frequency turbulence at the biosphere–atmosphere interface: Structural behavior

High-frequency (e.g., 10 Hz) eddy covariance measurements are typically used to estimate fluxes at the land–atmosphere interface at timescales of 15–60 min. These multivariate data contain information about the interdependency at high frequency between the interacting variables such as wind, humidity, temperature, and CO 2⁠ . We use data at 10 Hz from an eddy covariance instrument located at 25 m above agricultural land in the Midwestern US, which offers an opportunity to move beyond the traditional spectral analyses to explore causal dependency among variables. In this study, we quantify the structure of inter-dependencies of interacting variables at high frequency represented by a directed acyclic graph (DAG). We compare DAGs to investigate changes in structural differences in causal interactions. We then apply a distance-based classification and -means clustering approach to identify the evolution of the causal structure represented by a DAG. Our method selects an unbiased number of clusters of similar structures and characterizes the similarities and differences between them. We explore a range of dynamic behavior using data from a clear sky day and during a solar eclipse in 2017. Our results show well-defined clusters of similar causal dependencies as the system evolves. Furthermore, our approach provides a methodological framework to understand how causal dependence in turbulence manifests in high-frequency data when represented through a DAG.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2018

IR Laser Control of the Clustering of CF{sub 3}Br Molecules during the Gas-Dynamic Expansion of a CF{sub 3}Br/Ar Mixture: Bromine Isotope Selectivity

The infrared (IR) laser radiation control of the clustering of CF3Br molecules during the gas-dynamic expansion of a CF{sub 3}Br/Ar mixture at the exit from a nozzle is investigated. Prominence is given to studying the possibility of bromine-isotope-selective suppression of the clustering of CF{sub 3}Br molecules due to their resonance vibrational excitation in the gas-dynamic expansion zone near the nozzle. A continuous CO{sub 2} laser is used in experiments to excite molecules and clusters in a beam, and a quadrupole mass spectrometer is used to detect them. The experimental setup and the experimental technique are described. The dependences of the efficiency of molecule clustering suppression on the exciting laser radiation parameters, the gas parameters (composition, pressure) above the nozzle, and the distance from the nozzle exit section to a molecule irradiation zone are obtained. Bromine-isotope-selective suppression of molecule clustering is shown to occur at the exit from the nozzle due to the resonance vibrational excitation of gas-dynamically cooled CF{sub 3}Br molecules. When CF{sub 3}Br/Ar mixtures are used at pressure ratios p(CF{sub 3}Br): p(Ar) = 1: 10 and 1: 30, the enrichment of a cluster beam by bromine isotopes are K{sub enr}({sup 81}Br) ≈ 1.18 ± 0.09 and 1.12 ± 0.07 during the 9R(30) laser line (1084.635 cm{sup –1}) irradiation of a jet. The clustering suppression selectivity is α ≈ 1.18 when the mixture at the pressure ratio p(CF{sub 3}Br): p(Ar) = 1: 10 is used. These results suggest that the proposed method can selectively control the clustering of the molecules containing the heavy element isotopes that have a small isotope shift in IR absorption spectra (OsO{sub 4}, WF{sub 6}, UF{sub 6}).

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2023

Hilbert space multireference coupled cluster tailored by matrix product states

In the past decade, the quantum chemical version of the density matrix renormalization group method has established itself as the method of choice for strongly correlated molecular systems. However, despite its favorable scaling, in practice, it is not suitable for computations of dynamic correlation. Several approaches to include that in post-DMRG methods exist; in our group, we focused on the tailored coupled cluster (TCC) approach. This method works well in many situations; however, in exactly degenerate cases (with two or more determinants of equal weight), it exhibits a bias toward the reference determinant representing the Fermi vacuum. Although sometimes it is possible to use a compensation scheme to avoid this bias for energy differences, it is certainly a drawback. In order to overcome this bias of the TCC method, we have developed a Hilbert-space multireference version of tailored CC, which can treat several determinants on an equal footing. We have implemented and compared the performance of three Hilbert-space multireference coupled cluster (MRCC) variants—the state universal one and the Brillouin–Wigner and Mukherjee’s state specific ones. We have assessed these approaches on the cyclobutadiene and tetramethyleneethane molecules, which are both diradicals with exactly degenerate determinants at a certain geometry. We have also investigated the sensitivity of the results on the orbital rotation of the highest occupied and lowest unoccupied molecular orbital (HOMO–LUMO) pair, as it is well known that Hilbert-space MRCC methods are not invariant to such transformations.

Chemistry↗
DOE OSTI2024

Jacobian-scaled K-means clustering for physics-informed segmentation of reacting flows

This work introduces Jacobian-scaled K-means (JSK-means) clustering, which is a physicsinformed clustering strategy centered on the K-means framework. The method allows for the injection of underlying physical knowledge into the clustering procedure through a distance function modification: instead of leveraging conventional Euclidean distance vectors, the JSKmeans procedure operates on distance vectors scaled by matrices obtained from dynamical system Jacobians evaluated at the cluster centroids. The goal of this work is to show how the JSKmeans algorithm - without modifying the input dataset - produces clusters that capture regions of dynamical similarity, in that the clusters are redistributed towards high-sensitivity regions in phase space and are described by similarity in the source terms of samples instead of the samples themselves. The algorithm is demonstrated on a complex reacting flow simulation dataset (a channel detonation configuration), where the dynamics in the thermochemical composition space are known through the highly nonlinear and stiff Arrhenius-based chemical source terms. Interpretations of cluster partitions in both physical space and composition space reveal how JSK-means shifts clusters produced by standard K-means towards regions of high chemical sensitivity (e.g., towards regions of peak heat release rate near the detonation reaction zone). Furthermore, the findings presented here illustrate the benefits of utilizing Jacobian-scaled distances in clustering techniques, and the JSK-means method in particular displays promising potential for improving former partition-based modeling strategies in reacting flow (and other multi-physics) applications.

Clustering↗
DOE OSTI2019

Global Optimization of Adsorbate Covered Supported Cluster Catalysts: The Case of Pt 7 H 10 CH 3 on α-Al 2 O 3

Determining structures of supported sub-nanometer catalytic clusters is important for finding binding sites, active sites, and reaction mechanisms. In realistic conditions, the cluster may be covered with adsorbed reactants and intermediates, which strongly affect the structure of the cluster compared to the low coverage regime. The global optimization of supported adsorbate-covered clusters is not possible with existing methods. In this paper, we present a customized Basin Hopping (BH) approach, with a core (metal cluster) – shell (adsorbates) separation scheme, and perform first applications to the search of low-energy isomers of Pt 7 /α-Al 2 O 3 at high hydrogen coverage (10H). The presence of adsorbates significantly alters the low-energy isomers compared to bare Pt 7 /α-Al 2 O 3 . Molecular dynamics simulations additionally show the different time-scales associated with the mobility of H and Pt atoms. The revised BH method with core-shell separation presents key advantages for the structural exploration of adsorbate-covered supported catalysts, relevant to realistic catalytic conditions.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS2021

Atacama Cosmology Telescope measurements of a large sample of candidates from the Massive and Distant Clusters of WISE Survey: Sunyaev-Zeldovich effect confirmation of MaDCoWS candidates using ACT

Context. Galaxy clusters are an important tool for cosmology, and their detection and characterization are key goals for current and future surveys. Using data from the Wide-field Infrared Survey Explorer (WISE), the Massive and Distant Clusters of WISE Survey (MaDCoWS) located 2839 significant galaxy overdensities at redshifts 0.7 . z . 1.5, which included extensive follow-up imaging from the Spitzer Space Telescope to determine cluster richnesses. Concurrently, the Atacama Cosmology Telescope (ACT) has produced large area millimeter-wave maps in three frequency bands along with a large catalog of Sunyaev-Zeldovich (SZ)-selected clusters as part of its Data Release 5 (DR5). Aims. We aim to verify and characterize MaDCoWS clusters using measurements of, or limits on, their thermal SZ effect signatures. We also use these detections to establish the scaling relation between SZ mass and the MaDCoWS-defined richness. Methods. Using the maps and cluster catalog from DR5, we explore the scaling between SZ mass and cluster richness. We do this by comparing cataloged detections and extracting individual and stacked SZ signals from the MaDCoWS cluster locations. We use complementary radio survey data from the Very Large Array, submillimeter data from Herschel, and ACT 224 GHz data to assess the impact of contaminating sources on the SZ signals from both ACT and MaDCoWS clusters. We use a hierarchical Bayesian model to fit the mass-richness scaling relation, allowing for clusters to be drawn from two populations: one, a Gaussian centered on the mass-richness relation, and the other, a Gaussian centered on zero SZ signal. Results. We find that MaDCoWS clusters have submillimeter contamination that is consistent with a gray-body spectrum, while the ACT clusters are consistent with no submillimeter emission on average. Additionally, the intrinsic radio intensities of ACT clusters are lower than those of MaDCoWS clusters, even when the ACT clusters are restricted to the same redshift range as the MaDCoWS clusters. We find the best-fit ACT SZ mass versus MaDCoWS richness scaling relation has a slope of p1 = 1.84+0.15 −0.14, where the slope is defined as M ∝ λ p1 15 and λ15 is the richness. We also find that the ACT SZ signals for a significant fraction (∼57%) of the MaDCoWS sample can statistically be described as being drawn from a noise-like distribution, indicating that the candidates are possibly dominated by low-mass and unvirialized systems that are below the mass limit of the ACT sample. Further, we note that a large portion of the optically confirmed ACT clusters located in the same volume of the sky as MaDCoWS are not selected by MaDCoWS, indicating that the MaDCoWS sample is not complete with respect to SZ selection. Finally, we find that the radio loud fraction of MaDCoWS clusters increases with richness, while we find no evidence that the submillimeter emission of the MaDCoWS clusters evolves with richness. Conclusions. We conclude that the original MaDCoWS selection function is not well defined and, as such, reiterate the MaDCoWS collaboration’s recommendation that the sample is suited for probing cluster and galaxy evolution, but not cosmological analyses. We find a best-fit mass-richness relation slope that agrees with the published MaDCoWS preliminary results. Additionally, we find that while the approximate level of infill of the ACT and MaDCoWS cluster SZ signals (1–2%) is subdominant to other sources of uncertainty for current generation experiments, characterizing and removing this bias will be critical for next-generation experiments hoping to constrain cluster masses at the sub-percent level.

large↗
NASA NTRS1993

Designers' models of the human-computer interface

Understanding design models of the human-computer interface (HCI) may produce two types of benefits. First, interface development often requires input from two different types of experts: human factors specialists and software developers. Given the differences in their backgrounds and roles, human factors specialists and software developers may have different cognitive models of the HCI. Yet, they have to communicate about the interface as part of the design process. If they have different models, their interactions are likely to involve a certain amount of miscommunication. Second, the design process in general is likely to be guided by designers' cognitive models of the HCI, as well as by their knowledge of the user, tasks, and system. Designers do not start with a blank slate; rather they begin with a general model of the object they are designing. The author's approach to a design model of the HCI was to have three groups make judgments of categorical similarity about the components of an interface: human factors specialists with HCI design experience, software developers with HCI design experience, and a baseline group of computer users with no experience in HCI design. The components of the user interface included both display components such as windows, text, and graphics, and user interaction concepts, such as command language, editing, and help. The judgments of the three groups were analyzed using hierarchical cluster analysis and Pathfinder. These methods indicated, respectively, how the groups categorized the concepts, and network representations of the concepts for each group. The Pathfinder analysis provides greater information about local, pairwise relations among concepts, whereas the cluster analysis shows global, categorical relations to a greater extent.

Gillan, Douglas J.↗
DOE OSTI2025

Slimmer Geminals For Accurate F12 Electronic Structure Models

The Slater-type F12 geminal length scales originally tuned for the second-order Mo̷ller-Plesset F12 method are too large for higher-order F12 methods formulated using the SP (diagonal fixed-coefficient spin-adapted) F12 ansatz. The new geminal parameters reported herein reduce the basis set incompleteness errors (BSIEs) of absolute coupled-cluster singles and doubles F12 correlation energies by a significant─and increase with the cardinal number of the basis─margin. The effect of geminal reoptimization is especially pronounced for the cc-pVXZ-F12 basis sets (specifically designed for use with F12 methods) relative to their conventional aug-cc-pVXZ counterparts. The BSIEs of relative energies are less affected, but substantial reductions can be obtained, especially for atomization energies and ionization potentials with the cc-pVXZ-F12 basis sets. The new geminal parameters are therefore recommended for all applications of high-order F12 methods, such as coupled-cluster F12 methods and transcorrelated F12 methods.

Powell, Samuel R. [Virginia Polytechnic Inst. and ↗
DOE OSTI2019

Identification of stable adsorption sites and diffusion paths on nanocluster surfaces: an automated scanning algorithm

The diverse coordination environments on the surfaces of discrete, three-dimensional (3D) nanoclusters contribute significantly to their unique catalytic properties. Identifying the numerous adsorption sites and diffusion paths on these clusters is however tedious and time-consuming, especially for large, asymmetric nanoclusters. Here, we present a simple, automated method for constructing approximate 2D potential energy surfaces for the adsorption of atomic species on the surfaces of 3D nanoclusters with minimal human intervention. These potential energy surfaces fully characterize the important adsorption sites and diffusion paths on the nanocluster surfaces with accuracies similar to current approaches and at comparable computational cost. Our method can treat complex nanoclusters, such as alloy nanoclusters, and accounts for cluster relaxation and adsorbate-induced reconstruction, important for obtaining accurate energetics. Moreover, its highly parallelizable nature is ideal for modern supercomputer architectures. We showcase our method using two clusters: Au 18 and Pt 55 . For Au 18 , diffusion of atomic hydrogen between the most stable sites occurs via non-intuitive paths, underlining the necessity of exploring the complete potential energy surface. By enabling the rapid and unbiased assessment of adsorption and diffusion on large, complex nanoclusters, which are particularly difficult to handle manually, our method will help advance materials discovery and the rational design of catalysts.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Observational constraints of an anisotropic boost due to the projection effects using redMaPPer clusters

Optical clusters identified from red-sequence galaxies suffer from projection effects, where interloper galaxies along the line of sight to a cluster are mistaken as genuine members of the cluster. In the previous study, we found that the projection effects cause the boost on the amplitudes of clustering and lensing on large scale compared to the expected amplitudes in the absence of any projection effects. These boosts are caused by preferential selections of filamentary structure aligned to the line of sight due to distance uncertainties in photometric surveys. We model the projection effects with two simple assumptions and develop a novel method to quantify the size of the boost using cluster-galaxy cross-correlation functions. We validate our method using mock cluster catalogues built from cosmological N-body simulations and find that we can obtain unbiased constraints on the boost parameter with our model. We then apply our analysis on the SDSS redMaPPer clusters and find that the size of the boost is roughly 20 per cent for all the richness bins except the cluster sample with the richness bin λ ∈ [30, 40]. This is the first study to constrain the boost parameter independent from cluster cosmology studies and provides a self-consistency test for the projection effects.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2017

Stochastic Formulation of the Resolution of Identity: Application to Second Order Møller–Plesset Perturbation Theory

A stochastic orbital approach to the resolution of identity (RI) approximation for 4-index electron repulsion integrals (ERIs) is presented. The stochastic RI-ERIs are then applied to second order Møller–Plesset perturbation theory (MP2) utilizing a multiple stochastic orbital approach. The introduction of multiple stochastic orbitals results in an O(N AO 3 ) scaling for both the stochastic RI-ERIs and stochastic RI-MP2, NAO being the number of basis functions. For a range of water clusters we demonstrate that this method exhibits a small prefactor and observed scalings of O(N e 2.4 ) for total energies and O(N e 3.1 ) for forces (N e being the number of correlated electrons), outperforming MP2 for clusters with as few as 21 water molecules.

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

Anion photoelectron spectroscopy and chemical bonding of ThS 2 – and ThSO –

Anion photoelectron spectra of ThSO – and ThS 2 – were recorded using the third (355 nm) harmonic of an Nd-YAG laser; these provided the measured vertical detachment energies of each anion. The experiments are supported by extensive coupled cluster calculations on ThSO, ThSO – , ThS 2 , and ThS 2 – , as well as the oxygen congeners ThO 2 and ThO 2 – . The ab initio calculations, which included complete basis set extrapolations, spin–orbit effects using four-component coupled cluster, and higher-order correlation contributions through CCSDT(Q), yielded an adiabatic electron affinity for ThO 2 – that was within 0.02 eV of the previously determined experimental value. The singly occupied molecular orbital (SOMO) in all three anions corresponds primarily to the 7s orbital on Th. Successive substitution of S for each O in ThO 2 leads to larger electron affinities and smaller bond angles in the neutral molecules, but larger angles in the anions. As demonstrated by Franck–Condon simulations of the spectra using the CCSD(T) spectroscopic constants, substitution of O by S significantly complicates the resulting detachment spectra due to the lower vibrational frequencies in the sulfur species. Altogether the calculated vertical detachment energies are in very good agreement with the experiment. In addition to the adiabatic electron affinities of each species, atomization energies and heats of formation have also been determined via the FPD approach with expected uncertainties of 1–2 kcal/mol.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2019

Beyond chemical accuracy in the heavy p-block: The first ionization potentials and electron affinities of Ga-Kr, In-Xe, and Tl-Rn

A relativistic coupled-cluster version of the Feller-Peterson-Dixon (FPD) composite method was previously used to accurately calculate the first ionization potentials (IP) and electron affinities (EAs) of the post-d, p-block elements Ga–Rn. Complete basis set (CBS) extrapolations including outer-core correlation at the CCSD(T) level of theory were combined with contributions from higher order electron correlation up to CCSDTQ, quantum electrodynamic effects (Lamb shift), and spin-orbit (SO) coupling including the Gaunt contribution. Several methods for including SO were investigated, in which all involved the four-component (4c) Dirac-Coulomb (DC) Hamiltonian. Here, the treatment of SO coupling was the contribution that limited the final accuracy of the present results. In the cases where 4c-DC-CCSD(T) could be reliably used for the SO contributions, the final composite IPs and EAs agreed with the available experimental values to within an unsigned average error of just 0.16 and 0.20 kcal/mol, respectively. In all cases the final IPs and EAs were within 1 kcal/mol of the available experimental values, except for the EAs of the group 13 elements (Ga, In, Tl), where the currently accepted experimental values appear to be too large by as much as 4 kcal/mol. The values predicted in this work, which have estimated uncertainties of ±0.5 kcal/mol, are 5.25 (Ga), 7.69 (In), and 7.39 (Tl) kcal/mol. For the EAs of Po and At, which do not have experimental values, the current calculations predict values of 34.2 and 55.8 kcal/mol with estimated uncertainties of ±0.6 and ±0.3 kcal/mol, respectively.

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

Coupled cluster spectroscopic properties of the coinage metal nitrosyls, M–NO (M = Cu, Ag, Au)

Ab initio near-equilibrium potential energy and dipole moment surfaces for the bent CuNO, AgNO, and AuNO molecules have been calculated under the Feller-Peterson-Dixon (FPD) composite framework at the coupled cluster level of theory including complete basis set extrapolation, outer-core correlation, scalar relativistic effects, and spin-orbit coupling. The Brueckner coupled cluster doubles with perturbative triples method, BCCD(T), was used to greatly improve upon CCSD(T), which was particularly problematic for CuNO. In the latter case the BCCD(T) vibrational frequencies showed significant differences compared to CCSD(T), e.g., nearly 65 cm -1 for the NO stretching frequency, and BCCD(T) also resulted in much better agreement with the available experimental frequencies. A full range of ro-vibrational spectroscopic constants are given for all three molecules of this study using the accurate composite potential energy functions and employing 2nd-order vibrational perturbation theory.

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

Centre-excised X-ray luminosity as an efficient mass proxy for future galaxy cluster surveys

The cosmological constraining power of modern galaxy cluster catalogues can be improved by obtaining low-scatter mass proxy measurements for even a small fraction of sources. In the context of large upcoming surveys that will reveal the cluster population down to the group scale and out to high redshifts, efficient strategies for obtaining such mass proxies will be valuable. Here in this work, we use high-quality weak-lensing and X-ray mass estimates for massive clusters in current X-ray-selected catalogues to revisit the scaling relations of the projected, centre-excised X-ray luminosity (L ce ), which previous work suggests correlates tightly with total mass. Our data confirm that this is the case with Lce having an intrinsic scatter at fixed mass comparable to that of gas mass, temperature or YX. Compared to the other proxies, however, Lce is less susceptible to systematic uncertainties due to background modelling, and can be measured precisely with shorter exposures. This opens up the possibility of using L ce to estimate masses for large numbers of clusters discovered by new X-ray surveys (e.g. eROSITA) directly from the survey data, as well as for clusters discovered at other wavelengths with relatively short follow-up observations. We describe a simple procedure for making such estimates from X-ray surface brightness data, and comment on the spatial resolution required to apply this method as a function of cluster mass and redshift. Lastly, we also explore the potential impact of Chandra and XMM–Newton follow-up observations over the next decade on dark energy constraints from new cluster surveys.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2018

Structural and chemical orders in N i 64.5 Z r 35.5 metallic glass by molecular dynamics simulation

The atomic structure of Ni 64.5 Zr 35.5 metallic glass has been investigated by molecular dynamics (MD) simulations. The calculated structure factors from the MD glassy sample at room temperature agree well with the X-ray diffraction (XRD) and neutron diffraction (ND) experimental data. Using the pairwise cluster alignment and clique analysis methods, we show that there are three types dominant short-range order (SRO) motifs around Ni atoms in the glass sample of Ni 64.5 Zr 35.5 , i.e., Mixed- Icosahedron(ICO)-Cube, Twined-Cube and icosahedron-like clusters. Furthermore, chemical order and medium-range order (MRO) analysis show that the Mixed-ICOCube and Twined-Cube clusters exhibit the characteristics of the crystalline B2 phase. In conclusion, our simulation results suggest that the weak glass-forming ability (GFA) of Ni 64.5 Zr 35.5 can be attributed to the competition between the glass forming ICO SRO and the crystalline Mixed-ICO-Cube and Twined-Cube motifs.

36 MATERIALS SCIENCE↗