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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 OSTI2022

Fermi–Löwdin orbital self-interaction correction of adsorption energies on transition metal ions

Density functional theory (DFT)-based descriptions of the adsorption of small molecules on transition metal ions are prone to self-interaction errors. Here, we show that such errors lead to a large over-estimation of adsorption energies of small molecules on Cu + , Zn + , Zn 2+ , and Mn + in local spin density approximation (LSDA) and Perdew, Burke, Ernzerhof (PBE) generalized gradient approximation calculations compared to reference values computed using the coupled-cluster with single, doubles, and perturbative triple excitations method. These errors are significantly reduced by removing self-interaction using the Perdew–Zunger self-interaction correction (PZ-SIC) in the Fermi–Löwdin Orbital (FLO) SIC framework. In the case of FLO-PBE, typical errors are reduced to less than 0.1 eV. Furthermore, analysis of the results using DFT energies evaluated on self-interaction-corrected densities [DFT(@FLO)] indicates that the density-driven contributions to the FLO-DFT adsorption energy corrections are roughly the same size in DFT = LSDA and PBE, but the total corrections due to removing self-interaction are larger in LSDA.

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

Importance of imposing gauge invariance in time-dependent density functional theory calculations with meta-generalized gradient approximations

It has been known for more than a decade that the gauge variance of the kinetic energy density τ leads to additional terms in the magnetic orbital rotation Hessian used in linear-response time-dependent density functional theory (TDDFT), affecting excitation energies obtained with τ-dependent exchange–correlation functionals. While previous investigations found that a correction scheme based on the paramagnetic current density has a small effect on benchmark results, we report more pronounced effects here, in particular, for the popular M06-2X functional and for some other meta-generalized gradient approximations (mGGAs). In the first part of this communication, this is shown by a reassessment of a set of five Ni(II) complexes for which a previous benchmark study that did not impose gauge invariance has found surprisingly large errors for excitation energies obtained with M06-2X. These errors are more than halved by restoring gauge invariance. The variable importance of imposing gauge invariance for different mGGA-based functionals can be rationalized by the derivative of the mGGA exchange energy integrand with respect to τ. In the second part, a large set of valence excitations in small main-group molecules is analyzed. For M06-2X, several selected n → π* and π→π$^{*}_{⊥}$ excitations are heavily gauge-dependent with average changes of –0.17 and –0.28 eV, respectively, while π→π$^{*}_{∥}$ excitations are marginally affected (–0.04 eV). Similar patterns, but of the opposite signs, are found for SCAN0. Here, the results suggest that reevaluation of previous gauge variant TDDFT results based on M06-2X and other mGGA functionals is warranted.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

L1448-MM OBSERVATIONS BY THE HERSCHEL KEY PROGRAM, ''DUST, ICE, AND GAS IN TIME'' (DIGIT)

We present Herschel/Photodetector Array Camera and Spectrometer (PACS) observations of L1448-MM, a Class 0 protostar with a prominent outflow. Numerous emission lines are detected at 55 <λ < 210 μm including CO, OH, H{sub 2}O, and [O I]. We investigate the spatial distribution of each transition to find that lines from low energy levels tend to distribute along the outflow direction while lines from high energy levels peak at the central spatial pixel. Spatial maps reveal that OH emission lines are formed in a relatively small area, while [O I] emission is extended. According to the rotational diagram analysis, the CO emission can be fitted by two (warm and hot) temperature components. For H{sub 2}O, the ortho-to-para ratio is close to 3. The non-LTE large velocity gradient (LVG) calculations suggest that CO and H{sub 2}O lines could instead be formed in a high kinetic temperature (T > 1000 K) environment, indicative of a shock origin. For OH, IR-pumping processes play an important role in the level population. The molecular emission in L1448-MM is better explained with a C-shock model, but the atomic emission of PACS [O I] and Spitzer/Infrared Spectrograph [Si II] emission is not consistent with C-shocks, suggesting multiple shocks in this region. Water is the major line coolant of L1448-MM in the PACS wavelength range, and the best-fit LVG models predict that H{sub 2}O and CO emit (50%-80%) of their line luminosity in the PACS wavelength range.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2015

Structure and magnetism in LaCoO 3

In this paper, the temperature dependence of the hexagonal lattice parameter c of single crystal LaCoO 3 (LCO) with H = 0 and 800 Oe, as well as LCO bulk powders with H = 0, was measured using high-resolution x-ray scattering near the transition temperature T o ≈ 35 K. The change of c(T ) is well characterized by a power law in T – T o for T > T o and by a temperature independent constant for T < T o when convoluted with a Gaussian function of width 8.5 K. Finally, this behavior is discussed in the context of the unusual magnetic behavior observed in LCO as well as recent generalized gradient approximation calculations.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2017

A Monte Carlo model for 3D grain evolution during welding

Welding is one of the most wide-spread processes used in metal joining. However, there are currently no open-source software implementations for the simulation of microstructural evolution during a weld pass. Here we describe a Potts Monte Carlo based model implemented in the SPPARKS kinetic Monte Carlo computational framework. The model simulates melting, solidification and solid-state microstructural evolution of material in the fusion and heat-affected zones of a weld. The model does not simulate thermal behavior, but rather utilizes user input parameters to specify weld pool and heat-affect zone properties. Weld pool shapes are specified by Bezier curves, which allow for the specification of a wide range of pool shapes. Pool shapes can range from narrow and deep to wide and shallow representing different fluid flow conditions within the pool. Surrounding temperature gradients are calculated with the aide of a closest point projection algorithm. Furthermore, the model also allows simulation of pulsed power welding through time-dependent variation of the weld pool size. Example simulation results and comparisons with laboratory weld observations demonstrate microstructural variation with weld speed, pool shape, and pulsed-power.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Computation of forces and stresses in solids: Towards accurate structural optimization with auxiliary-field quantum Monte Carlo

The accurate computation of forces and other energy derivatives has been a long-standing challenge for quantum Monte Carlo methods. A number of technical obstacles contribute to this challenge. We discuss how these obstacles can be removed with the auxiliary-field quantum Monte Carlo (AFQMC) approach. AFQMC is a general, high-accuracy, many-body total-energy method for molecules and solids. The implementation of back-propagation for pure estimators allows direct calculation of gradients of the energy via the Hellmann-Feynman theorem. A planewave basis with norm-conserving pseudopotentials is used for the study of periodic bulk materials. Completeness of the planewave basis minimizes the effect of so-called Pulay terms. The ionic pseudopotentials, which can be incorporated in AFQMC in exactly the same manner as in standard independent-electron methods, regulate the force and stress estimators and eliminate any potential divergence of the Monte Carlo variances. The resulting approach allows applications of full geometry optimizations in bulk materials. As a result, it also paves the way for many-body computations of the phonon spectrum in solids.

36 MATERIALS SCIENCE↗
DOE OSTI2022

Neural Networks for Supercapacitor Modeling

This software implements a one-dimensional model of a supercapacitor and calibrates it to experimental data. A system of coupled partial differential equation models the salt concentration and the ionic and electronic potentials. The term in the equation modeling the capacitance contains a neural network, whose parameters are optimized to fit the provided experimental data. The software is written in python using the open-source library JAX to calculate the gradients needed for the optimization.

Salazar de Troya, Miquel↗
DOE OSTI2026

Field and Model Data Associated with the Manuscript “Drivers of Streamflow Intermittency in Humid Regions: 2. Evaluating Controls on Flow Persistence in an Urbanized Catchment”

This package contains field data, modeling files, and scripts supporting the investigation of the drivers of streamflow intermittency in an urbanized catchment. It includes the field data collected from electrical resistivity tomography (ERT) surveys, distributed temperature sensing (DTS), continuous self-potential (SP) monitoring, groundwater and stilling well. In addition, it contains the data and results of the coupled water- and electrical-flow model developed using the COMSOL Multiphysics and Advanced Terrestrial Simulator (ATS), as well as software files and Jupyter notebooks used to process the data and generate figures in the manuscript submitted for peer review. The data archive is organized in the following directories: 1) Climate Includes hourly precipitation and daily evapotranspiration time series (2024 – 2025) provided as CSV files, alongside a text file detailing dataset units. 2) Coupled_model Field_Application subfolder contains the ATS XML input scripts, data files, output data for the SP site. It also contains the Jupyter notebook (Plot_final_calib.ipynb) to visualize the results of the modeled SP, stream-groundwater exchange and moisture content. The flow model simulation is executed using the ATS XML scripts and the included Python script (generate_data_set.py) to convert ATS output to COMSOL-ready input. COMSOL Multiphysics template (.m can only be used with COMSOL with MATLAB) is executed using the ATS output data to simulate the potential field. 3) Discharge Includes the electrical conductivity (EC) time series (provided as CSV files) from salt slug injections. It also includes the Jupyter notebook (Discharge_process.ipynyb) used to estimate discharge. All discharge measurements collated into rating_curve_processed.csv 4) DTS Contains collated DTS data including raw Stokes and anti-Stokes measurement (provided as .h5 file). It also includes DTS processing.ipynb, a Jupyter notebook for calibrating the DTS data using dts_calibration Python package. cooler_calibration.csv is the DTS calibration CSV used in the calibration sequence. 5) ERT Contains raw resistivity data (provided as CSV files), spatial location of each of the electrodes (provided as CSV files), and files used for the resistivity inversion. 6) Slug_test Includes the slug test data at all the groundwater wells provided as CSV files, as well as the Jupyter notebook (Slug_test.ipynb) for calculating hydraulic conductivity. 7) SP Contains the SP data collected in field at the SP sites (provided as CSV files). 8) Well_data Contains two subfolders: 1) Raw, which provides unprocessed pressure, electrical conductivity and temperature timeseries downloaded from the loggers in all the groundwater and stilling wells, and 2) Processed, which contains sorted, QA/QC timeseries data for each well. The data archive also contains data_process.ipynb, a Jupyter notebook used for field data analysis and generating figures (plotting well, SP, climate, and discharge data, as well as calculating head gradient at sites with nested groundwater wells). Note: Code files (.ipynb, .py, .xml) can be opened in any standard code editor, .exo file can be viewed using Paraview, .h5 files can be opened using HDFView software and h5py Python package, and .resipy file can be opened with the open-source ResIPy software.

ATS↗
DOE OSTI2021

End-to-End Differentiable Modeling and Management of the Environment

Focal Area: (2) Data acquisition and assimilation enabled by machine learning, AI, and advanced methods including experimental/network design/optimization. We emphasize the importance of leveraging optimization techniques from AI/machine learning (ML) to solve challenging problems in Earth system modeling. Science Challenge: Automatic differentiation has had a transformative effect on ML by allowing the calculation of gradients of arbitrary functions in an incredibly large class of models. We can potentially realize similar improvements in parameter estimation and control for Earth system models (ESMs) by reimplementing them in computational frameworks from ML. Practitioners working with large (>10 7 parameters) models in ML and AI can obtain good predictive performance in a range of spatiotemporal tasks by making use of optimization via stochastic gradient descent and incorporating prior knowledge at multiple levels. We propose writing ESMs in open-source computational frameworks such as Torch, Tensorflow, and JAX to greatly expand the scope of environmental forecasting and management challenges, which can be addressed by leveraging automatic differentiation and gradient descent-like algorithms. We do not call for a wholesale replacement of physical models with data-driven surrogates, but rather advocate for interleaving physical and empirical equations in a manner that is most faithful to the extent of our scientific knowledge and observational data. Central to this topic is the merging of differentiable physical simulations with differentiable optimization layers, which are now both beginning to come to the forefront.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2019

Air-to-air background oriented schlieren technique

An air-to-air background-oriented Schlieren system and method for measuring and rendering visible density changes in air that cause a refractive index change by an airborne vehicle. A sensor aircraft equipped with a high-speed visible spectrum camera travels at low airspeed on a predetermined route and on a level altitude over a background having consistent contrast and sunlight reflectivity. The target aircraft, traveling on the same predetermined route but at an altitude between the sensor aircraft and the ground (background) passes beneath the sensor aircraft. The camera on the sensor aircraft captures a series of images including a reference image immediately before the target aircraft enters the image frame followed by several data images as the target aircraft passes through the image frame. The data images are processed to calculate density gradients around the target aircraft. These density gradients include shockwaves, vortices, engine exhaust, and wakes. Air density gradients cause a refractive index change in the fluid and a slight distortion in the background pattern of the data image. Image processing that compares the data image to the reference image yields the difference caused by the density gradient.

Heineck, James Thomas↗
DOE OSTI2014

Gradient Theory simulations of pure fluid interfaces using a generalized expression for influence parameters and a Helmholtz energy equation of state for fundamentally consistent two-phase calculations

The fidelity of Gradient Theory simulations depends on the accuracy of saturation properties and influence parameters, and require equations of state (EoS) which exhibit a fundamentally consistent behavior in the two-phase regime. Widely applied multi-parameter EoS, however, are generally invalid inside this region. Hence, they may not be fully suitable for application in concert with Gradient Theory despite their ability to accurately predict saturation properties. The commonly assumed temperature-dependence of pure component influence parameters usually restricts their validity to subcritical temperature regimes. This may distort predictions for general multi-component interfaces where temperatures often exceed the critical temperature of vapor phase components. Then, the calculation of influence parameters is not well defined. In this paper, one of the first studies is presented in which Gradient Theory is combined with a next-generation Helmholtz energy EoS which facilitates fundamentally consistent calculations over the entire two-phase regime. Illustrated on pentafluoroethane as an example, reference simulations using this method are performed. They demonstrate the significance of such high-accuracy and fundamentally consistent calculations for the computation of interfacial properties. These reference simulations are compared to corresponding results from cubic PR EoS, widely-applied in combination with Gradient Theory, and mBWR EoS. The analysis reveals that neither of those two methods succeeds to consistently capture the qualitative distribution of obtained key thermodynamic properties in Gradient Theory. Furthermore, a generalized expression of the pure component influence parameter is presented. This development is informed by its fundamental definition based on the direct correlation function of the homogeneous fluid and by presented high-fidelity simulations of interfacial density profiles. As a result, the new model preserves the accuracy of previous temperature-dependent expressions, remains well-defined at supercritical temperatures, and is fully suitable for calculations of general multi-component two-phase interfaces.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2014

Results for aliovalent doping of CeBr{sub 3} with Ca{sup 2+}

Despite the outstanding scintillation performance characteristics of cerium tribromide (CeBr{sub 3}) and cerium-activated lanthanum tribromide, their commercial availability and application are limited due to the difficulties of growing large, crack-free single crystals from these fragile materials. This investigation employed aliovalent doping to increase crystal strength while maintaining the optical properties of the crystal. One divalent dopant (Ca{sup 2+}) was used as a dopant to strengthen CeBr{sub 3} without negatively impacting scintillation performance. Ingots containing nominal concentrations of 1.9% of the Ca{sup 2+} dopant were grown, i.e., 1.9% of the CeBr{sub 3} molecules were replaced by CaBr{sub 2} molecules, to match our target replacement of 1 out of 54 cerium atoms be replaced by a calcium atom. Precisely the mixture was composed of 2.26 g of CaBr{sub 2} added to 222.14 g of CeBr{sub 3}. Preliminary scintillation measurements are presented for this aliovalently doped scintillator. Ca{sup 2+}-doped CeBr{sub 3} exhibited little or no change in the peak fluorescence emission for 371 nm optical excitation for CeBr{sub 3}. The structural, electronic, and optical properties of CeBr{sub 3} crystals were studied using the density functional theory within the generalized gradient approximation. Calculated lattice parameters are in agreement with the experimental data. The energy band structures and density of states were obtained. The optical properties of CeBr{sub 3}, including the dielectric function, were calculated.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2013

Approximate error conjugation gradient minimization methods

In one embodiment, a method includes selecting a subset of rays from a set of all rays to use in an error calculation for a constrained conjugate gradient minimization problem, calculating an approximate error using the subset of rays, and calculating a minimum in a conjugate gradient direction based on the approximate error. In another embodiment, a system includes a processor for executing logic, logic for selecting a subset of rays from a set of all rays to use in an error calculation for a constrained conjugate gradient minimization problem, logic for calculating an approximate error using the subset of rays, and logic for calculating a minimum in a conjugate gradient direction based on the approximate error. In other embodiments, computer program products, methods, and systems are described capable of using approximate error in constrained conjugate gradient minimization problems.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2016

Nonequilibrium solvent effects in Born-Oppenheimer molecular dynamics for ground and excited electronic states

The effects of solvent on molecular processes such as excited state relaxation and photochemical reaction often occurs in a nonequilibrium regime. Dynamic processes such as these can be simulated using excited state molecular dynamics. In this work, we describe methods of simulating nonequilibrium solvent effects in excited state molecular dynamics using linear-response time-dependent density functional theory and apparent surface charge methods. These developments include a propagation method for solvent degrees of freedom and analytical energy gradients for the calculation of forces. Molecular dynamics of acetaldehyde in water or acetonitrile are demonstrated where the solute-solvent system is out of equilibrium due to photoexcitation and emission.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2013

Grazing-incidence x-ray fluorescence analysis for non-destructive determination of In and Ga depth profiles in Cu(In,Ga)Se{sub 2} absorber films

Development of highly efficient thin film solar cells involves band gap engineering by tuning their elemental composition with depth. Here we show that grazing incidence X-ray fluorescence (GIXRF) analysis using monochromatic synchrotron radiation and well-characterized instrumentation is suitable for a non-destructive and reference-free analysis of compositional depth profiles in thin films. Variation of the incidence angle provides quantitative access to the in-depth distribution of the elements, which are retrieved from measured fluorescence intensities by modeling parameterized gradients and fitting calculated to measured fluorescence intensities. Our results show that double Ga gradients in Cu(In{sub 1−x},Ga{sub x})Se{sub 2} can be resolved by GIXRF.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Fast model-based scenario optimization in NSTX-U enabled by analytic gradient computation

Model-based optimization offers a systematic approach to advanced scenario planning. In this case, the feedforward-control inputs (actuator trajectories) that are needed to attain and sustain a desired scenario are obtained by solving a nonlinear constrained optimization problem. This class of problems generally minimize a cost function that measures the difference between desired and actual plasma states. Several numerical optimization algorithms, such as sequential quadratic programming, require repeated calculation of the cost function gradients with respect to the input trajectories. Calculating these gradients numerically can be computationally intensive, increasing the time needed to solve the feedforward-control optimization problem. Here, this work introduces a method to analytically calculate these cost function gradients from the current profile evolution model. This can significantly reduce the computational time and allow for fast feedforward-control optimization, which would eventually enable optimal scenario planning between discharges. The performance of the feedforward optimizer with analytical gradients is compared to a traditional optimization algorithm based on numerical gradients for different NSTX-U scenarios. The plasma dynamics in the optimization algorithm are simulated using the Control Oriented Transport SIMulator (COTSIM). Results of the work show that analytical gradients consistently reduce the computation time while achieving trajectories that are comparable to those obtained by traditional optimization algorithms based on numerical gradients.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

A benchmark of Gutzwiller conjugate gradient minimization method in ground state energy calculations of dimers

Herein we present numerical results of ground-state energies of 9 molecules in the well-established G2 molecule set given by the Gutzwiller conjugate gradient minimization (GCGM) method. The method, beyond the commonly used Gutzwiller approximation, was recently developed based on Gutzwiller variational wave functions. We find that compared to benchmark data given by full configuration interaction, GCGM total energies are reasonably well reproduced with the minimum basis set. To include the dynamical correlation beyond the minimal basis calculations, we adopt the local density approximation for the dynamical correlation energy $E_c$. By comparing the results with benchmark data given by experiments and large-basis configuration interaction, the GCGM total energies with $E_c$ are in general better reproduced, but discrepancies are still observed for some dimers.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2014

Investigation of structural stability and elastic properties of Zrh and Zrh{sub 2}: A first principles study

The electronic, structural and mechanical properties of ZrH and ZrH{sub 2} are investigated by means of first principles calculation based on density functional theory as implemented in VASP code with generalized gradient approximation. The calculated ground state properties are in good agreement with previous experimental and other theoretical results. Among the six crystallographic structures considered for ZrH, ZB phase is found to be the most stable phase, whereas ZrH{sub 2} is energetically stable in tetragonal structure at ambient condition. A structural phase transition from ZB→NaCl at a pressure 10 GPa is predicted for ZrH.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗