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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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At least 37 records · Page 2
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Lagrangian formulation of nuclear–electronic orbital Ehrenfest dynamics with real-time TDDFT for extended periodic systems

Here, we present a Lagrangian-based implementation of Ehrenfest dynamics with nuclear–electronic orbital (NEO) theory and real-time time-dependent density functional theory for extended periodic systems. In addition to a quantum dynamical treatment of electrons and selected protons, this approach allows for the classical movement of all other nuclei to be taken into account in simulations of condensed matter systems. Furthermore, we introduce a Lagrangian formulation for the traveling proton basis approach and propose new schemes to enhance its application for extended periodic systems. Validation and proof-of-principle applications are performed on electronically excited proton transfer in the o-hydroxybenzaldehyde molecule with explicit solvating water molecules. These simulations demonstrate the importance of solvation dynamics and a quantum treatment of transferring protons. This work broadens the applicability of the NEO Ehrenfest dynamics approach for studying complex heterogeneous systems in the condensed phase.

Calculus of variations↗
DOE OSTI2022

Simultaneous Optimization of Nuclear–Electronic Orbitals

Accurate modeling of important nuclear quantum effects, such as nuclear delocalization, zero-point energy, and tunneling, as well as non-Born-Oppenheimer effects, requires treatment of both nuclei and electrons quantum mechanically. The nuclear–electronic orbital (NEO) method provides an elegant framework to treat specified nuclei, typically protons, on the same level as the electrons. In conventional electronic structure theory, finding a converged ground state can be a computationally demanding task; converging NEO wavefunctions, due to their coupled electronic and nuclear nature, is even more demanding. Herein, we present an efficient simultaneous optimization method that uses the direct inversion in the iterative subspace method to simultaneously converge wavefunctions for both the electrons and quantum nuclei. In conclusion, benchmark studies show that the simultaneous optimization method can significantly reduce the computational cost compared to the conventional stepwise method for optimizing NEO wavefunctions for multicomponent systems.

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

Reliable p K a Prediction through Efficient Incorporation of Anharmonicity within the Nuclear–Electronic Orbital Framework

Accurate pK a prediction is critical for understanding chemical reactivity and molecular properties across a wide range of applications. Computational approaches usually invoke a harmonic treatment of the vibrational modes for zero-point energies, as well as thermal and entropic contributions. Herein, we present a general protocol for relative pK a prediction that incorporates the significant anharmonic effects using nuclear–electronic orbital (NEO) theory. This protocol is validated against experimental data for a range of molecules in acetonitrile, including protonated nitrogen bases, nitrophenols, anilines, and diamines, as well as cobalt electrocatalysts. For simple acids, the NEO approach offers only a slight improvement over conventional density functional theory with the standard harmonic vibrational treatment, whereas for hydrogen-bonded acids, the NEO approach offers more significantly improved performance at a comparable computational cost. This accessible methodology provides a practical route for accurate pKa prediction in challenging systems and is extendable to related thermodynamic properties such as hydricities and proton-coupled redox potentials.

Density functional theory↗
DOE OSTI2026

Nuclear–Electronic Orbital General Rate Theory: Predicting Hydrogen Kinetic Isotope Effects in the Deep Tunneling Regime

Hydrogen transfer is a critical component of many chemical and biological processes. The ratio of rate constants for hydrogen and deuterium transfer defines the H/D kinetic isotope effect (KIE), which is a powerful tool for elucidating hydrogen transfer mechanisms. Interpretation of experimental H/D KIEs relies on accurate and affordable computational methods. However, due to their light mass, hydrogen and deuterium can undergo tunneling, which is challenging to describe in multidimensional molecular systems. Herein, we introduce the nuclear–electronic orbital general rate theory (NEO-GRT), which enables the efficient prediction of H/D KIEs based on full-dimensional molecular quantum chemistry calculations. The NEO-GRT approach describes the hydrogen transfer rate constant with a general expression that spans the vibrationally adiabatic and nonadiabatic hydrogen tunneling regimes. The input quantities are computed using NEO density functional theory, which treats the transferring hydrogen or deuterium nucleus quantum mechanically on the same level as the electrons. We investigate two intramolecular proton transfer reactions in organic molecules at temperatures down to 50 K to evaluate the performance of NEO-GRT by comparison to transition state theory and ring-polymer instanton theory. The KIEs computed with NEO-GRT agree with those calculated using ring-polymer instanton theory for the full-dimensional molecular systems at the same level of electronic structure theory. This agreement indicates that NEO-GRT captures the deep hydrogen tunneling effects, in contrast to transition state theory, which neglects such effects. Given its relatively low computational cost, NEO-GRT is a promising approach for predicting H/D KIEs in large organic and organometallic systems.

Hydrogen↗
DOE OSTI2023

Observation of electron orbital signatures of single atoms within metal-phthalocyanines using atomic force microscopy

Resolving the electronic structure of a single atom within a molecule is of fundamental importance for understanding and predicting chemical and physical properties of functional molecules such as molecular catalysts. However, the observation of the orbital signature of an individual atom is challenging. We report here the direct identification of two adjacent transition-metal atoms, Fe and Co, within phthalocyanine molecules using high-resolution noncontact atomic force microscopy (HR-AFM). HR-AFM imaging reveals that the Co atom is brighter and presents four distinct lobes on the horizontal plane whereas the Fe atom displays a “square” morphology. Pico-force spectroscopy measurements show a larger repulsion force of about 5 pN on the tip exerted by Co in comparison to Fe. Our combined experimental and theoretical results demonstrate that both the distinguishable features in AFM images and the variation in the measured forces arise from Co’s higher electron orbital occupation above the molecular plane. The ability to directly observe orbital signatures using HR-AFM should provide a promising approach to characterizing the electronic structure of an individual atom in a molecular species and to understand mechanisms of certain chemical reactions.

36 MATERIALS SCIENCE↗
NASA NTRS2018

Prelaunch and On-Orbit Electronic Calibration for Earth Observing Instruments

"The Electronic Calibration (Ecal) tests are performed during various stages of instrument development to examinethe linearity of the instrument electronics. During this process, charges with stepwise increments are injected inthe analog electronics circuitry to generate a ramp signal that can be used to characterize any nonlinearities in theelectronics. The prelaunch characterization of MODIS (on the Terra and Aqua platforms) and VIIRS (on SNPP,JPSS-1 and JPSS-2) involved a regular evaluation of the electronics linearity using the Ecal tests. On orbit,the Ecal tests have been regularly performed over the mission for both the MODIS instruments to derive theelectronics gain and linearity. Unlike MODIS, the Ecal tests on the VIIRS instruments are performed on an as-needed basis. To date, no Ecal tests were performed for S-NPP VIIRS on orbit. The VIIRS instrument on JPSS-1(now NOAA 20) was launched on November 18, 2017. An Ecal test was performed to support the instrumentsinitial post-launch performance assessment. Shortly after the first on-orbit emissive band calibration, degradationin the instrument gain was observed for the LWIR bands (M15, M16 and I5). As a part of the investigationrelated to this anomaly, a second Ecal test was performed and results were compared with the prelaunch results.In this paper, we discuss the prelaunch Ecal tests and representative results from MODIS and VIIRS prelaunchcharacterization. Also, discussed are the on-orbit results from the two MODIS instruments as well as from therecently launched VIIRS instrument."

ECAL↗
NASA NTRS2016

Assessments and Applications of Terra and Aqua MODIS On-Orbit Electronic Calibration

MODIS has 36 spectral bands located on four focal plane assemblies (FPAs), covering wavelengths from 0.41 to 14.4 micrometers. MODIS bands 1-30 collect data using photovoltaic (PV) detectors and, therefore, are referred to as the PV bands. Similarly, bands 31-36 using photoconductive (PC) detectors are referred to as the PC bands.The MODIS instrument was built with a set of on-board calibrators (OBCs) in order to track on-orbit changes of its radiometric, spatial, and spectral characteristics. In addition, an electronic calibration (ECAL) function can be used to monitor on-orbit changes of its electronic responses (gains). This is accomplished via a series of stair step signals generated by the ECAL function. These signals, in place of the FPA detector signals, are amplified and digitized just like the detector signals. Over the entire mission of both Terra and Aqua MODIS,the ECAL has been performed for the PV bands and used to assess their on-orbit performance. This paper provides an overview of MODIS on-orbit calibration activities with a focus on the PV ECAL, including its calibration process and approaches used to monitor the electronic performance. It presents the results derived and lessons learned from Terra and Aqua MODIS on-orbit ECAL. Also discussed are some of the applications performed with the information provided by the ECAL data.

Xiong, Xiaoxiong↗
DOE OSTI2025

Multiscale Nuclear-Electronic Orbital Quantum Dynamics in Complex Environments

Many renewable energy conversion processes rely on the movement of protons as well as electrons through either electrocatalysis or photoexcitation. The simulation of such processes requires a quantum mechanical description of coupled nuclear-electronic dynamics in a solvent or heterogeneous chemical environment. The overall objective of this project is the development of theoretical and computational capabilities for simulating nuclear-electronic quantum dynamics in complex environments and the creation of high-performance, open-source software. This multiscale framework will enable simulations of the real-time dynamics of nonequilibrium excited state proton-coupled electron transfer, quantum decoherence, vibronic energy transfer, and ultrafast radiolysis, as well as their associated time-resolved multidimensional spectroscopies. An important outcome of this project will be a sustainable, reusable, and interoperable open-source software ecosystem. This software will be designed for emerging exascale and future national leadership computers. Another key outcome will be a multiscale quantum dynamics method and software enabling simulations of nonequilibrium nuclear-electronic quantum dynamics in complex environments.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1986

On the estimation of metal-metal distortions for metal-metal orbital electronic ionizations and excitations

Reference is made to the work of Lichtenberger and Blevins (1984), who resolved a nu(Mo2) vibronic structure in the metal-metal delta-orbital photoelectron ionization band of Mo2(O2CCH3) in the gas phase at 200 C and performed a Franck-Condon analysis of the observed band profile. In the analysis, 'hot bands' were explicitly excluded as having any important effect on the Franck-Condon results. In the analytical study reported in the present paper, it is demonstrated that the thermal effects are indeed significant.

Miskowski, Vincent M.↗
NASA NTRS1976

Orbital electron capture by the nucleus

The theory of nuclear electron capture is reviewed in the light of current understanding of weak interactions. Experimental methods and results regarding capture probabilities, capture ratios, and EC/Beta(+) ratios are summarized. Radiative electron capture is discussed, including both theory and experiment. Atomic wave function overlap and electron exchange effects are covered, as are atomic transitions that accompany nuclear electron capture. Tables are provided to assist the reader in determining quantities of interest for specific cases.

Bambynek, W.↗
NASA NTRS1989

Relativistic electrons at geosynchronous orbit, interplanetary electron flux, and the 13-month Jovian synodic year

Results are reported from a search to determine the correlation, if any, between the temporal behaviors of 0.2-7 MeV or higher electrons at GEO (6.6 earth radii) and 6-10 MeV electrons in the interplanetary region near earth at the period of the Jovian synodic year (about 13 months). The 13-month intensity variation results from the synodic interplanetary magnetic field conection of earth to Jupiter. Direct compariosn of intensity-time flux profiles for the years 1976-1984, about 7 synodic Jovian electron seasons, shows that the intensity envelope of peak electron flux at GEO does not appear to be correlated to the observed 13 month intensity envelope of relativistic electron flux in the interplanetary region near earth. A persistent 13-month variation of GEO flux is not obvious, thus indicating that the intensity of electron flux at GEO is not directly and soley related to the intensity of Jovian electron flux near earth. It is concluded that dynamic erergization and redistribution processes in earth's magnetosphere must be invoked to produce the intensity variations of relativistic electron flux at GEO and not interplanetary magnetic field connection to Jupiter.

Christon, S. P.↗
DOE OSTI2026

Discovery of correlated electron molecular orbital materials using graph representations

Correlated electron molecular orbital (CEMO) materials host emergent electronic states built from molecular orbitals localized over clusters of transition metal ions yet have historically been discovered sporadically and generally been treated as isolated case studies. Here we establish CEMO materials as a systematically discoverable class and introduce a graph-based framework to identify, classify, and organize transition-metal cluster motifs in inorganic solids. Starting from crystal structures in the Materials Project, we construct transition metal connectivity graphs, extract cluster motifs using a bond-cutting algorithm, and determine cluster point groups, effective cluster sublattice dimensionality, and translational symmetry. Applying this approach in a high-throughput screen of 34,548 compounds yields 5,306 cluster-containing materials, including 2,627 stable or metastable compounds with isolated clusters and 984 materials featuring mixed-metal clusters. The resulting dataset reveals symmetry and element dependent trends in cluster formation. By integrating cluster classification with flat band lattice topology and battery-relevant information, we provide further relevant information to multiple scientific communities. The accompanying open dataset, Cluster Finder software, and interactive web platform enable systematic exploration of cluster driven electronic phenomena and establish a general pathway for discovering correlated quantum materials and functional materials with cluster-based or extended metal-metal bonding in inorganic solids.

Akhond, Md. Rajbanul [Department of Chemistry, 800↗
DOE OSTI2025

Beyond Epitaxy: Ion Implantation as a Tool for Orbital Engineering

Manipulating electronic orbital states in quantum materials provides a powerful means of controlling their physical properties and technological functionality. Here, we demonstrate that orbital populations in strongly correlated oxide thin films can be continuously and reversibly tuned through postsynthesis He ion implantation. Using LaNiO 3 as a model system, we show that the orbital preference can be systematically adjusted from favoring in-plane d x 2 –y 2 occupation toward out-of-plane d z 2 states through precise control of ion fluence. Unlike conventional heteroepitaxial approaches that lock in orbital configurations during growth, this strain-doping technique enables continuous orbital tuning and the selective modification of specific film regions after device fabrication. We demonstrate the practical impact of this control by achieving a 7-fold enhancement in oxygen reduction reaction catalysis. This work establishes ion implantation as a powerful approach for orbital engineering that complements existing synthesis-based strategies while offering unique advantages for both basic research and device development.

Doping↗
DOE OSTI2024

Emergence of flat bands and ferromagnetic fluctuations via orbital-selective electron correlations in Mn-based kagome metal

Kagome lattice has been actively studied for the possible realization of frustration-induced two-dimensional flat bands and a number of correlation-induced phases. Currently, the search for kagome systems with a nearly dispersionless flat band close to the Fermi level is ongoing. Here, by combining theoretical and experimental tools, we present Sc 3 Mn 3 Al 7 Si 5 as a novel realization of correlation-induced almost-flat bands in the kagome lattice in the vicinity of the Fermi level. Our magnetic susceptibility, 27 Al nuclear magnetic resonance, transport, and optical conductivity measurements provide signatures of a correlated metallic phase with tantalizing ferromagnetic instability. Our dynamical mean-field calculations suggest that such ferromagnetic instability observed originates from the formation of nearly flat dispersions close to the Fermi level, where electron correlations induce strong orbital-selective renormalization and manifestation of the kagome-frustrated bands. In addition, a significant negative magnetoresistance signal is observed, which can be attributed to the suppression of flat-band-induced ferromagnetic fluctuation, which further supports the formation of flat bands in this compound. These findings broaden a new prospect to harness correlated topological phases via multiorbital correlations in 3d-based kagome systems.

36 MATERIALS SCIENCE↗