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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 1,369 records · Page 76
All sourcesNASA NTRSDOE OSTI
DOE OSTI2023

Graphic contrastive learning analyses of discontinuous molecular dynamics simulations: Study of protein folding upon adsorption

A comprehensive understanding of the interfacial behaviors of biomolecules holds great significance in the development of biomaterials and biosensing technologies. In this work, we used discontinuous molecular dynamics (DMD) simulations and graphic contrastive learning analysis to study the adsorption of ubiquitin protein on a graphene surface. Our high-throughput DMD simulations can explore the whole protein adsorption process including the protein structural evolution with sufficient accuracy. Contrastive learning was employed to train a protein contact map feature extractor aiming at generating contact map feature vectors. Subsequently, these features were grouped using the k-means clustering algorithm to identify the protein structural transition stages throughout the adsorption process. The machine learning analysis can illustrate the dynamics of protein structural changes, including the pathway and the rate-limiting step. Our study indicated that the protein–graphene surface hydrophobic interactions and the π–π stacking were crucial to the seven-stage adsorption process. Upon adsorption, the secondary structure and tertiary structure of ubiquitin disintegrated. The unfolding stages obtained by contrastive learning-based algorithm were not only consistent with the detailed analyses of protein structures but also provided more hidden information about the transition states and pathway of protein adsorption process and structural dynamics. Our combination of efficient DMD simulations and machine learning analysis could be a valuable approach to studying the interfacial behaviors of biomolecules.

97 MATHEMATICS AND COMPUTING↗
DOE OSTI2022

Determination of the structure of lithium niobosilicate glasses by molecular dynamics simulation with a new Nb-O potential

A partial charge empirical potential for the Nb-O pair has been developed based on existing parameters of other pairs in a Teter potential to enable molecular dynamics simulations of both lithium niobate crystal and lithium niobosilicate glasses. The developed potential is capable of describing structural features of lithium niobosilicate glasses in a wide composition range, including niobium coordination number and bond length, density, bond angle distribution, polyhedral distribution and fraction of bridging oxygen. Furthermore, the results obtained using this new potential show good agreement with experimental data of density and structure from Raman spectroscopy of lithium niobosilicate glasses and X-ray absorption spectroscopy near Nb K-edge.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Final Technical Report

The capture of CO2 and its simultaneously conversion to useful chemical fuels driven by solar energy represents one of the best solutions to resolve our growing energy and environmental concerns. The most critical challenge to this endeavor is the rational design of a photocatalytic architecture that can effectively couple a given photosensitizer (PS) with an appropriate catalyst, thereby enabling efficient photosensitization of a multi-electron reduction catalysis. This research program aims to address this challenge using an interdisciplinary approach that combines innovative material design and synthesis, fundamental mechanistic studies, and photocatalytic performance evaluation. The strategies include 1) constructing and investigating a novel class of 2D COF hybrid photocatalysts with an effective photoactive organic building block as PS and a precisely incorporated CO2 reduction molecular catalyst (MC); and 2) mechanistic origins of CO2 photoreduction using a set of complementary time-resolved and in situ spectroscopic techniques. The novelty of the proposed hybrid system lies in the unprecedented combination of the unique advantage of porous crystalline COF PS with the precise catalytic function of MC for photocatalytic CO2 reduction. In the periods of the support (09/01/2019-12/31/2022), we have made research progress in four projects: 1) Exploring 2D COFs with incorporated Mn complex for light driven CO2 reduction; 2) The dependence of excited state and charge transfer dynamics on monomer structure of 2D COFs; and 3) Control over Charge Separation by Imine Structural Isomerization in Covalent Organic Frameworks with Implications on CO2 Photoreduction; and 4) The impact of monomer structure on the photoluminescence properties of COFs. We found that both monomer structure and linker chemistry can effectively impact the excited state dynamics, charge transfer properties, and photoluminescence quantum yields, the important properties that dictate their applications in photocatalysis. In addition, we found that the direction of imine linker determines charge transfer direction and thus controls the types of catalytic reactions (e.g. water oxidation or CO2 reduction reactions). The result from these fundamental studies provides important information for correlating the structure of the COF photocatalysts with their photophysical properties and catalytic functions, paving the way for their novel application in photocatalysis. We expect that our findings will contribute to addressing current shortcomings of semiconductor- and molecular-based photocatalytic systems that suffer from inefficient light harvesting and charge separation and poor adsorption and activation of reactants. In turn, this research will contribute towards the development of novel photocatalytic systems for CO2 reduction to generate renewable chemical fuels and simultaneously address the problem of mitigating climate change due to CO2 accumulation. In addition, the experimental approaches employed in this research can be easily transferred to other energy technologies and are expected to broadly impact fields involving photocatalysis, optoelectronic devices, and solar energy conversion. The proposed research has also been integrated with educational activities and serve as a basis to raise awareness around the critical issues of global energy production and consumption, and to develop the next generation of solar energy scientists.

14 SOLAR ENERGY↗
DOE OSTI2025

On-chip terahertz emission from Floquet-Bloch states [Invited]

Floquet engineering uses time-periodic electromagnetic fields to modify the electronic properties of quantum materials via the creation of Floquet-Bloch states. These photon-dressed states inherit features from both the material and the driving field, enabling the exploration and control of quantum phenomena in light-matter hybrid systems. In non-centrosymmetric materials, shift currents can arise from the quantum geometric properties of electronic wavefunctions. However, shift currents from Floquet-Bloch states remain experimentally unexplored. Here, we employ an on-chip optoelectronic circuit to detect intrinsic terahertz emission from Floquet-Bloch states in T d -WTe 2 under intense optical driving. We observe strong edge-localized terahertz emission that scales linearly with the driving field, consistent with the theoretical prediction for shift currents generated by Floquet-Bloch states. The results advance our understanding of strongly driven quantum materials and provide insights for developing efficient, bias-free terahertz sources for future optoelectronic technologies.

Li, Xinyu [Max Planck Institute for the Structure ↗
DOE OSTI2024

Tracking dissociation pathways of nitrobenzene via mega-electron-volt ultrafast electron diffraction

As the simplest nitroaromatic compound, nitrobenzene is an interesting model system to explore the rich photochemistry of nitroaromatic compounds. Previous investigations of nitrobenzene's photochemical dynamics have probed structural and electronic properties. These investigations paint, at times, a convoluted and sometimes contradictory description of the photochemical landscape. Here, we investigate the ultrafast dynamics of nitrobenzene triggered by photoexcitation at 267 nm for the first time using a structural probe with femtosecond time resolution. Our probe complements previous measurements of nitrobenzene's electronic structure evolution and aids in determining the photochemical dynamics with less ambiguity. We employ megaelectronvolt ultrafast electron diffraction to follow nitrobenzene's structural evolution within the first 5 ps after photoexcitation. We observe ground state recovery within 160 ± 60 fs through nonadiabatic dynamics. Based on comparisons of the experimental signal with molecular dynamics simulations, we exclude a significant population of the triplet manifold. Furthermore, we do not observe fragmentation of nitrobenzene within the investigated time window, which indicates that previously observed photofragmentation reactions take place in the vibrationally 'hot' ground state on timescales considerably beyond 5 ps.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2022

Oxygen vacancy dynamics in monoclinic metallic VO 2 domain structures

It was demonstrated recently that the nano-optical and nanoelectronic properties of VO 2 can be spatially programmed through the local injection of oxygen vacancies by atomic force microscope writing. In this work, we study the dynamic evolution of the patterned domain structures as a function of the oxygen vacancy concentration and the time. A threshold doping level is identified that is critical for both the metal–insulator transition and the defect stabilization. The diffusion of oxygen vacancies in the monoclinic phase is also characterized, which is directly responsible for the short lifetimes of sub-100 nm domain structures. This information is imperative for the development of oxide nanoelectronics through defect manipulations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2021

Fine structure of pentaquark multiplets in the dynamical diquark model

In this work, we apply the dynamical diquark model to predict the spectrum of hidden-charm pentaquark states in both unflavored and open-strange sectors. Using only Hamiltonian parameters introduced in the tetraquark S - and P -wave multiplets, the model naturally produces the level spacing supported by the most recent LHCb results for P c structures. Furthermore, using model inputs obtained from data of hidden-charm, open-strange tetraquarks ( Z c s ), we predict the spectrum of P c s states, including the recently observed P c s ( 4459 ) . We find all pentaquark candidates observed to date to belong to the 1 P multiplet and hence have positive parity.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Nanoscale Ion Transport Enhances Conductivity in Solid Polymer-Ceramic Lithium Electrolytes

The predictive design of flexible and solvent-free polymer electrolytes for solid-state batteries requires an understanding of the fundamental principles governing the ion transport. In this work, we establish a correlation among the composite structures, polymer segmental dynamics, and lithium ion (Li + ) transport in a ceramic-polymer composite. Elucidating this structure–property relationship will allow tailoring of the Li + conductivity by optimizing the macroscopic electrochemical stability of the electrolyte. The ion dissociation from the slow polymer segmental dynamics was found to be enhanced by controlling the morphology and functionality of the polymer/ceramic interface. The chemical structure of the Li + salt in the composite electrolyte was correlated with the size of the ionic cluster domains, the conductivity mechanism, and the electrochemical stability of the electrolyte. Polyethylene oxide (PEO) filled with lithium bis(trifluoromethanesulfonyl)imide (LiTFSI) or lithium bis(fluorosulfonyl) imide (LiFSI) salts was used as a matrix. A garnet electrolyte, aluminum substituted lithium lanthanum zirconium oxide (Al-LLZO) with a planar geometry, was used for the ceramic nanoparticle moieties. Further, the dynamics of the strongly bound and highly mobile Li + were investigated using dielectric relaxation spectroscopy. The incorporation of the Al-LLZO platelets increased the number density of more mobile Li + . The structure of the nanoscale ion-agglomeration was investigated by small-angle X-ray scattering, while molecular dynamics (MD) simulation studies were conducted to obtain the fundamental mechanism of the decorrelation of the Li + in the LiTFSI and LiFSI salts from the long PEO chain.

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

Lattice dynamics of the hybrid improper ferroelectrics (Ca, Sr) 3 Ti 2 O 7

The structure and lattice dynamics of the hybrid improper ferroelectric compound Ca 3 - x Sr x Ti 2 O 7 (for x = 0 , 0.6 , and 0.9) have been studied with a combination of diffraction, inelastic scattering experiments, Raman spectroscopy, and calorimetry measurements, as well as first-principles simulations. Using inelastic neutron scattering, we have measured the phonon density of states (DOS) for x = 0.9 , which revealed a strong broadening but little change in phonon energies on heating from 10 K to 728 K across the ferroelectric phase transition temperature, T F E . Using inelastic x-ray scattering, the momentum-resolved phonon dispersions were measured from 80 K to 950 K on a single crystal (for x = 0.6 ), and also revealed a strong phonon broadening but a small energy shift for acoustic modes on heating across T F E . Additionally, our Raman measurements (for x = 0.6 ) showed robust rotational and oxygen breathing modes but soft tilt modes, consistent with previous measurements on similar compounds. Our density functional calculations achieve good agreement with both the phonon DOS and dispersions measured. We did not observe any unusual quadratic dispersion for c -polarized transverse acoustic modes, at odds with a recently predicted quasi-2D character, for either undoped ( x = 0 ) or doped ( x = 0.6 ) compounds. 0.6) compounds.

36 MATERIALS SCIENCE↗
DOE OSTI2024

On the importance of species immiscibility in mixing-layer dynamics at supercritical pressures

The mixing dynamics of injected propellants is a key factor in determining the ignition performance and combustion-instability response of rocket engines, internal combustion engines, and gas turbines. A key source of uncertainty in the prediction of phase-exchange dynamics is the immiscibility of the injected propellants at supercritical pressure conditions, which induces liquid/vapor phase separation and surface-tension dynamics. While experimental observations indicate the presence of liquid/vapor interfacial structures, this interfacial dynamics is typically neglected in numerical analyses. To address this issue, the objective of the present study is to systematically evaluate the importance of species immiscibility on the phase-exchange dynamics of cryogenic LOX/GH2 mixing layers at typical rocket engine injection conditions. This is accomplished by comparing simulations of (i) a recently developed interface-capturing Regularized-Interface Method (RIM) formulation, and (ii) the commonly employed Diffuse-Interface Method (DIM) formulation. Analysis shows that the interfacial dynamics significantly impact the atomization and mixing of the propellants in the near-injector region, which is not captured by the DIM formulation. The findings of this study extend to other immiscible injection systems, such as LOX/kerosene and hydrocarbon-fuel/air, thereby highlighting the importance of resolving species immiscibility in simulating high-pressure combustion engines.

diffused-interface method↗
DOE OSTI2020

Probing the Electronic Structure of Warm Dense Nickel via Resonant Inelastic X-Ray Scattering

The development of bright free-electron lasers (FEL) has revolutionized our ability to create and study matter in the high-energy-density (HED) regime. Current diagnostic techniques have been successful in yielding information on fundamental thermodynamic plasma properties, but provide only limited or indirect information on the detailed quantum structure of these systems, and on how it is affected by ionization dynamics. In this work we show how the valence electronic structure of solid-density nickel, heated to temperatures of around 10 of eV on femtosecond timescales, can be probed by single-shot resonant inelastic x-ray scattering (RIXS) at the Linac Coherent Light Source FEL. The RIXS spectrum provides a wealth of information on the HED system that goes well beyond what can be extracted from x-ray absorption or emission spectroscopy alone, and is particularly well suited to time-resolved studies of electronic-structure dynamics.

36 MATERIALS SCIENCE↗
DOE OSTI2025

Cavity electrodynamics of van der Waals heterostructures

Van der Waals heterostructures host many-body quantum phenomena that are tunable in situ using electrostatic gates. Their constituent two-dimensional materials and gates can naturally form plasmonic self-cavities, confining light in standing waves of current density due to finite-size effects. The plasmonic resonances of typical graphite gates fall in the gigahertz to terahertz range, corresponding to the same microelectronvolt to millielectronvolt energy scale as the phenomena in van der Waals heterostructures that they electrically control. This raises the possibility that the built-in cavity modes of graphite gates are relevant for shaping the low-energy physics of these heterostructures. However, probing these cavity-coupled electrodynamics is challenging as devices are notably smaller than the diffraction limit at the relevant wavelengths. Here we report on the intrinsic cavity conductivity of gate-tunable graphene heterostructures. As the carrier density is tuned, we observe coupling and spectral weight transfer between graphene and graphite plasmonic cavity modes in the ultrastrong coupling regime. We present an analytical model to describe the results and provide general principles for cavity design. Our findings show that intrinsic cavity effects are important for understanding the low-energy electrodynamics of van der Waals heterostructures and open a pathway for useful functionality through cavity control.

Electronic properties and materials↗
DOE OSTI2020

TeraChem: A graphical processing unit-accelerated electronic structure package for large-scale ab initio molecular dynamics

TeraChem was born in 2008 with the goal of providing fast on-the-fly electronic structure calculations to facilitate ab initio molecular dynamics studies of large biochemical systems such as photoswitchable proteins and multichromophoric antenna complexes. Originally developed for videogaming applications, graphics processing units (GPUs) offered a low-cost parallel computer architecture that became more accessible for general-purpose GPU computing with the release of CUDA in 2007. The evaluation of the electron repulsion integrals (ERIs) is a major bottleneck in electronic structure codes and provides an attractive target for acceleration on GPUs. Thus, highly efficient routines for evaluation of and contractions between the ERIs and density matrices were implemented in TeraChem. Here, electronic structure methods were developed and implemented to leverage these integral contraction routines, resulting in the first quantum chemistry package designed from the ground up for GPUs. This GPU acceleration makes TeraChem capable of performing large-scale ground and excited state calculations in the gas and condensed phase. Today, TeraChem's speed forms the basis for a suite of quantum chemistry applications, including optimization and dynamics of proteins, automated and interactive chemical discovery tools, and large-scale nonadiabatic dynamics simulations.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2024

ELECTRONIC STRUCTURE METHODS AND PROTOCOLS WITH APPLICATION TO DYNAMICS, KINETICS AND THERMOCHEMISTRY

Hydrocarbon combustion involves the reaction dynamics of a tremendous number of species beginning with many-component fuel mixtures and proceeding via a complex system of intermediates to form primary and secondary products. Combustion conditions corresponding to new advanced engines and/or alternative fuels rely increasingly on autoignition and low-temperature-combustion chemistry. In these regimes various transient radical species such as HO2, ROO·, ·QOOH, HCO, NO2, HOCO, and Criegee intermediates play important roles in determining the detailed as well as more general dynamics. A clear understanding and accurate representation of these processes is needed for effective modeling. Given the difficulties associated with making reliable experimental measurements of these systems, computation can play an important role in developing these energy technologies. Accurate calculations have their own challenges since even within the simplest dynamical approximations such as transition state theory, the rates depend exponentially on critical barrier heights and these may be sensitive to the level of quantum chemistry. Moreover, it is well-known that in many cases it is necessary to go beyond statistical theories and consider the dynamics. Quantum tunneling, resonances, radiative transitions, and non-adiabatic effects governed by spin-orbit or derivative coupling can be determining factors in those dynamics. Building upon progress made during a period of prior support through the DOE Early Career Program, this project combines developments in the areas of potential energy surface (PES) fitting and multistate multireference quantum chemistry to allow spectroscopically and dynamically/kinetically accurate investigations of key molecular systems (such as those mentioned above), many of which are radicals with strong multireference character and have the possibility of multiple electronic states contributing to the observed dynamics. An ongoing area of investigation is to develop general strategies for robustly convergent electronic structure theory for global multichannel reactive surfaces including diabatization of energy and other relevant surfaces such as dipole transition. Combining advances in ab initio methods with automated interpolative PES fitting allows the construction of high-quality PESs (incorporating thousands of high-level data) to be done rapidly through parallel processing on high-performance computing (HPC) clusters. In addition, new methods and approaches to electronic structure theory will be developed and tested through applications. This project will explore limitations in traditional multireference calculations (e.g., MRCI) such as those imposed by internal contraction, lack of high-order correlation treatment and poor scaling. Methods such as DMRG-based extended active-space CASSCF and various Quantum Monte Carlo (QMC) methods will be applied (including VMC/DMC and FCIQMC). Insight into the relative significance of different orbital spaces and the robustness of application of these approaches on leadership class computing architectures will be gained. Synergy with other components of this research program such as automated PES fitting and multireference quantum chemistry will be used to address challenges encountered by the standard approaches to computational thermochemistry (those being single-reference quantum chemistry and perturbative treatments of the anharmonic vibrational energy, which break down for some cases of electronic structure or floppy strongly coupled vibrational modes).

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Shaker-structure interaction modeling and analysis for nonlinear force appropriation testing

Nonlinear force appropriation is an extension of its linear counterpart where sinusoidal excitation is applied to a structure with a modal shaker and phase quadrature is achieved between the excitation and response. While a standard practice in modal testing, modal shaker excitation has the potential to alter the dynamics of the structure under test. Previous studies have been conducted to address several concerns, but this work specifically focuses on a shaker-structure interaction phenomenon which arises during the force appropriation testing of a nonlinear structure. Under pure-tone sinusoidal forcing, a nonlinear structure may respond not only at the fundamental harmonic but also potentially at sub- or superharmonics, or it can even produce aperiodic and chaotic motion in certain cases. Shaker-structure interaction occurs when the response physically pushes back against the shaker attachment, producing non-fundamental harmonic content in the force measured by the load cell, even for pure tone voltage input to the shaker. This work develops a model to replicate these physics and investigates their influence on the response of a nonlinear normal mode of the structure. Experimental evidence is first provided that demonstrates the generation of harmonic content in the measured load cell force during a force appropriation test. This interaction is replicated by developing an electromechanical model of a modal shaker attached to a nonlinear, three-mass dynamical system. Several simulated experiments are conducted both with and without the shaker model in order to identify which effects are specifically due to the presence of the shaker. Finally, the results of these simulations are then compared to the undamped nonlinear normal modes of the structure under test to evaluate the influence of shaker-structure interaction on the identified system’s dynamics.

42 ENGINEERING↗
DOE OSTI2021

Revealing the Dynamics and Roles of Iron Incorporation in Nickel Hydroxide Water Oxidation Catalysts

We report the surface of an electrocatalyst undergoes dynamic chemical and structural transformations under electro-chemical operating conditions. There is a dynamic exchange of metal cations between the electrocatalyst and electrolyte. Understanding how iron in the electrolyte gets incorporated in the nickel hydroxide electrocatalyst is critical for pinpointing the roles of Fe during water oxidation. Here, we report that iron incorporation and oxygen evolution reaction (OER) are highly coupled, especially at high working potentials. The iron incorporation rate is much higher at OER potentials than that at the OER dormant state (low potentials). At OER potentials, iron incorporation favors electrochemically more reactive edge sites, as visualized by synchrotron X-ray fluorescence microscopy. Using X-ray absorption spectroscopy and density functional theory calculations, we show that Fe incorporation can suppress the oxidation of Ni and enhance the Ni reducibility, leading to improved OER catalytic activity. Our findings provide a holistic approach to understanding and tailoring Fe incorporation dynamics across the electrocatalyst-electrolyte interface, thus controlling catalytic processes.

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

Investigating Bacterial-Fungal Interactions using Fungal Highway Columns in Diverse Environments and Substrates

Bacterial-fungal interactions (BFIs) play an integral role in shaping microbial community composition, biogeochemical functions, spatial dynamics, and microbial dispersal. Mycelial networks created by filamentous fungi or other filamentous microorganisms (e.g., Oomycetes) act as 'fungal highways' that can be utilized by bacteria for transport throughout heterogeneous environments, greatly facilitating their mobility and granting them access to regions that may be challenging or impossible to reach on their own (e.g., due to air pockets within the soil). Several devices and experimental protocols have been created to study these fungal highways, including fungal highway columns. The fungal highway column designed by our group can be used for a variety of in situ or in vitro applications, as well as with diverse environmental and host-associated sample types. Herein, we describe the methods for performing experiments with these columns, including designing, printing, sterilizing, and preparing the devices. The options for analyzing data obtained from the use of these devices are also discussed here, and troubleshooting advice regarding potential pitfalls associated with experiments using fungal highway columns is offered. These devices can be used to gain a more comprehensive understanding of the diversity, mechanisms, and dynamics of fungal highway BFIs to provide valuable insights into the structural and functional dynamics within complex environments (e.g., soils) and across diverse habitats in which bacteria and fungi co-exist.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Atomic-Scale Visualization of Surface Segregation and Ordering of Pt in a Dilute Cu(Pt) Alloy under a Hydrogen Atmosphere

Surface segregation is a common phenomenon in alloys exposed to reactive atmospheres, yet the atomic mechanisms underlying surface structure and composition dynamics remain largely unexplored. Using a combination of environmental transmission electron microscopy observations and atomistic modeling, here we report the surface segregation process of Pt atoms in a dilute Pt(Cu) alloy and determine the distribution of Pt atoms at both atomically flat and stepped surfaces of the Pt(Cu) alloy at elevated temperatures and in a hydrogen gas atmosphere. Through directly probing Pt segregation, we find that Pt atoms segregated on the (100) surface exhibit a p(2 × 2) ordering, with ~25% Pt occupancy. In contrast, on the stepped (410) surface, hydrogen adsorption induces Pt segregation, initially occurring at the step edges, which then expands to the terrace sites upon increased hydrogen coverage, resulting in an ordered distribution of segregated Pt atoms with ~22% occupancy. Finally, these observations offer mechanistic insights into the structure and composition dynamics of the topmost atomic layer of the alloy in response to environmental stimuli and hold practical implications for the design and optimization of catalysts based on Pt group metals.

36 MATERIALS SCIENCE↗