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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 919 records · Page 51
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Precise Linker Length and Dynamic Bond Exchange Control Penetrant Diffusion in Dense Vitrimers

Polymer networks with dynamic covalent bonds have been investigated for their self-healing ability, recyclability, and potential as more sustainable materials. Recent results have indicated that in some cases, bond exchange can enhance the transport of penetrants in dense networks, pointing to their potential for separations of membranes. Here, imine dynamic bonds in ethylene oxide (EO) networks with precise linker lengths were synthesized to investigate the transport of N,N′-bis(2,5-di-tert-butylphenyl)-3,4,9,10-perylenedicarboximide (BTBP), a large, anisotropic dye molecule. Networks with mesh sizes smaller than, comparable to, and greater than the size of the penetrant axes were investigated to probe the effects of bond exchange and network confinement on transport. Mesh sizes, which ranged from 0.5 to 1.62 nm, were determined from shear rheology, glass transitions by calorimetry, and probe diffusion coefficients by fluorescence recovery after photobleaching. Permanent networks with identical EO chain lengths were prepared as control samples, and up to a 3 orders of magnitude increase in diffusion coefficient is observed in the dynamic systems for short linkers containing 13 backbone atoms. The longest linkers with 71 backbone atoms show no difference between the permanent and dynamic networks. Linkers shorter than 11 backbone atoms, corresponding to a mesh size smaller than the penetrant small axis, diffusion is no longer observable on the experimental time scale, indicating a sharp cutoff attributed to the precise linkers and narrow mesh size distribution. The dynamic imine exchange time scales were compared to the diffusive hopping times of penetrants and indicate that exchange can occur during a diffusive displacement. Furthermore, these findings provide insights into the factors affecting penetrant transport in dense polymers and inspire the development of next-generation selective polymer membranes.

Diffusion↗
DOE OSTI2020

Quantifying the Dynamics of Protein Self-Organization Using Deep Learning Analysis of Atomic Force Microscopy Data

The dynamics of protein self-assembly on the inorganic surface and the resultant geometric patterns are visualized using high-speed atomic force microscopy. The time dynamics of the classical macroscopic descriptors such as 2D fast Fourier transforms, correlation, and pair distribution functions are explored using the unsupervised linear unmixing, demonstrating the presence of static ordered and dynamic disordered phases and establishing their time dynamics. Here, the deep learning (DL)-based workflow is developed to analyze detailed particle dynamics and explore the evolution of local geometries. Finally, we use a combination of DL feature extraction and mixture modeling to define particle neighborhoods free of physics constraints, allowing for a separation of possible classes of particle behavior and identification of the associated transitions. Overall, this work establishes the workflow for the analysis of the self-organization processes in complex systems from observational data and provides insight into the fundamental mechanisms.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Anaerobic Dynamic Membrane Bioreactor Development to Facilitate Organic Waste Conversion to Medium-Chain Carboxylic Acids and Their Downstream Recovery

Platform chemicals such as medium-chain carboxylic acids (MCCAs) can be produced from organic waste streams via chain elongation in anaerobic mixed-culture bioreactors. A product recovery system is needed to collect MCCAs from the bioreactor effluent. Membrane-based liquid–liquid extraction, the most commonly used product recovery approach, requires suspended solids removal from the bioreactor effluent to avoid membrane fouling. An anaerobic dynamic membrane bioreactor (AnDMBR) was developed to evaluate MCCA production from brewery and prefermented food waste and to produce a permeate with low suspended solids to facilitate downstream product recovery. The AnDMBR employed an inexpensive stainless-steel mesh as the support material for the development of a biofilm or dynamic membrane, which was responsible for solids–liquid separation. The AnDMBR produced a permeate quality with an average total suspended solids (TSS) concentration of 0.12 g L –1 , while the average bioreactor TSS concentration was two orders of magnitude higher (21.6 g L –1 ). A maximum solids removal efficiency of ≥99% was achieved and good permeate quality was sustained for over 200 days without fouling control or cleaning the support material. In addition to solids–liquid separation, the dynamic membrane was responsible for a substantial fraction of the biological activity of the AnDMBR. The relative activity of Clostridiales, as determined by 16S rRNA sequencing, correlated with MCCA production and was higher in the dynamic membrane (20.0 ± 4.9%) than in the suspended biomass (5.2 ± 2.7%) in the bioreactor. This observation was consistent with MCCA production data as the permeate MCCA concentrations were significantly (p = 8.2 × 10 –5 ) higher than that in the bioreactor, suggesting that the dynamic membrane biofilm contributed to chain elongation.

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

Dynamic Implications of Noncovalent Interactions in Amphiphilic Single-Chain Polymer Nanoparticles

Single-chain polymer nanoparticles (SCNPs) combine the chemical diversity of synthetic polymers with the intricate structure of biopolymers, generating versatile biomimetic materials. The mobility of polymer chain segments at length scales similar to secondary structural elements in proteins is critical to SCNP structure and thus function. However, the influence of noncovalent interactions used to form SCNPs (e.g., hydrogen-bonding and biomimetic secondary-like structure) on these conformational dynamics is challenging to quantitatively assess. To isolate the effects of noncovalent interactions on SCNP structure and conformational dynamics, we synthesized a series of amphiphilic copolymers containing dimethylacrylamide and monomers capable of forming these different interactions: (1) di(phenylalanine) acrylamide that forms intramolecular β-sheet-like cross-links, (2) phenylalanine acrylamide that forms hydrogen-bonds but lacks a defined local structure, and (3) benzyl acrylamide that has the lowest propensity for hydrogen-bonding. Each SCNP formed folded structures comparable to those of intrinsically disordered proteins, as observed by size exclusion chromatography and small angle neutron scattering. The dynamics of these polymers, as characterized by a combination of dynamic light scattering and neutron spin echo spectroscopy, was well described using the Zimm with internal friction (ZIF) model, highlighting the role of each noncovalent interaction to additively restrict the internal relaxations of SCNPs. These results demonstrate the utility of local scale interactions to control SCNP polymer dynamics, guiding the design of functional biomimetic materials with refined binding sites and tunable kinetics.

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

Correlating Broadband Photoluminescence with Structural Dynamics in Layered Hybrid Halide Perovskites

The emission of white light from a single material is atypical and is of interest for solid-state lighting applications. Broadband light emission has been observed in some layered perovskite derivatives, A 2 PbBr 4 (A = R-NH 3 + ), and correlates with static structural distortions corresponding to out-of-plane tilting of the lead bromide octahedra. While materials with different organic cations can yield distinct out-of-plane tilts, the underlying origin of the octahedral tilting remains poorly understood. Using high energy resolution (e.g., quasi-elastic) neutron scattering, this contribution details the rotational dynamics of the organic cations in A 2 PbBr 4 materials where A = n-butylammonium (nBA), 1,8-diaminooctammonium (ODA), and 4-aminobutyric acid (GABA). The organic cation dynamics differentiate (nBA) 2 PbBr 4 from (ODA)PbBr 4 or (GABA) 2 PbBr 4 in that the larger spatial extent of dynamics of nBA yields a larger effective cation radius. The larger effective volume of the nBA cation in (nBA) 2 PbBr 4 yields a closer to ideal A-site geometry, preventing the out-of-plane tilt and broadband luminescence. In all three compounds, we observe hydrogen dynamics attributed to rotation of the ammonium headgroup and at a time scale faster than the white light photoluminescence studied by time-correlated single photon counting spectroscopy. This supports a previous assignment of the broadband emission as resulting from a single ensemble, such that the emissive excited state experiences many local structures faster than the emissive decay. Furthermore, the findings presented here highlight the role of the organic cation and its dynamics in hybrid organic–inorganic perovskites and white light emission.

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

Understanding the Impacts of Support–Polymer Interactions on the Dynamics of Poly(ethyleneimine) Confined in Mesoporous SBA-15

Supported amines are a promising class of CO 2 sorbents offering large uptake capacities and fast uptake rates. Additionally, among supported amines, poly(ethyleneimine) (PEI) physically impregnated in the mesopores of SBA-15 silica is widely used. Within these composite materials, the chain dynamics and morphologies of PEI strongly influence the CO 2 capture performance, yet little is known about chain and macromolecule mobility in confined pores. Here, we probe the impact of the support–PEI interactions on the dynamics and structures of PEI at the support interface and the corresponding impact on CO 2 uptake performance, which yields critical structure–property relationships. The pore walls of the support are grafted with organosilanes with different chemical end groups to differentiate interaction modes (spanning from strong attraction to repulsion) between the pore surface and PEI. Combinations of techniques, such as quasi-elastic neutron scattering (QENS), 1 H T 1 –T 2 relaxation correlation solid-state NMR, and molecular dynamics (MD) simulations, are used to comprehensively assess the physical properties of confined PEI. We hypothesized that PEI would have faster dynamics when subjected to less attractive or repulsive interactions. However, we discover that complex interfacial interactions resulted in complex structure–property relationships. Indeed, both the chain conformation of the surface-grafted chains and of the PEI around the surface influenced the chain mobility and CO 2 uptake performance. By coupling knowledge of the dynamics and distributions of PEI with CO 2 sorption performance and other characteristics, we determine that the macroscopic structures of the hybrid materials dictate the first rapid CO 2 uptake, and the rate of CO 2 sorption during the subsequent gradual uptake stage is determined by PEI chain motions that promote diffusive jumps of CO 2 through PEI-packed domains.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2023

Rapid Electron Transfer Self-Exchange in Conformationally Dynamic Copper Coordination Complexes

Here we report the electron transfer (ET) self-exchange rate constants (k 11 ) for a pair of Cu II/I complexes utilizing dpa R (dpa = dipicolylaniline, R = OMe, SMe) ligands assessed by NMR line-broadening experiments. These ligands afford copper complexes that are conformationally dynamic in one oxidation state. With R = OMe, the Cu I complex is dynamic, while with R= SMe, the Cu II complex is dynamic. Both complexes exhibit unexpectedly large k 11 of 2.48(6) x 10 5 and 2.21(9) × 10 6 M –1 s –1 for [CuCl(dpa OMe )] +/0 and [CuCl(dpa SMe )] +/0 , respectively. Among the fastest reported for molecular copper coordination complexes to date, that of [CuCl(dpa SMe )] +/0 exceeds all others by an order of magnitude and compares only to those observed in type 1 blue copper proteins. The dynamicity of these complexes establish pre-steady-state con-formational equilibria that minimize the inner sphere reorganization energies to 0.71 and 0.62 eV for R = OMe and SMe, respectively. In contrast to the emphasis on rigidity in the formulation of entatic states applied to blue copper proteins, the success of these two systems highlight the relevance of conformational dynamicity in mediating rapid ET.

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

Quantifying Dynamic Water Storage in Unsaturated Bedrock with Borehole Nuclear Magnetic Resonance

Quantifying the volume of water that is stored in the subsurface is critical to studies of water availability to ecosystems, slope stability, and water-rock interactions. In a variety of settings, water is stored in fractured and weathered bedrock as rock moisture. However, few techniques are available to measure rock moisture in unsaturated rock, making direct estimates of water storage dynamics difficult to obtain. Here, we use borehole nuclear magnetic resonance (NMR) at two sites in seasonally dry California to quantify dynamic rock moisture storage. Additionally, we show strong agreement between NMR estimates of dynamic storage and estimates derived from neutron logging and mass balance techniques. The depths of dynamic storage are up to 9 m and likely reflect the depth extent of root water uptake. To our knowledge, these data are the first to quantify the volume and depths of dynamic water storage in the bedrock vadose zone via NMR.

58 GEOSCIENCES↗
DOE OSTI2021

Sensitivity of Carbonaceous Aerosol Properties to the Implementation of a Dynamic Aging Parameterization in the Regional Climate Model RegCM

Freshly emitted soot is hydrophobic, but condensation of secondary aerosols and coagulation with other particles modify its hygroscopic optical properties. This conversion is referred to as “aerosol aging.” Many climate models represent this aging process with a fixed aging time scale, whereas in reality, it is a dynamic process that depends on environmental conditions. Here, we implement a dynamic aging parameterization scheme in the regional climate model RegCM4 in place of the fixed aging timescale of 1.15 days (~27.6 h) and examine its impact on the aerosol life cycle over the Indian subcontinent. The conversion from hydrophobic to hydrophilic aerosol is usually lower than 27.6 h over the entire landmass and lower than 10 h over the polluted Indo-Gangetic Basin (IGB), with seasonal variability. Due to the implementation of the dynamic aging scheme, the column burden and surface mass concentration of carbonaceous aerosols increase during the drier season (December–February) when washout is negligible. The burden is reduced during the wet season (June–September) due to a more efficient washout except over the IGB, where a reduction in precipitation as a result of radiative feedbacks increases the aerosol concentrations. Over the polluted IGB, surface dimming increases due to the dynamic aging scheme, with the top of the atmosphere forcing remaining mostly unchanged. As a result, atmospheric heating increases by at least 1.2 W/m 2 . Our results suggest that climate models should incorporate dynamic aging for a more realistic representation of aerosol simulations, especially in highly polluted regions.

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

Empirical Dynamic Modeling Reveals Complexity of Methane Fluxes in a Temperate Salt Marsh

Abstract Methane dynamics within salt marshes are complex because vegetation types, temperature, oscillating water levels, and changes in salinity and redox conditions influence CH 4 production, consumption, oxidation, and emissions. These non‐linear and complex interactions among variables affect the traditionally expected functional relationships and present challenges for interpreting and developing process‐based models. We employed empirical dynamic modeling (EDM) and convergent cross mapping (CCM) as a novel approach for characterizing seasonal/multiday and diurnal CH 4 dynamics by inferring causal variables, lags, and interconnections among multiple biophysical variables within a temperate salt marsh using 5 years of eddy covariance data. EDM/CCM is a nonparametric approach capable of quantifying the coupling between variables while determining time scales where variable interactions are the most relevant. We found that gross primary productivity, tidal creek dissolved oxygen, and temperature were important for seasonal/multiday dynamics (rho = 0.73–0.80), while water level was most important for diurnal dynamics during both the growing and dormancy phenoperiods (rho = 0.72 and 0.56, respectively). Lags for the top‐ranked variables (i.e., gross primary productivity, dissolved oxygen, temperature, water level) occurred between 1 and 5 weeks at the seasonal scale and 1–24 hr at the diurnal scale. The EDM had high prediction capabilities for intra‐/inter‐seasonal patterns and annual CH 4 sums but had limitations in representing large, infrequent fluxes. Results highlight the importance of non‐linearity, drivers, lag times, and interconnections among multiple biophysical variables that regulate CH 4 fluxes in tidal wetlands. This research introduces a novel approach to examining CH 4 fluxes, which will aid in evaluating current paradigms in wetlands and other ecosystems.

Environmental Sciences & Ecology↗
DOE OSTI2023

Leveraging Groundwater Dynamics to Improve Predictions of Summer Low-Flow Discharges

Summer streamflow predictions are critical for managing water resources; however, warming-induced shifts from snow to rain regimes impact low-flow predictive models. Additionally, reductions in snowpack drive earlier peak flows and lower summer flows across the western United States increasing reliance on groundwater for maintaining summer streamflow. However, it remains poorly understood how groundwater contributions vary interannually. Here, we quantify recession limb groundwater (RLGW), defined as the proportional groundwater contribution to the stream during the period between peak stream flow and low flow, to predict summer low flows across three diverse western US watersheds. We ask (a) how do snow and rain dynamics influence interannual variations of RLGW contributions and summer low flows?; (b) which watershed attributes impact the effectiveness of RLGW as a predictor of summer low flows? Linear models reveal that RLGW is a strong predictor of low flows across all sites and drastically improves low-flow prediction compared to snow metrics at a rain-dominated site. Results suggest that strength of RLGW control on summer low flows may be mediated by subsurface storage. Subsurface storage can be divided into dynamic (i.e., variability saturated) and deep (i.e., permanently saturated) components, and we hypothesize that interannual variability in dynamic storage contribution to streamflow drives RLGW variability. In systems with a higher proportion of dynamic storage, RLGW is a better predictor of summer low flow because the stream is more responsive to dynamic storage contributions compared to deep-storage-dominated systems. Overall, including RLGW improved low-flow prediction across diverse watersheds.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2021

Pseudoknot length modulates the folding, conformational dynamics, and robustness of Xrn1 resistance of flaviviral xrRNAs

To understand how RNA dynamics is regulated and connected to its function, we investigate the folding, conformational dynamics and robustness of Xrn1 resistance of a set of flaviviral xrRNAs using SAXS, smFRET and in vitro enzymatic assay. Flaviviral xrRNAs form discrete ring-like 3D structures, in which the length of a conserved longrange pseudoknot (PK2) ranges from 2 bp to 7 bp. We find that xrRNAs’ folding, conformational dynamics and Xrn1 resistance are strongly correlated and highly Mg 2+ - dependent, furthermore, the Mg 2+ -dependence is modulated by PK2 length variations. xrRNAs with long PK2 require less Mg 2+ to stabilize its folding, exhibits reduced conformational dynamics and strong Xrn1 resistance even at low Mg 2+ , and tolerates mutations at key tertiary motifs at high Mg 2+ , which generally are destructive to xrRNAs with short PK2. These results demonstrate an unusual regulatory mechanism of RNA dynamics providing insights into the functions and future biomedical applications of xrRNAs.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2023

Persistent dynamic magnetic state in artificial honeycomb spin ice

Abstract Topological magnetic charges, arising due to the non-vanishing magnetic flux on spin ice vertices, serve as the origin of magnetic monopoles that traverse the underlying lattice effortlessly. Unlike spin ice materials of atomic origin, the dynamic state in artificial honeycomb spin ice is conventionally described in terms of finite size domain wall kinetics that require magnetic field or current application. Contrary to this common understanding, here we show that a thermally tunable artificial permalloy honeycomb lattice exhibits a perpetual dynamic state due to self-propelled magnetic charge defect relaxation in the absence of any external tuning agent. Quantitative investigation of magnetic charge defect dynamics using neutron spin echo spectroscopy reveals sub-ns relaxation times that are comparable to the relaxation of monopoles in bulk spin ices. Most importantly, the kinetic process remains unabated at low temperature where thermal fluctuation is negligible. This suggests that dynamic phenomena in honeycomb spin ice are mediated by quasi-particle type entities, also confirmed by dynamic Monte-Carlo simulations that replicate the kinetic behavior. Our research unveils a macroscopic magnetic particle that shares many known traits of quantum particles, namely magnetic monopole and magnon.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Quantum fluctuations lead to glassy electron dynamics in the good metal regime of electron doped KTaO 3

One of the central challenges in condensed matter physics is to comprehend systems that have strong disorder and strong interactions. In the strongly localized regime, their subtle competition leads to glassy electron dynamics which ceases to exist well before the insulator-to-metal transition is approached as a function of doping. Here, we report on the discovery of glassy electron dynamics deep inside the good metal regime of an electron-doped quantum paraelectric system: KTaO 3 . We reveal that upon excitation of electrons from defect states to the conduction band, the excess injected carriers in the conduction band relax in a stretched exponential manner with a large relaxation time, and the system evinces simple aging phenomena—a telltale sign of glassy dynamics. Most significantly, we observe a critical slowing down of carrier dynamics below 35 K, concomitant with the onset of quantum paraelectricity in the undoped KTaO 3 . Our combined investigation using second harmonic generation technique, density functional theory and phenomenological modeling demonstrates quantum fluctuation-stabilized soft polar modes as the impetus for the glassy behavior. This study addresses one of the most fundamental questions regarding the potential promotion of glassiness by quantum fluctuations and opens a route for exploring glassy dynamics of electrons in a well-delocalized regime.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

Dynamical phase-field model of coupled electronic and structural processes

Abstract Many functional and quantum materials derive their functionality from the responses of both their electronic and lattice subsystems to thermal, electric, and mechanical stimuli or light. Here we propose a dynamical phase-field model for predicting and modeling the dynamics of simultaneous electronic and structural processes and the accompanying mesoscale pattern evolution under static or ultrafast external stimuli. As an illustrative example of application, we study the transient dynamic response of ferroelectric domain walls excited by an ultrafast above-bandgap light pulse. We discover a two-stage relaxational electronic carrier evolution and a structural evolution containing multiple oscillational and relaxational components across picosecond to nanosecond timescales. The phase-field model offers a general theoretical framework which can be applied to a wide range of functional and quantum materials with interactive electronic and lattice orders and phase transitions to understand, predict, and manipulate their ultrafast dynamics and rich mesoscale evolution dynamics of domains, domain walls, and charges.

36 MATERIALS SCIENCE↗
DOE OSTI2023

Machine learning nonequilibrium electron forces for spin dynamics of itinerant magnets

Abstract We present a generalized potential theory for conservative as well as nonconservative forces for the Landau-Lifshitz magnetization dynamics. Importantly, this formulation makes possible an elegant generalization of the Behler-Parrinello machine learning (ML) approach, which is a cornerstone of ML-based quantum molecular dynamics methods, to the modeling of force fields in adiabatic spin dynamics of out-of-equilibrium itinerant magnetic systems. We demonstrate our approach by developing a deep-learning neural network that successfully learns the electron-mediated exchange fields in a driven s-d model computed from the nonequilibrium Green’s function method. We show that dynamical simulations with forces predicted from the neural network accurately reproduce the voltage-driven domain-wall propagation. Our work also lays the foundation for ML modeling of spin transfer torques and opens a avenue for ML-based multi-scale modeling of nonequilibrium dynamical phenomena in itinerant magnets and spintronics.

36 MATERIALS SCIENCE↗
DOE OSTI2024

Nanosecond solvation dynamics in a polymer electrolyte for lithium batteries

Solvation dynamics critically affect charge transport. Spectroscopic experiments and computer simulations show that these dynamics in aqueous systems occur on a picosecond timescale. In the case of organic electrolytes, however, conflicting values ranging from 1 to several 100 picoseconds have been reported. We resolve this conflict by studying mixtures of an organic polymer and a lithium salt. Lithium ions coordinate with multiple polymer chains, resulting in temporary crosslinks. Relaxation of these crosslinks, detected by quasielastic neutron scattering, are directly related to solvation dynamics. Simulations reveal a broad spectrum of relaxation times. The average timescale for solvation dynamics in both experiment and simulation is one nanosecond. Here we present the direct measurement of ultraslow dynamics of solvation shell break-up in an electrolyte.

25 ENERGY STORAGE↗
DOE OSTI2023

Operando characterization and regulation of metal dissolution and redeposition dynamics near battery electrode surface

Mn dissolution has been a longstanding, ubiquitous issue that negatively impacts the performance of Mn-based battery materials. Mn dissolution involves complex chemical and structural transformations at the electrode-electrolyte interface. The continuously evolving electrodeelectrolyte interface has posed great challenges for characterizing the dynamic interfacial process and quantitatively establishing the correlation with battery performance. In this study, we visualize and quantify the temporally and spatially resolved Mn dissolution/redeposition (D/R) dynamics of electrochemically operating Mn-containing cathodes. The particle-level and electrode-level analyses reveal that the D/R dynamics is associated with distinct interfacial degradation mechanisms at different states of charge. Our results statistically differentiate the contributions of surface reconstruction and Jahn-Teller distortion to the Mn dissolution at different operating voltages. Introducing sulfonated polymers (Nafion) into composite electrodes can modulate the D/R dynamics through trapping the dissolved Mn species and rapidly establishing the local Mn D/R equilibrium. This work represents an inaugural effort to pinpoint the chemical and structural transformations responsible for Mn dissolution via an operando synchrotron study and develops an effective method to regulate Mn interfacial dynamics for improving battery performance.

25 ENERGY STORAGE↗