Search NASA⌕ Search

SEARCH · Search NASA

Results for “Reaction dynamics”

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.

Quote a phrase for an exact phrase match. Source license links do not imply unrestricted reuse.

At least 109 records · Page 6
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

Deep learning-enabled probing of irradiation-induced defects in time-series micrographs

Modeling time-series data with convolutional neural networks (CNNs) requires building a model to learn in batches as opposed to training sequentially. Coupling CNNs with in situ or operando techniques opens the possibility of accurately segmenting dynamic reactions and mass transport phenomena to understand how materials behave under the conditions in which they are used. In this article, in situ ion irradiation transmission electron microscopy (TEM) images are used as inputs into the CNN to assess the defect generation rate, defect cluster density, and saturation of defects. We then use the output segmentation maps to correlate with conventional TEM micrographs to assess the model’s ability to detail nanoscale interactions. Next, we discuss the implications of preprocessing and hyperparameters on model variability, accuracy when expanded to other datasets, and the role of regularization when controlling model variance. Ultimately, we eliminate human bias when extrapolating physical metrics, speed up analysis time, decouple reactions that happen at 100 ms intervals, and deploy models that are both accurate and transferable to similar experiments.

Burns, Kory (ORCID:0000000158019909)↗
DOE OSTI2025

Direct structural retrieval from gas-phase ultrafast diffraction data using a genetic algorithm

Ultrafast scattering techniques such as ultrafast electron diffraction and ultrafast x-ray diffraction have been utilized to elucidate the structural dynamics, reaction intermediates, and final products in molecular reactions following photoexcitation. The time-dependent structures are typically not directly retrieved from the experimental data, but they rely on comparison with calculations. The genetic algorithm (GA), a global optimization strategy, can be used to retrieve the molecular structures directly from diffraction patterns without any theoretical input. However, the robustness of the GA with respect to real experimental conditions such as a limited momentum transfer range, noise, and artifacts has not been studied in detail. In this work, we characterize the performance of the GA with simulated data that mimic realistic experimental conditions. We have developed and implemented a variant of the GA specific to diffraction measurements which performs better in the presence of imperfect data compared to the standard implementation of the GA. We demonstrate this method with both synthetic data and experimental ultrafast electron diffraction data on the UV-induced photodissociation of trifluoroiodomethane (C⁢F 3⁡ I) molecules.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2026

New framework for extracting GPDs from exclusive photon electroproduction

Recently, a new framework for studying generic 2 → 3 hard exclusive reactions, referred to as single-diffractive hard exclusive processes, has been introduced to provide a cleaner separation of the underlying physical mechanisms. In this work, we expand this formalism to the case of exclusive real-photon electroproduction off a nucleon, 𝑒⁡(ℓ) +𝑁⁡(𝑝) →𝑒⁡(ℓ′) +𝑁⁡(𝑝′) + 𝛾⁡(𝑞′), which represents the classical channel for accessing generalized parton distributions (GPDs) in nucleons and nuclei. This extension enables a more systematic and physically transparent formulation of the reaction dynamics, paving the way for improved extractions of GPDs from experimental data as compared to existing approaches.

Qiu, Jian-Wei [Thomas Jefferson National Accelerat↗
DOE OSTI2022

The time-resolved atomic, molecular and optical science instrument at the Linac Coherent Light Source

The newly constructed time-resolved atomic, molecular and optical science instrument (TMO) is configured to take full advantage of both linear accelerators at SLAC National Accelerator Laboratory, the copper accelerator operating at a repetition rate of 120 Hz providing high per-pulse energy as well as the superconducting accelerator operating at a repetition rate of about 1 MHz providing high average intensity. Both accelerators power a soft X-ray free-electron laser with the new variable-gap undulator section. With this flexible light source, TMO supports many experimental techniques not previously available at LCLS and will have two X-ray beam focus spots in line. Thereby, TMO supports atomic, molecular and optical, strong-field and nonlinear science and will also host a designated new dynamic reaction microscope with a sub-micrometer X-ray focus spot. The flexible instrument design is optimized for studying ultrafast electronic and molecular phenomena and can take full advantage of the sub-femtosecond soft X-ray pulse generation program.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗
DOE OSTI2025

In situ atomic-resolution imaging of water vapor–driven multistep oxidation dynamics in strontium cobaltite

Understanding how water vapor interacts with transition metal oxides (TMOs) is critical for tailoring material properties to improve performance and enable new technologies. Despite extensive research efforts, atomic-scale mechanisms underpinning dynamic reactions and reaction-induced phase transitions remain elusive. Here, we use in situ environmental transmission electron microscopy to investigate how water vapor oxidizes vacancy-ordered SrCoO 2.5 at moderately elevated temperatures, demonstrating that water molecules can initiate oxidation more effectively than oxygen under comparable conditions. We discover a distinct “staging” behavior during the oxidation process: A fully ordered intermediate phase, SrCoO 2.75 , forms before transitioning into a near-perovskite SrCoO 3−δ . In addition, antiphase boundaries, originating at step terraces of SrTiO 3 , alleviate strain by creating reversible nanoscale “gaps” during lattice contraction under oxidation, providing a pathway for preserving structural integrity throughout redox cycling. This work provides atomic-level guidance for engineering TMOs by leveraging water vapor to control their redox behavior and tailor functional properties.

Science & Technology - Other Topics↗
DOE OSTI2022

Imaging elliptically polarized infrared near-fields on nanoparticles by strong-field dissociation of functional surface groups

Abstract We investigate the strong-field ion emission from the surface of isolated silica nanoparticles aerosolized from an alcoholic solution, and demonstrate the applicability of the recently reported near-field imaging at 720 nm [Rupp et al., Nat. Comm., 10(1):4655, 2019] to longer wavelength (2 $$\mu $$ μ m) and polarizations with arbitrary ellipticity. Based on the experimental observations, we discuss the validity of a previously introduced semi-classical model, which is based on near-field driven charge generation by a Monte-Carlo approach and classical propagation. We furthermore clarify the role of the solvent in the surface composition of the nanoparticles in the interaction region. We find that upon injection of the nanoparticles into the vacuum, the alcoholic solvent evaporates on millisecond time scales, and that the generated ions originate predominantly from covalent bonds with the silica surface rather than from physisorbed solvent molecules. These findings have important implications for the development of future theoretical models of the strong-field ion emission from silica nanoparticles, and the application of near-field imaging and reaction dynamics of functional groups on isolated nanoparticles. Graphical abstract

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
DOE OSTI2024

First Experimental Test of the Ratio Method

The ratio is a new reaction observable suggested to extract accurately structure information on halo nuclei. It corresponds to the ratio of differential cross sections for scattering and breakup, which is predicted to remove the uncertainty related to the reaction dynamics. We present here the first experimental test of the method for the 11 Be + 12 C collision at E Lab = 20A MeV performed at Texas A&M University. Differential cross sections for scattering and inclusive one-neutron breakup have been measured with the new detector array BlueSTEAl. The ratio of cross sections is very smooth and independent of the projectile-target interaction, which demonstrates the validity of the ratio method. We extend our analysis to existing 11 Be + 208 Pb data, confirming that the method works well on any target.

11Be↗
DOE OSTI2026

Time-, space-, and molecule-resolved multiple plasma reactive species in complex settings using an innovative approach of cavity ringdown spectroscopy (Project Final Report)

The primary research goal of this 2-year project is to demonstrate the feasibility of an innovative approach to measure reactive plasma species in the most challenging settings: right on the surface of water and under water. We propose to use the Brewster angle-cavity ringdown spextroscopy (BA-CRDS). Research objectives include: 1) Measurements of OH and NO in the plasma gas-phase zone (Z1) using different types of LTP sources including continuous and pulsed plasma jets, sheets, torches, etc. 2) Measurements of OH and NO in the multiphase reaction zones, right on the surface of water (Z2) and under water (Z3). 3) RS formation and loss mechanisms and reaction dynamics in the three zones. 4) Generalization of the proposed system to be configurable with other selected innovative techniques for other LTP parameters; invitation of selected PIs to form a strong collaborative team to pursue the follow-up effort (Category-2).

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2026

Transient Catalytic Reaction Analysis Through Signal Defragmentation

The Temporal Analysis of Products (TAP) pulse response technique provides valuable insights into catalytic function and reaction kinetics. However, complex fragmentation patterns in the TAP mass spectrometry signals can complicate precise quantification, particularly when analyzing transient gas flux data typical of TAP experiments. This work demonstrates a standard defragmentation method that deconvolves transient TAP signals while maintaining the temporal resolution of the experiment. First, the integrals of calibration gas fluxes are used to determine the fingerprint fragmentation pattern and construct a fragmentation matrix. This matrix is then used to defragment experimental flux data at each recorded time point via a non-negative least squares regression. The effectiveness of this method is demonstrated using virtual data and control experiments with a TAP reactor system. The defragmentation is then applied to the more complex propane dehydrogenation reaction on a chromia/alumina catalyst, which can contain up to ten significant gas species in the reactor outlet. Initial propane pulsing reveals an induction period during which propane is fully oxidized to CO2, followed by partial reduction to CO. Afterwards, there is a transition in chemistries towards coking and propylene production. Our example illustrates a practical method for the accurate determination of the time-dependent reactant/product concentrations and rates for a thorough analysis of the propane dehydrogenation kinetics. This approach can be broadly applied to any transient mass spectrometry experiment for a better understanding of catalyst-reaction dynamics.

36 - MATERIALS SCIENCE↗
DOE OSTI2026

Burn mode signatures enabled by high dynamic range fusion reaction history

The evolution of the fusion burn of a compressed inertial confinement fusion (ICF) implosion gives information about the evolution of the temperature, mass, and volume of the hot spot. Currently, the fusion reaction history has been measured with about a decade of dynamic range, giving information about just the peak of the fusion burn. There are proposals for extending the dynamic range to 1000×, measuring the rising edge of the burn earlier in time. Using fusion hot spot theory and a set of ICF simulations, we identify and categorize different stages of fusion burn and what signatures could be measured. For ice layered implosions, the details, conditions, and dynamics of the fusion burn propagation could be observed. For double shell and OMEGA scale implosions, the evolution of the final compression and rebounding shock before ignition could be observed. Higher dynamic range expands investigation into the logarithmic derivative, α, as a signature of various mechanisms.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2021

Flyby reaction trajectories: Chemical dynamics under extrinsic force

Dynamic effects are an important determinant of chemical reactivity and selectivity, but the deliberate manipulation of atomic motions during a chemical transformation is not straightforward. In this work, we demonstrate that extrinsic force exerted upon cyclobutanes by stretching pendant polymer chains influences product selectivity through force-imparted nonstatistical dynamic effects on the stepwise ring-opening reaction. The high product stereoselectivity is quantified by carbon-13 labeling and shown to depend on external force, reactant stereochemistry, and intermediate stability. Computational modeling and simulations show that, besides altering energy barriers, the mechanical force activates reactive intramolecular motions nonstatistically, setting up “flyby trajectories” that advance directly to product without isomerization excursions. A mechanistic model incorporating nonstatistical dynamic effects accounts for isomer-dependent mechanochemical stereoselectivity.

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

Reversible Reactions, Mesh Size, and Segmental Dynamics Control Penetrant Diffusion in Ethylene Vitrimers

The diffusion of two aromatic dyes with nearly identical sizes was measured in ethylene vitrimers with precise linker lengths and borate ester cross-links using fluorescence recovery after photobleaching (FRAP). One dye possessed a reactive hydroxyl group, while the second was inert. The reaction of the hydroxyl group with the network is slow relative to the hopping times of the dye, resulting in a large slowdown by a factor of 50 for a reactive probe molecule. A kinetic model was fit to the fluorescence intensity data to determine rate constants for the reversible reaction of the dye from the network, which confirms the role of slow reaction kinetics. A second network cross-linker was also investigated with a substituted boronic ester showing ∼10,000 times faster exchange kinetics. In this system, the two dyes show the same diffusion coefficient, as the reaction is no longer the rate-limiting step. The role of dense meshes on small and large dyes is also discussed in the context of the existing theories. Finally, these results highlight the potential of dynamic networks to control penetrant transport through synergistic effects of the mesh size, dynamic bond kinetics, and penetrant–network interactions.

confinement↗
DOE OSTI2025

Effect of interparticle fields and radiation reaction on beam dynamics

The dynamics of relativistic particles in an intense electromagnetic field can be described by the Landau-Lifshitz (LL) equation, where the radiation reaction (RR) is accounted for via a self-force, and interparticle fields are often neglected as an approximation. However, the inclusion of interparticle fields is necessary to ensure energy-momentum conservation, particularly during coherent emission. Here we present (i) an analytical proof showing that the energy-momentum conservation law of the Hamilton-Rohrlich-Dirac action, which is divergence free and describes a generic system of interacting charges, respects causality and provides physically sensible results; (ii) a simple generalization of the LL equation for many particles evaluated as a function of the total field, i.e., the sum of the external and interparticle fields. By performing first-principles numerical simulations of a neutral, relativistic bunch of electrons and positrons (e − /e + ) colliding with a laser pulse, this theory is shown to satisfy energy-momentum conservation when interparticle fields and RR are simultaneously taken into account; and (iii) the combined effect of interparticle fields and RR primarily affects the tail of the particle energy distribution. Additionally, our first-principles simulations show that the effect of interparticle fields on beam energy loss becomes smaller when most of the radiated energy is incoherent.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Robust Self-Healing Adhesives Based on Dynamic Urethane Exchange Reactions

Thermoset polyurethanes (PUs) have been successfully reprocessed as covalent adaptable networks (CANs) by catalyzing carbamate exchange. Here we extend bond exchange beyond the internal network cross-links to create a dynamic urethane adhesive. Interfacing PU CANs to substrates with nucleophilic functional groups creates adhesives capable of reversible transcarbamoylation with the substrate, which has not been demonstrated previously by CAN adhesives. Two types of thermoset PU films were synthesized, one containing the green carbamate exchange catalyst Zr(tmhd)4 and the other containing no catalyst. Although otherwise identical in chemical and network properties, as indicated by FT-IR spectroscopy and dynamic mechanical thermal analysis (DMTA), the film containing catalyst showed dynamic bond exchange behavior through stress relaxation analysis. When evaluated as an adhesive, the CAN film exhibited self-healing properties and retained its adhesive strength for five cycles, which is attributed to reversible covalent bonding to the glass substrate. Furthermore, this work expands industrially relevant CANs to structural adhesives and demonstrates their potential value in an application that presently employs PUs as single-use materials.

adhesive↗
DOE OSTI2024

Gold–Thiolate Nanocluster Dynamics and Intercluster Reactions Enabled by a Machine Learned Interatomic Potential

Monolayer protected metal clusters comprise a rich class of molecular systems and are promising candidate materials for a variety of applications. While a growing number of protected nanoclusters have been synthesized and characterized in crystalline forms, their dynamical behavior in solution, including prenucleation cluster formation, is not well understood due to limitations both in characterization and first-principles modeling techniques. Recent advancements in machine-learned interatomic potentials are rapidly enabling the study of complex interactions such as dynamical behavior and reactivity on the nanoscale. Here, we develop an Au-S-C-H atomic cluster expansion (ACE) interatomic potential for efficient and accurate molecular dynamics simulations of thiolate-protected gold nanoclusters (Au n (SCH 3 ) m ). Trained on more than 30,000 density functional theory calculations of gold nanoclusters, the interatomic potential exhibits ab initio level accuracy in energies and forces and replicates nanocluster dynamics including thermal vibration and chiral inversion. Long dynamics simulations (up to 0.1 μs time scale) reveal a mechanism explaining the thermal instability of neutral Au 25 (SR) 18 clusters. Specifically, we observe multiple stages of isomerization of the Au 25 (SR) 18 cluster, including a chiral isomer. Additionally, we simulate coalescence of two Au 25 (SR) 18 clusters and observe series of clusters where the formation mechanisms are critically mediated by ligand exchange in the form of [Au-S] n rings.

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

Rapid data-driven model reduction of nonlinear dynamical systems including chemical reaction networks using ℓ 1 -regularization

We develop a new data-driven paradigm for efficient model reduction of a broad class of nonlinear dynamical systems. Our model reduction method directly enables the interpretation of key components of the dynamical system, unlike traditional projection-based model reduction methods that focus on reducing computational complexity more than interpretability. Our method is not application specific and is simple to implement on nonlinear dynamical systems arising from a variety of different fields. It requires minimal parameterization using a single parameter to trade-off between model complexity and estimation error. We use a data-driven paradigm to formulate model reduction as an efficient convex optimization problem that scales polynomially in the original size of the complex system, enabling systems with as many as thousands of components to be reduced in a matter of minutes.

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

Origin of the “odd” behavior in the ultraviolet photochemistry of ozone

Significance This study solves a 30-y mystery about the origin of dramatic oscillations in the quantum product states of 16 O 3 upon photodissociation. Ozone is a key component of the atmosphere and undergoes complex cycles of formation and destruction by photodissociation and reaction. These dynamics are a rich proving ground for theories of quantum reaction dynamics as well as subtleties such as nuclear spin-statistics and symmetry. A previous theory constructed to explain the observed oscillations, although plausible, was not fully consistent with experimental measurements. Our quantum model and calculations show conclusively the origin of the effect, and match new more detailed experiments.

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

Multichannel dynamics in the OH+ n -butane reaction revealed by crossed-beam slice imaging and quasiclassical trajectory calculations

Multidimensional reactions present various channels that can exhibit very different dynamics and give products of varying subsequent reactivity. Here, we present a combination of experiment and theory to reveal the dynamics of hydrogen abstraction by OH radical at primary and secondary sites in n-butane at a collision energy of 8 kcal/mol. Crossed molecular beam slice imaging experiments unequivocally probe the secondary abstraction channel showing backward angular distributions with mild energy release to product translation, which are accurately captured by trajectory calculations using a specific-reaction-parameter Hamiltonian. Additionally, experiments containing both reaction channels indicate a less marked backward character in the angular distribution, whose origin is shown by trajectory calculations to appear as an evolution toward more sideways scattering from the secondary to primary channel. While the two channels have markedly different angular distributions, their energy release is largely comparable, showing ample energy release into the water product. The synergistic combination of crossed-beam imaging and trajectories opens the door to detailed reaction-dynamics studies of chemical reactions with ever-increasing complexity.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗