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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 343 records · Page 19
All sourcesNASA NTRSDOE OSTI
DOE OSTI2025

Joint Experimental and Computational Characterization of Sum-Frequency Generation between a Continuous Wave Laser and an Ultrafast Frequency Comb Laser for Tunable Laser Development

Ultrafast optical frequency combs allow for both high spectral and temporal resolution in molecular spectroscopy and have become a powerful tool in many areas of chemistry and physics. Ultrafast lasers and frequency combs generated from ultrafast mode-locked lasers often need to be converted to other wavelengths. Commonly used wavelength conversions are optical parametric oscillators, which require an external optical cavity, and supercontinuum generation combined with optical parametric amplifiers. Whether commercial or home-built, these systems are complex and costly. Here, we investigate an alternative, simple, and easy-to-implement approach to tunable frequency comb ultrafast lasers enabled by new continuous-wave laser technology. Sum-frequency generation between an Nd:YAG continuous-wave laser and a Yb:fiber femtosecond frequency comb in a beta-barium borate (BBO) crystal is explored. The resulting sum-frequency beam is a pulsed frequency comb with the same repetition rate as the Yb:fiber source. SNLO simulation software is used to simulate the results and provide benchmarks for designing future systems to achieve wavelength conversion and tunability in otherwise difficult-to-reach spectral regions.

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

Development of Lipid-Coated Semiconductor Nanosensors for Recording of Membrane Potential in Neurons

In the past decade, optical imaging methods have significantly improved our understanding of the information processing principles in the brain. Although many promising tools have been designed, sensors of membrane potential are lagging behind the rest. Semiconductor nanoparticles are an attractive alternative to classical voltage indicators, such as voltage-sensitive dyes and proteins. Such nanoparticles exhibit high sensitivity to external electric fields via the quantum-confine Stark effect. Here we report the development of semiconductor voltage-sensitive nanorods (vsNRs) that self-insert into the neuronal membrane. To facilitate interaction of the nanorods with the membrane, we functionalized their surface with the lipid mixture derived from brain extract. We describe a workflow to detect and process the photoluminescent signal of vsNRs after widefield time-lapse recordings. We also present data indicating that vsNRs are feasible for sensing membrane potential in neurons at a single-particle level. This shows the potential of vsNRs for the detection of neuronal activity with unprecedentedly high spatial and temporal resolution.

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

Terahertz Spectroscopy of Gas Mixtures with Dual Quantum Cascade Laser Frequency Combs

Terahertz laser frequency combs based on quantum cascade lasers provide coherent, broadband, electrically pumped, THz radiation sources for use in future spectroscopic applications. In this work, we explore the feasibility of such lasers in a dual-comb spectroscopy configuration for the detection of multiple molecular samples in the gas phase. The lasers span approximately 180 GHz of optical bandwidth, centered at 3.4 THz, with submilliwatt total optical power. One of the main advantages of dual-comb spectroscopy is its high speed, which opens up the possibility for direct observations of chemical reaction dynamics in the terahertz spectral region. As a proof-of-concept, we recorded continuously evolving spectra from gas mixtures with 1 ms temporal resolution.

42 ENGINEERING↗
DOE OSTI2026

Imaging from Macro to Nanoscale: Multimodal Advances in Chemical and Biomedical Imaging

Imaging increasingly serves as a multiscale framework for linking molecular mechanisms to cellular behavior, tissue architecture, and organ phenotypes in biology and unraveling fundamental processes in chemistry, physics and materials science. This Perspective highlights recent advances in chemical and biomedical imaging across macro-, micro-, and nanoscales, using representative examples published in Chemical and Biomedical Imaging (CBMI). At the macroscale, we discuss chemically selective MRI, including endogenous and exogenous CEST strategies, together with photoacoustic imaging as a hybrid modality with functional and chemical contrast. At the microscale, we consider fluorescence, label-free optical and vibrational imaging, and selected X-ray approaches that expand sensitivity, specificity, and temporal resolution in biological and materials systems. At the nanoscale, we highlight super-resolution fluorescence microscopy, single-molecule methods, tip-enhanced Raman spectroscopy, and correlative imaging strategies that resolve local heterogeneity and molecular organization. Across scales, a common theme emerges that advances in probes, contrast mechanisms, instrumentation, and sample handling are enabling chemically informed imaging that connects molecular specificity with biological context.

multiscale imaging↗
DOE OSTI2021

Redox Mediated Control of Electrochemical Potential in Liquid Cell Electron Microscopy

Liquid cell electron microscopy enables the study of nanoscale transformations in solvents with high spatial and temporal resolution, but for the technique to achieve its potential requires a new level of control over the reactivity caused by radical generation under electron beam irradiation. An understanding of how to control electron-solvent interactions is needed to further advance the study of structural dynamics for complex materials at the nanoscale. Additionally, we developed an approach that scavenges radicals with redox species that form well-defined redox couples and control the electrochemical potential in situ . This approach enables the observation of electrochemical structural dynamics at near-atomic resolution with precise control of the liquid environment. Analysis of nanocrystal etching trajectories indicates that this approach can be generalized to several chemical systems. The ability to simultaneously observe heterogeneous reactions at near-atomic resolution and precisely control the electrochemical potential enables the fundamental study of complex nanoscale dynamics with unprecedented detail.

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

Resolving the Heat of Trimethylaluminum and Water Atomic Layer Deposition Half-Reactions

We report that atomic layer deposition (ALD) is a surface synthesis technique that is characterized by self-limiting reactions between gas-phase precursors and a solid substrate. Although ALD processes have been demonstrated that span the periodic table, a greater understanding of the surface chemistry that affords ALD is necessary to enable greater precision, including area- and site-selective growth. We offer new insight into the thermodynamics and kinetics of the trimethylaluminum (TMA) and H 2 O ALD half-reactions with calibrated and time-resolved in situ pyroelectric calorimetry. The half-reactions produce 3.46 and 2.76 eV/Al heat, respectively, which is greater than the heat predicted by computational models based on crystalline Al 2 O 3 substrates and closely aligned with the heat predicted by standard heats of formation. The pyroelectric thin-film calorimeter offers submilisecond temporal resolution that uniquely and clearly resolves precursor delivery and reaction kinetics. Both half-reactions are observed to exhibit multiple kinetic rates, with average TMA half-reaction rates at least 2 orders of magnitude faster than the H 2 O half-reaction kinetics. Comparing the experimental heat with published computational literature and additional first-principles modeling highlights the need to refine our models and mechanistic understanding of even the most ubiquitous ALD reactions.

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

UV-Induced Reaction Pathways in Bromoform Probed with Ultrafast Electron Diffraction

For many chemical reactions, it remains notoriously difficult to predict and experimentally determine the rates and branching ratios between different reaction channels. This is particularly the case for reactions involving short-lived intermediates, whose observation requires ultrafast methods. The UV photochemistry of bromoform (CHBr 3 ) is among the most intensely studied photoreactions. Yet, a detailed understanding of the chemical pathways leading to the production of atomic Br and molecular Br 2 fragments has proven challenging. In particular, the role of isomerization and/or roaming and their competition with direct C–Br bond scission has been a matter of continued debate. Here, in this work, gas-phase ultrafast megaelectronvolt electron diffraction (MeV-UED) is used to directly study structural dynamics in bromoform after single 267 nm photon excitation with femtosecond temporal resolution. The results show unambiguously that isomerization contributes significantly to the early stages of the UV photochemistry of bromoform. In addition to direct C–Br bond breaking within <200 fs, formation of iso-CHBr 3 (Br-CH-Br-Br) is observed on the same time scale and with an isomer lifetime of >1.1 ps. The branching ratio between direct dissociation and isomerization is determined to be 0.4 ± 0.2:0.6 ± 0.2, i.e., approximately 60% of molecules undergo isomerization within the first few hundred femtoseconds after UV excitation. The structure and time of formation of iso-CHBr 3 compare favorably with the results of an ab initio molecular dynamics simulation. The lifetime and interatomic distances of the isomer are consistent with the involvement of a roaming reaction mechanism.

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

Prolonging All-Optical Molecular Electron Spin Coherence in the Tissue Transparency Window

Coherent electron spin states within paramagnetic molecules hold significant potential for microscopic quantum sensing. However, all-optical coherence measurements amenable to high spatial and temporal resolution under ambient conditions remain a significant challenge. Here we conduct room-temperature, picosecond time-resolved Faraday ellipticity/rotation (TRFE/R) measurements of the electron spin decoherence time T 2 * in [IrBr 6 ] 2- . Decoherence is strongly sensitive to solution phase viscosity, pointing to molecular tumbling as an important decoherence mechanism. Accordingly, immobilization of [IrBr 6 ] 2- molecules in thin polymer films results in an order-of-magnitude increase in coherence lifetime and significantly greater magnetic field sensitivity. Here, by tuning energies of ligand-to-metal charge transfer (LMCT) states, TRFE/R enables spin initialization and readout in the tissue transparency window, paving the way toward all-optical, ultrafast molecular electron spin coherence imaging in biological systems.

Electron paramagnetic resonance spectroscopy↗
DOE OSTI2026

In Situ Insights into Enhanced Cooperative Ligand Exchange Kinetics via Solvent-Induced Restacking in a 2D Metal–Organic Framework

Understanding the reaction kinetics at catalytically active sites is crucial for integrating catalytic two-dimensional (2D) materials into industrial processes. This study focuses on in situ observation of ligand exchange kinetics and solvent-assisted structural restacking transition in the 2D paddle wheel-based MOF [Cu 2 (dttc) 2 ] n (DUT-134(Cu), dttc = dithieno[3,2-b:2′,3′- d]thiophene-2,6-dicarboxylate). The ligand exchange process, involving the replacement of dimethylformamide (DMF) with nitriles such as acetonitrile (ACN), pentanenitrile, and heptanenitrile, was investigated using advanced in situ characterization techniques with high temporal resolution, including powder X-ray diffraction and Raman spectroscopy. The larger analytes exhibited reduced exchange rates, consistent with enhanced steric hindrance and greater diffusion constraints. Interestingly, the study revealed that the exchange of DMF with ACN induces a structural transition to higher symmetry within few seconds, a transition from AB to AA stacking mode of the layers, and a widening of the interlayer distance. Crucially, this structural transition dramatically accelerates the solvent exchange process through cooperative effects, offering critical advantages for catalytic applications. Notably, the reverse exchange from ACN to DMF proceeds more slowly and does not reverse the structural changes, but a new phase is formed with preserved AA stacking. By isotope labeling of linker molecules in combination with two complementary theoretical vibrational simulation methods, the precise assignment of Raman bands and the vibrational modes associated with the ligand exchange process could be achieved. These pioneering insights into the dynamic behavior of 2D MOFs, coupled with ligand exchange, establish a highly promising and transformative approach to achieving enhanced tunability and responsiveness in future catalytic applications.

Layers↗
DOE OSTI2020

Numerically Relevant Timescales in the MG2 Microphysics Model

Climate models rely on parameterizations of a variety of processes in the atmospheric physics, but a common concern is that the temporal resolution is too coarse to consistently resolve the behavior that individual parameterizations are designed to capture. This study examines timescales numerically derived from the Morrison-Gettelman (MG2) microphysics as implemented within the Energy Exascale Earth System Model, version 1 (E3SMv1). Numerically relevant timescales in MG2 are derived by computing the eigenspectrum of its Jacobian. These timescales are found to often be smaller than the default 5 min time step used for MG2. The fast timescales are then heuristically connected to individual microphysics processes. By substepping a few particular rain processes within MG2, the time discretization error for those processes was considerably reduced with minimal additional expense to the overall microphysics. While this improvement has a substantial effect on the target processes and on the vertical distribution of stratiform-derived rain within E3SMv1, the overall model climate is found to not be sensitive to MG2 time step. Here, we hypothesize that this is because the surface climate does not depend strongly on certain process rates, especially MG2's rain evaporation rate.

58 GEOSCIENCES↗
DOE OSTI2021

Observations and Simulations of Dropout Events and Flux Decays in October 2013: Comparing MEO Equatorial With LEO Polar Orbit

We compare ESA PROBA-V observations of electron flux at LEO with those from the NASA Van Allen Probes mostly at MEO for October 2013. Dropouts are visible at all energy during four storms from both satellites. Equatorially trapped electron fluxes are higher than at LEO by 10 2 (<1 MeV) to 10 5 (>2.5 MeV). We observe a quite isotropic structure of the outer belt during quiet times, contrary to the inner belt, and pitch angle dependence of high energy injection. We find a very good overlap of the outer belt at MEO and LEO at ~0.5 MeV. We use test-particle simulations of the energetic electrons trapped in the terrestrial magnetic field to study the outer radiation belt electron flux changes during geomagnetic storms. We show that the Dst (Disturbance storm time) effect during the main phase of a geomagnetic storm results in a betatron mechanism causing outward radial drift and a deceleration of the electrons. This outward drift motion is energy independent, pitch angle-dependent, and represents a significant distance (~1 L-shell at L = 5 for moderate storms). At fixed L-shell, this causes a decay of the LEO precipitating flux (adiabatic outward motion), followed by a return to the normal state (adiabatic inward motion) during main and recovery phases. Dst effect, associated with magnetopause shadowing and radial diffusion can explain the main characteristics of outer radiation belt electron dropouts in October 2013. We also use Fokker-Planck simulations with event-driven diffusion coefficients at high temporal resolution, to distinguish instantaneous loss from the gradual scattering that depopulates the slot region and the outer belt after storms. Simulations reproduce the slot formation and the gradual loss in the outer belt. The typical energy dependence of these losses leads to the absence of scattering for relativistic and ultra-relativistic electrons in the outer belt, oppositely to dropouts.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2022

A Differentiable Hydrology Approach for Modeling With Time-Varying Parameters

In the analysis of observational data with mathematical models, it is often desirable to let one or more model parameters vary with time to account for changing environmental conditions or to offer more flexibility. A standard approach for dynamic models is to allow for the number of parameters to grow as a function of time, leading to a high-dimensional inference problem for long data records. We propose using Hamiltonian Monte Carlo, a gradient-based Markov chain Monte Carlo (MCMC) method, to perform Bayesian inference for time-varying parameters (TVP) in hydrology models. As derivatives of model error functions with regard to parameters are not available in closed form, we implemented the GR4J rainfall-runoff models in Theano/PyMC3, and Jax/NumPyro, allowing for the application of automatic differentiation techniques. A simulation experiment assessing the viability of these methods for recovering underlying temporal variation in parameters indicates that a discrete Gaussian random walk-based prior appears to be best suited across a range of scenarios while the continuous-time Gaussian process compares relatively poorly. In an analysis of 20 years of daily real-world streamflow records from the Model Parameter Estimation Experiment (MOPEX) hydrology data set with increasing data sparsity and at multiple temporal resolutions, we find that TVP inference with gradient-based MCMC is a flexible and reliable approach for analyzing hydrology models with dynamic parameter sets.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Distributed Fiber Optics Measurements of Rock Deformation and Failure in Triaxial Tests

The implementation of distributed strain measurement methods in triaxial and uniaxial tests have demonstrated the development of strain localization, even at early stages. This implies that single point measurement methods are location dependent. The use of distributed methods is required not only to improve the interpreted constitutive parameters obtained from triaxial tests, but also to understand the implications of strain localization in the failure process. Here, this work uses optical fibers in triaxial tests. The developed distributed measurement method was implemented on granite, gabbro, and sandstone samples and tested under different confining pressures, reaching 200 MPa on the granite sample. Using a temporal resolution of 0.25 Hz and 5 mm of spatial resolution, the strain evolution at over 300 locations at the sample surface was measured during testing. When compared to point sensing methods, the use of optical fiber greatly increases the number of measurements at the surface of the sample, and their interpolation provides the entire deformation of the sample surface. In all the tests performed, strain localizations were revealed before failure. A three-dimensional interpretation of a test, combining an optical scan of the sample and the distributed measurements, show good correlation between the fractures and the strain localization.

58 GEOSCIENCES↗
DOE OSTI2022

Aircraft Observations of Turbulence in Cloudy and Cloud-Free Boundary Layers Over the Western North Atlantic Ocean From ACTIVATE and Implications for the Earth System Model Evaluation and Development

This study examines boundary layer turbulence derived from high temporal resolution meteorological measurements from 40 research flights over the western North Atlantic Ocean during the 2020 deployments of ACTIVATE. Frequency distributions of various turbulent quantities reveal stronger turbulence during the winter deployment than in summer and for cloud‐topped than in cloud‐free boundary layers during the summer deployment. Maximum turbulence kinetic energy (TKE) is most often within cloud from observations in winter and summer, whereas it is mostly below cloud in both seasons by a global model turbulence parameterization. Further, bivariate frequency distributions are consistent with the bivariate Gaussian probability distribution functions assumed for the closure of higher‐order turbulence/shallow convection parameterizations used by some global models. Turbulence simulated by the Community Atmosphere Model version 6 and the Energy Exascale Earth System Model Atmosphere Model version 2 using such parameterizations is not as strong as observed, with more TKE going into vertical wind perturbations rather than into zonal wind perturbations as observed, suggesting that the treatment of turbulence in Earth system models still needs to be further improved.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Subseasonal Tropical Cyclone Prediction and Modulations by MJO and ENSO in CESM2

Subseasonal tropical cyclone (TC) reforecasts from the Community Earth System Model version 2 (CAM6) subseasonal prediction system are examined in this study. Here, we evaluate the modeled TC climatology and the probabilistic forecast skill of basin-wide TC genesis at weekly temporal resolution. Prediction skill is calculated using the Brier skill score relative to a constant annual mean climatology and to a monthly varying seasonal climatology during TC season. The model captures the observed basin-wide climatological TC seasonality and spatial distributions at weeks 1–6, but TC genesis is largely underestimated from Week 2 onward. For some basins and lead times, the predicted TC genesis is primarily controlled by the number of TC “seeds” and the mean-state climate condition. The model has good prediction skill relative to the constant climatology across all the basins and lead times, but is only skillful in the eastern Pacific, North Indian Ocean, and Southern Hemisphere at Week 1 when compared to the seasonal climatology, indicating limited skill in predicting deviations from the seasonal cycle. We find strong modulations of the predicted TC genesis at up to 3 weeks of forecast lead time by the Madden-Julian Oscillation. The interannual variability of predicted TC genesis and accumulated cyclone energy are skillfully predicted in the North Atlantic and the Northwestern Pacific, with a strong modulation by the El Nino-Southern Oscillation.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Cycles-L: A Coupled, 3-D, Land Surface, Hydrologic, and Agroecosystem Landscape Model

Managing landscapes to increase agricultural productivity and environmental stewardship can be informed by spatially-distributed models that operate at spatial and temporal scales that are intervention-relevant. This paper presents Cycles-L, a landscape-scale agroecosystem and hydrologic modeling system, using as a test case a watershed in Pennsylvania. Cycles-L emerges from melding the landscape and hydrology structure of Flux-PIHM, a 3-D land surface hydrologic model, with the agroecosystem processes in the Cycles model. Consequently, Cycles-L can simulate processes affected by topography, soil heterogeneity, and management practices, owing to its physically-based hydrology that can simulate horizontal and vertical transport of solutes with water. The model was tested at a 730-ha experimental watershed within the Mahantango Creek watershed. Cycles-L simulated well stream water and mineral nitrogen discharge (Nash-Sutcliffe coefficient 0.55 and 0.60, respectively) and grain yield (root mean square error 1.2 Mg ha -1 ). Cycles-L outputs are as good or better than those obtained with the uncoupled Flux-PIHM (water discharge) and Cycles (grain yield) models. Modeled spatial patterns of nitrogen fluxes like denitrification illustrate the combined control of crop management and topography. For example, denitrification is almost twice as high when simulated with Cycles-L than when simulated with Cycles 1-D. Due to its spatial and temporal resolution, Cycles-L fills a gap in the availability of models that operate at a scale relevant to evaluate interventions in the landscape. Cycles-L can become a central component in tools for climate change scenario analysis, precision agriculture, precision conservation, and artificial intelligence-based decision support systems.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2024

Lightning Characteristics Associated With Storm Modes Observed During RELAMPAGO

Global satellite studies show a maximum in deep convection and lightning downstream of the Andes in subtropical South America. The Remote sensing of Electrification, Lightning, And Mesoscale/microscale Processes with Adaptive Ground Observations (RELAMPAGO) field campaign was designed to investigate the physical processes that contribute to the rapid development of deep convection and mesoscale convective systems (MCSs) in Argentina. A lightning mapping array (LMA) was deployed to Argentina as part of RELAMPAGO to collect lightning observations from extreme storms in the region. This study combines lightning data from the LMA and the Geostationary Lightning Mapper onboard GOES-16 with 1-km gridded radar data to examine the electrical characteristics of a variety of convective storms throughout their life cycle observed during RELAMPAGO. Results from the full campaign show 48% of flashes are associated with deep convection that occurs along the eastern edge of the Sierras de Córdoba (SDC) overnight. These flashes are 65 km 2 smaller on average compared to stratiform flashes, which occur most frequently 50–100 km east of the SDC in the early morning hours, consistent with the upscale growth of MCSs off the terrain. Analysis of the 13–14 December MCS shows that sharp increases in flash rates correspond to deep and wide convective cores that have high graupel and hail mass, 35-dBZ volume, and ice water path. This work validates previous satellite studies of lightning in the region, but also provides higher spatial and temporal resolution information across the convective life cycle that has not been available in previous studies.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Theory of an Automatic Seepage Meter and Ramifications for Applications

A new approach for measuring fluxes across surface water—groundwater interfaces was recently proposed. The Automatic Seepage Meter (ASM) is equipped with a precise water level sensor and digital memory that analyzes water level time series in a vertical tube inserted into a streambed. The ability to infer flux values with high temporal resolution relies on an accurate interpretation of water level dynamics inside the tube. Here, we reduce the three-dimensional hydrodynamic problem that describes the ASM water level in a variety of field conditions to a single ordinary differential equation. This novel general analytical solution for estimating ASM responses is more comprehensive and flexible than previous approaches and is applicable to the entire range of field conditions, including steady or transient stream stages, evaporation, rainfall, and noise. For example, our analysis determines the timing of the nonmonotonic ASM response to a monotonic linear stream stage variation and explains previously used empirical parabolic approximation for estimating fluxes. We present algorithms for simultaneous inference of vertical interface flux and hydraulic conductivity values together with an example code. We quantify how the accuracy of parameter estimation depends on test duration and noise amplitude and propose how our analysis can be used to optimize field test protocols. On this basis, changing the ASM geometry by increasing the radius and decreasing tube insertion depth may enable ASM field test protocols that estimate interface flux and hydraulic conductivity faster while maintaining desired accuracy. Potential applications of joint parameter estimation are suggested.

47 OTHER INSTRUMENTATION↗