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Results for “time resolve scattering”

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 163 records · Page 9
All sourcesNASA NTRSDOE OSTI
DOE OSTI2024

minimpl (b1)

The micropulse lidar (MPL) is a ground-based, optical, remote-sensing system designed primarily to determine the altitude of clouds; however, it is also used for detection of atmospheric aerosols. The physical principle is the same as for radar. Pulses of energy are transmitted into the atmosphere; the energy scattered back to the transceiver is collected and measured as a time-resolved signal, thereby detecting clouds and aerosols in real time. From the time delay between each outgoing pulse and the backscattered signal, the distance to the scatterer is inferred. Post-processing of the lidar return characterizes the extent and properties of aerosols or other particles in a region.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2022

Lactoferricins impair the cytosolic membrane of Escherichia coli within a few seconds and accumulate inside the cell

We report the real-time response of Escherichia coli to lactoferricin-derived antimicrobial peptides (AMPs) on length scales bridging microscopic cell sizes to nanoscopic lipid packing using millisecond time-resolved synchrotron small-angle X-ray scattering. Coupling a multiscale scattering data analysis to biophysical assays for peptide partitioning revealed that the AMPs rapidly permeabilize the cytosolic membrane within less than 3 s—much faster than previously considered. Final intracellular AMP concentrations of ~80–100 mM suggest an efficient obstruction of physiologically important processes as the primary cause of bacterial killing. On the other hand, damage of the cell envelope and leakage occurred also at sublethal peptide concentrations, thus emerging as a collateral effect of AMP activity that does not kill the bacteria. This implies that the impairment of the membrane barrier is a necessary but not sufficient condition for microbial killing by lactoferricins. The most efficient AMP studied exceeds others in both speed of permeabilizing membranes and lowest intracellular peptide concentration needed to inhibit bacterial growth.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2024

Microsecond dynamics control the HIV-1 Envelope conformation

The HIV-1 Envelope (Env) glycoprotein facilitates host cell fusion through a complex series of receptor-induced structural changes. Although remarkable progress has been made in understanding the structures of various Env conformations, microsecond timescale dynamics have not been studied experimentally. Here, we used time-resolved, temperature-jump small-angle x-ray scattering to monitor structural rearrangements in an HIV-1 Env SOSIP ectodomain construct with microsecond precision. In two distinct Env variants, we detected a transition that correlated with known Env structure rearrangements with a time constant in the hundreds of microseconds range. A previously unknown structural transition was also observed, which occurred with a time constant below 10 μs, and involved an order-to-disorder transition in the trimer apex. Using this information, we engineered an Env SOSIP construct that locks the trimer in the prefusion closed state by connecting adjacent protomers via disulfides. Our findings show that the microsecond timescale structural dynamics play an essential role in controlling the Env conformation with impacts on vaccine design.

59 BASIC BIOLOGICAL SCIENCES↗
DOE OSTI2021

Theory of subcycle time-resolved photoemission: Application to terahertz photodressing in graphene

Here, motivated by recent experimental progress we revisit the theory of pump–probe time- and angle-resolved photoemission spectroscopy (trARPES), which is one of the most powerful techniques to trace transient pump-driven modifications of the electronic properties. The pump-induced dynamics can be described in different gauges for the light–matter interaction. Standard minimal coupling leads to the velocity gauge, defined by linear coupling to the vector potential. In the context of tight-binding (TB) models, the Peierls substitution is the commonly employed scheme for single-band models. Multi-orbital extensions – including the coupling of the dipole moments to the electric field – have been introduced and tested recently. In this work, we derive the theory of time-resolved photoemission within both gauges from the perspective of nonequilibrium Green’s functions. This approach naturally incorporates the photoelectron continuum, which allows for a direct calculation of the observable photocurrent. Following this route we introduce gauge-invariant expressions for the time-resolved photoemission signal. The theory is applied to graphene pumped with short terahertz pulses, which we treat within a first-principles TB model. We investigate the gauge invariance and discuss typical effects observed in subcycle time-resolved photoemission. Our formalism is an ideal starting point for realistic trARPES simulations including scattering effects.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗
DOE OSTI2024

Accessing metal-specific orbital interactions in C–H activation with resonant inelastic X-ray scattering

Photochemically prepared transition-metal complexes are known to be effective at cleaving the strong C–H bonds of organic molecules in room temperature solutions. There is also ample theoretical evidence that the two-way, metal to ligand (MLCT) and ligand to metal (LMCT), charge-transfer between an incoming alkane C–H group and the transition metal is the decisive interaction in the C–H activation reaction. What is missing, however, are experimental methods to directly probe these interactions in order to reveal what determines reactivity of intermediates and the rate of the reaction. Here, using quantum chemical simulations we predict and propose future time-resolved valence-to-core resonant inelastic X-ray scattering (VtC-RIXS) experiments at the transition metal L-edge as a method to provide a full account of the evolution of metal–alkane interactions during transition-metal mediated C–H activation reactions. For the model system cyclopentadienyl rhodium dicarbonyl (CpRh(CO) 2 ), we demonstrate, by simulating the VtC-RIXS signatures of key intermediates in the C–H activation pathway, how the Rh-centered valence-excited states accessible through VtC-RIXS directly reflect changes in donation and back-donation between the alkane C–H group and the transition metal as the reaction proceeds via those intermediates. We benchmark and validate our quantum chemical simulations against experimental steady-state measurements of CpRh(CO) 2 and Rh(acac)(CO)2 (where acac is acetylacetonate). Our study constitutes the first step towards establishing VtC-RIXS as a new experimental observable for probing reactivity of C–H activation reactions. More generally, the study further motivates the use of time-resolved VtC-RIXS to follow the valence electronic structure evolution along photochemical, photoinitiated and photocatalytic reactions with transition metal complexes.

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

Impact of Processing on Structural and Compositional Evolution in Mixed Metal Halide Perovskites during Film Formation

Understanding crystallization processes and their pathways in metal-halide perovskites is of crucial importance as this strongly affects the film microstructure, its stability, and device performance. While many approaches are developed to control perovskite formation, the mechanisms of film formation are still poorly known. Using time-resolved in situ grazing incidence wideangle X-ray scattering, the film formation of perovskites is investigated with average stoichiometry Cs 0.15 FA 0.85 PbI 3 , where FA is formamidinium, using the popular antisolvent dropping and gas jet treatments and this is contrasted with untreated films. i) The crystallization pathways during spin coating, ii) the subsequent postdeposition thermal annealing, and iii) crystallization during blade coating are studied. The findings reveal that the formation of a nonperovskite FAPbI 3 phase during spin coating is initially dominant regardless of the processing and that the processing treatment (e.g., antisolvent dropping, gas jet) has a significant impact on the as-cast film structure and affects the phase evolution during subsequent thermal treatment. It is shown that blade coating can be used to overcome the nonperovskite phase formation via solvothermal direct crystallization of perovskite phase. This work shows how real-time investigation of perovskite formation can help to establish processing–microstructure–functionality relationships.

36 MATERIALS SCIENCE↗
DOE OSTI2021

Evidence for Trapping-Induced Nonlinear Frequency Shifts in Langmuir Waves Driven via Stimulated Raman Scattering

Thomson scattering is used to detect the spectra of Langmuir waves driven through the backward stimulated Raman scattering process in a diffraction limited laser focal spot. Measured Langmuir wave spectral frequencies are found to vary in time and have broadened spectral power, consistent with a nonlinear frequency shift of the driven Langmuir wave due to electron-trapping. Broadening of the Langmuir wave spectral power is observed to decrease in time, consistent with measured variations in the frequency shift of the driven Langmuir waves. Furthermore, the observed spectral broadening is consistent with the temporally short (ps), bursty nature of backward stimulated Raman scattered light observed in simulations that cannot be resolved by the Thomson scattering diagnostic. Comparison of the broadened spectrum with time integrated spectra from two-dimensional particle-in-cell simulations shows favorable comparison in the broadened spectral widths, supporting the supposition of electron-trapping induced, nonlinear shifting of daughter Langmuir wave frequencies.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗
DOE OSTI2020

Nonequilibrium Thermodynamics of Colloidal Gold Nanocrystals Monitored by Ultrafast Electron Diffraction and Optical Scattering Microscopy

Metal nanocrystals exhibit important optoelectronic and photocatalytic functionalities in response to light. These dynamic energy conversion processes have been commonly studied by transient optical probes to date, but an understanding of the atomistic response following photoexcitation has remained elusive. In this paper, we use femtosecond resolution electron diffraction to investigate transient lattice responses in optically excited colloidal gold nanocrystals, revealing the effects of nanocrystal size and surface ligands on the electron–phonon coupling and thermal relaxation dynamics. First, we uncover a strong size effect on the electron–phonon coupling, which arises from reduced dielectric screening at the nanocrystal surfaces and prevails independent of the optical excitation mechanism (i.e., inter- and intraband). Second, we find that surface ligands act as a tuning parameter for hot carrier cooling. Particularly, gold nanocrystals with thiol-based ligands show significantly slower carrier cooling as compared to amine-based ligands under intraband optical excitation due to electronic coupling at the nanocrystal/ligand interfaces. Finally, we spatiotemporally resolve thermal transport and heat dissipation in photoexcited nanocrystal films by combining electron diffraction with stroboscopic elastic scattering microscopy. Taken together, we resolve the distinct thermal relaxation time scales ranging from 1 ps to 100 ns associated with the multiple interfaces through which heat flows at the nanoscale. Our findings provide insights into optimization of gold nanocrystals and their thin films for photocatalysis and thermoelectric applications.

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

Consequences of sp 2 –sp 3 boron isomerization in supercooled liquid borates

In this study, time-resolved high-energy synchrotron x-ray total scattering measurements on supercooled molten lithium metaborate (LiBO 2 ) reveal an isomerization reaction involving conversion of trigonal sp 2 boron to tetrahedral sp 3 boron during quenching and glass formation. Van't Hoff analysis yields an accurate enthalpy change, ΔH = 21(1) kJ mol –1 boron, from which we develop an analytical model for the sp 3 isomer fraction and its contribution to configurational heat capacity (C p conf ) and entropy as a function of temperature and composition. Isomerization constitutes 40% of the total calorimetric C p conf at the glass transition for LiBO 2 and directly contributes to the observed rise in liquid fragility with the lithium content.

74 ATOMIC AND MOLECULAR PHYSICS↗
DOE OSTI2021

Interplays of electron and nuclear motions along CO dissociation trajectory in myoglobin revealed by ultrafast X-rays and quantum dynamics calculations

Significance In this multidisciplinary study, we investigated local and global structural responses upon carbon monoxide (CO) dissociation from the heme iron(II) in myoglobin in solution using ultrafast X-ray absorption and scattering. CO dissociation was optically triggered and pulsed X-rays probed structural and electronic changes as a function of time, revealing an iron(II) spin state transition and nuclear motions propagating from the active site throughout the entire protein. Quantum mechanical computational results were used to assign the iron K-edge absorption features, and to map out electronic and nuclear trajectories during Fe–CO bond elongation and heme macrocycle doming. The study has important implications for heme–protein function and the interaction of small molecule substrates with the metal active centers in enzymes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
DOE OSTI2021

Laser-induced transient magnons in Sr 3 Ir 2 O 7 throughout the Brillouin zone

Although ultrafast manipulation of magnetism holds great promise for new physical phenomena and applications, targeting specific states is held back by our limited understanding of how magnetic correlations evolve on ultrafast timescales. Using ultrafast resonant inelastic X-ray scattering we demonstrate that femtosecond laser pulses can excite transient magnons at large wavevectors in gapped antiferromagnets and that they persist for several picoseconds, which is opposite to what is observed in nearly gapless magnets. Overall, our work suggests that materials with isotropic magnetic interactions are preferred to achieve rapid manipulation of magnetism.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2022

The dark side of galaxy stellar populations – II. The dependence of star-formation histories on halo mass and on the scatter of the main sequence

Nearby galaxies are the end result of their cosmological evolution, which is predicted to be influenced by the growth of their host dark matter haloes. This co-evolution potentially leaves signatures in present-day observed galaxy properties, which might be essential to further understand how the growth and properties of galaxies are connected to those of their host haloes. In this work, we study the evolutionary histories of nearby galaxies both in terms of their host haloes and the scatter of the star-forming main sequence by investigating their time-resolved stellar populations using absorption optical spectra drawn from the Sloan Digital Sky Survey. We find that galaxy star-formation histories depend on the masses of their host haloes, and hence they shape the evolution of the star-forming main sequence over cosmic time. Additionally, we also find that the scatter around the z = 0 star-forming main sequence is not (entirely) stochastic, as galaxies with currently different star-formation rates have experienced, on average, different star-formation histories. Furthermore, our findings suggest that dark matter haloes might play a key role in modulating the evolution of star formation in galaxies, and thus of the main sequence, and further demonstrate that galaxies at different evolutionary stages contribute to the observed scatter of this relation.

79 ASTRONOMY AND ASTROPHYSICS↗
DOE OSTI2026

Surface Reordering During Layer‐by‐Layer Growth on SrTiO 3

With the development of layer‐by‐layer growth techniques such as molecular beam epitaxy (MBE), it is now possible to construct materials with atomic‐level precision, with the layer sequence primarily determined by the growth recipe. However, materials can still restructure in the high‐temperature growth environment with surface thermodynamics strongly influencing growth behavior. Here, we demonstrate that growth on ${\rm SrTiO}_{3}$ (001), the principal platform for oxide electronics, does not occur in a layer‐by‐layer fashion but follows a more complex process in which a ${\rm TiO}_{2}$ plane continually diffuses toward the growth surface. Employing in situ synchrotron X‐ray scattering combined with ab initio thermodynamic calculations, we discover the existence of a stable ${\rm TiO}_{2}$ double‐layer structure on the pristine substrate and the occurrence of dynamic layer rearrangement during homoepitaxial growth by oxide MBE. Our findings suggest that the current methods used to precisely control ${\rm SrTiO}_{3}$ surfaces are limited, as well as our ability to dictate the composition of ultrathin films, resulting in important ramifications regarding the surface reactivity of perovskite materials grown on ${\rm SrTiO}_{3}$.

Coherent Bragg Rod Analysis↗
DOE OSTI2026

Nanoscale ultrafast lattice modulation with a free-electron laser

Ultrafast optical laser-based techniques have enabled the probing of atomistic processes at their intrinsic temporal scales with femto- and attosecond resolution. However, the long wavelengths of optical lasers have prevented their interrogation and manipulation with nanoscale spatial specificity. Advances in hard X-ray free-electron lasers have enabled progress in developing X-ray transient-grating spectroscopy, a technique that aims to coherently control elementary excitations with nanoscale X-ray standing waves. Thus far, the realization of this technique at the nanoscale has been a challenge. Here we demonstrate X-ray transient-grating spectroscopy with spatial periods of the order of 10 nm via the subfemtosecond synchronization of two hard X-ray pump pulses at a precisely controlled crossing angle. This creates a thermal grating and preferentially excites coherent longitudinal acoustic phonon modes with the transient-grating wavevector. On probing with a third, variably delayed, X-ray pulse with the same photon energy, time-and-wavevector-resolved measurements of the modulation of the induced scattering intensity provide evidence of ballistic thermal transport at nanometre scales. Finally, these results highlight the potential of X-ray transient gratings as a powerful platform for studying nanoscale transport in condensed matter and the coherent control of nanoscale dynamics.

nonlinear optics↗
DOE OSTI2024

Operando investigations of the solid electrolyte interphase in the lithium mediated nitrogen reduction reaction

The lithium-mediated nitrogen reduction reaction (Li-NRR) represents a promising approach for electrochemical nitrogen activation, in which the solid electrolyte interphase (SEI) layer formed on the electrochemically plated lithium plays a key role. Herein, we used time-resolved, operando, grazing incidence wide-angle X-ray scattering (GI WAXS) to identify SEI species and reaction intermediates in the Li-NRR, comparing LiBF 4 and LiClO 4 as electrolyte salts. In this study, we demonstrated how the SEI composition influences the Li-NRR performance by regulating proton transport to the plated Li. When LiBF 4 is used as the electrolyte salt, the formation of LiF and lithium ethoxide (LiEtO) is observed. Reaction intermediates such as LiH and LiN x H y species were found and provide insight into reaction pathways towards undesired and desired products, respectively. Observed restructuring of the Cu (111) single crystal substrate also indicates interaction with plated Li that could possibly influence the Li-NRR performance. Together, these experiments give molecular insight into how to design Li-NRR systems and their SEI layers for optimal performance.

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

A Multi-Instrument Cloud Condensation Nuclei Spectrum Product (Final Technical Report)

A wealth of observational data exists on the characteristics of atmospheric particulate matter, over multiple years, at the DOE ARM Southern Great Plains (SGP) Central Facility site. This site is located in a region of the country that frequently experiences weather extremes, and that is removed from many local sources of pollution but is affected by transported smoke, dust, and urban emissions. The relationships between particulate matter, cloud formation and evolution, and precipitation are therefore of strong interest, and are being explored via modeling on a variety of scales. These models require as input detailed information on the characteristics of particles capable of serving as the nuclei for cloud formation. Sufficient data exist to be able to put together a picture of the nature of the total aerosol and the cloud condensation nuclei (CCN) subset, and their variability, through merged data products. This study was aimed at exploiting the multiple measurement types at SGP to develop the first such multi-year estimates. Further, the resulting data were analyzed to understand temporal patterns ranging from hourly to seasonal, thereby gaining insights into the particle sources affecting the atmosphere in this region. DOE-funded datasets that were analyzed in this study include total particle number concentrations, submicron aerosol scattering coefficients, dry aerosol size distributions, and more recently, time-resolved submicron aerosol chemical composition. Data are also available for the number concentrations of particles that are activated in a cloud condensation nucleus instrument at a series of setpoint supersaturations, providing direct observations of the number concentrations of “CCN”. This variable is the quantity that is generally desired for inclusion in numerical models that seek to represent and predict the impacts of varying aerosol characteristics on the formation and microphysical properties of clouds. One limitation of the use of direct CCN observations is that they are not available for supersaturations larger than about 1%, which is insufficient for deep convection and may be insufficient even for shallow convection, depending on the nature of the available CCN and the dynamics of the cloud. We developed a data-based approach to representing the full aerosol size spectrum with size-dependent hygroscopicity, and used this to extrapolate CCN spectra beyond the limited measurements. Five years of SGP aerosol data (2009 -2013) were analyzed. As a side product of our work, we identified and communicated several previously-unflagged data quality issues. The resulting merged aerosol distributions, along with fits for seasonal averages, were published and submitted to the ARM archive as a special value-added product (VAP; submitted as a PI product). CCN spectra were computed for the same data period and will similarly be published and submitted to the archive for use by the community. We also note that our methodologies and findings have been discussed at several Joint ARM User Facility/Atmospheric System Research (ASR) Principal Investigators Meetings and that recent ARM/ASR aerosol data reporting strategies have included similar ideas for data merging, indicating that this work has had a lasting impact on ARM aerosol data acquisition and reporting. The proposed work advances the science of the interactions of aerosols, clouds and precipitation, with direct application to improve representation of such interactions for clouds in regional and global climate models. The archived data will continue to serve research studies in the future.

54 ENVIRONMENTAL SCIENCES↗
DOE OSTI2023

Multi-scale time-resolved electron diffraction: A case study in moiré materials

Ultrafast-optical-pump — structural-probe measurements, including ultrafast electron and x-ray scattering, provide direct experimental access to the fundamental timescales of atomic motion, and are thus foundational techniques for studying matter out of equilibrium. High-performance detectors are needed in scattering experiments to obtain maximum scientific value from every probe particle. Here we deploy a hybrid pixel array direct electron detector to perform ultrafast electron diffraction experiments on a WSe 2 /MoSe 2 2D heterobilayer, resolving the weak features of diffuse scattering and moiré superlattice structure without saturating the zero order peak. Enabled by the detector’s high frame rate, we show that a chopping technique provides diffraction difference images with signal-to-noise at the shot noise limit. Finally, we demonstrate that a fast detector frame rate coupled with a high repetition rate probe can provide continuous time resolution from femtoseconds to seconds, enabling us to perform a scanning ultrafast electron diffraction experiment that maps thermal transport in WSe 2 /MoSe 2 and resolves distinct diffusion mechanisms in space and time.

36 MATERIALS SCIENCE↗