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DOE OSTI2026

Ultrafast x-ray imaging of coherently controlled molecular dynamics in real space and time

Coherent control aims to manipulate chemical processes on the latent length and timescales of atoms and bonds, scales that are intrinsic to molecular dynamics but not directly resolved by most experimental probes. As a result, existing coherent-control experiments, which overwhelmingly rely on spectroscopic observables, leave a crucial blind spot: the direct, real-space recovery of all atomic and molecular rearrangements in response to coherently controlled excitations. Here, we overcome this limitation by integrating a Tannor-Kosloff-Rice pump-control-probe scheme with ultrafast X-ray scattering to capture snapshots of the wavepacket motion in a benchmark molecular system. We demonstrate this by photoexciting diatomic iodine vapor with a visible pump pulse, selectively steering the wavepacket toward ground-state recombination or dissociative pathways with a time-delayed near-IR control pulse, and recording the dynamics with angstrom and femtosecond precision with an ultrashort hard X-ray probe pulse. By comparing these structural observations with numerical solutions of the time-dependent Schrödinger equation, we reveal how coherent control actively reshapes the molecular charge density distribution. Our results pave the way for leveraging structural feedback as a control handle and provide a fundamental microscopic visualization of quantum decoherence and energy redistribution at the atomic level.

Hopper, Thomas R. [SLAC National Accelerator Labor↗

DOE OSTI2026

Upgrades to the Thomson Scattering Diagnostic on the Lithium Tokamak eXperiment-Beta (LTX-$β$)

We describe the upgrades to the Thomson scattering (TS) diagnostic on the Lithium Tokamak eXperiment-beta (LTX- β ) to provide complete radial coverage of the plasma. LTX- β is a spherical tokamak with plasma limited at a major radius of R = 14 cm and R = 66 cm. Flat temperature profiles with peaked density were observed in LTX- β using an existing multipoint TS diagnostic with radial coverage of the plasma core. There is a need for more comprehensive core and edge TS measurements to thoroughly examine beam fueling, beam heating, and transport under low recycling conditions with liquid lithium walls and a lower collisionality scrape-off layer (SOL). The core TS set up provides plasma profiles from R = 40–60 cm. To extend the TS diagnostic coverage: 1) we added a TS viewing optics to cover the SOL region at five radial points from R = 57–64 cm, and 2) another TS viewing optics in the HFS region from R = 15–45 cm to obtain TS data from ten radial positions while making use of the original laser beam. The main focus of this article is on the new HFS TS setup that is equipped with better-matched collection optics located in the horizontal midplane where the laser polarization lies and views from a scattering angle of 130°–150° with respect to the laser path. A set of unequal-length Y-branched fiber bundles transports the TS light from two radial points to each polychromator. The new HFS view is better matched in spot size, scattering angle, and throughput to the laser and polychromators and has new V-grooved style viewing dumps. The new HFS TS view, along with the core and SOL TS views, will provide a full radial measurement coverage from R = 15–64 cm to explore the flat temperature profiles.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2026

How alkyl branching shapes structure in imidazolium and pyrrolidinium NTf 2 ionic liquids

High-energy X-ray scattering experiments and molecular dynamics (MD) simulations were carried out on ionic liquids (ILs) consisting of 1-alkyl-3-methylimidazolium and 1-alkyl-1-methylpyrrolidinium cations. These cations were paired with bis(trifluoromethylsulfonyl)amide anions and identical alkyl tails were used for both cationic species. The goal of this work is to investigate how the nanoscale structure of the ionic liquid changes with the length and with the degree of branching of the alkyl tail, for ILs having a common anion. We investigate spatial correlations in the intermolecular region, focusing on the intrinsic charge-charge interactions that characterize all ionic liquids, as well as the nanoscale domain segregation that is present in IL species with significant nonpolar components.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2025

Flower‐Type Organized Trade‐Wind Cumulus: A Multi‐Day Lagrangian Large Eddy Simulation Intercomparison Study

Shallow cumulus cloud fields in subtropical marine trade wind environments, particularly over the tropical Atlantic Ocean, show distinct organizational patterns. Among these, Flower‐type clouds are characterized by expansive stratiform cloud patches surrounded by regions of scattered convection. The objectives of this study were (a) to construct a case study of a time period during the EUREC 4 A/ATOMIC field campaign when Flower‐type organization was observed, (b) to evaluate the fidelity of a multi‐model ensemble of large eddy simulations of that case, and (c) to analyze the interaction between cloud and precipitation processes and mesoscale organization in the simulations. The simulations follow a quasi‐Lagrangian trajectory, allowing mesoscale features to develop over time in a domain that follows the boundary‐layer airmass. The results show a broad agreement in simulated thermodynamic properties across different LES codes, with Flower‐type cloud patches appearing within hours of each other. The consensus among models is consistent with observations made during the EUREC 4 A/ATOMIC field campaign on the specific day of interest. The cloud structure reveals three distinct peaks in the joint probability densities of cloud base and cloud top height, with the dominant peak at any given time influenced by the stage of cloud organization. The simulated cloud system evolution reveals consistent occurrence of maxima in liquid water path and rain rate before Flower reaches its maximum length scale. Targeted sensitivity tests reveal a weak relationship between Cloud Droplet Number concentration and the extent/degree/type of organization.

EUREC4A↗

NASA NTRS2014

The Lunar Atmosphere and Dust Environment Explorer (LADEE): Initial Science Results

On September 6, 2013, a near-perfect launch of the first Minotaur V rocket successfully carried NASA's Lunar Atmosphere and Dust Environment Explorer (LADEE) into a high-eccentricity geocentric orbit. LADEE arrived at the Moon on October 6, 2013, dur-ing the government shutdown. The spacecraft impact-ed the lunar surface on April 18, 2014, following a completely successful mission. LADEE's science objectives were twofold: (1) De-termine the composition and variability of the lunar atmosphere; (2) Characterize the lunar exospheric dust environment, and its variability. The LADEE science payload consisted of the Lunar Dust Experiment (LDEX), which sensed dust impacts in situ, for parti-cles between 100 nm and 5 micrometers; a neutral mass spectrometer (NMS), which sampled lunar exo-spheric gases in situ, over the 2-150 Dalton mass range; an ultraviolet/visible spectrometer (UVS) ac-quired spectra of atmospheric emissions and scattered light from tenuous dust, spanning a 250-800 nm wave-length range. UVS also performed dust extinction measurements via a separate solar viewer optic. The following are preliminary results for the lunar exosphere: (1) The helium exosphere of the Moon, first observed during Apollo, is clearly dominated by the delivery of solar wind He++. (2) Neon 20 is clearly seen as an important constituent of the exosphere. (3) Argon 40, also observed during Apollo and arising from interior outgassing, exhibits variations related to surface temperature-driven condensation and release, and is also enhanced over specific selenographic longi-tudes. (4) The sodium abundance varies with both lu-nar phase and with meteoroid influx, implicating both solar wind sputtering and impact vaporization process-es. (5) Potassium was also routinely monitored and exhibits some of the same properties as sodium. (6) Other candidate species were seen by both NMS and UVS, and await confirmation. Dust measurements have revealed a persistent "shroud" of small dust particles between 0.7 and sev-eral micrometers in size, present over the pre-dawn and morning sector of the Moon. This tenuous dust exosphere, with densities of approximately 10(exp -5) m(exp -3), appears to be sustained by the ejecta of micrometeoroid impacts.

lunar atmosphere↗

NASA NTRS1986

Global large scale structures in the F region

Measurements of neutral densities, temperatures and ion density and temperature by the Atmosphere Explorer C and E satellites exhibit fluctuations made up of coherent waves of scale size from hundreds to thousands of kilometers. The fluctuations in the AE-C data are found at times of low magnetic activity to extend from the auroral region in one hemisphere across the equator to the corresponding region in the other hemisphere with little change in apparent wavelength. The fluctuations in the AE-E data similarly exhibit at times of low magnetic activity nearly uniform wave structure encircling the equatorial belt. Typical examples of waves of more than 1000 km apparent wavelength in both the AE-C and AE-E data are presented. These observations during quiet times may be explained by a system of quasi-stationary waves excited by the auroral belts that are distributed about the Earth possibly with tidal or sub-tidal periods and scale lengths determined by the structure of the belts. According to this interpretation, Traveling Ionospheric Disturbance (TID's) are manifestations of transient wave systems moving past a ground observatory that result from changes in magnetic activity with periods and scale sizes associated with the regions of enhanced auroral activity. Some evidence suggesting tidal-like stationary waves from the Millstone Hill incoherent scatter radar is presented.

Gross, S. H.↗

DOE OSTI2026

Divertor detachment characterization in negative triangularity discharges in DIII-D via 2D edge-plasma transport modeling

Edge fluid modeling of the first divertor-plasma detachment experiments in negative triangularity (NT) discharges in the DIII-D tokamak is presented using the 2D multifluid edge transport code UEDGE, including cross-field particle drifts. Experiments were performed where the lower single-null magnetic equilibrium had a strong NT (δ≈−0.5), that is, where the magnetic X-point is at a larger major radius than the core magnetic axis. Divertor-plasma detachment was induced by increasing the core plasma density in DIII-D via intrinsic gas puffing. Here density scans are performed with UEDGE to reach a detached plasma and to quantitatively recover the experimental rollover of the ion saturation current on the outer divertor target plate. The simulations cover experiments with both signs of the toroidal magnetic field, B T , where the ion magnetic Grad-B drifts are directed into (forward B T ) and out of (reverse B T ) the divertor region. Consistent with experiments with neutral beam power injection, the NT simulations reproduce: 40% higher density is needed to reach detachment onset with forward B T compared with reverse B T , and the absence of deep detachment is found with reverse B T . Similarly, comparison between Ohmic discharges in NT and positive triangularity (PT) shaping confirms that a substantially higher density is needed to achieve detachment in NT than in PT, with NT requiring an line-average density of at least the Greenwald density or higher. Simulation results suggest that higher densities are needed to reach detachment in negative compared to PT because these discharges have a shorter midplane-to-target distance along the total magnetic field B, a shorter outer divertor poloidal leg length (0.06 m vs 0.2 m), and reduced radial transport [near-scrape-off layer (SOL) D ⊥ /χ ⊥ =0.3/0.5 vs D ⊥ /χ ⊥ =1.0/1.0, all in (m 2 /s)].

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

NASA NTRS1996

Jet Evolution Visualized and Quantified Using Filtered Rayleigh Scattering

Filtered Rayleigh scattering was utilized as a flow diagnostic in an investigation of a method for enhancing mixing in supersonic jets. The primary objectives of the study were to visualize the effect of vortex generating tabs on supersonic jets, to exact quantitative data from these planar visualizations, and to detect the presence of secondary flows (i.e., streamwise vorticity) generated by the tabs. An injection seeded frequency-doubled Nd:YAG was the light source and a 14 bit Princeton Instruments iodine charge coupled display (ICCD) camera recorded the image through an iodine cell. The incident wave length of the laser was held constant for each flow case so that the filter absorbed unwanted background light, but permitted part of the thermally broadened Rayleigh scattering light to pas through. The visualizations were performed for axisymmetric jets (D=1.9 cm) operated at perfectly expanded conditions for Mach 1.0, 1.5, and 2.0. All data were recorded for the jet cross section at x/D=3. One hundred instantaneous images were recorded and averaged for each case, with a threshold set to eliminate unavoidable particulate scattering. A key factor in these experiments was that the stagnation air was heated such that the expansion of the flow in the nozzle resulted in the static temperature in the jet being equal to the ambient temperature, assuming isentropic flow. Since the thermodynamic conditions of the flow were approximately the same for each case, increases in the intensity recorded by the ICCD camera could be directly attributed to the Doppler shift, and hence velocity. Visualizations were performed for Mach 1.5 and Mach 2.0 jets with tabs inserted at the nozzle exit. The distortion of the jet was readily apparent and was consistent with Mie scattering-based visualizations. Asymmetry in the intensities of the images indicate the presence of secondary flow patterns which are consistent with the streamwise vortices measured using more traditional diagnostics in subsonic jets with the same tab configurations. Because each tab causes shocks to form, the assumption of isentropic flow is not valid for these cases. However, within a reasonable first-order estimation,the intensity across the illuminated plane for these cases can be related to a value combining density and velocity.

Reeder, Mark F.↗

NASA NTRS1997

Characterization of Aircraft Produced Soot and Contrails Near the Tropopause

Participation in the SUCCESS project primarily involved development and deployment of specific instruments for characterizing jet aircraft exhaust emissions as particulates and their subsequent evolution as contrail particles, either liquid or solid, as cirrus. Observations can be conveniently considered in two categories - close or distant from the aircraft. Thus close to the aircraft the exhaust is mixing through the engine turbulence with a much drier and colder environment and developing water/ ice supersaturation along the trail depending on circumstances (near field), whereas distant from the aircraft (far field) the exhaust has cooled essentially to ambient temperature, the turbulence has decayed and any particle growth or evaporation is controlled by the prevailing ambient conditions. Intermediate between these two regions the main aircraft vortices form (one on each side of the aircraft) which tend to inhibit mixing under some conditions, a region extending from a few aircraft lengths to sometimes a hundred times this distance. Our approach to the problem lay in experience gained in characterizing the smoke from hydrocarbon combustion in terms of its cloud forming properties and its potential influence on the radiation properties of the smoke and subsequent cloud from the viewpoint of reduction (absorbtion and scattering ) of solar radiation flux leading to significant global cooling (Hudson et al 1991; Hallett and Hudson 1991). Engine exhaust contains a much smaller proportion of the fuel carbon than is sometimes present in ordinary combustion (less than 0.01% compared with 10%) and influences condensation in quite different ways, to be characterized by the Cloud Condensation Nucleus, CCN - supersaturation spectrum. The transition to ice is to be related to the dilution of solution droplets to freeze by homogeneous nucleation at temperatures somewhat below -40C (Pueschel et al 1998). The subsequent growth of ice particles depends critically on temperature, supersaturation and to some extent pressure, as is demonstrated in an NSF funded project being carried out in parallel with the work reported here. As will be discussed below, nucleation processes themselves and also exhaust impurities also influence the growth of ice particles and may control some aspects of growth of ice in contrails. Instrumentation was designed to give insight into these questions and to be flown on the NASA DC- 8 as a platform. In addition a modest program was undertaken to investigate the properties of laboratory produced smoke produced under controlled conditions from the viewpoint of forming both CCN and CN. The composition of the smoke could inferred from a thermal characterization technique; larger particles were captured by formvar replicator for detailed analysis; ice particles were captured and evaporated in flight on a new instrument, the cloudscope, to give their mass, density and impurity content.

Hallett, John↗

DOE OSTI2025

Resolving the Solvation Structure and Transport Properties of Aqueous Zinc Electrolytes from Salt-in-Water to Water-in-Salt Using Neural Network Potential

Zn Cl 2 solutions are promising electrolytes for aqueous zinc-ion batteries. Here, we report a joint computational and experimental study of the structural and dynamic properties of aqueous Zn Cl 2 electrolytes with concentrations ranging from salt-in-water to water-in-salt (WIS). By developing a neural network potential (NNP) model, we perform molecular dynamics (MD) simulations with accuracy but at much larger lengths and longer timescales. The NNP predicted structures are validated by the structure factors measured by X-ray total scattering experiments. The MD trajectories provide a comprehensive and quantitative picture of the Zn 2 + solvation shell structures. Additionally, we find that the O − H covalent bonds in water are strengthened with increasing salt concentration, thus expanding the electrochemical stability window of aqueous electrolytes. In terms of dynamic properties, the calculated and experimentally measured conductivities are in good agreement. Through the analysis of the calculated cation transference number, we propose a three-stage charge carrier transport mechanism with increasing concentration: independent ion transport, strongly correlated ion transport, and small positive charge carrier diffusion through negatively charged polymeric clusters. Our study provides fundamental atomic scale insights into the structure and transport properties of the Zn Cl 2 electrolyte that can aid the optimization and development of WIS electrolytes. Published by the American Physical Society 2025

25 ENERGY STORAGE↗

NASA NTRS1999

Chain Dynamics in Magnetorheological Suspensions

Magnetorheological (MR) suspensions are composed of colloidal particles which acquire dipole moments when subjected to an external magnetic field. At sufficient field strengths and concentrations, the dipolar particles rapidly aggregate to form long chains. Subsequent lateral cross-linking of the dipolar chains is responsible for a rapid liquid-to-solid-like rheological transition. The unique, magnetically-activated rheological properties of MR suspensions make them ideal for interfacing mechanical systems to electronic controls. Additionally, the ability to experimentally probe colloidal suspensions interacting through tunable anisotropic potentials is of fundamental interest. Our current experimental work has focused on understanding the fluctuations of dipolar chains. It has been proposed by Halsey and Toor (HT) that the strong Landau-Peierls thermal fluctuations of dipolar chains could be responsible for long-range attractions between chains. Such interactions will govern the long-time relaxation of MR suspensions. We have synthesized monodisperse neutrally buoyant MR suspensions by density matching stabilized ferrofluid emulsion droplets with D2O. This allows us to probe the dynamics of the dipolar chains using light scattering without gravitational, interfacial, and polydispersity effects to resolve the short-wavelength dynamics of the dipolar chains. We used diffusing wave spectroscopy to measure these dynamics. The particle displacements at short times that show an independence to the field strength, but at long times exhibit a constrained, sub-diffusive motion that slows as the dipole strength is increased. The experiments are in good qualitative agreement with Brownian dynamics simulations of dipolar chains. Although there have been several important and detailed studies of the structure and interactions in MR suspensions, there has not been conclusive evidence that supports or contradicts the HT model prediction that long-range interactions exist between fluctuating chains of dipolar particles. Resolving this issue would contribute greatly to the understanding of these interesting and important materials. We have begun to test the predictions of the HT model by both examining the dynamics of individual chains and by measuring the forces between dipolar chains directly to accurately and quantitatively assess the interactions that they experience. To do so, we employ optical trapping techniques and video-microscopy to manipulate and observe our samples on the microscopic level. With these techniques, it is possible to observe chains that are fluctuating freely in three-dimensions, independent of interfacial effects. More importantly, we are able to controllably observe the interactions of two chains at various separations to measure the force-distance profile. The techniques also allow us to study the mechanical properties of individual chains and chain clusters. Our work to this point has focused on reversibly-formed dipolar chains due to field induced dipoles where the combination of this chaining, the dipolar forces, and the hydrodynamic interactions that dictate the rheology of the suspensions. One can envision, however, many situations where optical, electronic, or rheological behavior may be optimized with magneto-responsive anisotropic particles. Chains of polarizable particles may have the best properties as they can coil and flex in the absence of a field and stiffen and orient when a field is applied. We have recently demonstrated a synthesis of stable, permanent paramagnetic chains by both covalently and physically linking paramagnetic colloidal particles. The method employed allows us to create monodisperse chains of controlled length. We observed the stability, field-alignment, and rigidity of this new class of materials. The chains may exhibit unique rheological properties in an applied magnetic field over isotropic suspensions of paramagnetic particles. They are also useful rheological models as bead-spring systems. These chains form the basis for our current experiments with optical traps.

Gast, A. P.↗

NASA NTRS1994

Raman-shifting an ArF excimer laser to generate new lines for obtaining optical diagnostic based information in flow fields

The application of tunable excimer lasers in combustion and flow diagnostics is almost routine nowadays. The properties of this laser system that enable density and temperature measurements in supersonic and hypersonic flow fields to be conducted are its high power, high repetition rate, and high spectral brightness. The limitation imposed by this system on these measurements is the paucity of lines in the wavelength region, the vacuum-ultraviolet, where species of interest, such as OH, N2, O2, H2, H2O, CO, NO, etc., are susceptible to electronic excitation to high-lying states. To circumvent this problem one normally resorts to nonlinear optical techniques such as frequency conversion via stimulated Raman scattering (SRS), more commonly known as Raman shifting or Raman mixing, to extend these nonintrusive and nonperturbing techniques to the shorter wavelengths in the VUV region and, for that matter, to longer wavelengths in the infrared region, if the need arises. The theoretical basis of SRS and its application are well documented in the literature. In essence, the Raman shift is a consequence of the inelastic scattering of the incident radiation by the sample. Most of the scattered radiation from the molecules of the sample is unchanged in frequency. However, a small fraction of the incident radiation is changed in frequency. This shift is a result of the fact that some of the incident photons on colliding with the molecules of the sample give up some of their energy and emerge with a lower energy resulting in the lower-frequency Stokes radiation. Other incident photons may increase their energy by colliding with the vibrationally excited molecules of the medium and emerge as higher-frequency antistokes radiation. The generation of the latter is the main objective of this project. The process, however, depends on several factors, including the beam quality of the pump laser, the cross-section of the gaseous medium, the gas pressure, and the ambient temperature of the gas near the focal region. Furthermore, since the Raman shifting process is polarization sensitive, it is necessary to have all of the laser energy in a single polarization. These factors were taken into consideration in the execution of the project. The implementation of the Raman shift was accomplished by focusing the 193 nm output of an ArF excimer laser (Lamda-Physik LPX 150) into a 1-meter long high pressure recirculating Raman cell filled with H2 gas. The laser system was modified in order to improve the mode quality of the pump beam to enhance the Raman shifting. To accomplish this feat, a prism beam expander and grating on the oscillator discharge provided wavelength tuning over the excimer gain profile. Furthermore, a triple-pass configuration, as opposed to unstable resonator optics, was employed in the operation of the amplifier cavity so that when the oscillator output radiation, focused by a 51-cm focal length fused silica lens through a 50 micron pinhole (serving as a spatial filter) and recollimated with a 25-cm focal length lens, was fed into the amplifier, it was injection locked, thereby providing tunable radiation with relatively low divergence. The forward scattered radiation emanating from the impingement of the modified pump beam on the Raman cell was detected using an energy meter after the latter had been separated from it using a dispersing prism.

Koker, Edmond B.↗