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DOE OSTI2026

Signatures of Antisymmetric Vibrations in the Ultrafast Dynamics of Quadrupolar Dyes

Antisymmetric molecular vibrations are central to ultrafast, nonadiabatic photophysical and photochemical processes such as conical intersection dynamics, Herzberg–Teller couplings and, potentially, singlet fission. Direct spectroscopic identification of such vibrations is, however, challenging, since they are typically Raman inactive and affect optical transitions only weakly. Here, we report experimental signatures of vibronic couplings to a high-frequency antisymmetric vibration in the excited state dynamics of a quasi-quadrupolar molecule by ultrafast two-dimensional electronic spectroscopy (2DES). The early time, sub-50 fs 2DES maps reveal an asymmetric peak pattern with characteristic low-energy cross-peaks. We show that these peaks arise from stimulated emission transitions from an anharmonic, double-minimum excited state potential energy surface formed by vibronic coupling to a high-frequency antisymmetric mode. Simulations based on a phenomenological essential state model support the results. Our findings offer a new approach for identifying antisymmetric vibrations in ultrafast 2DES and track excited state wavepacket motion before relaxation washes out the spectra.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Fire–precipitation interactions amplify the quasi-biennial variability in fires over southern Mexico and Central America

Fires have great ecological, social, and economic impact. However, fire prediction and management remain challenges due to a limited understanding of their roles in the Earth system. Fires over southern Mexico and Central America (SMCA) are a good example of this, greatly impacting local air quality and regional climate. Here we report that the spring peak (April–May) of fire activities in this region has a distinct quasi-biennial signal based on multiple satellite datasets measuring different fire characteristics. The variability is initially driven by quasi-biennial variations in precipitation. Composite analysis indicates that strong fire years correspond to suppressed ascending motion and weakened precipitation over the SMCA. The anomalous precipitation over the SMCA is further found to be mostly related to the East Pacific–North Pacific (EP-NP) pattern 2 months prior to the fire season. The positive phase of the EP-NP leads to enhanced precipitation over the eastern US but suppressed precipitation over the SMCA, similar to the spatial pattern of precipitation differences between strong and weak fire years. Meanwhile, the quasi-biennial signals in precipitation and fires appear to be amplified by their interactions through a positive feedback loop at short timescales. Model simulations show that in strong fire years, more aerosol particles are released and transported downstream over the Gulf of Mexico and the eastern US, where suspended light-absorbing aerosols warm the atmosphere and cause the ascending motion of the air aloft. Subsequently, a compensating downward motion is formed over the region of the fire source and ultimately suppresses precipitation and intensifies fires. Statistical analysis shows the different durations of the two-way interaction, where the fire suppression effect of precipitation lasts for more than 20 d, while fire leads to a decrease in precipitation at shorter timescales (3–5 d). This study demonstrates the importance of fire–climate interactions in shaping the fire activities on an interannual scale and highlights how precipitation–fire interactions at short timescales contribute to the interannual variability in both fire and precipitation.

54 ENVIRONMENTAL SCIENCES↗

NASA NTRS1981

Radiometry with nighttime DMSP images in digital form

The USAF Defense Meteorological Satellite Program (DMSP) spacecraft sends images to earth in the form of numbers. It has been common practice to erase the only digital records, the magnetic tapes, for reuse, after films (resembling photographs) have been created from the numbers. While the DMSP images have been widely used, their application in research has been hindered by both the lack of digital data and the lack of an authoritative source of related technical information. The character of the digital form is considered. Each image is essentially a three-dimensional list (X,Y,Z) in which X and Y represent the position coordinates of a pixel and Z is its associated radiance. Only the value of Z is given and the X-Y position must be deduced from adjunct information. Each original scan composed of 1464 pixels represents an area on the earth's surface about 3 km wide and 3000 km long. Strengths and weaknesses of the system with respect to research applications are considered, and concepts for the design of a nocturnal imager are discussed.

Croft, T. A.↗

NASA NTRS1983

2-165 keV observations of active galaxies and the diffuse background

HEAO 1 spectral observations of 12 active galaxies in the 12-165 keV and 2-50 keV ranges are reported. The spectra of these galaxies in the 2-165 keV range are well represented by a single power law model; within experimental uncertainties a narrow dispersion in power law index attributable to the individual galaxies is observed, while the 2-165 keV luminosities of these galaxies ranged from 3 x 10 to the 43rd to 3 x 10 to the 45th ergs/s. An apparent universality of the spectral form is found which can be interpreted as due to a common electron distribution with a temperature of tens of keV in the Compton scattering region or as a common nonthermal power-law distribution generating the observed flux through synchrotron-Compton processes. The data indicate that relativistic particles are likely to be responsible for the X-rays from cores of active galaxies through synchroton-Compton processes. In addition, it is noted that only weak number evolution, if any at all, is present in active galaxies.

Rothschild, R. E.↗

NASA NTRS1990

Effects of grain size and grain boundary on critical current density of high T(sub c) superconducting oxides

By means of adding impurity elements in high T sub c oxides, the effects were studied of grain size and grain boundary on the critical current density of the following systems: YBa2Cu3O(7-y) and Bi-Pr-Sr-Ca-Cu-O. In order to only change the microstructure instead of the superconductivity of the grains in the samples, the impurity elements were added into the systems in terms of the methods like this: (1) substituting Y with the lanthanide except Pr, Ce, and Tb in YBa2Cu3O(7-y) system to finning down grains in the samples, therefore, the effect can be investigated of the grain size on the critical current density of 1:2:3 compounds; (2) mixing the high T sub c oxides with the metal elements, such as Ag, according to the composition of (high T sub c oxide)1-xAgx to metallize the grain boundaries in the samples, studying the effect of the electric conductivity of the grain boundaries on the critical current density; (3) adding SiO2, PbO2, and SnO2 into the high T sub c oxide to form impurity phases in the grain boundaries, trying to find out the effects of the impurity phases or metalloid grain boundaries on the critical current density of the high T sub c superconductors. The experimental results indicate that in the case of of the presence of the metalloid grain boundaries finning down grains fails to enhance the j sub c, but restrains it strongly, the granular high T sub c superconductors with the small size grains coupled weakly is always the low j sub c system.

Zhao, Y.↗

NASA NTRS1993

Solitary waves in the atmosphere

The weakly nonlinear theory for internal solitary waves is reviewed, and theoretical results of the vertical and horizontal structure of temperature, vertical displacements, and vertical and horizontal perturbations to the wind field associated with steadily propagating solitary waves are presented in two idealized atmospheric configurations. One configuration is representative of solitary waves observed in the lower troposphere and the other of solitary waves that occupy the entire troposphere. The important results of the theory are presented in a form that can be readily used by observationalists. The results obtained are then analyzed using actual rawinsonde data for two well-documented observations of atmospheric solitary waves, which are analogous to the two idealized configurations. The importance and difficulties of properly identifying the waveguide within which the solitary wave is confined are discussed. The fundamental role of a critical level in ducting the disturbances and thus in defining the thickness of the waveguide is illustrated in the example dealing with the solitary wave occupying the entire troposphere. Together, these two examples illustrate the decisions and compromises that must be made in applying the theory to the real atmosphere.

Rottman, James W.↗

NASA NTRS1993

Comprehensive investigation of HgCdTe metalorganic chemical vapor deposition

The principal objective of this experimental and theoretical research program was to explore the possibility of depositing high quality epitaxial CdTe and HgCdTe at very low pressures through metalorganic chemical vapor deposition (MOCVD). We explored two important aspects of this potential process: (1) the interaction of molecular flow transport and deposition in an MOCVD reactor with a commercial configuration, and (2) the kinetics of metal alkyl source gas adsorption, decomposition and desorption from the growing film surface using ultra high vacuum surface science reaction techniques. To explore the transport-reaction issue, we have developed a reaction engineering analysis of a multiple wafer-in-tube ultrahigh vacuum chemical vapor deposition (UHV/CVD) reactor which allows an estimate of wafer or substrate throughput for a reactor of fixed geometry and a given deposition chemistry with specified film thickness uniformity constraints. The model employs a description of ballistic transport and reaction based on the pseudo-steady approximation to the Boltzmann equation in the limit of pure molecular flow. The model representation takes the form of an integral equation for the flux of each reactant or intermediate species to the wafer surfaces. Expressions for the reactive sticking coefficients (RSC) for each species must be incorporated in the term which represents reemission from a wafer surface. The interactions of MOCVD precursors with Si and CdTe were investigated using temperature programmed desorption (TPD) in ultra high vacuum combined with Auger electron spectroscopy (AES). These studies revealed that diethyltellurium (DETe) and dimethylcadmium (DMCd) adsorb weakly on clean Si(100) and desorb upon heating without decomposing. These precursors adsorb both weakly and strongly on CdTe(111)A, with DMCd exhibiting the stronger interaction with the surface than DETe.

Raupp, Gregory B.↗

NASA NTRS2011

Concerning the Motion and Orientation of Flux Transfer Events Produced by Component and Antiparallel Reconnection

We employ the Cooling et al. (2001) model to predict the location, orientation, motion, and signatures of flux transfer events (FTEs) generated at the solstices and equinoxes along extended subsolar component and high ]latitude antiparallel reconnection curves for typical solar wind plasma conditions and various interplanetary magnetic field (IMF) strengths and directions. In general, events generated by the two mechanisms maintain the strikingly different orientations they begin with as they move toward the terminator in opposite pairs of magnetopause quadrants. The curves along which events generated by component reconnection form bow toward the winter cusp. Events generated by antiparallel reconnection form on the equatorial magnetopause during intervals of strongly southward IMF orientation during the equinoxes, form in the winter hemisphere and only reach the dayside equatorial magnetopause during the solstices when the IMF strength is very large and the IMF points strongly southward, never reach the equatorial dayside magnetopause when the IMF has a substantial dawnward or duskward component, and never reach the equatorial flank magnetopause during intervals of northward and dawnward or duskward IMF orientation. Magnetosheath magnetic fields typically have strong components transverse to events generated by component reconnection but only weak components transverse to the axes of events generated by antiparallel reconnection. As a result, much stronger bipolar magnetic field signatures normal to the nominal magnetopause should accompany events generated by component reconnection. The results presented in this paper suggest that events generated by component reconnection predominate on the dayside equatorial and flank magnetopause for most solar wind conditions.

Sibeck, D. G.↗

DOE OSTI2020

Learning how structures form in drift-wave turbulence

Drift-wave turbulence produces anomalous transport via cross-correlations between fluctuations. This transport has profound implications for confinement, structure formation, and virtually all aspects of the non-linear turbulent dynamics. Herein, we use a data-driven method based on deep learning in order to study turbulent transport in the 2D Hasegawa–Wakatani system and infer a reduced mean-field model from numerical solution. In addition to the usual turbulent diffusion, we find an effect which couples the particle flux to the local gradient of vorticity, which tends to modulate the density profile. The direct coupling to the shear is relatively weak. In addition, the deep learning method finds a model for spontaneous zonal flow generation by negative viscosity, stabilized by non-linear and hyperviscous terms. We compare these results to analytic calculations using quasilinear theory and wave kinetics, finding qualitative agreement, though the calculations miss certain higher-order effects. A simplified, 1-D model for the evolution of the profile, flow, and intensity based on the deep learning results is solved numerically and compared to previous models for staircasing based on bistability. We see that the physics uncovered by the deep learning method provided simple explanations for the formation of zonal structures in the density, flow, and turbulence fields. We highlight the important role of symmetry in the deep learning method and speculate on the portability of the method to other applications.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

DOE OSTI2025

High-significance detection of correlation between the unresolved gamma-ray background and the large-scale cosmic structure

Our understanding of the γ-ray sky has improved dramatically in the past decade, however, the unresolved γ-ray background (UGRB) still has a potential wealth of information about the faintest γ-ray sources pervading the Universe. Statistical cross-correlations with tracers of cosmic structure can indirectly identify the populations that most characterize the γ-ray background. In this study, we analyze the angular correlation between the γ-ray background and the matter distribution in the Universe as traced by gravitational lensing, leveraging more than a decade of observations from the Fermi-Large Area Telescope (LAT) and 3 years of data from the Dark Energy Survey (DES). We detect a correlation at signal-to-noise ratio of 8.9. Most of the statistical significance comes from large scales, demonstrating, for the first time, that a substantial portion of the UGRB aligns with the mass clustering of the Universe as traced by weak lensing. Blazars provide a plausible explanation for this signal, especially if those contributing to the correlation reside in halos of large mass (∼ 10 14 M ⊙ ) and account for approximately 30–40% of the UGRB above 10 GeV. Additionally, we observe a preference for a curved γ-ray energy spectrum, with a log-parabolic shape being favored over a power-law. We also discuss the possibility of modifications to the blazar model and the inclusion of additional γ-ray sources, such as star-forming galaxies, misalinged active galactic nuclei, or particle dark matter.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2022

Carbodiimide‐Induced Formation of Transient Polyether Cages**

Abstract The use of “fuel” compounds to drive chemical systems out of equilibrium is currently of interest because of the potential for temporally controlled, responsive behavior. We have recently shown that transiently formed crown ethers exhibit counterintuitive templation effects when generated in the presence of alkali metal cations: “matched” cations, such as K + with an 18‐crown‐6 analogue, suppress the formation of the macrocycles (negative templation). In this work, we describe two macrocyclic diacids that, on treatment with carbodiimides, give transient macrobicyclic cages analogous to polyether cages. Negative templation effects are observed for the smaller cage when generated in the presence of K + and Na + , but there is a weak, but reproducible, positive templation effect in the presence of Li + . The larger cage behaves similarly in the presence of Li + , K + , Rb + , and Cs + , but differently with Na + , which appears to bind to both the cage and the initial macrocycle.

Hossain, Mohammad Mosharraf↗

DOE OSTI2021

Applications of Strain-Coupled Magnetoelectric Composites

This article deals with research, development and future directions of magnetoelectric composites for practical devices applications. In the past 20 years there has been a surge of research in the area of multiferroics (MF) and magnetoelectrics (ME) due to their potential to replace existing technologies based only on ferroelectric or ferromagnetic materials. Some of the magnetoelectric composites show exceptionally high potential in the area of magnetic field sensors, however, work remains before commercialization can be realized. The cross coupling among various ferroic parameters in magnetoelectric composites is several orders higher than single phase magetoelectrics, which make its favorable for low detection (nT or pT) magnetic field sensors. Advances in both layered structures or controlled three-dimensional matrix composites for applications as magnetoelectric nonvolatile memory elements are both required. Robust cross-coupling among various parameters with more than four logic states and its compatibility with complementary-symmetry metal–oxide–semiconductor (CMOS) technology are the main requirements for heterostructure magnetoelectric thin films. The major hurdles in the area of magnetoelectric nonvolatile memory elements are poor interfacial properties and weak magnetoelectric coupling for high density fast read and write processes. Another potential area is strained coupled magneto-electric composites where magnetostriction mediated dimensional change in the magnetic layer effectively modulate the change in the dimension of piezoelectric layers via piezostriction, which leads to a strong ME coupling where their coupling magnitude is sufficient for magnetic field sensors. Energy harvesters based on magnetoelectric composites are also intriguing concepts to capture various types of waste energy, in the form mechanical vibration, pressure, wind energy, hydrothermal and waste temperature.

36 MATERIALS SCIENCE↗

DOE OSTI2022

Hydrokinetic energy conversion using flow induced oscillations of single-cylinder with large passive turbulence control

Various types of flow-induced oscillations (FIOs) have been implemented in development of marine hydrokinetic (MHK) energy converters. With passive turbulence control (PTC), energy harvesting starts at a flow speed of about 0.5 m/s. However, there is worldwide MHK energy available in even slower currents. In the present study, the effect of damping on FIO and power extraction is investigated for a converter with large turbulence stimulation (PTC) consisting of straight strips with a height of 15% of the cylinder diameter and placed symmetrically on the cylinder surface. The oscillating amplitude decreases, as the damping ratio increases, with unchanged sinusoidal pattern of the displacement time-history. The frequency ratio is also affected by damping especially in the VIV initial branch and transition region between VIV and galloping. An important flow characteristic of the large-PTC cylinder is that a recirculation region is formed behind the PTC, causing appreciable disturbance to the flow past the cylinder. Power can be harvested in the whole FIO range and the harnessed power maximum appears at the largest inflow velocity tested. However, the optimum of harnessing efficiency is located at the beginning of the VIV upper branch. The gap between VIV and galloping is bridged when large PTC is used, eliminating the drop in power and efficiency even at higher damping, which would be a weakness of regular-PTC cylinder for energy harvesting. Finally, the mechanism behind the variation of harnessing efficiency with inflow velocity and damping ratio is revealed, and the optimality criterion for the converter design is discussed.

16 TIDAL AND WAVE POWER↗

DOE OSTI2026

Mechanism of ion pairing–induced co-ion penetration into the stern layer

In classical electric double layer (EDL) theory, co-ions—ions carrying the same charge as the electrode—are assumed to be excluded from the Stern layer because of electrostatic repulsion. However, ion pairing with adsorbed counterions may enable co-ions to access the EDL, a phenomenon that remains underexplored. Key questions therefore remain unresolved, including how deeply co-ions penetrate, how ion-specific properties govern them, and how ion pairing within the EDL differs from bulk solution. Here, in this study, we employ molecular dynamics simulations combined with well-tempered metadynamics to quantify co-ion penetration and ion-pairing thermodynamics at positively charged Mg-Al layered double hydroxide interfaces (σ = +20.6 μC/cm 2 ) in aqueous chloride electrolytes across 0.005–3 M range. We reveal a concentration-driven crossover: at dilute conditions, counterion–co-ion contact ion pairing (CIP) is thermodynamically unfavorable or only weakly favorable (ΔG CIP = +0.12 kcal/mol for Li + to −0.42 kcal/mol for K + ), leading to co-ion exclusion. As concentration increases (≥0.5 M), enhanced screening reduces surface repulsion and stabilizes CIP thermodynamics (ΔG CIP = −0.89 kcal/mol for Li + to −1.05 kcal/mol for K + at 3 M), enabling monovalent co-ions to penetrate the Stern layer following the hydration hierarchy K + > Na + > Li + , while divalent co-ions (Mg 2+ , Ca 2+ ) remain in the diffuse layer, forming only solvent-separated pairs. Comparison with bulk solution shows interfacial ion pairing is suppressed at low concentrations but converges to bulk-like thermodynamics at high concentrations, indicating surface effects vanish under strong screening. These results establish a quantitative framework linking ion-pairing thermodynamics to co-ion penetration and providing strategies to design electrochemical interfaces.

Co-ion penetration↗

DOE OSTI2024

Physical properties of asteroid Dimorphos as derived from the DART impact

On 26 September 2022, NASA’s Double Asteroid Redirection Test (DART) mission successfully impacted Dimorphos, the natural satellite of the binary near-Earth asteroid (65803) Didymos. Numerical simulations of the impact provide a means to find the surface material properties and structures of the target that are consistent with the observed momentum deflection efficiency, ejecta cone geometry and ejected mass. Our simulation that best matches the observations indicates that Dimorphos is weak, with a cohesive strength of less than a few pascals, like asteroids (162173) Ryugu and (101955) Bennu. We find that the bulk density of Dimorphos ρ B is lower than ~2,400 kg m – 3 and that it has a low volume fraction of boulders (≲40 vol%) on the surface and in the shallow subsurface, which are consistent with data measured by the DART experiment. These findings suggest that Dimorphos is a rubble pile that might have formed through rotational mass shedding and reaccumulation from Didymos. Our simulations indicate that the DART impact caused global deformation and resurfacing of Dimorphos. ESA’s upcoming Hera mission may find a reshaped asteroid rather than a well-defined crater.

79 ASTRONOMY AND ASTROPHYSICS↗

NASA NTRS1982

Characteristics of downdrafts and turbulence within thunderstorms

Triple Doppler radar observations are presented of downdrafts and turbulence within three convective cloud systems that formed over the South Park region of central Colorado. Downdrafts and turbulence are treated together here because of the relationship suggested by the fact that both can be produced by the mixing of cloudy and dry environmental air. What is more, overlays of estimated turbulent kinetic energy dissipation on general flow patterns yield additional information (including the locations of entrainment) on circulations within convective clouds. The relationship between downdrafts and turbulence is established, and examples are presented of weak to moderate downdrafts and turbulence within three convective storms. The differences in downdraft strength and turbulence intensity in the three cases examined are analyzed.

Knupp, K. R.↗

NASA NTRS1985

Magnetotails of the terrestrial planets: A comparative study

Spacecraft observations have established that all of the terrestrial planets interact strongly with the solar wind and possess well developed magnetic tails. At Mercury, Earth, and possibly Mars the tail forms as a result of the solar wind dragging back field lines intrinsic to the planet. Venus differs dramatically from the other planets in that its magnetotail is composed of interplanetary field lines draped about the ionopause. Accordingly, the observations made at the terrestrial planets provide an opportunity to compare not only induced (Venus) magnetic tail properties with those of intrinsic field tails, but also the variation among intrinsic field tails ion the limits of no ionosphere (Mercury), weak intrinsic magnetic field (Mars), and strong magnetic field and ionosphere (Earth). A comparative investigation is made of terrestrial planet magnetotail structure and dynamics. The results are discussed in terms of the physical properties of these planets and their interactions with the solar wind.

Slavin, J. A.↗

NASA NTRS1992

The lunar environment and its effect on optical astronomy

The Moon's geologic environment features: (1) gravity field one-sixth that of Earth; (2) sidereal rotation period of 27.3 days; (3) surface with greater curvature than Earth's surface (a chord along a 10 km baseline would have a bulge of 7.2 m); (4) seismically and tidally stable platform on which to make astronomical observations (most moonquakes have magnitudes of 1 to 2 on the Richter scale, within the earth's seismic noise, resulting in ground motions only 1 nm); (5) tenuous atmosphere (the total mass at night is only 10(exp 4) kg) that has an optical depth of 10(exp -6) and does not cause wind induced stresses and vibrations on structures; (6) large diurnal temperature variation (100 to 385 K in equatorial regions), which telescopes must be designed to withstand; (7) weak magnetic field, ranging from 3 to 330 x 10(exp -9) T, compared to 3 x 10(exp -5) T on Earth at the equator; (8) surface exposed to radiation, the most dangerous of which are high energy (1 to 100 Mev) particles resulting from solar flares; (9) high flux of micrometeorites which are not slowed down from their cosmic velocities because of the lack of air (data indicate that microcraters greater than 10 microns across will form at the rate of 3000/sq m/yr); (10) regolith 2 to 30 m thick which blankets the entire lunar surface (this layer is fine-grained (average grain sizes range from 40 to 268 microns), has a low density (800 to 1000 kg/cu m in the upper few mm, rising to 1500 to 1800 kg/cu m at depths of 10 to 20 cm), is porous (35 to 45 pct), cohesive (0.1 to 1.0 kN/sq m), and has a low thermal diffusivity (0.7 to 1.0 x 110-8 sq m/sec); about 29 pct of the regolith is less than 20 micron in size (this dust could pose a hazard to optical telescopes); (11) rubbly upper several hundred meters in which intact bedrock is uncommon, especially in the lunar highlands; and (12) craters with diameter-to-depth ratios of 5 if fresh and less than km across (larger and eroded craters have diameter-to-depth ratios greater than 5).

Taylor, G. Jeffrey↗