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All sourcesNASA NTRSDOE OSTI
NASA NTRS1978

Energetic protons associated with interplanetary active regions 1-5 AU from the sun

Pioneer 11 has yielded data on approximately 100 energetic proton events at heliocentric distances between 1 and 2 AU. Measurements of absolute intensities, anisotropies, and crude energy spectra are studied in connection with interplanetary active regions (IAR's). It is found that in close vicinity to IAR's, the number of events observed per unit time interval is 10 times greater than in other areas of interplanetary space, and that the frequency of events has a maximum at plus or minus 5 hours of the time IAR edges are crossed. It is also noted that events in IAR vicinity have greater particle densities, softer energy spectra, and smaller time widths than other events. For many events associated with IAR's, particle anisotropies correspond to the net flow of particles along the interplanetary magnetic field toward the sun. This suggests that a mechanism in MHD shocks is responsible for local acceleration in the interplanetary medium.

Pesses, M. E.↗
NASA NTRS2006

Low-Velocity Impact Response of Sandwich Beams with Functionally Graded Core

The problem of low-speed impact of a one-dimensional sandwich panel by a rigid cylindrical projectile is considered. The core of the sandwich panel is functionally graded such that the density, and hence its stiffness, vary through the thickness. The problem is a combination of static contact problem and dynamic response of the sandwich panel obtained via a simple nonlinear spring-mass model (quasi-static approximation). The variation of core Young's modulus is represented by a polynomial in the thickness coordinate, but the Poisson's ratio is kept constant. The two-dimensional elasticity equations for the plane sandwich structure are solved using a combination of Fourier series and Galerkin method. The contact problem is solved using the assumed contact stress distribution method. For the impact problem we used a simple dynamic model based on quasi-static behavior of the panel - the sandwich beam was modeled as a combination of two springs, a linear spring to account for the global deflection and a nonlinear spring to represent the local indentation effects. Results indicate that the contact stiffness of thc beam with graded core Increases causing the contact stresses and other stress components in the vicinity of contact to increase. However, the values of maximum strains corresponding to the maximum impact load arc reduced considerably due to grading of thc core properties. For a better comparison, the thickness of the functionally graded cores was chosen such that the flexural stiffness was equal to that of a beam with homogeneous core. The results indicate that functionally graded cores can be used effectively to mitigate or completely prevent impact damage in sandwich composites.

Apetre, N. A.↗
NASA NTRS1993

Gravity investigation of the Manson impact structure, Iowa

The Manson crater, of probable Cretaceous/Tertiary age, is located in northwestern Iowa (center at 42 deg. 34.44 min N; 94 deg. 33.60 min W). A seismic reflection profile along an east west line across the crater and drill hole data indicate a crater about 35 km in diameter having the classic form for an impact crater, an uplifted central peak composed of uplifted Proterozoic crystalline bedrock, surrounded by a 'moat' filled with impact produced breccia and a ring graben zone composed of tilted fault blocks of the Proterozoic and Paleozoic country rocks. The structure has been significantly eroded. This geologic structure would be expected to produce a significant gravity signature and study of that signature would shed additional light on the details of the crater structure. A gravity study was undertaken to better resolve the crustal structure. The regional Bouguer gravity field is characterized by a southeastward decreasing field. To first order, the Bouguer gravity field can be understood in the context of the geology of the Precambrian basement. The high gravity at the southeast corner is associated with the mid-continent gravity high; the adjacent low to the northwest results from a basin containing low-density clastic sediments shed from the basement high. Modeling of a simple basin and adjacent high predicts much of the observed Bouguer gravity signature. A gravity signature due to structure associated with the Manson impact is not apparent in the Bouguer data. To resolve the gravity signature of the impact, a series of polynomial surfaces were fit to the Bouguer gravity field to isolate the small wavelength residual anomalies. The residual gravity obtained after subtracting a 5th- or 6th-order polynomial seems to remove most of the regional effects and isolate local anomalies. The pattern resolved in the residual gravity is one of a gravity high surrounded by gravity lows and in turn surrounded by isolated gravity highs. The central portion of the crater is characterized by two positive anomalies having amplitudes of about plus 4 mGal separated by a gentle saddle located approximately at the crater center.

Plescia, J. B.↗
DOE OSTI2023

Injection mechanisms in a III -nitride light-emitting diode as seen by self-emissive electron microscopy

Here, we report on the investigation of an electrically biased high efficiency green III-nitride light-emitting diode (LED) by electron emission microscopy (EEM) using a low-energy electron microscope (LEEM). The surface of the LED was activated to negative electron affinity via deposition of a submonolayer of Cs. With the illumination column of the LEEM turned off, upon electrical injection of the LED, we directly image the hot electrons generated by eeh Auger-Meitner nonradiative processes that diffuse through the top p-Ga N layer and emit out the surface of the biased LED. By determining the source of emitted electrons using complementary electron emission spectroscopy measurements, EEM allows us to effectively map the carrier density within the LED. Using EEM, we observed nonelectron emitting regions with a density of approximately 3 × 10 8 cm -2 , identified as V-shaped defects (V-defects). This is confirmed through the corresponding dark spots of panchromatic cathodoluminescence measurements of the same sample and by plan-view transmission electron microscopy. The absence of electron emission at the sidewall of the V-defects can be attributed to several factors, including reduced carrier density in the sidewall quantum wells due to carriers traveling fast through the semipolar sidewalls before being injected into the planar quantum wells, the reduced population of hot electrons surviving diffusion through the thicker p-GaN filling in the V-defect before emission onto vacuum, and a smaller Auger-Meitner coefficient for the low In content semipolar sidewall quantum wells. The stronger electron emission observed at the ridges of most V-defects compared to the planar quantum well regions indicates larger local injected carrier densities, confirming that V-defect sidewalls allow for strong lateral carrier injection when compared to the weaker vertical injection away from the V-defect as evidenced by the weaker electron emission intensity away from the V-defects.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗
NASA NTRS1981

Heat transfer on a flat plate in continuum to rarefied hypersonic flows at Mach numbers of 19.2 and 25.4

Local heat transfer rates were measured on a flat steel plate (10 in. wide and 16 in. long) with sharp and blunt leading edges (0.001 and 0.010 in.) in the transition from the strong interaction boundary layer regime with no slip at the surface to the free molecule regime. The tests were conducted in a combustion driven hypersonic shock tunnel, with the nominal free stream Mach numbers of 19.2 and 25.4, and a reflected stagnation temperature of approximately 2340 R. The twelve heat transfer gages were made of platinum sputtered on a Pyrex backing to a thickness of approximately 350 A, insulated by a silicone dioxide film. For both Mach numbers the heat transfer data agreed reasonably well with the strong interaction prediction of Li and Nagamatsu (1953, 1955) for unit Reynolds numbers greater than approximately 100,000 and leading edge Knudsen numbers less than approximately 4. At lower density conditions the rarefied flow effects began to dominate the flow phenomena near the leading edge region of the sharp flat plate. A systematic reduction in the heat transfer rate close to the leading edge was observed for both Mach number tests as the leading edge density was reduced and the mean free path was increased.

Nagamatsu, H. T.↗
DOE OSTI2022

The importance of maldistribution matching for thermal performance of compact heat exchangers

Compact heat exchangers have gained increased attention in recent years, particularly in demanding applications where high temperatures, high pressures, and/or high power densities are required. For decades, the heat exchanger (HX) community believes that flow maldistribution is a key factor for HX effectiveness, that is, reducing the degree of flow maldistribution (MALD) can help increase the HX effectiveness. Therefore, significant efforts have been devoted in the past to optimizing the header geometry to minimize flow maldistribution. This work was initially motivated by this, and the original goal was to figure out a HX header design with the lowest maldistribution. However, by systematically constructing a comprehensive maldistribution matrix, the analysis revealed that the HX effectiveness is not actually determined by the MALD, but instead dominated by the degree of maldistribution mismatch (MISM). This conclusion was also theoretically generalized, which indicated that matching of the local heat capacity rate is key for achieving maximum performance. The MISM provides a local means of tracking this information, while the MALD only provides a global approximation of the maldistribution itself. With this new perspective, flow maldistribution needs not necessarily be avoided, but instead matched between two fluid streams, to improve the HX performance. We demonstrated that by carefully designing the header geometry to match the velocity profiles of the two fluids in a 2 MW PCHE with molten salt and supercritical carbon dioxide (sCO2) as the heat transfer fluids, the HX could achieve a higher effectiveness even when the maldistribution increased. Finally, a technoeconomic study using a CSP system as an example revealed that the use of this new HX design paradigm could result in CSP capital cost savings as large as 16.6%.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗
DOE OSTI2022

AmeriFlux FLUXNET-1F US-Me2 Metolius mature ponderosa pine

This is the AmeriFlux Management Project (AMP) created FLUXNET-1F version of the carbon flux data for the site US-Me2 Metolius mature ponderosa pine. This is the FLUXNET version of the carbon flux data for the site US-Me2 Metolius mature ponderosa pine produced by applying the standard ONEFlux (1F) software. Site Description - Site Description before Fire (January, 2002 - August, 2020): The mean stand age is 71 years old and the stand age of the oldest 10% of trees is about 108 years old. This site is one of the Metolius core cluster sites with different age and disturbance classes and part of the AmeriFlux network. The overstory is almost exclusively composed of ponderosa pine trees (Pinus ponderosa Doug. Ex P. Laws) with a few scattered incense cedars (Calocedrus decurrens (Torr.) Florin) and has a peak leaf area index (LAI) of 2.1 m2 m-2. Tree height is relatively homogeneous at about 18 m, and the mean tree density is approximately 339 trees ha-1 (Irvine et al., 2008). The understory is sparse with an LAI of 0.2 m2 m-2 and primarily composed of bitterbrush (Purshia tridentata (Push) DC.) and greenleaf manzanita (Arctostaphylos patula Greene). Soils at the site are sandy (69%/24%/7% sand/silt/clay at 0–0.2 m depth and 66%/27%/7% at 0.2–0.5 m depth, and 54%/ 35%/11% at 0.5–1.0 m depth), freely draining with a soil depth of approximately 1.5 m (Irvine et al., 2008; Law et al., 2001b; Schwarz et al., 2004). Green Ridge Fire: On August 20, 2020, the Green Ridge Fire burned through Us-Me2. The fire was ignited by lightning on August 16th, and grew rapidly to the east over the first few days driven by strong, downslope (westerly) afternoon winds. Fire behavior and observed fire effects were highly heterogeneous due to the localized wind pattern carrying the flaming head of the fire forward, and the efforts being made by suppression resources to contain the fire. The site experienced the full range of fire effects, from <1 m high surface fire that charred litter and duff and only consumed shrubs and herbaceous material to full tree (>15 m) crown fire that consumed 100% of needles, small limbs, and surface fuels at high intensity, leaving only ash and bare soil post-fire. Salvage Logging: From late March to late April 2021, salvage logging by the landowner occurred at the site. Almost all trees within the flux footprint were logged except a small area with lower burn severity, where sap flow and automatic soil respiration measurements are continued since the fire. In August 2022 the primary flux system was moved from the top of the damaged tall tower to a nearby shorter tower centering on the salvage/regenerating footprint.

Hanson, Chad↗
DOE OSTI2024

Hole doping and electronic correlations in Cr substituted BaFe$_{2}$As$_{2}$

For a significant composition range, the suppression of the spin density wave transition temperature (T SDW ) in Cr- and Mn-substituted BaFe 2 As 2 (CrBFA and MnBFA, respectively) coincides as a function of Cr/Mn content, despite the distinct electronic effects of these substitutions. Additionally, for any Cr/Mn content superconductivity (SC) is absent and this topic is particularly less explored in the case of CrBFA. Here, in this work, we employ angle-resolved photoemission spectroscopy (ARPES) and combined density functional theory plus dynamical mean field theory (DFT+DMFT) to address the evolution of the Fermi surface (FS) and electronic correlations in CrBFA. Our findings reveal that incorporating Cr leads to an effective hole doping of the states near the FS, which is well described within the virtual crystal approximation (VCA). Moreover, analysis of the ARPES spectra of the bands with main d yz -orbital character reveals a fractional scaling of the imaginary part of self-energy as a function of the binding energy, a signature property of Hund's correlations. Our DFT+DMFT calculations support these experimental findings. We conclude that CrBFA is a correlated electron system for which the changes in the FS as a function of Cr are unrelated to the suppression of T SDW . In addition, we suggest that the absence of SC is primarily due to the competition between Cr local moments and the Fe-derived itinerant spin fluctuations.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗
DOE OSTI2022

High temperature stability and transport characteristics of hydrogen in alumina via multiscale computation

Here, the impact of hydrogen charge states on the stability and transport characteristics of hydrogen interstitials in alumina polymorphs is evaluated by multiscale computational methods including density functional theory (DFT), ab initio molecular dynamics (AIMD) and machine learned force fields. Thermodynamic calculations show that the protonic H i +1 interstitial is the most stable defect species for most values of the electronic bandgap in both and amorphous alumina (Al 2 O 3 ). Further, active learned Gaussian approximation potentials (GAP) were developed using AIMD data to study temperature dependent long time proton diffusion in alumina. Diffusivity calculations from GAP-MD simulations are found to be comparable with of the AIMD data, while being ~340 times faster and scalable to larger systems. Comparisons with diffusivity values for other interstitial charge states (H i 0 and H i -1 ) and published experimental literature indicate that H i +1 diffusion is the likely mechanism of hydrogen transport. A good agreement is obtained between H i +1 diffusivity calculated in α-Al 2 O 3 from DFT: 5.05 10 -3 exp(-0.81 eV/k B /T) cm 2 /s and reported experiment: 9.7X10 -4 exp(-0.83 eV/k B /T) cm 2 /s. Computationally and experimentally calculated energy barriers (0.81 and 0.83 eV respectively) only differ by 2.5%. Similarly, the pre-exponential diffusion coefficients only differ by 0.5 orders of magnitude. Moreover, the diffusivity of H i +1 in amorphous Al 2 O 3 in the 1000–2000 K range is calculated to be 2.53X10 -2 exp(-0.89 eV/k B /T), just one order of magnitude higher than the corresponding value in α-Al 2 O 3 . This suggests that local structural disorder does not significantly affect the energy landscape and diffusion behavior of H i +1 in Al 2 O 3 . Overall, these results show promise for the application of alumina polymorphs as hydrogen permeation barriers.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗
DOE OSTI2025

Multiple Slater Determinants and Strong Spin-Fluctuations as Key Ingredients of the Electronic Structure of Electron- and Hole-Doped Pb 10− x Cu x (PO 4 ) 6 O

LK-99, with chemical formula Pb 10−x Cu x (PO 4 ) 6 O, was recently reported to be a room-temperature superconductor. While this claim has met with little support in a flurry of ensuing work, a variety of calculations (mostly based on density-functional theory) have demonstrated that the system possesses some unusual characteristics in the electronic structure, in particular flat bands. We have established previously that within DFT, the system is insulating with many characteristics resembling the classic cuprates, provided the structure is not constrained to the P3(143) symmetry nominally assigned to it. Here we describe the basic electronic structure of LK-99 within self-consistent many-body perturbative approach, quasiparticle self-consistent GW (QSGW) approximation and their diagrammatic extensions. QSGW predicts that pristine LK-99 is indeed a Mott/charge transfer insulator, with a bandgap gap in excess of 3 eV, whether or not constrained to the P3(143) symmetry. When Pb 9 Cu(PO 4 ) 6 O is hole-doped, the valence bands modify only slightly, and a hole pocket appears. However, two solutions emerge: a high-moment solution with the Cu local moment aligned parallel to neighbors, and a low-moment solution with Cu aligned antiparallel to its environment. In the electron-doped case the conduction band structure changes significantly: states of mostly Pb character merge with the formerly dispersionless Cu d state, and high-spin and low spin solutions once again appear. Thus we conclude that with suitable doping, the ground state of the system is not adequately described by a band picture, and that strong correlations are likely. Irrespective of whether this system class hosts superconductivity or not, the transition of Pb 10 (PO 4 ) 6 O from being a band insulator to Pb 9 Cu(PO 4 ) 6 O, a Mott insulator, and multi-determinantal nature of doped Mott physics make this an extremely interesting case-study for strongly correlated many-body physics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗
NASA NTRS1994

Quiet-time intensifications along the poleward auroral boundary near midnight

Radar and optical measurements from Sondrestrom are combined with satellite and Goose Bay data in a study of the poleward edge of the nightside auroral oval during a quiet period. The B(sub y) and B(sub z) components of the interplanetary magnetic field were close to zero, and the B(sub x) component was approximately 8 nT for more than 24 hours. On a large scale, the convection and precipitation patterns remained almost constant during this period; on a small scale, however, the conditions were quite dynamic. At 10- to 20-min intervals the arc that marked the poleward auroral boundary intensified, and a new arc appeared poleward of it. About once per hour, stronger intensifications were observed. One such event is examined in detail. The auroral arcs first appeared to dim, and then they brightened, with a factor of 10 increase in E region electron density. At the time of the brightening a new arc formed poleward of all the arcs. The arcs then drifted southward at velocities of approximately 270 m/s. A plasma drift disturbance, characterized by a doubling of the southward velocity and a reversal in the east-west component, propagated westward at 900 m/s through the fields of view of the Sondrestrom and Goose Bay radars. A simultaneous satellite overpass close to the radars revealed the presence of an energetic ion event similar to the 'velocity dispersed ion structures' observed on the Aureol satellite and presumed to be the signature of fast ion beams within the plasma sheet boundary layer. The stronger arc intensification events observed by the Sondrestrom radar are associated with an increase in plasma flow across the boundary between open and closed magnetic field lines. We interpret this increased flow as the ionospheric signature of abrupt, localized increases in the reconnection rate in the midnight sector.

De La Beaujardiere, O.↗
DOE OSTI2022

Between Harmonic Crystal and Glass: Solids with Dimpled Potential-Energy Surfaces Having Multiple Local Energy Minima

Solids with dimpled potential-energy surfaces are ubiquitous in nature and, typically, exhibit structural (elastic or phonon) instabilities. Dimpled potentials are not harmonic; thus, the conventional quasiharmonic approximation at finite temperatures fails to describe anharmonic vibrations in such solids. At sufficiently high temperatures, their crystal structure is stabilized by entropy; in this phase, a diffraction pattern of a periodic crystal is combined with vibrational properties of a phonon glass. As temperature is lowered, the solid undergoes a symmetry-breaking transition and transforms into a lower-symmetry phase with lower lattice entropy. Here, we identify specific features in the potential-energy surface that lead to such polymorphic behavior; we establish reliable estimates for the relative energies and temperatures associated with the anharmonic vibrations and the solid–solid symmetry-breaking phase transitions. We show that computational phonon methods can be applied to address anharmonic vibrations in a polymorphic solid at fixed temperature. To illustrate the ubiquity of this class of materials, we present a range of examples (elemental metals, a shape-memory alloy, and a layered charge-density-wave system); we show that our theoretical predictions compare well with known experimental data.

36 MATERIALS SCIENCE↗
NASA NTRS1973

Photoelectrons and solar wind/lunar limb interaction.

It is suggested that boundary conditions for solar wind/lunar limb interactions are active. The 'whole-moon' limb does not evoke a shock cone, because warm (approximately equal 13 eV/electron) solar wind electrons are replaced by cool (less than or equal to 2 eV/electron) photoelectrons that are ejected from the generally smooth areas of the lunar terminator illuminated at glazing angles by the sun. A localized volume of low thermal pressure is created in the solar wind by these cool photoelectrons. The solar wind expands into this turbulence-suppressive volume without shock production. Conversely, directly illuminated highland areas exchange hot photoelectrons (greater than 20 eV/electron) for warm solar wind electrons. The hot electrons generate a localized pressure increase in the adjacent solar wind flow which evokes a shock streamer in the solar wind. Shock streamers are identifiable by a coincident increase in the magnitude of the solar wind magnetic field immediately external to the lunar wake. Shock occurrence is controlled by lunar topography, solar activity in the hard ultraviolet (greater than 20 eV), solar wind electron density and thermal velocity, and the intensity of the solar wind magnetic field.

Criswell, D. R.↗
NASA NTRS1992

SAGE II stratospheric density and temperature retrieval experiment

This paper describes a stratospheric density and temperature retrieval experiment based on the solar occultation measurement of the Stratospheric Aerosol and Gas Experiment (SAGE II). The entire retrieval analysis involves two inversion steps: the vertical structure inversion, which derives the profile of local atmospheric extinction from SAGE II limb optical depth data, and the species inversion, which inverts the concentration of air molecules, aerosols, ozone, and nitrogen dioxide from the derived atmospheric extinction at five SAGE II short wavelengths (0.385, 0.448, 0.453, 0.525, and 0.600 microns). The derived density profile is then used to infer the temperature distribution, assuming that the atmosphere is in hydrostatic equilibrium and obeys the ideal gas law. The temperature profiles retrieved from the SAGE II observations are compared with near-coincident, in both time and space, French Rayleigh lidar and NASA Wallops Flight Facility rocket datasonde soundings as well as the National Meteorological Center (NMC) data analyses. The results indicate that the mean SAGE II temperature agrees with the mean lidar measurements to within 2 C at altitudes from 30.5 to 52.5 km. The SAGE II and datasonde observations agree to within about 4 C in approximately the same altitude region.

Wang, Pi-Huan↗
DOE OSTI2026

Real-time observation of toroidal current redistributions induced by three-dimensional MHD phenomena triggering vertical displacement events in tokamak plasmas

Three-dimensional MHD instabilities, including edge-localized modes (ELMs) and internal reconnection events (IREs), have been observed to precipitate loss of vertical stability in tokamak plasmas, resulting in vertical displacement events (VDEs). This vertical destabilization can occur due to toroidal current redistributions and/or shape changes resulting from these phenomena. Using a recently introduced method for rapidly reconstructing the two-dimensional toroidal plasma current density profile in real-time, results are presented that demonstrate the specific current distribution changes that occur during ELMs (on KSTAR) and IREs (on MAST-U) that lead to loss of vertical control. The method most efficiently reconstructs the toroidal current density profile by doing so on a basis of principal components of historical profiles. These principal components isolate dominant current profile dynamics, improving interpretability, increasing speed, and reducing dimensionality of the profile computation. On KSTAR, this computation is executed in the real-time plasma control system at a rate of 10 kHz (limited by available CPU cycle times), allowing the current profile evolution to be assessed at several times over the course of each ELM event. Further, by incorporating the reconstructions into a novel vertical stability metric, the contribution of specific current profile dynamics to the loss of vertical stability can be assessed in real-time for VDE avoidance and improved understanding of the causal relationship between three-dimensional MHD phenomena and VDEs. The success of this method in approximating toroidal current density profiles from kinetic equilibrium reconstructions is also presented ($R^2=0.990$), along with its capability to produce other equilibrium quantities of interest in real-time at high time resolution.

edge-localized modes↗
DOE OSTI2020

Magnetic phase transitions in quantum spin-orbital liquids

Here, we investigate the spin and orbital correlations of a superexchange model with spin $\textit{S}$ = 1 and orbital $\textit{L}$ = 1 relevant for $5d^4$ transition-metal Mott insulators, using exact diagonalization and density matrix renormalization group (DMRG). For spin-orbit coupling λ = 0, the orbitals are in an entangled state that is decoupled from the spins. We find two phases with increasing λ: (I) the $\textit{S}$2 phase with two peaks in the structure factor for λ ≤ λ$_{c1}$ ≈ 0.34$\textit{J}$ where $\textit{J}$ is the ferromagnetic exchange; and, (II) the $\textit{S}$1 phase for λ$_{c1}$ < λ ≤ λ$_{c2}$ ≈ 1.2$\textit{J}$ with emergent antiferromagnetic correlations. Both $\textit{S}$1 and $\textit{S}$2 phases are shown to exhibit power-law correlations, indicative of a gapless spectrum. Upon increasing λ > λ$_{c2}$ leads to a product state of local spin-orbital singlets that exhibit exponential decay of correlations, indicative of a gapped phase. We obtain insights into the phases from the well-known Uimin-Lai-Sutherland model in an external field that provides an approximate description of our model within mean-field theory.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗
DOE OSTI2023

Probing the self-ionization of liquid water with ab initio deep potential molecular dynamics

The chemical equilibrium between self-ionized and molecular water dictates the acid–base chemistry in aqueous solutions, yet understanding the microscopic mechanisms of water self-ionization remains experimentally and computationally challenging. Herein, Density Functional Theory (DFT)–based deep neural network (DNN) potentials are combined with enhanced sampling techniques and a global acid–base collective variable to perform extensive atomistic simulations of water self-ionization for model systems of increasing size. The explicit inclusion of long-range electrostatic interactions in the DNN potential is found to be crucial to accurately reproduce the DFT free energy profile of solvated water ion pairs in small (64 and 128 H 2 O) cells. The reversible work to separate the hydroxide and hydronium to a distance S is found to converge for simulation cells containing more than 500 H 2 O, and a distance of ∼ 8 Å is the threshold beyond which the work to further separate the two ions becomes approximately zero. The slow convergence of the potential of mean force with system size is related to a restructuring of water and an increase of the local order around the water ions. Calculation of the dissociation equilibrium constant illustrates the key role of long-range electrostatics and entropic effects in the water autoionization process.

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

Magnon damping and mode softening in quantum double-exchange ferromagnets

We present a comprehensive analysis of the magnetic excitations and electronic properties of fully quantum double-exchange ferromagnets, i.e. systems where ferromagnetic (FM) ordering emerges from the competition between spin, charge, and orbital degrees of freedom, but without the canonical approximation of using classical localized spins. Specifically, we investigate spin excitations within the Kondo lattice-like model, as well as a two-orbital Hubbard Hamiltonian in proximity to the orbital-selective Mott phase. Computational analysis of the magnon dispersion, damping, and spectral weight within these models reveals unexpected phenomena, such as magnon mode softening and the anomalous decoherence of magnetic excitations as observed in earlier experimental efforts, but explained here without the use of the phononic degrees of freedom. We show that these effects are intrinsically linked to incoherent spectral features near the Fermi level, which arise due to the quantum nature of the local (on-site) triplets. This incoherent spectrum leads to a Stoner-like continuum on which spin excitations scatter, governing magnon lifetime and strongly influencing the dynamical spin structure factor. Our study explores the transition from coherent to incoherent magnon spectra by varying the electron density. Furthermore, we demonstrate that the magnitude of the localized spin mitigates decoherence by suppressing the incoherent spectral contributions near the Fermi level. We also discuss the effective J 1 –J 2 spin Hamiltonian, which can accurately describe the large doping region characterized by the magnon-mode softening. Finally, we show that this behavior is also present in multiorbital models with partially filled orbitals, namely, in systems without localized spin moments, provided that the model is in a strong coupling regime. Our results potentially have far-reaching implications for understanding FM ordering in various multi-band systems. These findings establish a previously unknown direct connection between the electronic correlations of those materials and spin excitations.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗