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At least 973 records · Page 54

Constraining nucleation, condensation, and chemistry in oxidation flow reactors using size-distribution measurements and aerosol microphysical modeling

Oxidation flow reactors (OFRs) allow the concentration of a given atmospheric oxidant to be increased beyond ambient levels in order to study secondary organic aerosol (SOA) formation and aging over varying periods of equivalent aging by that oxidant. Previous studies have used these reactors to determine the bulk OA mass and chemical evolution. To our knowledge, no OFR study has focused on the interpretation of the evolving aerosol size distributions. In this study, we use size-distribution measurements of the OFR and an aerosol microphysics model to learn about size-dependent processes in the OFR. Specifically, we use OFR exposures between 0.09 and 0.9 equivalent days of OH aging from the 2011 BEACHON-RoMBAS and GoAmazon2014/5 field campaigns. We use simulations in the TOMAS (TwO-Moment Aerosol Sectional) microphysics box model to constrain the following parameters in the OFR: (1) the rate constant of gas-phase functionalization reactions of organic compounds with OH, (2) the rate constant of gas-phase fragmentation reactions of organic compounds with OH, (3) the reactive uptake coefficient for heterogeneous fragmentation reactions with OH, (4) the nucleation rate constants for three different nucleation schemes, and (5) an effective accommodation coefficient that accounts for possible particle diffusion limitations of particles larger than 60 nm in diameter. We find the best model-to-measurement agreement when the accommodation coefficient of the larger particles ( D p > 60 nm) was 0.1 or lower (with an accommodation coefficient of 1 for smaller particles), which suggests a diffusion limitation in the larger particles. When using these low accommodation-coefficient values, the model agrees with measurements when using a published H 2 SO 4 -organics nucleation mechanism and previously published values of rate constants for gas-phase oxidation reactions. Further, gas-phase fragmentation was found to have a significant impact upon the size distribution, and including fragmentation was necessary for accurately simulating the distributions in the OFR. The model was insensitive to the value of the reactive uptake coefficient on these aging timescales. Monoterpenes and isoprene could explain 24 %–95 % of the observed change in total volume of aerosol in the OFR, with ambient semivolatile and intermediate-volatility organic compounds (S/IVOCs) appearing to explain the remainder of the change in total volume. These results provide support to the mass-based findings of previous OFR studies, give insight to important size-distribution dynamics in the OFR, and enable the design of future OFR studies focused on new particle formation and/or microphysical processes.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Evolution of primoridal gas clouds

The dynamical, chemical, and thermal evolution of zero-metal gas clouds was modeled to study conditions of star formation in the early universe. Numerical results are given for the collapse of spherical clouds of mass 1000 and 50000 solar mass. Cooling by H2 lines and by photons emitted in H + e(-) yields H(-) = h (sup nu) maintains collapse until formation of an equilibrium protostellar core of mass 0.02 solar mass. The cooling by photons produced with H is essential for low mass star formation. If the cloud is fragmented, the evolution of the pieces is similar to that of the parent cloud, but the equilibrium core has larger density and mass.

Bodenheimer, P. H.↗

Pulsed acceleration in solar flares

We study the nonlinear dynamics of particle acceleration in solar flares by analyzing the time series of various quasi-periodic radio signatures during flares. In particular we present the radio and hard X-ray data of three flares which suppport the following tentative conclusions: (1) Particle acceleration and injection into magnetic structures occurs intrinsically in a pulsed mode (with a typical period of 1-2 s), produced by a single, spatially coherent, nonlinear system, rather than by a stochastic system with many spatially independent components ('statistical flare' produced by a fragmented primary energy release). (2) The nonlinear (quasi-periodic) mode of pulsed particle acceleration and injection into a coronal loop can be stabilized by phase locking with an MHD wave (oscillation) mode, if both periods are close to each other. (3) Pulsed injection of electron beams into a coronal loop may trigger nonlinear relaxational oscillations of wave-particle interactions. This is particularly likely when the limit cycles of both systems are similar.

Aschwanden, Markus J.↗

Cosmic-Ray-Exposure Ages of Diogenites and the Collisional History of the HED Parent Body or Bodies

Cosmic-ray-exposure ages of meteorites provide information on the collisional history of their parent bodies and the delivery mechanism of meteorites to Earth. The exposure-age distributions of ordinary chondrites show distinct patterns for H, L, and LL types, consistent with their origin on different parent bodies. The exposure-age distributions of howardites, eucrites. and diogenites (HEDS) show a common pattern with major peaks at 22 Ma and 38 Ma This provides additional evidence for a common origin of the HED meteorites, possibly 4 Vesta, although orbital dynamics calculations showed that the delivery of meteorites from Vesta to Earth is difficult. However, the discovery of several kilometer-sized Vesta-like asteroids in the region between Vesta and the 3:1 resonance suggested that these seem more likely parent bodies of the HEDs than Vesta itself. This implies that the exposure-age clusters may represent samples of several parent bodies. Therefore, the near-absence of diogenites with ages <20 Ma might be of interest for the composition of these kilometer-sized fragments of Vesta. Here we present cosmic-ray-exposure ages of 20 diogenites, including 9 new meteorites. In addition, we calculate the probability for each peak to occur by chance, assuming a constant production rate of HED fragments.

Welten, K. C.↗

Dissecting the structural heterogeneity of proteins by native mass spectrometry

Abstract A single gene yields many forms of proteins via combinations of posttranscriptional/posttranslational modifications. Proteins also fold into higher‐order structures and interact with other molecules. The combined molecular diversity leads to the heterogeneity of proteins that manifests as distinct phenotypes. Structural biology has generated vast amounts of data, effectively enabling accurate structural prediction by computational methods. However, structures are often obtained heterologously under homogeneous states in vitro. The lack of native heterogeneity under cellular context creates challenges in precisely connecting the structural data to phenotypes. Mass spectrometry (MS) based proteomics methods can profile proteome composition of complex biological samples. Most MS methods follow the “bottom‐up” approach, which denatures and digests proteins into short peptide fragments for ease of detection. Coupled with chemical biology approaches, higher‐order structures can be probed via incorporation of covalent labels on native proteins that are maintained at the peptide level. Alternatively, native MS follows the “top‐down” approach and directly analyzes intact proteins under nondenaturing conditions. Various tandem MS activation methods can dissect the intact proteins for in‐depth structural elucidation. Herein, we review recent native MS applications for characterizing heterogeneous samples, including proteins binding to mixtures of ligands, homo/hetero‐complexes with varying stoichiometry, intrinsically disordered proteins with dynamic conformations, glycoprotein complexes with mixed modification states, and active membrane protein complexes in near‐native membrane environments. We summarize the benefits, challenges, and ongoing developments in native MS, with the hope to demonstrate an emerging technology that complements other tools by filling the knowledge gaps in understanding the molecular heterogeneity of proteins.

59 BASIC BIOLOGICAL SCIENCES↗

Intelligent Experiments through Real-Time AI: Fast Data Processing and Autonomous Detector Control for High-Energy Nuclear Experiments

The aim of this project is to develop software and hardware for fast real-time data processing and autonomous detector control and calibration for the sPHENIX and the future EIC experiments. Below summarizes Georgia Tech team efforts in the past year: 1. We developed a real-time clustering algorithm and FPGA-based pipeline architecture for processing fired pixel data from ALPIDE sensors in sPHENIX experiments. Our Columnar Clustering Co-Design introduces a hardware-aware, stream-friendly approach that segments pixel data by column pairs using a Column Pair Clustering (CPC) strategy, followed by Cluster Stitching to merge adjacent subclusters. Implemented in Vitis HLS, the pipeline comprises five stages—read-in, subclustering, stitching, analysis, and write-out—connected by tagged HLS streams with custom end-of-event signaling for robust synchronization. We designed a pipelined dataflow model optimized for throughput, low latency, and minimal buffering, enabling scalable clustering across events of arbitrary size. Our system maintains spatial precision via center-of-mass and shape key extraction and efficiently handles edge cases such as fragmented or nested clusters. Compared against DBSCAN in both software and hardware, our approach demonstrates competitive performance under FPGA constraints. 2. We also conducted a comprehensive algorithm-to-hardware co-design of connected component analysis tailored for sPHENIX experiments, focusing on real-time, low-latency processing using FPGAs and High-Level Synthesis (HLS). Starting from a Python-based particle tracking pipeline, the team translated the core logic—graph traversal via DFS and Union-Find—into an HLS-compatible C++ model, replacing dynamic memory and recursion with static arrays and pipelined control flow. The final design includes a fully streamed and dataflow-compatible Union-Find kernel optimized across five iterations, incorporating loop pipelining, array partitioning, AXI/FIFO interface tuning, and function flattening. Experimental results show up to 14.8× speedup over the CPU baseline, reducing per-graph latency to 1.58 μs and demonstrating strong resource efficiency with only ~7k LUTs and zero BRAM usage. The design maintains functional correctness against the Python reference using a Python-based C-simulation framework and Mean Squared Error metrics. This work validates the potential of HLS-driven FPGA designs for edge-level HEP data acquisition, laying a scalable foundation for future integration with real-time detector pipelines and multi-graph processing systems.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Communication: On the competition between adiabatic and nonadiabatic dynamics in vibrationally mediated ammonia photodissociation in its A band

Non-adiabatic processes play an important role in photochemistry, but the mechanism for conversion of electronic energy to chemical energy is still poorly understood. To explore the possibility of vibrational control of non-adiabatic dynamics in a prototypical photoreaction, namely, the A-band photodissociation of NH{sub 3}(X{sup ~1}A{sub 1}), full-dimensional state-to-state quantum dynamics of symmetric or antisymmetric stretch excited NH{sub 3}(X{sup ~1}A{sub 1}) is investigated on recently developed coupled diabatic potential energy surfaces. The experimentally observed H atom kinetic energy distributions are reproduced. However, contrary to previous inferences, the NH{sub 2}(A{sup ~2}A{sub 1})/NH{sub 2}(X{sup ~2}B{sub 1}) branching ratio is found to be small regardless of the initial preparation of NH{sub 3}(X{sup ~1}A{sub 1}), while the internal state distribution of the preeminent fragment, NH{sub 2}(X{sup ~2}B{sub 1}), is found to depend strongly on the initial vibrational excitation of NH{sub 3}(X{sup ~1}A{sub 1}). The slow H atoms in photodissociation mediated by the antisymmetric stretch fundamental state are due to energy sequestered in the internally excited NH{sub 2}(X{sup ~2}B{sub 1}) fragment, rather than in NH{sub 2}(A{sup ~2}A{sub 1}) as previously proposed. The high internal excitation of the NH{sub 2}(X{sup ~2}B{sub 1}) fragment is attributed to the torques exerted on the molecule as it passes through the conical intersection seam to the ground electronic state of NH{sub 3}. Thus in this system, contrary to previous assertions, the control of electronic state branching by selective excitation of ground state vibrational modes is concluded to be ineffective. The juxtaposition of precise quantum mechanical results with complementary results based on quasi-classical surface hopping trajectories provides significant insights into the non-adiabatic process.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

QLBT: a linear Boltzmann transport model for heavy quarks in a quark-gluon plasma of quasi-particles

Abstract We develop a new heavy quark transport model, QLBT, to simulate the dynamical propagation of heavy quarks inside the quark-gluon plasma (QGP) created in relativistic heavy-ion collisions. Our QLBT model is based on the linear Boltzmann transport (LBT) model with the ideal QGP replaced by a collection of quasi-particles to account for the non-perturbative interactions among quarks and gluons of the hot QGP. The thermal masses of quasi-particles are fitted to the equation of state from lattice QCD simulations using the Bayesian statistical analysis method. Combining QLBT with our advanced hybrid fragmentation-coalescence hadronization approach, we calculate the nuclear modification factor $$R_\mathrm {AA}$$ R AA and the elliptic flow $$v_2$$ v 2 of D mesons at the Relativistic Heavy-Ion Collider and the Large Hadron Collider. By comparing our QLBT calculation to the experimental data on the D meson $$R_\mathrm {AA}$$ R AA and $$v_2$$ v 2 , we extract the heavy quark transport parameter $$\hat{q}$$ q ^ and diffusion coefficient $$D_\mathrm {s}$$ D s in the temperature range of $$1-4~T_\mathrm {c}$$ 1 - 4 T c , and compare them with the lattice QCD results and other phenomenological studies.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Meso-scale modeling of UO2 nuclear fuel to high burnup

To improve the economics of light water reactors for commercial nuclear energy generation, utility operators are seeking to obtain regulatory approval to run UO2 fuel to higher levels of burnup. One potential impediment to obtaining this approval is the phenomenon of fuel fragmentation, relocation, and dispersal (FFRD). FFRD can result when fuel experiences a rapid temperature transient, such as that occurring during a Loss Of Coolant Accident (LOCA). FFRD has historically been most associated with the rim region in UO2 fuel pellets, where the phenomenon of fragmentation is also referred to as pulverization due to the small size of the fragments. More recent evidence suggests that the so-called “dark zone” (due to its appearance in micrographs) that can be observed in the mid-radial regions of high burnup fuel is also susceptible to FFRD. Although empirical fuel performance models have been developed that can adequately predict pulverization in the rim region under typical LWR conditions, a scientific understanding of what underlies fuel restructuring and subsequent FFRD is lacking even in the rim region, and no models are currently available for the behavior the dark zone. To address these challenges, the U.S. Department of Energy’s Nuclear Energy Advanced Modeling and Simulation (NEAMS) program has employed a multi-scale modeling approach to improve scientific understanding and develop new fuel performance models. In this talk, I will focus on meso-scale efforts, which form a crucial link between atomic-scale and engineering-scale models. Phase-field modeling combined with cluster dynamics is used to predict the restructuring process in the rim region. Phase-field fracture modeling, informed by atomistic simulations, is used to predict the onset of pulverization in the rim region. Combining these techniques together allows the extent of rim pulverization to be predicted. The formation and evolution of the dark zone has also been simulated with the phase-field method, using an improved approach to vacancy source term parameterization. The work shows the important impact of microstructure on fuel performance.

fracture↗

High-speed (20 kHz) digital in-line holography for transient particle tracking and sizing in multiphase flows

High-speed (20 kHz) digital in-line holography (DIH) is applied for 3D quantification of the size and velocity of fragments formed from the impact of a single water drop onto a thin film of water and burning aluminum particles from the combustion of a solid rocket propellant. To address the depth-of-focus problem in DIH, a regression-based multiframe tracking algorithm is employed, and out-of-plane experimental displacement accuracy is shown to be improved by an order-of-magnitude. Comparison of the results with previous DIH measurements using low-speed recording shows improved positional accuracy with the added advantage of detailed resolution of transient dynamics from single experimental realizations. Furthermore, the method is shown to be particularly advantageous for quantification of particle mass flow rates. For the investigated particle fields, the mass flows rates, which have been automatically measured from single experimental realizations, are found to be within 8% of the expected values.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Measurement of isolated-photon plus two-jet production in p p collisions at s = 13 TeV with the ATLAS detector

The dynamics of isolated-photon plus two-jet production in pp collisions at a centre-of-mass energy of 13 TeV are studied with the ATLAS detector at the LHC using a dataset corresponding to an integrated luminosity of 36.1 fb−1. Cross sections are measured as functions of a variety of observables, including angular correlations and invariant masses of the objects in the final state, γ+jet+jet. Measurements are also performed in phase-space regions enriched in each of the two underlying physical mechanisms, namely direct and fragmentation processes. The measurements cover the range of photon (jet) transverse momenta from 150 GeV (100 GeV) to 2 TeV. The tree-level plus parton-shower predictions from SHERPA and PYTHIA as well as the next-to-leading-order QCD predictions from SHERPA are compared with the measurements. The next-to-leading-order QCD predictions describe the data adequately in shape and normalisation except for regions of phase space such as those with high values of the invariant mass or rapidity separation of the two jets, where the predictions overestimate the data.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Photofragmentation of Tetranitromethane: Spin-Unrestricted Time-Dependent Excited-State Molecular Dynamics

In this study, the photofragmentation dynamics of tetranitromethane (TNM) is explored by a spin-unrestricted time-dependent excited-state molecular dynamics (u-TDESMD) algorithm based on Rabi oscillations and principles similar to trajectory surface hopping, with a midintensity field approximation. The leading order process is represented by the molecule undergoing cyclic excitations and de-excitations. During excitation cycles, the nuclear kinetic energy is accumulated to overcome the dissociation barriers in the reactant and a sequence of intermediates. The dissociation pathway includes the ejection of NO 2 groups followed by the formation of NO and CO. The simulated mass spectra at the ab initio level, based on the bond length in possible fragments, are extracted from simulation trajectories. Finally, the recently developed methodology has the potential to model and monitor photoreactions with open-shell intermediates and radicals.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Dynamics in the quantum/classical limit based on selective use of the quantum potential

A classical limit of quantum dynamics can be defined by compensation of the quantum potential in the time-dependent Schrödinger equation. The quantum potential is a non-local quantity, defined in the trajectory-based form of the Schrödinger equation, due to Madelung, de Broglie, and Bohm, which formally generates the quantum-mechanical features in dynamics. Selective inclusion of the quantum potential for the degrees of freedom deemed “quantum,” defines a hybrid quantum/classical dynamics, appropriate for molecular systems comprised of light and heavy nuclei. The wavefunction is associated with all of the nuclei, and the Ehrenfest, or mean-field, averaging of the force acting on the classical degrees of freedom, typical of the mixed quantum/classical methods, is avoided. The hybrid approach is used to examine evolution of light/heavy systems in the harmonic and double-well potentials, using conventional grid-based and approximate quantum-trajectory time propagation. The approximate quantum force is defined on spatial domains, which removes unphysical coupling of the wavefunction fragments corresponding to distinct classical channels or configurations. The quantum potential, associated with the quantum particle, generates forces acting on both quantum and classical particles to describe the backreaction.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Orbital Deflection of Comets by Directed Energy

Cometary impacts pose a long-term hazard to life on Earth. Impact mitigation techniques have been studied extensively, but they tend to focus on asteroid diversion. Typical asteroid interdiction schemes involve spacecraft physically intercepting the target, a task feasible only for targets identified decades in advance and in a narrow range of orbits—criteria unlikely to be satisfied by a threatening comet. Comets, however, are naturally perturbed from purely gravitational trajectories via solar heating of their surfaces, which activates sublimation-driven jets. Artificial heating of a comet, such as by a laser, may supplement natural heating by the Sun to purposefully manipulate its path and thereby avoid an impact. Deflection effectiveness depends on the comet’s heating response, which varies dramatically depending on factors including nucleus size, orbit, and dynamical history. These factors are incorporated into a numerical orbital model to assess the effectiveness and feasibility of using high-powered laser arrays in Earth orbit and on the ground for comet deflection. Simulation results suggest that a diffraction-limited 500 m orbital or terrestrial laser array operating at 10 GW for 1% of each day over 1 yr is sufficient to fully avert the impact of a typical 500 m diameter comet with primary nongravitational parameter A {sub 1} = 2 × 10{sup −8} au day{sup −2}. Strategies to avoid comet fragmentation during deflection are also discussed.

79 ASTRONOMY AND ASTROPHYSICS↗

Effect of Heat Treatment and Combination of Cold Rolling and Heat Treatment on Microstructure and Mechanical Properties of Titanium Alloy Ti6Al2V2Zr1.5Mo

The heat treatment and cold rolling combinations have been carried out on titanium alloy Ti6Al2V2Zr1.5Mo, and microstructure evolution and mechanical behavior have been studied. Solution treatment below the β-transus temperature, followed by air cooling, resulted in higher microhardness/strength as compared to the same with water quenching. A sudden drop in microhardness/strength is observed in sample solution heat-treated above β-transus temperature followed by air cooling. The former is attributed to the additional presence of fine secondary α-phase formed by dynamic aging during air cooling as compared to water-quenched samples which did not have fine secondary α-phase. Solution treatment above β-transus temperature resulted in Widmanstatten microstructure with no significant fine secondary α in air-cooled samples. Among the studied conditions of cold rolling (CR), gain in strength of the alloy from annealed condition is significant with first 15% reduction and thereafter it is marginal for 30% reduction. Initiation of cracks at the edges has been observed in 30% CR. The microstructure of cold-rolled samples confirms the fragmentation of α-plates with the presence of high dislocation density. Heat treatment of cold-rolled samples resulted in significant reduction in strength from the as-cold-rolled conditions. The marginally lower strength than the as-received (annealed) or heat-treated alloy samples is due to the recrystallization in CR samples and the formation of Widmanstatten microstructure in air-cooled samples. The alloy does not have fine secondary α or regions with large dislocation density in this condition. The microstructure in the samples heat-treated (with air cooling) below as well as above β-transus temperature (after CR) is similar to air-cooled samples (without prior CR) with heat treatment above β-transus temperature. This indicates the reduction in recrystallization temperature with cold working, which is substantiated with the reduction in strength as well.

36 MATERIALS SCIENCE↗

Origin of Stabilization of Ligand-Centered Mixed Valence Ruthenium Azopyridine Complexes: DFT Insights for Neuromorphic Applications

Redox-driven conductance changes are critical processes in molecular- and coordination-complex-based memristive thin films and devices that are envisioned for neuromorphic technologies, but fundamental mechanisms of conductance switching are not fully understood. Here, we explore charge disproportionation (CD) processes in [Ru II L 2 ](PF 6 ) 2 molecular systems that intrinsically involve interfragment charge transfer (IFCT). Using a combination of ab initio molecular dynamics simulation (AIMD), time-dependent density functional theory (TD-DFT), and density functional theory (DFT) calculations, we investigate the electron transfer mechanisms and the roles of temperature and cell volumetric expansion in facilitating the counterion movements and electronic transitions required for low-cost IFCT and charge redistribution. A detailed analysis of the density of states and TD-DFT calculations highlights that unpaired electrons play a crucial role in low-energy transitions, with the azo (N=N) groups of the ligand serving as the primary sites for electronic transport between molecular fragments, further stabilizing the asymmetric state. Localization of added electrons on azo ligands occurs with negligible change at the Ru centers, supported by atomic volume expansions up to +4.74 bohr 3 , and goes along with a progressive reduction of the HOMO−LUMO gap across redox states, suggesting enhanced conductivity. The TD-DFT analysis reveals a dominant IFCT excitation at 2082.76 nm in the doubly reduced (22) state, while a stabilization energy of 1.20 eV of the asymmetric (13) state relative to the symmetric (22) state is predicted by constrained DFT. Periodic DFT and AIMD simulations emulating a molecular film show that the stabilization of the asymmetric state, relative to a symmetric one, translates in net charge separation values (order of ∼0.33 e) that are strongly linked to increased counterion mobility (average counterion displacements exceeding 0.7 Å per atom during CD events) and the involvement of azo groups in electron redistribution. These findings, which align with previously reported experimental and computational data, provide key insights into the IFCT mechanisms and electronic transport facilitated by azo groups, with important implications for redox-driven memristive and neuromorphic technologies.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Reconstruction of neutral-triggered charged recoil jets in √ s = 200 GeV p+p collisions at the STAR experiment

Jets — collimated sprays of hadrons — are produced by hard-scattered partons during the early stages of heavy ion collisions. Hence, they provide a valuable probe of the complex multi-particle dynamics within the hot, dense medium produced in such collisions. In particular, the study of jets recoiling from direct photons (γ dir +jet) and those recoiling from energetic π 0 (π 0 +jet) may shed light on the path-length and initial flavor (quark vs. gluon) dependence of the energy-loss experienced by a parton as it traverses the medium. We present here measurements of the yields of charged recoil jets tagged by γ dir and π 0 in p+p collisions at √S = 200 GeV. These measurements will serve as a vacuum fragmentation reference for an upcoming measurement in Au + Au collisions.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗