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At least 1,009 records · Page 56

Structure and properties of densified silica glass: characterizing the order within disorder

The broken symmetry in the atomic-scale ordering of glassy versus crystalline solids leads to a daunting challenge to provide suitable metrics for describing the order within disorder, especially on length scales beyond the nearest neighbor that are characterized by rich structural complexity. Here, we address this challenge for silica, a canonical network-forming glass, by using hot versus cold compression to (i) systematically increase the structural ordering after densification and (ii) prepare two glasses with the same high-density but contrasting structures. The structure was measured by high-energy X-ray and neutron diffraction, and atomistic models were generated that reproduce the experimental results. The vibrational and thermodynamic properties of the glasses were probed by using inelastic neutron scattering and calorimetry, respectively. Traditional measures of amorphous structures show relatively subtle changes upon compacting the glass. The method of persistent homology identifies, however, distinct features in the network topology that change as the initially open structure of the glass is collapsed. The results for the same high-density glasses show that the nature of structural disorder does impact the heat capacity and boson peak in the low-frequency dynamical spectra. Densification is discussed in terms of the loss of locally favored tetrahedral structures comprising oxygen-decorated SiSi 4<:sub> tetrahedra.

36 MATERIALS SCIENCE↗

Assignment of Freight Traffic in a Large-scale Intermodal Network under Uncertainty

This paper presents a methodology for freight traffic assignment in a large-scale road-rail intermodal network under uncertainty. Network uncertainties caused by natural disasters have dramatically increased in recent years. Several of these disasters (e.g., Hurricane Sandy, Mississippi River Flooding, and Hurricane Harvey) severely disrupted the U.S. freight transportation network, and consequently, the supply chain. To account for these network uncertainties, a stochastic freight traffic assignment model is formulated. An algorithmic framework, involving the sample average approximation and gradient projection algorithm, is proposed to solve this challenging problem. The developed methodology is tested on the U.S. intermodal network with freight flow data from the Freight Analysis Framework. The experiments consider three types of natural disasters that have different risks and impacts on transportation networks: earthquakes, hurricanes, and floods. It is found that for all disaster scenarios, freight ton-miles are higher compared to the base case without uncertainty. The increase in freight ton-miles is the highest under the flooding scenario; this is because there are more states in the flood-risk areas, and they are scattered throughout the U.S.

42 ENGINEERING↗

High energy-resolution studies of electron impact optical excitation functions. I - The second positive system of N2.

The relative emission cross section for the N2 second positive system (0,0) and (1,0) bands excited by electron impact was measured for incident electron energies from threshold to 17 eV. The use of a high energy-resolution electron spectrometer coupled to an optical detection system made it possible to obtain the measurements with an incident electron beam having an energy half width of 50 meV. Calibration of the incident electron energy was provided by observing the scattering resonances in nitrogen and helium. The maximum of the (0,0) and (1,0) bands were found to be at approximately 14.02 and 14.3 eV, respectively. A small structural feature that was pressure-independent appeared only in the (0,0) band emission cross section. Another such feature was pressure-dependent and appeared more strongly in the (1,0) band cross section.

Finn, T. G.↗

Coastal Zone Color Scanner atmospheric correction algorithm - Multiple scattering effects

Errors due to multiple scattering which are expected to be encountered in application of the current Coastal Zone Color Scanner (CZCS) atmospheric correction algorithm are analyzed. The analysis is based on radiative transfer computations in model atmospheres, in which the aerosols and molecules are distributed vertically in an exponential manner, with most of the aerosol scattering located below the molecular scattering. A unique feature of the analysis is that it is carried out in scan coordinates rather than typical earth-sun coordinates, making it possible to determine the errors along typical CZCS scan lines. Information provided by the analysis makes it possible to judge the efficacy of the current algorithm with the current sensor and to estimate the impact of the algorithm-induced errors on a variety of applications.

Gordon, Howard R.↗

Phytoplankton and Climate

Ocean phytoplankton supply about half of the oxygen that humans utilize to sustain life. In this lecture, we will explore how phytoplankton plays a critical role in modulating the Earth's climate. These tiny organisms are the base of the Ocean's food web. They can modulate the rate at which solar heat is absorbed by the ocean, either through direct absorption or through production of highly scattering cellular coverings. They take up and help sequester carbon dioxide, a key greenhouse gas that modulated the Earth's climate. They are the source of cloud nucleation gases that are key to cloud formation/processes. They are also able to modify the nutrient budgets of the ocean through active uptake of inert atmospheric nitrogen. Climate variations have a pronounced impact on phytoplankton dynamics. Long term variations in the climate have been studied through geological interpretations on its influence on phytoplankton populations. The presentation will focus on presenting the numerous linkages that have been observed between climate and phytoplankton and further discuss how present climate change scenarios are likely to impact phytoplankton populations as well as present findings from several studies that have tried to understand how the climate might react to the feedbacks from these numerous climate-phytop|ankton linkages.

Moisan, John R.↗

Profiling Transboundary Aerosols over Taiwan and Assessing Their Radiative Effects

A synergistic process was developed to study the vertical distributions of aerosol optical properties and their effects on solar heating using data retrieved from ground-based radiation measurements and radiative transfer simulations. Continuous MPLNET and AERONET observations were made at a rural site in northern Taiwan from 2005 to 2007. The aerosol vertical extinction profiles retrieved from ground-based lidar measurements were categorized into near-surface, mixed, and two-layer transport types, representing 76% of all cases. Fine-mode (Angstrom exponent, alpha, approx.1.4) and moderate-absorbing aerosols (columnar single-scattering albedo approx.0.93, asymmetry factor approx.0.73 at 440 nm wavelength) dominated in this region. The column-integrated aerosol optical thickness at 500 nm (tau(sub 500nm)) ranges from 0.1 to 0.6 for the near-surface transport type, but can be doubled in the presence of upper-layer aerosol transport. We utilize aerosol radiative efficiency (ARE; the impact on solar radiation per unit change of tau(sub 500nm)) to quantify the radiative effects due to different vertical distributions of aerosols. Our results show that the ARE at the top-of-atmosphere (-23 W/ sq m) is weakly sensitive to aerosol vertical distributions confined in the lower troposphere. On the other hand, values of the ARE at the surface are -44.3, -40.6 and -39.7 W/sq m 38 for near-surface, mixed, and two-layer transport types, respectively. Further analyses show that the impact of aerosols on the vertical profile of solar heating is larger for the near-surface transport type than that of two-layer transport type. The impacts of aerosol on the surface radiation and the solar heating profiles have implications for the stability and convection in the lower troposphere.

Wang, Sheng-Hsiang↗

Investigating the Aerosol Optical and Radiative Characteristics of Heavy Haze Episodes in Beijing During January of 2013

Several heavy atmospheric haze pollution episodes occurred over eastern and northern China during January of 2013. The pollution covered more than 100 sq km and caused serious impacts on environmental quality, human health, and transportation. In this study, we characterize aerosol microphysical, optical, and radiative characteristics using a combination of ground-based Sun/sky radiometer retrievals and a radiative transfer model. Our results show that during about half of the total number of days, daily PM2.5 and PM10 concentrations are larger than 100 microg/cu m, with maxima of 462 and 433 microg/cu m, respectively, during the haze events. Fine-mode (PM2.5) particles dominated the aerosol size during the episodes. The volume size distribution and median radius of fine-mode particles generally increase as aerosol optical depth at 440 nm (AOD440) increases. The median effective radius of fine-mode particles increases from 0.15 microns at low AOD value (AOD440~0.3) to a radius of 0.25-0.30 microns at high AOD value (AOD440> or = 1.0). The daily mean single-scattering albedo (SSA), imaginary part of refractive index (RI), and asymmetry factor display pronounced spectral behaviors. The overall mean SSA440 and SSA675 are 0.892 and 0.905, respectively. The corresponding RI440 and RI675 are 0.016 and 0.011, respectively. This indicates that a significant amount of absorption occurred under the haze event in Beijing during January 2013. Approximately half of the incident solar radiation energy went into heating the atmosphere as a result of strong aerosol loading and absorption. The daily averaged heating rate in the haze particle layer (0-3.2 km) varies from 0.12 to 0.81 K/day in Beijing, which might exert profound impact on the atmospheric thermodynamic and dynamical structures and cloud development, which should be further studied.

bejing↗

Aerosol-Water Cycle Interaction: A New Challenge in Monsoon Climate Research

Long recognized as a major environmental hazard, aerosol is now known to have strong impacts on both regional and global climate. It has been estimated that aerosol may reduce by up to 10% of the seasonal mean solar radiation reaching the earth surface, producing a global cooling effect that opposes global warming (Climate Change 2001). This means that the potential perils that humans have committed to global warming may be far greater than what we can detect at the present. As a key component of the Earth climate system, the water cycle is profoundly affected by the presence of aerosols in the atmosphere. Through the so-called direct effect , aerosol scatters and/or absorbs solar radiation, thus cooling the earth surface and changing the horizontal and vertical radiational heating contrast in the atmosphere. The heating contrast drives anomalous atmospheric circulation, resulting in changes in convection, clouds, and rainfall. Another way aerosol can affect the water cycle is through the so-called indirect effects, whereby aerosol increases the number of cloud condensation nuclei, prolongs life time of clouds, and inhibits the growth of cloud drops to raindrops. This leads to more clouds, and increased reflection of solar radiation, and further cooling at the earth surface. In monsoon regions, the response of the water cycle to aerosol forcing is especially complex, not only because of presence of diverse mix of aerosol species with vastly different radiative properties, but also because the monsoon is strongly influenced by ocean and land surface processes, land use, land change, as well as regional and global greenhouse warming effects. Thus, sorting out the impacts of aerosol forcing, and interaction with the monsoon water cycle is a very challenging problem. In this talk, I will offer some insights into how aerosols may impact the Asian monsoon based on preliminary results from satellite observations and climate model experiments. Specifically, I will discuss the elevated heat pump hypothesis, involving atmospheric heating by absorbing aerosols (dust and black carbon) over the southern slopes of the Himalayas, and feedback with the deep convection, in modifying monsoon water cycle over South .and East Asia. The role of aerosol forcing relative to those due to sea surface temperature and land surface processes, as well as observation requirements to verify such a hypothesis will also be discussed.

Lau, William K. M.↗

Aerosol-Water Cycle Interaction: A New Challenge in Monsoon Climate Research

Long recognized as a major environmental hazard, aerosol is now known to have strong impacts on both regional and global climate. It has been estimated that aerosol may reduce by up to 10% of the seasonal mean solar radiation reaching the earth surface, producing a global cooling effect that opposes global warming (Climate Change 2001). This means that the potential perils that humans have committed to global warming may be far greater than what we can detect at the present. As a key component of the Earth climate system, the water cycle is profoundly affected by the presence of aerosols in the atmosphere. Through the so-called "direct effect", aerosol scatters and/or absorbs solar radiation, thus cooling the earth surface and changing the horizontal and vertical radiational heating contrast in the atmosphere. The heating contrast drives anomalous atmospheric circulation, resulting in changes in convection, clouds, and rainfall. Another way aerosol can affect the water cycle is through the so-called "indirect effects", whereby aerosol increases the number of cloud condensation nuclei, prolongs life time of clouds, and inhibits the growth of cloud drops to raindrops. This leads to more clouds, and increased reflection of solar radiation, and further cooling at the earth surface. In monsoon regions, the response of the water cycle to aerosol forcing is especially complex, not only because of presence of diverse mix of aerosol species with vastly different radiative properties, but also because the monsoon is strongly influenced by ocean and land surface processes, land use, land change, as well as regional and global greenhouse warming effects. Thus, sorting out the impacts of aerosol forcing, and interaction with the monsoon water cycle is a very challenging problem. In this talk, I will offer some insights into how aerosols may impact the Asian monsoon based on preliminary results from satellite observations and climate model experiments. Specifically, I will discuss the "elevated heat pump" hypothesis, involving atmospheric heating by absorbing aerosols (dust and black carbon) over the southern slopes of the Himalayas, and feedback with the deep convection, in modifying monsoon water cycle over South and East Asia. The role of aerosol forcing relative to those due to sea surface temperature and land surface processes, as well as observation requirements to verify such a hypothesis will also be discussed.

Lau, William K. M.↗

Interactions of an Imine Polymer with Nanoporous Silica and Carbon in Hybrid Adsorbents for Carbon Capture

Efficient carbon capture from stationary point sources can be achieved using hybrid adsorbents comprising nanoporous substrates coated with imine polymers. The physical properties of the CO 2 -adsorbing, nanodispersed polymers are altered by their interactions with the substrate, which in turn may impact their capture capacity. We study silica and carbon nanoporous substrates with different pore morphologies that were impregnated with polymer imine with the goal of characterizing the polymer dispersions in the pores. For silica and carbon samples, the mean densities of confined poly(ethylene imine) (PEI) were measured as functions of polymer loading and temperature using small-angle neutron scattering. Strong densification is found for imine polymers imbibed in mesoporous carbon. PEI in nanoporous silica does not experience this strong densification. At high loadings, plugs form, preferably at the pore throats, and can reduce accessible porosity. CO 2 capture measurements show that PEI interactions with the substrate play an important role. In conclusion, PEI in carbon shows the highest capture capacity at low temperatures and the lowest CO 2 adsorption at high temperatures, making it well-suited for temperature swing adsorption applications.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Interface Evolutionand Long-Term Performance of NegativeCarbon Fiber Structural Electrodes

Abstract Laminated structural batteries present a transformative solution to reducing weight constraints in electric vehicles. These structural batteries are based on a multifunctional material that incorporates an energy storage function within a carbon fiber-reinforced polymer. Despite the potential of this technology, the intricate morphology of fiber–matrix or electrode–electrolyte interfaces and the impact of long-term cycling at low current rates (C-rates) on these interfaces remain insufficiently understood. This study addresses these critical knowledge gaps by examining the influence of matrix composition on the long-term electrochemical performance of structural battery electrodes and exploring advanced techniques to investigate carbon fiber–matrix interfaces. Localized imaging and X-ray scattering techniques were used to characterize morphological changes at the electrode–electrolyte interfaces by analyzing negative structural electrodes. The findings revealed that the matrix composition influences long-term electrochemical behavior and fiber–matrix interface formation. While the intrinsic properties of carbon fibers largely remain unaffected by long-term cycling, cycling promotes debonding at fiber–matrix interfaces. Nonetheless, residual regions of adhesion persist, underscoring the potential for preserving multifunctionality even under prolonged cycling conditions. These insights advance the understanding of interface dynamics, which is critical for optimizing structural battery technologies.

Chemistry↗

Summertime Carbonaceous Aerosol in Interior Versus Coastal Northern Alaska

Abstract Rapid warming is likely increasing primary production and wildfire occurrence in the Arctic. Projected changes in carbonaceous aerosols during the summer will impact atmospheric chemistry and climate, but our understanding of these processes is limited by sparse observations. Here, we characterize carbonaceous aerosol in Alaska, USA: Toolik Field Station in the Interior and the Atmospheric Radiation Measurement facility at Utqiaġvik on the Arctic coast, during the summers of 2022 and 2023. We estimated PM 2.5 and PM 10 concentrations using laser light scattering (PurpleAir sensors) and examined total carbon (TC) and its organic carbon (OC) and elemental carbon (EC) fractions in total suspended particles (TSP). We investigated the dominant sources of carbonaceous aerosol using air mass backward‐trajectories from the NOAA HYSPLIT model and radiocarbon source apportionment of TC. TC concentrations were about twice as high in the Interior compared to the coast, with contemporary sources dominating at both Toolik (95%–99%) and Utqiaġvik (86%–89%) over minor contributions from fossil sources. Elevated PM, TC, OC, and EC concentrations coincided with major boreal forest fire activity in North America that brought smoke to the region. The radiocarbon signature of EC measured at Toolik during these wildfire events indicated that over 90% of the EC came from contemporary sources. Our measurements demonstrate the potential for Arctic aerosol concentrations to respond significantly to climate warming‐induced changes to the landscape and emphasize the need for continuous atmospheric monitoring to advance our understanding of this rapidly changing environment.

Welch, Allison M. [Department of Earth System Scie↗

Exactly solvable model of light-scattering errors in quantum simulations with metastable trapped-ion qubits

Here, we analytically solve a model for light scattering in Ising dynamics of metastable atomic qubits, generalizing the approach of Foss-Feig et al. to include leakage outside the qubit manifold. We analyze the influence of these fundamental errors in simulations of proposed experiments with metastable levels of 40 Ca + ions in a Penning trap. We find that “effective magnetic fields” generated by leaked qubits have significant impacts on spin-spin correlation functions for Greenberger-Horne-Zeilinger state preparation or for quantum simulations with strong coupling, while spin squeezing uses a much weaker coupling and is largely insensitive to the simulated leakage errors, even with a few hundred ions. Our theory and results are expected to be useful in modeling a variety of metastable qubit experiments in the future.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

TRINIDI: Time-of-Flight Resonance Imaging With Neutrons for Isotopic Density Inference

Accurate reconstruction of 2D and 3D isotope densities is a desired capability with great potential impact in applications such as evaluation and development of next-generation nuclear fuels. Neutron time-of-flight (TOF) resonance imaging offers a potential approach by exploiting the characteristic neutron absorption spectra of each isotope. However, it is a major challenge to compute quantitatively accurate images due to a variety of confounding effects such as severe Poisson noise, background scatter, beam non-uniformity, absorption non-linearity, and extended source pulse duration. We present the TRINIDI algorithm which is based on a two-step process in which we first estimate the neutron flux and background counts, and then reconstruct the areal densities of each isotope and pixel. Both components are based on the inversion of a forward model that accounts for the highly non-linear absorption, energy-dependent emission profile, and Poisson noise, while also modeling the substantial spatio-temporal variation of the background and flux. Further, to do this, we formulate the non-linear inverse problem as two optimization problems that are solved in sequence. We demonstrate on both synthetic and measured data that TRINIDI can reconstruct quantitatively accurate 2D views of isotopic areal density that can then be reconstructed into quantitatively accurate 3D volumes of isotopic volumetric density.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Simulating Electron Impact Ionization using a General Particle Tracer (GPT) Custom Element

A new C++ custom element has been developed with the framework of General Particle Tracer (GPT) to simulate electron impact ionization of residual gas molecules. The custom element uses Monte-Carlo routines to determine both the ion production rate and the secondary electron kinetic energy based on user-defined gas densities and theoretical values for the ionization cross section and the secondary electron differential cross section. It then uses relativistic kinematics to track the secondary electron, the scattered electron, and the newly formed ion after ionization. The ion production rate and the secondary electron energy distribution determined by the custom element have been benchmarked against theoretical calculations and against simulations made using the simulation package IBSimu. While the custom element was originally built for particle accelerator simulations, it is readily extensible to other applications. The custom element will be described in detail and examples of applications at the Thomas Jefferson National Accelerator Facility will be presented for ion production in a DC high voltage photo-gun.

Yoskowitz, J. T.↗

Natural Resources Assessment for the SNS Second Target Station, Oak Ridge, Tennessee

The US Department of Energy’s Oak Ridge National Laboratory (ORNL) is a leading institution in advanced materials, supercomputing, neutrons, and nuclear science. As a research laboratory managed by UT-Battelle, LLC for DOE, ORNL has national priorities in energy, security, and scientific discovery that necessitate facility improvements and expansions. DOE is also committed to environmental stewardship. The laboratory is located on the ~32,000-acre Oak Ridge Reservation (ORR), much of which is categorized as a National Environmental Research Park and a state Wildlife Management Area. DOE works with the Tennessee Wildlife Resources Agency (TWRA), Tennessee Department of Environment and Conservation (TDEC), US Fish and Wildlife Service (USFWS), US Department of Agriculture, and other agencies to serve as an effective steward of the ORR. Accordingly, project managers must conform to environmental regulations, agreements, and policies at the federal, state, and institutional levels. Per 40 CFR (Code of Federal Regulations) 1508.14, potential effects on research and science education on the National Environmental Research Park represent potential impacts of federal actions. Moreover, federal actions that affect the quantity and quality of hunting opportunities and deer reduction harvest on the Oak Ridge Wildlife Management Area must be considered whenever other aspects of the human environment (as defined by NEPA) are affected. The Spallation Neutron Source (SNS) is a premiere facility at ORNL that provides advanced capabilities in neutron scattering to promote new discoveries and research opportunities in material sciences, physics, chemistry, biological sciences, and others. A conceptual design for a Second Target Station (STS) has been in consideration for several years. The STS is intended to complement and enhance existing ORNL capabilities, notably research and exploration of complex materials. The proposed STS will involve development of existing natural areas on the ORR, which might contain sensitive resources that require mitigation or avoidance in accordance with existing policies and regulation. This report summarizes current knowledge of natural and cultural resources within the STS project area. At the time of this report, the proposed STS project consisted of an operations area comprising 55.4 acres (22.4 ha) and a total review area for potential construction comprising ~224 acres (90.6 ha). The review area is located primarily within forested natural areas of the ORR with minor development in the form of power-line rights-of-way and secondary/graveled roads (Figure 1). The primary goal was to evaluate potential effects on sensitive resources that might result from development of the STS. In addition to onthe-ground surveys during summer 2009 and fall 2019 to summer 2020 by ORNL Natural Resources Management Program and Aquatic Ecology Group staff, this report makes use of historical (pre-1995) and contemporary (1995 to present) data from additional confirmed sources (e.g., TDEC). Likewise, forest conditions were compiled primarily from a 2013 forest inventory effort for Forest Management Compartment 17 and supplemented with limited ground observations in 2019. The individuals who obtained and compiled the data that are presented here are familiar with and routinely assess sensitive resources on the ORR.

54 ENVIRONMENTAL SCIENCES↗

Notes on Asay Foil Analysis

As is the norm for momentum diagnostic analyses (i.e., both piezopin and Asay foil measurements), we begin by assuming all particles are created instantaneously at the moment of shock breakout; that all particles move collinearly through a perfect vacuum from source to sensor with a long mean free path to scattering (i.e., so that particle velocities and areal masses do not change in flight); and that the particles collide perfectly inelastically with the sensor. We also assume the foil supports have a negligible effect on the trajectory, as has been demonstrated experimentally, and the foil is sufficiently thin that corrections for thick-plate effects (e.g., time delays between particle impacts on the collecting side and velocity changes on the probe side) can be disregarded. We seek an exact analytic treatment of an ideal system that perfectly embodies these characteristics.

36 MATERIALS SCIENCE↗

Universality of Collective Density Fluctuations in Liquids at and away from Equilibrium – An Integrated Neutron Scattering, Theoretical, and Computational Study (Final Technical Report)

Liquids, ubiquitous on earth, are prototypical disordered condensed matter. As the mediate phase between non-structured gases and ordered solids, liquids p ossess intriguing complexities that are absent on either extreme counter phase, especially when they are driven away from equilibrium. Despite decades of studies, the physics of liquids still keeps surprising us and challenges our understanding of condensed matter, emergent phenomena, and complex systems. Among the many interesting properties, the nature of collective dynamics in liquids remains elusive because of both the presence of strong interactions and the absence of translational invariance. This project studied the universal features of collective density fluctuations (or collective modes), which include both phonon-like excitations and collective relaxations, in the Q-dependent generalized hydrodynamic regime in liquids and liquid-like matter both at and away from equilibrium. We performed systematic studies of the fast collective dynamics (including both phonon-like excitations and collective relaxations) of four classes of liquids characterized by different fragilities and interactions using synergistically integrated coherent neutron scattering experiments (Inelastic Neutron Scattering (INS), Quasi-Elastic Neutron Scattering (QENS), and Neutron Spin Echo (NSE)), a ViscoElastic Hydrodynamics theory we have been developing, andMolecular Dynamics (MD) simulations and our analysis package LiquidLib. The transformative knowledge of the collective dynamics in liquids is important to understand and ultimately control the transport of mass, energy, and charge in liquids, both at and away from thermal equilibrium, which may will likely impact a wide range of disciplines.

36 MATERIALS SCIENCE↗