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DOE OSTI2022

Driving force and pathway in polyelectrolyte complex coacervation

There is notable discrepancy between experiments and coarse-grained model studies regarding the thermodynamic driving force in polyelectrolyte complex coacervation: experiments find the free energy change to be dominated by entropy, while simulations using coarse-grained models with implicit solvent usually report a large, even dominant energetic contribution in systems with weak to intermediate electrostatic strength. Here, using coarse-grained, implicit-solvent molecular dynamics simulation combined with thermodynamic analysis, we study the potential of mean force (PMF) in the two key stages on the coacervation pathway for symmetric polyelectrolyte mixtures: polycation–polyanion complexation and polyion pair–pair condensation. We show that the temperature dependence in the dielectric constant of water gives rise to a substantial entropic contribution in the electrostatic interaction. By accounting for this electrostatic entropy, which is due to solvent reorganization, we find that under common conditions (monovalent ions, room temperature) for aqueous systems, both stages are strongly entropy-driven with negligible or even unfavorable energetic contributions, consistent with experimental results. Furthermore, for weak to intermediate electrostatic strengths, this electrostatic entropy, rather than the counterion-release entropy, is the primary entropy contribution. From the calculated PMF, we find that the supernatant phase consists predominantly of polyion pairs with vanishingly small concentration of bare polyelectrolytes, and we provide an estimate of the spinodal of the supernatant phase. Finally, we show that prior to contact, two neutral polyion pairs weakly attract each other by mutually induced polarization, providing the initial driving force for the fusion of the pairs.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Climate forcing controls on carbon terrestrial fluxes during shale weathering

Climate influences near-surface biogeochemical processes and thereby determines the partitioning of carbon dioxide (CO 2 ) in shale, and yet the controls on carbon (C) weathering fluxes remain poorly constrained. Using a dataset that characterizes biogeochemical responses to climate forcing in shale regolith, we implement a numerical model that describes the effects of water infiltration events, gas exchange, and temperature fluctuations on soil respiration and mineral weathering at a seasonal timescale. Our modeling approach allows us to quantitatively disentangle the controls of transient climate forcing and biogeochemical mechanisms on C partitioning. We find that ~3% of soil CO 2 (1.02 mol C/m 2 /y) is exported to the subsurface during large infiltration events. Here, net atmospheric CO 2 drawdown primarily occurs during spring snowmelt, governs the aqueous C exports (61%), and exceeds the CO 2 flux generated by pyrite and petrogenic organic matter oxidation (~0.2 mol C/m 2 /y). We show that shale CO 2 consumption results from the temporal coupling between soil microbial respiration and carbonate weathering. This coupling is driven by the impacts of hydrologic fluctuations on fresh organic matter availability and CO 2 transport to the weathering front. Diffusion-limited transport of gases under transient hydrological conditions exerts an important control on CO 2 (g) egress patterns and thus must be considered when inferring soil CO 2 drawdown from the gas phase composition. Our findings emphasize the importance of seasonal climate forcing in shaping the net contribution of shale weathering to terrestrial C fluxes and suggest that warmer conditions could reduce the potential for shale weathering to act as a CO 2 sink.

58 GEOSCIENCES↗

DOE OSTI2025

New Class of Three-Nucleon Forces and Their Implications

Here, we identify a new class of three-nucleon forces that arises in the low-energy effective theory of nuclear interactions including pions. We estimate their contribution to the energy of neutron and nuclear matter and find that it can be as important as the leading-order three-nucleon forces previously considered in the literature. The magnitude of this force is set by the strength of the coupling of pions to two nucleons and is presently not well constrained by experiments. The implications for nuclei, nuclear matter, and the equation of state of neutron matter are briefly discussed.

chiral perturbation theory↗

DOE OSTI2021

Many-body forces and nucleon clustering near the QCD critical point

It has been proposed that one can look for the QCD critical point (CP) by the Beam Energy Scan accurately monitoring event-by-event fluctuations. This experimental program is under way at the BNL RHIC collider. Separately, it has been studied how clustering of nucleons at freeze out affects proton multiplicity distribution and light nuclei production. It was found that even a minor increase of the range of nuclear forces dramatically increases clustering, while large correlation length ξ near CP makes attraction due to binary forces unrealistically large. Here, in this paper, we show that repulsive many-body forces near CP should overcome the binary ones and effectively suppress clustering. We also discuss current experimental data and point out locations at which a certain drop in clustering may already be observed.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

DOE OSTI2021

Discovering new forces with gravitational waves from supermassive black holes

Supermassive black hole binary mergers generate a stochastic gravitational wave background detectable by pulsar timing arrays. While the amplitude of this background is subject to significant uncertainties, the frequency dependence is a robust prediction of general relativity. Here we show that the effects of new forces beyond the Standard Model can modify this prediction and introduce unique features into the spectral shape. In particular, we consider the possibility that black holes in binaries are charged under a new long-range force, and we find that pulsar timing arrays are capable of robustly detecting such forces. Supermassive black holes and their environments can acquire charge due to high-energy particle production or dark sector interactions, making the measurement of the spectral shape a powerful test of fundamental physics.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

DOE OSTI2023

Many-Body Effects in Aqueous Systems: Synergies Between Interaction Analysis Techniques and Force Field Development

Interaction analysis techniques, including the many-body expansion (MBE), symmetry-adapted perturbation theory, and energy decomposition analysis, allow for an intuitive understanding of complex molecular interactions. We review these methods by first providing a historical context for the study of many-body interactions and discussing how nonadditivities emerge from Hamiltonians containing strictly pairwise-additive interactions. We then elaborate on the synergy between these interaction analysis techniques and the development of advanced force fields aimed at accurately reproducing the Born–Oppenheimer potential energy surface. In particular, we focus on ab initio–based force fields that aim to explicitly reproduce many-body terms and are fitted to high-level electronic structure results. These force fields generally incorporate many-body effects through ( a) parameterization of distributed multipoles, ( b) explicit fitting of the MBE, ( c) inclusion of many-atom features in a neural network, and ( d) coarse-graining of many-body terms into an effective two-body term. We also discuss the emerging use of the MBE to improve the accuracy and speed of ab initio molecular dynamics.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2024

Gridded Sub-daily Climate Forcings for North America Based on Daymet and GSWP3 (Daymet-GSWP3)

To support high spatial and temporal resolution land surface modeling, this dataset provides 3-hourly time step historic weather forcing at 1-km spatial resolution for the entire North America. The latest Daymet V4 data provides gridded historic daily weather observations at 1-km spatial resolution from 1980 to 2014. Using sub-daily temporal information from the Global Soil Wetness Project Phase 3 (GSWP3), Daymet was further temporally downscaled to 3-hourly time steps and provided in the format required for land surface model simulations. The process of temporal downscaling preserves the relative magnitude in each sub-daily time step from GSWP3 while maintaining the total and average values from Daymet for each day. This results in a blended 1980-2014 Daymet-GSWP3 dataset. Available variables include surface air temperature, precipitation, specific humidity, shortwave and longwave radiation, wind speed, and pressure. These data can be used as a high-resolution meteorological forcing dataset to support high-resolution land surface modeling where accurate meteorological forcing datasets built from historic observations and/or reanalysis datasets are desirable.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2024

Gridded Sub-daily Climate Forcings for North America Based on Daymet and GSWP3 (Daymet-GSWP3)

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

Proof that Combining the Forced-collision and DXTRAN Monte Carlo Variance-reduction Techniques is Fair

This report provides mathematical proof that the MCNP DXTRAN (also known in other codes as forced-flight) and forced-collision variance-reduction techniques do not bias the expected value of Monte Carlo simulation estimates when combined. Proof is also provided that the techniques are unbiased when used independently. To prove that the techniques are unbiased, this report derives the first History Score Moment Equation (HSME) for non-multiplying media employing only forced collisions, only DXTRAN, and then both the variance-reduction techniques combined, as defined next. The HSMEs are found by forming the History Score Probability Density Functions (HSPDFs) and then taking the first score moment. Following its derivation, each HSME with a variance-reduction technique employed is reduced to the HSME for an analog simulation. Because the HSME represents the expected contribution to estimators in the simulation, reducing the HSME with variance reduction to the analog HSME shows that the simulation is unbiased despite the variance-reduction technique considered in the HSME. Analysis regarding higher-score moments of each technique is the subject of prior work and is not addressed herein. Throughout this work, the phase space p is defined to be the particle position x, direction-of-flight unit vector $\hat{Ω}$, energy E, and statistical weight w, $$p ≡ (x; \hat{Ω}; E; w).$$ A reduced phase-space excluding the statistical weight of the particle, $$r ≡ (x; \hat{Ω}; E),$$ is also used.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2021

History of and Aftermath from the Withdrawal of the Intermediate-Range Nuclear Forces Treaty

On February 1, 2019, the United States and Russia withdrew from the three-decades old Intermediate-Range Nuclear Forces (INF) treaty. Events precipitating the withdrawal were allegations by both the United States and Russia of a variety of treaty violations. Until that point, the treaty had been a centerpiece of arms control and a key agreement of the global security architecture. The absence of such a pillar has the potential destabilize the status quo of arms control, creating significant uncertainty in global nuclear stability and security. In this paper, we present a historical review as overture to an analysis on the impacts of this development on force structure. This analysis examines the changes in U.S., Russian, and Chinese nuclear forces which may occur as a result of the treaty's demise. The article concludes with commentary on potential actions to preserve stability in a post-INF world.

45 MILITARY TECHNOLOGY, WEAPONRY, AND NATIONAL DEF↗

DOE OSTI2022

2022 FORCE Development Status Update

Integrated energy systems (IESs) are essential for decarbonizing electricity and industrial sectors and fully exploiting these systems requires sophisticated planning, scheduling, and dispatching tools to maximize their socio-economic benefits. The Framework for Optimization of Resources and Economics (FORCE) is a tool suite developed at Idaho National Laboratory and is dedicated to making robust analyses of IESs easier for analysts and researchers. The report summarizes the improvements and updates to FORCE during the most recent development cycle. Particularly, we demonstrate improvements to user accessibility, stochastic time-series analysis, and vertical integration with the software tools provided in FORCE.

97 MATHEMATICS AND COMPUTING↗

DOE OSTI2020

Long-lasting strong electrostatic attraction and adhesion forces of dust particles on photovoltaic modules

Photovoltaic (PV) energy-yield loss due to solar module soiling has become increasingly important as solar module deployment is now at the hundreds of gigawatts scale and continues to grow rapidly. The electrostatic attraction and adhesion force (F es ) of dust particles by the high voltages from solar panels have been reported to be 1 to 2 orders of magnitude stronger than the van der Waals and water capillary forces, which has been corroborated by observing the increase in system voltage-induced soiling rate by setting up an outdoor test. Here, we report another characteristic of F es on soiling - long-lasting or slow decay after turning off the high voltage applied to solar panels. The F es decay time varies across a wide time range of 1 to 10 h, depending on two factors: 1) whether the cell, the particle, or both were charged with high voltage before the voltages were turned off; and 2) how the cell was connected to the ground after the voltage was turned off - either connected through the power-supply electronics, directly connected to the ground, or electrically floated. The Fes decay is understood in terms of 1) net electrical charge dissipations in both particle and cell, 2) thermal disordering of dipole polarization in the module glass dielectrics, and 3) charge redistribution by the electrostatic interaction of particle and module glass. This long-lasting F es for hours can affect the solar panel soiling after sunset, and it can have an even greater effect when combined with water condensation at night.

14 SOLAR ENERGY↗

DOE OSTI2020

Autonomous Self-Healing Elastomers with Unprecedented Adhesion Force

Self-healable elastomers are extremely attractive due to their ability to prolong product lifetime. An additional function that could further expand their applications is strong adhesion force to clean and dusty surfaces. This study reports a series of autonomous self-healable and highly adhesive elastomers (ASHA-Elastomer) that are fabricated via a simple, efficient, and scalable process. The obtained elastomers exhibit outstanding mechanical properties with elongation at break up to 2102% and toughness (modulus of toughness) of 1.73 MJ m -3 . The damaged ASHA-Elastomer can autonomously self-heal with full recovery of functionalities, and the healing process is not affected by the presence of water. The elastomers are found to possess an ultrahigh adhesion force up to 3488 N m -1 , greatly outperforming previously reported self-healing adhesive elastomers. Furthermore, the adhesion force of the ASHA-Elastomer is negligibly affected by dust on the surface, in stark contrast with regular adhesive polymers that have adhesion strengths extremely sensitive to dust. The successful development of high-toughness, autonomous self-healable, and ultra-adhesive elastomers will enable a wide range of applications with enhanced longevity and versatility, including their use in sealants, adhesives, and stretchable devices.

36 MATERIALS SCIENCE↗

DOE OSTI2024

Impact of the cosmic neutrino background on long-range force searches

Light bosons can mediate long-range forces. We show that light bosonic mediators interacting with a background medium, in particular, with the cosmic neutrino background (CνB), may induce medium-dependent masses which could effectively screen long-range forces from detection. This leads to profound implications for long-range force searches in e.g. the Eöt-Wash, MICROSCOPE, and lunar laser-ranging (LLR) experiments. For instance, we find that when the coupling of the mediator to neutrinos is above 3 × 10 −10 or 5 × 10 −13 , bounds from LLR and experiments employing the Sun as an attractor, respectively, would be entirely eliminated. Larger values of the coupling can also substantially alleviate bounds from searches conducted at shorter distances.

79 ASTRONOMY AND ASTROPHYSICS↗

DOE OSTI2020

What causes the spread of model projections of ocean dynamic sea-level change in response to greenhouse gas forcing?

Abstract Sea levels of different atmosphere–ocean general circulation models (AOGCMs) respond to climate change forcing in different ways, representing a crucial uncertainty in climate change research. We isolate the role of the ocean dynamics in setting the spatial pattern of dynamic sea-level ( ζ ) change by forcing several AOGCMs with prescribed identical heat, momentum (wind) and freshwater flux perturbations. This method produces a ζ projection spread comparable in magnitude to the spread that results from greenhouse gas forcing, indicating that the differences in ocean model formulation are the cause, rather than diversity in surface flux change. The heat flux change drives most of the global pattern of ζ change, while the momentum and water flux changes cause locally confined features. North Atlantic heat uptake causes large temperature and salinity driven density changes, altering local ocean transport and ζ . The spread between AOGCMs here is caused largely by differences in their regional transport adjustment, which redistributes heat that was already in the ocean prior to perturbation. The geographic details of the ζ change in the North Atlantic are diverse across models, but the underlying dynamic change is similar. In contrast, the heat absorbed by the Southern Ocean does not strongly alter the vertically coherent circulation. The Arctic ζ change is dissimilar across models, owing to differences in passive heat uptake and circulation change. Only the Arctic is strongly affected by nonlinear interactions between the three air-sea flux changes, and these are model specific.

54 ENVIRONMENTAL SCIENCES↗

DOE OSTI2021

The repulsive Casimir-type forces in binary mixture of weakly interacting Bose–Einstein condensates gases

Highlights: • The equations of the state of a binary mixture weakly interacting Bose gases are established based on the Lagrangian of the system. • The formulae of the Casimir-type energy and the resulting Casimir-type force are produced from the quantum part of the grand canonical energy. • The results for the Casimir-type effect in the one-field case can be re-obtained by using the results of the two-field case. Within the framework of the quantum field theory (QFT) in the one-loop approximation, we investigate the Casimir-type effect in a mixture of two-component weakly interacting Bose-Einstein condensates (BECs) gases confined between two parallel plates at zero temperature. The Casimir-type forces in the miscible state of BECs for different boundary conditions (BCs) are discovered and compared to each other. The repulsive nature of the Casimir-type force in BECs is defined for the first time. Our calculations are finished in both grand canonical ensemble (GCE) and canonical ensemble (CE).

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

DOE OSTI2022

Deep learning for drag force modelling in dilute, poly-dispersed particle-laden flows with irregular-shaped particles

Here, this study applies machine learning-based approaches to develop a drag force model for irregular-shaped particles in incompressible flows. The particle-laden flows are studied through an in-house particle-resolved direct numerical simulation (PR-DNS) at low-intermediate Reynolds numbers (Re). We utilize the PR-DNS to obtain drag force coefficients and flow fields of single particles. A variational auto-encoder model is used to obtain latent vectors to represent the geometrical features of the particles, and artificial neural networks (ANN) are developed to predict drag force coefficients and flow fields of the single particles. This study applies a pairwise interaction extended point-particle (PIEP) model to obtain the coefficients assuming the flow fields of neighboring particles can be linearly superposed. The PIEP method shows significant improvement on prediction for a few neighbored particles. In addition, the results reveal R2 scores of 0.56-0.62 and errors of 9.1-10.0 % for the dilute, polydispersed systems with a volume fraction of 0.5 %.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

DOE OSTI2022

Retrofitting stoves with forced jets of primary air improves speed, emissions, and efficiency: Evidence from six types of biomass cookstoves

Incorporating jets of forced air into biomass cookstove combustion has been shown to potentially decrease harmful emissions, leading to a variety of designs in recent years. These have shown mixed success in terms of real-world performance, usability, and durability. The Jet-Flame forced draft retrofit accessory was recently developed to implement forced jets of primary air at a low cost into a wide range of types of cookstoves using a small 1.5-W fan housed in a low-cost cast iron body to be inserted beneath the fuel bed of a biomass cooking fire. This research sought to quantify the potential efficiency and emissions performance impacts of the Jet-Flame when installed in six different types of biomass cookstoves (three open or shielded fires and three rocket stoves) versus the natural draft performance of each. The effect of the operating fan voltage was also measured. A series of tests following a modified ISO 19867-1:2018 protocol were performed in the laboratory using the Aprovecho Laboratory Emissions Measurement System (LEMS) equipped with additional oxygen and temperature sensors. Results for each stove carefully tended with a single layer of sticks showed that the global average PM 2.5 reduction with the Jet-Flame was 89 % relative to the natural draft cases, with larger relative improvements seen in the most rudimentary stoves. CO was reduced by a global average of 74 %, reaching tier 4 or 5 for all stoves. Thermal efficiency was also improved by 34 % when calculated without taking into account the energy content of the remaining char (or 21 % with char), illustrating the value of burning char to provide cooking energy rather than leaving it unburned in the combustion chamber as is common in many natural draft stoves. Time to boil was also reduced by 8 %. In addition, adjusting the voltage of the jet-flame assisted in modulating firepower, improving the usability of the stove. These results indicate a strong potential for the Jet-Flame to help reduce emissions and fuel consumption in a wide range of cookstove designs at a relatively low cost or need for changes in behavior, fuel, or cooking device. The unit also provides enhanced usability in terms of ease of startup, cooking speed, low PM emissions at high power, and burning char. Additional studies are needed to measure performance in the field and under a variety of operational conditions.

32 ENERGY CONSERVATION, CONSUMPTION, AND UTILIZATI↗