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At least 451 records · Page 25

Global and Regional Radiative Forcing from 20 Reductions in BC, OC and SO4 an HTAP2 Multi-Model Study

In the Hemispheric Transport of Air Pollution Phase 2 (HTAP2) exercise, a range of global atmospheric general circulation and chemical transport models performed coordinated perturbation experiments with 20% reductions in emissions of anthropogenic aerosols, or aerosol precursors, in a number of source regions. Here, we compare the resulting changes in the atmospheric load and vertically resolved profiles of black carbon (BC), organic aerosols (OA) and sulfate (SO4/ from 10 models that include treatment of aerosols. We use a set of temporally, horizontally and vertically resolved profiles of aerosol forcing efficiency (AFE) to estimate the impact of emission changes in six major source regions on global radiative forcing (RF) pertaining to the direct aerosol effect, finding values between. 51.9 and 210.8mW/sq m/Tg for BC, between -2.4 and -17.9mW/sq m/Tg for OA and between -3.6 and -10.3W/sq m/Tg for SO4. In most cases, the local influence dominates, but results show that mitigations in south and east Asia have substantial impacts on the radiative budget in all investigated receptor regions, especially for BC. In Russia and the Middle East, more than 80 % of the forcing for BC and OA is due to extra-regional emission reductions. Similarly, for North America, BC emissions control in east Asia is found to be more important than domestic mitigations, which is consistent with previous findings. Comparing fully resolved RF calculations to RF estimates based on vertically averaged AFE profiles allows us to quantify the importance of vertical resolution to RF estimates. We find that locally in the source regions, a 20% emission reduction strengthens the radiative forcing associated with SO4 by 25% when including the vertical dimension, as the AFE for SO4 is strongest near the surface. Conversely, the local RF from BC weakens by 37% since BC AFE is low close to the ground. The fraction of BC direct effect forcing attributable to intercontinental transport, on the other hand, is enhanced by one-third when accounting for the vertical aspect, because long-range transport primarily leads to aerosol changes at high altitudes, where the BC AFE is strong. While the surface temperature response may vary with the altitude of aerosol change, the analysis in the present study is not extended to estimates of temperature or precipitation changes.

profiles of aerosol forcing efficiency (AFE)↗

Drag-Free Control and Drag Force Recovery of Small Satellites

Drag-free satellites provide autonomous precision orbit determination, accurately map the static and time varying components of Earth's mass distribution, aid in our understanding of the fundamental force of gravity, and will ultimately open up a new window to our universe through the detection and observation of gravitational waves. At the heart of this technology is a gravitational reference sensor, which (a) contains and shields a free-floating proof mass from all non-gravitational forces, and (b) precisely measures the position of the test mass inside the sensor. Thus, both test mass and spacecraft follow a pure geodesic in spacetime. By tracking the position of a low Earth orbiting drag-free satellite we can directly determine the detailed shape of geodesics and through analysis, the higher order harmonics of the Earths geopotential. This paper explores two different drag-free control systems on small satellites. The first drag-free control system is a continuously compensated single thruster 3-unit CubeSat with a suspension-free spherical proof-mass. A feedback control system commands the thruster and Attitude and Determination Control System to fly the tender spacecraft with respect to the test mass. The spheres position is sensed with a LED-based differential optical shadow sensor, its electric charge controlled by photoemission using UV LEDs, and the spacecraft position is maintained with respect to the sphere using an ion electrospray propulsion system. This configuration is the most fuel-efficient drag-free system possible today. The second drag-free control system is an electro-statically suspended cubical proof-mass that is operated with a low duty cycle, limiting suspension force noise over brief, known time intervals on a small GRACE-II -like satellite. The readout is performed using a laser interferometer, which is immune to the dynamic range limitations of voltage references. This system eliminates the need for a thruster, enabling drag-free control systems for passive satellites. In both cases, the test mass position, GPS tracking data, and commanded actuation, either thrust or suspension system, can be analyzed to estimate the 3-axis drag forces acting on the satellite. The data produces the most precise maps of upper atmospheric drag forces and with additional information, detailed models that describe the dynamics of the upper atmosphere and its impact on all satellites that orbit the Earth. This paper highlights the history, applications, design, laboratory technology development and highly detailed simulation results of each control system.

Small Satellites↗

Validated Reactive Force Field Quantifies MXene Interfacial Properties, Mechanics, and Thermal Transport

MXenes combine rich surface chemistry, mechanical strength, and high conductivity for a multitude of emerging applications. Predictive modeling supports accelerated materials designs and has been limited by the absence of validated and transferable force fields. Here, we introduce an interpretable, reactive INTERFACE force field (IFF and IFF-R) for Ti 3 C 2 T x MXenes that is trained based on chemical knowledge and achieves quantitative agreement with experiments across lattice parameters (<0.5%), density (<0.2%), liquid contact angles, Raman spectra, and the in-plane elastic modulus (∼320 GPa). The models cover surface terminations from hydroxyl (−OH) to fluorine (−F) groups and are extensible to other chemistries. We introduce pH-resolved surface chemistry and identify dopamine adsorption mechanisms at MXene–aqueous interfaces supported by QCM-D and UV–Vis experiments. The data reveal coplanar and perpendicular binding modes and concentration-dependent multilayer assembly. We predict previously inaccessible properties, including termination-dependent cleavage energies, interlayer shear moduli and dynamic shear failure, nanoindentation and brittle fracture, anisotropic in-plane and out-of-plane thermal conductivities, including the role of defects. Agreement with available experimental data is consistently close and exceeds DFT accuracy across the benchmark properties examined. The IFF/IFF-R model is compatible with CHARMM, AMBER, OPLS, and CVFF force fields for simulations of MXenes with diverse surface terminations, electrolyte interfaces, biointerfaces, and polymer composites without additional parameters. Parameter sets, 3D models, and analysis scripts are provided for community use. The validated, reactive, and transferable IFF framework facilitates predictive design of MXene-based films, membranes, sensing interfaces, and composites.

MXene↗

Utilization of coupled eigenmodes in Akiyama atomic force microscopy probes for bimodal multifrequency sensing

Akiyama atomic force microscopy probes represent a unique means of combining several of the desirable properties of tuning fork and cantilever probe designs. As a hybridized mechanical resonator, the vibrational characteristics of Akiyama probes result from a complex coupling between the intrinsic vibrational eigenmodes of its constituent tuning fork and bridging cantilever components. Here, through a combination of finite element analysis modeling and experimental measurements of the thermal vibrations of Akiyama probes, we identify a complex series of vibrational eigenmodes and measure their frequencies, quality factors, and spring constants. We then demonstrate the viability of Akiyama probes to perform bimodal multi-frequency force sensing by performing a multimodal measurement of a surface's nanoscale photothermal response using photo-induced force microscopy imaging techniques. Further performing a parametric search over alternative Akiyama probe geometries, we propose two modified probe designs to enhance the capability of Akiyama probes to perform sensitive bimodal multifrequency force sensing measurements.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Drag force to all orders in gradients

We study the energy loss of a heavy quark slowly moving through an evolving strongly coupled plasma. We use the linearized fluid/gravity correspondence to describe small perturbations of the medium flow with general spacetime dependence. This all order linearized hydrodynamics results in a drag force exerted on a heavy quark even when it is at rest with the fluid element. We show how the general contribution to the drag force can be derived order by order in the medium velocity gradients and provide explicit results valid up to the third order. We then obtain an approximate semi-analytic result for the drag force to all orders in the gradient expansion but linearized in the medium velocity. Thus, the effects of a class of hydrodynamic gradients on the drag force are re-summed, giving further insight into the dissipative properties of strongly coupled plasmas. The all order result allows us to study the drag force in the non-hydrodynamic regime of linear medium perturbations that vary rapidly in space and time.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

The neutrino force in neutrino backgrounds: Spin dependence and parity-violating effects

The neutrino force results from the exchange of a pair of neutrinos. A neutrino background can significantly influence this force. In this work, we present a comprehensive calculation of the neutrino force in various neutrino backgrounds with spin dependence taken into account. In particular, we calculate the spin-independent and spin-dependent parity-conserving neutrino forces, in addition to the spin-dependent parity-violating neutrino forces with and without the presence of a neutrino background for both isotropic and anisotropic backgrounds. Compared with the vacuum case, the neutrino background can effectively violate Lorentz invariance and lead to additional parity-violating terms that are not suppressed by the velocity of external particles. We estimate the magnitude of the effect of atomic parity-violation experiments, and it turns out to be well below the current experimental sensitivity.

72 PHYSICS OF ELEMENTARY PARTICLES AND FIELDS↗

Greenhouse-gas forced changes in the Atlantic meridional overturning circulation and related worldwide sea-level change

Abstract The effect of anthropogenic climate change in the ocean is challenging to project because atmosphere-ocean general circulation models (AOGCMs) respond differently to forcing. This study focuses on changes in the Atlantic Meridional Overturning Circulation (AMOC), ocean heat content ( $$\Delta$$ Δ OHC), and the spatial pattern of ocean dynamic sea level ( $$\Delta \zeta$$ Δ ζ ). We analyse experiments following the FAFMIP protocol, in which AOGCMs are forced at the ocean surface with standardised heat, freshwater and momentum flux perturbations, typical of those produced by doubling $$\hbox {CO}_{{2}}$$ CO 2 . Using two new heat-flux-forced experiments, we find that the AMOC weakening is mainly caused by and linearly related to the North Atlantic heat flux perturbation, and further weakened by a positive coupled heat flux feedback. The quantitative relationships are model-dependent, but few models show significant AMOC change due to freshwater or momentum forcing, or to heat flux forcing outside the North Atlantic. AMOC decline causes warming at the South Atlantic-Southern Ocean interface. It does not strongly affect the global-mean vertical distribution of $$\Delta$$ Δ OHC, which is dominated by the Southern Ocean. AMOC decline strongly affects $$\Delta \zeta$$ Δ ζ in the North Atlantic, with smaller effects in the Southern Ocean and North Pacific. The ensemble-mean $$\Delta \zeta$$ Δ ζ and $$\Delta$$ Δ OHC patterns are mostly attributable to the heat added by the flux perturbation, with smaller effects from ocean heat and salinity redistribution. The ensemble spread, on the other hand, is largely due to redistribution, with pronounced disagreement among the AOGCMs.

54 ENVIRONMENTAL SCIENCES↗

Third-body stabilization of supercritical CO 2 in CO oxidation: development and application of a ReaxFF force field for the CO/O/CO 2 system

Supercritical CO 2 (scCO 2 ) plays a crucial role as a solvent in separation processes, advanced power cycles, and materials processing. Nonetheless, the atomistic comprehension of how the dense scCO 2 matrix influences the fundamental reaction of carbon monoxide (CO) is still insufficiently explored. Experimental studies and molecular dynamics (MD) simulations frequently fail to detect the highly reactive, transient intermediates, such as atomic oxygen (O), that drive these reactions. Here, to address this issue, we have developed a novel ReaxFF reactive force field for the CO 2 /CO/O system. The force field parameters were calibrated using density functional theory and second-order Møller-Plesset calculations to model CO 2 crystal properties, intermolecular interactions, bond dissociation curves, and reaction energy barriers. The force field reproduces the cohesive energy of the CO 2 crystal, the pressure characteristics of bulk scCO 2 , the equation-of-state behavior over a wide pressure–density range, the pressure dependence of the C–O bond length under compression, and the structural properties of liquid and scCO 2 , as documented by experiments, ab-initio MD, and prominent non-reactive models. The force field was subsequently applied to study the CO + O → CO 2 reaction. In a dilute environment, the reaction is inefficient as the newly formed CO 2 rapidly dissociates due to excess kinetic and potential energy acquired from the exothermic reaction. Conversely, in a dense scCO 2 environment, the surrounding matrix acts as an efficient third body, stabilizing the emerging CO2 product via molecular collisions. Statistical analysis confirms an average excess energy dissipation of 133.9 ± 3.6 kcal/mol over 112.4 ± 17.9 ps. Kinetic energy decomposition reveals that ∼ 92% of the excess kinetic energy is stored in internal (rotational and vibrational) degrees of freedom. This ReaxFF force field establishes a mechanistic foundation for third-body stabilization in dense reactive environments.

Chowdhury, Emdadul Haque [Pennsylvania State Univ.↗

Trunk muscle forces and spinal loads while walking in persons with lower limb amputation: Influences of chronic low back pain

Persons with lower limb amputation (LLA) are at high risk for developing chronic low back pain (LBP), often with biomechanical factors considered as likely contributors. Here, trunk and pelvis kinematics, muscle forces, and resultant spinal loads were characterized in persons with LLA, with and without chronic LBP. Thirty-five persons with unilateral LLA – 19 with chronic LBP (“LLA-cLBP”), 16 without LBP (“LLA-nLBP”) – and 15 (uninjured) persons without LBP (“CTR-nLBP”) walked overground (1.3 m/s) while thorax and pelvis kinematics were tracked (and ranges of motion [ROM] computed), and used as inputs for a non-linear finite element model of the spine to estimate global and local muscle forces, and resultant spinal loads. In the frontal and transverse planes, thorax ROM were up to 66.6% smaller in LLA-nLBP versus LLA-cLBP (P < 0.001) and CTR-nLBP (P < 0.001). In the sagittal plane, pelvis ROM was 50.4% smaller in LLA-nLBP versus LLA-cLBP (P = 0.014). LLA-cLBP exhibited 45.5% and 34.2% greater peak local and global muscle forces, respectively, versus CTR-nLBP (P < 0.011). Up to 48.1% greater spinal loads were observed in LLA-cLBP versus CTR-nLBP (P < 0.013); peak compression and local muscle forces were respectively 20.2% and 41.0% larger in LLA-nLBP versus CTR-nLBP (P < 0.005). Despite differences in trunk and pelvis kinematics between LLA-cLBP and LLA-nLBP, trunk muscle forces and spinal loads were similar (P > 0.101) between these groups. Similar loading parameters regardless of LBP presence, while highly dependent on trunk muscle activation strategies, may mitigate further accumulation of mechanical fatigue. Finally, it remains important to understand the temporality of loading with respect to LBP onset following LLA.

60 APPLIED LIFE SCIENCES↗

Correlating inter-particle forces and particle shape to shear-induced aggregation/fragmentation and rheology for dilute anisotropic particle suspensions: A complementary study via capillary rheometry and in-situ small and ultra-small angle X-ray scattering

Predicting the stability of suspensions composed of anisotropic particles is difficult due to the complexity and interplay of hydrodynamic and colloidal forces. For example, it is not well understood how non-spherical particle shapes affect suspension-rheological responses. This study presents evidence showing how the stacking of boehmite platelets dispersed in aqueous solution leads to moderate shear thinning, even at low boehmite mass fractions. Wide angle X-ray, small angle X-ray, and ultra-small angle X-ray scattering were used to simultaneously monitor changes to the size and fractal dimensions of boehmite aggregates from 6 – 10,000 Å as the sample was recirculated through an in situ capillary rheometer. The latter also provided simultaneous measurements of the viscosity of the suspensions. Computational fluid dynamics modeling of the apparatus was used to provide a more rigorous analysis of the fluid flow. In addition to shear-induced aggregation/fragmentation correlated to a complicated balance between hydrodynamic and colloidal forces, the results indicate that orientationally-dependent interactions, arising from non-spherical boehmite aggregate sub-units, may explain the relatively large experimental viscosity when the hydrodynamic force is small compared to colloidal forces. Ultimately, the results from this study can provide a foundation for future work investigating particle shape effects on colloidal and hydrodynamics forces.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Digital force prediction for milling

This paper presents a fully digital, integrated approach for milling force prediction with arbitrary end mill-work material combinations. The approach includes: 1) structured light scanning to identify the end mill’s cutting edge macro-geometry along the tool axis; 2) structured light scanning to measure the cutting edge cross-sectional rake and relief profiles; 3) finite element analysis of orthogonal cutting to determine the force model coefficients that relate the force to chip area using the work material’s constitutive model and tool’s rake and relief profiles; and 4) time domain simulation with inputs that include the measured cutting edge macro-geometry, finite element-based force model, and measured structural dynamics. Milling force predictions are compared to in-process measurements to validate the method.

42 ENGINEERING↗

Symmetrized Drude Oscillator Force Fields Improve Numerical Performance of Polarizable Molecular Dynamics

Drude oscillator potentials are a popular and computationally efficient class of polarizable models that represent each polarizable atom as a positively charged Drude core harmonically bound to a negatively charged Drude shell. Here we show that existing force fields that place all non-Coulomb forces on the Drude core and none on the shell inadvertently couple the dipole to non-Coulombic forces. This introduces errors where interactions with neutral particles can erroneously induce atomic polarization, leading to spurious polarizations in the absence of an electric field, exacerbating violations of equipartition in the employed Carr–Parinello scheme. A suitable symmetrization of the interaction potential that correctly splits the force between the Drude core and shell can correct this shortcoming, improving the stability and numerical performance of Drude oscillator-based simulations. The symmetrization procedure is straightforward and only requires the rescaling of a few force field parameters.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Understanding Differences in Water Adsorption Isotherms: Structural Variations, Force Fields, and Monte Carlo Simulation Approaches

Accurate prediction of water adsorption in micro- and mesoporous materials with hydrophobic pores is essential for the design and characterization of advanced adsorbent materials for separation and energy applications. Here, we assess the reproducibility and consistency of water adsorption isotherms in two microporous all-silica MFI zeolite structures (MFI-K and MFI-O) using two different zeolite force fields and three simulation approaches: grand canonical Monte Carlo (GCMC), Gibbs ensemble Monte Carlo (GEMC), and transition matrix Monte Carlo (TMMC). We demonstrate that consistent treatment of the bulk fluid phase in GCMC and TMMC simulations is critical for reconciling isotherms across methods, and we construct simulation-based equations of state for the TIP4P water model to enable rigorous fugacity-to-pressure conversions. Large shifts in the isotherms are observed for two zeolite force fields developed using different parametrization strategies, with the GCS force field representing implicitly a defect-containing all-silica zeolite, whereas the TraPPE-zeo force field accurately represents an essentially defect-free all-silica zeolite. While water in the van Koningsveld structure of MFI exhibits a first-order phase transition and condensation-like step for adsorption near room temperature, water in the Olson structure of MFI displays continuous adsorption, attributed to differences in the adsorption free energy landscapes. Structural analysis reveals that small geometric variations, particularly Si–O–Si bond angles near the strongest adsorption sites, lead to these substantial differences in adsorption behavior. Furthermore, our results highlight the sensitivity of simulated water adsorption isotherms in hydrophobic frameworks to seemingly small differences in the framework structures, force field parametrization, and simulation approaches.

36 MATERIALS SCIENCE↗

Surface Reconstruction in Hydrated Amphiphilic Block Copolymer Thin Films Probed by Fluid Cell Atomic Force Microscopy

In many thin film materials, nuanced interplays of interfacial energies control the surface morphology and rearrangement. This work evaluates polymer−solvent interactions and solvent-driven surface reconstructions via ex situ and in situ fluid cell Atomic Force Microscopy (fc-AFM) analysis of amphiphilic block copolymer (BCP) thin films upon exposure to deionized (DI) water. We examine the differences in surface morphology, whole-film swelling, and force response in thin films of polystyrene-block-poly(ethylene oxide) (PS-b-PEO) and polystyrene- block-poly[(allyl glycidyl ether)-co-(ethylene oxide)] (PS-b- P[AGE-co-EO]) processed into standing-up cylinder morphologies perpendicular to a silicon substrate (⊥C). Using Amplitude Modulation AFM (AM-AFM) and Amplitude-Phase Distance (APD) force spectroscopy, this work probes the mechanoresponsive nature of the dynamic surface layers of these films, unveiling surface layer stratification and surface chain rearrangement via minimal tip−sample stimulation. To help rationalize the observed reconfigurations, the energetic driving forces were estimated using the harmonic mean approximations of interfacial energies. Given the nonionizable nature of the minority P(AGE-co-EO) block and the energetic driving forces for chain mobility, this work shows how the elimination of unfavorable PS−water interfaces drives chain rearrangement and coverage of the PS surface by chains of the hydrophilic block. This work highlights considerations for increasing the heterogeneity and complexity of BCP thin films via random blocks and how those changes to local interfacial energies may drive larger scale film morphology reconstructions, with broader implications for tuning interface hydrophilicity.

Copolymers↗

Reconciling the Driving Force and the Barrier to Charge Separation in Donor–Nonfullerene Acceptor Films

We investigate the dependence of charge yields on the driving force for photoinduced electron transfer in a series of all-small-molecule, semiconducting films made from indacenodithiophene nonfullerene acceptors (IDT NFAs). In contrast to reports of efficient, barrierless charge separation at near zero driving force for NFA-containing organic photovoltaics, we find that barrierless charge separation occurs only if the driving force is sufficient to overcome the Coulomb potential, =300 meV, based on time-resolved microwave conductivity and PL quenching measurements of 5 mmolal sensitized and 700 mmolal blended films comprising IDT NFAs paired with three different donors. This discrepancy with recent literature is caused by a difference in the way that we calculate driving force. Far from being semantic, the driving force calculation is crucial because its value controls the mechanisms needed to explain experimental observations. We provide a candid assessment of the uncertainties for our methods and popular ones used in the literature and emphasize the importance of standardizing methods across this field.

14 SOLAR ENERGY↗

Energy Budget Constraints on the Time History of Aerosol Forcing and Climate Sensitivity

Abstract An observationally constrained time series of historical aerosol effective radiative forcing (ERF) from 1750 to 2019 is developed in this study. We find that the time history of aerosol ERFs diagnosed in CMIP6 models exhibits considerable variation and explore how the time history of aerosol forcing influences the probability distributions of present‐day aerosol forcing and emergent metrics such as climate sensitivity. Using a simple energy balance model, trained on CMIP6 climate models and constrained by observed near‐surface warming and ocean heat uptake, we derive estimates for the historical aerosol forcing. We find 2005–2014 mean aerosol ERF to be −1.1 (−1.8 to −0.5) W m −2 relative to 1750. Assuming recently published historical emissions from fossil fuel and industrial sectors and biomass burning emissions from SSP2‐4.5, aerosol ERF in 2019 is −0.9 (−1.5 to −0.4) W m −2 . There is a modest recovery in aerosol forcing (+0.025 W m −2 decade −1 ) between 1980 and 2014. This analysis also gives a 5%–95% range of equilibrium climate sensitivity of 1.8°C –5.1°C (best estimate 3.1°C) with a transient climate response of 1.2°C –2.6°C (best estimate 1.8°C).

54 ENVIRONMENTAL SCIENCES↗

Little Change in Apparent Hydrological Sensitivity at Large CO 2 Forcing

Apparent hydrological sensitivity (η a ), the change in the global mean precipitation per degree K of global surface warming, is a key aspect of the climate system's response to increasing CO 2 forcing. To determine whether ηa depends on the forcing amplitude we analyze idealized experiments over a broad range of abrupt CO 2 forcing, from 2× to 8× preindustrial values, with two distinct climate models. We find little change in η a between 2× and 4×CO 2 , and almost no change beyond 5×CO 2 . We validate this finding under transient CO 2 forcing at 1%-per-year, up to 8×CO 2 . We further corroborate this result by analyzing the 1%-per-year output of more than 15 CMIP5/6 models. Lastly, we examine the 1,000-year long LongrunMIP model output, and again find little change in η a . This wealth of results demonstrates that η a is a very weak function of CO 2 forcing.

54 ENVIRONMENTAL SCIENCES↗

Frequency domain measurements of melt pool recoil force using modal analysis

Recoil pressure is a critical factor affecting the melt pool dynamics during Laser Powder Bed Fusion (LPBF) processes. Recoil pressure depresses the melt pool. When the recoil pressure is low, thermal conduction and capillary forces may be inadequate to provide proper fusion between layers. However, excessive recoil pressure can produce a keyhole inside the melt pool, which is associated with gas porosity. Direct recoil pressure measurements are challenging because it is localized over an area proportionate to the laser spot size producing a force in the mN range. This paper reports a vibrationbased approach to quantify the recoil force exerted on a part in a commercial LPBF machine. The measured recoil force is consistent with estimates from high speed synchrotron imaging of entrained particles, and the results show that the recoil force scales with applied laser power and is inversely related to the laser scan speed. These results facilitate further studies of melt pool dynamics and have the potential to aid process development for new materials.

42 ENGINEERING↗