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At least 1,369 records · Page 76

The Chocolate Chip Cookie Model: Dust Geometry of Milky Way–like Disk Galaxies

We present a new two-component dust geometry model, the Chocolate Chip Cookie model, where the clumpy nebular regions are embedded in a diffuse stellar/interstellar medium disk, like chocolate chips in a cookie. By approximating the binomial distribution of the clumpy nebular regions with a continuous Gaussian distribution and omitting the dust scattering effect, our model solves the dust attenuation process for both the emission lines and stellar continua via analytical approaches. Our Chocolate Chip Cookie model successfully fits the inclination dependence of both the effective dust reddening of the stellar components derived from stellar population synthesis and that of the emission lines characterized by the Balmer decrement for a large sample of Milky Way–like (MW-like) disk galaxies selected from the main galaxy sample of the Sloan Digital Sky Survey. Our model shows that the clumpy nebular disk is about 0.55 times thinner and 1.6 times larger than the stellar disk for MW-like galaxies, whereas each clumpy region has a typical optical depth of τ cl,V ~ 0.5 in the V band. After considering the aperture effect, our model prediction on the inclination dependence of dust attenuation is also consistent with observations. Not only that, in our model, the dust attenuation curve of the stellar population naturally depends on the inclination, and its median case is consistent with the classical Calzetti law. As the modeling constraints are from the optical wavelengths, our model is unaffected by the optically thick dust component, which however could bias the model's prediction of the infrared emissions.

79 ASTRONOMY AND ASTROPHYSICS↗

Impact of phase state and non-ideal mixing on equilibration timescales of secondary organic aerosol partitioning

Abstract. Evidence has accumulated that secondary organic aerosols (SOAs) exhibit complex morphologies with multiple phases that can adopt amorphous semisolid or glassy phase states. However, experimental analysis and numerical modeling on the formation and evolution of SOA still often employ equilibrium partitioning with an ideal mixing assumption in the particle phase. Here we apply the kinetic multilayer model of gas–particle partitioning (KM-GAP) to simulate condensation of semi-volatile species into a core–shell phase-separated particle to evaluate equilibration timescales of SOA partitioning. By varying bulk diffusivity and the activity coefficient of the condensing species in the shell, we probe the complex interplay of mass transfer kinetics and the thermodynamics of partitioning. We found that the interplay of non-ideality and phase state can impact SOA partitioning kinetics significantly. The effect of non-ideality on SOA partitioning is slight for liquid particles but becomes prominent in semisolid or solid particles. If the condensing species is miscible with a low activity coefficient in the viscous shell phase, the particle can reach equilibrium with the gas phase long before the dissolution of concentration gradients in the particle bulk. For the condensation of immiscible species with a high activity coefficient in the semisolid shell, the mass concentration in the shell may become higher or overshoot its equilibrium concentration due to slow bulk diffusion through the viscous shell for excess mass to be transferred to the core phase. Equilibration timescales are shorter for the condensation of lower-volatility species into semisolid shell; as the volatility increases, re-evaporation becomes significant as desorption is faster for volatile species than bulk diffusion in a semisolid matrix, leading to an increase in equilibration timescale. We also show that the equilibration timescale is longer in an open system relative to a closed system especially for partitioning of miscible species; hence, caution should be exercised when interpreting and extrapolating closed-system chamber experimental results to atmosphere conditions. Our results provide a possible explanation for discrepancies between experimental observations of fast particle–particle mixing and predictions of long mixing timescales in viscous particles and provide useful insights into description and treatment of SOA in aerosol models.

54 ENVIRONMENTAL SCIENCES↗

Unified understanding of the impact of semiflexibility, concentration, and molecular weight on macromolecular-scale ring diffusion

Conformationally fluctuating, globally compact macromolecules such as polymeric rings, single-chain nanoparticles, microgels, and many-arm stars display complex dynamic behaviors due to their rich topological structure and intermolecular organization. Synthetic rings are hybrid objects with conformations that display both ideal random walk and compact globular features, which can serve as models of genomic DNA. To date, emphasis has been placed on the effect of ring molecular weight on their unusual behaviors. Here, we combine simulations and a microscopic force-level theory to build a unified understanding for how key aspects of ring dynamics depend on different tunable molecular properties including backbone rigidity, monomer concentration, degree of traditional entanglement, and molecular weight. Our large-scale molecular dynamics simulations of ring melts with very different backbone stiffnesses reveal unanticipated behaviors which agree well with our generalized theory. This includes a universal master curve for center-of-mass diffusion constants as a function of molecular weight scaled by a chemistry and thermodynamic state-dependent critical molecular weight that generalizes the concept of an entanglement cross-over for linear chains. The key physics is how backbone rigidity and monomer concentration induced changes of the entanglement length, interring packing, degree of interpenetration, and liquid compressibility slow down space-time dynamic-force correlations on macromolecular scales. A power law decay of the center-of-mass diffusion constant with inverse molecular weight squared is the first consequence, followed by an ultraslow activated hopping transport regime. Our results set the stage to address slow dynamics and kinetic arrest in different families of compact synthetic and biological polymeric systems.

Science & Technology - Other Topics↗

Steric effects of central dogma processes on the compaction and segregation of bacterial nucleoids

The bacterial cytoplasm is characterized by a distinctive membrane-less organelle, the nucleoid, which harbors the chromosomal DNA. Here, we investigate the steric effects of dynamic processes associated with transcription and translation on the structure of this organelle using coarse-grained molecular dynamics simulations that incorporate out-of-equilibrium reactions. Our model captures the scale of the entire cell and incorporates a reaction-diffusion system for ribosomes and polyribosomes, coupling their nonequilibrium kinetics to DNA excluded volume interactions. Our findings demonstrate that out-of-equilibrium reactions increase the size of the nucleoid and the number of ribosomes in this subcellular region. In addition, we show that nucleoid size is proportional to transcriptional activity. Our model reproduces the time-dependent change in nucleoid size observed in rifampicin treatment experiments, where the pool of polyribosomes is depleted. Furthermore, we find that these active processes are essential for complete sister chromosome separation and correct nucleoid positioning within the cell. Overall, our study reveals the effects of the central dogma processes on the internal organization and localization of bacterial nucleoids.

Chang, Mu-Hung [Univ. of Tennessee, Knoxville, TN ↗

Effective description of ajar systems with a 𝑈⁡(1) symmetry

We introduce the concept of “ajar systems” as an intermediate case between closed and open systems, where the time scale for charge exchange with the environment is parametrically larger than all other characteristic time scales. The Schwinger-Keldysh effective action for such finite-temperature systems exhibits a symmetry group G 1 × G 2 weakly broken to its diagonal subgroup G diag , which we systematically describe using spurion techniques. For G = U(1), we calculate leading-order corrections to correlation functions in both diffusive and spontaneously broken phases. Unlike systems with approximate symmetries where both real and imaginary parts of dispersion relations receive corrections, ajar systems modify only the imaginary part—preserving gapless modes while adding finite damping.

Effective field theory↗

Avalanche gain and its effect on energy resolution in GEM-based detectors

Here, we present avalanche gain and associated resolution measurements recorded with a 4 He:CO 2 (70:30) gas mixture and pure SF 6 , a Negative Ion (NI) gas. SF 6 is of particular interest to the directional dark matter detection community, as its low thermal diffusion helps to retain recoil ionization track features over long drift lengths. With the aid of a general form of the reduced first Townsend coefficient (RFTC), multiple GEM-based detector data sets are used to study the high-gain behavior of the 4 He:CO 2 gas mixture. The high-gain data is well described purely in terms of the reduced electric field strength and the number of GEMs, and the robust relationship between the RFTC and the average, reduced, electric field strength across the GEMs is emphasized. The associated (pulse-height) resolution measurements are used to discuss the variance of the avalanche distribution and to describe and estimate the lower limits of energy resolution one should expect to measure using a simple relationship with the RFTC. In the end, a description of avalanche gain, its effect on energy resolution, and the contributing experimental parameters in GEM-based detectors is developed over a broad parameter space for further use.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Reversible Reactions, Mesh Size, and Segmental Dynamics Control Penetrant Diffusion in Ethylene Vitrimers

The diffusion of two aromatic dyes with nearly identical sizes was measured in ethylene vitrimers with precise linker lengths and borate ester cross-links using fluorescence recovery after photobleaching (FRAP). One dye possessed a reactive hydroxyl group, while the second was inert. The reaction of the hydroxyl group with the network is slow relative to the hopping times of the dye, resulting in a large slowdown by a factor of 50 for a reactive probe molecule. A kinetic model was fit to the fluorescence intensity data to determine rate constants for the reversible reaction of the dye from the network, which confirms the role of slow reaction kinetics. A second network cross-linker was also investigated with a substituted boronic ester showing ∼10,000 times faster exchange kinetics. In this system, the two dyes show the same diffusion coefficient, as the reaction is no longer the rate-limiting step. The role of dense meshes on small and large dyes is also discussed in the context of the existing theories. Finally, these results highlight the potential of dynamic networks to control penetrant transport through synergistic effects of the mesh size, dynamic bond kinetics, and penetrant–network interactions.

confinement↗

Electrochemical measurement and analysis of YCl 3 , ScCl 3 , GdCl 3 and MgCl 2 in molten eutectic LiCl-KCl

For this work, electrochemical measurements of YCl 3 , ScCl 3 , GdCl 3 and MgCl 2 were obtained in molten LiCl-KCl eutectic at 773 K using a three-electrode configuration. Tungsten rods were used as the working and counter electrodes. Two quasi- and one reference electrode(s) (glassy carbon, nickel wire, and Ni/NiO) were used to collect electrochemical measurements of the analyte salts. Cyclic voltammetry data were analyzed to calculate values of diffusion coefficient, exchange current density, and charge transfer resistance and were determined to be on the order of 10 –5 cm 2 s –1 , 10 –2 A cm –2 , and 10 0 Ω; respectively. In general, the values of diffusion coefficients were found to be consistent with those reported of high-temperature molten salts. Relatively large values of exchange current density corresponded with smaller values of charge transfer resistance. These values were found to be reasonable in comparison to results available in the literature. The measured cyclic voltammograms were normalized with respect to both lithium reduction and chloride ion oxidation potentials. Such a normalization technique is effective for comparing experimentally obtained cyclic voltammetry data to those that have been published. An analysis of experimentally obtained results indicates the relation of electrode reactions (e.g., differences of reduction potentials) are independent of the choice of reference electrode. Additionally, the choice of reference electrode did not affect the electrochemical window, exchange current density, or diffusion coefficient values.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

Effects of polarization-reversed EMIC waves on the ring current dynamics

Electromagnetic ion cyclotron (EMIC) waves are widely believed to play an important role in influencing the radiation belt and ring current dynamics. Most studies have investigated the effects or characteristics of EMIC waves by assuming their left-handed polarization. However, recent studies have found that the reversal of polarization, which occurs at higher latitudes along the wave propagation path, can change the wave-induced pitch angle diffusion coefficients. Whether such a polarization reversal can influence the global ring current dynamics remains unknown. In this study, we investigate the ring current dynamics and proton precipitation loss in association with polarization-reversed EMIC waves by using the ring current–atmosphere interactions model (RAM). The results indicate that the polarization reversal of H-band EMIC waves can truly decrease the scattering rates of protons of 10 to 50 keV or >100 keV in comparison with the scenario in which the EMIC waves are considered purely left-handed polarized. Additionally, the global ring current intensity and proton precipitation may be slightly affected by the polarization reversal, especially during prestorm time and the recovery phase, but the effects are not large during the main phase. This is probably because the H-band EMIC waves contribute to the proton scattering loss primarily at E < 10 keV, an energy range that is not strongly affected by the polarization reversal.

79 ASTRONOMY AND ASTROPHYSICS↗

Reaction dynamics and in-medium nucleon-nucleon cross section with 12 C+ 1 H at 95 MeV/nucleon

Reaction dynamics and effective in-medium nucleon-nucleon (NN) cross section are studied, using the antisymmetrized molecular dynamics (AMD) model with one of the simplest heavy ion collisions, 12 C+ ⁢1 H. The roles of different stochastic processes are studied, which are installed in the original AMD. One is the diffusion process as a part of the quantum fluctuation originated from the Fermi motion during the time evolution of the wave packets in the mean field (AMD/D). The second is a coalescence treatment for light clusters with A ≤ 8 (AMD/D-COALS). The third is the collision process, installed in AMD with different form of the in-medium NN cross sections. These different processes are examined, using the experimental angular distributions and energy spectra of light charged particles and intermediate mass fragments. The effective in-medium NN cross sections are evaluated from the simulated AMD events and compared with the experimentally extracted values. A good agreement is obtained between the AMD values from the 12 C + 1 H reaction at 95 MeV/nucleon and the experimental results for nuclear matter.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

The effects of dose, dose rate, and irradiation type and their equivalence on radiation-induced segregation in binary alloy systems via phase-field simulations

Radiation-induced segregation is a phenomenon commonly observed in many alloys which consists of the redistribution of elements (solute or interstitial impurities) under irradiation. The onset and development of radiation-induced segregation can only occur when a sufficient flux of defects is sustained and defect sinks are present. Irradiation dose, dose rate, and particle types all affect defect flux. In this work, we employ a phase-field model to examine the effects of dose, dose rate, and type of incident particles on radiation-induced segregation behavior in a model binary alloy. The phase-field model takes into account the formation and evolution of point defects as well as defect clusters, the diffusion and clustering of alloy species, the presence of additional extrinsic defect sinks in the form of dislocations, and two different methods of radiation-damage insertion, which are intended to simulate either light-ion/electron irradiation via Frenkel pairs or heavy-ion irradiation in the form of cascades. Our results show a dose-rate and particle-type dependence on the amount of solute segregation. We show that the material systems exposed to higher dose rates are less subjected to solute segregation at equivalent doses. We also show that such dose-rate-dependence behavior is due to a delay of the incubation dose at which radiation-induced segregation effectively starts. Particle type and the presence of dislocations can accentuate this behavior. Our model predictions correlate with many experimental observations made over the years on radiation-induced segregation providing credence to the simulation results. The methodology presented in this study allows for a first-order prediction of the dose rate at which proxy irradiation experiments could be performed to approximate radiation-induced segregation behaviors seen in targeted irradiation conditions.

36 MATERIALS SCIENCE↗

Low Temperature Water-Gas Shift: Enhancing Stability through Optimizing Rb Loading on Pt/ZrO 2

Recent studies have shown that appropriate levels of alkali promotion can significantly improve the rate of low-temperature water gas shift (LT-WGS) on a range of catalysts. At sufficient loadings, the alkali metal can weaken the formate C–H bond and promote formate dehydrogenation, which is the proposed rate determining step in the formate associative mechanism. In a continuation of these studies, the effect of Rb promotion on Pt/ZrO 2 is examined herein. Pt/ZrO 2 catalysts were prepared with several different Rb loadings and characterized using temperature programmed reduction mass spectrometry (TPR-MS), temperature programmed desorption (TPD), diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS), an X-ray absorption near edge spectroscopy (XANES) difference procedure, extended X-ray absorption fine structure spectroscopy (EXAFS) fitting, TPR-EXAFS/XANES, and reactor testing. At loadings of 2.79% Rb or higher, a significant shift was seen in the formate ν(CH) band. The results showed that a Rb loading of 4.65%, significantly improves the rate of formate decomposition in the presence of steam via weakening the formate C–H bond. However, excessive rubidium loading led to the increase in stability of a second intermediate, carbonate and inhibited hydrogen transfer reactions on Pt through surface blocking and accelerated agglomeration during catalyst activation. Optimal catalytic performance was achieved with loadings in the range of 0.55–0.93% Rb, where the catalyst maintained high activity and exhibited higher stability in comparison with the unpromoted catalyst.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

The Effect of Large-scale Magnetic Fluctuations on Energetic Particle Profiles across Interplanetary Shocks

In situ observations of energetic particles associated with interplanetary (IP) shocks, known as energetic storm particle (ESP) events, often show time-intensity profiles quite different from predictions of classical diffusive shock acceleration theory. We use numerical simulations, including test-particle simulations and hybrid simulations (with fluid electrons and kinetic protons) for shocks propagating into a turbulent magnetic field to study the ESP intensity-time profiles across a strong IP shock. We find that several types of energetic particle intensity profiles similar to in situ observations can be produced in our simulations. The peak of energetic particle count is often near, but can be shifted from, the locations of the shock front, with the peak usually being observed downstream of the shock. These findings may help understand particle acceleration at both traveling IP shocks and shocks in other heliospheric and astrophysical environments.

Lo, Ming-Yuan [New Mexico Consortium (NMC), Los Al↗

Pulsating Poiseuille flow of a cement slurry

In this paper, we investigate the pulsatile flow of a cement slurry in a pipe. The constitutive relation for the viscous stress tensor is based on the power-law model, where the shear viscosity not only depends on the shear rate but also the volume fraction of the cement particles. To solve for the volume fraction field, a convection-diffusion equation is used. The dimensionless form of the governing equations and the boundary conditions are solved numerically at different pulsatile cycles. Further, a parametric study is conducted to study the effect of different dimensionless numbers at different cycles on the velocity and the volume fraction profiles.

36 MATERIALS SCIENCE↗

Gradient microstructure induced shear band constraint, delocalization, and delayed failure in CuZr nanoglasses

The mechanical properties of metallic glasses (MGs) can be significantly tuned by introducing a nanoscale glass-glass interface microstructure. Here, we design three types of Cu 64 Zr 36 MG seamless gradient microstructures by combining glassy grain sizes from 3 to 15 nm. We perform tensile loading molecular dynamics simulations on the named gradient nanoglasses to characterize their mechanical behavior. In all cases, results indicate the generation of gradient plasticity following the gradient in grain size, i.e. local plasticity increases from large to small grain size regions. Loading parallel to the gradient direction results in initial broad necking followed by catastrophic failure. In contrast, loading perpendicular to the gradient direction results in diffused shear band propagation from large to small grain size regions, delaying the generation of a dominant shear band and further delocalizing plastic deformation. In conclusion, the results demonstrate the synergistic effects generated by heterogeneous gradient designs in the mechanical behavior of metallic glasses.

36 MATERIALS SCIENCE↗

Sputtered indium tin oxide as a recombination layer formed on the tunnel oxide/poly-Si passivating contact enabling the potential of efficient monolithic perovskite/Si tandem solar cells

We focus on utilizing sputtered indium tin oxide (ITO) as a recombination layer, having low junction damage to an n-type silicon solar cell with a front-side tunnel oxide passivating electron contact, thereby enabling the development of a high efficiency monolithic perovskite/Si tandem device. High transparency and low resistivity ITO films are deposited via low power DC magnetron sputtering at room temperature onto a front-side thin SiO x /n + poly-Si contact in a complete Cz n-Si cell with a back-side Al 2 O 3 /SiN x passivating boron-diffused p + -emitter on a random pyramid textured surface. We report the cell characteristics before and after ITO sputtering, and we find a cure at 250 °C in air is highly effective at mitigating any sputtering induced damage. Our ITO coated sample resulted in an implied open-circuit voltage (iV oc ) of 684.7 ± 11.3 mV with the total saturation current density of 49.2 ± 14.8 fA/cm 2 , an implied fill factor (iFF) of 81.9 ± 0.8%, and a contact resistivity in the range of 60 mΩ-cm 2 to 90 mΩ-cm 2 . After formation of a local Ag contact to the rear emitter and sputtered ITO film as the front-side contact without grid fingers, the pseudo-efficiency of 20.2 ± 0.5% was obtained with the V oc of 670.4 ± 7 mV and pseudo FF of 77.3 ± 1.3% under simulated one sun with the calculated short-circuit current density of 30.9 mA/cm 2 from the measured external quantum efficiency. Furthermore, our modelling result shows that efficiency exceeding 25% under one sun is practically achievable in perovskite/Si tandem configuration using the ITO recombination layer connecting a perovskite top cell and a poly-Si bottom cell.

14 SOLAR ENERGY↗

Dissolved CO 2 Modulates the Electrochemical Capacitance on Gold Electrodes

The presence of CO 2 at an electrified interface between an aqueous electrolyte and a metal electrode is the prerequisite for many electrochemical CO 2 capture technologies. To understand the behavior of dissolved CO 2 at an aqueous electrified interface, we characterized the electrochemical interface of planar gold electrodes with cyclic voltammetry, electrochemical impedance spectroscopy (EIS), electrochemical surface plasmon resonance (EC–SPR), and attenuated total reflectance surface-enhanced infrared spectroscopy (ATR–SEIRAS). Under all investigated conditions, we observed a decrease in the electrochemical capacitance upon saturation of the electrolyte with CO 2 , as compared to an electrolyte saturated with Ar. EIS and EC–SPR showed that this capacitance reduction was also potential dependent: it reached a minimum near the point of zero charge and became more significant as the applied potential moved further away from the point of zero charge. Hybrid quantum–classical simulations of the gold/aqueous electrolyte interface indicate that bicarbonate decreases the capacitance and modifies the composition of the electric double layer. In addition to the binding of bicarbonate under positive bias, we propose that molecular CO 2 can be induced by applied potential to concentrate in the diffuse layer of the electric double layer, leading to a reduction in the electrochemical capacitance under both negative and positive bias. Furthermore, this work advances the understanding of non-Faradaic effects of dissolved CO 2 at aqueous electrified interfaces of relevance for electrochemical CO 2 capture.

25 ENERGY STORAGE↗

Hydrodynamics in long-range interacting systems with center-of-mass conservation

In systems with a conserved density, the additional conservation of the center of mass (dipole moment) has been shown to slow down the associated hydrodynamics. At the same time, long-range interactions generally lead to faster transport and information propagation. Here, we explore the competition of these two effects and develop a hydrodynamic theory for long-range center-of-mass-conserving systems. Here we demonstrate that these systems can exhibit a rich dynamical phase diagram containing subdiffusive, diffusive, and superdiffusive behaviors, with continuously varying dynamical exponents. We corroborate our theory by studying quantum lattice models whose emergent hydrodynamics exhibit these phenomena.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗