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At least 595 records · Page 33

Highly uniform, multi-stacked InGaAs/GaAs quantum dots embedded in a GaAs nanowire

We demonstrate a highly uniform, dense stack of In{sub 0.22}Ga{sub 0.78}As/GaAs quantum dot (QD) structures in a single GaAs nanowire (NW). The size (and hence emission energy) of individual QD is tuned by careful control of the growth conditions based on a diffusion model of morphological evolution of NWs and optical characterization. By carefully tailoring the emission energies of individual QD, dot-to-dot inhomogeneous broadening of QD stacks in a single NW can be as narrow as 9.3 meV. This method provides huge advantages over traditional QD stack using a strain-induced Stranski-Krastanow growth scheme. We show that it is possible to fabricate up to 200 uniform QDs in single GaAs NWs using this growth technique without degradation of the photoluminescence intensity.

77 NANOSCIENCE AND NANOTECHNOLOGY↗

Evolving radon diffusion through earthen barriers at uranium waste disposal sites

Field measurements of Rn-222 fluxes from the tops and bottoms of compacted clay radon barriers were used to calculate effective Rn diffusion coefficients (D Rn ) at four uranium waste disposal sites in the western United States to assess cover performance after more than 20 years of service. Values of D Rn ranged from 7.4 × 10 -7 to 6.0 × 10 -9 m 2 /s, averaging 1.42 × 10 -7 . Water saturation (S W ) from soil cores indicated that there was relatively little control of D Rn by S W , especially at higher moisture levels, in contrast to estimates from most steady-state diffusion models. Further, this is attributed to preferential pathways intrinsic to construction of the barriers or to natural process that have developed over time including desiccation cracks, root channels, and insect burrows in the engineered earthen barriers. A modification to some models in which fast and slow pathway D Rn values are partitioned appears to give a good representation of the data; 4% of the fast pathway was needed to fit the data regression. For locations with high S w and highest D Rn (and fluxes) at each site, the proportion of fast pathway ranged from 1.7% to 34%, but for many locations with lower fluxes, little if any fast pathway was needed.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Enhanced performance of quantum dot solar cells based on type II quantum dots

The characteristics of quantum dot solar cells (QDSCs) based on type II QDs are investigated theoretically. Based on a drift-diffusion model, we obtained a much higher open circuit voltage (V{sub oc}) as well as conversion efficiency in a type II QDSC, compared to type I QDSCs. The improved V{sub oc} and efficiency are mainly attributed to the much longer Auger recombination lifetime in type II QDs. Moreover, the influence of the carrier lifetime on devices' performance is discussed and clarified. In addition, an explicit criterion to determine the role of quantum dots in solar cells is put forward.

75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND↗

Measurement and simulation of top- and bottom-illuminated solar-blind AlGaN metal-semiconductor-metal photodetectors with high external quantum efficiencies

A comprehensive study on top- and bottom-illuminated Al{sub 0.5}Ga{sub 0.5}N/AlN metal-semiconductor-metal (MSM) photodetectors having different AlGaN absorber layer thickness is presented. The measured external quantum efficiency (EQE) shows pronounced threshold and saturation behavior as a function of applied bias voltage up to 50 V reaching about 50% for 0.1 μm and 67% for 0.5 μm thick absorber layers under bottom illumination. All experimental findings are in very good accordance with two-dimensional drift-diffusion modeling results. By taking into account macroscopic polarization effects in the hexagonal metal-polar +c-plane AlGaN/AlN heterostructures, new insights into the general device functionality of AlGaN-based MSM photodetectors are obtained. The observed threshold/saturation behavior is caused by a bias-dependent extraction of photoexcited holes from the Al{sub 0.5}Ga{sub 0.5}N/AlN interface. While present under bottom illumination for any AlGaN layer thickness, under top illumination this mechanism influences the EQE-bias characteristics only for thin layers.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Calculation of the evaporation residue cross sections for the synthesis of the superheavy element Z=119 via the {sup 50}Ti+{sup 249}Bk hot fusion reaction

The evaporation residue (ER) cross sections for 3n and 4n evaporation channels in the {sup 50}Ti + {sup 249}Bk reaction leading the formation of {sup 296}119 and {sup 295}119 isotopes are evaluated by means of a modified fusion-by-diffusion model. In the model, the dynamic evolution from dinucleus to mononucleus is taken into account with the two-dimensional coupled Langenvin equations. The calculated maximum ER cross sections in 3n and 4n evaporation channels of the {sup 50}Ti + {sup 249}Bk reaction are 0.17 and 0.57 pb, respectively. The cross section of 0.57 pb is close to the present experimental limit for the registration of the evaporation residual nuclei. Therefore, superheavy element 119 may be the most hopeful new element with Z>118 to be synthesized under somehow improved experimental conditions in the near future.

73 NUCLEAR PHYSICS AND RADIATION PHYSICS↗

Development of Corrosion Resistant Coatings for Structural Materials for Liquid Fueled Molten Salts Reactors Applications (Final Report)

Current structural alloys, code certified for the MSRs temperature ranges, contain high levels of chromium, making them highly susceptible to molten halide salt corrosion. One potential solution to circumvent the need for code certification of novel alloys, which is expensive and time consuming, is to design claddings that will protect the underlying code certified materials from corrosion damage during operation. In this work, we examined the corrosion of Ni and Cu electroplated, Ni and CuNi weld overlay, Mo-laser clad, and carburized claddings on SS316H for use in molten salt reactor environments. After characterization of the cladded materials (Task 1), static corrosion tests were used to assess corrosion resistance of the claddings in typical molten fluoride salts (Task 2). The corrosion tests were performed in molten FLiNaK at 700°C up to 1000 hours. Pre- and post-corrosion Scanning Electron Microscopy (SEM), energy-dispersive-spectroscopy (EDS), Transmission Electron Microscopy (TEM), X-ray Diffraction (XRD) and glow-discharge-optical-emission-spectroscopy (GDOES) were performed on cladding cross-sections and surfaces to evaluate degradation. The Cu and Ni electroplated samples, as well as the carburized samples, showed excellent corrosion resistance relative to the bare SS316H. To assess high temperature cladding stability, ageing experiments were performed at temperatures up to 900 C in inert atmosphere for the electroplated and carburized samples and a diffusion model was developed to predict long term cladding behavior (Task 3). It was found that the Cu cladding was basically insensitive to the high temperature ageing, except for small secondary phases forming at the interface. On the other hand, the Ni electroplated cladding experienced significant interdiffusion. Nevertheless, the gain in corrosion resistance for a 100μm Ni electroplated cladding is phenomenal, with more than 50% reduction in chromium dissolution from the substrate material for the first 15 years of salt exposure at 700°C. To assess radiation resistance and phase stability, high-temperature 4MeV Ni heavy ion irradiation was performed across the cladding/substrate interface up to 50 displacement-per-atom (DPA) at 500°C and 700°C to assess the phase stability and irradiation behaviors of the electroplated systems (Task 4). The Ni and Cu electroplated systems did not experience void swelling at the contrary to the SS316H substrate due to their nanocrystalline nature. Some level of recrystallization was observed in the cladding, as well as radiation induced segregation and enhanced diffusion. The interface acted as a potent sink for point defects with the presence of a void denuded zone. The mechanical properties of the claddings were assessed using thermal shock, micro-indentation, nano-indentation, and four-point bend testing experiments (Task 5). These experiments were performed on the claddings in as-received, corroded, irradiated, and thermally aged states to determine the effects of typical molten salt reactor environments on cladding integrity. No significant mass loss was observed after repeated thermal shocks. While the electroplated samples softened after high-temperature ageing, irradiation hardening compensate this effect, such that there is little different with the as-received materials. The results of these experiments suggest that the electroplated (copper/nickel) show the greatest promise for application in molten salt reactor development. These claddings prevented any chromium dissolution from occurring during the static corrosion experiments. Additionally, they demonstrated favorable properties for high temperature diffusion, phase stability, interfacial mechanical properties, and irradiation resistance. Weld-overlay cladding are also of great interest and could reach properties similar to the electroplated samples upon optimization (especially with multiple weld passes). The carburized SS316H showed excellent behavior as well, but more work needs to be done to assess their long-term stability. Finally, the Mo-laser clad system was not pursued further due to the manufacturing challenges. It is also worth noting that the Ni cladding systems should behave relatively well in terms of weldability since the Ni-weld overlay microstructure and associated corrosion rate are sound. While the NiCu weld-overlay has even lower corrosion rates than the Ni-weld overlay, more studies on welding of Cu-electroplated systems are necessary since Cu clusters are known to embrittle steels.

36 MATERIALS SCIENCE↗

Nucleation and structural growth of cluster crystals

We study the nucleation of crystalline cluster phases in the generalized exponential model with exponent n = 4. Due to the finite value of this pair potential for zero separation, at high densities the system forms cluster crystals with multiply occupied lattice sites. Here, we investigate the microscopic mechanisms that lead to the formation of cluster crystals from a supercooled liquid in the low-temperature region of the phase diagram. Using molecular dynamics and umbrella sampling, we calculate the free energy as a function of the size of the largest crystalline nucleus in the system, and compare our results with predictions from classical nucleation theory. Employing bond-order parameters based on a Voronoi tessellation to distinguish different crystal structures, we analyze the average composition of crystalline nuclei. We find that even for conditions where a multiply occupied fcc crystal is the thermodynamically stable phase, the nucleation into bcc cluster crystals is strongly preferred. Furthermore, we study the particle mobility in the supercooled liquid and in the cluster crystal. In the cluster crystal, the motion of individual particles is captured by a simple reaction-diffusion model introduced previously to model the kinetics of hydrogen bonds.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Physical and mechanical metallurgy of zirconium alloys for nuclear applications: a multi-scale computational study

In the post-Fukushima world, the stability of materials under extreme conditions is an important issue for the safety of nuclear reactors. Because the nuclear industry is going to continue using advanced zirconium cladding materials in the foreseeable future, it become critical to gain fundamental understanding of the several interconnected problems. First, what are the thermodynamic and kinetic factors affecting the oxidation and hydrogen pick-up by these materials at normal, off-normal conditions, and in long-term storage? Secondly, what protective coatings (if any) could be used in order to gain extremely valuable time at off-normal conditions, e.g., when temperature exceeds the critical value of 2200°F? Thirdly, the kinetics of oxidation of such protective coating or braiding needs to be quantified. Lastly, even if some degree of success is achieved along this path, it is absolutely critical to have automated inspection algorithms allowing identifying defects of cladding as soon as possible. This work strives to explore these interconnected factors from the most advanced computational perspective, utilizing such modern techniques as first-principles atomistic simulations, computational thermodynamics of materials, diffusion modeling, and the morphological algorithms of image processing for defect identification. Consequently, it consists of the four parts dealing with these four problem areas preceded by the introduction and formulation of the studied problems. In the 1st part an effort was made to employ computational thermodynamics and ab initio calculations to shed light upon the different stages of oxidation of ziraloys (2 and 4), the role of microstructure optimization in increasing their thermal stability, and the process of hydrogen pick-up, both in normal working conditions and in long-term storage. The 2nd part deals with the need to understand the influence and respective roles of the two different plasticity mechanisms in Zr nuclear alloys: twinning (at low T) and crystallographic slip (higher T’s). For that goal, a description of the advanced plasticity model is outlined featuring the non-associated flow rule in hcp materials including Zr. The 3rd part describes the kinetic theory of oxidation of the several materials considered to be perspective coating materials for Zr alloys: SiC and ZrSiO 4 . In the 4th part novel and advanced projectional algorithms for defect identification in zircaloy coatings are described. In so doing, the author capitalized on some 12 years of his applied industrial research in this area. Our conclusions and recommendations are presented in the 5th part of this work, along with the list of used literature and the scripts for atomistic, thermodynamic, kinetic, and morphological computations.

36 MATERIALS SCIENCE↗

Report on the AAPM grand challenge on deep generative modeling for learning medical image statistics

Abstract Background The findings of the 2023 AAPM Grand Challenge on Deep Generative Modeling for Learning Medical Image Statistics are reported in this Special Report. Purpose The goal of this challenge was to promote the development of deep generative models for medical imaging and to emphasize the need for their domain‐relevant assessments via the analysis of relevant image statistics. Methods As part of this Grand Challenge, a common training dataset and an evaluation procedure was developed for benchmarking deep generative models for medical image synthesis. To create the training dataset, an established 3D virtual breast phantom was adapted. The resulting dataset comprised about 108 000 images of size 512 512. For the evaluation of submissions to the Challenge, an ensemble of 10 000 DGM‐generated images from each submission was employed. The evaluation procedure consisted of two stages. In the first stage, a preliminary check for memorization and image quality (via the Fréchet Inception Distance [FID]) was performed. Submissions that passed the first stage were then evaluated for the reproducibility of image statistics corresponding to several feature families including texture, morphology, image moments, fractal statistics, and skeleton statistics. A summary measure in this feature space was employed to rank the submissions. Additional analyses of submissions was performed to assess DGM performance specific to individual feature families, the four classes in the training data, and also to identify various artifacts. Results Fifty‐eight submissions from 12 unique users were received for this Challenge. Out of these 12 submissions, 9 submissions passed the first stage of evaluation and were eligible for ranking. The top‐ranked submission employed a conditional latent diffusion model, whereas the joint runners‐up employed a generative adversarial network, followed by another network for image superresolution. In general, we observed that the overall ranking of the top 9 submissions according to our evaluation method (i) did not match the FID‐based ranking, and (ii) differed with respect to individual feature families. Another important finding from our additional analyses was that different DGMs demonstrated similar kinds of artifacts. Conclusions This Grand Challenge highlighted the need for domain‐specific evaluation to further DGM design as well as deployment. It also demonstrated that the specification of a DGM may differ depending on its intended use.

Radiology, Nuclear Medicine & Medical Imaging↗

Mechanism of heat-modification inside a glass after irradiation with high-repetition rate femtosecond laser pulses

Accumulation of thermal energies by highly repeated irradiation of femtosecond laser pulses inside a glass induces the heat-modification whose volume is much larger than that of the photoexcited region. It has been proposed that the heat-modification occurs in the region in which the temperature had overcome a threshold temperature during exposure of laser pulses. In order to understand the mechanism of the heat-modification, we investigated the temperature distribution during laser exposure and the threshold temperature by analyzing the volume of the modification based on a thermal diffusion model. We found that the threshold temperature becomes lower with increasing laser exposure time. The dependence of the threshold temperature on the laser exposure time was explained by the deformation mechanism based on the temperature-dependent viscosity and viscoelastic behavior of a glass under a stress loading by thermal expansion. The deformation mechanism also could simulate a tear-drop shape of a heat-modification by simultaneous double-beams' irradiation and the distribution of birefringence in a heat-modification. The mechanism proposed in this study means that the temperature-dependence of the viscosity of a glass should be essential for predicting and controlling the heat-modification.

36 MATERIALS SCIENCE↗

Computational diagnostics for flame acceleration and transition to detonation in a hydrogen/air mixture

A new computational diagnostic method for pressure-induced compressibility is proposed by projecting its local contribution to the chemical explosive mode (CEM) in the chemical explosive mode analysis (CEMA) framework. The new method is validated for the study of detonation development during the deflagration-to-detonation transition (DDT) process. The flame characteristics are identified through the quantification of individual CEM contributions of chemical reaction, diffusion, and pressure-induced compressibility. Numerical simulations are performed to investigate the DDT processes in a stoichiometric hydrogen-air mixture. A Godunov algorithm, fifth-order in space, and third-order in time are used to solve the fully compressible Navier-Stokes equations on a dynamically adapting mesh. A single-step, calibrated chemical diffusive model (CDM) described by Arrhenius kinetics is used for energy release and conservation between the fuel and the product. The new diagnostic method is first applied to onedimensional (1D) canonical flame configurations followed by two-dimensional (2D) simulations of DDT in an obstructed channel where different detonation initiation scenarios are examined using the new CEMA projection formulation. Detailed examinations of the idealized configuration of detonation initiation through shock focusing mechanism at a flame front are also studied using the new formulation. A comparison of the currently proposed CEMA projection and the original formulation by the authors suggests that including the pressure-induced compressibility is essential for the use of CEMA in DDT process. The results also show that the new formulation of CEMA projection can successively capture the detonation initiation through either a gradient mechanism or a direct initiation mechanism, and therefore can be used as an effective local analytical tool for the computational diagnostics of detonation initiation in a DDT process. It was found that detonation development is characterized by a strong contribution of chemistry role to the CEM which is pivotal to the initiation of detonation. The role of compressibility is found enhanced at the edge of the detonation front where diffusion was found to have minimal effects on detonation development.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Numerical studies of transient gain reduction process in a multi-wire proportional chamber

A gain reduction process caused by successive beam irradiation in a multi-wire proportional chamber was numerically investigated to clarify the relations between the gas gain variation and the ion density distribution. A numerical code was developed based on a two-dimensional drift-diffusion model in order to evaluate the ion and electron density distributions and the electric field variation caused by the space charge effect. In order to consider the gain reduction process which occurs under the high rate and successive irradiation, the simulations were performed for the time period of {approx}10-100 {mu}s, which is much longer than the time required for ions to travel from an anode to a cathode. The numerical simulation results showed that for the low gas gain regime of {approx}10, quasi-stationary density distribution of the ions was formed by the high-rate beams of {approx}10{sup 8}- 10{sup 10} particles per second, and that the transient variation of the gas gain became constant after establishment of the quasi-stationary ion density distributions.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

SUPERLUMINOUS LIGHT CURVES FROM SUPERNOVAE EXPLODING IN A DENSE WIND

Observations from the last decade have indicated the existence of a general class of superluminous supernovae (SLSNe), in which the peak luminosity exceeds 10{sup 44} erg s{sup -1}. Here we focus on a subclass of these events, where the light curve is also tens of days wide, so the total radiated energy is of order 10{sup 51} erg. If the origin of these SLSNe is a core-collapse-driven explosion of a massive star, then the mechanism that converts the explosion energy into radiation must be very efficient (much more than in typical core-collapse SNe, where this efficiency is of order 1%). We examine the scenario where the radiated luminosity is due to efficient conversion of kinetic energy of the ejected stellar envelope into radiation by interaction with an optically thick, pre-existing circumstellar material, presumably the product of a steady wind from the progenitor. We base the analysis on analytical derivations of various limits, and on a simple, numerically solved, hydrodynamic diffusion model, which allows us to explore the regime of interest, which does not correspond to the analytical limits. In our results, we identify the qualitative behavior of the observable light curves, and relate them to the parameters of the wind. We specifically show that a wide and superluminous supernova requires the mass of the relevant wind material to be comparable to that of the ejected material from the exploding progenitor. We find the wind parameters that explain the peak luminosity and width of the bolometric light curves of three particular SLSNe, namely, SN 2005ap, SN 2006gy, and SN 2010gx, and show that they are best fitted with a wind that extends to a radius of order 10{sup 15} cm. These results serve as an additional indication that at least some SLSNe may be powered by interaction of the ejected material with a steady wind of similar mass.

79 ASTRONOMY AND ASTROPHYSICS↗

The interaction of high-speed turbulence with flames: Turbulent flame speed

Direct numerical simulations of the interaction of a premixed flame with driven, subsonic, homogeneous, isotropic, Kolmogorov-type turbulence in an unconfined system are used to study the mechanisms determining the turbulent flame speed, S{sub T}, in the thin reaction zone regime. High intensity turbulence is considered with the r.m.s. velocity 35 times the laminar flame speed, S{sub L}, resulting in the Damkoehler number Da=0.05. The simulations were performed with Athena-RFX, a massively parallel, fully compressible, high-order, dimensionally unsplit, reactive-flow code. A simplified reaction-diffusion model, based on the one-step Arrhenius kinetics, represents a stoichiometric H{sub 2}-air mixture under the assumption of the Lewis number Le=1. Global properties and the internal structure of the flame were analyzed in an earlier paper, which showed that this system represents turbulent combustion in the thin reaction zone regime. This paper demonstrates that: (1) The flame brush has a complex internal structure, in which the isosurfaces of higher fuel mass fractions are folded on progressively smaller scales. (2) Global properties of the turbulent flame are best represented by the structure of the region of peak reaction rate, which defines the flame surface. (3) In the thin reaction zone regime, S{sub T} is predominantly determined by the increase of the flame surface area, A{sub T}, caused by turbulence. (4) The observed increase of S{sub T} relative to S{sub L} exceeds the corresponding increase of A{sub T} relative to the surface area of the planar laminar flame, on average, by {approx}14%, varying from only a few percent to as high as {approx}30%. (5) This exaggerated response is the result of tight flame packing by turbulence, which causes frequent flame collisions and formation of regions of high flame curvature >or similar 1/{delta}{sub L}, or ''cusps,'' where {delta}{sub L} is the thermal width of the laminar flame. (6) The local flame speed in the cusps substantially exceeds its laminar value, which results in a disproportionately large contribution of cusps to S{sub T} compared with the flame surface area in them. (7) A criterion is established for transition to the regime significantly influenced by cusp formation. In particular, at Karlovitz numbers Ka >or similar 20, flame collisions provide an important mechanism controlling S{sub T}, in addition to the increase of A{sub T} by large-scale motions and the potential enhancement of diffusive transport by small-scale turbulence. (author)

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Curvature effects in the reaction-diffusion system governing frontal polymerization

Frontal polymerization is a fast and energy-efficient curing process of thermoset polymers involving the self-sustained propagation of a sharp front that transforms a liquid monomer or gel into a polymer. The temperature, speed, and geometry of the polymerization front are closely intertwined quantities that can affect the curing process and the mechanical properties of the polymer. This work investigates the effect of the front curvature on the front propagation speed based on a reaction-diffusion model. The proposed analytical relations between front speed and curvature are verified by finite element simulations and validated through experiments. The models show that a concave front has a higher front temperature and speed than its convex counterpart. When the curvature of a convex front reaches a critical value, the reaction can no longer be sustained, and the front is quenched. The relation between the speed of a steadily propagating front and its geometry is derived, showing good agreement with experimental observations. This study also provides analytical estimates of the thickness of the polymerization front and insight into the relationship between the front curvature and the kinetics of the exothermic reaction.

42 ENGINEERING↗

Increasing the solar photovoltaic energy capture on sunny and cloudy days

This report analyzes an extensive set of measurements of the solar irradiance made using four identical solar arrays and associated solar sensors (collectively referred to as solar collectors) with different tilt angles relative to the earth's surface, and thus the position of the sun, in order to determine an optimal tracking algorithm for capturing solar radiation. The study included a variety of ambient conditions including different seasons and both cloudy and cloud-free conditions. One set of solar collectors was always approximately pointed directly toward the sun (DTS) for a period around solar noon. These solar collectors thus captured the direct beam component of the solar radiation that predominates on sunny days. We found that on sunny days, solar collectors with a DTS configuration captured more solar energy in accordance with the well-known cosine dependence for the response of a flat-surfaced solar collector to the angle of incidence with direct beam radiation. In particular, a DTS orientation was found to capture up to twice as much solar energy as a horizontal (H) orientation in which the array is tilted toward the zenith. Another set of solar collectors always had an H orientation, and this best captured the diffuse component of the solar radiation that predominates on cloudy days. The dependence of the H/DTS ratio on the solar-collector tilt angle was in approximate agreement with the Isotropic Diffuse Model derived for heavily overcast conditions. During cloudy periods, we found that an H configuration increased the solar energy capture by nearly 40% compared to a DTS configuration during the same period, and we estimate the solar energy increase of an H configuration over a system that tracks the obscured solar disk could reach 50% over a whole heavily-overcast day. On an annual basis the increase is predicted to be much less, typically only about 1%, because the contribution of cloudy days to the total annual solar energy captured by a photovoltaic system is small. These results are consistent with the solar tracking algorithm optimized for cloudy conditions that we proposed in an earlier report and that was based on a much smaller data set. Improving the harvesting of solar energy on cloudy days deserves wider attention due to increasing efforts to utilize renewable solar energy. In particular, increasing the output of distributed solar power systems on cloudy days is important to developing solar-powered home fueling and charging systems for hydrogen-powered fuel-cell electric and battery-powered vehicles, respectively, because it reduces the system size and cost for solar power systems that are designed to have sufficient energy output on the worst (cloudy) days. (author)

14 SOLAR ENERGY↗

Equilibrium Fe isotope fractionation between olivine, pyroxene, spinel and MORB glass: Implications for mantle partial melting to generate MORBs

Primitive mid-ocean ridge basalts (MORBs) exhibit Fe isotopic compositions heavier than the upper mantle by +0.074 ± 0.028 ‰ for δ 56 Fe. The processes responsible for this isotopic difference remain unclear. Modeling of Fe isotope fractionation during mantle partial melting requires reliable equilibrium Fe isotope fractionation factors between minerals and melts, for which consistent data are still lacking. Here, in this study, we used Nuclear Resonant Inelastic X-ray Scattering (NRIXS) technique to measure Fe force constants for a MORB glass (ALV 519-4-1) and natural mantle minerals (olivine, orthopyroxene, clinopyroxene, and spinel) to determine the equilibrium Fe isotope fractionation factors between them. The force constants determined in this study, in increasing order, are 167 ± 26 N/m for spinel, 175 ± 17 N/m for olivine, 176 ± 20 N/m for MORB glass, 205 ± 26 N/m for clinopyroxene, and 219 ± 36 N/m for orthopyroxene. We evaluated the previously proposed mechanisms for the heavy Fe isotopic composition of MORBs, including (i) mantle partial melting, (ii) mantle lithological heterogeneity, with pyroxenite in the source, (iii) mantle metasomatism by low-degree melts, and (iv) fractional crystallization of olivine from melts. For (i), we used the pMELTS program to simulate adiabatic decompression melting of mantle peridotites, and calculated Fe isotope fractionation based on Fe 3+ –Fe 2+ equilibrium-controlled fractionation, where Fe 3+ forms stronger bonds and is more incompatible than Fe 2+ . At 10 wt% peridotite melting, corresponding to MORB generation, only +0.03 ‰ Fe isotope fractionation between the melt and the original bulk composition (Δ 56 Fe = δ 56 Fe melt - δ 56 Fe 0 ) was produced, insufficient to account for the observed MORB-upper mantle difference. For (ii), melting of pyroxenites yields smaller Fe isotope fractionation than melting of peridotites, making it unlikely the cause for the MORB-upper mantle isotopic difference. For (iii), both the Fe 3+ /ΣFe ratio and the δ 56 Fe of melts increase with the degree of partial melting, indicating that low-degree melts are not isotopically heavy enough to significantly alter the isotopic composition of lithospheric mantle through metasomatism. For (iv), equilibrium isotope fractionation between olivine and melt is near zero. These results suggest that equilibrium Fe isotope fractionation alone cannot explain the MORB isotopic signature, highlighting the potential role of kinetic isotope fractionation. Using a diffusion model, we calculated kinetic Fe and Mg isotope fractionations associated with (iv) olivine crystallization from a melt, and found that the predicted Fe and Mg isotope fractionations were inconsistent with observations in MORBs. Qualitatively, two processes could have induced kinetic Fe isotope fractionation during MORB generation: (a) Fe-Mg interdiffusion between melt and solid during melt migration and (b) reactive melt-rock interactions during melt focusing. However, a quantitative understanding of their role in modifying the melt isotopic composition remains limited and requires further investigation.

Fe isotopes↗

Atomic layer deposition of nanofilms on porous polymer substrates: Strategies for success

Atomic layer deposition (ALD) is a versatile technique for engineering the surfaces of porous polymers, imbuing the flexible, high-surface-area substrates with inorganic and hybrid material properties. Previously reported enhancements include fouling resistance, electrical conductance, thermal stability, photocatalytic activity, hydrophilicity, and oleophilicity. However, there are many poorly understood phenomena that introduce challenges in applying ALD to porous polymers. In this paper, we address five common challenges and ways to overcome them: (1) entrapped precursor, (2) embrittlement, (3) film fracture, (4) deformation, and (5) pore collapse. These challenges are often interrelated and can exacerbate one another. To investigate these phenomena, we applied various ALD chemistries to porous polymers including polyethersulfone, polysulfone, polyvinylidene fluoride, and polycarbonate track-etched membranes. Reaction-diffusion modeling revealed why certain precursors and processing conditions result in embrittling subsurface material growth, entrapment of unreacted precursors, and nongrowth. We quantify the limits of ALD processing temperatures that are dictated by thermal expansion mismatch and can lead to fractured ALD films. The results herein allow us to make recommendations to avoid, mitigate, or overcome the difficulties encountered when performing ALD and plasma-enhanced ALD on porous polymers. We intend this article to serve as a “lessons learned” guide informed by previous experience to provide a better understanding of the difficulties and limitations of ALD on porous polymers and knowledge-based guidelines for successful depositions. This knowledge can accelerate future research and help experimentalists navigate and troubleshoot as they expose porous polymers to reactive precursor vapors.

36 MATERIALS SCIENCE↗