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At least 559 records · Page 31

Time dependent chlorination of CeO 2 , La 2 O 3 and Nd 2 O 3 by ZrCl 4 dissolved in eutectic LiCl–KCl

Partial chlorination of CeO 2 , La 2 O 3 , and Nd 2 O 3 was achieved using ZrCl 4 dissolved in molten LiCl-KCl at 450°C over a period of 4-5 hr. ZrCl 4 was pre-volatilized into an argon stream to maintain a constant vapor pressure for equilibration with the salt. This approach was effective at maintaining the ZrCl 4 concentration at the solubility limit of 1.3 mol% in the molten salt throughout the duration of two of the chlorination experiments and within about 60% of the solubility limit in the third experiment. Based on the analysis of salt samples, fractional conversion after four hours of reaction for CeO 2 , and five hours for La 2 O 3 , and Nd 2 O 3 were calculated to be 0.97, 0.28, and 0.65 respectively. Assuming a shrinking core diffusion-limited model, the diffusivity of ZrCl 4 through the hypothesized ZrO 2 layer was calculated for the chlorination of CeO 2 , La 2 O 3 , and Nd 2 O 3 were 1.76 x 10 -10 cm 2 /sec, 7.85 x 10 -12 cm 2 /sec, and 7.42 x 10 -12 cm 2 /sec, respectively. Given the extremely low values calculated for diffusivity, it was concluded that the process is chemical reaction rate limited and that a complete reaction of each rare earth oxide could be achieved. Furthermore, a chemically controlled shrinking core model was shown to also fit the experimental data closely.

11 NUCLEAR FUEL CYCLE AND FUEL MATERIALS↗

On how structures convey non-diffusive turbulence spreading

Abstract We report on comprehensive experimental studies of turbulence spreading in edge plasmas. These studies demonstrate the relation of turbulence spreading and entrainment to intermittent convective density fluctuation events or bursts (i.e. blobs and holes). The non-diffusive character of turbulence spreading is thus elucidated. The turbulence spreading velocity (or mean jet velocity) manifests a linear correlation with the skewness of density fluctuations, and increases with the auto-correlation time of density fluctuations. Turbulence spreading by positive density fluctuations is outward, while spreading by negative density fluctuations is inward. The degree of symmetry breaking between outward propagating blobs and inward propagating holes increases with the amplitude of density fluctuations. Thus, blob-hole asymmetry emerges as crucial to turbulence spreading. These results highlight the important role of intermittent convective events in conveying the spreading of turbulence, and constitute a fundamental challenge to existing diffusive models of spreading.

70 PLASMA PHYSICS AND FUSION TECHNOLOGY↗

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↗

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↗

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↗

Edge-Based Viscous Method for Mixed-Element Node-Centered Finite-Volume Solvers

A novel, efficient, edge-based viscous (EBV) discretization method has been recently developed, implemented in a practical, unstructured-grid, node-centered, finite-volume flow solver, and applied to viscous-kernel computations that include evaluations of meanflow viscous fluxes, turbulence-model and chemistry-model diffusion terms, and the corresponding Jacobian contributions. Initially, the EBV method had been implemented for tetrahedral grids and demonstrated multifold acceleration of all viscous-kernel computations. This paper presents an extension of the EBV method for mixed-element grids. In addition to the primal edges of a given mixed-element grid, virtual edges are introduced to connect cell nodes that are not connected by a primal edge. The EBV method uses an efficient loop over all (primal and virtual) edges and features a compact discretization stencil based on the nearest neighbors. This study verifies the EBV method and assesses its efficiency on mixed-element grids by comparing the EBV solution accuracy and iterative convergence with those of well-established solutions obtained using a cell-based viscous (CBV) discretization method. The EBV solver’s memory footprint is optimized and often smaller than the memory footprint of the CBV solver. A multifold speedup is demonstrated for all viscous-kernel computations resulting in significant reduction of the time to solutions for several benchmark mixed-element-grid computations, including simulations of a flow around NASA’s juncture-flow model and a hypersonic, chemically reacting flow around a blunt body.

CFD↗

Edge-Based Viscous Method for Mixed-Element Node-Centered Finite-Volume Solvers

A novel, efficient, edge-based viscous (EBV) discretization method has been recently developed, implemented in a practical, unstructured-grid, node-centered, finite-volume flow solver, and applied to viscous-kernel computations that include evaluations of meanflow viscous fluxes, turbulence-model and chemistry-model diffusion terms, and the corresponding Jacobian contributions. Initially, the EBV method had been implemented for tetrahedral grids and demonstrated multifold acceleration of all viscous-kernel computations. This paper presents an extension of the EBV method for mixed-element grids. In addition to the primal edges of a given mixed-element grid, virtual edges are introduced to connect cell nodes that are not connected by a primal edge. The EBV method uses an efficient loop over all (primal and virtual) edges and features a compact discretization stencil based on the nearest neighbors. This study verifies the EBV method and assesses its efficiency on mixed-element grids by comparing the EBV solution accuracy and iterative convergence with those of well-established solutions obtained using a cell-based viscous (CBV) discretization method. The EBV solver’s memory footprint is optimized and often smaller than the memory footprint of the CBV solver. A multifold speedup is demonstrated for all viscous-kernel computations resulting in significant reduction of the time to solutions for several benchmark mixed-element-grid computations, including simulations of a flow around NASA’s juncture-flow model and a hypersonic, chemically reacting flow around a blunt body.

Edge-based viscous method↗

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↗

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↗

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↗

Mathematical model of diffusion-limited gas bubble dynamics in unstirred tissue with finite volume

Models of gas bubble dynamics for studying decompression sickness have been developed by considering the bubble to be immersed in an extravascular tissue with diffusion-limited gas exchange between the bubble and the surrounding unstirred tissue. In previous versions of this two-region model, the tissue volume must be theoretically infinite, which renders the model inapplicable to analysis of bubble growth in a finite-sized tissue. We herein present a new two-region model that is applicable to problems involving finite tissue volumes. By introducing radial deviations to gas tension in the diffusion region surrounding the bubble, the concentration gradient can be zero at a finite distance from the bubble, thus limiting the tissue volume that participates in bubble–tissue gas exchange. It is shown that these deviations account for the effects of heterogeneous perfusion on gas bubble dynamics, and are required for the tissue volume to be finite. The bubble growth results from a difference between the bubble gas pressure and an average gas tension in the surrounding diffusion region that explicitly depends on gas uptake and release by the bubble. For any given decompression, the diffusion region volume must stay above a certain minimum in order to sustain bubble growth.

NASA Discipline Environmental Health↗

Experimental and computational design tools for industrial drying processes: Challenges in process‐limit prediction

Abstract The coating and drying of inks and slurries are important steps to manufacture a plethora of products. Drying processes, particularly, comprise energy‐intensive steps that affect product cost and quality. Prior work has highlighted failures of various multicomponent diffusivity models to conserve mass in dryer modeling and challenges in predicting process limits given variability in published values of key thermodynamic parameters. Herein, we develop a computational model and benchtop drying experiments to investigate these concerns for drying polymer‐laden coatings. Model predictions of process limits in a single‐zone drying oven demonstrate that published variability in Flory–Huggins parameter yields large variations in predicted operating temperatures above which blistering occurs. This indicates that caution should be exercised when choosing approaches to obtain or predict the Flory–Huggins parameter, and that both benchtop drying experiments and a set of additional experiments, such as sorption experiments, are needed to fully characterize and optimize a given drying process.

Parrish, Chance↗

DNA Reaction–Diffusion Attractor Patterns

Abstract Living systems can form and recover complex chemical patterns with precisely sized features in the ranges of tens or hundreds of microns. We show how designed reaction–diffusion processes can likewise produce precise patterns, termed attractor patterns, that reform their precise shape after being perturbed. We use oligonucleotide reaction networks, photolithography, and microfluidic delivery to form precisely controlled attractor patterns and study the responses of these patterns to different localized perturbations. Linear and “hill”‐shaped patterns formed and stabilized into shapes and at time scales consistent with reaction–diffusion models. When patterns were perturbed in particular locations with UV light, they reliably reformed their steady‐state profiles. Recovery also occurred after repeated perturbations. By designing the far‐from‐equilibrium dynamics of a chemical system, this study shows how it is possible to design spatial patterns of molecules that are sustained and regenerated by continually evolving towards a specific steady state configuration.

Dorsey, Phillip James↗

DNA Reaction–Diffusion Attractor Patterns

Living systems can form and recover complex chemical patterns with precisely sized features in the ranges of tens or hundreds of microns. We show how designed reaction-diffusion processes can likewise produce precise patterns, termed attractor patterns, that reform their precise shape after being perturbed. We use oligonucleotide reaction networks, photolithography and microfluidic delivery to form precisely controlled attractor patterns and study the responses of these patterns to different localized perturbations. Linear and ‘hill’-shaped patterns formed and stabilized into shapes and at time scales consistent with reaction-diffusion models. When patterns were perturbed in particular locations with UV light, they reliably reformed their steady state profiles. Recovery also occurred after repeated perturbations. As a result, by designing the far-from-equilibrium dynamics of a chemical system, this study shows how it is possible to design spatial patterns of molecules that are sustained and regenerated by continually evolving towards a specific steady state configuration

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Side chain dynamics in semiconducting polymer MEH-PPV

We report that the characteristic nanoscale dynamics of the alkyl side groups in the light-emitting polymer poly[2-methoxy-5-(2'-ethyl-hexyloxy)-1,4-phenylene vinylene] have been investigated using quasi-elastic neutron scattering (QENS). The measurements were taken below the polymer's glass transition (T ≤ T g ≃ 353 K), where the main backbone is in a rigid state and does not contribute to the broadening of the QENS signal. An analytical diffusion model consisting of a static term and two dynamical components, characterizing the flexible side groups, provide an excellent fit to the experimental data. The two observed dynamical processes are all localized in character, with no meaningful dependence on temperature. The faster process, with characteristic timescale of ~18 ps at room temperature (RT), can be linked to the average mobility of the terminal protons of the alkyl chain, while the slower process, with characteristic timescale of ~170 ps at RT, to those protons at the other end of the alkyl chain, closest to the backbone. Lastlyl, while the fraction of mobile protons contributing to the QENS signal increases with increasing temperature, the characteristic timescale and confining volume within which the protons are able to move locally depend chiefly on the polymer conformational state.

36 MATERIALS SCIENCE↗

Development of a Novel Equilibrium Passive Sampling Device for Methylmercury in Sediment and Soil Porewaters

In this work, we explored the concept of equilibrium passive sampling for methylmercury (MeHg) using the strategy developed for hydrophobic organic chemicals. Passive sampling should allow prediction of the concentration of the chemically labile fraction of MeHg in sediment porewaters based on equilibrium partitioning into the sampler, without modeling diffusion rates through the sampler material. Our goals were to identify sampler materials with the potential to mimic MeHg partitioning into animals and sediments and provide reversible sorption in a time frame appropriate for in situ samplers. Candidate materials tested included a range of polymers embedded with suitable sorbents for MeHg. The most promising were activated carbon (AC) embedded in agarose, thiol–self-assembled monolayers on mesoporous supports embedded in agarose, and cysteine-functionalized polyethylene terephthalate, which yielded log sampler–water partition coefficients of 2.8 to 5 for MeHgOH and MeHg complexed with dissolved organic matter (Suwannee River humic acid). Sampler equilibration time in sediments was approximately 1 to 2 wk. Investigation of the MeHg accumulation mechanism by AC embedded in agarose suggested that sampling was kinetically influenced by MeHg interactions with AC particles and not limited by diffusion through the gel for this material. Also, AC exhibited relatively rapid desorption of Hg and MeHg, indicating that this sorbent is capable of reversible, equilibrium measurements. In sediment:water microcosms, porewater concentrations made with isotherm-calibrated passive samplers agreed within a factor of 2 (unamended sediment) or 4 (AC-amended sediment) with directly measured concentrations. The present study demonstrates a potential new approach to passive sampling of MeHg.

54 ENVIRONMENTAL SCIENCES↗

Effect of interface recombination on the efficiency of intracavity double diode structures

In the past ten years, there has been significant progress in solid-state optical refrigeration, causing a renewed interest in the possibility of electroluminescent cooling (ELC) in light emitting diodes (LEDs). More recently, our work on III-As based intracavity double diode structures (DDSs) indicates that the threshold for ELC can be reached, in practice, at high powers and 300 K if certain non-radiative recombination mechanisms and photodetector (PD) losses are minimized. The studied DDSs consist of a LED, incorporating a high-quality GaAs active layer, optically coupled to a GaAs p–n homojunction PD. Both the LED and PD are integrated in a single device, offering a unique environment for studying ELC. In this paper, we provide a brief overview of the DDS characteristics and investigate the impact of non-radiative interface recombination on the LED, showing how the choice of the barrier layer materials can suppress this effect. We use experimental characterization techniques to calibrate numerical simulations, coupling the drift-diffusion model for charge transport to a photon transport model. To explore the interface effects, we compare DDSs with either GaInP/GaAs or AlGaAs/GaAs double heterojunctions. The results suggest that GaInP barriers allow interface recombination suppression that is sufficient to reach internal cooling in the LED.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗