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Tang, M.

Publications and source records attributed to Tang, M..

Observation of a mixed close-packed structure in superionic water

The study of superionic (SI) water has been a highly active research area since its theoretical prediction. Despite significant experimental and computational efforts, its melting curve and the stability of different oxygen lattices remain debated, impacting our understanding of SI ice’s peculiar transport properties. Experimental results at lower pressures show disagreement, whereas data at higher pressures are scarce due to the extreme challenges of such experiments. In this work, we present ultrafast X-ray diffraction results of water compressed by multiple shocks to pressures up to ~ 180 GPa. At pressures exceeding 150 GPa and temperatures around 2500 K, our diffraction patterns challenge the pure FCC-SI phase model, providing experimental evidence of the mixed close-packed superionic phase predicted by advanced ab initio calculations. At lower pressures, we observe simultaneous signatures of BCC and FCC structures within a pressure-temperature range consistent with some static-compression experiments, helping to resolve contradictory results in literature. These insights offer new constraints on the stability domains of SI phases and reveal detailed structural features, such as stacking faults. Our results advance the structural understanding of high-pressure SI ice to a level approaching that of ice I polymorphs, with potential implications for water-rich interiors of giant planets.

Andriambariarijaona, Leon [Centre National de la R↗

Temperature dependence of the radiation tolerance of nanocrystalline pyrochlores A 2 Ti 2 O 7 (A = Gd, Ho and Lu)

A potentially enhanced radiation resistance of nanocrystalline materials, as a consequence of the high density of interfaces and surfaces, has attracted much attention both to understand the fundamental role of these defect sinks and to develop them for high-radiation environments. Here, irradiation response of nanocrystalline A 2 Ti 2 O 7 (A = Gd, Ho and Lu) pyrochlore powders with grain sizes of 20–30 nm was investigated by 1-MeV Kr 2+ ion bombardment. In situ transmission electron microscopy (TEM) revealed that the critical amorphization fluence for each nanocrystalline compound at room temperature was greater than that for their coarse-grained counterparts, indicating an enhanced amorphization resistance. The effect of temperature on the irradiation response of one of these compounds, nanocrystalline Lu 2 Ti 2 O 7 , was further examined by performing ion irradiation at an elevated temperature range of 480–600 K. The critical amorphization temperature (T c ) was found to be noticeably higher in nanocrystalline Lu 2 Ti 2 O 7 (610 K) than its coarse-grained counterpart (480 K), revealing that nanocrystalline Lu 2 Ti 2 O 7 is less resistant to amorphization compared to its coarse-grained phase under high temperatures. We interpret these results with the aid of atomistic simulations. Molecular statics calculations find that cation antisite defects are less energetically costly to form near surfaces than in the bulk, suggesting that the nanocrystalline form of these materials is generally less susceptible to amorphization than coarse-grained counterparts at low temperatures where defect kinetics are negligible. In contrast, at high temperatures, the annealing efficiency of antisite defects by cation interstitials is significantly reduced due to the sink properties of the surfaces in the nanocrystalline pyrochlore, which contributes to the observed higher amorphization temperature in the nano-grained phase than in coarse-grained counterpart. Altogether, these results provide new insight into the behavior of nanocrystalline materials under irradiation.

36 MATERIALS SCIENCE↗

Effect of Mn substitution on the transport properties of co-sputtered Fe{sub 3−x}Mn{sub x}Si epilayers

Motivated by the theoretical calculations that Fe{sub 3−x}Mn{sub x}Si can simultaneously exhibit a high spin polarization with a high Curie temperature to be applied in spintronic devices, and in order to further study the effect of Mn contents on the physical properties of Fe{sub 3−x}Mn{sub x}Si, we have investigated the effect of Mn substitution on the transport properties of epitaxial Fe{sub 3−x}Mn{sub x}Si (0≤x≤1) films systematically. The Fe{sub 3−x}Mn{sub x}Si films were epitaxially grown on MgO(001) plane with 45° rotation. The magnetization for various x shows enhanced irreversibility, implying the antiferromagnetic ordering induced by the substitution of Mn. A metal-semiconductor crossover was observed due to the enhanced disorders of interactions and the local lowering of symmetry induced by the substitution of Mn. The single-domain state in the Fe{sub 3−x}Mn{sub x}Si films leads to twofold symmetric curves of the anisotropic magnetoresistance and planar Hall resistivity.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Design rules for dislocation filters

The efficacy of strained layer threading dislocation filter structures in single crystal epitaxial layers is evaluated using numerical modeling for (001) face-centred cubic materials, such as GaAs or Si{sub 1−x}Ge{sub x}, and (0001) hexagonal materials such as GaN. We find that threading dislocation densities decay exponentially as a function of the strain relieved, irrespective of the fraction of threading dislocations that are mobile. Reactions between threading dislocations tend to produce a population that is a balanced mixture of mobile and sessile in (001) cubic materials. In contrast, mobile threading dislocations tend to be lost very rapidly in (0001) GaN, often with little or no reduction in the immobile dislocation density. The capture radius for threading dislocation interactions is estimated to be approximately 40 nm using cross section transmission electron microscopy of dislocation filtering structures in GaAs monolithically grown on Si. We find that the minimum threading dislocation density that can be obtained in any given structure is likely to be limited by kinetic effects to approximately 10{sup 4}–10{sup 5 }cm{sup −2}.

71 CLASSICAL AND QUANTUM MECHANICS, GENERAL PHYSIC↗

Mesoscale Modeling Framework Design: Subcontract Report

This subcontract is aimed at developing the mesoscale computational capability to help ensure success of the project “Multiscale Capability for Exploring Transport Phenomena in Battery” at the Lawrence Livermore National Laboratory (LLNL). We develop an efficient computer code that implements the smoothed boundary method for simulating charge transport and coupled microstructure evolution in battery electrode architectures.

25 ENERGY STORAGE↗

Crystalline Ceramic Waste Forms: Comparison Of Reference Process For Ceramic Waste Form Fabrication

The research conducted in this work package is aimed at taking advantage of the long term thermodynamic stability of crystalline ceramics to create more durable waste forms (as compared to high level waste glass) in order to reduce the reliance on engineered and natural barrier systems. Durable ceramic waste forms that incorporate a wide range of radionuclides have the potential to broaden the available disposal options and to lower the storage and disposal costs associated with advanced fuel cycles. Assemblages of several titanate phases have been successfully demonstrated to incorporate radioactive waste elements, and the multiphase nature of these materials allows them to accommodate variation in the waste composition. Recent work has shown that they can be produced from a melting and crystallization process. The objective of this report is to explore the phase formation and microstructural differences between lab scale melt processing in varying gas environments with alternative densification processes such as Hot Pressing (HP) and Spark Plasma Sintering (SPS). The waste stream used as the basis for the development and testing is a simulant derived from a combination of the projected Cs/Sr separated stream, the Trivalent Actinide - Lanthanide Separation by Phosphorous reagent Extraction from Aqueous Komplexes (TALSPEAK) waste stream consisting of lanthanide fission products, the transition metal fission product waste stream resulting from the transuranic extraction (TRUEX) process, and a high molybdenum concentration with relatively low noble metal concentrations. Melt processing as well as solid state sintering routes SPS and HP demonstrated the formation of the targeted phases; however differences in microstructure and elemental partitioning were observed. In SPS and HP samples, hollandite, pervoskite/pyrochlore, zirconolite, metallic alloy and TiO 2 and Al 2 O 3 were observed distributed in a network of fine grains with small residual pores. The titanate phases that incorporate M +3 rare earth elements were observed to be distinct phases (ex. Nd 2 Ti 2 O 7 with less degree of substitution as compared to the more homogeneous melt processed samples where a high degree of substitution and variation of composition within grains was observed. Liquid phase sintering was enhanced in reducing gas environments and resulted in large (10-200 microns) irregular shaped grains along with large voids associated with the melt process; SPS and HP samples exhibited finer grain size with smaller voids. Metallic alloys were observed in the bulk of the sample for SPS and HP samples, but were found at the bottom of the crucible in melt processed trials. These results indicate that for a first melter trial, the targeted phases can be formed in air by utilizing Ti/TiO 2 additives which aid phase formation and improve the electrical conductivity. Ultimately, a melter run in reducing gas environments would be beneficial to study differences in phase formation and elemental partitioning.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Antimony mediated growth of high-density InAs quantum dots for photovoltaic cells

We report enhanced solar cell performance using high-density InAs quantum dots. The high-density quantum dot was grown by antimony mediated molecular beam epitaxy. In-plane quantum dot density over 1 × 10{sup 11} cm{sup −2} was achieved by applying a few monolayers of antimony on the GaAs surface prior to quantum dot growth. The formation of defective large clusters was reduced by optimization of the growth temperature and InAs coverage. Comparing with a standard quantum dot solar cell without the incorporation of antimony, the high-density quantum dot solar cell demonstrates a distinct improvement in short-circuit current from 7.4 mA/cm{sup 2} to 8.3 mA/cm{sup 2}.

36 MATERIALS SCIENCE↗

Crystalline Ceramic Waste Forms: Report Detailing Data Collection In Support Of Potential FY13 Pilot Scale Melter Test

The research conducted in this work package is aimed at taking advantage of the long term thermodynamic stability of crystalline ceramics to create more durable waste forms (as compared to high level waste glass) in order to reduce the reliance on engineered and natural barrier systems. Durable ceramic waste forms that incorporate a wide range of radionuclides have the potential to broaden the available disposal options and to lower the storage and disposal costs associated with advanced fuel cycles. Assemblages of several titanate phases have been successfully demonstrated to incorporate radioactive waste elements, and the multiphase nature of these materials allows them to accommodate variation in the waste composition. Recent work has shown that they can be successfully produced from a melting and crystallization process. The objective of this report is to summarize the data collection in support of future melter demonstration testing for crystalline ceramic waste forms. The waste stream used as the basis for the development and testing is a combination of the projected Cs/Sr separated stream, the Trivalent Actinide - Lanthanide Separation by Phosphorous reagent Extraction from Aqueous Komplexes (TALSPEAK) waste stream consisting of lanthanide fission products, the transition metal fission product waste stream resulting from the transuranic extraction (TRUEX) process, and a high molybdenum concentration with relatively low noble metal concentrations. The principal difficulties encountered during processing of the “reference ceramic” waste form by a melt and crystallization process were the incomplete incorporation of Cs into the hollandite phase and the presence of secondary Cs-Mo non-durable phases. In the single phase hollandite system, these issues were addressed in this study by refining the compositions to include Cr as a transition metal element and the use of Ti/TiO 2 buffer to maintain reducing conditions. Initial viscosity studies of ceramic waste forms indicated that the pour spout must be maintained above 1400°C to avoid flow blockages due to crystallization. In-situ electron irradiations simulate radiolysis effects indicated hollandite undergoes a crystalline to amorphous transition after a radiation dose of 10 13 Gy which corresponds to approximately 1000 years at anticipated doses (2 10 10 -2 10 11 Gy). Dual-beam ion irradiations employing light ion beam (such as 5 MeV alpha) and heavy ion beam (such as 100 keV Kr) studies indicate that reference ceramic waste forms are radiation tolerant to the α-particles and β-particles, but are susceptible to a crystalline to amorphous transition under recoil nuclei effects. A path forward for refining the processing steps needed to form the targeted phase assemblages is outlined in this report. Processing modifications including melting in a reducing atmosphere with the use of Ti/TiO 2 buffers, and the addition of Cr to the transition metal additives to facilitate Cs-incorporation in the hollandite phase. In addition to melt processing, alternative fabrication routes are being considered including Spark Plasma Sintering (SPS) and Hot Isostatic Pressing (HIP).

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Crystalline Ceramic Waste Forms: Reference Formulation Report

The research conducted in this work package is aimed at taking advantage of the long term thermodynamic stability of crystalline ceramics to create more durable waste forms (as compared to high level waste glass) in order to reduce the reliance on engineered and natural barrier systems. Durable ceramic waste forms that incorporate a wide range of radionuclides have the potential to broaden the available disposal options and to lower the storage and disposal costs associated with advanced fuel cycles. Assemblages of several titanate phases have been successfully demonstrated to incorporate radioactive waste elements, and the multiphase nature of these materials allows them to accommodate variation in the waste composition. Recent work has shown that they can be successfully produced from a melting and crystallization process. The objective of this report is to explain the design of ceramic host systems culminating in a reference ceramic formulation for use in subsequent studies on process optimization and melt property data assessment in support of FY13 melter demonstration testing. The waste stream used as the basis for the development and testing is a combination of the projected Cs/Sr separated stream, the Trivalent Actinide - Lanthanide Separation by Phosphorous reagent Extraction from Aqueous Komplexes (TALSPEAK) waste stream consisting of lanthanide fission products, the transition metal fission product waste stream resulting from the transuranic extraction (TRUEX) process, and a high molybdenum concentration with relatively low noble metal concentrations. In addition to the combined CS/LN/TM High Mo waste stream, variants without Mo and without Mo and Zr were also evaluated. Based on the results of fabricating and characterizing several simulated ceramic waste forms, two reference ceramic waste form compositions are recommended in this report. The first composition targets the CS/LN/TM combined waste stream with and without Mo. The second composition targets with CS/LN/TM combined waste stream with Mo and Zr removed. Waste streams that contain Mo must be produced in reducing environments to avoid Cs-Mo oxide phase formation. Waste streams without Mo have the ability to be melt processed in air. A path forward for further optimizing the processing steps needed to form the targeted phase assemblages is outlined in this report. Processing modifications including melting in a reducing atmosphere, and controlled heat treatment schedules are anticipated to improve the targeted elemental partitioning.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗