Publications

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Argon is the most abundant noble gas on Earth and its noble, atomic fluid nature makes it an excellent candidate for comparison of experiment and theory at extreme conditions. We performed a combined computational and experimental study on shock compressed cryogenic liquid argon. Using Sandia's Z machine, we shock compressed liquid argon to 600 GPa and reshock states up to 950 GPa. Laser shock experiments at the Omega Laser facility extend the principal Hugoniot to 1000 GPa and provided temperature data along the principal Hugoniot. The plate impact experiments and laser shock experiments used well-characterized impedance matching standards and demonstrate consistent results between the two platforms over a common range. Density functional theory based molecular dynamics simulations provided additional data on the Hugoniot to 600 GPa. The combined experimental data and simulation results provide constraints on the development of new equation of state models at extreme conditions.

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Here we present a new analysis methodology that allows for the self-consistent integration of multiple diagnostics including nuclear measurements, x-ray imaging, and x-ray power detectors to determine the primary stagnation parameters, such as temperature, pressure, stagnation volume, and mix fraction in magnetized liner inertial fusion (MagLIF) experiments. The analysis uses a simplified model of the stagnation plasma in conjunction with a Bayesian inference framework to determine the most probable configuration that describes the experimental observations while simultaneously revealing the principal uncertainties in the analysis. We validate the approach by using a range of tests including analytic and three-dimensional MHD models. An ensemble of MagLIF experiments is analyzed, and the generalized Lawson criterion χ is estimated for all experiments.

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Quantum Monte Carlo (QMC) methods are useful for studies of strongly correlated materials because they are many body in nature and use the physical Hamiltonian. Typical calculations assume as a starting point a wave function constructed from single-particle orbitals obtained from one-body methods, e.g., density functional theory. However, mean-field-derived wave functions can sometimes lead to systematic QMC biases if the mean-field result poorly describes the true ground state. Here, we study the accuracy and flexibility of QMC trial wave functions using variational and fixed-node diffusion QMC estimates of the total spin density and lattice distortion of antiferromagnetic iron oxide (FeO) in the ground state B1 crystal structure. We found that for relatively simple wave functions the predicted lattice distortion was controlled by the choice of single-particle orbitals used to construct the wave function, rather than by subsequent wave function optimization techniques within QMC. By optimizing the orbitals with QMC, we then demonstrate starting-point independence of the trial wave function with respect to the method by which the orbitals were constructed by demonstrating convergence of the energy, spin density, and predicted lattice distortion for two qualitatively different sets of orbitals. The results suggest that orbital optimization is a promising method for accurate many-body calculations of strongly correlated condensed phases.

We present experimental results from the first systematic study of performance scaling with drive parameters for a magnetoinertial fusion concept. In magnetized liner inertial fusion experiments, the burn-averaged ion temperature doubles to 3.1 keV and the primary deuterium-deuterium neutron yield increases by more than an order of magnitude to 1.1×1013 (2 kJ deuterium-tritium equivalent) through a simultaneous increase in the applied magnetic field (from 10.4 to 15.9 T), laser preheat energy (from 0.46 to 1.2 kJ), and current coupling (from 16 to 20 MA). Individual parametric scans of the initial magnetic field and laser preheat energy show the expected trends, demonstrating the importance of magnetic insulation and the impact of the Nernst effect for this concept. A drive-current scan shows that present experiments operate close to the point where implosion stability is a limiting factor in performance, demonstrating the need to raise fuel pressure as drive current is increased. Simulations that capture these experimental trends indicate that another order of magnitude increase in yield on the Z facility is possible with additional increases of input parameters.

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Mixing of cold, higher-Z elements into the fuel region of an inertial confinement fusion target spoils the fusion burn efficiency. This mixing process is driven by both "turbulent" and "atomic" mixing processes, the latter being modeled through transport corrections to the basic hydrodynamic models. Recently, there has been a surge in the development of dense plasma transport modeling and the associated transport coefficients; however, experimental validation remains in its infancy.

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By deploying a photon Doppler velocimetry based plasma diagnostic, we have directly observed low density plasma in the load anode/cathode gap of cylindrically converging pulsed power targets. The arrival of this plasma is temporally correlated with gross current loss and subtle power flow differences between the anode and the cathode. The density is in the range where Hall terms in the electromagnetic equations are relevant, but this physics is lacking in the magnetohydrodynamics codes commonly used to design, analyze, and optimize pulsed power experiments. Here, the present work presents evidence of the importance of physics beyond traditional resistive magnetohydrodynamics for the design of pulsed power targets and drivers.

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The shock Hugoniot for full-density and porous CeO2 was investigated in the liquid regime using ab initio molecular dynamics (AIMD) simulations with Erpenbeck's approach based on the Rankine-Hugoniot jump conditions. The phase space was sampled by carrying out NVT simulations for isotherms between 6000 and 100 000 K and densities ranging from ρ=2.5 to 20g/cm3. The impact of on-site Coulomb interaction corrections +U on the equation of state (EOS) obtained from AIMD simulations was assessed by direct comparison with results from standard density functional theory simulations. Classical molecular dynamics (CMD) simulations were also performed to model atomic-scale shock compression of larger porous CeO2 models. Results from AIMD and CMD compression simulations compare favorably with Z-machine shock data to 525 GPa and gas-gun data to 109 GPa for porous CeO2 samples. Using results from AIMD simulations, an accurate liquid-regime Mie-Grüneisen EOS was built for CeO2. In addition, a revised multiphase SESAME-Type EOS was constrained using AIMD results and experimental data generated in this work. This study demonstrates the necessity of acquiring data in the porous regime to increase the reliability of existing analytical EOS models.

Presented are the results from the liner ablation experiments conducted at 550 kA on the Michigan Accelerator for Inductive Z-Pinch Experiments. These experiments were performed to evaluate a hypothesis that the electrothermal instability (ETI) is responsible for the seeding of magnetohydrodynamic instabilities and that the cumulative growth of ETI is primarily dependent on the material-specific ratio of critical temperature to melting temperature. This ratio is lower in refractory metals (e.g., tantalum) than in non-refractory metals (e.g., aluminum or titanium). The experimental observations presented herein reveal that the plasma-vacuum interface is remarkably stable in tantalum liner ablations. This stability is particularly evident when contrasted with the observations from aluminum and titanium experiments. These results are important to various programs in pulsed-power-driven plasma physics that depend on liner implosion stability. Examples include the magnetized liner inertial fusion (MagLIF) program and the cylindrical dynamic material properties program at Sandia National Laboratories, where liner experiments are conducted on the 27-MA Z facility.

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Hydrodynamic instability growth is a fundamentally limiting process in many applications. In High Energy Density Physics (HEDP) systems such as inertial confinement fusion implosions and stellar explosions, hydro instabilities can dominate the evolution of the object and largely determine the final state achievable. Of particular interest is the process by which instabilities cause perturbations at a density or material interface to grow nonlinearly, introducing vorticity and eventually causing the two species to mix across the interface. Although quantifying instabilities has been the subject of many investigations in planar geometry, few have been done in converging geometry. During FY17, the team executed six convergent geometry instability experiments. Based on earlier results, the platform was redesigned and improved with respect to load centering at installation making the installation reproducible and development of a new 7.2 keV, Co He-a backlighter system to better penetrate the liner. Together, the improvements yielded significantly improved experimental results. The results in FY17 demonstrate the viability of using experiments on Z to quantify instability growth in cylindrically convergent geometry. Going forward, we will continue the partnership with staff and management at LANL to analyze the past experiments, compare to hydrodynamics growth models, and design future experiments.

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Materials in nuclear and conventional weapons can reach multi-megabar pressures and 1000s of degree temperatures on timescales ranging from microseconds to nanoseconds. Understanding the response of complex materials under these conditions is important for designing and assessing changes to nuclear weapons. In the next few decades, a major concern will be evaluating the behavior of aging materials and remanufactured components. The science to enable the program to underwrite decisions quickly and confidently on use, remanufacturing, and replacement of these materials will be critical to NNSA’s new Stockpile Responsiveness Program. Material response is also important for assessing the risks posed by adversaries or proliferants. Dynamic materials research, which refers to the use of high-speed experiments to produce extreme conditions in matter, is an important part of NNSA’s Stockpile Stewardship Program.

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We report on a new technique for obtaining off-Hugoniot pressure vs. density data for solid metals compressed to extreme pressure by a magnetically driven liner implosion on the Z-machine (Z) at Sandia National Laboratories. In our experiments, the liner comprises inner and outer metal tubes. The inner tube is composed of a sample material (e.g., Ta and Cu) whose compressed state is to be inferred. The outer tube is composed of Al and serves as the current carrying cathode. Another aluminum liner at much larger radius serves as the anode. A shaped current pulse quasi-isentropically compresses the sample as it implodes. The iterative method used to infer pressure vs. density requires two velocity measurements. Photonic Doppler velocimetry probes measure the implosion velocity of the free (inner) surface of the sample material and the explosion velocity of the anode free (outer) surface. These two velocities are used in conjunction with magnetohydrodynamic simulation and mathematical optimization to obtain the current driving the liner implosion, and to infer pressure and density in the sample through maximum compression. This new equation of state calibration technique is illustrated using a simulated experiment with a Cu sample. Monte Carlo uncertainty quantification of synthetic data establishes convergence criteria for experiments. Results are presented from experiments with Al/Ta, Al/Cu, and Al liners. Symmetric liner implosion with quasi-isentropic compression to peak pressure ∼1000 GPa is achieved in all cases. These experiments exhibit unexpectedly softer behavior above 200 GPa, which we conjecture is related to differences in the actual and modeled properties of aluminum.

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The moon-forming impact and the subsequent evolution of the proto-Earth is strongly dependent on the properties of materials at the extreme conditions generated by this violent collision. We examine the high pressure behavior of MgO, one of the dominant constituents in Earth's mantle, using high-precision, plate impact shock compression experiments performed on Sandia National Laboratories' Z Machine and extensive quantum calculations using density functional theory (DFT) and quantum Monte Carlo (QMC) methods. The combined data span from ambient conditions to 1.2 TPa and 42 000 K, showing solid-solid and solid-liquid phase boundaries. Furthermore our results indicate that under impact the solid and liquid phases coexist for more than 100 GPa, pushing complete melting to pressures in excess of 600 GPa. The high pressure required for complete shock melting has implications for a broad range of planetary collision events.

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We report on experiments where cylindrical beryllium liners filled with liquid deuterium were compressed to extreme pressure and density with current pulse shaping. In one set of experiments the pressure at stagnation is inferred to be & 100 Mbar using penetrating radiography. A peak liner convergence ratio (initial radius over final radius) of 7.6 was measured resulting in an average deuterium density of 10 g=cm³ and areal density of 0.45 g=cm². The stagnation shock propagating radially outward through the liner wall was directly measured with a strength of ≈ 120 Mbar. In a second set of experiments the liner was imploded to a peak convergence of 19 resulting in a density of 55 g=cm³ and areal density of 0.5 g=cm². The pressure at stagnation in this experiment is estimated to be 2 Gbar. This platform enables the study of high-pressure, high-density, implosion deceleration and stagnation dynamics at spatial scales that are readily diagnosable (R ~ 0.1 -- 0.4 mm). Thus, these experiments are directly relevant to both Inertial Con nement Fusion and the study of material properties under extreme conditions.

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Mixtures of light elements with heavy elements are important in inertial confinement fusion. We explore the physics of molecular scale mixing through a validation study of equation of state (EOS) properties. Density functional theory molecular dynamics (DFT-MD) at elevated temperature and pressure is used to obtain the thermodynamic state properties of pure xenon, ethane, and various compressed mixture compositions along their principal Hugoniots. To validate these simulations, we have performed shock compression experiments using the Sandia Z-Machine. A bond tracking analysis correlates the sharp rise in the Hugoniot curve with the completion of dissociation in ethane. The DFT-based simulation results compare well with the experimental data along the principal Hugoniots and are used to provide insight into the dissociation and temperature along the Hugoniots as a function of mixture composition. Interestingly, we find that the compression ratio for complete dissociation is similar for several compositions suggesting a limiting compression for C-C bonded systems.

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Motivated by the disagreement between recent diffusion Monte Carlo calculations of the phase transition pressure between the ambient and beta-Sn phases of silicon and experiments, we present a study of the HCP to BCC phase transition in beryllium. This lighter element provides an opportunity for directly testing many of the approximations required for calculations on silicon and may suggest a path towards increasing the practical accuracy of diffusion Monte Carlo calculations of solids in general. We demonstrate that the single largest approximation in these calculations is the pseudopotential approximation and after removing this we find excellent agreement with experiment for the ambient HCP phase and results similar to careful calculations using density functional theory for the phase transition pressure.

We use Sandia's Z machine and magnetically accelerated flyer plates to shock compress liquid krypton to 850 GPa and compare with results from density-functional theory (DFT) based simulations using the AM05 functional. We also employ quantum Monte Carlo calculations to motivate the choice of AM05. We conclude that the DFT results are sensitive to the quality of the pseudopotential in terms of scattering properties at high energy/temperature. A new Kr projector augmented wave potential was constructed with improved scattering properties which resulted in excellent agreement with the experimental results to 850 GPa and temperatures above 10 eV (110 kK). Finally, we present comparisons of our data from the Z experiments and DFT calculations to current equation of state models of krypton to determine the best model for high energy-density applications.

We present an improved first-principles description of melting under pressure based on thermodynamic integration comparing density functional theory (DFT) and quantum Monte Carlo (QMC) treatments. The method is applied to address the longstanding discrepancy between DFT calculations and diamond anvil cell (DAC) experiments on the melting curve of xenon, a noble gas solid where van der Waals binding is challenging for traditional DFT methods. The calculations show agreement with data below 20 GPa and that the high-pressure melt curve is well described by a Lindemann behavior up to at least 80 GPa, in contrast to DAC data.

The fifth Fundamental Science with Pulsed Power: Research Opportunities and User Meeting was held in Albuquerque, NM, July 20-­23, 2014. The purpose of the workshop was to bring together leading scientists in four research areas with active fundamental science research at Sandia’s Z facility: Magnetized Liner Inertial Fusion (MagLIF), Planetary Science, Astrophysics, and Material Science. The workshop was focused on discussing opportunities for high-­impact research using Sandia’s Z machine, a future 100 GPa class facility, and possible topics for growing the academic (off-Z-campus) science relevant to the Z Fundamental Science Program (ZFSP) and related projects in astrophysics, planetary science, MagLIF- relevant magnetized HED science, and materials science. The user meeting was for Z collaborative users to: a) hear about the Z accelerator facility status and plans, b) present the status of their research, and c) be provided with a venue to meet and work as groups. Following presentations by Mark Herrmann and Joel Lash on the fundamental science program on Z and the status of the Z facility where plenary sessions for the four research areas. The third day of the workshop was devoted to breakout sessions in the four research areas. The plenary-­ and breakout sessions were for the four areas organized by Dan Sinars (MagLIF), Dylan Spaulding (Planetary Science), Don Winget and Jim Bailey (Astrophysics), and Thomas Mattsson (Material Science). Concluding the workshop were an outbrief session where the leads presented a summary of the discussions in each working group to the full workshop. A summary of discussions and conclusions from each of the research areas follows and the outbrief slides are included as appendices.

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Density Functional Theory (DFT) based molecular dynamics has been established as a method capable of yielding high fidelity results for many materials at a wide range of pressures and temperatures and has recently been applied to complex polymers such as polyethylene, compounds such as ethane or CO2, and oxides such as MgO. We use this method to obtain a Grïneisen Γ and thereby build a Mie-Grüneisen equation of state (EOS) and a Rice-Walsh EOS for tantalum pentoxide (Ta2O5 or tantala) and compare to experimental data. The experimental data have initial densities (ρ00) of approximately 1.13, 3, and 7.4 g/cm 3 reduced from a crystalline of 8.36 g/cm3. We found that r becomes constant at higher temperatures and pressure, but is a function of both density and temperature at lower densities and temperatures. Finally, the Mie-Gruneisen EOS is adequate for modeling the slightly distended Hugoniot with an initial density of 7.4 g/cm3 however it is inadequate for the more porous Hugoniot, while the Rice-Walsh EOS combined with a P-λ crush model approximates the experimental data quite well. © Published under licence by IOP Publishing Ltd.

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We apply diffusion quantum Monte Carlo to a broad set of solids, benchmarking the method by comparing bulk structural properties (equilibrium volume and bulk modulus) to experiment and density functional theory (DFT) based theories. The test set includes materials with many different types of binding including ionic, metallic, covalent, and van der Waals. We show that, on average, the accuracy is comparable to or better than that of DFT when using the new generation of functionals, including one hybrid functional and two dispersion corrected functionals. The excellent performance of quantum Monte Carlo on solids is promising for its application to heterogeneous systems and high-pressure/high-density conditions. Important to the results here is the application of a consistent procedure with regards to the several approximations that are made, such as finite-size corrections and pseudopotential approximations. This test set allows for any improvements in these methods to be judged in a systematic way.

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Hydrocarbon polymers, foams and nanocomposites are increasingly being subjected to extreme environments. Molecular scale modeling of these materials offers insight into failure mechanisms and complex response. Prior classical molecular dynamics (MD) simulations of the principal shock Hugoniot for two hydrocarbon polymers, polyethylene (PE) and poly (4-methyl-1-pentene) (PMP) have shown good agreement with density functional theory (DFT) calculations and experiments conducted at Sandia National Laboratories. We extended these results to include low-density polymer foams using nonequilibrium MD techniques and found good quantitative agreement with experiment. Here, we have measured the local temperature during void collapse to investigate the formation of hot spots and their relationship to polymer dissociation in foams. © 2013 Elsevier B.V. All rights reserved.

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Hydrocarbon polymers and foams are utilized in high energy-density physics (HEDP) and inertial confinement fusion (ICF) experiments as tampers, energy conversion and radiation pulse shaping layers in dynamic hohlraum Z-pinches, and ablators in ICF capsule implosions. Shocked foams frequently are found to be mixed with other materials either by intentional doping with high-Z elements or by instabilities and turbulent mixing with surrounding materials. In this paper we present one-dimensional and three-dimensional mesoscale hydrodynamic simulations of high-Z doped poly-(4-methyl-1-pentene) (PMP or TPX) foams in order to examine the validity of various equation of state (EOS) mixing rules available in two state-of-the-art simulation codes. Platinum-doped PMP foam experiments conducted at Sandia's Z facility provide data that can be used to test EOS mixing rules. We apply Sandia's ALEGRA-MHD code and the joint LLNL/SNL KULL HEDP code to model these doped foam experiments and exercise the available EOS mixing methods. One-dimensional simulations homogenize the foam with platinum dopant and show which EOS mixing methods produce results that are consistent with measured Hugoniot states. These simulations produce sharp shock fronts that are well described by traditional Hugoniot relations. Three-dimensional mesoscale simulations explicitly model the foam structure embedded with discrete platinum particles. The heterogeneous structure of the foam results in diffuse shock fronts and an unsteady post-shock state with large fluctuations about an average state. We compare shock propagation through pure foam and Pt-doped foams (50-50 mixture by weight) at equal average initial density, and examine how well the results compare to the experimentally measured Hugoniot states. © 2013 The Authors.

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Hydrocarbon foams are commonly used in high energy-density physics (HEDP) applications, for example as tamper and ablation materials for dynamic materials or inertial confinement fusion (ICF) experiments, and as such are subject to shock compression from tens to hundreds of GPa. Modeling of macro-molecular materials like hydrocarbon foams is challenging due to the heterogeneous character of the polymers and the complexity of voids and large-scale structure. Under shock conditions, these factors contribute to a relatively larger uncertainty of the post-shock state compared to that encountered for homogenous materials; therefore a quantitative understanding of foams under strong dynamic compression is sought. We use Sandia's ALEGRA-MHD code to simulate 3D mesoscale models of poly-(4-methyl-1-pentene) (PMP) foams. We devise models of the initial polymer-void structure of the foam and analyze the statistical properties of the initial and shocked states. We compare the simulations to multi-Mbar shock experiments conducted on Sandia's Z machine at various initial foam densities and flyer impact velocities. Scatter in the experimental data may be a consequence of the initial foam inhomogeneity. We compare the statistical properties of the simulations with the scatter in the experimental data. © 2012 American Institute of Physics.

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Hydrocarbon polymers, foams and nanocomposites are increasingly being subjected to extreme environments. Molecular scale modeling of these materials offers insight into failure mechanisms and complex response. Classical molecular dynamics (MD) simulations of the principal shock Hugoniot were conducted for two hydrocarbon polymers, polyethylene (PE) and poly(4-methyl-1-pentene) (PMP). We compare these results with recent density functional theory (DFT) calculations and experiments conducted at Sandia National Laboratories. Here, we extend these results to include low-density polymer foams using nonequilibrium MD techniques. We find good quantitative agreement with experiment. Further, we have measured local temperatures to investigate the formation of hot spots and polymer dissociation near foam voids.

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Hydrocarbon foams are commonly used in HEDP experiments, and are subject to shock compression from tens to hundreds of GPa. Modeling foams is challenging due to the heterogeneous character of the foam. A quantitative understanding of foams under strong dynamic compression is sought. We use Sandia's ALEGRA-MHD code to simulate 3D mesoscale models of pure poly(4-methyl-1-petene) (PMP) foams. We employ two models of the initial polymer-void structure of the foam and analyze the statistical properties of the initial and shocked states. We compare the simulations to multi-Mbar shock experiments at various initial foam densities and flyer impact velocities. Scatter in the experimental data may be a consequence of the initial foam inhomogeneity. We compare the statistical properties the simulations with the scatter in the experimental data.

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Density Functional Theory (DFT) has over the last few years emerged as an indispensable tool for understanding the behavior of matter under extreme conditions. DFT based molecular dynamics simulations (MD) have for example confirmed experimental findings for shocked deuterium,1 enabled the first experimental evidence for a triple point in carbon above 850 GPa,2 and amended experimental data for constructing a global equation of state (EOS) for water, carrying implications for planetary physics.3 The ability to perform high-fidelity calculations is even more important for cases where experiments are impossible to perform, dangerous, and/or prohibitively expensive. For solid explosives, and other molecular crystals, similar success has been severely hampered by an inability of describing the materials at equilibrium. The binding mechanism of molecular crystals (van der Waals' forces) is not well described within traditional DFT.4 Among widely used exchange-correlation functionals, neither LDA nor PBE balances the strong intra-molecular chemical bonding and the weak inter-molecular attraction, resulting in incorrect equilibrium density, negatively affecting the construction of EOS for undetonated high explosives. We are exploring a way of bypassing this problem by using the new Armiento-Mattsson 2005 (AM05) exchange-correlation functional.5, 6 The AM05 functional is highly accurate for a wide range of solids,4, 7 in particular in compression.8 In addition, AM05 does not include any van der Waals' attraction,4 which can be advantageous compared to other functionals: Correcting for a fictitious van der Waals' like attraction with unknown origin can be harder than correcting for a complete absence of all types of van der Waals' attraction. We will show examples from other materials systems where van der Waals' attraction plays a key role, where this scheme has worked well,9 and discuss preliminary results for molecular crystals and explosives.

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The noble gas xenon is a particularly interesting element. At standard pressure xenon is an fcc solid which melts at 161 K and then boils at 165 K, thus displaying a rather narrow liquid range on the phase diagram. On the other hand, under pressure the melting point is significantly higher: 3000 K at 30 GPa. Under shock compression, electronic excitations become important at 40 GPa. Finally, xenon forms stable molecules with fluorine (XeF{sub 2}) suggesting that the electronic structure is significantly more complex than expected for a noble gas. With these reasons in mind, we studied the xenon Hugoniot using DFT/QMD and validated the simulations with multi-Mbar shock compression experiments. The results show that existing equation of state models lack fidelity and so we developed a wide-range free-energy based equation of state using experimental data and results from first-principles simulations.

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Significant progress has been made over the last few years in understanding properties of matter subject to strong shocks and other extreme conditions. High-accuracy multi-Mbar experiments and first-principles theoretical studies together provide detailed insights into the physics and chemistry of high energy-density matter. While comprehensive advances have been made for pure elements like deuterium, helium, and carbon, progress has been slower for equally important, albeit more challenging, materials like molecular crystals, polymers, and foams. Hydrocarbon based polymer foams are common materials and in particular they are used in designing shock- and inertial confinement fusion experiments. Depending on their initial density, foams shock to relatively higher pressure and temperature compared to shocked dense polymers/plastics. As foams and polymers are shocked, they exhibit both structural and chemical transitions. We will present experimental and theoretical results for shocked polymers in the Mbar regime. By shock impact of magnetically launched flyer plates on poly(4-methyl-1-pentene) foams, we create multi-Mbar pressures in a dense plasma mixture of hydrogen, carbon, at temperatures of several eV. Concurrently with executing experiments, we analyze the system by multi-scale simulations, from density functional theory to continuum magneto-hydrodynamics simulations. In particular, density functional theory (DFT) molecular dynamics (MD) and classical MD simulations of the principal shock Hugoniot will be presented in detail for two hydrocarbon polymers: polyethylene (PE) and poly(4-methyl-1-pentene) (PMP).

The difficulty of calculating the ambient properties of molecular crystals, such as the explosive PETN, has long hampered much needed computational investigations of these materials. One reason for the shortcomings is that the exchange-correlation functionals available for Density Functional Theory (DFT) based calculations do not correctly describe the weak intermolecular van der Waals' forces present in molecular crystals. However, this weak interaction also poses other challenges for the computational schemes used. We will discuss these issues in the context of calculations of lattice constants and structure of PETN with a number of different functionals, and also discuss if these limitations can be circumvented for studies at non-ambient conditions.

Xenon is not only a technologically important element used in laser technologies and jet propulsion, but it is also one of the most accessible materials in which to study the metal-insulator transition with increasing pressure. Because of its closed shell electronic configuration, xenon is often assumed to be chemically inert, interacting almost entirely through the van der Waals interaction, and at liquid density, is typically modeled well using Leonard-Jones potentials. However, such modeling has a limited range of validity as xenon is known to form compounds under normal conditions and likely exhibits considerably more chemistry at higher densities when hybridization of occupied orbitals becomes significant. We present DFT-MD simulations of shocked liquid xenon with the goal of developing an improved equation of state. The calculated Hugoniot to 2 MPa compares well with available experimental shock data. Sandia is a mul-tiprogram laboratory operated by Sandia Corporation, a Lockheed Martin Company, for the United States Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000. © 2009 American Institute of Physics.

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We present extensive simulations modeling the casting of multiblock polymer films by evaporation. The domain structure of the resulting film is strongly affected by varying the relative stiffness of the coblocks. The morphology changes from a bicontinuous lamellar phase when both blocks are flexible to a small-scale phase-separated phase with isolated domains as the stiffness of one of the blocks increases. As the relative stiffness of the blocks changes, the rate of evaporation, interfacial width, and morphology of the system changes. The findings can be used to tailor membrane morphology of interest to fuel-cell applications where the morphology is important for proton conduction.

Warm dense matter is the region in phase space of density and temperature where the thermal, Fermi, and Coulomb energies are approximately equal. The lack of a dominating scale and physical behavior makes it challenging to model the physics to high fidelity. For Sandia, a fundamental understanding of the region is of importance because of the needs of our experimental HEDP programs for high fidelity descriptive and predictive modeling. We show that multi-scale simulations of macroscopic physical phenomena now have predictive capability also for difficult but ubiquitous materials such as stainless steel, a transition metal alloy.

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Mechanisms for enhanced low-dose-rate sensitivity are described. In these mechanisms, bimolecular reactions dominate the kinetics at high dose rates thereby causing a sub-linear dependence on total dose, and this leads to a dose-rate dependence. These bimolecular mechanisms include electron-hole recombination, hydrogen recapture at hydrogen source sites, and hydrogen dimerization to form hydrogen molecules. The essence of each of these mechanisms is the dominance of the bimolecular reactions over the radiolysis reaction at high dose rates. However, at low dose rates, the radiolysis reaction dominates leading to a maximum effect of the radiation.

Density functional calculations show that the electric field effect on Si ad-dimer diffusion on Si(0 0 1) is largely a reflection of the position dependence of the ad-dimer's dipole moment. Surface diffusion barriers' dependence on perpendicular electric fields can be used to discriminate between diffusion mechanisms. Since the previously accepted mechanism for ad-dimer diffusion on Si(0 0 1) has the opposite field dependence to what is observed, it cannot be the one that dominates mass-transport. We identify an alternate process, with a similar barrier at zero electric field and field dependence in agreement with measurements. For rotation, calculations to date show linear field dependence, in contrast to experiments. © 2003 Elsevier Science B.V. All rights reserved.

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We change the diffusion mechanism of adsorbed Ge-Si dimers on Si(001) using the electric field of a scanning tunneling microscope tip. By comparing the measured field dependence with first-principles calculations we conclude that, in negative field, i.e., when electrons are attracted towards the vacuum, the dimer diffuses as a unit, rotating as it translates, whereas, in positive field the dimer bond is substantially stretched at the transition state as it slides along the substrate. Furthermore, the active mechanism in positive fields facilitates intermixing of Ge in the Si lattice, whereas intermixing is suppressed in negative fields. © 2003 The American Physical Society.

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