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Numerical implementation of time-dependent density functional theory for extended systems in extreme environments

Baczewski, Andrew D.; Shulenburger, Luke N.; Desjarlais, Michael P.; Magyar, Rudolph J.

In recent years, DFT-MD has been shown to be a useful computational tool for exploring the properties of WDM. These calculations achieve excellent agreement with shock compression experiments, which probe the thermodynamic parameters of the Hugoniot state. New X-ray Thomson Scattering diagnostics promise to deliver independent measurements of electronic density and temperature, as well as structural information in shocked systems. However, they require the development of new levels of theory for computing the associated observables within a DFT framework. The experimentally observable x-ray scattering cross section is related to the electronic density-density response function, which is obtainable using TDDFT - a formally exact extension of conventional DFT that describes electron dynamics and excited states. In order to develop a capability for modeling XRTS data and, more generally, to establish a predictive capability for rst principles simulations of matter in extreme conditions, real-time TDDFT with Ehrenfest dynamics has been implemented in an existing PAW code for DFT-MD calculations. The purpose of this report is to record implementation details and benchmarks as the project advances from software development to delivering novel scienti c results. Results range from tests that establish the accuracy, e ciency, and scalability of our implementation, to calculations that are veri ed against accepted results in the literature. Aside from the primary XRTS goal, we identify other more general areas where this new capability will be useful, including stopping power calculations and electron-ion equilibration.

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On the scaling of the magnetically accelerated flyer plate technique to currents greater than 20 MA

Journal of Physics: Conference Series

Lemke, Raymond W.; Knudson, Marcus D.; Cochrane, Kyle C.; Desjarlais, Michael P.; Asay, J.R.

In this article we discuss scaling the magnetically accelerated flyer plate technique to currents greater than is available on the Z accelerator. Peak flyer plate speeds in the range 7-46 km/s are achieved in pulsed power driven, hyper-velocity impact experiments on Z for peak currents in the range 8-20 MA. The highest (lowest) speeds are produced using aluminum (aluminum-copper) flyer plates. In either case, the ≈1 mm thick flyer plate is shocklessly accelerated by magnetic pressure to ballistic speed in ≈400 ns; it arrives at the target with a fraction of material at standard density. During acceleration a melt front, due to resistive heating, moves from the drive-side toward the target-side of the flyer plate; the speed of the melt front increases with increasing current. Peak flyer speeds on Z scale quadratically (linearly) with current at the low (high) end of the range. Magnetohydrodynamic simulation shows that the change in scaling is due to geometric deformation, and that linear scaling continues as current increases. However, the combined effects of shockless acceleration and resistive heating lead to an upper bound on the magnetic field feasible for pulsed power driven flyer plate experiments, which limits the maximum possible speed of a useful flyer plate to < 100 km/s. © Published under licence by IOP Publishing Ltd.

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Density Functional Theory (DFT) simulations of porous tantalum pentoxide

Journal of Physics: Conference Series

Cochrane, K.R.; Vogler, Tracy V.; Desjarlais, Michael P.; Mattsson, Thomas M.

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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First-principles calculation of entropy for liquid metals

Physical Review E - Statistical, Nonlinear, and Soft Matter Physics

Desjarlais, Michael P.

We demonstrate the accurate calculation of entropies and free energies for a variety of liquid metals using an extension of the two-phase thermodynamic (2PT) model based on a decomposition of the velocity autocorrelation function into gas-like (hard sphere) and solid-like (harmonic) subsystems. The hard sphere model for the gas-like component is shown to give systematically high entropies for liquid metals as a direct result of the unphysical Lorentzian high-frequency tail. Using a memory function framework we derive a generally applicable velocity autocorrelation and frequency spectrum for the diffusive component which recovers the low-frequency (long-time) behavior of the hard sphere model while providing for realistic short-time coherence and high-frequency tails to the spectrum. This approach provides a significant increase in the accuracy of the calculated entropies for liquid metals and is compared to ambient pressure data for liquid sodium, aluminum, gallium, tin, and iron. The use of this method for the determination of melt boundaries is demonstrated with a calculation of the high-pressure bcc melt boundary for sodium. With the significantly improved accuracy available with the memory function treatment for softer interatomic potentials, the 2PT model for entropy calculations should find broader application in high energy density science, warm dense matter, planetary science, geophysics, and material science. © 2013 American Physical Society.

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Electrical conductivity in oxygen-deficient phases of transition metal oxides from first-principles calculations

Desjarlais, Michael P.; Thompson, Aidan P.; Brennecka, Geoffrey L.; Marinella, Matthew J.

Density-functional theory calculations, ab-initio molecular dynamics, and the Kubo-Greenwood formula are applied to predict electrical conductivity in Ta2Ox (0 x 5) as a function of composition, phase, and temperature, where additional focus is given to various oxidation states of the O monovacancy (VOn; n=0,1+,2+). Our calculations of DC conductivity at 300K agree well with experimental measurements taken on Ta2Ox thin films and bulk Ta2O5 powder-sintered pellets, although simulation accuracy can be improved for the most insulating, stoichiometric compositions. Our conductivity calculations and further interrogation of the O-deficient Ta2O5 electronic structure provide further theoretical basis to substantiate VO0 as a donor dopant in Ta2O5 and other metal oxides. Furthermore, this dopant-like behavior appears specific to neutral VO cases in both Ta2O5 and TiO2 and was not observed in other oxidation states. This suggests that reduction and oxidation reactions may effectively act as donor activation and deactivation mechanisms, respectively, for VO0 in transition metal oxides.

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ALEGRA Update: Modernization and Resilience Progress

Robinson, Allen C.; Petney, Sharon P.; Drake, Richard R.; Weirs, Vincent G.; Adams, Brian M.; Vigil, Dena V.; Carpenter, John H.; Garasi, Christopher J.; Wong, Michael K.; Robbins, Joshua R.; Siefert, Christopher S.; Strack, Otto E.; Wills, Ann E.; Trucano, Timothy G.; Bochev, Pavel B.; Summers, Randall M.; Stewart, James R.; Ober, Curtis C.; Rider, William J.; Haill, Thomas A.; Lemke, Raymond W.; Cochrane, Kyle C.; Desjarlais, Michael P.; Love, Edward L.; Voth, Thomas E.; Mosso, Stewart J.; Niederhaus, John H.

Abstract not provided.

Results 76–100 of 175
Results 76–100 of 175