The calculations of small molecular conformation energy differences by density functional method

NASA Astrophysics Data System (ADS)

Topol, I. A.; Burt, S. K.

1993-03-01

The differences in the conformational energies for the gauche (G) and trans(T) conformers of 1,2-difluoroethane and for myo-and scyllo-conformer of inositol have been calculated by local density functional method (LDF approximation) with geometry optimization using different sets of calculation parameters. It is shown that in the contrast to Hartree—Fock methods, density functional calculations reproduce the correct sign and value of the gauche effect for 1,2-difluoroethane and energy difference for both conformers of inositol. The results of normal vibrational analysis for1,2-difluoroethane showed that harmonic frequencies calculated in LDF approximation agree with experimental data with the accuracy typical for scaled large basis set Hartree—Fock calculations.

Total-energy Assisted Tight-binding Method Based on Local Density Approximation of Density Functional Theory

NASA Astrophysics Data System (ADS)

Fujiwara, Takeo; Nishino, Shinya; Yamamoto, Susumu; Suzuki, Takashi; Ikeda, Minoru; Ohtani, Yasuaki

2018-06-01

A novel tight-binding method is developed, based on the extended Hückel approximation and charge self-consistency, with referring the band structure and the total energy of the local density approximation of the density functional theory. The parameters are so adjusted by computer that the result reproduces the band structure and the total energy, and the algorithm for determining parameters is established. The set of determined parameters is applicable to a variety of crystalline compounds and change of lattice constants, and, in other words, it is transferable. Examples are demonstrated for Si crystals of several crystalline structures varying lattice constants. Since the set of parameters is transferable, the present tight-binding method may be applicable also to molecular dynamics simulations of large-scale systems and long-time dynamical processes.

DFTB3: Extension of the self-consistent-charge density-functional tight-binding method (SCC-DFTB).

PubMed

Gaus, Michael; Cui, Qiang; Elstner, Marcus

2012-04-10

The self-consistent-charge density-functional tight-binding method (SCC-DFTB) is an approximate quantum chemical method derived from density functional theory (DFT) based on a second-order expansion of the DFT total energy around a reference density. In the present study we combine earlier extensions and improve them consistently with, first, an improved Coulomb interaction between atomic partial charges, and second, the complete third-order expansion of the DFT total energy. These modifications lead us to the next generation of the DFTB methodology called DFTB3, which substantially improves the description of charged systems containing elements C, H, N, O, and P, especially regarding hydrogen binding energies and proton affinities. As a result, DFTB3 is particularly applicable to biomolecular systems. Remaining challenges and possible solutions are also briefly discussed.

A mathematical method for quantifying in vivo mechanical behaviour of heel pad under dynamic load.

PubMed

Naemi, Roozbeh; Chatzistergos, Panagiotis E; Chockalingam, Nachiappan

2016-03-01

Mechanical behaviour of the heel pad, as a shock attenuating interface during a foot strike, determines the loading on the musculoskeletal system during walking. The mathematical models that describe the force deformation relationship of the heel pad structure can determine the mechanical behaviour of heel pad under load. Hence, the purpose of this study was to propose a method of quantifying the heel pad stress-strain relationship using force-deformation data from an indentation test. The energy input and energy returned densities were calculated by numerically integrating the area below the stress-strain curve during loading and unloading, respectively. Elastic energy and energy absorbed densities were calculated as the sum of and the difference between energy input and energy returned densities, respectively. By fitting the energy function, derived from a nonlinear viscoelastic model, to the energy density-strain data, the elastic and viscous model parameters were quantified. The viscous and elastic exponent model parameters were significantly correlated with maximum strain, indicating the need to perform indentation tests at realistic maximum strains relevant to walking. The proposed method showed to be able to differentiate between the elastic and viscous components of the heel pad response to loading and to allow quantifying the corresponding stress-strain model parameters.

Effects of various light curing methods on the leachability of uncured substances and hardness of a composite resin.

PubMed

Moon, H-J; Lee, Y-K; Lim, B-S; Kim, C-W

2004-03-01

The purpose of this study was to evaluate the effect of the various light curing units (plasma arc, halogen and light-emitting diodes) and irradiation methods (one-step, two-step and pulse) using different light energy densities on the leachability of unreacted monomers (Bis-GMA and UDMA) and the surface hardness of a composite resin (Z250, 3M). Leachability of the specimens immersed for 7 days in ethanol was analysed by HPLC. Vicker's hardness number (VHN) was measured immediately after curing (IC) and after immersion in ethanol for 7 days. Various irradiation methods with three curing units resulted in differences in the amount of leached monomers and VHN of IC when light energy density was lower than 17.0 J cm(-2) (P = 0.05). However, regardless of curing units and irradiation methods, these results were not different when the time or light energy density increased. When similar light energy density was irradiated (15.6-17.7 J cm(-2)), the efficiency of irradiation methods was different by the following order: one-step > or = two-step > pulse. These results suggest that the amount of leached monomers and VHN were influenced by forming polymer structure in activation and initiation stages of polymerization process with different light source energies and curing times.

Low cost estimation of the contribution of post-CCSD excitations to the total atomization energy using density functional theory calculations

NASA Astrophysics Data System (ADS)

Sánchez, H. R.; Pis Diez, R.

2016-04-01

Based on the Aλ diagnostic for multireference effects recently proposed [U.R. Fogueri, S. Kozuch, A. Karton, J.M. Martin, Theor. Chem. Acc. 132 (2013) 1], a simple method for improving total atomization energies and reaction energies calculated at the CCSD level of theory is proposed. The method requires a CCSD calculation and two additional density functional theory calculations for the molecule. Two sets containing 139 and 51 molecules are used as training and validation sets, respectively, for total atomization energies. An appreciable decrease in the mean absolute error from 7-10 kcal mol-1 for CCSD to about 2 kcal mol-1 for the present method is observed. The present method provides atomization energies and reaction energies that compare favorably with relatively recent scaled CCSD methods.

Method for obtaining electron energy-density functions from Langmuir-probe data using a card-programmable calculator

DOE Office of Scientific and Technical Information (OSTI.GOV)

Longhurst, G.R.

This paper presents a method for obtaining electron energy density functions from Langmuir probe data taken in cool, dense plasmas where thin-sheath criteria apply and where magnetic effects are not severe. Noise is filtered out by using regression of orthogonal polynomials. The method requires only a programmable calculator (TI-59 or equivalent) to implement and can be used for the most general, nonequilibrium electron energy distribution plasmas. Data from a mercury ion source analyzed using this method are presented and compared with results for the same data using standard numerical techniques.

An empirical model for parameters affecting energy consumption in boron removal from boron-containing wastewaters by electrocoagulation.

PubMed

Yilmaz, A Erdem; Boncukcuoğlu, Recep; Kocakerim, M Muhtar

2007-06-01

In this study, it was investigated parameters affecting energy consumption in boron removal from boron containing wastewaters prepared synthetically, via electrocoagulation method. The solution pH, initial boron concentration, dose of supporting electrolyte, current density and temperature of solution were selected as experimental parameters affecting energy consumption. The obtained experimental results showed that boron removal efficiency reached up to 99% under optimum conditions, in which solution pH was 8.0, current density 6.0 mA/cm(2), initial boron concentration 100mg/L and solution temperature 293 K. The current density was an important parameter affecting energy consumption too. High current density applied to electrocoagulation cell increased energy consumption. Increasing solution temperature caused to decrease energy consumption that high temperature decreased potential applied under constant current density. That increasing initial boron concentration and dose of supporting electrolyte caused to increase specific conductivity of solution decreased energy consumption. As a result, it was seen that energy consumption for boron removal via electrocoagulation method could be minimized at optimum conditions. An empirical model was predicted by statistically. Experimentally obtained values were fitted with values predicted from empirical model being as following; [formula in text]. Unfortunately, the conditions obtained for optimum boron removal were not the conditions obtained for minimum energy consumption. It was determined that support electrolyte must be used for increase boron removal and decrease electrical energy consumption.

Magnetic exchange couplings from constrained density functional theory: an efficient approach utilizing analytic derivatives.

PubMed

Phillips, Jordan J; Peralta, Juan E

2011-11-14

We introduce a method for evaluating magnetic exchange couplings based on the constrained density functional theory (C-DFT) approach of Rudra, Wu, and Van Voorhis [J. Chem. Phys. 124, 024103 (2006)]. Our method shares the same physical principles as C-DFT but makes use of the fact that the electronic energy changes quadratically and bilinearly with respect to the constraints in the range of interest. This allows us to use coupled perturbed Kohn-Sham spin density functional theory to determine approximately the corrections to the energy of the different spin configurations and construct a priori the relevant energy-landscapes obtained by constrained spin density functional theory. We assess this methodology in a set of binuclear transition-metal complexes and show that it reproduces very closely the results of C-DFT. This demonstrates a proof-of-concept for this method as a potential tool for studying a number of other molecular phenomena. Additionally, routes to improving upon the limitations of this method are discussed. © 2011 American Institute of Physics

Temperature dependence of the symmetry energy and neutron skins in Ni, Sn, and Pb isotopic chains

NASA Astrophysics Data System (ADS)

Antonov, A. N.; Kadrev, D. N.; Gaidarov, M. K.; Sarriguren, P.; de Guerra, E. Moya

2017-02-01

The temperature dependence of the symmetry energy for isotopic chains of even-even Ni, Sn, and Pb nuclei is investigated in the framework of the local density approximation (LDA). The Skyrme energy density functional with two Skyrme-class effective interactions, SkM* and SLy4, is used in the calculations. The temperature-dependent proton and neutron densities are calculated through the hfbtho code that solves the nuclear Skyrme-Hartree-Fock-Bogoliubov problem by using the cylindrical transformed deformed harmonic-oscillator basis. In addition, two other density distributions of 208Pb, namely the Fermi-type density determined within the extended Thomas-Fermi (TF) method and symmetrized-Fermi local density obtained within the rigorous density functional approach, are used. The kinetic energy densities are calculated either by the hfbtho code or, for a comparison, by the extended TF method up to second order in temperature (with T2 term). Alternative ways to calculate the symmetry energy coefficient within the LDA are proposed. The results for the thermal evolution of the symmetry energy coefficient in the interval T =0 -4 MeV show that its values decrease with temperature. The temperature dependence of the neutron and proton root-mean-square radii and corresponding neutron skin thickness is also investigated, showing that the effect of temperature leads mainly to a substantial increase of the neutron radii and skins, especially in the more neutron-rich nuclei, a feature that may have consequences on astrophysical processes and neutron stars.

Density functional theory calculations of the water interactions with ZrO2 nanoparticles Y2O3 doped

NASA Astrophysics Data System (ADS)

Subhoni, Mekhrdod; Kholmurodov, Kholmirzo; Doroshkevich, Aleksandr; Asgerov, Elmar; Yamamoto, Tomoyuki; Lyubchyk, Andrei; Almasan, Valer; Madadzada, Afag

2018-03-01

Development of a new electricity generation techniques is one of the most relevant tasks, especially nowadays under conditions of extreme growth in energy consumption. The exothermic heterogeneous electrochemical energy conversion to the electric energy through interaction of the ZrO2 based nanopowder system with atmospheric moisture is one of the ways of electric energy obtaining. The questions of conversion into the electric form of the energy of water molecules adsorption in 3 mol% Y2O3 doped ZrO2 nanopowder systems were investigated using the density functional theory calculations. The density functional theory calculations has been realized as in the Kohn-Sham formulation, where the exchange-correlation potential is approximated by a functional of the electronic density. The electronic density, total energy and band structure calculations are carried out using the all-electron, full potential, linear augmented plane wave method of the electronic density and related approximations, i.e. the local density, the generalized gradient and their hybrid approximations.

Substrate Engineered Interconnected Graphene Electrodes with Ultrahigh Energy and Power Densities for Energy Storage Applications.

PubMed

Chaichi, Ardalan; Wang, Ying; Gartia, Manas Ranjan

2018-06-27

Supercapacitors combine the advantages of electrochemical storage technologies such as high energy density batteries and high power density capacitors. At 5-10 W h kg -1 , the energy densities of current supercapacitors are still significantly lower than the energy densities of lead acid (20-35 W h kg -1 ), Ni-metal hydride (40-100 W h kg -1 ), and Li-ion (120-170 W h kg -1 ) batteries. Recently, graphene-based supercapacitors have shown an energy density of 40-80 W h kg -1 . However, their performance is mainly limited because of the reversible agglomeration and restacking of individual graphene layers caused by π-π interactions. The restacking of graphene layers leads to significant decrease of ion-accessible surface area and the low capacitance of graphene-based supercapacitors. Here, we introduce a microstructure substrate-based method to produce a fully delaminated and stable interconnected graphene structure using flash reduction of graphene oxide in a few seconds. With this structure, we achieve the highest amount of volumetric capacitance obtained so far by any type of a pure carbon-based material. The affordable and scalable production method is capable of producing electrodes with an energy density of 0.37 W h cm -3 and a power density of 416.6 W cm -3 . This electrode maintained more than 91% of its initial capacitance after 5000 cycles. Moreover, combining with ionic liquid, this solvent-free graphene electrode material is highly promising for on-chip electronics, micro-supercapacitors, as well as high-power applications.

First-Principles Prediction of Densities of Amorphous Materials: The Case of Amorphous Silicon

NASA Astrophysics Data System (ADS)

Furukawa, Yoritaka; Matsushita, Yu-ichiro

2018-02-01

A novel approach to predict the atomic densities of amorphous materials is explored on the basis of Car-Parrinello molecular dynamics (CPMD) in density functional theory. Despite the determination of the atomic density of matter being crucial in understanding its physical properties, no first-principles method has ever been proposed for amorphous materials until now. We have extended the conventional method for crystalline materials in a natural manner and pointed out the importance of the canonical ensemble of the total energy in the determination of the atomic densities of amorphous materials. To take into account the canonical distribution of the total energy, we generate multiple amorphous structures with several different volumes by CPMD simulations and average the total energies at each volume. The density is then determined as the one that minimizes the averaged total energy. In this study, this approach is implemented for amorphous silicon (a-Si) to demonstrate its validity, and we have determined the density of a-Si to be 4.1% lower and its bulk modulus to be 28 GPa smaller than those of the crystal, which are in good agreement with experiments. We have also confirmed that generating samples through classical molecular dynamics simulations produces a comparable result. The findings suggest that the presented method is applicable to other amorphous systems, including those for which experimental knowledge is lacking.

Size-Dependent Surface Energy Density of Spherical Face-Centered-Cubic Metallic Nanoparticles.

PubMed

Wei, Yaochi; Chen, Shaohua

2015-12-01

The surface energy density of nano-sized elements exhibits a significantly size-dependent behavior. Spherical nanoparticle, as an important element in nano-devices and nano-composites, has attracted many interesting studies on size effect, most of which are molecular dynamics (MD) simulations. However, the existing MD calculations yield two opposite size-dependent trends of surface energy density of nanoparticles. In order to clarify such a real underlying problem, atomistic calculations are carried out in the present paper for various spherical face-centered-cubic (fcc) metallic nanoparticles. Both the embedded atom method (EAM) potential and the modified embedded atom method (MEAM) one are adopted. It is found that the size-dependent trend of surface energy density of nanoparticles is not governed by the chosen potential function or variation trend of surface energy, but by the defined radius of spherical nanoparticles in MD models. The finding in the present paper should be helpful for further theoretical studies on surface/interface effect of nanoparticles and nanoparticle-reinforced composites.

Generalization of the Kohn-Sham system that can represent arbitrary one-electron density matrices

DOE PAGES

Hubertus J. J. van Dam

2016-04-27

Density functional theory is currently the most widely applied method in electronic structure theory. The Kohn-Sham method, based on a fictitious system of noninteracting particles, is the workhorse of the theory. The particular form of the Kohn-Sham wave function admits only idempotent one-electron density matrices whereas wave functions of correlated electrons in post-Hartree-Fock methods invariably have fractional occupation numbers. Here we show that by generalizing the orbital concept and introducing a suitable dot product as well as a probability density, a noninteracting system can be chosen that can represent the one-electron density matrix of any system, even one with fractionalmore » occupation numbers. This fictitious system ensures that the exact electron density is accessible within density functional theory. It can also serve as the basis for reduced density matrix functional theory. Moreover, to aid the analysis of the results the orbitals may be assigned energies from a mean-field Hamiltonian. This produces energy levels that are akin to Hartree-Fock orbital energies such that conventional analyses based on Koopmans' theorem are available. Lastly, this system is convenient in formalisms that depend on creation and annihilation operators as they are trivially applied to single-determinant wave functions.« less

Correlation of the neutron star crust-core properties with the slope of the symmetry energy and the lead skin thickness

NASA Astrophysics Data System (ADS)

Pais, H.; Sulaksono, A.; Agrawal, B. K.; Providência, C.

2016-04-01

The correlations of the crust-core transition density and pressure in neutron stars with the slope of the symmetry energy and the neutron skin thickness are investigated, using different families of relativistic mean-field parametrizations with constant couplings and nonlinear terms mixing the σ - , ω - , and ρ -meson fields. It is shown that the modification of the density dependence of the symmetry energy, involving the σ or the ω meson, gives rise to different behaviors: the effect of the ω meson may also be reproduced within nonrelativistic phenomenological models, while the effect of the σ meson is essentially relativistic. Depending on the parametrization with σ -ρ or ω -ρ mixing terms, different values of the slope of the symmetry energy at saturation must be considered in order to obtain a neutron matter equation of state compatible with results from chiral effective field theory. This difference leads to different pressures at the crust-core transition density. A linear correlation between the transition density and the symmetry energy slope or the neutron skin thickness of the 208Pb nucleus is obtained, only when the ω meson is used to describe the density dependence of the symmetry energy. A comparison is made between the crust-core transition properties of neutron stars obtained by three different methods, the relativistic random phase approximation (RRPA), the Vlasov equation, and thermodynamical method. It is shown that the RRPA and the Vlasov methods predict similar transition densities for p n e β -equilibrium stellar matter.

Estimation of Metal Acceleration by an SF5 Containing Explosive

DTIC Science & Technology

1991-06-30

cylinder wall acceleration, the wall energies for the baseline composition and for the composition CW2 were calculated by three different methods : KSM, 6...computaticno! method to calculate the cylinder energies needed for comparison with expermental data, it was decided to compare data from three known methods ...detonation pressure given for the GAB method in Reference 8. They are E(6mm) = 0.1272 (Isp X density)1 .5 - 0.021, and E(l9mm) = 0.1580 (Isp x density) 1 .5

Simple and exact approach to the electronic polarization effect on the solvation free energy: formulation for quantum-mechanical/molecular-mechanical system and its applications to aqueous solutions.

PubMed

Takahashi, Hideaki; Omi, Atsushi; Morita, Akihiro; Matubayasi, Nobuyuki

2012-06-07

We present a simple and exact numerical approach to compute the free energy contribution δμ in solvation due to the electron density polarization and fluctuation of a quantum-mechanical solute in the quantum-mechanical/molecular-mechanical (QM/MM) simulation combined with the theory of the energy representation (QM/MM-ER). Since the electron density fluctuation is responsible for the many-body QM-MM interactions, the standard version of the energy representation method cannot be applied directly. Instead of decomposing the QM-MM polarization energy into the pairwise additive and non-additive contributions, we take sum of the polarization energies in the QM-MM interaction and adopt it as a new energy coordinate for the method of energy representation. Then, it is demonstrated that the free energy δμ can be exactly formulated in terms of the energy distribution functions for the solution and reference systems with respect to this energy coordinate. The benchmark tests were performed to examine the numerical efficiency of the method with respect to the changes in the individual properties of the solvent and the solute. Explicitly, we computed the solvation free energy of a QM water molecule in ambient and supercritical water, and also the free-energy change associated with the isomerization reaction of glycine from neutral to zwitterionic structure in aqueous solution. In all the systems examined, it was demonstrated that the computed free energy δμ agrees with the experimental value, irrespective of the choice of the reference electron density of the QM solute. The present method was also applied to a prototype reaction of adenosine 5'-triphosphate hydrolysis where the effect of the electron density fluctuation is substantial due to the excess charge. It was demonstrated that the experimental free energy of the reaction has been accurately reproduced with the present approach.

Functional renormalization group and Kohn-Sham scheme in density functional theory

NASA Astrophysics Data System (ADS)

Liang, Haozhao; Niu, Yifei; Hatsuda, Tetsuo

2018-04-01

Deriving accurate energy density functional is one of the central problems in condensed matter physics, nuclear physics, and quantum chemistry. We propose a novel method to deduce the energy density functional by combining the idea of the functional renormalization group and the Kohn-Sham scheme in density functional theory. The key idea is to solve the renormalization group flow for the effective action decomposed into the mean-field part and the correlation part. Also, we propose a simple practical method to quantify the uncertainty associated with the truncation of the correlation part. By taking the φ4 theory in zero dimension as a benchmark, we demonstrate that our method shows extremely fast convergence to the exact result even for the highly strong coupling regime.

Nuclear shape evolution based on microscopic level densities

DOE PAGES

Ward, D. E.; Carlsson, B. G.; Døssing, T.; ...

2017-02-27

Here, by combining microscopically calculated level densities with the Metropolis walk method, we develop a consistent framework for treating the energy and angular-momentum dependence of the nuclear shape evolution in the fission process. For each nucleus under consideration, the level density is calculated microscopically for each of more than five million shapes with a recently developed combinatorial method. The method employs the same single-particle levels as those used for the extraction of the pairing and shell contributions to the macroscopic-microscopic deformation-energy surface. Containing no new parameters, the treatment is suitable for elucidating the energy dependence of the dynamics of warmmore » nuclei on pairing and shell effects. It is illustrated for the fission fragment mass distribution for several uranium and plutonium isotopes of particular interest.« less

Exact kinetic energy enables accurate evaluation of weak interactions by the FDE-vdW method.

PubMed

Sinha, Debalina; Pavanello, Michele

2015-08-28

The correlation energy of interaction is an elusive and sought-after interaction between molecular systems. By partitioning the response function of the system into subsystem contributions, the Frozen Density Embedding (FDE)-vdW method provides a computationally amenable nonlocal correlation functional based on the adiabatic connection fluctuation dissipation theorem applied to subsystem density functional theory. In reproducing potential energy surfaces of weakly interacting dimers, we show that FDE-vdW, either employing semilocal or exact nonadditive kinetic energy functionals, is in quantitative agreement with high-accuracy coupled cluster calculations (overall mean unsigned error of 0.5 kcal/mol). When employing the exact kinetic energy (which we term the Kohn-Sham (KS)-vdW method), the binding energies are generally closer to the benchmark, and the energy surfaces are also smoother.

Exact kinetic energy enables accurate evaluation of weak interactions by the FDE-vdW method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sinha, Debalina; Pavanello, Michele, E-mail: m.pavanello@rutgers.edu

2015-08-28

The correlation energy of interaction is an elusive and sought-after interaction between molecular systems. By partitioning the response function of the system into subsystem contributions, the Frozen Density Embedding (FDE)-vdW method provides a computationally amenable nonlocal correlation functional based on the adiabatic connection fluctuation dissipation theorem applied to subsystem density functional theory. In reproducing potential energy surfaces of weakly interacting dimers, we show that FDE-vdW, either employing semilocal or exact nonadditive kinetic energy functionals, is in quantitative agreement with high-accuracy coupled cluster calculations (overall mean unsigned error of 0.5 kcal/mol). When employing the exact kinetic energy (which we term themore » Kohn-Sham (KS)-vdW method), the binding energies are generally closer to the benchmark, and the energy surfaces are also smoother.« less

Interference of interchromophoric energy-transfer pathways in π-conjugated macrocycles

DOE PAGES

Alfonso Hernandez, Laura; Nelson, Tammie Renee; Gelin, Maxim F.; ...

2016-11-10

The interchromophoric energy-transfer pathways between weakly coupled units in a π-conjugated phenylene–ethynylene macrocycle and its half-ring analogue have been investigated using the nonadiabatic excited-state molecular dynamics approach. To track the flow of electronic transition density between macrocycle units, we formulate a transition density flux analysis adapted from the statistical minimum flow method previously developed to investigate vibrational energy flow. Following photoexcitation, transition density is primarily delocalized on two chromophore units and the system undergoes ultrafast energy transfer, creating a localized excited state on a single unit. In the macrocycle, distinct chromophore units donate transition density to a single acceptor unitmore » but do not interchange transition density among each other. We find that energy transfer in the macrocycle is slower than in the corresponding half ring because of the presence of multiple interfering energy-transfer pathways. Finally, simulation results are validated by modeling the fluorescence anisotropy decay.« less

Method using a density field for locating related items for data mining

DOEpatents

Wylie, Brian N.

2002-01-01

A method for locating related items in a geometric space transforms relationships among items to geometric locations. The method locates items in the geometric space so that the distance between items corresponds to the degree of relatedness. The method facilitates communication of the structure of the relationships among the items. The method makes use of numeric values as a measure of similarity between each pairing of items. The items are given initial coordinates in the space. An energy is then determined for each item from the item's distance and similarity to other items, and from the density of items assigned coordinates near the item. The distance and similarity component can act to draw items with high similarities close together, while the density component can act to force all items apart. If a terminal condition is not yet reached, then new coordinates can be determined for one or more items, and the energy determination repeated. The iteration can terminate, for example, when the total energy reaches a threshold, when each item's energy is below a threshold, after a certain amount of time or iterations.

Indirect Measurement of Energy Density of Soft PZT Ceramic Utilizing Mechanical Stress

NASA Astrophysics Data System (ADS)

Unruan, Muangjai; Unruan, Sujitra; Inkong, Yutthapong; Yimnirun, Rattikorn

2017-11-01

This paper reports on an indirect measurement of energy density of soft PZT ceramic utilizing mechanical stress. The method works analogous to the Olsen cycle and allows for a large amount of electro-mechanical energy conversion. A maximum energy density of 350 kJ/m3/cycle was found under 0-312 MPa and 1-20 kV/cm of applied mechanical stress and electric field, respectively. The obtained result is substantially higher than the results reported in previous studies of PZT materials utilizing a direct piezoelectric effect.

Longitudinal density modulation and energy conversion in intense beams.

PubMed

Harris, J R; Neumann, J G; Tian, K; O'Shea, P G

2007-08-01

Density modulation of charged particle beams may occur as a consequence of deliberate action, or may occur inadvertently because of imperfections in the particle source or acceleration method. In the case of intense beams, where space charge and external focusing govern the beam dynamics, density modulation may, under some circumstances, be converted to velocity modulation, with a corresponding conversion of potential energy to kinetic energy. Whether this will occur depends on the properties of the beam and the initial modulation. This paper describes the evolution of discrete and continuous density modulations on intense beams and discusses three recent experiments related to the dynamics of density-modulated electron beams.

Analysis of multi-layered films. [determining dye densities by applying a regression analysis to the spectral response of the composite transparency

NASA Technical Reports Server (NTRS)

Scarpace, F. L.; Voss, A. W.

1973-01-01

Dye densities of multi-layered films are determined by applying a regression analysis to the spectral response of the composite transparency. The amount of dye in each layer is determined by fitting the sum of the individual dye layer densities to the measured dye densities. From this, dye content constants are calculated. Methods of calculating equivalent exposures are discussed. Equivalent exposures are a constant amount of energy over a limited band-width that will give the same dye content constants as the real incident energy. Methods of using these equivalent exposures for analysis of photographic data are presented.

Generalized variational approach to Kim-Gordon electron gas theory for ionic crystals

NASA Astrophysics Data System (ADS)

Ivanov, O. V.; Maksimov, E. G.

1996-01-01

The generalized approach to the Kim-Gordon electron gas model is proposed. The total density of a crystal is considered as a superposition of densities of individual overlapping ions. The possible distortions of individual ion densities are calculated in the presence of some auxiliary external potentials. The real values of these distortions are calculated by a variational method from the minimum total energy of a crystal. The proper prescription of the ion self-energy with a distorted density is given using the method elaborated in the nonequilibrium thermodynamics. Some examples of the calculation for phonon frequencies are presented and demonstrate a good agreement with experimental data.

Probability density of tunneled carrier states near heterojunctions calculated numerically by the scattering method.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wampler, William R.; Myers, Samuel M.; Modine, Normand A.

2017-09-01

The energy-dependent probability density of tunneled carrier states for arbitrarily specified longitudinal potential-energy profiles in planar bipolar devices is numerically computed using the scattering method. Results agree accurately with a previous treatment based on solution of the localized eigenvalue problem, where computation times are much greater. These developments enable quantitative treatment of tunneling-assisted recombination in irradiated heterojunction bipolar transistors, where band offsets may enhance the tunneling effect by orders of magnitude. The calculations also reveal the density of non-tunneled carrier states in spatially varying potentials, and thereby test the common approximation of uniform- bulk values for such densities.

Talbot-Lau x-ray interferometry for high energy density plasma diagnostic.

PubMed

Stutman, D; Finkenthal, M

2011-11-01

High resolution density diagnostics are difficult in high energy density laboratory plasmas (HEDLP) experiments due to the scarcity of probes that can penetrate above solid density plasmas. Hard x-rays are one possible probe for such dense plasmas. We study the possibility of applying an x-ray method recently developed for medical imaging, differential phase-contrast with Talbot-Lau interferometers, for the diagnostic of electron density and small-scale hydrodynamic instabilities in HEDLP experiments. The Talbot method uses micro-periodic gratings to measure the refraction and ultra-small angle scatter of x-rays through an object and is attractive for HEDLP diagnostic due to its capability to work with incoherent and polychromatic x-ray sources such as the laser driven backlighters used for HEDLP radiography. Our paper studies the potential of the Talbot method for HEDLP diagnostic, its adaptation to the HEDLP environment, and its extension of high x-ray energy using micro-periodic mirrors. The analysis is illustrated with experimental results obtained using a laboratory Talbot interferometer. © 2011 American Institute of Physics

Performance of the DFTB method in comparison to DFT and semiempirical methods for geometries and energies of C20-C86fullerene isomers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zheng, Guishan; Irle, Stephan; Morokuma, Keiji

2005-07-20

The research described in this product was performed in part in the Environmental Molecular Sciences Laboratory, a national scientific user facility sponsored by the Department of Energy's Office of Biological and Environmental Research and located at Pacific Northwest National Laboratory. The performance of both non-iterative (NCC) and self-consistent charge (SCC) versions of the density functional tight binding (DFTB) method, as well as AM1 and PM3 methods, has been compared with the B3LYP method, a hybrid density functional theory (DFT) method, for equilibrium geometries and relative energies of various isomers of C20–C86 fullerenes. Both NCC- and SCCDFTB methods compare very favorablymore » with B3LYP both in geometries and isomer relative energies, while AM1 and PM3 do noticeably worse.« less

Handling Density Conversion in TPS.

PubMed

Isobe, Tomonori; Mori, Yutaro; Takei, Hideyuki; Sato, Eisuke; Tadano, Kiichi; Kobayashi, Daisuke; Tomita, Tetsuya; Sakae, Takeji

2016-01-01

Conversion from CT value to density is essential to a radiation treatment planning system. Generally CT value is converted to the electron density in photon therapy. In the energy range of therapeutic photon, interactions between photons and materials are dominated with Compton scattering which the cross-section depends on the electron density. The dose distribution is obtained by calculating TERMA and kernel using electron density where TERMA is the energy transferred from primary photons and kernel is a volume considering spread electrons. Recently, a new method was introduced which uses the physical density. This method is expected to be faster and more accurate than that using the electron density. As for particle therapy, dose can be calculated with CT-to-stopping power conversion since the stopping power depends on the electron density. CT-to-stopping power conversion table is also called as CT-to-water-equivalent range and is an essential concept for the particle therapy.

Spin-Multiplet Components and Energy Splittings by Multistate Density Functional Theory.

PubMed

Grofe, Adam; Chen, Xin; Liu, Wenjian; Gao, Jiali

2017-10-05

Kohn-Sham density functional theory has been tremendously successful in chemistry and physics. Yet, it is unable to describe the energy degeneracy of spin-multiplet components with any approximate functional. This work features two contributions. (1) We present a multistate density functional theory (MSDFT) to represent spin-multiplet components and to determine multiplet energies. MSDFT is a hybrid approach, taking advantage of both wave function theory and density functional theory. Thus, the wave functions, electron densities and energy density-functionals for ground and excited states and for different components are treated on the same footing. The method is illustrated on valence excitations of atoms and molecules. (2) Importantly, a key result is that for cases in which the high-spin components can be determined separately by Kohn-Sham density functional theory, the transition density functional in MSDFT (which describes electronic coupling) can be defined rigorously. The numerical results may be explored to design and optimize transition density functionals for configuration coupling in multiconfigurational DFT.

An accurate cost effective DFT approach to study the sensing behaviour of polypyrrole towards nitrate ions in gas and aqueous phases.

PubMed

Wasim, Fatima; Mahmood, Tariq; Ayub, Khurshid

2016-07-28

Density functional theory (DFT) calculations have been performed to study the response of polypyrrole towards nitrate ions in gas and aqueous phases. First, an accurate estimate of interaction energies is obtained by methods calibrated against the gold standard CCSD(T) method. Then, a number of low cost DFT methods are also evaluated for their ability to accurately estimate the binding energies of polymer-nitrate complexes. The low cost methods evaluated here include dispersion corrected potential (DCP), Grimme's D3 correction, counterpoise correction of the B3LYP method, and Minnesota functionals (M05-2X). The interaction energies calculated using the counterpoise (CP) correction and DCP methods at the B3LYP level are in better agreement with the interaction energies calculated using the calibrated methods. The interaction energies of an infinite polymer (polypyrrole) with nitrate ions are calculated by a variety of low cost methods in order to find the associated errors. The electronic and spectroscopic properties of polypyrrole oligomers nPy (where n = 1-9) and nPy-NO3(-) complexes are calculated, and then extrapolated for an infinite polymer through a second degree polynomial fit. Charge analysis, frontier molecular orbital (FMO) analysis and density of state studies also reveal the sensing ability of polypyrrole towards nitrate ions. Interaction energies, charge analysis and density of states analyses illustrate that the response of polypyrrole towards nitrate ions is considerably reduced in the aqueous medium (compared to the gas phase).

Continuum Level Density in Complex Scaling Method

NASA Astrophysics Data System (ADS)

Suzuki, R.; Myo, T.; Katō, K.

2005-11-01

A new calculational method of continuum level density (CLD) at unbound energies is studied in the complex scaling method (CSM). It is shown that the CLD can be calculated by employing the discretization of continuum states in the CSM without any smoothing technique.

Committor of elementary reactions on multistate systems

NASA Astrophysics Data System (ADS)

Király, Péter; Kiss, Dóra Judit; Tóth, Gergely

2018-04-01

In our study, we extend the committor concept on multi-minima systems, where more than one reaction may proceed, but the feasible data evaluation needs the projection onto partial reactions. The elementary reaction committor and the corresponding probability density of the reactive trajectories are defined and calculated on a three-hole two-dimensional model system explored by single-particle Langevin dynamics. We propose a method to visualize more elementary reaction committor functions or probability densities of reactive trajectories on a single plot that helps to identify the most important reaction channels and the nonreactive domains simultaneously. We suggest a weighting for the energy-committor plots that correctly shows the limits of both the minimal energy path and the average energy concepts. The methods also performed well on the analysis of molecular dynamics trajectories of 2-chlorobutane, where an elementary reaction committor, the probability densities, the potential energy/committor, and the free-energy/committor curves are presented.

Conformational analysis, spectroscopic study (FT-IR, FT-Raman, UV, 1H and 13C NMR), molecular orbital energy and NLO properties of 5-iodosalicylic acid

NASA Astrophysics Data System (ADS)

Karaca, Caglar; Atac, Ahmet; Karabacak, Mehmet

2015-02-01

In this study, 5-iodosalicylic acid (5-ISA, C7H5IO3) is structurally characterized by FT-IR, FT-Raman, NMR and UV spectroscopies. There are eight conformers, Cn, n = 1-8 for this molecule therefore the molecular geometry for these eight conformers in the ground state are calculated by using the ab-initio density functional theory (DFT) B3LYP method approach with the aug-cc-pVDZ-PP basis set for iodine and the aug-cc-pVDZ basis set for the other elements. The computational results identified that the most stable conformer of 5-ISA is the C1 form. The vibrational spectra are calculated DFT method invoking the same basis sets and fundamental vibrations are assigned on the basis of the total energy distribution (TED) of the vibrational modes, calculated with scaled quantum mechanics (SQM) method with PQS program. Total density of state (TDOS) and partial density of state (PDOS) and also overlap population density of state (COOP or OPDOS) diagrams analysis for C1 conformer were calculated using the same method. The energy and oscillator strength are calculated by time-dependent density functional theory (TD-DFT) results complement with the experimental findings. Besides, charge transfer occurring in the molecule between HOMO and LUMO energies, frontier energy gap, molecular electrostatic potential (MEP) are calculated and presented. The NMR chemical shifts (1H and 13C) spectra are recorded and calculated using the gauge independent atomic orbital (GIAO) method. Mulliken atomic charges of the title molecule are also calculated, interpreted and compared with salicylic acid. The optimized bond lengths, bond angles and calculated NMR and UV, vibrational wavenumbers showed the best agreement with the experimental results.

Proton elastic scattering from stable and unstable nuclei - Extraction of nuclear densities

NASA Astrophysics Data System (ADS)

Sakaguchi, H.; Zenihiro, J.

2017-11-01

Progress in proton elastic scattering at intermediate energies to determine nuclear density distributions is reviewed. After challenges of about 15 years to explain proton elastic scattering and associated polarization phenomena at intermediate energies, we have reached to some conclusions regarding proton elastic scattering as a means of obtaining nuclear densities. During this same period, physics of unstable nuclei has become of interest, and the density distributions of protons and neutrons play more important roles in unstable nuclei, since the differences in proton and neutron numbers and densities are expected to be significant. As such, proton elastic scattering experiments at intermediate energies using the inverse kinematic method have started to determine density distributions of unstable nuclei. In the region of unstable nuclei, we are confronted with a new problem when attempting to find proton and neutron densities separately from elastic proton scattering data, since electron scattering data for unstable nuclei are not presently available. We introduce a new means of determining proton and neutron densities separately by double-energy proton elastic scattering at intermediate energies.

Bypassing the malfunction junction in warm dense matter simulations

NASA Astrophysics Data System (ADS)

Cangi, Attila; Pribram-Jones, Aurora

2015-03-01

Simulation of warm dense matter requires computational methods that capture both quantum and classical behavior efficiently under high-temperature and high-density conditions. The state-of-the-art approach to model electrons and ions under those conditions is density functional theory molecular dynamics, but this method's computational cost skyrockets as temperatures and densities increase. We propose finite-temperature potential functional theory as an in-principle-exact alternative that suffers no such drawback. In analogy to the zero-temperature theory developed previously, we derive an orbital-free free energy approximation through a coupling-constant formalism. Our density approximation and its associated free energy approximation demonstrate the method's accuracy and efficiency. A.C. has been partially supported by NSF Grant CHE-1112442. A.P.J. is supported by DOE Grant DE-FG02-97ER25308.

Experimental results of use of triple-energy X-ray beam with K-edge filter in multi-energy imaging

NASA Astrophysics Data System (ADS)

Kim, D.; Lee, S.; Jeon, P.-H.

2016-04-01

Multi-energy imaging is useful for contrast enhancement of lesions, quantitative analysis of specific materials and material separation in the human body. Generally, dual-energy methods are applied to discriminating two materials, but this method cannot discriminate more than two materials. Photon-counting detectors provide spectral information from polyenergetic X-rays using multiple energy bins. In this work, we developed triple-energy X-ray beams using a filter with K-edge energy and applied them experimentally. The energy spectra of triple-energy X-ray beams were assessed by using a spectrometer. The designed triple-energy X-ray beams were validated by measuring quantitative evaluations with mean energy ratio (MER), contrast variation ratio (CVR) and exposure efficiency (EE). Then, triple-energy X-ray beams were used to extract density map of three materials, iodine (I), aluminum (Al) and polymethyl methacrylate (PMMA). The results of the thickness density maps obtained with the developed triple-energy X-ray beams were compared to those acquired using the photon-counting method. As a result, it was found experimentally that the proposed triple-energy X-ray beam technique can separate the three materials as well as the photon-counting method.

A new method to measure electron density and effective atomic number using dual-energy CT images

NASA Astrophysics Data System (ADS)

Ramos Garcia, Luis Isaac; Pérez Azorin, José Fernando; Almansa, Julio F.

2016-01-01

The purpose of this work is to present a new method to extract the electron density ({ρ\\text{e}} ) and the effective atomic number (Z eff) from dual-energy CT images, based on a Karhunen-Loeve expansion (KLE) of the atomic cross section per electron. This method was used to calibrate a Siemens Definition CT using the CIRS phantom. The predicted electron density and effective atomic number using 80 kVp and 140 kVp were compared with a calibration phantom and an independent set of samples. The mean absolute deviations between the theoretical and calculated values for all the samples were 1.7 %  ±  0.1 % for {ρ\\text{e}} and 4.1 %  ±  0.3 % for Z eff. Finally, these results were compared with other stoichiometric method. The application of the KLE to represent the atomic cross section per electron is a promising method for calculating {ρ\\text{e}} and Z eff using dual-energy CT images.

Sequential limiting in continuous and discontinuous Galerkin methods for the Euler equations

NASA Astrophysics Data System (ADS)

Dobrev, V.; Kolev, Tz.; Kuzmin, D.; Rieben, R.; Tomov, V.

2018-03-01

We present a new predictor-corrector approach to enforcing local maximum principles in piecewise-linear finite element schemes for the compressible Euler equations. The new element-based limiting strategy is suitable for continuous and discontinuous Galerkin methods alike. In contrast to synchronized limiting techniques for systems of conservation laws, we constrain the density, momentum, and total energy in a sequential manner which guarantees positivity preservation for the pressure and internal energy. After the density limiting step, the total energy and momentum gradients are adjusted to incorporate the irreversible effect of density changes. Antidiffusive corrections to bounds-compatible low-order approximations are limited to satisfy inequality constraints for the specific total and kinetic energy. An accuracy-preserving smoothness indicator is introduced to gradually adjust lower bounds for the element-based correction factors. The employed smoothness criterion is based on a Hessian determinant test for the density. A numerical study is performed for test problems with smooth and discontinuous solutions.

Density functional theory for molecular and periodic systems using density fitting and continuous fast multipole method: Analytical gradients.

PubMed

Łazarski, Roman; Burow, Asbjörn Manfred; Grajciar, Lukáš; Sierka, Marek

2016-10-30

A full implementation of analytical energy gradients for molecular and periodic systems is reported in the TURBOMOLE program package within the framework of Kohn-Sham density functional theory using Gaussian-type orbitals as basis functions. Its key component is a combination of density fitting (DF) approximation and continuous fast multipole method (CFMM) that allows for an efficient calculation of the Coulomb energy gradient. For exchange-correlation part the hierarchical numerical integration scheme (Burow and Sierka, Journal of Chemical Theory and Computation 2011, 7, 3097) is extended to energy gradients. Computational efficiency and asymptotic O(N) scaling behavior of the implementation is demonstrated for various molecular and periodic model systems, with the largest unit cell of hematite containing 640 atoms and 19,072 basis functions. The overall computational effort of energy gradient is comparable to that of the Kohn-Sham matrix formation. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.

Exchange-correlation energies of atoms from efficient density functionals: influence of the electron density

DOE PAGES

Tao, Jianmin; Ye, Lin -Hui; Duan, Yuhua

2017-11-20

The primary goal of Kohn–Sham density functional theory is to evaluate the exchange-correlation contribution to electronic properties. However, the accuracy of a density functional can be affected by the electron density. Here we apply the nonempirical Tao–Mo (TM) semilocal functional to study the influence of the electron density on the exchange and correlation energies of atoms and ions, and compare the results with the commonly used nonempirical semilocal functionals local spin-density approximation (LSDA), Perdew–Burke–Ernzerhof (PBE), Tao–Perdew–Staroverov–Scuseria (TPSS), and hybrid functional PBE0. We find that the spin-restricted Hartree–Fock density yields the exchange and correlation energies in good agreement with the Optimizedmore » Effective Potential method, particularly for spherical atoms and ions. However, the errors of these semilocal and hybrid functionals become larger for self-consistent densities. We further find that the quality of the electron density have greater effect on the exchange-correlation energies of kinetic energy density-dependent meta-GGA functionals TPSS and TM than on those of the LSDA and GGA, and therefore, should have greater influence on the performance of meta-GGA functionals. Lastly, we show that the influence of the density quality on PBE0 is slightly reduced, compared to that of PBE, due to the exact mixing.« less

Exchange-correlation energies of atoms from efficient density functionals: influence of the electron density

NASA Astrophysics Data System (ADS)

Tao, Jianmin; Ye, Lin-Hui; Duan, Yuhua

2017-12-01

The primary goal of Kohn-Sham density functional theory is to evaluate the exchange-correlation contribution to electronic properties. However, the accuracy of a density functional can be affected by the electron density. Here we apply the nonempirical Tao-Mo (TM) semilocal functional to study the influence of the electron density on the exchange and correlation energies of atoms and ions, and compare the results with the commonly used nonempirical semilocal functionals local spin-density approximation (LSDA), Perdew-Burke-Ernzerhof (PBE), Tao-Perdew-Staroverov-Scuseria (TPSS), and hybrid functional PBE0. We find that the spin-restricted Hartree-Fock density yields the exchange and correlation energies in good agreement with the Optimized Effective Potential method, particularly for spherical atoms and ions. However, the errors of these semilocal and hybrid functionals become larger for self-consistent densities. We further find that the quality of the electron density have greater effect on the exchange-correlation energies of kinetic energy density-dependent meta-GGA functionals TPSS and TM than on those of the LSDA and GGA, and therefore, should have greater influence on the performance of meta-GGA functionals. Finally, we show that the influence of the density quality on PBE0 is slightly reduced, compared to that of PBE, due to the exact mixing.

Exchange-correlation energies of atoms from efficient density functionals: influence of the electron density

DOE Office of Scientific and Technical Information (OSTI.GOV)

Tao, Jianmin; Ye, Lin -Hui; Duan, Yuhua

The primary goal of Kohn–Sham density functional theory is to evaluate the exchange-correlation contribution to electronic properties. However, the accuracy of a density functional can be affected by the electron density. Here we apply the nonempirical Tao–Mo (TM) semilocal functional to study the influence of the electron density on the exchange and correlation energies of atoms and ions, and compare the results with the commonly used nonempirical semilocal functionals local spin-density approximation (LSDA), Perdew–Burke–Ernzerhof (PBE), Tao–Perdew–Staroverov–Scuseria (TPSS), and hybrid functional PBE0. We find that the spin-restricted Hartree–Fock density yields the exchange and correlation energies in good agreement with the Optimizedmore » Effective Potential method, particularly for spherical atoms and ions. However, the errors of these semilocal and hybrid functionals become larger for self-consistent densities. We further find that the quality of the electron density have greater effect on the exchange-correlation energies of kinetic energy density-dependent meta-GGA functionals TPSS and TM than on those of the LSDA and GGA, and therefore, should have greater influence on the performance of meta-GGA functionals. Lastly, we show that the influence of the density quality on PBE0 is slightly reduced, compared to that of PBE, due to the exact mixing.« less

An actuarial approach to retrofit savings in buildings

DOE Office of Scientific and Technical Information (OSTI.GOV)

Subbarao, Krishnappa; Etingov, Pavel V.; Reddy, T. A.

An actuarial method has been developed for determining energy savings from retrofits from energy use data for a number of buildings. This method should be contrasted with the traditional method of using pre- and post-retrofit data on the same building. This method supports the U.S. Department of Energy Building Performance Database of real building performance data and related tools that enable engineering and financial practitioners to evaluate retrofits. The actuarial approach derives, from the database, probability density functions (PDFs) for energy savings from retrofits by creating peer groups for the user’s pre post buildings. From the energy use distribution ofmore » the two groups, the savings PDF is derived. This provides the basis for engineering analysis as well as financial risk analysis leading to investment decisions. Several technical issues are addressed: The savings PDF is obtained from the pre- and post-PDF through a convolution. Smoothing using kernel density estimation is applied to make the PDF more realistic. The low data density problem can be mitigated through a neighborhood methodology. Correlations between pre and post buildings are addressed to improve the savings PDF. Sample size effects are addressed through the Kolmogorov--Smirnov tests and quantile-quantile plots.« less

DOE Office of Scientific and Technical Information (OSTI.GOV)

Alfonso Hernandez, Laura; Nelson, Tammie Renee; Gelin, Maxim F.

The interchromophoric energy-transfer pathways between weakly coupled units in a π-conjugated phenylene–ethynylene macrocycle and its half-ring analogue have been investigated using the nonadiabatic excited-state molecular dynamics approach. To track the flow of electronic transition density between macrocycle units, we formulate a transition density flux analysis adapted from the statistical minimum flow method previously developed to investigate vibrational energy flow. Following photoexcitation, transition density is primarily delocalized on two chromophore units and the system undergoes ultrafast energy transfer, creating a localized excited state on a single unit. In the macrocycle, distinct chromophore units donate transition density to a single acceptor unitmore » but do not interchange transition density among each other. We find that energy transfer in the macrocycle is slower than in the corresponding half ring because of the presence of multiple interfering energy-transfer pathways. Finally, simulation results are validated by modeling the fluorescence anisotropy decay.« less

Differential heating: A versatile method for thermal conductivity measurements in high-energy-density matter

DOE PAGES

Ping, Y.; Fernandez-Panella, A.; Sio, H.; ...

2015-09-04

We propose a method for thermal conductivity measurements of high energy density matter based on differential heating. A temperature gradient is created either by surface heating of one material or at an interface between two materials by different energy deposition. The subsequent heat conduction across the temperature gradient is observed by various time-resolved probing techniques. Conceptual designs of such measurements using laser heating, proton heating, and x-ray heating are presented. As a result, the sensitivity of the measurements to thermal conductivity is confirmed by simulations.

A High Power Density Single-Phase PWM Rectifier with Active Ripple Energy Storage

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ning, Puqi; Wang, Ruxi; Wang, Fei

It is well known that there exist second-order harmonic current and corresponding ripple voltage on dc bus for single phase PWM rectifiers. The low frequency harmonic current is normally filtered using a bulk capacitor in the bus which results in low power density. This paper proposed an active ripple energy storage method that can effectively reduce the energy storage capacitance. The feed-forward control method and design considerations are provided. Simulation and 15 kW experimental results are provided for verification purposes.

Spectral densities for Frenkel exciton dynamics in molecular crystals: A TD-DFTB approach

NASA Astrophysics Data System (ADS)

Plötz, Per-Arno; Megow, Jörg; Niehaus, Thomas; Kühn, Oliver

2017-02-01

Effects of thermal fluctuations on the electronic excitation energies and intermonomeric Coulomb couplings are investigated for a perylene-tetracarboxylic-diimide crystal. To this end, time dependent density functional theory based tight binding (TD-DFTB) in the linear response formulation is used in combination with electronic ground state classical molecular dynamics. As a result, a parametrized Frenkel exciton Hamiltonian is obtained, with the effect of exciton-vibrational coupling being described by spectral densities. Employing dynamically defined normal modes, these spectral densities are analyzed in great detail, thus providing insight into the effect of specific intramolecular motions on excitation energies and Coulomb couplings. This distinguishes the present method from approaches using fixed transition densities. The efficiency by which intramolecular contributions to the spectral density can be calculated is a clear advantage of this method as compared with standard TD-DFT.

High Discharge Energy Density at Low Electric Field Using an Aligned Titanium Dioxide/Lead Zirconate Titanate Nanowire Array.

PubMed

Zhang, Dou; Liu, Weiwei; Guo, Ru; Zhou, Kechao; Luo, Hang

2018-02-01

Polymer-based capacitors with high energy density have attracted significant attention in recent years due to their wide range of potential applications in electronic devices. However, the obtained high energy density is predominantly dependent on high applied electric field, e.g., 400-600 kV mm -1 , which may bring more challenges relating to the failure probability. Here, a simple two-step method for synthesizing titanium dioxide/lead zirconate titanate nanowire arrays is exploited and a demonstration of their ability to achieve high discharge energy density capacitors for low operating voltage applications is provided. A high discharge energy density of 6.9 J cm -3 is achieved at low electric fields, i.e., 143 kV mm -1 , which is attributed to the high relative permittivity of 218.9 at 1 kHz and high polarization of 23.35 µC cm -2 at this electric field. The discharge energy density obtained in this work is the highest known for a ceramic/polymer nanocomposite at such a low electric field. The novel nanowire arrays used in this work are applicable to a wide range of fields, such as energy harvesting, energy storage, and photocatalysis.

Density function theory study of the adsorption and dissociation of carbon monoxide on tungsten nanoparticles.

PubMed

Weng, Meng-Hsiung; Ju, Shin-Pon; Chen, Hsin-Tsung; Chen, Hui-Lung; Lu, Jian-Ming; Lin, Ken-Huang; Lin, Jenn-Sen; Hsieh, Jin-Yuan; Yang, Hsi-Wen

2013-02-01

The adsorption and dissociation properties of carbon monoxide (CO) molecule on tungsten W(n) (n = 10-15) nanoparticles have been investigated by density-functional theory (DFT) calculations. The lowest-energy structures for W(n) (n = 10-15) nanoparticles are found by the basin-hopping method and big-bang method with the modified tight-binding many-body potential. We calculated the corresponding adsorption energies, C-O bond lengths and dissociation barriers for adsorption of CO on nanoparticles. The electronic properties of CO on nanoparticles are studied by the analysis of density of state and charge density. The characteristic of CO on W(n) nanoparticles are also compared with that of W bulk.

Significantly Enhanced Energy Storage Density by Modulating the Aspect Ratio of BaTiO3 Nanofibers

PubMed Central

Zhang, Dou; Zhou, Xuefan; Roscow, James; Zhou, Kechao; Wang, Lu; Luo, Hang; Bowen, Chris R.

2017-01-01

There is a growing need for high energy density capacitors in modern electric power supplies. The creation of nanocomposite systems based on one-dimensional nanofibers has shown great potential in achieving a high energy density since they can optimize the energy density by exploiting both the high permittivity of ceramic fillers and the high breakdown strength of the polymer matrix. In this paper, BaTiO3 nanofibers (NFs) with different aspect ratio were synthesized by a two-step hydrothermal method and the permittivity and energy storage of the P(VDF-HFP) nanocomposites were investigated. It is found that as the BaTiO3 NF aspect ratio and volume fraction increased the permittivity and maximum electric displacement of the nanocomposites increased, while the breakdown strength decreased. The nanocomposites with the highest aspect ratio BaTiO3 NFs exhibited the highest energy storage density at the same electric field. However, the nanocomposites with the lowest aspect ratio BaTiO3 NFs achieved the maximal energy storage density of 15.48 J/cm3 due to its higher breakdown strength. This contribution provides a potential route to prepare and tailor the properties of high energy density capacitor nanocomposites. PMID:28332636

Significantly Enhanced Energy Storage Density by Modulating the Aspect Ratio of BaTiO3 Nanofibers

NASA Astrophysics Data System (ADS)

Zhang, Dou; Zhou, Xuefan; Roscow, James; Zhou, Kechao; Wang, Lu; Luo, Hang; Bowen, Chris R.

2017-03-01

There is a growing need for high energy density capacitors in modern electric power supplies. The creation of nanocomposite systems based on one-dimensional nanofibers has shown great potential in achieving a high energy density since they can optimize the energy density by exploiting both the high permittivity of ceramic fillers and the high breakdown strength of the polymer matrix. In this paper, BaTiO3 nanofibers (NFs) with different aspect ratio were synthesized by a two-step hydrothermal method and the permittivity and energy storage of the P(VDF-HFP) nanocomposites were investigated. It is found that as the BaTiO3 NF aspect ratio and volume fraction increased the permittivity and maximum electric displacement of the nanocomposites increased, while the breakdown strength decreased. The nanocomposites with the highest aspect ratio BaTiO3 NFs exhibited the highest energy storage density at the same electric field. However, the nanocomposites with the lowest aspect ratio BaTiO3 NFs achieved the maximal energy storage density of 15.48 J/cm3 due to its higher breakdown strength. This contribution provides a potential route to prepare and tailor the properties of high energy density capacitor nanocomposites.

Significantly Enhanced Energy Storage Density by Modulating the Aspect Ratio of BaTiO3 Nanofibers.

PubMed

Zhang, Dou; Zhou, Xuefan; Roscow, James; Zhou, Kechao; Wang, Lu; Luo, Hang; Bowen, Chris R

2017-03-23

There is a growing need for high energy density capacitors in modern electric power supplies. The creation of nanocomposite systems based on one-dimensional nanofibers has shown great potential in achieving a high energy density since they can optimize the energy density by exploiting both the high permittivity of ceramic fillers and the high breakdown strength of the polymer matrix. In this paper, BaTiO 3 nanofibers (NFs) with different aspect ratio were synthesized by a two-step hydrothermal method and the permittivity and energy storage of the P(VDF-HFP) nanocomposites were investigated. It is found that as the BaTiO 3 NF aspect ratio and volume fraction increased the permittivity and maximum electric displacement of the nanocomposites increased, while the breakdown strength decreased. The nanocomposites with the highest aspect ratio BaTiO 3 NFs exhibited the highest energy storage density at the same electric field. However, the nanocomposites with the lowest aspect ratio BaTiO 3 NFs achieved the maximal energy storage density of 15.48 J/cm 3 due to its higher breakdown strength. This contribution provides a potential route to prepare and tailor the properties of high energy density capacitor nanocomposites.

Postmortem validation of breast density using dual-energy mammography

PubMed Central

Molloi, Sabee; Ducote, Justin L.; Ding, Huanjun; Feig, Stephen A.

2014-01-01

Purpose: Mammographic density has been shown to be an indicator of breast cancer risk and also reduces the sensitivity of screening mammography. Currently, there is no accepted standard for measuring breast density. Dual energy mammography has been proposed as a technique for accurate measurement of breast density. The purpose of this study is to validate its accuracy in postmortem breasts and compare it with other existing techniques. Methods: Forty postmortem breasts were imaged using a dual energy mammography system. Glandular and adipose equivalent phantoms of uniform thickness were used to calibrate a dual energy basis decomposition algorithm. Dual energy decomposition was applied after scatter correction to calculate breast density. Breast density was also estimated using radiologist reader assessment, standard histogram thresholding and a fuzzy C-mean algorithm. Chemical analysis was used as the reference standard to assess the accuracy of different techniques to measure breast composition. Results: Breast density measurements using radiologist reader assessment, standard histogram thresholding, fuzzy C-mean algorithm, and dual energy were in good agreement with the measured fibroglandular volume fraction using chemical analysis. The standard error estimates using radiologist reader assessment, standard histogram thresholding, fuzzy C-mean, and dual energy were 9.9%, 8.6%, 7.2%, and 4.7%, respectively. Conclusions: The results indicate that dual energy mammography can be used to accurately measure breast density. The variability in breast density estimation using dual energy mammography was lower than reader assessment rankings, standard histogram thresholding, and fuzzy C-mean algorithm. Improved quantification of breast density is expected to further enhance its utility as a risk factor for breast cancer. PMID:25086548

Postmortem validation of breast density using dual-energy mammography

DOE Office of Scientific and Technical Information (OSTI.GOV)

Molloi, Sabee, E-mail: symolloi@uci.edu; Ducote, Justin L.; Ding, Huanjun

2014-08-15

Purpose: Mammographic density has been shown to be an indicator of breast cancer risk and also reduces the sensitivity of screening mammography. Currently, there is no accepted standard for measuring breast density. Dual energy mammography has been proposed as a technique for accurate measurement of breast density. The purpose of this study is to validate its accuracy in postmortem breasts and compare it with other existing techniques. Methods: Forty postmortem breasts were imaged using a dual energy mammography system. Glandular and adipose equivalent phantoms of uniform thickness were used to calibrate a dual energy basis decomposition algorithm. Dual energy decompositionmore » was applied after scatter correction to calculate breast density. Breast density was also estimated using radiologist reader assessment, standard histogram thresholding and a fuzzy C-mean algorithm. Chemical analysis was used as the reference standard to assess the accuracy of different techniques to measure breast composition. Results: Breast density measurements using radiologist reader assessment, standard histogram thresholding, fuzzy C-mean algorithm, and dual energy were in good agreement with the measured fibroglandular volume fraction using chemical analysis. The standard error estimates using radiologist reader assessment, standard histogram thresholding, fuzzy C-mean, and dual energy were 9.9%, 8.6%, 7.2%, and 4.7%, respectively. Conclusions: The results indicate that dual energy mammography can be used to accurately measure breast density. The variability in breast density estimation using dual energy mammography was lower than reader assessment rankings, standard histogram thresholding, and fuzzy C-mean algorithm. Improved quantification of breast density is expected to further enhance its utility as a risk factor for breast cancer.« less

Electronic structure and electron momentum densities of Ag2CrO4

NASA Astrophysics Data System (ADS)

Meena, Seema Kumari; Ahuja, B. L.

2018-05-01

We present the first-ever experimental electron momentum density of Ag2CrO4 using 661.65 keV γ-rays from 20 Ci 137Cs source. To validate our experimental data, we have also deduced theoretical Compton profiles, energy bands and density of states using linear combination of atomic orbitals (LCAO) method in the framework of density functional theory. It is seen that the DFT-LDA gives a better agreement with experimental data than free atom model. The energy bands and density of states are also discussed.

A turnkey data logger program for field-scale energy flux density measurements using eddy covariance and surface renewal

USDA-ARS?s Scientific Manuscript database

Micrometeorological methods and ecosystem-scale energy and mass flux density measurements have become increasingly important in soil, agricultural, and environmental sciences. For many scientists without formal training in atmospheric science, these techniques are relatively inaccessible. Eddy cov...

Gallium Nitride Direct Energy Conversion Betavoltaic Modeling and Optimization

DTIC Science & Technology

2017-03-01

require high energy density battery systems. Radioisotopes are the most energy dense materials that can be converted into electrical energy. Pure...beta radioisotopes can be used towards making a long-lasting battery. However, the process to convert the energy provided by a pure beta radioisotope ...betavoltaic. Each energy conversion method has different challenges to overcome to improve thesystem efficiency. These energy conversion methods that are

High energy density and efficiency achieved in nanocomposite film capacitors via structure modulation

NASA Astrophysics Data System (ADS)

Zeng, Yi; Shen, Zhong-Hui; Shen, Yang; Lin, Yuanhua; Nan, Ce-Wen

2018-03-01

Flexible dielectric polymer films with high energy storage density and high charge-discharge efficiency have been considered as promising materials for electrical power applications. Here, we design hierarchical structured nanocomposite films using nonlinear polymer poly(vinylidene fluoride-HFP) [P(VDF-HFP)] with inorganic h-boron nitride (h-BN) nanosheets by electrospinning and hot-pressing methods. Our results show that the addition of h-BN nanosheets and the design of the hierarchical multilayer structure in the nanocomposites can remarkably enhance the charge-discharge efficiency and energy density. A high charge-discharge efficiency of 78% and an energy density of 21 J/cm3 can be realized in the 12-layered PVDF/h-BN nanocomposite films. Phase-field simulation results reveal that the spatial distribution of the electric field in these hierarchical structured films affects the charge-discharge efficiency and energy density. This work provides a feasible route, i.e., structure modulation, to improve the energy storage performances for nanocomposite films.

Determination of the density of surface states at the semiconductor-insulator interface in a metal-insulator-semiconductor structure

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gulyamov, G., E-mail: Gulyamov1949@rambler.ru; Sharibaev, N. U.

2011-02-15

The temporal dependence of thermal generation of electrons from occupied surface states at the semiconductor-insulator interface in a metal-insulator-semiconductor structure is studied. It is established that, at low temperatures, the derivative of the probability of depopulation of occupied surface states with respect to energy is represented by the Dirac {delta} function. It is shown that the density of states of a finite number of discrete energy levels under high-temperature measurements manifests itself as a continuous spectrum, whereas this spectrum appears discrete at low temperatures. A method for processing the continuous spectrum of the density of surface states is suggested thatmore » method makes it possible to determine the discrete energy spectrum. The obtained results may be conducive to an increase in resolution of the method of non-stationary spectroscopy of surface states.« less

Fission Dynamics with Microscopic Level Densities

DOE PAGES

Ward, D.; Carlsson, B. G.; Dossing, Th.; ...

2017-01-01

We present a consistent framework for treating the energy and angularmomentum dependence of the shape evolution in the nuclear fission. It combines microscopically calculated level densities with the Metropolis-walk method, has no new parameters, and can elucidate the energy-dependent influence of pairing and shell effects on the dynamics of warm nuclei.

Kaon condensation in dense matter

DOE Office of Scientific and Technical Information (OSTI.GOV)

Carlson, J.; Heiselberg, H.; Pandharipande, V. R.

The kaon energy in neutron matter is calculated analytically with the Klein-Gordon equation, by making a Wigner-Seitz cell approximation and employing a K{sup -}N square well potential. The transition from the low density Lenz potential, proportional to scattering length, to the high density Hartree potential is found to begin at fairly low densities. Exact nonrelativistic calculations of the kaon energy in a simple cubic crystal of neutrons are used to test the Wigner-Seitz and the Ericson-Ericson approximation methods. In this case the frequently used Erickson-Erickson approximation is found to be fairly accurate up to twice nuclear matter density. All themore » calculations indicate that by {approx}4 times nuclear matter density the Hartree limit is reached. We also show that in the Hartree limit the energy of zero momentum kaons does not have relativistic energy dependent factors present in the low density expansions. The results indicate that the density for kaon condensation is higher than previously estimated.« less

Development of optics for x-ray phase-contrast imaging of high energy density plasmas.

PubMed

Stutman, D; Finkenthal, M; Moldovan, N

2010-10-01

Phase-contrast or refraction-enhanced x-ray radiography can be useful for the diagnostic of low-Z high energy density plasmas, such as imploding inertial confinement fusion (ICF) pellets, due to its sensitivity to density gradients. To separate and quantify the absorption and refraction contributions to x-ray images, methods based on microperiodic optics, such as shearing interferometry, can be used. To enable applying such methods with the energetic x rays needed for ICF radiography, we investigate a new type of optics consisting of grazing incidence microperiodic mirrors. Using such mirrors, efficient phase-contrast imaging systems could be built for energies up to ∼100 keV. In addition, a simple lithographic method is proposed for the production of the microperiodic x-ray mirrors based on the difference in the total reflection between a low-Z substrate and a high-Z film. Prototype mirrors fabricated with this method show promising characteristics in laboratory tests.

Determination of bulk and interface density of states in metal oxide semiconductor thin-film transistors by using capacitance-voltage characteristics

NASA Astrophysics Data System (ADS)

Wei, Xixiong; Deng, Wanling; Fang, Jielin; Ma, Xiaoyu; Huang, Junkai

2017-10-01

A physical-based straightforward extraction technique for interface and bulk density of states in metal oxide semiconductor thin film transistors (TFTs) is proposed by using the capacitance-voltage (C-V) characteristics. The interface trap density distribution with energy has been extracted from the analysis of capacitance-voltage characteristics. Using the obtained interface state distribution, the bulk trap density has been determined. With this method, for the interface trap density, it is found that deep state density nearing the mid-gap is approximately constant and tail states density increases exponentially with energy; for the bulk trap density, it is a superposition of exponential deep states and exponential tail states. The validity of the extraction is verified by comparisons with the measured current-voltage (I-V) characteristics and the simulation results by the technology computer-aided design (TCAD) model. This extraction method uses non-numerical iteration which is simple, fast and accurate. Therefore, it is very useful for TFT device characterization.

Excitation energies from particle-particle random phase approximation with accurate optimized effective potentials

NASA Astrophysics Data System (ADS)

Jin, Ye; Yang, Yang; Zhang, Du; Peng, Degao; Yang, Weitao

2017-10-01

The optimized effective potential (OEP) that gives accurate Kohn-Sham (KS) orbitals and orbital energies can be obtained from a given reference electron density. These OEP-KS orbitals and orbital energies are used here for calculating electronic excited states with the particle-particle random phase approximation (pp-RPA). Our calculations allow the examination of pp-RPA excitation energies with the exact KS density functional theory (DFT). Various input densities are investigated. Specifically, the excitation energies using the OEP with the electron densities from the coupled-cluster singles and doubles method display the lowest mean absolute error from the reference data for the low-lying excited states. This study probes into the theoretical limit of the pp-RPA excitation energies with the exact KS-DFT orbitals and orbital energies. We believe that higher-order correlation contributions beyond the pp-RPA bare Coulomb kernel are needed in order to achieve even higher accuracy in excitation energy calculations.

Energy resolved actinometry for simultaneous measurement of atomic oxygen densities and local mean electron energies in radio-frequency driven plasmas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Greb, Arthur, E-mail: ag941@york.ac.uk; Niemi, Kari; O'Connell, Deborah

2014-12-08

A diagnostic method for the simultaneous determination of atomic oxygen densities and mean electron energies is demonstrated for an atmospheric pressure radio-frequency plasma jet. The proposed method is based on phase resolved optical emission measurements of the direct and dissociative electron-impact excitation dynamics of three distinct emission lines, namely, Ar 750.4 nm, O 777.4 nm, and O 844.6 nm. The energy dependence of these lines serves as basis for analysis by taking into account two line ratios. In this frame, the method is highly adaptable with regard to pressure and gas composition. Results are benchmarked against independent numerical simulations and two-photon absorption laser-inducedmore » fluorescence experiments.« less

Density-based Energy Decomposition Analysis for Intermolecular Interactions with Variationally Determined Intermediate State Energies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Q.; Ayers, P.W.; Zhang, Y.

2009-10-28

The first purely density-based energy decomposition analysis (EDA) for intermolecular binding is developed within the density functional theory. The most important feature of this scheme is to variationally determine the frozen density energy, based on a constrained search formalism and implemented with the Wu-Yang algorithm [Q. Wu and W. Yang, J. Chem. Phys. 118, 2498 (2003) ]. This variational process dispenses with the Heitler-London antisymmetrization of wave functions used in most previous methods and calculates the electrostatic and Pauli repulsion energies together without any distortion of the frozen density, an important fact that enables a clean separation of these twomore » terms from the relaxation (i.e., polarization and charge transfer) terms. The new EDA also employs the constrained density functional theory approach [Q. Wu and T. Van Voorhis, Phys. Rev. A 72, 24502 (2005)] to separate out charge transfer effects. Because the charge transfer energy is based on the density flow in real space, it has a small basis set dependence. Applications of this decomposition to hydrogen bonding in the water dimer and the formamide dimer show that the frozen density energy dominates the binding in these systems, consistent with the noncovalent nature of the interactions. A more detailed examination reveals how the interplay of electrostatics and the Pauli repulsion determines the distance and angular dependence of these hydrogen bonds.« less

Multiconfiguration pair-density functional theory for doublet excitation energies and excited state geometries: the excited states of CN.

PubMed

Bao, Jie J; Gagliardi, Laura; Truhlar, Donald G

2017-11-15

Multiconfiguration pair-density functional theory (MC-PDFT) is a post multiconfiguration self-consistent field (MCSCF) method with similar performance to complete active space second-order perturbation theory (CASPT2) but with greater computational efficiency. Cyano radical (CN) is a molecule whose spectrum is well established from experiments and whose excitation energies have been used as a testing ground for theoretical methods to treat excited states of open-shell systems, which are harder and much less studied than excitation energies of closed-shell singlets. In the present work, we studied the adiabatic excitation energies of CN with MC-PDFT. Then we compared this multireference (MR) method to some single-reference (SR) methods, including time-dependent density functional theory (TDDFT) and completely renormalized equation-of-motion coupled-cluster theory with singles, doubles and noniterative triples [CR-EOM-CCSD(T)]; we also compared to some other MR methods, including configuration interaction singles and doubles (MR-CISD) and multistate CASPT2 (MS-CASPT2). Through a comparison between SR and MR methods, we achieved a better appreciation of the need to use MR methods to accurately describe higher excited states, and we found that among the MR methods, MC-PDFT stands out for its accuracy for the first four states out of the five doublet states studied this paper; this shows its efficiency for calculating doublet excited states.

Molecular structure and interactions in the ionic liquid 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide.

PubMed

Dhumal, Nilesh R; Noack, Kristina; Kiefer, Johannes; Kim, Hyung J

2014-04-03

Electronic structure theory (density functional and Møller-Plesset perturbation theory) and vibrational spectroscopy (FT-IR and Raman) are employed to study molecular interactions in the room-temperature ionic liquid 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)imide. Different conformers of a cation-anion pair based on their molecular interactions are simulated in the gas phase and in a dielectric continuum solvent environment. Although the ordering of conformers in energy varies with theoretical methods, their predictions for three lowest energy conformers in the gas phase are similar. Strong C-H---N interactions between the acidic hydrogen atom of the cation imidazole ring and the nitrogen atom of the anion are predicted for either the lowest or second lowest energy conformer. In a continuum solvent, different theoretical methods yield the same ion-pair conformation for the lowest energy state. In both phases, the density functional method predicts that the anion is in a trans conformation in the lowest energy ion pair state. The theoretical results are compared with experimental observations from Raman scattering and IR absorption spectroscopies and manifestations of the molecular interactions in the vibrational spectra are discussed. The directions of the frequency shifts of the characteristic vibrations relative to the free anion and cation are explained by calculating the difference electron density coupled with electron density topography.

Bubbler: A Novel Ultra-High Power Density Energy Harvesting Method Based on Reverse Electrowetting

PubMed Central

Hsu, Tsung-Hsing; Manakasettharn, Supone; Taylor, J. Ashley; Krupenkin, Tom

2015-01-01

We have proposed and successfully demonstrated a novel approach to direct conversion of mechanical energy into electrical energy using microfluidics. The method combines previously demonstrated reverse electrowetting on dielectric (REWOD) phenomenon with the fast self-oscillating process of bubble growth and collapse. Fast bubble dynamics, used in conjunction with REWOD, provides a possibility to increase the generated power density by over an order of magnitude, as compared to the REWOD alone. This energy conversion approach is particularly well suited for energy harvesting applications and can enable effective coupling to a broad array of mechanical systems including such ubiquitous but difficult to utilize low-frequency energy sources as human and machine motion. The method can be scaled from a single micro cell with 10−6 W output to power cell arrays with a total power output in excess of 10 W. This makes the fabrication of small light-weight energy harvesting devices capable of producing a wide range of power outputs feasible. PMID:26567850

Bubbler: A Novel Ultra-High Power Density Energy Harvesting Method Based on Reverse Electrowetting.

PubMed

Hsu, Tsung-Hsing; Manakasettharn, Supone; Taylor, J Ashley; Krupenkin, Tom

2015-11-16

We have proposed and successfully demonstrated a novel approach to direct conversion of mechanical energy into electrical energy using microfluidics. The method combines previously demonstrated reverse electrowetting on dielectric (REWOD) phenomenon with the fast self-oscillating process of bubble growth and collapse. Fast bubble dynamics, used in conjunction with REWOD, provides a possibility to increase the generated power density by over an order of magnitude, as compared to the REWOD alone. This energy conversion approach is particularly well suited for energy harvesting applications and can enable effective coupling to a broad array of mechanical systems including such ubiquitous but difficult to utilize low-frequency energy sources as human and machine motion. The method can be scaled from a single micro cell with 10(-6) W output to power cell arrays with a total power output in excess of 10 W. This makes the fabrication of small light-weight energy harvesting devices capable of producing a wide range of power outputs feasible.

Self-Consistent Optimization of Excited States within Density-Functional Tight-Binding.

PubMed

Kowalczyk, Tim; Le, Khoa; Irle, Stephan

2016-01-12

We present an implementation of energies and gradients for the ΔDFTB method, an analogue of Δ-self-consistent-field density functional theory (ΔSCF) within density-functional tight-binding, for the lowest singlet excited state of closed-shell molecules. Benchmarks of ΔDFTB excitation energies, optimized geometries, Stokes shifts, and vibrational frequencies reveal that ΔDFTB provides a qualitatively correct description of changes in molecular geometries and vibrational frequencies due to excited-state relaxation. The accuracy of ΔDFTB Stokes shifts is comparable to that of ΔSCF-DFT, and ΔDFTB performs similarly to ΔSCF with the PBE functional for vertical excitation energies of larger chromophores where the need for efficient excited-state methods is most urgent. We provide some justification for the use of an excited-state reference density in the DFTB expansion of the electronic energy and demonstrate that ΔDFTB preserves many of the properties of its parent ΔSCF approach. This implementation fills an important gap in the extended framework of DFTB, where access to excited states has been limited to the time-dependent linear-response approach, and affords access to rapid exploration of a valuable class of excited-state potential energy surfaces.

High Discharge Energy Density at Low Electric Field Using an Aligned Titanium Dioxide/Lead Zirconate Titanate Nanowire Array

PubMed Central

Zhang, Dou; Liu, Weiwei; Guo, Ru; Zhou, Kechao

2017-01-01

Abstract Polymer‐based capacitors with high energy density have attracted significant attention in recent years due to their wide range of potential applications in electronic devices. However, the obtained high energy density is predominantly dependent on high applied electric field, e.g., 400–600 kV mm−1, which may bring more challenges relating to the failure probability. Here, a simple two‐step method for synthesizing titanium dioxide/lead zirconate titanate nanowire arrays is exploited and a demonstration of their ability to achieve high discharge energy density capacitors for low operating voltage applications is provided. A high discharge energy density of 6.9 J cm−3 is achieved at low electric fields, i.e., 143 kV mm−1, which is attributed to the high relative permittivity of 218.9 at 1 kHz and high polarization of 23.35 µC cm−2 at this electric field. The discharge energy density obtained in this work is the highest known for a ceramic/polymer nanocomposite at such a low electric field. The novel nanowire arrays used in this work are applicable to a wide range of fields, such as energy harvesting, energy storage, and photocatalysis. PMID:29610724

Many-particle theory of nuclear systems with application to neutron star matter

NASA Technical Reports Server (NTRS)

Chakkalakal, D. A.; Yang, C.

1973-01-01

The research is reported concerning energy-density relation for the normal state of neutron star matter, and the effects of superfluidity and polarization on neutron star matter. Considering constraints on variation, and the theory of quantum fluids, three methods for calculating the energy-density range are presented. The effects of polarization on neutron star structure, and polarization effects on condensation and superfluid-state energy are discussed.

Resolving Rapid Variation in Energy for Particle Transport

DOE Office of Scientific and Technical Information (OSTI.GOV)

Haut, Terry Scot; Ahrens, Cory Douglas; Jonko, Alexandra

2016-08-23

Resolving the rapid variation in energy in neutron and thermal radiation transport is needed for the predictive simulation capability in high-energy density physics applications. Energy variation is difficult to resolve due to rapid variations in cross sections and opacities caused by quantized energy levels in the nuclei and electron clouds. In recent work, we have developed a new technique to simultaneously capture slow and rapid variations in the opacities and the solution using homogenization theory, which is similar to multiband (MB) and to the finite-element with discontiguous support (FEDS) method, but does not require closure information. We demonstrated the accuracymore » and efficiency of the method for a variety of problems. We are researching how to extend the method to problems with multiple materials and the same material but with different temperatures and densities. In this highlight, we briefly describe homogenization theory and some results.« less

Monte Carlo Approach for Estimating Density and Atomic Number From Dual-Energy Computed Tomography Images of Carbonate Rocks

NASA Astrophysics Data System (ADS)

Victor, Rodolfo A.; Prodanović, Maša.; Torres-Verdín, Carlos

2017-12-01

We develop a new Monte Carlo-based inversion method for estimating electron density and effective atomic number from 3-D dual-energy computed tomography (CT) core scans. The method accounts for uncertainties in X-ray attenuation coefficients resulting from the polychromatic nature of X-ray beam sources of medical and industrial scanners, in addition to delivering uncertainty estimates of inversion products. Estimation of electron density and effective atomic number from CT core scans enables direct deterministic or statistical correlations with salient rock properties for improved petrophysical evaluation; this condition is specifically important in media such as vuggy carbonates where CT resolution better captures core heterogeneity that dominates fluid flow properties. Verification tests of the inversion method performed on a set of highly heterogeneous carbonate cores yield very good agreement with in situ borehole measurements of density and photoelectric factor.

Dietary Energy Density in the Australian Adult Population from National Nutrition Surveys 1995 to 2012.

PubMed

Grech, Amanda Lee; Rangan, Anna; Allman-Farinelli, Margaret

2017-12-01

It is hypothesized that the observed proliferation of energy-dense, nutrient-poor foods globally is an important contributing factor to the development of the obesity epidemic. However, evidence that the population's dietary energy density has increased is sparse. The World Cancer Research Fund recommends that dietary energy density be <1.25 kcal/g to prevent weight gain. The aim of this research was to determine whether the dietary energy density of the Australian population has changed between 1995 and 2012. A secondary analysis of two cross-sectional Australian national nutrition surveys from 1995 and 2011/2012 was conducted. Participants of the surveys included adults aged 18 years and older (1995 n=10,986 and 2011/2012 n=9,435) completing 24-hour dietary recalls, including a second recall for a subset of the population (10.4% in 1995 and 64.6% in 2011/2012). Outcome measures included the change in dietary energy density (calculated as energy/weight of food [kcal/g] for food only) between surveys. The National Cancer Institute method for "estimating ratios of two dietary components that are consumed nearly every day" was used to determine the usual distribution and the percentage of participants reporting energy density <1.25 kcal/g. The mean (standard deviation) dietary energy density was 1.59 (0.26) kcal/g and 1.64 (0.32) kcal/g (P<0.0001) in 1995 and 2011/2012, respectively, with 13% and 5% (P<0.0001) of the population meeting dietary energy-density recommendations. For those aged 70 years and older, the percentage with energy density <1.25 kcal/g decreased from 22% to 6% (P<0.0001) for men and from 33% to 11% (P<0.0001) for women in 1995 and 2011/2012, respectively. Among those aged 18 to 29 years, 1% of men in both surveys (P=0.8) and 4% of women in 1995 and 2% in 2011/2012 (P=0.01) reported energy density <1.25 kcal/g. Dietary energy density has increased between the two surveys and few people consumed low energy-dense diets in line with recommendations. The change was largely due to increased energy density of older adult's diets, while young adults had high dietary energy density at both time points. These data suggest efforts now focus on the evaluation of the role of modifying energy density of the diet to reduce the risk of weight gain in adults. Copyright © 2017 Academy of Nutrition and Dietetics. Published by Elsevier Inc. All rights reserved.

Partition coefficients of methylated DNA bases obtained from free energy calculations with molecular electron density derived atomic charges.

PubMed

Lara, A; Riquelme, M; Vöhringer-Martinez, E

2018-05-11

Partition coefficients serve in various areas as pharmacology and environmental sciences to predict the hydrophobicity of different substances. Recently, they have also been used to address the accuracy of force fields for various organic compounds and specifically the methylated DNA bases. In this study, atomic charges were derived by different partitioning methods (Hirshfeld and Minimal Basis Iterative Stockholder) directly from the electron density obtained by electronic structure calculations in a vacuum, with an implicit solvation model or with explicit solvation taking the dynamics of the solute and the solvent into account. To test the ability of these charges to describe electrostatic interactions in force fields for condensed phases, the original atomic charges of the AMBER99 force field were replaced with the new atomic charges and combined with different solvent models to obtain the hydration and chloroform solvation free energies by molecular dynamics simulations. Chloroform-water partition coefficients derived from the obtained free energies were compared to experimental and previously reported values obtained with the GAFF or the AMBER-99 force field. The results show that good agreement with experimental data is obtained when the polarization of the electron density by the solvent has been taken into account, and when the energy needed to polarize the electron density of the solute has been considered in the transfer free energy. These results were further confirmed by hydration free energies of polar and aromatic amino acid side chain analogs. Comparison of the two partitioning methods, Hirshfeld-I and Minimal Basis Iterative Stockholder (MBIS), revealed some deficiencies in the Hirshfeld-I method related to the unstable isolated anionic nitrogen pro-atom used in the method. Hydration free energies and partitioning coefficients obtained with atomic charges from the MBIS partitioning method accounting for polarization by the implicit solvation model are in good agreement with the experimental values. © 2018 Wiley Periodicals, Inc. © 2018 Wiley Periodicals, Inc.

Understanding limiting factors in thick electrode performance as applied to high energy density Li-ion batteries

DOE PAGES

Du, Zhijia; Wood, David L.; Daniel, Claus; ...

2017-02-09

We present that increasing electrode thickness, thus increasing the volume ratio of active materials, is one effective method to enable the development of high energy density Li-ion batteries. In this study, an energy density versus power density optimization of LiNi 0.8Co 0.15Al 0.05O 2 (NCA)/graphite cell stack was conducted via mathematical modeling. The energy density was found to have a maximum point versus electrode thickness (critical thickness) at given discharging C rates. The physics-based factors that limit the energy/power density of thick electrodes were found to be increased cell polarization and underutilization of active materials. The latter is affected bymore » Li-ion diffusion in active materials and Li-ion depletion in the electrolyte phase. Based on those findings, possible approaches were derived to surmount the limiting factors. Finally, the improvement of the energy–power relationship in an 18,650 cell was used to demonstrate how to optimize the thick electrode parameters in cell engineering.« less

Empirical prediction intervals improve energy forecasting

PubMed Central

Kaack, Lynn H.; Apt, Jay; Morgan, M. Granger; McSharry, Patrick

2017-01-01

Hundreds of organizations and analysts use energy projections, such as those contained in the US Energy Information Administration (EIA)’s Annual Energy Outlook (AEO), for investment and policy decisions. Retrospective analyses of past AEO projections have shown that observed values can differ from the projection by several hundred percent, and thus a thorough treatment of uncertainty is essential. We evaluate the out-of-sample forecasting performance of several empirical density forecasting methods, using the continuous ranked probability score (CRPS). The analysis confirms that a Gaussian density, estimated on past forecasting errors, gives comparatively accurate uncertainty estimates over a variety of energy quantities in the AEO, in particular outperforming scenario projections provided in the AEO. We report probabilistic uncertainties for 18 core quantities of the AEO 2016 projections. Our work frames how to produce, evaluate, and rank probabilistic forecasts in this setting. We propose a log transformation of forecast errors for price projections and a modified nonparametric empirical density forecasting method. Our findings give guidance on how to evaluate and communicate uncertainty in future energy outlooks. PMID:28760997

Dual energy approach for cone beam artifacts correction

NASA Astrophysics Data System (ADS)

Han, Chulhee; Choi, Shinkook; Lee, Changwoo; Baek, Jongduk

2017-03-01

Cone beam computed tomography systems generate 3D volumetric images, which provide further morphological information compared to radiography and tomosynthesis systems. However, reconstructed images by FDK algorithm contain cone beam artifacts when a cone angle is large. To reduce the cone beam artifacts, two-pass algorithm has been proposed. The two-pass algorithm considers the cone beam artifacts are mainly caused by high density materials, and proposes an effective method to estimate error images (i.e., cone beam artifacts images) by the high density materials. While this approach is simple and effective with a small cone angle (i.e., 5 - 7 degree), the correction performance is degraded as the cone angle increases. In this work, we propose a new method to reduce the cone beam artifacts using a dual energy technique. The basic idea of the proposed method is to estimate the error images generated by the high density materials more reliably. To do this, projection data of the high density materials are extracted from dual energy CT projection data using a material decomposition technique, and then reconstructed by iterative reconstruction using total-variation regularization. The reconstructed high density materials are used to estimate the error images from the original FDK images. The performance of the proposed method is compared with the two-pass algorithm using root mean square errors. The results show that the proposed method reduces the cone beam artifacts more effectively, especially with a large cone angle.

Transport of phase space densities through tetrahedral meshes using discrete flow mapping

NASA Astrophysics Data System (ADS)

Bajars, Janis; Chappell, David J.; Søndergaard, Niels; Tanner, Gregor

2017-01-01

Discrete flow mapping was recently introduced as an efficient ray based method determining wave energy distributions in complex built up structures. Wave energy densities are transported along ray trajectories through polygonal mesh elements using a finite dimensional approximation of a ray transfer operator. In this way the method can be viewed as a smoothed ray tracing method defined over meshed surfaces. Many applications require the resolution of wave energy distributions in three-dimensional domains, such as in room acoustics, underwater acoustics and for electromagnetic cavity problems. In this work we extend discrete flow mapping to three-dimensional domains by propagating wave energy densities through tetrahedral meshes. The geometric simplicity of the tetrahedral mesh elements is utilised to efficiently compute the ray transfer operator using a mixture of analytic and spectrally accurate numerical integration. The important issue of how to choose a suitable basis approximation in phase space whilst maintaining a reasonable computational cost is addressed via low order local approximations on tetrahedral faces in the position coordinate and high order orthogonal polynomial expansions in momentum space.

Hierarchical MoS2 nanowires/NiCo2O4 nanosheets supported on Ni foam for high-performance asymmetric supercapacitors

NASA Astrophysics Data System (ADS)

Wen, Shiyang; Liu, Yu; Zhu, Fangfang; Shao, Rong; Xu, Wei

2018-01-01

The hierarchical MoS2 nanowires/NiCo2O4 nanosheets (MS/NCO) supercapacitor electrode materials supported on Ni foam were synthesized by a two-step hydrothermal method. The capacitance was investigated by using various electrochemical methods including cyclic voltammetry, constant-current galvanostatic charge/discharge curves and electrochemical impedance spectroscopy. The MS/NCO networks show 7 times more capacitance (7.1 F cm-2) than pure NiCo2O4 nanosheets by CV at a scan rate of 2 mV s-1. The specific capacitance of the assembled MS/NCO//active carbon (AC) asymmetric supercapacitor could reach up to 51.7 F g-1 at a current density of 1.5 A g-1. Also, the maximum energy density of 18.4 W h kg-1 at a power density of 1200.2 W kg-1 was achieved, with 98.2% specific capacitance retention after 8000 cycles. These exciting results exhibit potential application in developing energy storage devices with high energy density and high power density.

Energy Deficit Required for Rapid Weight Loss in Elite Collegiate Wrestlers.

PubMed

Kondo, Emi; Sagayama, Hiroyuki; Yamada, Yosuke; Shiose, Keisuke; Osawa, Takuya; Motonaga, Keiko; Ouchi, Shiori; Kamei, Akiko; Nakajima, Kohei; Higaki, Yasuki; Tanaka, Hiroaki; Takahashi, Hideyuki; Okamura, Koji

2018-04-26

To determine energy density for rapid weight loss (RWL) of weight-classified sports, eight male elite wrestlers were instructed to lose 6% of body mass (BM) within 53 h. Energy deficit during the RWL was calculated by subtracting total energy expenditure (TEE) determined using the doubly labeled water method (DLW) from energy intake (EI) assessed with diet records. It was also estimated from body composition change estimated with the four-component model (4C) and other conventional methods. BM decreased significantly by 4.7 ± 0.5 kg (6.4 ± 0.5%). Total body water loss was the major component of the BM loss (71.0 ± 7.6%). TEE was 9446 ± 1422 kcal, and EI was 2366 ± 1184 kcal during the RWL of 53-h; therefore, the energy deficit was 7080 ± 1525 kcal. Thus, energy density was 1507 ± 279 kcal/kg ∆BM during the RWL, comparable with values obtained using the 4C, three-component model, dual energy X-ray absorptiometry, and stable isotope dilution. Energy density for RWL of wrestlers is lower than that commonly used (7400 or 7700 kcal/kg ΔBM). Although RWL is not recommended, we propose that commonly practiced extreme energy restriction such as 7400 or 7700 kcal/kg ΔBM during RWL appears to be meaningless.

Derivation of general analytic gradient expressions for density-fitted post-Hartree-Fock methods: An efficient implementation for the density-fitted second-order Møller–Plesset perturbation theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bozkaya, Uğur, E-mail: ugur.bozkaya@atauni.edu.tr

General analytic gradient expressions (with the frozen-core approximation) are presented for density-fitted post-HF methods. An efficient implementation of frozen-core analytic gradients for the second-order Møller–Plesset perturbation theory (MP2) with the density-fitting (DF) approximation (applying to both reference and correlation energies), which is denoted as DF-MP2, is reported. The DF-MP2 method is applied to a set of alkanes, conjugated dienes, and noncovalent interaction complexes to compare the computational cost of single point analytic gradients with MP2 with the resolution of the identity approach (RI-MP2) [F. Weigend and M. Häser, Theor. Chem. Acc. 97, 331 (1997); R. A. Distasio, R. P. Steele,more » Y. M. Rhee, Y. Shao, and M. Head-Gordon, J. Comput. Chem. 28, 839 (2007)]. In the RI-MP2 method, the DF approach is used only for the correlation energy. Our results demonstrate that the DF-MP2 method substantially accelerate the RI-MP2 method for analytic gradient computations due to the reduced input/output (I/O) time. Because in the DF-MP2 method the DF approach is used for both reference and correlation energies, the storage of 4-index electron repulsion integrals (ERIs) are avoided, 3-index ERI tensors are employed instead. Further, as in case of integrals, our gradient equation is completely avoid construction or storage of the 4-index two-particle density matrix (TPDM), instead we use 2- and 3-index TPDMs. Hence, the I/O bottleneck of a gradient computation is significantly overcome. Therefore, the cost of the generalized-Fock matrix (GFM), TPDM, solution of Z-vector equations, the back transformation of TPDM, and integral derivatives are substantially reduced when the DF approach is used for the entire energy expression. Further application results show that the DF approach introduce negligible errors for closed-shell reaction energies and equilibrium bond lengths.« less

Use of nonlinear programming to optimize performance response to energy density in broiler feed formulation.

PubMed

Guevara, V R

2004-02-01

A nonlinear programming optimization model was developed to maximize margin over feed cost in broiler feed formulation and is described in this paper. The model identifies the optimal feed mix that maximizes profit margin. Optimum metabolizable energy level and performance were found by using Excel Solver nonlinear programming. Data from an energy density study with broilers were fitted to quadratic equations to express weight gain, feed consumption, and the objective function income over feed cost in terms of energy density. Nutrient:energy ratio constraints were transformed into equivalent linear constraints. National Research Council nutrient requirements and feeding program were used for examining changes in variables. The nonlinear programming feed formulation method was used to illustrate the effects of changes in different variables on the optimum energy density, performance, and profitability and was compared with conventional linear programming. To demonstrate the capabilities of the model, I determined the impact of variation in prices. Prices for broiler, corn, fish meal, and soybean meal were increased and decreased by 25%. Formulations were identical in all other respects. Energy density, margin, and diet cost changed compared with conventional linear programming formulation. This study suggests that nonlinear programming can be more useful than conventional linear programming to optimize performance response to energy density in broiler feed formulation because an energy level does not need to be set.

Thermodynamic analysis of energy density in pressure retarded osmosis: The impact of solution volumes and costs

DOE Office of Scientific and Technical Information (OSTI.GOV)

Reimund, Kevin K.; McCutcheon, Jeffrey R.; Wilson, Aaron D.

A general method was developed for estimating the volumetric energy efficiency of pressure retarded osmosis via pressure-volume analysis of a membrane process. The resulting model requires only the osmotic pressure, π, and mass fraction, w, of water in the concentrated and dilute feed solutions to estimate the maximum achievable specific energy density, uu, as a function of operating pressure. The model is independent of any membrane or module properties. This method utilizes equilibrium analysis to specify the volumetric mixing fraction of concentrated and dilute solution as a function of operating pressure, and provides results for the total volumetric energy densitymore » of similar order to more complex models for the mixing of seawater and riverwater. Within the framework of this analysis, the total volumetric energy density is maximized, for an idealized case, when the operating pressure is π/(1+√w⁻¹), which is lower than the maximum power density operating pressure, Δπ/2, derived elsewhere, and is a function of the solute osmotic pressure at a given mass fraction. It was also found that a minimum 1.45 kmol of ideal solute is required to produce 1 kWh of energy while a system operating at “maximum power density operating pressure” requires at least 2.9 kmol. Utilizing this methodology, it is possible to examine the effects of volumetric solution cost, operation of a module at various pressure, and operation of a constant pressure module with various feed.« less

A randomized controlled trial for obesity and binge eating disorder: Low-energy-density dietary counseling and cognitive behavioral therapy

PubMed Central

Masheb, Robin M.; Grilo, Carlos M.; Rolls, Barbara J.

2011-01-01

The present study examined a dietary approach – lowering energy density – for producing weight loss in obese patients with binge eating disorder (BED) who also received cognitive-behavioral therapy (CBT) to address binge eating. Fifty consecutive participants were randomly assigned to either a six-month individual treatment of CBT plus a low-Energy-Density diet (CBT+ED) or CBT plus General Nutrition counseling not related to weight loss (CBT+GN). Assessments occurred at six- and twelve-months. Eighty-six percent of participants completed treatment, and of these, 30% achieved at least a 5% weight loss with rates of binge remission ranging from 55–75%. The two treatments did not differ significantly in weight loss or binge remission outcomes. Significant improvements were found for key dietary and metabolic outcomes, with CBT+ED producing significantly better dietary outcomes on energy density, and fruit and vegetable consumption, than CBT+GN. Reductions in energy density and weight loss were significantly associated providing evidence for the specificity of the treatment effect. These favorable outcomes, and that CBT+ED was significantly better at reducing energy density and increasing fruit and vegetable consumption compared to CBT+GN, suggest that low-energy-density dietary counseling has promise as an effective method for enhancing CBT for obese individuals with BED. PMID:22005587

Adsorption energies of benzene on close packed transition metal surfaces using the random phase approximation

NASA Astrophysics Data System (ADS)

Garrido Torres, José A.; Ramberger, Benjamin; Früchtl, Herbert A.; Schaub, Renald; Kresse, Georg

2017-11-01

The adsorption energy of benzene on various metal substrates is predicted using the random phase approximation (RPA) for the correlation energy. Agreement with available experimental data is systematically better than 10% for both coinage and reactive metals. The results are also compared with more approximate methods, including van der Waals density functional theory (DFT), as well as dispersion-corrected DFT functionals. Although dispersion-corrected DFT can yield accurate results, for instance, on coinage metals, the adsorption energies are clearly overestimated on more reactive transition metals. Furthermore, coverage dependent adsorption energies are well described by the RPA. This shows that for the description of aromatic molecules on metal surfaces further improvements in density functionals are necessary, or more involved many-body methods such as the RPA are required.

Density-functional expansion methods: evaluation of LDA, GGA, and meta-GGA functionals and different integral approximations.

PubMed

Giese, Timothy J; York, Darrin M

2010-12-28

We extend the Kohn-Sham potential energy expansion (VE) to include variations of the kinetic energy density and use the VE formulation with a 6-31G* basis to perform a "Jacob's ladder" comparison of small molecule properties using density functionals classified as being either LDA, GGA, or meta-GGA. We show that the VE reproduces standard Kohn-Sham DFT results well if all integrals are performed without further approximation, and there is no substantial improvement in using meta-GGA functionals relative to GGA functionals. The advantages of using GGA versus LDA functionals becomes apparent when modeling hydrogen bonds. We furthermore examine the effect of using integral approximations to compute the zeroth-order energy and first-order matrix elements, and the results suggest that the origin of the short-range repulsive potential within self-consistent charge density-functional tight-binding methods mainly arises from the approximations made to the first-order matrix elements.

Communication: Density functional theory overcomes the failure of predicting intermolecular interaction energies

DOE Office of Scientific and Technical Information (OSTI.GOV)

Podeszwa, Rafal; Department of Physics and Astronomy, University of Delaware, Newark, Delaware 19716; Szalewicz, Krzysztof

2012-04-28

Density-functional theory (DFT) revolutionized the ability of computational quantum mechanics to describe properties of matter and is by far the most often used method. However, all the standard variants of DFT fail to predict intermolecular interaction energies. In recent years, a number of ways to go around this problem has been proposed. We show that some of these approaches can reproduce interaction energies with median errors of only about 5% in the complete range of intermolecular configurations. Such errors are comparable to typical uncertainties of wave-function-based methods in practical applications. Thus, these DFT methods are expected to find broad applicationsmore » in modelling of condensed phases and of biomolecules.« less

High energy density aluminum battery

DOE Office of Scientific and Technical Information (OSTI.GOV)

Brown, Gilbert M.; Parans Paranthaman, Mariappan; Dai, Sheng

Compositions and methods of making are provided for a high energy density lithium-aluminum battery. The battery comprises an anode comprising aluminum metal. The battery further comprises a cathode comprising a lithium metal oxide. The battery further comprises an electrolyte capable of supporting reversible deposition and stripping of aluminum at the anode, and reversible intercalation and deintercalation of lithium at the cathode.

On the numerical calculation of hydrodynamic shock waves in atmospheres by an FCT method

NASA Astrophysics Data System (ADS)

Schmitz, F.; Fleck, B.

1993-11-01

The numerical calculation of vertically propagating hydrodynamic shock waves in a plane atmosphere by the ETBFCT-version of the Flux Corrected Transport (FCT) method by Boris and Book is discussed. The results are compared with results obtained by a characteristic method with shock fitting. We show that the use of the internal energy density as a dependent variable instead of the total energy density can give very inaccurate results. Consequent discretization rules for the gravitational source terms are derived. The improvement of the results by an additional iteration step is discussed. It appears that the FCT method is an excellent method for the accurate calculation of shock waves in an atmosphere.

Perturbation theory corrections to the two-particle reduced density matrix variational method.

PubMed

Juhasz, Tamas; Mazziotti, David A

2004-07-15

In the variational 2-particle-reduced-density-matrix (2-RDM) method, the ground-state energy is minimized with respect to the 2-particle reduced density matrix, constrained by N-representability conditions. Consider the N-electron Hamiltonian H(lambda) as a function of the parameter lambda where we recover the Fock Hamiltonian at lambda=0 and we recover the fully correlated Hamiltonian at lambda=1. We explore using the accuracy of perturbation theory at small lambda to correct the 2-RDM variational energies at lambda=1 where the Hamiltonian represents correlated atoms and molecules. A key assumption in the correction is that the 2-RDM method will capture a fairly constant percentage of the correlation energy for lambda in (0,1] because the nonperturbative 2-RDM approach depends more significantly upon the nature rather than the strength of the two-body Hamiltonian interaction. For a variety of molecules we observe that this correction improves the 2-RDM energies in the equilibrium bonding region, while the 2-RDM energies at stretched or nearly dissociated geometries, already highly accurate, are not significantly changed. At equilibrium geometries the corrected 2-RDM energies are similar in accuracy to those from coupled-cluster singles and doubles (CCSD), but at nonequilibrium geometries the 2-RDM energies are often dramatically more accurate as shown in the bond stretching and dissociation data for water and nitrogen. (c) 2004 American Institute of Physics.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Guo, Z.; Department of Applied Mathematics and Mechanics, University of Science and Technology Beijing, Beijing 100083; Lin, P.

In this paper, we investigate numerically a diffuse interface model for the Navier–Stokes equation with fluid–fluid interface when the fluids have different densities [48]. Under minor reformulation of the system, we show that there is a continuous energy law underlying the system, assuming that all variables have reasonable regularities. It is shown in the literature that an energy law preserving method will perform better for multiphase problems. Thus for the reformulated system, we design a C{sup 0} finite element method and a special temporal scheme where the energy law is preserved at the discrete level. Such a discrete energy lawmore » (almost the same as the continuous energy law) for this variable density two-phase flow model has never been established before with C{sup 0} finite element. A Newton method is introduced to linearise the highly non-linear system of our discretization scheme. Some numerical experiments are carried out using the adaptive mesh to investigate the scenario of coalescing and rising drops with differing density ratio. The snapshots for the evolution of the interface together with the adaptive mesh at different times are presented to show that the evolution, including the break-up/pinch-off of the drop, can be handled smoothly by our numerical scheme. The discrete energy functional for the system is examined to show that the energy law at the discrete level is preserved by our scheme.« less

Evaluation of effective energy for QA and QC: measurement of half-value layer using radiochromic film density.

PubMed

Gotanda, T; Katsuda, T; Gotanda, R; Tabuchi, A; Yamamoto, K; Kuwano, T; Yatake, H; Takeda, Y

2009-03-01

The effective energy of diagnostic X-rays is important for quality assurance (QA) and quality control (QC). However, the half-value layer (HVL), which is necessary to evaluate the effective energy, is not ubiquitously monitored because ionization-chamber dosimetry is time-consuming and complicated. To verify the applicability of GAFCHROMIC XR type R (GAF-R) film for HVL measurement as an alternative to monitoring with an ionization chamber, a single-strip method for measuring the HVL has been evaluated. Calibration curves of absorbed dose versus film density were generated using this single-strip method with GAF-R film, and the coefficient of determination (r2) of the straight-line approximation was evaluated. The HVLs (effective energies) estimated using the GAF-R film and an ionization chamber were compared. The coefficient of determination (r2) of the straight-line approximation obtained with the GAF-R film was more than 0.99. The effective energies (HVLs) evaluated using the GAF-R film and the ionization chamber were 43.25 keV (5.10 mm) and 39.86 keV (4.45 mm), respectively. The difference in the effective energies determined by the two methods was thus 8.5%. These results suggest that GAF-R might be used to evaluate the effective energy from the film-density growth without the need for ionization-chamber measurements.

Influence of Force Fields and Quantum Chemistry Approach on Spectral Densities of BChl a in Solution and in FMO Proteins

DOE Office of Scientific and Technical Information (OSTI.GOV)

Chandrasekaran, Suryanarayanan; Aghtar, Mortaza; Valleau, Stéphanie

2015-08-06

Studies on light-harvesting (LH) systems have attracted much attention after the finding of long-lived quantum coherences in the exciton dynamics of the Fenna–Matthews–Olson (FMO) complex. In this complex, excitation energy transfer occurs between the bacteriochlorophyll a (BChl a) pigments. Two quantum mechanics/molecular mechanics (QM/MM) studies, each with a different force-field and quantum chemistry approach, reported different excitation energy distributions for the FMO complex. To understand the reasons for these differences in the predicted excitation energies, we have carried out a comparative study between the simulations using the CHARMM and AMBER force field and the Zerner intermediate neglect of differential orbitalmore » (ZINDO)/S and time-dependent density functional theory (TDDFT) quantum chemistry methods. The calculations using the CHARMM force field together with ZINDO/S or TDDFT always show a wider spread in the energy distribution compared to those using the AMBER force field. High- or low-energy tails in these energy distributions result in larger values for the spectral density at low frequencies. A detailed study on individual BChl a molecules in solution shows that without the environment, the density of states is the same for both force field sets. Including the environmental point charges, however, the excitation energy distribution gets broader and, depending on the applied methods, also asymmetric. The excitation energy distribution predicted using TDDFT together with the AMBER force field shows a symmetric, Gaussian-like distribution.« less

Relativistic density functional theory with picture-change corrected electron density based on infinite-order Douglas-Kroll-Hess method

NASA Astrophysics Data System (ADS)

Oyama, Takuro; Ikabata, Yasuhiro; Seino, Junji; Nakai, Hiromi

2017-07-01

This Letter proposes a density functional treatment based on the two-component relativistic scheme at the infinite-order Douglas-Kroll-Hess (IODKH) level. The exchange-correlation energy and potential are calculated using the electron density based on the picture-change corrected density operator transformed by the IODKH method. Numerical assessments indicated that the picture-change uncorrected density functional terms generate significant errors, on the order of hartree for heavy atoms. The present scheme was found to reproduce the energetics in the four-component treatment with high accuracy.

Aqueous lithium air batteries

DOEpatents

Visco, Steven J.; Nimon, Yevgeniy S.; De Jonghe, Lutgard C.; Petrov, Alexei; Goncharenko, Nikolay

2017-05-23

Aqueous Li/Air secondary battery cells are configurable to achieve high energy density and prolonged cycle life. The cells include a protected a lithium metal or alloy anode and an aqueous catholyte in a cathode compartment. The aqueous catholyte comprises an evaporative-loss resistant and/or polyprotic active compound or active agent that partakes in the discharge reaction and effectuates cathode capacity for discharge in the acidic region. This leads to improved performance including one or more of increased specific energy, improved stability on open circuit, and prolonged cycle life, as well as various methods, including a method of operating an aqueous Li/Air cell to simultaneously achieve improved energy density and prolonged cycle life.

Trial densities for the extended Thomas-Fermi model

NASA Astrophysics Data System (ADS)

Yu, An; Jimin, Hu

1996-02-01

A new and simplified form of nuclear densities is proposed for the extended Thomas-Fermi method (ETF) and applied to calculate the ground-state properties of several spherical nuclei, with results comparable or even better than other conventional density profiles. With the expectation value method (EVM) for microscopic corrections we checked our new densities for spherical nuclei. The binding energies of ground states almost reproduce the Hartree-Fock (HF) calculations exactly. Further applications to nuclei far away from the β-stability line are discussed.

Microscopically based energy density functionals for nuclei using the density matrix expansion. II. Full optimization and validation

NASA Astrophysics Data System (ADS)

Navarro Pérez, R.; Schunck, N.; Dyhdalo, A.; Furnstahl, R. J.; Bogner, S. K.

2018-05-01

Background: Energy density functional methods provide a generic framework to compute properties of atomic nuclei starting from models of nuclear potentials and the rules of quantum mechanics. Until now, the overwhelming majority of functionals have been constructed either from empirical nuclear potentials such as the Skyrme or Gogny forces, or from systematic gradient-like expansions in the spirit of the density functional theory for atoms. Purpose: We seek to obtain a usable form of the nuclear energy density functional that is rooted in the modern theory of nuclear forces. We thus consider a functional obtained from the density matrix expansion of local nuclear potentials from chiral effective field theory. We propose a parametrization of this functional carefully calibrated and validated on selected ground-state properties that is suitable for large-scale calculations of nuclear properties. Methods: Our energy functional comprises two main components. The first component is a non-local functional of the density and corresponds to the direct part (Hartree term) of the expectation value of local chiral potentials on a Slater determinant. Contributions to the mean field and the energy of this term are computed by expanding the spatial, finite-range components of the chiral potential onto Gaussian functions. The second component is a local functional of the density and is obtained by applying the density matrix expansion to the exchange part (Fock term) of the expectation value of the local chiral potential. We apply the UNEDF2 optimization protocol to determine the coupling constants of this energy functional. Results: We obtain a set of microscopically constrained functionals for local chiral potentials from leading order up to next-to-next-to-leading order with and without three-body forces and contributions from Δ excitations. These functionals are validated on the calculation of nuclear and neutron matter, nuclear mass tables, single-particle shell structure in closed-shell nuclei, and the fission barrier of 240Pu. Quantitatively, they perform noticeably better than the more phenomenological Skyrme functionals. Conclusions: The inclusion of higher-order terms in the chiral perturbation expansion seems to produce a systematic improvement in predicting nuclear binding energies while the impact on other observables is not really significant. This result is especially promising since all the fits have been performed at the single-reference level of the energy density functional approach, where important collective correlations such as center-of-mass correction, rotational correction, or zero-point vibrational energies have not been taken into account yet.

Extended screened exchange functional derived from transcorrelated density functional theory.

PubMed

Umezawa, Naoto

2017-09-14

We propose a new formulation of the correlation energy functional derived from the transcorrelated method in use in density functional theory (TC-DFT). An effective Hamiltonian, H TC , is introduced by a similarity transformation of a many-body Hamiltonian, H, with respect to a complex function F: H TC =1FHF. It is proved that an expectation value of H TC for a normalized single Slater determinant, D n , corresponds to the total energy: E[n] = ⟨Ψ n |H|Ψ n ⟩/⟨Ψ n |Ψ n ⟩ = ⟨D n |H TC |D n ⟩ under the two assumptions: (1) The electron density nr associated with a trial wave function Ψ n = D n F is v-representable and (2) Ψ n and D n give rise to the same electron density nr. This formulation, therefore, provides an alternative expression of the total energy that is useful for the development of novel correlation energy functionals. By substituting a specific function for F, we successfully derived a model correlation energy functional, which resembles the functional form of the screened exchange method. The proposed functional, named the extended screened exchange (ESX) functional, is described within two-body integrals and is parametrized for a numerically exact correlation energy of the homogeneous electron gas. The ESX functional does not contain any ingredients of (semi-)local functionals and thus is totally free from self-interactions. The computational cost for solving the self-consistent-field equation is comparable to that of the Hartree-Fock method. We apply the ESX functional to electronic structure calculations for a solid silicon, H - ion, and small atoms. The results demonstrate that the TC-DFT formulation is promising for the systematic improvement of the correlation energy functional.

Assessment of Ab Initio and Density Functional Theory Methods for the Excitations of Donor-Acceptor Complexes: The Case of the Benzene-Tetracyanoethylene Model.

PubMed

Xu, Peng; Zhang, Cai-Rong; Wang, Wei; Gong, Ji-Jun; Liu, Zi-Jiang; Chen, Hong-Shan

2018-04-10

The understanding of the excited-state properties of electron donors, acceptors and their interfaces in organic optoelectronic devices is a fundamental issue for their performance optimization. In order to obtain a balanced description of the different excitation types for electron-donor-acceptor systems, including the singlet charge transfer (CT), local excitations, and triplet excited states, several ab initio and density functional theory (DFT) methods for excited-state calculations were evaluated based upon the selected model system of benzene-tetracyanoethylene (B-TCNE) complexes. On the basis of benchmark calculations of the equation-of-motion coupled-cluster with single and double excitations method, the arithmetic mean of the absolute errors and standard errors of the electronic excitation energies for the different computational methods suggest that the M11 functional in DFT is superior to the other tested DFT functionals, and time-dependent DFT (TDDFT) with the Tamm-Dancoff approximation improves the accuracy of the calculated excitation energies relative to that of the full TDDFT. The performance of the M11 functional underlines the importance of kinetic energy density, spin-density gradient, and range separation in the development of novel DFT functionals. According to the TDDFT results, the performances of the different TDDFT methods on the CT properties of the B-TCNE complexes were also analyzed.

Beyond Kohn-Sham Approximation: Hybrid Multistate Wave Function and Density Functional Theory.

PubMed

Gao, Jiali; Grofe, Adam; Ren, Haisheng; Bao, Peng

2016-12-15

A multistate density functional theory (MSDFT) is presented in which the energies and densities for the ground and excited states are treated on the same footing using multiconfigurational approaches. The method can be applied to systems with strong correlation and to correctly describe the dimensionality of the conical intersections between strongly coupled dissociative potential energy surfaces. A dynamic-then-static framework for treating electron correlation is developed to first incorporate dynamic correlation into contracted state functions through block-localized Kohn-Sham density functional theory (KSDFT), followed by diagonalization of the effective Hamiltonian to include static correlation. MSDFT can be regarded as a hybrid of wave function and density functional theory. The method is built on and makes use of the current approximate density functional developed in KSDFT, yet it retains its computational efficiency to treat strongly correlated systems that are problematic for KSDFT but too large for accurate WFT. The results presented in this work show that MSDFT can be applied to photochemical processes involving conical intersections.

Single-particle spectral density of the unitary Fermi gas: Novel approach based on the operator product expansion, sum rules and the maximum entropy method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gubler, Philipp, E-mail: pgubler@riken.jp; RIKEN Nishina Center, Wako, Saitama 351-0198; Yamamoto, Naoki

2015-05-15

Making use of the operator product expansion, we derive a general class of sum rules for the imaginary part of the single-particle self-energy of the unitary Fermi gas. The sum rules are analyzed numerically with the help of the maximum entropy method, which allows us to extract the single-particle spectral density as a function of both energy and momentum. These spectral densities contain basic information on the properties of the unitary Fermi gas, such as the dispersion relation and the superfluid pairing gap, for which we obtain reasonable agreement with the available results based on quantum Monte-Carlo simulations.

Stochastic density functional theory at finite temperatures

NASA Astrophysics Data System (ADS)

Cytter, Yael; Rabani, Eran; Neuhauser, Daniel; Baer, Roi

2018-03-01

Simulations in the warm dense matter regime using finite temperature Kohn-Sham density functional theory (FT-KS-DFT), while frequently used, are computationally expensive due to the partial occupation of a very large number of high-energy KS eigenstates which are obtained from subspace diagonalization. We have developed a stochastic method for applying FT-KS-DFT, that overcomes the bottleneck of calculating the occupied KS orbitals by directly obtaining the density from the KS Hamiltonian. The proposed algorithm scales as O (" close=")N3T3)">N T-1 and is compared with the high-temperature limit scaling O Random-Phase Approximation Methods

NASA Astrophysics Data System (ADS)

Chen, Guo P.; Voora, Vamsee K.; Agee, Matthew M.; Balasubramani, Sree Ganesh; Furche, Filipp

2017-05-01

Random-phase approximation (RPA) methods are rapidly emerging as cost-effective validation tools for semilocal density functional computations. We present the theoretical background of RPA in an intuitive rather than formal fashion, focusing on the physical picture of screening and simple diagrammatic analysis. A new decomposition of the RPA correlation energy into plasmonic modes leads to an appealing visualization of electron correlation in terms of charge density fluctuations. Recent developments in the areas of beyond-RPA methods, RPA correlation potentials, and efficient algorithms for RPA energy and property calculations are reviewed. The ability of RPA to approximately capture static correlation in molecules is quantified by an analysis of RPA natural occupation numbers. We illustrate the use of RPA methods in applications to small-gap systems such as open-shell d- and f-element compounds, radicals, and weakly bound complexes, where semilocal density functional results exhibit strong functional dependence.

Subsystem density functional theory with meta-generalized gradient approximation exchange-correlation functionals.

PubMed

Śmiga, Szymon; Fabiano, Eduardo; Laricchia, Savio; Constantin, Lucian A; Della Sala, Fabio

2015-04-21

We analyze the methodology and the performance of subsystem density functional theory (DFT) with meta-generalized gradient approximation (meta-GGA) exchange-correlation functionals for non-bonded molecular systems. Meta-GGA functionals depend on the Kohn-Sham kinetic energy density (KED), which is not known as an explicit functional of the density. Therefore, they cannot be directly applied in subsystem DFT calculations. We propose a Laplacian-level approximation to the KED which overcomes this limitation and provides a simple and accurate way to apply meta-GGA exchange-correlation functionals in subsystem DFT calculations. The so obtained density and energy errors, with respect to the corresponding supermolecular calculations, are comparable with conventional approaches, depending almost exclusively on the approximations in the non-additive kinetic embedding term. An embedding energy error decomposition explains the accuracy of our method.

Density scaling for multiplets

NASA Astrophysics Data System (ADS)

Nagy, Á.

2011-02-01

Generalized Kohn-Sham equations are presented for lowest-lying multiplets. The way of treating non-integer particle numbers is coupled with an earlier method of the author. The fundamental quantity of the theory is the subspace density. The Kohn-Sham equations are similar to the conventional Kohn-Sham equations. The difference is that the subspace density is used instead of the density and the Kohn-Sham potential is different for different subspaces. The exchange-correlation functional is studied using density scaling. It is shown that there exists a value of the scaling factor ζ for which the correlation energy disappears. Generalized OPM and Krieger-Li-Iafrate (KLI) methods incorporating correlation are presented. The ζKLI method, being as simple as the original KLI method, is proposed for multiplets.

Ionization energies and electron affinities from a random-phase-approximation many-body Green's-function method including exchange interactions

NASA Astrophysics Data System (ADS)

Heßelmann, Andreas

2017-06-01

A many-body Green's-function method employing an infinite order summation of ring and exchange-ring contributions to the self-energy is presented. The individual correlation and relaxation contributions to the quasiparticle energies are calculated using an iterative scheme which utilizes density fitting of the particle-hole, particle-particle and hole-hole densities. It is shown that the ionization energies and electron affinities of this approach agree better with highly accurate coupled-cluster singles and doubles with perturbative triples energy difference results than those obtained with second-order Green's-function approaches. An analysis of the correlation and relaxation terms of the self-energy for the direct- and exchange-random-phase-approximation (RPA) Green's-function methods shows that the inclusion of exchange interactions leads to a reduction of the two contributions in magnitude. These differences, however, strongly cancel each other when summing the individual terms to the quasiparticle energies. Due to this, the direct- and exchange-RPA methods perform similarly for the description of ionization energies (IPs) and electron affinities (EAs). The coupled-cluster reference IPs and EAs, if corrected to the adiabatic energy differences between the neutral and charged molecules, were shown to be in very good agreement with experimental measurements.

Analytical excited state forces for the time-dependent density-functional tight-binding method.

PubMed

Heringer, D; Niehaus, T A; Wanko, M; Frauenheim, Th

2007-12-01

An analytical formulation for the geometrical derivatives of excitation energies within the time-dependent density-functional tight-binding (TD-DFTB) method is presented. The derivation is based on the auxiliary functional approach proposed in [Furche and Ahlrichs, J Chem Phys 2002, 117, 7433]. To validate the quality of the potential energy surfaces provided by the method, adiabatic excitation energies, excited state geometries, and harmonic vibrational frequencies were calculated for a test set of molecules in excited states of different symmetry and multiplicity. According to the results, the TD-DFTB scheme surpasses the performance of configuration interaction singles and the random phase approximation but has a lower quality than ab initio time-dependent density-functional theory. As a consequence of the special form of the approximations made in TD-DFTB, the scaling exponent of the method can be reduced to three, similar to the ground state. The low scaling prefactor and the satisfactory accuracy of the method makes TD-DFTB especially suitable for molecular dynamics simulations of dozens of atoms as well as for the computation of luminescence spectra of systems containing hundreds of atoms. (c) 2007 Wiley Periodicals, Inc.

Efficient exact-exchange time-dependent density-functional theory methods and their relation to time-dependent Hartree-Fock.

PubMed

Hesselmann, Andreas; Görling, Andreas

2011-01-21

A recently introduced time-dependent exact-exchange (TDEXX) method, i.e., a response method based on time-dependent density-functional theory that treats the frequency-dependent exchange kernel exactly, is reformulated. In the reformulated version of the TDEXX method electronic excitation energies can be calculated by solving a linear generalized eigenvalue problem while in the original version of the TDEXX method a laborious frequency iteration is required in the calculation of each excitation energy. The lowest eigenvalues of the new TDEXX eigenvalue equation corresponding to the lowest excitation energies can be efficiently obtained by, e.g., a version of the Davidson algorithm appropriate for generalized eigenvalue problems. Alternatively, with the help of a series expansion of the new TDEXX eigenvalue equation, standard eigensolvers for large regular eigenvalue problems, e.g., the standard Davidson algorithm, can be used to efficiently calculate the lowest excitation energies. With the help of the series expansion as well, the relation between the TDEXX method and time-dependent Hartree-Fock is analyzed. Several ways to take into account correlation in addition to the exact treatment of exchange in the TDEXX method are discussed, e.g., a scaling of the Kohn-Sham eigenvalues, the inclusion of (semi)local approximate correlation potentials, or hybrids of the exact-exchange kernel with kernels within the adiabatic local density approximation. The lowest lying excitations of the molecules ethylene, acetaldehyde, and pyridine are considered as examples.

Excited State Studies of Polyacenes Using the All-Order Constricted Variational Density Functional Theory with Orbital Relaxation.

PubMed

Senn, Florian; Krykunov, Mykhaylo

2015-10-22

For the polyacenes series from naphthalene to hexacene, we present the vertical singlet excitation energies 1 (1)La and 1 (1)Lb, as well as the first triplet excitation energies obtained by the all-order constricted variational density functional theory with orbital relaxation (R-CV(∞)-DFT). R-CV(∞)-DFT is a further development of variational density functional theory (CV(∞)-DFT), which has already been successfully applied for the calculation of the vertical singlet excitation energies (1)La and (1)Lb for polyacenes,15 and we show that one obtains consistent excitation energies using the local density approximation as a functional for singlet as well as for triplet excitations when going beyond the linear response theory. Furthermore, we apply self-consistent field density functional theory (ΔSCF-DFT) and compare the obtained excitation energies for the first triplet excitations T1, where, due to the character of the transition, ΔSCF-DFT and R-CV(∞)-DFT become numerically equivalent, and for the singlet excitations 1 (1)La and 1 (1)Lb, where the two methods differ.

A density difference based analysis of orbital-dependent exchange-correlation functionals

NASA Astrophysics Data System (ADS)

Grabowski, Ireneusz; Teale, Andrew M.; Fabiano, Eduardo; Śmiga, Szymon; Buksztel, Adam; Della Sala, Fabio

2014-03-01

We present a density difference based analysis for a range of orbital-dependent Kohn-Sham functionals. Results for atoms, some members of the neon isoelectronic series and small molecules are reported and compared with ab initio wave function calculations. Particular attention is paid to the quality of approximations to the exchange-only optimised effective potential (OEP) approach: we consider both the localised Hartree-Fock as well as the Krieger-Li-Iafrate methods. Analysis of density differences at the exchange-only level reveals the impact of the approximations on the resulting electronic densities. These differences are further quantified in terms of the ground state energies, frontier orbital energy differences and highest occupied orbital energies obtained. At the correlated level, an OEP approach based on a perturbative second-order correlation energy expression is shown to deliver results comparable with those from traditional wave function approaches, making it suitable for use as a benchmark against which to compare standard density functional approximations.

Analytic second derivative of the energy for density-functional tight-binding combined with the fragment molecular orbital method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nakata, Hiroya, E-mail: hiroya.nakata.gt@kyocera.jp; Nishimoto, Yoshio; Fedorov, Dmitri G.

2016-07-28

The analytic second derivative of the energy is developed for the fragment molecular orbital (FMO) method combined with density-functional tight-binding (DFTB), enabling simulations of infrared and Raman spectra of large molecular systems. The accuracy of the method is established in comparison to full DFTB without fragmentation for a set of representative systems. The performance of the FMO-DFTB Hessian is discussed for molecular systems containing up to 10 041 atoms. The method is applied to the study of the binding of α-cyclodextrin to polyethylene glycol, and the calculated IR spectrum of an epoxy amine oligomer reproduces experiment reasonably well.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Do, Hainam, E-mail: h.do@nottingham.ac.uk, E-mail: richard.wheatley@nottingham.ac.uk; Wheatley, Richard J., E-mail: h.do@nottingham.ac.uk, E-mail: richard.wheatley@nottingham.ac.uk

A robust and model free Monte Carlo simulation method is proposed to address the challenge in computing the classical density of states and partition function of solids. Starting from the minimum configurational energy, the algorithm partitions the entire energy range in the increasing energy direction (“upward”) into subdivisions whose integrated density of states is known. When combined with the density of states computed from the “downward” energy partitioning approach [H. Do, J. D. Hirst, and R. J. Wheatley, J. Chem. Phys. 135, 174105 (2011)], the equilibrium thermodynamic properties can be evaluated at any temperature and in any phase. The methodmore » is illustrated in the context of the Lennard-Jones system and can readily be extended to other molecular systems and clusters for which the structures are known.« less

Monte Carlo method for computing density of states and quench probability of potential energy and enthalpy landscapes.

PubMed

Mauro, John C; Loucks, Roger J; Balakrishnan, Jitendra; Raghavan, Srikanth

2007-05-21

The thermodynamics and kinetics of a many-body system can be described in terms of a potential energy landscape in multidimensional configuration space. The partition function of such a landscape can be written in terms of a density of states, which can be computed using a variety of Monte Carlo techniques. In this paper, a new self-consistent Monte Carlo method for computing density of states is described that uses importance sampling and a multiplicative update factor to achieve rapid convergence. The technique is then applied to compute the equilibrium quench probability of the various inherent structures (minima) in the landscape. The quench probability depends on both the potential energy of the inherent structure and the volume of its corresponding basin in configuration space. Finally, the methodology is extended to the isothermal-isobaric ensemble in order to compute inherent structure quench probabilities in an enthalpy landscape.

Mass density images from the diffraction enhanced imaging technique.

PubMed

Hasnah, M O; Parham, C; Pisano, E D; Zhong, Z; Oltulu, O; Chapman, D

2005-02-01

Conventional x-ray radiography measures the projected x-ray attenuation of an object. It requires attenuation differences to obtain contrast of embedded features. In general, the best absorption contrast is obtained at x-ray energies where the absorption is high, meaning a high absorbed dose. Diffraction-enhanced imaging (DEI) derives contrast from absorption, refraction, and extinction. The refraction angle image of DEI visualizes the spatial gradient of the projected electron density of the object. The projected electron density often correlates well with the projected mass density and projected absorption in soft-tissue imaging, yet the mass density is not an "energy"-dependent property of the object, as is the case of absorption. This simple difference can lead to imaging with less x-ray exposure or dose. In addition, the mass density image can be directly compared (i.e., a signal-to-noise comparison) with conventional radiography. We present the method of obtaining the mass density image, the results of experiments in which comparisons are made with radiography, and an application of the method to breast cancer imaging.

Determination of Energy Independent Neutron Densities using Dirac Phenomenology based on the RIA

NASA Astrophysics Data System (ADS)

Clark, B. C.; Kerr, L. J.; Hama, S.; Mercer, R. L.

2002-04-01

A new method for extracting neutron densities from intermediate energy elastic proton-nucleus scattering observables using a global Dirac phenomenological (DP) approach based on the Relativistic Impulse Approximation (RIA) is presented. (B. C. Clark, et al.) BAPS Vol 46, No. 7 pg.139, 2001. We have considered data sets for ^40Ca, ^48Ca and ^208Pb and energies from 500 MeV to 1040 MeV. The global fits are successful in reproducing the data and in predicting data sets not included in the analysis. Using this global DP approach we have obtained energy independent neutron densities. The vector point proton density distribution, ρ^p_v, is determined from the empirical charge density after unfolding the proton form factor. The other densities, ρ^n_v, ρ^p_s, ρ^n_s, are parameterized using the cosh form given in our paper on global DP optical potentials.(E. D. Cooper, et al.) Phys Rev. 47C, pg. 297, 1993 Neutron skin thicknesses extracted using the global analysis are compared to predictions from theoretical models.

Electron momentum density and band structure calculations of α- and β-GeTe

NASA Astrophysics Data System (ADS)

Vadkhiya, Laxman; Arora, Gunjan; Rathor, Ashish; Ahuja, B. L.

2011-12-01

We have measured isotropic experimental Compton profile of α-GeTe by employing high energy (662 keV) γ-radiation from a 137Cs isotope. To compare our experiment, we have also computed energy bands, density of states, electron momentum densities and Compton profiles of α- and β-phases of GeTe using the linear combination of atomic orbitals method. The electron momentum density is found to play a major role in understanding the topology of bands in the vicinity of the Fermi level. It is seen that the density functional theory (DFT) with generalised gradient approximation is relatively in better agreement with the experiment than the local density approximation and hybrid Hartree-Fock/DFT.

Method and apparatus for measuring the momentum, energy, power, and power density profile of intense particle beams

DOEpatents

Gammel, George M.; Kugel, Henry W.

1992-10-06

A method and apparatus for determining the power, momentum, energy, and power density profile of high momentum mass flow. Small probe projectiles of appropriate size, shape and composition are propelled through an intense particle beam at equal intervals along an axis perpendicular to the beam direction. Probe projectiles are deflected by collisions with beam particles. The net beam-induced deflection of each projectile is measured after it passes through the intense particle beam into an array of suitable detectors.

A methodology for mapping forest latent heat flux densities using remote sensing

NASA Technical Reports Server (NTRS)

Pierce, Lars L.; Congalton, Russell G.

1988-01-01

Surface temperatures and reflectances of an upper elevation Sierran mixed conifer forest were monitored using the Thematic Mapper Simulator sensor during the summer of 1985 in order to explore the possibility of using remote sensing to determine the distribution of solar energy on forested watersheds. The results show that the method is capable of quantifying the relative energy allocation relationships between the two cover types defined in the study. It is noted that the method also has the potential to map forest latent heat flux densities.

BiFeO3-doped (K0.5,Na0.5)(Mn0.005,Nb0.995)O3 ferroelectric thin film capacitors for high energy density storage applications

NASA Astrophysics Data System (ADS)

Won, Sung Sik; Kawahara, Masami; Kuhn, Lindsay; Venugopal, Vineeth; Kwak, Jiyeon; Kim, Ill Won; Kingon, Angus I.; Kim, Seung-Hyun

2017-04-01

Environmentally benign lead-free ferroelectric (K0.5,Na0.5)(Mn0.005,Nb0.995)O3 (KNMN) thin film capacitors with a small concentration of a BiFeO3 (BF) dopant were prepared by a cost effective chemical solution deposition method for high energy density storage device applications. 6 mol. % BF-doped KNMN thin films showed very slim hysteresis loops with high maximum and near-zero remanent polarization values due to a phase transition from the orthorhombic structure to the pseudo-cubic structure. Increasing the electric field up to 2 MV/cm, the total energy storage density (Jtotal), the effective recoverable energy density (Jeff), and the energy conversion efficiency (η) of lead-free KNMN-BF thin film capacitors were 31.0 J/cm3, 28.0 J/cm3, and 90.3%, respectively. In addition, these thin film capacitors exhibited a fast discharge time of a few μs and a high temperature stability up to 200 °C, proving their strong potential for high energy density storage and conversion applications.

Towards the blackbox computation of magnetic exchange coupling parameters in polynuclear transition-metal complexes: theory, implementation, and application.

PubMed

Phillips, Jordan J; Peralta, Juan E

2013-05-07

We present a method for calculating magnetic coupling parameters from a single spin-configuration via analytic derivatives of the electronic energy with respect to the local spin direction. This method does not introduce new approximations beyond those found in the Heisenberg-Dirac Hamiltonian and a standard Kohn-Sham Density Functional Theory calculation, and in the limit of an ideal Heisenberg system it reproduces the coupling as determined from spin-projected energy-differences. Our method employs a generalized perturbative approach to constrained density functional theory, where exact expressions for the energy to second order in the constraints are obtained by analytic derivatives from coupled-perturbed theory. When the relative angle between magnetization vectors of metal atoms enters as a constraint, this allows us to calculate all the magnetic exchange couplings of a system from derivatives with respect to local spin directions from the high-spin configuration. Because of the favorable computational scaling of our method with respect to the number of spin-centers, as compared to the broken-symmetry energy-differences approach, this opens the possibility for the blackbox exploration of magnetic properties in large polynuclear transition-metal complexes. In this work we outline the motivation, theory, and implementation of this method, and present results for several model systems and transition-metal complexes with a variety of density functional approximations and Hartree-Fock.

High-Performance Li-Ion Capacitor Based on an Activated Carbon Cathode and Well-Dispersed Ultrafine TiO2 Nanoparticles Embedded in Mesoporous Carbon Nanofibers Anode.

PubMed

Yang, Cheng; Lan, Jin-Le; Liu, Wen-Xiao; Liu, Yuan; Yu, Yun-Hua; Yang, Xiao-Ping

2017-06-07

A novel Li-ion capacitor based on an activated carbon cathode and a well-dispersed ultrafine TiO 2 nanoparticles embedded in mesoporous carbon nanofibers (TiO 2 @PCNFs) anode was reported. A series of TiO 2 @PCNFs anode materials were prepared via a scalable electrospinning method followed by carbonization and a postetching method. The size of TiO 2 nanoparticles and the mesoporous structure of the TiO 2 @PCNFs were tuned by varying amounts of tetraethyl orthosilicate (TEOS) to increase the energy density and power density of the LIC significantly. Such a subtle designed LIC displayed a high energy density of 67.4 Wh kg -1 at a power density of 75 W kg -1 . Meanwhile, even when the power density was increased to 5 kW kg -1 , the energy density can still maintain 27.5 Wh kg -1 . Moreover, the LIC displayed a high capacitance retention of 80.5% after 10000 cycles at 10 A g -1 . The outstanding electrochemical performance can be contributed to the synergistic effect of the well-dispersed ultrafine TiO 2 nanoparticles, the abundant mesoporous structure, and the conductive carbon networks.

Uncovering the nonadiabatic response of geosynchronous electrons to geomagnetic disturbance

USGS Publications Warehouse

Gannon, Jennifer; Elkington, Scot R.; Onsager, Terrance G.

2012-01-01

We describe an energy spectrum method for scaling electron integral flux, which is measured at a constant energy, to phase space density at a constant value of the first adiabatic invariant which removes much of the variation due to reversible adiabatic effects. Applying this method to nearly a solar cycle (1995 - 2006) of geosynchronous electron integral flux (E>2.0MeV) from the GOES satellites, we see that much of the diurnal variation in electron phase space density at constant energy can be removed by the transformation to phase space density at constant μ (4000 MeV/G). This allows us a clearer picture of underlying non-adiabatic electron population changes due to geomagnetic activity. Using scaled phase space density, we calculate the percentage of geomagnetic storms resulting in an increase, decrease or no change in geosynchronous electrons as 38%, 7%, and 55%, respectively. We also show examples of changes in the electron population that may be different than the unscaled fluxes alone suggest. These examples include sudden electron enhancements during storms which appear during the peak of negative Dst for μ-scaled phase space density, contrary to the slow increase seen during the recovery phase for unscaled phase space density for the same event.

Extending density functional embedding theory for covalently bonded systems.

PubMed

Yu, Kuang; Carter, Emily A

2017-12-19

Quantum embedding theory aims to provide an efficient solution to obtain accurate electronic energies for systems too large for full-scale, high-level quantum calculations. It adopts a hierarchical approach that divides the total system into a small embedded region and a larger environment, using different levels of theory to describe each part. Previously, we developed a density-based quantum embedding theory called density functional embedding theory (DFET), which achieved considerable success in metals and semiconductors. In this work, we extend DFET into a density-matrix-based nonlocal form, enabling DFET to study the stronger quantum couplings between covalently bonded subsystems. We name this theory density-matrix functional embedding theory (DMFET), and we demonstrate its performance in several test examples that resemble various real applications in both chemistry and biochemistry. DMFET gives excellent results in all cases tested thus far, including predicting isomerization energies, proton transfer energies, and highest occupied molecular orbital-lowest unoccupied molecular orbital gaps for local chromophores. Here, we show that DMFET systematically improves the quality of the results compared with the widely used state-of-the-art methods, such as the simple capped cluster model or the widely used ONIOM method.

Effect of laser irradiation on the early-stage seed formation of laser-induced submicrometer-scale silica spheres

NASA Astrophysics Data System (ADS)

Kim, H. J.; Ha, S. Y.; Hong, Y. J.; Nam, S.; Oh, S. Y.; Lim, C.

2014-04-01

We describe the effect of irradiation on the early-stage seed formation of submicrometer-scale (SS) SiO2 spheres by a laser-induced process. A quartz cell containing chemical reagents was exposed to a pulsed laser (Nd:YAG, 532 nm) tuned to various energy densities, while SiO2 SS spheres are synthesized in the quartz cell by the Stöber, Fink, and Bohn method. Higher laser energy densities typically produce wider size distributions. In particular, bidisperse SiO2 spheres were obtained when the laser energy density was 1.15 J/cm2. The size distributions were widest with 1.15 J/cm2 and narrowest with 0.33 J/cm2 laser energy density. However, the compositions of the SiO2 SS spheres were not affected by laser irradiation, and we observed by the energy-dispersive X-ray spectroscopy that the compositions of the irradiated and nonirradiated SiO2 SS spheres were the same.

Temporal soil bulk density following tillage

USDA-ARS?s Scientific Manuscript database

Soil is the medium for air, energy, water, and chemical transport between the atmosphere and the solid earth. Soil bulk density is a key variable impacting the rate at which this transport occurs. Typically, soil bulk density is measured by the gravimetric method, where a sample of known volume is t...

Assessment of satiety depends on the energy density and portion size of the test meal

PubMed Central

Williams, Rachel A.; Roe, Liane S.; Rolls, Barbara J.

2013-01-01

Objective Foods that enhance satiety can reduce overconsumption, but the availability of large portions of energy-dense foods may counter their benefits. We tested the influence on meal energy intake of varying the energy density and portion size of food consumed after a preload shown to promote satiety. Design and Methods In a crossover design, 46 women were served lunch on six days. On four days they ate a compulsory salad (300 g, 0.33 kcal/g). Unlike previous studies, instead of varying the preload, the subsequent test meal of pasta was varied between standard and increased levels of both energy density (1.25 or 1.66 kcal/g) and portion size (450 or 600 g). On two control days a salad was not served. Results Following the salad, the energy density and portion size of the test meal independently affected meal energy intake (both p<0.02). Serving the higher-energy-dense pasta increased test meal intake by 153±19 kcal and serving the larger portion of pasta increased test meal intake by 40±16 kcal. Compared to having no salad, consuming the salad decreased test meal intake by 123±18 kcal. Conclusions The effect of satiety-enhancing foods can be influenced by the energy density and portion size of other foods at the meal. PMID:23929544

Defense Small Business Innovation Research Program (SBIR). Volume 4. ARPA, DNA, BMDO, and SOC0M Abstracts of Phase 1 Awards 1993

DTIC Science & Technology

1993-01-01

C-R248 Phone: (619) 455-9741 PI: DAVID ANDING Title: Method for Incorporating High -Fidelity Engineering Models Into Distributed Simulations Abstract...Ferroelectric Capacitors for Pulse Power Electronics Abstract: High -density energy storage and fast discharge will be critical in a variety of high ...to meet the design objectives of High Energy Density Capacitors (HEDC) for energy storage in pulsed power systems (15 to 45 mJ/kg). In the proposed

THE FIRST FERMI IN A HIGH ENERGY NUCLEAR COLLISION.

DOE Office of Scientific and Technical Information (OSTI.GOV)

KRASNITZ,A.

1999-08-09

At very high energies, weak coupling, non-perturbative methods can be used to study classical gluon production in nuclear collisions. One observes in numerical simulations that after an initial formation time, the produced partons are on shell, and their subsequent evolution can be studied using transport theory. At the initial formation time, a simple non-perturbative relation exists between the energy and number densities of the produced partons, and a scale determined by the saturated parton density in the nucleus.

A High Power Density Single-Phase PWM Rectifier With Active Ripple Energy Storage

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Ruxi; Wang, Fei; Boroyevich, Dushan

It is well known that single-phase pulse width modulation rectifiers have second-order harmonic currents and corresponding ripple voltages on the dc bus. The low-frequency harmonic current is normally filtered using a bulk capacitor in the bus, which results in low power density. However, pursuing high power density in converter design is a very important goal in the aerospace applications. This paper studies methods for reducing the energy storage capacitor for single-phase rectifiers. The minimum ripple energy storage requirement is derived independently of a specific topology. Based on theminimum ripple energy requirement, the feasibility of the active capacitor s reduction schemesmore » is verified. Then, we propose a bidirectional buck boost converter as the ripple energy storage circuit, which can effectively reduce the energy storage capacitance. The analysis and design are validated by simulation and experimental results.« less

A comparison of food pattern, macro- and some micronutrients density of the diet across different socio-economic zones of Tehran

PubMed Central

Abdollahi, Morteza; Salehi, Forouzan; Kalantari, Naser; Asadilari, Mohsen; Khoshfetrat, Mohammad Reza; Ajami, Marjan

2016-01-01

Background: The consumption of low quality foods is common in low socioeconomic areas; and according to epidemiological studies, the density of nutrients often proves the quality of diet. This study aimed to compare the density of macronutrients and micronutrients in various parts of Tehran. Methods: This was a cross-sectional study performed from September to December 2007 in all the 22 districts of the municipality of Tehran including 1,807 households. Experienced interviewers completed a 24-hour recall questionnaire. To estimate the nutrient densities, nutrient intake (grams or milligrams) was calculated per 1,000 kcal energy intake. To calculate the density of energy intake, energy intake (kcal) was divided by 100 g of foodstuff. The 22 districts of Tehran were divided into five zones of north, center, east, west and south. ANOVA and Tukey tests were used. Results: The highest density of protein and fat intake was observed in the north of Tehran, while carbohydrate density was highest in the west, east and south zones, and energy density was highest in the south zone (p<0.05). Calcium and vitamin C had the highest density in the north of Tehran, and vitamin A and riboflavin had the highest density in the north and center of Tehran, and the lowest level in the south of Tehran (p<0.05). Conclusion: Despite the high density of energy in the south of Tehran, a deficiency of micronutrient intake was obvious, reflecting the importance of the impact of socioeconomic factors. PMID:27390710

Choosing the best method to estimate the energy density of a population using food purchase data.

PubMed

Wrieden, W L; Armstrong, J; Anderson, A S; Sherriff, A; Barton, K L

2015-04-01

Energy density (ED) is a measure of the energy content of a food component or diet relative to a standard unit of weight. Widespread variation in ED assessment methodologies exist. The present study aimed to explore the feasibility of calculating the ED of the Scottish diet using UK food purchase survey data and to identify the most appropriate method for calculating ED for use in the development of a Scottish Dietary Goal that captures any socioeconomic differences. Energy density was calculated using five different methods [food; food and milk; food, milk and energy containing (non-alcoholic) beverages; food, milk and all non-alcoholic beverages; and all food and beverages]. ED of the Scottish diet was estimated for each of the ED methods and data were examined by deprivation category. Mean ED varied from 409 to 847 kJ 100 g(-1) depending on the method used. ED values calculated from food (847 kJ 100 g(-1) ) and food and milk (718 kJ 100 g(-1) ) were most comparable to other published data, with the latter being a more accurate reflection of all food consumed. For these two methods, there was a significant gradient between the most and least deprived quintiles (892-807 and 737-696 kJ 100 g(-1) for food and food and milk, respectively). Because the World Cancer Research Fund recommendations are based on ED from food and milk, it was considered prudent to use this method for policy purposes and for future monitoring work of the Scottish Diet to ensure consistency of reporting and comparability with other published studies. © 2014 The British Dietetic Association Ltd.

Thermal imaging diagnostics of high-current electron beams.

PubMed

Pushkarev, A; Kholodnaya, G; Sazonov, R; Ponomarev, D

2012-10-01

The thermal imaging diagnostics of measuring pulsed electron beam energy density is presented. It provides control of the electron energy spectrum and a measure of the density distribution of the electron beam cross section, the spatial distribution of electrons with energies in the selected range, and the total energy of the electron beam. The diagnostics is based on the thermal imager registration of the imaging electron beam thermal print in a material with low bulk density and low thermal conductivity. Testing of the thermal imaging diagnostics has been conducted on a pulsed electron accelerator TEU-500. The energy of the electrons was 300-500 keV, the density of the electron current was 0.1-0.4 kA/cm(2), the duration of the pulse (at half-height) was 60 ns, and the energy in the pulse was up to 100 J. To register the thermal print, a thermal imager Fluke-Ti10 was used. Testing showed that the sensitivity of a typical thermal imager provides the registration of a pulsed electron beam heat pattern within one pulse with energy density over 0.1 J/cm(2) (or with current density over 10 A/cm(2), pulse duration of 60 ns and electron energy of 400 keV) with the spatial resolution of 0.9-1 mm. In contrast to the method of using radiosensitive (dosimetric) materials, thermal imaging diagnostics does not require either expensive consumables, or plenty of processing time.

The Potential Energy Density in Transverse String Waves Depends Critically on Longitudinal Motion

ERIC Educational Resources Information Center

Rowland, David R.

2011-01-01

The question of the correct formula for the potential energy density in transverse waves on a taut string continues to attract attention (e.g. Burko 2010 "Eur. J. Phys." 31 L71), and at least three different formulae can be found in the literature, with the classic text by Morse and Feshbach ("Methods of Theoretical Physics" pp 126-127) stating…

Calculating electronic correlation effects from densities of transitions

NASA Astrophysics Data System (ADS)

Haydock, Roger

Adding a localized electron to a system of interacting electrons induces a density of transitions described by the time-independent Heisenberg equation. Sequences of these transitions generate interacting states whose total energy is the sum of energies of the constituent transitions. A calculation of magnetic moments for itinerant electrons with Ising interactions illustrates this method. supported by the H. V. Snyder Gift to the University of Oregon.

Quantum Monte Carlo analysis of a charge ordered insulating antiferromagnet: The Ti 4O 7 Magneli phase

DOE PAGES

Benali, Anouar; Shulenburger, Luke; Krogel, Jaron T.; ...

2016-06-07

The Magneli phase Ti 4O 7 is an important transition metal oxide with a wide range of applications because of its interplay between charge, spin, and lattice degrees of freedom. At low temperatures, it has non-trivial magnetic states very close in energy, driven by electronic exchange and correlation interactions. We have examined three low- lying states, one ferromagnetic and two antiferromagnetic, and calculated their energies as well as Ti spin moment distributions using highly accurate Quantum Monte Carlo methods. We compare our results to those obtained from density functional theory- based methods that include approximate corrections for exchange and correlation.more » Our results confirm the nature of the states and their ordering in energy, as compared with density-functional theory methods. However, the energy differences and spin distributions differ. Here, a detailed analysis suggests that non-local exchange-correlation functionals, in addition to other approximations such as LDA+U to account for correlations, are needed to simultaneously obtain better estimates for spin moments, distributions, energy differences and energy gaps.« less

Coupled double-distribution-function lattice Boltzmann method for the compressible Navier-Stokes equations.

PubMed

Li, Q; He, Y L; Wang, Y; Tao, W Q

2007-11-01

A coupled double-distribution-function lattice Boltzmann method is developed for the compressible Navier-Stokes equations. Different from existing thermal lattice Boltzmann methods, this method can recover the compressible Navier-Stokes equations with a flexible specific-heat ratio and Prandtl number. In the method, a density distribution function based on a multispeed lattice is used to recover the compressible continuity and momentum equations, while the compressible energy equation is recovered by an energy distribution function. The energy distribution function is then coupled to the density distribution function via the thermal equation of state. In order to obtain an adjustable specific-heat ratio, a constant related to the specific-heat ratio is introduced into the equilibrium energy distribution function. Two different coupled double-distribution-function lattice Boltzmann models are also proposed in the paper. Numerical simulations are performed for the Riemann problem, the double-Mach-reflection problem, and the Couette flow with a range of specific-heat ratios and Prandtl numbers. The numerical results are found to be in excellent agreement with analytical and/or other solutions.

Quantum mechanical/molecular mechanical/continuum style solvation model: time-dependent density functional theory.

PubMed

Thellamurege, Nandun M; Cui, Fengchao; Li, Hui

2013-08-28

A combined quantum mechanical/molecular mechanical/continuum (QM/MMpol/C) style method is developed for time-dependent density functional theory (TDDFT, including long-range corrected TDDFT) method, induced dipole polarizable force field, and induced surface charge continuum model. Induced dipoles and induced charges are included in the TDDFT equations to solve for the transition energies, relaxed density, and transition density. Analytic gradient is derived and implemented for geometry optimization and molecular dynamics simulation. QM/MMpol/C style DFT and TDDFT methods are used to study the hydrogen bonding of the photoactive yellow protein chromopore in ground state and excited state.

A strategy for analysis of (molecular) equilibrium simulations: Configuration space density estimation, clustering, and visualization

NASA Astrophysics Data System (ADS)

Hamprecht, Fred A.; Peter, Christine; Daura, Xavier; Thiel, Walter; van Gunsteren, Wilfred F.

2001-02-01

We propose an approach for summarizing the output of long simulations of complex systems, affording a rapid overview and interpretation. First, multidimensional scaling techniques are used in conjunction with dimension reduction methods to obtain a low-dimensional representation of the configuration space explored by the system. A nonparametric estimate of the density of states in this subspace is then obtained using kernel methods. The free energy surface is calculated from that density, and the configurations produced in the simulation are then clustered according to the topography of that surface, such that all configurations belonging to one local free energy minimum form one class. This topographical cluster analysis is performed using basin spanning trees which we introduce as subgraphs of Delaunay triangulations. Free energy surfaces obtained in dimensions lower than four can be visualized directly using iso-contours and -surfaces. Basin spanning trees also afford a glimpse of higher-dimensional topographies. The procedure is illustrated using molecular dynamics simulations on the reversible folding of peptide analoga. Finally, we emphasize the intimate relation of density estimation techniques to modern enhanced sampling algorithms.

Evolution of metastable state molecules N2(A3 Σu+) in a nanosecond pulsed discharge: A particle-in-cell/Monte Carlo collisions simulation

NASA Astrophysics Data System (ADS)

Gao, Liang; Sun, Jizhong; Feng, Chunlei; Bai, Jing; Ding, Hongbin

2012-01-01

A particle-in-cell plus Monte Carlo collisions method has been employed to investigate the nitrogen discharge driven by a nanosecond pulse power source. To assess whether the production of the metastable state N2(A3 Σu+) can be efficiently enhanced in a nanosecond pulsed discharge, the evolutions of metastable state N2(A3 Σu+) density and electron energy distribution function have been examined in detail. The simulation results indicate that the ultra short pulse can modulate the electron energy effectively: during the early pulse-on time, high energy electrons give rise to quick electron avalanche and rapid growth of the metastable state N2(A3 Σu+) density. It is estimated that for a single pulse with amplitude of -9 kV and pulse width 30 ns, the metastable state N2(A3 Σu+) density can achieve a value in the order of 109 cm-3. The N2(A3 Σu+) density at such a value could be easily detected by laser-based experimental methods.

Excitation energies from range-separated time-dependent density and density matrix functional theory.

PubMed

Pernal, Katarzyna

2012-05-14

Time-dependent density functional theory (TD-DFT) in the adiabatic formulation exhibits known failures when applied to predicting excitation energies. One of them is the lack of the doubly excited configurations. On the other hand, the time-dependent theory based on a one-electron reduced density matrix functional (time-dependent density matrix functional theory, TD-DMFT) has proven accurate in determining single and double excitations of H(2) molecule if the exact functional is employed in the adiabatic approximation. We propose a new approach for computing excited state energies that relies on functionals of electron density and one-electron reduced density matrix, where the latter is applied in the long-range region of electron-electron interactions. A similar approach has been recently successfully employed in predicting ground state potential energy curves of diatomic molecules even in the dissociation limit, where static correlation effects are dominating. In the paper, a time-dependent functional theory based on the range-separation of electronic interaction operator is rigorously formulated. To turn the approach into a practical scheme the adiabatic approximation is proposed for the short- and long-range components of the coupling matrix present in the linear response equations. In the end, the problem of finding excitation energies is turned into an eigenproblem for a symmetric matrix. Assignment of obtained excitations is discussed and it is shown how to identify double excitations from the analysis of approximate transition density matrix elements. The proposed method used with the short-range local density approximation (srLDA) and the long-range Buijse-Baerends density matrix functional (lrBB) is applied to H(2) molecule (at equilibrium geometry and in the dissociation limit) and to Be atom. The method accounts for double excitations in the investigated systems but, unfortunately, the accuracy of some of them is poor. The quality of the other excitations is in general much better than that offered by TD-DFT-LDA or TD-DMFT-BB approximations if the range-separation parameter is properly chosen. The latter remains an open problem.

Development of advanced polymer nanocomposite capacitors

NASA Astrophysics Data System (ADS)

Mendoza, Miguel

The current development of modern electronics has driven the need for new series of energy storage devices with higher energy density and faster charge/discharge rate. Batteries and capacitors are two of the most widely used energy storage devices. Compared with batteries, capacitors have higher power density and significant higher charge/discharge rate. Therefore, high energy density capacitors play a significant role in modern electronic devices, power applications, space flight technologies, hybrid electric vehicles, portable defibrillators, and pulse power applications. Dielectric film capacitors represent an exceptional alternative for developing high energy density capacitors due to their high dielectric constants, outstanding breakdown voltages, and flexibility. The implementation of high aspect ratio dielectric inclusions such as nanowires into polymer capacitors could lead to further enhancement of its energy density. Therefore, this research effort is focused on the development of a new series of dielectric capacitors composed of nanowire reinforced polymer matrix composites. This concept of nanocomposite capacitors combines the extraordinary physical and chemical properties of the one-dimension (1D) nanoceramics and high dielectric strength of polymer matrices, leading to a capacitor with improved dielectric properties and energy density. Lead-free sodium niobate (NaNbO3) and lead-containing lead magnesium niobate-lead titanate (0.65PMN-0.35PT) nanowires were synthesized following hydrothermal and sol-gel approaches, respectively. The as-prepared nanowires were mixed with a polyvinylidene fluoride (PVDF) matrix using solution-casting method for nanocomposites fabrication. The dielectric constants and breakdown voltages of the NaNbO3/PVDF and 0.65PMN-0.35PT/PVDF nanocomposites were measured under different frequency ranges and temperatures in order to determine their maximum energy (J/cm3) and specific (J/g) densities. The electrical properties of the synthesized nanoceramics were compared with commercially available barium titanate (BaTiO3) and lead zirconate titanate Pb(ZrxTi1-x)O3 powders embedded into a PVDF matrix. The resulting dielectric film capacitors represent an excellent alternative energy storage device for future high energy density applications.

Evaluating interaction energies of weakly bonded systems using the Buckingham-Hirshfeld method

NASA Astrophysics Data System (ADS)

Krishtal, A.; Van Alsenoy, C.; Geerlings, P.

2014-05-01

We present the finalized Buckingham-Hirshfeld method (BHD-DFT) for the evaluation of interaction energies of non-bonded dimers with Density Functional Theory (DFT). In the method, dispersion energies are evaluated from static multipole polarizabilities, obtained on-the-fly from Coupled Perturbed Kohn-Sham calculations and partitioned into diatomic contributions using the iterative Hirshfeld partitioning method. The dispersion energy expression is distributed over four atoms and has therefore a higher delocalized character compared to the standard pairwise expressions. Additionally, full multipolar polarizability tensors are used as opposed to effective polarizabilities, allowing to retain the anisotropic character at no additional computational cost. A density dependent damping function for the BLYP, PBE, BP86, B3LYP, and PBE0 functionals has been implemented, containing two global parameters which were fitted to interaction energies and geometries of a selected number of dimers using a bi-variate RMS fit. The method is benchmarked against the S22 and S66 data sets for equilibrium geometries and the S22x5 and S66x8 data sets for interaction energies around the equilibrium geometry. Best results are achieved using the B3LYP functional with mean average deviation values of 0.30 and 0.24 kcal/mol for the S22 and S66 data sets, respectively. This situates the BHD-DFT method among the best performing dispersion inclusive DFT methods. Effect of counterpoise correction on DFT energies is discussed.

Evaluating interaction energies of weakly bonded systems using the Buckingham-Hirshfeld method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Krishtal, A.; Van Alsenoy, C.; Geerlings, P.

2014-05-14

We present the finalized Buckingham-Hirshfeld method (BHD-DFT) for the evaluation of interaction energies of non-bonded dimers with Density Functional Theory (DFT). In the method, dispersion energies are evaluated from static multipole polarizabilities, obtained on-the-fly from Coupled Perturbed Kohn-Sham calculations and partitioned into diatomic contributions using the iterative Hirshfeld partitioning method. The dispersion energy expression is distributed over four atoms and has therefore a higher delocalized character compared to the standard pairwise expressions. Additionally, full multipolar polarizability tensors are used as opposed to effective polarizabilities, allowing to retain the anisotropic character at no additional computational cost. A density dependent damping functionmore » for the BLYP, PBE, BP86, B3LYP, and PBE0 functionals has been implemented, containing two global parameters which were fitted to interaction energies and geometries of a selected number of dimers using a bi-variate RMS fit. The method is benchmarked against the S22 and S66 data sets for equilibrium geometries and the S22x5 and S66x8 data sets for interaction energies around the equilibrium geometry. Best results are achieved using the B3LYP functional with mean average deviation values of 0.30 and 0.24 kcal/mol for the S22 and S66 data sets, respectively. This situates the BHD-DFT method among the best performing dispersion inclusive DFT methods. Effect of counterpoise correction on DFT energies is discussed.« less

Full synergistic effect of hydrothermal NiCo2O4 nanosheets/CuCo2O4 nanocones supported on Ni foam for high-performance asymmetric supercapacitors

NASA Astrophysics Data System (ADS)

Wen, Shiyang; Liu, Yu; Bai, Hongye; Shao, Rong; Xu, Wei; Shi, Weidong

2018-06-01

In this work, a series of NiCo2O4/CuCo2O4 composites were prepared by a two-step hydrothermal method. The optimized NiCo2O4/CuCo2O4 electrode shows more than 5 times area capacitance (4.97 F cm-2) than pure NiCo2O4 at the current density of 1 mA cm-2. The best performance of sample assembled an asymmetric supercapacitor could reach up to 42 F g-1 at the current density of 1 A g-1. In addition, the maximum energy density of 15 W h kg-1 was achieved with the power density of 814 W kg-1. The as-prepared active electrode material also reveals excellent cycling stability with 90.6% capacitance retention after 5000 cycles. These results indicate potential application in developing energy storage devices with high energy density power density.

3D Freeze-Casting of Cellular Graphene Films for Ultrahigh-Power-Density Supercapacitors.

PubMed

Shao, Yuanlong; El-Kady, Maher F; Lin, Cheng-Wei; Zhu, Guanzhou; Marsh, Kristofer L; Hwang, Jee Youn; Zhang, Qinghong; Li, Yaogang; Wang, Hongzhi; Kaner, Richard B

2016-08-01

3D cellular graphene films with open porosity, high electrical conductivity, and good tensile strength, can be synthesized by a method combining freeze-casting and filtration. The resulting supercapacitors based on 3D porous reduced graphene oxide (RGO) film exhibit extremely high specific power densities and high energy densities. The fabrication process provides an effective means for controlling the pore size, electronic conductivity, and loading mass of the electrode materials, toward devices with high energy-storage performance. © 2016 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Simplified method for creating a density-absorbed dose calibration curve for the low dose range from Gafchromic EBT3 film.

PubMed

Gotanda, Tatsuhiro; Katsuda, Toshizo; Gotanda, Rumi; Kuwano, Tadao; Akagawa, Takuya; Tanki, Nobuyoshi; Tabuchi, Akihiko; Shimono, Tetsunori; Kawaji, Yasuyuki

2016-01-01

Radiochromic film dosimeters have a disadvantage in comparison with an ionization chamber in that the dosimetry process is time-consuming for creating a density-absorbed dose calibration curve. The purpose of this study was the development of a simplified method of creating a density-absorbed dose calibration curve from radiochromic film within a short time. This simplified method was performed using Gafchromic EBT3 film with a low energy dependence and step-shaped Al filter. The simplified method was compared with the standard method. The density-absorbed dose calibration curves created using the simplified and standard methods exhibited approximately similar straight lines, and the gradients of the density-absorbed dose calibration curves were -32.336 and -33.746, respectively. The simplified method can obtain calibration curves within a much shorter time compared to the standard method. It is considered that the simplified method for EBT3 film offers a more time-efficient means of determining the density-absorbed dose calibration curve within a low absorbed dose range such as the diagnostic range.

Simplified method for creating a density-absorbed dose calibration curve for the low dose range from Gafchromic EBT3 film

PubMed Central

Gotanda, Tatsuhiro; Katsuda, Toshizo; Gotanda, Rumi; Kuwano, Tadao; Akagawa, Takuya; Tanki, Nobuyoshi; Tabuchi, Akihiko; Shimono, Tetsunori; Kawaji, Yasuyuki

2016-01-01

Radiochromic film dosimeters have a disadvantage in comparison with an ionization chamber in that the dosimetry process is time-consuming for creating a density-absorbed dose calibration curve. The purpose of this study was the development of a simplified method of creating a density-absorbed dose calibration curve from radiochromic film within a short time. This simplified method was performed using Gafchromic EBT3 film with a low energy dependence and step-shaped Al filter. The simplified method was compared with the standard method. The density-absorbed dose calibration curves created using the simplified and standard methods exhibited approximately similar straight lines, and the gradients of the density-absorbed dose calibration curves were −32.336 and −33.746, respectively. The simplified method can obtain calibration curves within a much shorter time compared to the standard method. It is considered that the simplified method for EBT3 film offers a more time-efficient means of determining the density-absorbed dose calibration curve within a low absorbed dose range such as the diagnostic range. PMID:28144120

Influence of the nuclear level density on the odd-even staggering in 56Fe+p spallation at energies from 300 to 1500 MeV/nucleon

NASA Astrophysics Data System (ADS)

Su, Jun; Zhu, Long; Guo, Chenchen

2018-05-01

Background: Special attention has been paid to study the shell effect and odd-even staggering (OES) in the nuclear spallation. Purpose: In this paper, we investigate the influence of the nuclear level density on the OES in the 56Fe+p spallations at energies from 300 to 1500 MeV/nucleon. Method: The isospin-dependent quantum molecular dynamics (IQMD) model is applied to produce the highly excited and equilibrium remnants, which is then de-excited using the statistical model gemini. The excitation energy of the heaviest hot fragments is applied to match the IQMD model with the gemini model. In the gemini model, the statistical description of the evaporation are based on the Hauser-Feshbach formalism, in which level density prescriptions are applied. Results: By investigating the OES of the excited pre-fragments, it is found that the OES originates at the end of the decay process when the excitation energy is close to the nucleon-emission threshold energy, i.e., the smaller value of the neutron separation energy and proton separation energy. The strong influence of level density on the OES is noticed. Two types of the nuclear level densities, the discrepancy of which is only about 7% near the nucleon emission threshold energy, are used in the model. However, the calculated values of the OES differ by the factor of 3 for the relevant nuclei. Conclusions: It is suggested that, although the particle-separation energies play a key role in determining the OES, the level density at excitation energy lower than the particle-separation energies should be taken into consideration

Analytic second derivative of the energy for density functional theory based on the three-body fragment molecular orbital method

NASA Astrophysics Data System (ADS)

Nakata, Hiroya; Fedorov, Dmitri G.; Zahariev, Federico; Schmidt, Michael W.; Kitaura, Kazuo; Gordon, Mark S.; Nakamura, Shinichiro

2015-03-01

Analytic second derivatives of the energy with respect to nuclear coordinates have been developed for spin restricted density functional theory (DFT) based on the fragment molecular orbital method (FMO). The derivations were carried out for the three-body expansion (FMO3), and the two-body expressions can be obtained by neglecting the three-body corrections. Also, the restricted Hartree-Fock (RHF) Hessian for FMO3 can be obtained by neglecting the density-functional related terms. In both the FMO-RHF and FMO-DFT Hessians, certain terms with small magnitudes are neglected for computational efficiency. The accuracy of the FMO-DFT Hessian in terms of the Gibbs free energy is evaluated for a set of polypeptides and water clusters and found to be within 1 kcal/mol of the corresponding full (non-fragmented) ab initio calculation. The FMO-DFT method is also applied to transition states in SN2 reactions and for the computation of the IR and Raman spectra of a small Trp-cage protein (PDB: 1L2Y). Some computational timing analysis is also presented.

First-principle study of structural, electronic and magnetic properties of (FeC)n (n = 1-8) and (FeC)8TM (TM = V, Cr, Mn and Co) clusters.

PubMed

Li, Cheng-Gang; Zhang, Jie; Zhang, Wu-Qin; Tang, Ya-Nan; Ren, Bao-Zeng; Hu, Yan-Fei

2017-12-13

The structural, electronic and magnetic properties of the (FeC) n (n = 1-8) clusters are studied using the unbiased CALYPSO structure search method and density functional theory. A combination of the PBE functional and 6-311 + G* basis set is used for determining global minima on potential energy surfaces of (FeC) n clusters. Relatively stabilities are analyzed via computing their binding energies, second order difference and HOMO-LUMO gaps. In addition, the origin of magnetic properties, spin density and density of states are discussed in detail, respectively. At last, based on the same computational method, the structures, magnetic properties and density of states are systemically investigated for the 3d (V, Cr, Mn and Co) atom doped (FeC) 8 cluster.

Implementation of an approximate self-energy correction scheme in the orthogonalized linear combination of atomic orbitals method of band-structure calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Gu, Z.; Ching, W.Y.

Based on the Sterne-Inkson model for the self-energy correction to the single-particle energy in the local-density approximation (LDA), we have implemented an approximate energy-dependent and [bold k]-dependent [ital GW] correction scheme to the orthogonalized linear combination of atomic orbital-based local-density calculation for insulators. In contrast to the approach of Jenkins, Srivastava, and Inkson, we evaluate the on-site exchange integrals using the LDA Bloch functions throughout the Brillouin zone. By using a [bold k]-weighted band gap [ital E][sub [ital g

Hot spot formation and stagnation properties in simulations of direct-drive NIF implosions

NASA Astrophysics Data System (ADS)

Schmitt, Andrew J.; Obenschain, Stephen P.

2016-05-01

We investigate different proposed methods of increasing the hot spot energy and radius in inertial confinement fusion implosions. In particular, shock mistiming (preferentially heating the inner edge of the target's fuel) and increasing the initial vapor gas density are investigated as possible control mechanisms. We find that only the latter is effective in substantially increasing the hot spot energy and dimensions while achieving ignition. In all cases an increase in the hot spot energy is accompanied by a decrease in the hot spot energy density (pressure) and both the yield and the gain of the target drop substantially. 2D simulations of increased vapor density targets predict an increase in the robustness of the target with respect to surface perturbations but are accompanied by significant yield degradation.

Domain wall suppression in trapped mixtures of Bose-Einstein condensates

NASA Astrophysics Data System (ADS)

Pepe, Francesco V.; Facchi, Paolo; Florio, Giuseppe; Pascazio, Saverio

2012-08-01

The ground-state energy of a binary mixture of Bose-Einstein condensates can be estimated for large atomic samples by making use of suitably regularized Thomas-Fermi density profiles. By exploiting a variational method on the trial densities the energy can be computed by explicitly taking into account the normalization condition. This yields analytical results and provides the basis for further improvement of the approximation. As a case study, we consider a binary mixture of 87Rb atoms in two different hyperfine states in a double-well potential and discuss the energy crossing between density profiles with different numbers of domain walls, as the number of particles and the interspecies interaction vary.

Multireference Density Functional Theory with Generalized Auxiliary Systems for Ground and Excited States.

PubMed

Chen, Zehua; Zhang, Du; Jin, Ye; Yang, Yang; Su, Neil Qiang; Yang, Weitao

2017-09-21

To describe static correlation, we develop a new approach to density functional theory (DFT), which uses a generalized auxiliary system that is of a different symmetry, such as particle number or spin, from that of the physical system. The total energy of the physical system consists of two parts: the energy of the auxiliary system, which is determined with a chosen density functional approximation (DFA), and the excitation energy from an approximate linear response theory that restores the symmetry to that of the physical system, thus rigorously leading to a multideterminant description of the physical system. The electron density of the physical system is different from that of the auxiliary system and is uniquely determined from the functional derivative of the total energy with respect to the external potential. Our energy functional is thus an implicit functional of the physical system density, but an explicit functional of the auxiliary system density. We show that the total energy minimum and stationary states, describing the ground and excited states of the physical system, can be obtained by a self-consistent optimization with respect to the explicit variable, the generalized Kohn-Sham noninteracting density matrix. We have developed the generalized optimized effective potential method for the self-consistent optimization. Among options of the auxiliary system and the associated linear response theory, reformulated versions of the particle-particle random phase approximation (pp-RPA) and the spin-flip time-dependent density functional theory (SF-TDDFT) are selected for illustration of principle. Numerical results show that our multireference DFT successfully describes static correlation in bond dissociation and double bond rotation.

A Lagrangian discontinuous Galerkin hydrodynamic method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Xiaodong; Morgan, Nathaniel Ray; Burton, Donald E.

Here, we present a new Lagrangian discontinuous Galerkin (DG) hydrodynamic method for solving the two-dimensional gas dynamic equations on unstructured hybrid meshes. The physical conservation laws for the momentum and total energy are discretized using a DG method based on linear Taylor expansions. Three different approaches are investigated for calculating the density variation over the element. The first approach evolves a Taylor expansion of the specific volume field. The second approach follows certain finite element methods and uses the strong mass conservation to calculate the density field at a location inside the element or on the element surface. The thirdmore » approach evolves a Taylor expansion of the density field. The nodal velocity, and the corresponding forces, are explicitly calculated by solving a multidirectional approximate Riemann problem. An effective limiting strategy is presented that ensures monotonicity of the primitive variables. This new Lagrangian DG hydrodynamic method conserves mass, momentum, and total energy. Results from a suite of test problems are presented to demonstrate the robustness and expected second-order accuracy of this new method.« less

A Lagrangian discontinuous Galerkin hydrodynamic method

DOE PAGES

Liu, Xiaodong; Morgan, Nathaniel Ray; Burton, Donald E.

2017-12-11

Here, we present a new Lagrangian discontinuous Galerkin (DG) hydrodynamic method for solving the two-dimensional gas dynamic equations on unstructured hybrid meshes. The physical conservation laws for the momentum and total energy are discretized using a DG method based on linear Taylor expansions. Three different approaches are investigated for calculating the density variation over the element. The first approach evolves a Taylor expansion of the specific volume field. The second approach follows certain finite element methods and uses the strong mass conservation to calculate the density field at a location inside the element or on the element surface. The thirdmore » approach evolves a Taylor expansion of the density field. The nodal velocity, and the corresponding forces, are explicitly calculated by solving a multidirectional approximate Riemann problem. An effective limiting strategy is presented that ensures monotonicity of the primitive variables. This new Lagrangian DG hydrodynamic method conserves mass, momentum, and total energy. Results from a suite of test problems are presented to demonstrate the robustness and expected second-order accuracy of this new method.« less

Orthogonality of embedded wave functions for different states in frozen-density embedding theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zech, Alexander; Wesolowski, Tomasz A.; Aquilante, Francesco

2015-10-28

Other than lowest-energy stationary embedded wave functions obtained in Frozen-Density Embedding Theory (FDET) [T. A. Wesolowski, Phys. Rev. A 77, 012504 (2008)] can be associated with electronic excited states but they can be mutually non-orthogonal. Although this does not violate any physical principles — embedded wave functions are only auxiliary objects used to obtain stationary densities — working with orthogonal functions has many practical advantages. In the present work, we show numerically that excitation energies obtained using conventional FDET calculations (allowing for non-orthogonality) can be obtained using embedded wave functions which are strictly orthogonal. The used method preserves the mathematicalmore » structure of FDET and self-consistency between energy, embedded wave function, and the embedding potential (they are connected through the Euler-Lagrange equations). The orthogonality is built-in through the linearization in the embedded density of the relevant components of the total energy functional. Moreover, we show formally that the differences between the expectation values of the embedded Hamiltonian are equal to the excitation energies, which is the exact result within linearized FDET. Linearized FDET is shown to be a robust approximation for a large class of reference densities.« less

The experimental charge-density approach in the evaluation of intermolecular interactions. Application of a new module of the XD programming package to several solids including a pentapeptide.

PubMed

Abramov, Y A; Volkov, A; Wu, G; Coppens, P

2000-11-01

A new module interfaced to the XD programming package has been used in the evaluation of intermolecular interactions and lattice energies of the crystals of p-nitroaniline, L-asparagine monohydrate and the pentapeptide Boc-Gln-D-Iva-Hyp-Ala-Phol (Boc = butoxycarbonyl, Iva = isovaline = ethylalanine, Phol = phenylalaninol). The electrostatic interactions are evaluated with the atom-centered distributed multipoles from KRMM (kappa'-restricted multipole model) refinements, using the Buckingham expression for non-overlapping charge densities. Results for p-nitroaniline are compared with Hartree-Fock (HF), density functional (DFT) and Moller-Plesset (MP2) supermolecular calculations and with HF and DFT periodic calculations. The HF and DFT methods fail to predict the stability of the p-nitroaniline crystal but the results of the experimental charge-density approach (ECDA) are in good agreement with both MP2 interaction energies and the experimental lattice energy. ECDA results for L-asparagine monohydrate compare well with those from DFT supermolecular and periodic HF calculations. The disorder of the terminal group in the pentapeptide, which persists at the experimental temperature of 20 K, corresponds to an energy difference of only 0.35 kJ mol(-1), which is too small to be reproduced with current methods.

Exciplex-exciplex energy transfer and annihilation in solid films of porphyrin-fullerene dyads.

PubMed

Lehtivuori, Heli; Lemmetyinen, Helge; Tkachenko, Nikolai V

2006-12-20

Exciplex-exciplex annihilation was observed for the first time in porphyrin-fullerene molecular films. The films were prepared using Langmuir-Blodgett and drop casting methods. The exciplex-exciplex interactions were studied using femtosecond pump-probe method. The exciplex-exciplex annihilation can be seen as a fast (within few picoseconds) decay of the transient absorption at excitation densities higher than 0.4 mJ/cm2. Analysis of the excitation density dependences indicates that in average four dyads are involved in the exciplex-exciplex interaction, suggesting that an exciplex-exciplex energy transfer may precede the annihilation.

Performance of Frozen Density Embedding for Modeling Hole Transfer Reactions.

PubMed

Ramos, Pablo; Papadakis, Markos; Pavanello, Michele

2015-06-18

We have carried out a thorough benchmark of the frozen density-embedding (FDE) method for calculating hole transfer couplings. We have considered 10 exchange-correlation functionals, 3 nonadditive kinetic energy functionals, and 3 basis sets. Overall, we conclude that with a 7% mean relative unsigned error, the PBE and PW91 functionals coupled with the PW91k nonadditive kinetic energy functional and a TZP basis set constitute the most stable and accurate levels of theory for hole transfer coupling calculations. The FDE-ET method is found to be an excellent tool for computing diabatic couplings for hole transfer reactions.

Extension of the self-consistent-charge density-functional tight-binding method: third-order expansion of the density functional theory total energy and introduction of a modified effective coulomb interaction.

PubMed

Yang, Yang; Yu, Haibo; York, Darrin; Cui, Qiang; Elstner, Marcus

2007-10-25

The standard self-consistent-charge density-functional-tight-binding (SCC-DFTB) method (Phys. Rev. B 1998, 58, 7260) is derived by a second-order expansion of the density functional theory total energy expression, followed by an approximation of the charge density fluctuations by charge monopoles and an effective damped Coulomb interaction between the atomic net charges. The central assumptions behind this effective charge-charge interaction are the inverse relation of atomic size and chemical hardness and the use of a fixed chemical hardness parameter independent of the atomic charge state. While these approximations seem to be unproblematic for many covalently bound systems, they are quantitatively insufficient for hydrogen-bonding interactions and (anionic) molecules with localized net charges. Here, we present an extension of the SCC-DFTB method to incorporate third-order terms in the charge density fluctuations, leading to chemical hardness parameters that are dependent on the atomic charge state and a modification of the Coulomb scaling to improve the electrostatic treatment within the second-order terms. These modifications lead to a significant improvement in the description of hydrogen-bonding interactions and proton affinities of biologically relevant molecules.

Laser modification of graphene oxide layers

NASA Astrophysics Data System (ADS)

Malinský, Petr; Macková, Anna; Cutroneo, Mariapompea; Siegel, Jakub; Bohačová, Marie; Klímova, Kateřina; Švorčík, Václav; Sofer, Zdenĕk

2018-01-01

The effect of linearly polarized laser irradiation with various energy densities was successfully used for reduction of graphene oxide (GO). The ion beam analytical methods (RBS, ERDA) were used to follow the elemental composition which is expected as the consequence of GO reduction. The chemical composition analysis was accompanied by structural study showing changed functionalities in the irradiated GO foils using spectroscopy techniques including XPS, FTIR and Raman spectroscopy. The AFM was employed to identify the surface morphology and electric properties evolution were subsequently studied using standard two point method measurement. The used analytical methods report on reduction of irradiated graphene oxide on the surface and the decrease of surface resistivity as a growing function of the laser beam energy density.

Fast semi-analytical method for precise prediction of ion energy distribution functions and sheath electric field in multi-frequency capacitively coupled plasmas

NASA Astrophysics Data System (ADS)

Chen, Wencong; Zhang, Xi; Diao, Dongfeng

2018-05-01

We propose a fast semi-analytical method to predict ion energy distribution functions and sheath electric field in multi-frequency capacitively coupled plasmas, which are difficult to measure in commercial plasma reactors. In the intermediate frequency regime, the ion density within the sheath is strongly modulated by the low-frequency sheath electric field, making the time-independent ion density assumption employed in conventional models invalid. Our results are in a good agreement with experimental measurements and computer simulations. The application of this method will facilitate the understanding of ion–material interaction mechanisms and development of new-generation plasma etching devices.

Combining the modified Skyrme-like model and the local density approximation to determine the symmetry energy of nuclear matter

NASA Astrophysics Data System (ADS)

Liu, Jian; Ren, Zhongzhou; Xu, Chang

2018-07-01

Combining the modified Skyrme-like model and the local density approximation model, the slope parameter L of symmetry energy is extracted from the properties of finite nuclei with an improved iterative method. The calculations of the iterative method are performed within the framework of the spherical symmetry. By choosing 200 neutron rich nuclei on 25 isotopic chains as candidates, the slope parameter is constrained to be 50 MeV < L < 62 MeV. The validity of this method is examined by the properties of finite nuclei. Results show that reasonable descriptions on the properties of finite nuclei and nuclear matter can be obtained together.

The density matrix method in photonic bandgap and antiferromagnetic materials

NASA Astrophysics Data System (ADS)

Barrie, Scott B.

In this thesis, a theory for dispersive polaritonic bandgap (DPBG) and photonic bandgap (PBG) materials is developed. An ensemble of multi-level nanoparticles, such as non-interacting two-, three- and four-level atoms doped in DPBG and PBG materials is considered. The optical properties of these materials such as spontaneous emission, line broadening, fluorescence and narrowing of the natural linewidth have been studied using the density matrix method. Numerical simulations for these properties have been performed for the DPBG materials SiC and InAs, and for a PBG material with a 20 percent gap-to-midgap ratio. When a three-level nanoparticle is doped into a DPBG material, it is predicted that one or two bound states exist when one or both resonance energies, respectively, lie in the bandgap. It is shown when a resonance energy lies below the bandgap, its spectral density peak weakens and broadens as the resonance energy increases to the lower band edge. For the first time it is predicted that when a nanoparticle's resonance energy lies above the bandgap, its spectral density peak weakens and broadens as the resonance energy increases. A relation is also found between spectral structure and gap-to-midgap ratios. The dressed states of a two-level atom doped into a DPBG material under the influence of an intense monochromatic laser field are examined. The splitting of the dressed state energies is calculated, and it is predicted that the splitting depends on the polariton density of states and the Rabi frequency of laser field. The fluoresence is also examined, and for the first time two distinct control processes are found for the transition from one peak to three peaks. It was previously known that the Rabi frequency controlled the Stark effect, but this thesis predicts that the local of the peak with respect to the optical bandgap can cause a transition from one to three peaks even with a weak Rabi frequency. The transient linewidth narrowing of PBG crystal emission peaks doped with four-level atoms is studied. It is found that linewidth narrowing is only dependent upon time delay when the resonance energy is not near a band edge. This is a new discovery. The density matrix method is employed to find the critical magnetic field at which spin flopping occurs in antiferromagnetic high temperature superconductors. It is found that this magnetic field depends upon the temperature, the anisotropy parameter and the doping concentration. Results are calculated for 1-2-3 HTSCs. Keywords. Quantum Optics, Density Matrix, Photonic Bandgap Materials, Dispersive Polaritonic Bandgap Materials, Antiferromagnets.

DFT-based method for more accurate adsorption energies: An adaptive sum of energies from RPBE and vdW density functionals

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hensley, Alyssa J. R.; Ghale, Kushal; Rieg, Carolin

In recent years, the popularity of density functional theory with periodic boundary conditions (DFT) has surged for the design and optimization of functional materials. However, no single DFT exchange–correlation functional currently available gives accurate adsorption energies on transition metals both when bonding to the surface is dominated by strong covalent or ionic bonding and when it has strong contributions from van der Waals interactions (i.e., dispersion forces). Here we present a new, simple method for accurately predicting adsorption energies on transition-metal surfaces based on DFT calculations, using an adaptively weighted sum of energies from RPBE and optB86b-vdW (or optB88-vdW) densitymore » functionals. This method has been benchmarked against a set of 39 reliable experimental energies for adsorption reactions. Our results show that this method has a mean absolute error and root mean squared error relative to experiments of 13.4 and 19.3 kJ/mol, respectively, compared to 20.4 and 26.4 kJ/mol for the BEEF-vdW functional. For systems with large van der Waals contributions, this method decreases these errors to 11.6 and 17.5 kJ/mol. Furthermore, this method provides predictions of adsorption energies both for processes dominated by strong covalent or ionic bonding and for those dominated by dispersion forces that are more accurate than those of any current standard DFT functional alone.« less

DFT-based method for more accurate adsorption energies: An adaptive sum of energies from RPBE and vdW density functionals

DOE PAGES

Hensley, Alyssa J. R.; Ghale, Kushal; Rieg, Carolin; ...

2017-01-26

In recent years, the popularity of density functional theory with periodic boundary conditions (DFT) has surged for the design and optimization of functional materials. However, no single DFT exchange–correlation functional currently available gives accurate adsorption energies on transition metals both when bonding to the surface is dominated by strong covalent or ionic bonding and when it has strong contributions from van der Waals interactions (i.e., dispersion forces). Here we present a new, simple method for accurately predicting adsorption energies on transition-metal surfaces based on DFT calculations, using an adaptively weighted sum of energies from RPBE and optB86b-vdW (or optB88-vdW) densitymore » functionals. This method has been benchmarked against a set of 39 reliable experimental energies for adsorption reactions. Our results show that this method has a mean absolute error and root mean squared error relative to experiments of 13.4 and 19.3 kJ/mol, respectively, compared to 20.4 and 26.4 kJ/mol for the BEEF-vdW functional. For systems with large van der Waals contributions, this method decreases these errors to 11.6 and 17.5 kJ/mol. Furthermore, this method provides predictions of adsorption energies both for processes dominated by strong covalent or ionic bonding and for those dominated by dispersion forces that are more accurate than those of any current standard DFT functional alone.« less

Device and method for electron beam heating of a high density plasma

DOEpatents

Thode, Lester E.

1981-01-01

A device and method for relativistic electron beam heating of a high density plasma in a small localized region. A relativistic electron beam generator produces a high voltage electron beam which propagates along a vacuum drift tube and is modulated to initiate electron bunching within the beam. The beam is then directed through a low density gas chamber which provides isolation between the vacuum modulator and the relativistic electron beam target. The relativistic beam is then applied to a high density target plasma which typically comprises DT, DD, hydrogen boron or similar thermonuclear gas at a density of 10.sup.17 to 10.sup.20 electrons per cubic centimeter. The target plasma is ionized prior to application of the electron beam by means of a laser or other preionization source. Utilizing a relativistic electron beam with an individual particle energy exceeding 3 MeV, classical scattering by relativistic electrons passing through isolation foils is negligible. As a result, relativistic streaming instabilities are initiated within the high density target plasma causing the relativistic electron beam to efficiently deposit its energy into a small localized region within the high density plasma target.

Investigation of light induced effect on density of states of Pb doped CdSe thin films

NASA Astrophysics Data System (ADS)

Kaur, Jagdish; Singh, Baljinder; Tripathi, S. K.

2016-05-01

Thin films of Pb doped CdSe are deposited on the glass substrates by thermal evaporation technique using inert gas condensation method. The prepared thin films are light soaked under vacuum of 2×10-3 mbar for two hour. The absorption coefficient in the sub-band gap region has been studied using Constant Photocurrent Method (CPM). The absorption coefficient in the sub-band gap region follows an exponential Urbach tail. The value of Urbach energy and number density of defect states have been calculated from the absorption coefficient in the sub-band gap region and found to increase after light soaking treatment. The energy distribution of the occupied density of states below Fermi level has been evaluated using derivative procedure of the absorption coefficient.

Method and means for a spatial and temporal probe for laser-generated plumes based on density gradients

DOEpatents

Yeung, Edward S.; Chen, Guoying

1990-05-01

A method and means for a spatial and temporal probe for laser generated plumes based on density gradients includes generation of a plume of vaporized material from a surface by an energy source. The probe laser beam is positioned so that the plume passes through the probe laser beam. Movement of the probe laser beam caused by refraction from the density gradient of the plume is monitored. Spatial and temporal information, correlated to one another, is then derived.

Density functional theory and an experimentally-designed energy functional of electron density.

PubMed

Miranda, David A; Bueno, Paulo R

2016-09-21

We herein demonstrate that capacitance spectroscopy (CS) experimentally allows access to the energy associated with the quantum mechanical ground state of many-electron systems. Priorly, electrochemical capacitance, C [small mu, Greek, macron] [ρ], was previously understood from conceptual and computational density functional theory (DFT) calculations. Thus, we herein propose a quantum mechanical experiment-based variational method for electron charging processes based on an experimentally-designed functional of the ground state electron density. In this methodology, the electron state density, ρ, and an energy functional of the electron density, E [small mu, Greek, macron] [ρ], can be obtained from CS data. CS allows the derivative of the electrochemical potential with respect to the electron density, (δ[small mu, Greek, macron][ρ]/δρ), to be obtained as a unique functional of the energetically minimised system, i.e., β/C [small mu, Greek, macron] [ρ], where β is a constant (associated with the size of the system) and C [small mu, Greek, macron] [ρ] is an experimentally observable quantity. Thus the ground state energy (at a given fixed external potential) can be obtained simply as E [small mu, Greek, macron] [ρ], from the experimental measurement of C [small mu, Greek, macron] [ρ]. An experimental data-set was interpreted to demonstrate the potential of this quantum mechanical experiment-based variational principle.

Efficient iterative method for solving the Dirac-Kohn-Sham density functional theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Lin, Lin; Shao, Sihong; E, Weinan

2012-11-06

We present for the first time an efficient iterative method to directly solve the four-component Dirac-Kohn-Sham (DKS) density functional theory. Due to the existence of the negative energy continuum in the DKS operator, the existing iterative techniques for solving the Kohn-Sham systems cannot be efficiently applied to solve the DKS systems. The key component of our method is a novel filtering step (F) which acts as a preconditioner in the framework of the locally optimal block preconditioned conjugate gradient (LOBPCG) method. The resulting method, dubbed the LOBPCG-F method, is able to compute the desired eigenvalues and eigenvectors in the positive energy band without computing any state in the negative energy band. The LOBPCG-F method introduces mild extra cost compared to the standard LOBPCG method and can be easily implemented. We demonstrate our method in the pseudopotential framework with a planewave basis set which naturally satisfies the kinetic balance prescription. Numerical results for Ptmore » $$_{2}$$, Au$$_{2}$$, TlF, and Bi$$_{2}$$Se$$_{3}$$ indicate that the LOBPCG-F method is a robust and efficient method for investigating the relativistic effect in systems containing heavy elements.« less

Probabilistic Density Function Method for Stochastic ODEs of Power Systems with Uncertain Power Input

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Peng; Barajas-Solano, David A.; Constantinescu, Emil

Wind and solar power generators are commonly described by a system of stochastic ordinary differential equations (SODEs) where random input parameters represent uncertainty in wind and solar energy. The existing methods for SODEs are mostly limited to delta-correlated random parameters (white noise). Here we use the Probability Density Function (PDF) method for deriving a closed-form deterministic partial differential equation (PDE) for the joint probability density function of the SODEs describing a power generator with time-correlated power input. The resulting PDE is solved numerically. A good agreement with Monte Carlo Simulations shows accuracy of the PDF method.

Cosmic ray energy reconstruction from the S(500) observable recorded in the KASCADE-Grande air shower experiment

NASA Astrophysics Data System (ADS)

Apel, W. D.; Arteaga-Velázquez, J. C.; Bekk, K.; Bertaina, M.; Blümer, J.; Bozdog, H.; Brancus, I. M.; Cantoni, E.; Chiavassa, A.; Cossavella, F.; Daumiller, K.; de Souza, V.; Di Pierro, F.; Doll, P.; Engel, R.; Fuhrmann, D.; Gherghel-Lascu, A.; Gils, H. J.; Glasstetter, R.; Grupen, C.; Haungs, A.; Heck, D.; Hörandel, J. R.; Huber, D.; Huege, T.; Kampert, K.-H.; Kang, D.; Klages, H. O.; Link, K.; Łuczak, P.; Mathes, H. J.; Mayer, H. J.; Milke, J.; Mitrica, B.; Morello, C.; Oehlschläger, J.; Ostapchenko, S.; Palmieri, N.; Petcu, M.; Pierog, T.; Rebel, H.; Roth, M.; Schieler, H.; Schoo, S.; Schröder, F. G.; Sima, O.; Toma, G.; Trinchero, G. C.; Ulrich, H.; Weindl, A.; Wochele, J.; Zabierowski, J.

2016-04-01

The energy reconstruction at KASCADE-Grande is based on a combination of the shower size and the total muon number, which are both estimated for each individual air shower event. We present investigations where we employed a second method to reconstruct the primary energy using S(500), which are the charged particle densities inferred with the KASCADE-Grande detector at a distance of 500 m from the shower axis. We considered the attenuation of inclined showers by applying the "Constant Intensity Cut" method and we employed a simulation-derived calibration to convert the recorded S(500) into primary energy. We observed a systematic shift in the S(500)-derived energy compared with previously reported results obtained using the standard reconstruction technique. However, a comparison of the two methods based on simulated and measured data showed that this shift only appeared in the measured data. Our investigations showed that this shift was caused mainly by the inadequate description of the shape of the lateral density distribution in the simulations.

Grand canonical electronic density-functional theory: Algorithms and applications to electrochemistry

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sundararaman, Ravishankar; Goddard, III, William A.; Arias, Tomas A.

First-principles calculations combining density-functional theory and continuum solvation models enable realistic theoretical modeling and design of electrochemical systems. When a reaction proceeds in such systems, the number of electrons in the portion of the system treated quantum mechanically changes continuously, with a balancing charge appearing in the continuum electrolyte. A grand-canonical ensemble of electrons at a chemical potential set by the electrode potential is therefore the ideal description of such systems that directly mimics the experimental condition. We present two distinct algorithms: a self-consistent field method and a direct variational free energy minimization method using auxiliary Hamiltonians (GC-AuxH), to solvemore » the Kohn-Sham equations of electronic density-functional theory directly in the grand canonical ensemble at fixed potential. Both methods substantially improve performance compared to a sequence of conventional fixed-number calculations targeting the desired potential, with the GC-AuxH method additionally exhibiting reliable and smooth exponential convergence of the grand free energy. Lastly, we apply grand-canonical density-functional theory to the under-potential deposition of copper on platinum from chloride-containing electrolytes and show that chloride desorption, not partial copper monolayer formation, is responsible for the second voltammetric peak.« less

Grand canonical electronic density-functional theory: Algorithms and applications to electrochemistry.

PubMed

Sundararaman, Ravishankar; Goddard, William A; Arias, Tomas A

2017-03-21

First-principles calculations combining density-functional theory and continuum solvation models enable realistic theoretical modeling and design of electrochemical systems. When a reaction proceeds in such systems, the number of electrons in the portion of the system treated quantum mechanically changes continuously, with a balancing charge appearing in the continuum electrolyte. A grand-canonical ensemble of electrons at a chemical potential set by the electrode potential is therefore the ideal description of such systems that directly mimics the experimental condition. We present two distinct algorithms: a self-consistent field method and a direct variational free energy minimization method using auxiliary Hamiltonians (GC-AuxH), to solve the Kohn-Sham equations of electronic density-functional theory directly in the grand canonical ensemble at fixed potential. Both methods substantially improve performance compared to a sequence of conventional fixed-number calculations targeting the desired potential, with the GC-AuxH method additionally exhibiting reliable and smooth exponential convergence of the grand free energy. Finally, we apply grand-canonical density-functional theory to the under-potential deposition of copper on platinum from chloride-containing electrolytes and show that chloride desorption, not partial copper monolayer formation, is responsible for the second voltammetric peak.

Grand canonical electronic density-functional theory: Algorithms and applications to electrochemistry

DOE PAGES

Sundararaman, Ravishankar; Goddard, III, William A.; Arias, Tomas A.

2017-03-16

First-principles calculations combining density-functional theory and continuum solvation models enable realistic theoretical modeling and design of electrochemical systems. When a reaction proceeds in such systems, the number of electrons in the portion of the system treated quantum mechanically changes continuously, with a balancing charge appearing in the continuum electrolyte. A grand-canonical ensemble of electrons at a chemical potential set by the electrode potential is therefore the ideal description of such systems that directly mimics the experimental condition. We present two distinct algorithms: a self-consistent field method and a direct variational free energy minimization method using auxiliary Hamiltonians (GC-AuxH), to solvemore » the Kohn-Sham equations of electronic density-functional theory directly in the grand canonical ensemble at fixed potential. Both methods substantially improve performance compared to a sequence of conventional fixed-number calculations targeting the desired potential, with the GC-AuxH method additionally exhibiting reliable and smooth exponential convergence of the grand free energy. Lastly, we apply grand-canonical density-functional theory to the under-potential deposition of copper on platinum from chloride-containing electrolytes and show that chloride desorption, not partial copper monolayer formation, is responsible for the second voltammetric peak.« less

Device and method for relativistic electron beam heating of a high-density plasma to drive fast liners

DOEpatents

Thode, Lester E.

1981-01-01

A device and method for relativistic electron beam heating of a high-density plasma in a small localized region. A relativistic electron beam generator or accelerator produces a high-voltage electron beam which propagates along a vacuum drift tube and is modulated to initiate electron bunching within the beam. The beam is then directed through a low-density gas chamber which provides isolation between the vacuum modulator and the relativistic electron beam target. The relativistic beam is then applied to a high-density target plasma which typically comprises DT, DD, hydrogen boron or similar thermonuclear gas at a density of 10.sup.17 to 10.sup.20 electrons per cubic centimeter. The target gas is ionized prior to application of the electron beam by means of a laser or other preionization source to form a plasma. Utilizing a relativistic electron beam with an individual particle energy exceeding 3 MeV, classical scattering by relativistic electrons passing through isolation foils is negligible. As a result, relativistic streaming instabilities are initiated within the high-density target plasma causing the relativistic electron beam to efficiently deposit its energy and momentum into a small localized region of the high-density plasma target. Fast liners disposed in the high-density target plasma are explosively or ablatively driven to implosion by a heated annular plasma surrounding the fast liner which is generated by an annular relativistic electron beam. An azimuthal magnetic field produced by axial current flow in the annular plasma, causes the energy in the heated annular plasma to converge on the fast liner.

Fist Principles Approach to the Magneto Caloric Effect: Application to Ni2MnGa

NASA Astrophysics Data System (ADS)

Odbadrakh, Khorgolkhuu; Nicholson, Don; Rusanu, Aurelian; Eisenbach, Markus; Brown, Gregory; Evans, Boyd, III

2011-03-01

The magneto-caloric effect (MCE) has potential application in heating and cooling technologies. In this work, we present calculated magnetic structure of a candidate MCE material, Ni 2 MnGa. The magnetic configurations of a 144 atom supercell is first explored using first-principle, the results are then used to fit exchange parameters of a Heisenberg Hamiltonian. The Wang-Landau method is used to calculate the magnetic density of states of the Heisenberg Hamiltonian. Based on this classical estimate, the magnetic density of states is calculated using the Wang Landau method with energies obtained from the first principles method. The Currie temperature and other thermodynamic properties are calculated using the density of states. The relationships between the density of magnetic states and the field induced adiabatic temperature change and isothermal entropy change are discussed. This work was sponsored by the Laboratory Directed Research and Development Program (ORNL), by the Mathematical, Information, and Computational Sciences Division; Office of Advanced Scientific Computing Research (US DOE), and by the Materials Sciences and Engineering Division; Office of Basic Energy Sciences (US DOE).

Unitary Fermi gas in a harmonic trap

NASA Astrophysics Data System (ADS)

Chang, S. Y.; Bertsch, G. F.

2007-08-01

We present an ab initio calculation of small numbers of trapped, strongly interacting fermions using the Green’s function Monte Carlo method. The ground-state energy, density profile, and pairing gap are calculated for particle numbers N=2 22 using the parameter-free “unitary” interaction. Trial wave functions are taken in the form of correlated pairs in a harmonic oscillator basis. We find that the lowest energies are obtained with a minimum explicit pair correlation beyond that needed to exploit the degeneracy of oscillator states. We find that the energies can be well fitted by the expression aTFETF+Δmod(N,2) where ETF is the Thomas-Fermi energy of a noninteracting gas in the trap and Δ is the pairing gap. There is no evidence of a shell correction energy in the systematics, but the density distributions show pronounced shell effects. We find the value Δ=0.7±0.2ω for the pairing gap. This is smaller than the value found for the uniform gas at a density corresponding to the central density of the trapped gas.

Universal functions of nuclear proximity potential for Skyrme nucleus-nucleus interaction in a semiclassical approach

NASA Astrophysics Data System (ADS)

Gupta, Raj K.; Singh, Dalip; Kumar, Raj; Greiner, Walter

2009-07-01

The universal function of the nuclear proximity potential is obtained for the Skyrme nucleus-nucleus interaction in the semiclassical extended Thomas-Fermi (ETF) approach. This is obtained as a sum of the spin-orbit-density-independent and spin-orbit-density-dependent parts of the Hamiltonian density, since the two terms behave differently, the spin-orbit-density-independent part mainly attractive and the spin-orbit-density-dependent part mainly repulsive. The semiclassical expansions of kinetic energy density and spin-orbit density are allowed up to second order, and the two-parameter Fermi density, with its parameters fitted to experiments, is used for the nuclear density. The universal functions or the resulting nuclear proximity potential reproduce the 'exact' Skyrme nucleus-nucleus interaction potential in the semiclassical approach, within less than ~1 MeV of difference, both at the maximum attraction and in the surface region. An application of the resulting interaction potential to fusion excitation functions shows clearly that the parameterized universal functions of nuclear proximity potential substitute completely the 'exact' potential in the Skyrme energy density formalism based on the semiclassical ETF method, including also the modifications of interaction barriers at sub-barrier energies in terms of modifying the constants of the universal functions.

Proton and neutron density distributions at supranormal density in low- and medium-energy heavy-ion collisions

NASA Astrophysics Data System (ADS)

Stone, J. R.; Danielewicz, P.; Iwata, Y.

2017-07-01

Background: The distribution of protons and neutrons in the matter created in heavy-ion collisions is one of the main points of interest for the collision physics, especially at supranormal densities. These distributions are the basis for predictions of the density dependence of the symmetry energy and the density range that can be achieved in a given colliding system. We report results of the first systematic simulation of proton and neutron density distributions in central heavy-ion collisions within the beam energy range of Ebeam≤800 MeV /nucl . The symmetric 40Ca+40Ca , 48Ca+48Ca , 100Sn+100Sn , and 120Sn+120Sn and asymmetric 40Ca+48Ca and 100Sn+120Sn systems were chosen for the simulations. Purpose: We simulate development of proton and neutron densities and asymmetries as a function of initial state, beam energy, and system size in the selected collisions in order to guide further experiments pursuing the density dependence of the symmetry energy. Methods: The Boltzmann-Uhlenbeck-Uehling (pBUU) transport model with four empirical models for the density dependence of the symmetry energy was employed. Results of simulations using pure Vlasov dynamics were added for completeness. In addition, the time-dependent Hartree-Fock (TDHF) model, with the SV-bas Skyrme interaction, was used to model the heavy-ion collisions at Ebeam≤40 MeV /nucl . Maximum proton and neutron densities ρpmax and ρnmax, reached in the course of a collision, were determined from the time evolution of ρp and ρn. Results: The highest total densities predicted at Ebeam=800 MeV /nucl . were of the order of ˜2.5 ρ0 (ρ0=0.16 fm-3 ) for both Sn and Ca systems. They were found to be only weakly dependent on the initial conditions, beam energy, system size, and a model of the symmetry energy. The proton-neutron asymmetry δ =(ρnmax-ρpmax) /(ρnmax+ρpmax) at maximum density does depend, though, on these parameters. The highest value of δ found in all systems and at all investigated beam energies was ˜0.17 . Conclusions: We find that the initial state, beam energy, system size, and a symmetry energy model affect very little the maximum proton and neutron densities, but have a subtle impact on the proton-neutron asymmetry. Most importantly, the variations in the proton-neutron asymmetry at maximum densities are related at most at 50% level to the details in the symmetry energy at supranormal density. The reminder is due to the details in the symmetry energy at subnormal densities and proton and neutron distributions in the initial state. This result brings to the forefront the need for a proper initialization of the nuclei in the simulation, but also brings up the question of microscopy, such as shell effects, that affect initial proton and neutron densities, but cannot be consistently incorporated into semiclassical transport models.

Dispersion correction derived from first principles for density functional theory and Hartree-Fock theory.

PubMed

Guidez, Emilie B; Gordon, Mark S

2015-03-12

The modeling of dispersion interactions in density functional theory (DFT) is commonly performed using an energy correction that involves empirically fitted parameters for all atom pairs of the system investigated. In this study, the first-principles-derived dispersion energy from the effective fragment potential (EFP) method is implemented for the density functional theory (DFT-D(EFP)) and Hartree-Fock (HF-D(EFP)) energies. Overall, DFT-D(EFP) performs similarly to the semiempirical DFT-D corrections for the test cases investigated in this work. HF-D(EFP) tends to underestimate binding energies and overestimate intermolecular equilibrium distances, relative to coupled cluster theory, most likely due to incomplete accounting for electron correlation. Overall, this first-principles dispersion correction yields results that are in good agreement with coupled-cluster calculations at a low computational cost.

Vortex energy landscape from real space imaging analysis of YBa2Cu3O7 with different defect structures

NASA Astrophysics Data System (ADS)

Luccas, R. F.; Granados, X.; Obradors, X.; Puig, T.

2014-10-01

A methodology based on real space vortex image analysis is presented able to estimate semi-quantitatively the relevant energy densities of an arbitrary array of vortices, map the interaction energy distributions and evaluate the pinning energy associated to particular defects. The combined study using nanostructuration tools, a vortex visualization technique and the energy method is seen as an opportunity to estimate vortex pinning potentials strengths. Particularly, spatial distributions of vortex energy densities induced by surface nanoindented scratches are evaluated and compared to those of twin boundaries. This comparative study underlines the remarkable role of surface nanoscratches in pinning vortices and its potentiality in the design of novel devices for pinning and guiding vortex motion.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Isotalo, Aarno

A method referred to as tally nuclides is presented for accurately and efficiently calculating the time-step averages and integrals of any quantities that are weighted sums of atomic densities with constant weights during the step. The method allows all such quantities to be calculated simultaneously as a part of a single depletion solution with existing depletion algorithms. Some examples of the results that can be extracted include step-average atomic densities and macroscopic reaction rates, the total number of fissions during the step, and the amount of energy released during the step. Furthermore, the method should be applicable with several depletionmore » algorithms, and the integrals or averages should be calculated with an accuracy comparable to that reached by the selected algorithm for end-of-step atomic densities. The accuracy of the method is demonstrated in depletion calculations using the Chebyshev rational approximation method. Here, we demonstrate how the ability to calculate energy release in depletion calculations can be used to determine the accuracy of the normalization in a constant-power burnup calculation during the calculation without a need for a reference solution.« less

Calculating Time-Integral Quantities in Depletion Calculations

DOE PAGES

Isotalo, Aarno

2016-06-02

A method referred to as tally nuclides is presented for accurately and efficiently calculating the time-step averages and integrals of any quantities that are weighted sums of atomic densities with constant weights during the step. The method allows all such quantities to be calculated simultaneously as a part of a single depletion solution with existing depletion algorithms. Some examples of the results that can be extracted include step-average atomic densities and macroscopic reaction rates, the total number of fissions during the step, and the amount of energy released during the step. Furthermore, the method should be applicable with several depletionmore » algorithms, and the integrals or averages should be calculated with an accuracy comparable to that reached by the selected algorithm for end-of-step atomic densities. The accuracy of the method is demonstrated in depletion calculations using the Chebyshev rational approximation method. Here, we demonstrate how the ability to calculate energy release in depletion calculations can be used to determine the accuracy of the normalization in a constant-power burnup calculation during the calculation without a need for a reference solution.« less

Why Density Dependent Propulsion?

NASA Technical Reports Server (NTRS)

Robertson, Glen A.

2011-01-01

In 2004 Khoury and Weltman produced a density dependent cosmology theory they call the Chameleon, as at its nature, it is hidden within known physics. The Chameleon theory has implications to dark matter/energy with universe acceleration properties, which implies a new force mechanism with ties to the far and local density environment. In this paper, the Chameleon Density Model is discussed in terms of propulsion toward new propellant-less engineering methods.

Gentlest ascent dynamics for calculating first excited state and exploring energy landscape of Kohn-Sham density functionals.

PubMed

Li, Chen; Lu, Jianfeng; Yang, Weitao

2015-12-14

We develop the gentlest ascent dynamics for Kohn-Sham density functional theory to search for the index-1 saddle points on the energy landscape of the Kohn-Sham density functionals. These stationary solutions correspond to excited states in the ground state functionals. As shown by various examples, the first excited states of many chemical systems are given by these index-1 saddle points. Our novel approach provides an alternative, more robust way to obtain these excited states, compared with the widely used ΔSCF approach. The method can be easily generalized to target higher index saddle points. Our results also reveal the physical interest and relevance of studying the Kohn-Sham energy landscape.

A second-order unconstrained optimization method for canonical-ensemble density-functional methods

NASA Astrophysics Data System (ADS)

Nygaard, Cecilie R.; Olsen, Jeppe

2013-03-01

A second order converging method of ensemble optimization (SOEO) in the framework of Kohn-Sham Density-Functional Theory is presented, where the energy is minimized with respect to an ensemble density matrix. It is general in the sense that the number of fractionally occupied orbitals is not predefined, but rather it is optimized by the algorithm. SOEO is a second order Newton-Raphson method of optimization, where both the form of the orbitals and the occupation numbers are optimized simultaneously. To keep the occupation numbers between zero and two, a set of occupation angles is defined, from which the occupation numbers are expressed as trigonometric functions. The total number of electrons is controlled by a built-in second order restriction of the Newton-Raphson equations, which can be deactivated in the case of a grand-canonical ensemble (where the total number of electrons is allowed to change). To test the optimization method, dissociation curves for diatomic carbon are produced using different functionals for the exchange-correlation energy. These curves show that SOEO favors symmetry broken pure-state solutions when using functionals with exact exchange such as Hartree-Fock and Becke three-parameter Lee-Yang-Parr. This is explained by an unphysical contribution to the exact exchange energy from interactions between fractional occupations. For functionals without exact exchange, such as local density approximation or Becke Lee-Yang-Parr, ensemble solutions are favored at interatomic distances larger than the equilibrium distance. Calculations on the chromium dimer are also discussed. They show that SOEO is able to converge to ensemble solutions for systems that are more complicated than diatomic carbon.

Bactericide effect of methylene blue associated with low-level laser therapy in Escherichia coli bacteria isolated from pressure ulcers.

PubMed

Gomes, Thais Ferreira; Pedrosa, Matheus Masalskiene; de Toledo, Ana Claudia Laforga; Arnoni, Veridiana Wanshi; Dos Santos Monteiro, Mirian; Piai, Davi Cury; Sylvestre, Silvia Helena Zacarias; Ferreira, Bruno

2018-05-09

The present study analyzed the bactericidal effect of methylene blue associated with low-level lasers on Escherichia coli isolated from a pressure ulcer. Microbiological material from a pressure ulcer was isolated using an aseptic swab, and antimicrobial activity was verified using the diffusion disc method. Methylene blue was used at concentrations of 0.001 and 0.005%, and low-level lasers of 670, 830, and 904 nm, with the energy densities of 4, 8, 10, and 14 J/cm 2 , were tested on three plates each and combined with methylene blue of each concentration. In addition, three control plates were used, with each concentration and energy density separated without any interventions. The results were analyzed using the paired sample t test to determine the bactericidal effect of the methylene blue and using the ANOVA test to compare the effects of the energy densities and wavelengths among the low-level laser treatment protocols. The results showed bacterial reduction at wavelengths of 830 and 904 nm and more proliferation in wavelengths of 670 nm. In wavelength of 830 nm, a bacterial reduction was observed in the conditions with 0.001% methylene blue in all energy density utilized, with 0.005% methylene blue in energy density of 10 J/cm 2 , and without methylene blue in energy density at 10 J/cm 2 . And in a wavelength of 904 nm, all condition showed bacterial reduction with or without methylene blue. We concluded that the low-level lasers of 904 and 830 nm have bactericidal effects and at better energy densities (10 and 14 J/cm 2 ).

Pseudocapacitive and hierarchically ordered porous electrode materials supercapacitors

NASA Astrophysics Data System (ADS)

Saruhan, B.; Gönüllü, Y.; Arndt, B.

2013-05-01

Commercially available double layer capacitors store energy in an electrostatic field. This forms in the form of a double layer by charged particles arranged on two electrodes consisting mostly of active carbon. Such double layer capacitors exhibit a low energy density, so that components with large capacity according to large electrode areas are required. Our research focuses on the development of new electrode materials to realize the production of electrical energy storage systems with high energy density and high power density. Metal oxide based electrodes increase the energy density and the capacitance by addition of pseudo capacitance to the static capacitance present by the double layer super-capacitor electrodes. The so-called hybrid asymmetric cell capacitors combine both types of energy storage in a single component. In this work, the production routes followed in our laboratories for synthesis of nano-porous and aligned metal oxide electrodes using the electrochemical and sputter deposition as well as anodization methods will be described. Our characterisation studies concentrate on electrodes having redox metal-oxides (e.g. MnOx and WOx) and hierarchically aligned nano-porous Li-doped TiO2-NTs. The material specific and electrochemical properties achieved with these electrodes will be presented.

Assigning crystallographic electron densities with free energy calculations—The case of the fluoride channel Fluc

PubMed Central

2018-01-01

Approximately 90% of the structures in the Protein Data Bank (PDB) were obtained by X-ray crystallography or electron microscopy. Whereas the overall quality of structure is considered high, thanks to a wide range of tools for structure validation, uncertainties may arise from density maps of small molecules, such as organic ligands, ions or water, which are non-covalently bound to the biomolecules. Even with some experience and chemical intuition, the assignment of such disconnected electron densities is often far from obvious. In this study, we suggest the use of molecular dynamics (MD) simulations and free energy calculations, which are well-established computational methods, to aid in the assignment of ambiguous disconnected electron densities. Specifically, estimates of (i) relative binding affinities, for instance between an ion and water, (ii) absolute binding free energies, i.e., free energies for transferring a solute from bulk solvent to a binding site, and (iii) stability assessments during equilibrium simulations may reveal the most plausible assignments. We illustrate this strategy using the crystal structure of the fluoride specific channel (Fluc), which contains five disconnected electron densities previously interpreted as four fluoride and one sodium ion. The simulations support the assignment of the sodium ion. In contrast, calculations of relative and absolute binding free energies as well as stability assessments during free MD simulations suggest that four of the densities represent water molecules instead of fluoride. The assignment of water is compatible with the loss of these densities in the non-conductive F82I/F85I mutant of Fluc. We critically discuss the role of the ion force fields for the calculations presented here. Overall, these findings indicate that MD simulations and free energy calculations are helpful tools for modeling water and ions into crystallographic density maps. PMID:29771936

Energy level alignment and quantum conductance of functionalized metal-molecule junctions: Density functional theory versus GW calculations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jin, Chengjun; Markussen, Troels; Thygesen, Kristian S., E-mail: thygesen@fysik.dtu.dk

We study the effect of functional groups (CH{sub 3}*4, OCH{sub 3}, CH{sub 3}, Cl, CN, F*4) on the electronic transport properties of 1,4-benzenediamine molecular junctions using the non-equilibrium Green function method. Exchange and correlation effects are included at various levels of theory, namely density functional theory (DFT), energy level-corrected DFT (DFT+Σ), Hartree-Fock and the many-body GW approximation. All methods reproduce the expected trends for the energy of the frontier orbitals according to the electron donating or withdrawing character of the substituent group. However, only the GW method predicts the correct ordering of the conductance amongst the molecules. The absolute GWmore » (DFT) conductance is within a factor of two (three) of the experimental values. Correcting the DFT orbital energies by a simple physically motivated scissors operator, Σ, can bring the DFT conductances close to experiments, but does not improve on the relative ordering. We ascribe this to a too strong pinning of the molecular energy levels to the metal Fermi level by DFT which suppresses the variation in orbital energy with functional group.« less

Statistical properties of Pu 243 , and Pu 242 ( n , γ ) cross section calculation

DOE PAGES

Laplace, T. A.; Zeiser, F.; Guttormsen, M.; ...

2016-01-29

The level density and γ-ray strength function (γSF) of 243Pu have been measured in the quasicontinuum using the Oslo method. Excited states in 243Pu were populated using the 242Pu(d,p) reaction. The level density closely follows the constant-temperature level density formula for excitation energies above the pairing gap. The γSF displays a double-humped resonance at low energy as also seen in previous investigations of actinide isotopes. The structure is interpreted as the scissors resonance and has a centroid of ω SR = 2.42(5) MeV and a total strength of B SR = 10.1(15) μ 2 N, which is in excellent agreementmore » with sum-rule estimates. Lastly, the measured level density and γSF were used to calculate the 242Pu(n,γ) cross section in a neutron energy range for which there were previously no measured data.« less

From The Cover: The X3LYP extended density functional for accurate descriptions of nonbond interactions, spin states, and thermochemical properties.

PubMed

Xu, Xin; Goddard, William A

2004-03-02

We derive the form for an exact exchange energy density for a density decaying with Gaussian-like behavior at long range. Based on this, we develop the X3LYP (extended hybrid functional combined with Lee-Yang-Parr correlation functional) extended functional for density functional theory to significantly improve the accuracy for hydrogen-bonded and van der Waals complexes while also improving the accuracy in heats of formation, ionization potentials, electron affinities, and total atomic energies [over the most popular and accurate method, B3LYP (Becke three-parameter hybrid functional combined with Lee-Yang-Parr correlation functional)]. X3LYP also leads to a good description of dipole moments, polarizabilities, and accurate excitation energies from s to d orbitals for transition metal atoms and ions. We suggest that X3LYP will be useful for predicting ligand binding in proteins and DNA.

From The Cover: The X3LYP extended density functional for accurate descriptions of nonbond interactions, spin states, and thermochemical properties

NASA Astrophysics Data System (ADS)

Xu, Xin; Goddard, William A., III

2004-03-01

We derive the form for an exact exchange energy density for a density decaying with Gaussian-like behavior at long range. Based on this, we develop the X3LYP (extended hybrid functional combined with Lee-Yang-Parr correlation functional) extended functional for density functional theory to significantly improve the accuracy for hydrogen-bonded and van der Waals complexes while also improving the accuracy in heats of formation, ionization potentials, electron affinities, and total atomic energies [over the most popular and accurate method, B3LYP (Becke three-parameter hybrid functional combined with Lee-Yang-Parr correlation functional)]. X3LYP also leads to a good description of dipole moments, polarizabilities, and accurate excitation energies from s to d orbitals for transition metal atoms and ions. We suggest that X3LYP will be useful for predicting ligand binding in proteins and DNA.

The X3LYP extended density functional for accurate descriptions of nonbond interactions, spin states, and thermochemical properties

PubMed Central

Xu, Xin; Goddard, William A.

2004-01-01

We derive the form for an exact exchange energy density for a density decaying with Gaussian-like behavior at long range. Based on this, we develop the X3LYP (extended hybrid functional combined with Lee–Yang–Parr correlation functional) extended functional for density functional theory to significantly improve the accuracy for hydrogen-bonded and van der Waals complexes while also improving the accuracy in heats of formation, ionization potentials, electron affinities, and total atomic energies [over the most popular and accurate method, B3LYP (Becke three-parameter hybrid functional combined with Lee–Yang–Parr correlation functional)]. X3LYP also leads to a good description of dipole moments, polarizabilities, and accurate excitation energies from s to d orbitals for transition metal atoms and ions. We suggest that X3LYP will be useful for predicting ligand binding in proteins and DNA. PMID:14981235

Development of indirect EFBEM for radiating noise analysis including underwater problems

NASA Astrophysics Data System (ADS)

Kwon, Hyun-Wung; Hong, Suk-Yoon; Song, Jee-Hun

2013-09-01

For the analysis of radiating noise problems in medium-to-high frequency ranges, the Energy Flow Boundary Element Method (EFBEM) was developed. EFBEM is the analysis technique that applies the Boundary Element Method (BEM) to Energy Flow Analysis (EFA). The fundamental solutions representing spherical wave property for radiating noise problems in open field and considering the free surface effect in underwater are developed. Also the directivity factor is developed to express wave's directivity patterns in medium-to-high frequency ranges. Indirect EFBEM by using fundamental solutions and fictitious source was applied to open field and underwater noise problems successfully. Through numerical applications, the acoustic energy density distributions due to vibration of a simple plate model and a sphere model were compared with those of commercial code, and the comparison showed good agreement in the level and pattern of the energy density distributions.

Quantitative contrast-enhanced spectral mammography based on photon-counting detectors: A feasibility study.

PubMed

Ding, Huanjun; Molloi, Sabee

2017-08-01

To investigate the feasibility of accurate quantification of iodine mass thickness in contrast-enhanced spectral mammography. A computer simulation model was developed to evaluate the performance of a photon-counting spectral mammography system in the application of contrast-enhanced spectral mammography. A figure-of-merit (FOM), which was defined as the decomposed iodine signal-to-noise ratio (SNR) with respect to the square root of the mean glandular dose (MGD), was chosen to optimize the imaging parameters, in terms of beam energy, splitting energy, and prefiltrations for breasts of various thicknesses and densities. Experimental phantom studies were also performed using a beam energy of 40 kVp and a splitting energy of 34 keV with 3 mm Al prefiltration. A two-step calibration method was investigated to quantify the iodine mass thickness, and was validated using phantoms composed of a mixture of glandular and adipose materials, for various breast thicknesses and densities. Finally, the traditional dual-energy log-weighted subtraction method was also studied as a comparison. The measured iodine signal from both methods was compared to the known value to characterize the quantification accuracy and precision. The optimal imaging parameters, which lead to the highest FOM, were found at a beam energy between 42 and 46 kVp with a splitting energy at 34 keV. The optimal tube voltage decreased as the breast thickness or the Al prefiltration increased. The proposed quantification method was able to measure iodine mass thickness on phantoms of various thicknesses and densities with high accuracy. The root-mean-square (RMS) error for cm-scale lesion phantoms was estimated to be 0.20 mg/cm 2 . The precision of the technique, characterized by the standard deviation of the measurements, was estimated to be 0.18 mg/cm 2 . The traditional weighted subtraction method also predicted a linear correlation between the measured signal and the known iodine mass thickness. However, the correlation slope and offset values were strongly dependent on the total breast thickness and density. The results of this study suggest that iodine mass thickness for cm-scale lesions can be accurately quantified with contrast-enhanced spectral mammography. The quantitative information can potentially improve the differential power for malignancy. © 2017 American Association of Physicists in Medicine.

Cholesky-decomposed density MP2 with density fitting: Accurate MP2 and double-hybrid DFT energies for large systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maurer, Simon A.; Clin, Lucien; Ochsenfeld, Christian, E-mail: christian.ochsenfeld@uni-muenchen.de

2014-06-14

Our recently developed QQR-type integral screening is introduced in our Cholesky-decomposed pseudo-densities Møller-Plesset perturbation theory of second order (CDD-MP2) method. We use the resolution-of-the-identity (RI) approximation in combination with efficient integral transformations employing sparse matrix multiplications. The RI-CDD-MP2 method shows an asymptotic cubic scaling behavior with system size and a small prefactor that results in an early crossover to conventional methods for both small and large basis sets. We also explore the use of local fitting approximations which allow to further reduce the scaling behavior for very large systems. The reliability of our method is demonstrated on test sets formore » interaction and reaction energies of medium sized systems and on a diverse selection from our own benchmark set for total energies of larger systems. Timings on DNA systems show that fast calculations for systems with more than 500 atoms are feasible using a single processor core. Parallelization extends the range of accessible system sizes on one computing node with multiple cores to more than 1000 atoms in a double-zeta basis and more than 500 atoms in a triple-zeta basis.« less

Computational Design of Non-natural Sugar Alcohols to Increase Thermal Storage Density: Beyond Existing Organic Phase Change Materials.

PubMed

Inagaki, Taichi; Ishida, Toyokazu

2016-09-14

Thermal storage, a technology that enables us to control thermal energy, makes it possible to reuse a huge amount of waste heat, and materials with the ability to treat larger thermal energy are in high demand for energy-saving societies. Sugar alcohols are now one promising candidate for phase change materials (PCMs) because of their large thermal storage density. In this study, we computationally design experimentally unknown non-natural sugar alcohols and predict their thermal storage density as a basic step toward the development of new high performance PCMs. The non-natural sugar alcohol molecules are constructed in silico in accordance with the previously suggested molecular design guidelines: linear elongation of a carbon backbone, separated distribution of OH groups, and even numbers of carbon atoms. Their crystal structures are then predicted using the random search method and first-principles calculations. Our molecular simulation results clearly demonstrate that the non-natural sugar alcohols have potential ability to have thermal storage density up to ∼450-500 kJ/kg, which is significantly larger than the maximum thermal storage density of the present known organic PCMs (∼350 kJ/kg). This computational study suggests that, even in the case of H-bonded molecular crystals where the electrostatic energy contributes mainly to thermal storage density, the molecular distortion and van der Waals energies are also important factors to increase thermal storage density. In addition, the comparison between the three eight-carbon non-natural sugar alcohol isomers indicates that the selection of preferable isomers is also essential for large thermal storage density.

Level Density in the Complex Scaling Method

NASA Astrophysics Data System (ADS)

Suzuki, R.; Myo, T.; Katō, K.

2005-06-01

It is shown that the continuum level density (CLD) at unbound energies can be calculated with the complex scaling method (CSM), in which the energy spectra of bound states, resonances and continuum states are obtained in terms of L(2) basis functions. In this method, the extended completeness relation is applied to the calculation of the Green functions, and the continuum-state part is approximately expressed in terms of discretized complex scaled continuum solutions. The obtained result is compared with the CLD calculated exactly from the scattering phase shift. The discretization in the CSM is shown to give a very good description of continuum states. We discuss how the scattering phase shifts can inversely be calculated from the discretized CLD using a basis function technique in the CSM.

Site-occupation embedding theory using Bethe ansatz local density approximations

NASA Astrophysics Data System (ADS)

Senjean, Bruno; Nakatani, Naoki; Tsuchiizu, Masahisa; Fromager, Emmanuel

2018-06-01

Site-occupation embedding theory (SOET) is an alternative formulation of density functional theory (DFT) for model Hamiltonians where the fully interacting Hubbard problem is mapped, in principle exactly, onto an impurity-interacting (rather than a noninteracting) one. It provides a rigorous framework for combining wave-function (or Green function)-based methods with DFT. In this work, exact expressions for the per-site energy and double occupation of the uniform Hubbard model are derived in the context of SOET. As readily seen from these derivations, the so-called bath contribution to the per-site correlation energy is, in addition to the latter, the key density functional quantity to model in SOET. Various approximations based on Bethe ansatz and perturbative solutions to the Hubbard and single-impurity Anderson models are constructed and tested on a one-dimensional ring. The self-consistent calculation of the embedded impurity wave function has been performed with the density-matrix renormalization group method. It has been shown that promising results are obtained in specific regimes of correlation and density. Possible further developments have been proposed in order to provide reliable embedding functionals and potentials.

Analytic second derivative of the energy for density functional theory based on the three-body fragment molecular orbital method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Nakata, Hiroya, E-mail: nakata.h.ab@m.titech.ac.jp; RIKEN, Research Cluster for Innovation, Nakamura Lab, 2-1 Hirosawa, Wako, Saitama 351-0198; Japan Society for the Promotion of Science, Kojimachi Business Center Building, 5-3-1 Kojimachi, Chiyoda-ku, Tokyo 102-0083

2015-03-28

Analytic second derivatives of the energy with respect to nuclear coordinates have been developed for spin restricted density functional theory (DFT) based on the fragment molecular orbital method (FMO). The derivations were carried out for the three-body expansion (FMO3), and the two-body expressions can be obtained by neglecting the three-body corrections. Also, the restricted Hartree-Fock (RHF) Hessian for FMO3 can be obtained by neglecting the density-functional related terms. In both the FMO-RHF and FMO-DFT Hessians, certain terms with small magnitudes are neglected for computational efficiency. The accuracy of the FMO-DFT Hessian in terms of the Gibbs free energy is evaluatedmore » for a set of polypeptides and water clusters and found to be within 1 kcal/mol of the corresponding full (non-fragmented) ab initio calculation. The FMO-DFT method is also applied to transition states in S{sub N}2 reactions and for the computation of the IR and Raman spectra of a small Trp-cage protein (PDB: 1L2Y). Some computational timing analysis is also presented.« less

Combining two-body density functionals with multiconfigurational wavefunctions: diatomic molecules

NASA Astrophysics Data System (ADS)

McDouall, Joseph J. W.

The MCSCF method provides a correct zero-order wavefunction for all regions of molecular potential energy surfaces. To obtain quantitative accuracy a proper treatment of the dynamic correlation problem must be implemented. Traditionally this has been achieved through multireference variants of perturbation theory, configuration interaction and coupled cluster theory. The computational cost of such techniques makes them prohibitive for all but the smallest molecular problems. Reported here is an investigation into the efficacy of two-body density functionals in providing the dynamic correlation energy for MCSCF reference states. Tests were made on the two-body density functionals of Colle and Salvetti (CS), Moscardó and San-Fabián (MSF), and Moscardó and Pérez-Jiménez (MPJ5) in predicting the equilibrium bond lengths, harmonic frequencies and dissociation energies of fifteen diatomic molecules (3B2, 3BN, 2BS, 1C2, 2CN, 1CO, 1F2, 1FCl, 1N2, 3NCl, 3O2, 1PN, 3Si2, 3SiO, 3SO) using full valence-shell CASSCF reference wavefunctions. Also studied were modifications of these functionals recently suggested by Miehlich, Stoll and Savin (MSS) and Gräfenstein and Cremer (GC). The results obtained show accuracy comparable with and typically superior to the popular Kohn-Sham BLYP and B3LYP methods. However, the latter methods are not applicable in all regions of a potential energy surface, and even predict incorrect ground states for some systems. The use of two-body density functionals with MCSCF reference states does not share this shortcoming.

Development of Composite Materials with High Passive Damping Properties

DTIC Science & Technology

2006-05-15

frequency response function analysis. Sound transmission through sandwich panels was studied using the statistical energy analysis (SEA). Modal density...2.2.3 Finite element models 14 2.2.4 Statistical energy analysis method 15 CHAPTER 3 ANALYSIS OF DAMPING IN SANDWICH MATERIALS. 24 3.1 Equation of...sheets and the core. 2.2.4 Statistical energy analysis method Finite element models are generally only efficient for problems at low and middle frequencies

First-row diatomics: Calculation of the geometry and energetics using self-consistent gradient-functional approximations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kutzler, F.W.; Painter, G.S.

1992-02-15

A fully self-consistent series of nonlocal (gradient) density-functional calculations has been carried out using the augmented-Gaussian-orbital method to determine the magnitude of gradient corrections to the potential-energy curves of the first-row diatomics, Li{sub 2} through F{sub 2}. Both the Langreth-Mehl-Hu and the Perdew-Wang gradient-density functionals were used in calculations of the binding energy, bond length, and vibrational frequency for each dimer. Comparison with results obtained in the local-spin-density approximation (LSDA) using the Vosko-Wilk-Nusair functional, and with experiment, reveals that bond lengths and vibrational frequencies are rather insensitive to details of the gradient functionals, including self-consistency effects, but the gradient correctionsmore » reduce the overbinding commonly observed in the LSDA calculations of first-row diatomics (with the exception of Li{sub 2}, the gradient-functional binding-energy error is only 50--12 % of the LSDA error). The improved binding energies result from a large differential energy lowering, which occurs in open-shell atoms relative to the diatomics. The stabilization of the atom arises from the use of nonspherical charge and spin densities in the gradient-functional calculations. This stabilization is negligibly small in LSDA calculations performed with nonspherical densities.« less

Finite Temperature Densities via the S-Function Method with Application to Electron Screening in Plasmas

NASA Astrophysics Data System (ADS)

Watrous, Mitchell James

1997-12-01

A new approach to the Green's-function method for the calculation of equilibrium densities within the finite temperature, Kohn-Sham formulation of density functional theory is presented, which extends the method to all temperatures. The contour of integration in the complex energy plane is chosen such that the density is given by a sum of Green's function differences evaluated at the Matsubara frequencies, rather than by the calculation and summation of Kohn-Sham single-particle wave functions. The Green's functions are written in terms of their spectral representation and are calculated as the solutions of their defining differential equations. These differential equations are boundary value problems as opposed to the standard eigenvalue problems. For large values of the complex energy, the differential equations are further simplified from second to first-order by writing the Green's functions in terms of logarithmic derivatives. An asymptotic expression for the Green's functions is derived, which allows the sum over Matsubara poles to be approximated. The method is applied to the screening of nuclei by electrons in finite temperature plasmas. To demonstrate the method's utility, and to illustrate its advantages, the results of previous wave function type calculations for protons and neon nuclei are reproduced. The method is also used to formulate a new screening model for fusion reactions in the solar core, and the predicted reaction rate enhancements factors are compared with existing models.

Stability of mechanical joints in launching vehicles: Local and global stationary values of energy density

NASA Astrophysics Data System (ADS)

Chue, Ching-Hwei

A method was developed for predicting the behavior of mechanical joints in launch vehicles with particular emphasis placed on how the combined effects of loading, geometry, and materials could be optimized in terms of structure instability and/or integrity. What was considered to be essential is the fluctuation of the volume energy density with time in the structure. The peaks and valleys of the volume energy density function will be associated with failure by fracture and/or yielding while the distance between their local and global stationary values govern the structure instability. The Solid Rocket Booster (SRB) of the space shuttle was analyzed under axisymmetric and non-axisymmetric loadings. A semi-analytical finite element program was developed for solving the case of non-axisymmetric loading. Following a dynamic stress analysis, contours of the volume energy density in the structure were obtained as a function of time. The magnitudes and locations of these stationary values were then calculated locally and globally and related to possible failure by fracture. In the case of axisymmetric flight, the local and global instability behavior do not change appreciably. Fluctuations in the energy density and the dynamic stability length parameter become appreciable when the non-axisymmetric loads are considered. The magnitude of the energy in the shell structure is sensitive to alterations in the gas pressure induced by the solid propellant.

Nonlinear electronic excitations in crystalline solids using meta-generalized gradient approximation and hybrid functional in time-dependent density functional theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Sato, Shunsuke A.; Taniguchi, Yasutaka; Department of Medical and General Sciences, Nihon Institute of Medical Science, 1276 Shimogawara, Moroyama-Machi, Iruma-Gun, Saitama 350-0435

2015-12-14

We develop methods to calculate electron dynamics in crystalline solids in real-time time-dependent density functional theory employing exchange-correlation potentials which reproduce band gap energies of dielectrics; a meta-generalized gradient approximation was proposed by Tran and Blaha [Phys. Rev. Lett. 102, 226401 (2009)] (TBm-BJ) and a hybrid functional was proposed by Heyd, Scuseria, and Ernzerhof [J. Chem. Phys. 118, 8207 (2003)] (HSE). In time evolution calculations employing the TB-mBJ potential, we have found it necessary to adopt the predictor-corrector step for a stable time evolution. We have developed a method to evaluate electronic excitation energy without referring to the energy functionalmore » which is unknown for the TB-mBJ potential. For the HSE functional, we have developed a method for the operation of the Fock-like term in Fourier space to facilitate efficient use of massive parallel computers equipped with graphic processing units. We compare electronic excitations in silicon and germanium induced by femtosecond laser pulses using the TB-mBJ, HSE, and a simple local density approximation (LDA). At low laser intensities, electronic excitations are found to be sensitive to the band gap energy: they are close to each other using TB-mBJ and HSE and are much smaller in LDA. At high laser intensities close to the damage threshold, electronic excitation energies do not differ much among the three cases.« less

Topology-guided deformable registration with local importance preservation for biomedical images

NASA Astrophysics Data System (ADS)

Zheng, Chaojie; Wang, Xiuying; Zeng, Shan; Zhou, Jianlong; Yin, Yong; Feng, Dagan; Fulham, Michael

2018-01-01

The demons registration (DR) model is well recognized for its deformation capability. However, it might lead to misregistration due to erroneous diffusion direction when there are no overlaps between corresponding regions. We propose a novel registration energy function, introducing topology energy, and incorporating a local energy function into the DR in a progressive registration scheme, to address these shortcomings. The topology energy that is derived from the topological information of the images serves as a direction inference to guide diffusion transformation to retain the merits of DR. The local energy constrains the deformation disparity of neighbouring pixels to maintain important local texture and density features. The energy function is minimized in a progressive scheme steered by a topology tree graph and we refer to it as topology-guided deformable registration (TDR). We validated our TDR on 20 pairs of synthetic images with Gaussian noise, 20 phantom PET images with artificial deformations and 12 pairs of clinical PET-CT studies. We compared it to three methods: (1) free-form deformation registration method, (2) energy-based DR and (3) multi-resolution DR. The experimental results show that our TDR outperformed the other three methods in regard to structural correspondence and preservation of the local important information including texture and density, while retaining global correspondence.

Trapezium Bone Density-A Comparison of Measurements by DXA and CT.

PubMed

Breddam Mosegaard, Sebastian; Breddam Mosegaard, Kamille; Bouteldja, Nadia; Bæk Hansen, Torben; Stilling, Maiken

2018-01-18

Bone density may influence the primary fixation of cementless implants, and poor bone density may increase the risk of implant failure. Before deciding on using total joint replacement as treatment in osteoarthritis of the trapeziometacarpal joint, it is valuable to determine the trapezium bone density. The aim of this study was to: (1) determine the correlation between measurements of bone mineral density of the trapezium obtained by dual-energy X-ray absorptiometry (DXA) scans by a circumference method and a new inner-ellipse method; and (2) to compare those to measurements of bone density obtained by computerized tomography (CT)-scans in Hounsfield units (HU). We included 71 hands from 59 patients with a mean age of 59 years (43-77). All patients had Eaton-Glickel stage II-IV trapeziometacarpal (TM) joint osteoarthritis, were under evaluation for trapeziometacarpal total joint replacement, and underwent DXA and CT wrist scans. There was an excellent correlation (r = 0.94) between DXA bone mineral density measures using the circumference and the inner-ellipse method. There was a moderate correlation between bone density measures obtained by DXA- and CT-scans with (r = 0.49) for the circumference method, and (r = 0.55) for the inner-ellipse method. DXA may be used in pre-operative evaluation of the trapezium bone quality, and the simpler DXA inner-ellipse measurement method can replace the DXA circumference method in estimation of bone density of the trapezium.

Free energy calculations: an efficient adaptive biasing potential method.

PubMed

Dickson, Bradley M; Legoll, Frédéric; Lelièvre, Tony; Stoltz, Gabriel; Fleurat-Lessard, Paul

2010-05-06

We develop an efficient sampling and free energy calculation technique within the adaptive biasing potential (ABP) framework. By mollifying the density of states we obtain an approximate free energy and an adaptive bias potential that is computed directly from the population along the coordinates of the free energy. Because of the mollifier, the bias potential is "nonlocal", and its gradient admits a simple analytic expression. A single observation of the reaction coordinate can thus be used to update the approximate free energy at every point within a neighborhood of the observation. This greatly reduces the equilibration time of the adaptive bias potential. This approximation introduces two parameters: strength of mollification and the zero of energy of the bias potential. While we observe that the approximate free energy is a very good estimate of the actual free energy for a large range of mollification strength, we demonstrate that the errors associated with the mollification may be removed via deconvolution. The zero of energy of the bias potential, which is easy to choose, influences the speed of convergence but not the limiting accuracy. This method is simple to apply to free energy or mean force computation in multiple dimensions and does not involve second derivatives of the reaction coordinates, matrix manipulations nor on-the-fly adaptation of parameters. For the alanine dipeptide test case, the new method is found to gain as much as a factor of 10 in efficiency as compared to two basic implementations of the adaptive biasing force methods, and it is shown to be as efficient as well-tempered metadynamics with the postprocess deconvolution giving a clear advantage to the mollified density of states method.

Device and method for imploding a microsphere with a fast liner

DOEpatents

Thode, Lester E.

1981-01-01

A device and method for relativistic electron beam heating of a high-density plasma in a small localized region. A relativistic electron beam generator or accelerator produces a high-voltage electron beam which propagates along a vacuum drift tube and is modulated to initiate electron bunching within the beam. The beam is then directed through a low-density gas chamber which provides isolation between the vacuum modulator and the relativistic electron beam target. The relativistic beam is then applied to a high-density target plasma which typically comprises DT, DD, hydrogen boron or similar thermonuclear gas at a density of 10.sup.17 to 10.sup.20 electrons per cubic centimeter. The target gas is ionized prior to application of the electron beam by means of a laser or other preionization source to form a plasma. Utilizing a relativistic electron beam with an individual particle energy exceeding 3 MeV, classical scattering by relativistic electrons passing through isolation foils is negligible. As a result, relativistic streaming instabilities are initiated within the high-density target plasma causing the relativistic electron beam to efficiently deposit its energy and momentum into a small localized region of the high-density plasma target. Fast liners disposed in the high-density target plasma are explosively or ablatively driven to implosion by a heated annular plasma surrounding the fast liner generated by an annular relativistic electron beam. An azimuthal magnetic field produced by axial current flow in the annular plasma, causes the energy in the heated annular plasma to converge on the fast liner to drive the fast liner to implode a microsphere.

Characterizing the potential energy surface of the water dimer with DFT: failures of some popular functionals for hydrogen bonding.

PubMed

Anderson, Julie A; Tschumper, Gregory S

2006-06-08

Ten stationary points on the water dimer potential energy surface have been examined with ten density functional methods (X3LYP, B3LYP, B971, B98, MPWLYP, PBE1PBE, PBE, MPW1K, B3P86, and BHandHLYP). Geometry optimizations and vibrational frequency calculations were carried out with the TZ2P(f,d)+dif basis set. All ten of the density functionals correctly describe the relative energies of the ten stationary points. However, correctly describing the curvature of the potential energy surface is far more difficult. Only one functional (BHandHLYP) reproduces the number of imaginary frequencies from CCSD(T) calculations. The other nine density functionals fail to correctly characterize the nature of at least one of the ten (H(2)O)(2) stationary points studied here.

Statistical γ -decay properties of 64Ni and deduced (n ,γ ) cross section of the s -process branch-point nucleus 63Ni

NASA Astrophysics Data System (ADS)

Crespo Campo, L.; Bello Garrote, F. L.; Eriksen, T. K.; Görgen, A.; Guttormsen, M.; Hadynska-Klek, K.; Klintefjord, M.; Larsen, A. C.; Renstrøm, T.; Sahin, E.; Siem, S.; Springer, A.; Tornyi, T. G.; Tveten, G. M.

2016-10-01

Particle-γ coincidence data have been analyzed to obtain the nuclear level density and the γ -strength function of 64Ni by means of the Oslo method. The level density found in this work is in very good agreement with known energy levels at low excitation energies as well as with data deduced from particle-evaporation measurements at excitation energies above Ex≈5.5 MeV. The experimental γ -strength function presents an enhancement at γ energies below Eγ≈3 MeV and possibly a resonancelike structure centered at Eγ≈9.2 MeV. The obtained nuclear level density and γ -strength function have been used to estimate the (n ,γ ) cross section for the s -process branch-point nucleus 63Ni, of particular interest for astrophysical calculations of elemental abundances.

Modeling Electronic-Nuclear Interactions for Excitation Energy Transfer Processes in Light-Harvesting Complexes.

PubMed

Lee, Mi Kyung; Coker, David F

2016-08-18

An accurate approach for computing intermolecular and intrachromophore contributions to spectral densities to describe the electronic-nuclear interactions relevant for modeling excitation energy transfer processes in light harvesting systems is presented. The approach is based on molecular dynamics (MD) calculations of classical correlation functions of long-range contributions to excitation energy fluctuations and a separate harmonic analysis and single-point gradient quantum calculations for electron-intrachromophore vibrational couplings. A simple model is also presented that enables detailed analysis of the shortcomings of standard MD-based excitation energy fluctuation correlation function approaches. The method introduced here avoids these problems, and its reliability is demonstrated in accurate predictions for bacteriochlorophyll molecules in the Fenna-Matthews-Olson pigment-protein complex, where excellent agreement with experimental spectral densities is found. This efficient approach can provide instantaneous spectral densities for treating the influence of fluctuations in environmental dissipation on fast electronic relaxation.

Phosphorene quantum dot-fullerene nanocomposites for solar energy conversion: An unexplored inorganic-organic nanohybrid with novel photovoltaic properties

NASA Astrophysics Data System (ADS)

Rajbanshi, Biplab; Kar, Moumita; Sarkar, Pallavi; Sarkar, Pranab

2017-10-01

Using the self-consistent charge density-functional based tight-binding (SCC-DFTB) method, coupled with time-dependent density functional theory (TDDFT) calculations, for the first time we explore the possibility of use of phosphorene quantum dots in solar energy harvesting devices. The phosphorene quantum dots-fullerene (PQDs-PCBA) nanocomposites show type-II band alignment indicating spatial separation of charge carriers. The TDDFT calculations also show that the PQD-fullerene nanocomposites seem to be exciting material for future generation solar energy harvester, with extremely fast charge transfer and very poor recombination rate.

Application of the Interacting Quantum Atoms Approach to the S66 and Ionic-Hydrogen-Bond Datasets for Noncovalent Interactions.

PubMed

Suárez, Dimas; Díaz, Natalia; Francisco, Evelio; Martín Pendás, Angel

2018-04-17

The interacting quantum atoms (IQA) method can assess, systematically and in great detail, the strength and physics of both covalent and noncovalent interactions. The lack of a pair density in density functional theory (DFT), which precludes the direct IQA decomposition of the characteristic exchange-correlation energy, has been recently overcome by means of a scaling technique, which can largely expand the applicability of the method. To better assess the utility of the augmented IQA methodology to derive quantum chemical decompositions at the atomic and molecular levels, we report the results of Hartree-Fock (HF) and DFT calculations on the complexes included in the S66 and the ionic H-bond databases of benchmark geometry and binding energies. For all structures, we perform single-point and geometry optimizations using HF and selected DFT methods with triple-ζ basis sets followed by full IQA calculations. Pairwise dispersion energies are accounted for by the D3 method. We analyze the goodness of the HF-D3 and DFT-D3 binding energies, the magnitude of numerical errors, the fragment and atomic distribution of formation energies, etc. It is shown that fragment-based IQA decomposes the formation energies in comparable terms to those of perturbative approaches and that the atomic IQA energies hold the promise of rigorously quantifying atomic and group energy contributions in larger biomolecular systems. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Breast density evaluation using spectral mammography, radiologist reader assessment and segmentation techniques: a retrospective study based on left and right breast comparison

PubMed Central

Molloi, Sabee; Ding, Huanjun; Feig, Stephen

2015-01-01

Purpose The purpose of this study was to compare the precision of mammographic breast density measurement using radiologist reader assessment, histogram threshold segmentation, fuzzy C-mean segmentation and spectral material decomposition. Materials and Methods Spectral mammography images from a total of 92 consecutive asymptomatic women (50–69 years old) who presented for annual screening mammography were retrospectively analyzed for this study. Breast density was estimated using 10 radiologist reader assessment, standard histogram thresholding, fuzzy C-mean algorithm and spectral material decomposition. The breast density correlation between left and right breasts was used to assess the precision of these techniques to measure breast composition relative to dual-energy material decomposition. Results In comparison to the other techniques, the results of breast density measurements using dual-energy material decomposition showed the highest correlation. The relative standard error of estimate for breast density measurements from left and right breasts using radiologist reader assessment, standard histogram thresholding, fuzzy C-mean algorithm and dual-energy material decomposition was calculated to be 1.95, 2.87, 2.07 and 1.00, respectively. Conclusion The results indicate that the precision of dual-energy material decomposition was approximately factor of two higher than the other techniques with regard to better correlation of breast density measurements from right and left breasts. PMID:26031229

Method and means for a spatial and temporal probe for laser-generated plumes based on density gradients

DOEpatents

Yeung, E.S.; Chen, G.

1990-05-01

A method and means are disclosed for a spatial and temporal probe for laser generated plumes based on density gradients includes generation of a plume of vaporized material from a surface by an energy source. The probe laser beam is positioned so that the plume passes through the probe laser beam. Movement of the probe laser beam caused by refraction from the density gradient of the plume is monitored. Spatial and temporal information, correlated to one another, is then derived. 15 figs.

Radiometric analysis of photographic data by the effective exposure method

DOE Office of Scientific and Technical Information (OSTI.GOV)

Constantine, B J

1972-04-01

The effective exposure method provides for radiometric analysis of photographic data. A three-dimensional model, where density is a function of energy and wavelength, is postulated to represent the film response function. Calibration exposures serve to eliminate the other factors which affect image density. The effective exposure causing an image can be determined by comparing the image density with that of a calibration exposure. If the relative spectral distribution of the source is known, irradiance and/or radiance can be unfolded from the effective exposure expression.

A new time dependent density functional algorithm for large systems and plasmons in metal clusters

DOE Office of Scientific and Technical Information (OSTI.GOV)

Baseggio, Oscar; Fronzoni, Giovanna; Stener, Mauro, E-mail: stener@univ.trieste.it

2015-07-14

A new algorithm to solve the Time Dependent Density Functional Theory (TDDFT) equations in the space of the density fitting auxiliary basis set has been developed and implemented. The method extracts the spectrum from the imaginary part of the polarizability at any given photon energy, avoiding the bottleneck of Davidson diagonalization. The original idea which made the present scheme very efficient consists in the simplification of the double sum over occupied-virtual pairs in the definition of the dielectric susceptibility, allowing an easy calculation of such matrix as a linear combination of constant matrices with photon energy dependent coefficients. The methodmore » has been applied to very different systems in nature and size (from H{sub 2} to [Au{sub 147}]{sup −}). In all cases, the maximum deviations found for the excitation energies with respect to the Amsterdam density functional code are below 0.2 eV. The new algorithm has the merit not only to calculate the spectrum at whichever photon energy but also to allow a deep analysis of the results, in terms of transition contribution maps, Jacob plasmon scaling factor, and induced density analysis, which have been all implemented.« less

Level densities and γ-ray strength functions in Sn isotopes

NASA Astrophysics Data System (ADS)

Toft, H. K.; Larsen, A. C.; Agvaanluvsan, U.; Bürger, A.; Guttormsen, M.; Mitchell, G. E.; Nyhus, H. T.; Schiller, A.; Siem, S.; Syed, N. U. H.; Voinov, A.

2010-06-01

The nuclear level densities of Sn118,119 and the γ-ray strength functions of Sn116,118,119 below the neutron separation energy are extracted with the Oslo method using the (He3,αγ) and (He3,He3'γ) reactions. The level-density function of Sn119 displays steplike structures. The microcanonical entropies are deduced from the level densities, and the single neutron entropy of Sn119 is determined to be 1.7 ± 0.2 kB. Results from a combinatorial model support the interpretation that some of the low-energy steps in the level density function are caused by neutron pair breaking. An enhancement in all the γ-ray strength functions of Sn116-119, compared to standard models for radiative strength, is observed for the γ-ray energy region of ≃4-11 MeV. These small resonances all have a centroid energy of 8.0(1) MeV and an integrated strength corresponding to 1.7(9)% of the classical Thomas-Reiche-Kuhn sum rule. The Sn resonances may be due to electric dipole neutron skin oscillations or to an enhancement of the giant magnetic dipole resonance.

Conceptual DFT analysis of the fragility spectra of atoms along the minimum energy reaction coordinate.

PubMed

Ordon, Piotr; Komorowski, Ludwik; Jedrzejewski, Mateusz

2017-10-07

Theoretical justification has been provided to the method for monitoring the sequence of chemical bonds' rearrangement along a reaction path, by tracing the evolution of the diagonal elements of the Hessian matrix. Relations between the divergences of Hellman-Feynman forces and the energy and electron density derivatives have been demonstrated. By the proof presented on the grounds of the conceptual density functional theory formalism, the spectral amplitude observed on the atomic fragility spectra [L. Komorowski et al., Phys. Chem. Chem. Phys. 18, 32658 (2016)] reflects selectively the electron density modifications in bonds of an atom. In fact the spectral peaks for an atom reveal changes of the electron density occurring with bonds creation, breaking, or varying with the reaction progress.

Conceptual DFT analysis of the fragility spectra of atoms along the minimum energy reaction coordinate

NASA Astrophysics Data System (ADS)

Ordon, Piotr; Komorowski, Ludwik; Jedrzejewski, Mateusz

2017-10-01

Theoretical justification has been provided to the method for monitoring the sequence of chemical bonds' rearrangement along a reaction path, by tracing the evolution of the diagonal elements of the Hessian matrix. Relations between the divergences of Hellman-Feynman forces and the energy and electron density derivatives have been demonstrated. By the proof presented on the grounds of the conceptual density functional theory formalism, the spectral amplitude observed on the atomic fragility spectra [L. Komorowski et al., Phys. Chem. Chem. Phys. 18, 32658 (2016)] reflects selectively the electron density modifications in bonds of an atom. In fact the spectral peaks for an atom reveal changes of the electron density occurring with bonds creation, breaking, or varying with the reaction progress.

Electronic structure of the alkyne-bridged dicobalt hexacarbonyl complex Co(2) micro-C(2)H(2) (CO)(6): evidence for singlet diradical character and implications for metal-metal bonding.

PubMed

Platts, James A; Evans, Gareth J S; Coogan, Michael P; Overgaard, Jacob

2007-08-06

A series of ab initio calculations are presented on the alkyne-bridged dicobalt hexacarbonyl cluster Co2 micro-C2H2 (CO)6, indicating that this compound has substantial multireference character, which we interpret as evidence of singlet diradical behavior. As a result, standard theoretical methods such as restricted Hartree-Fock (RHF) or Kohn-Sham (RKS) density functional theory cannot properly describe this compound. We have therefore used complete active space (CAS) methods to explore the bonding in and spectroscopic properties of Co2 micro-C2H2 (CO)6. CAS methods identify significant population of a Co-Co antibonding orbital, along with Co-pi* back-bonding, and a relatively large singlet-triplet energy splitting. Analysis of the electron density and related quantities, such as energy densities and atomic overlaps, indicates a small but significant amount of covalent bonding between cobalt centers.

Molecular properties via a subsystem density functional theory formulation: a common framework for electronic embedding.

PubMed

Höfener, Sebastian; Gomes, André Severo Pereira; Visscher, Lucas

2012-01-28

In this article, we present a consistent derivation of a density functional theory (DFT) based embedding method which encompasses wave-function theory-in-DFT (WFT-in-DFT) and the DFT-based subsystem formulation of response theory (DFT-in-DFT) by Neugebauer [J. Neugebauer, J. Chem. Phys. 131, 084104 (2009)] as special cases. This formulation, which is based on the time-averaged quasi-energy formalism, makes use of the variation Lagrangian techniques to allow the use of non-variational (in particular: coupled cluster) wave-function-based methods. We show how, in the time-independent limit, we naturally obtain expressions for the ground-state DFT-in-DFT and WFT-in-DFT embedding via a local potential. We furthermore provide working equations for the special case in which coupled cluster theory is used to obtain the density and excitation energies of the active subsystem. A sample application is given to demonstrate the method. © 2012 American Institute of Physics

WE-DE-207B-04: Quantitative Contrast-Enhanced Spectral Mammography Based On Photon-Counting Detectors: A Feasibility Study

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ding, H; Zhou, B; Beidokhti, D

Purpose: To investigate the feasibility of accurate quantification of iodine mass thickness in contrast-enhanced spectral mammography. Methods: Experimental phantom studies were performed on a spectral mammography system based on Si strip photon-counting detectors. Dual-energy images were acquired using 40 kVp and a splitting energy of 34 keV with 3 mm Al pre-filtration. The initial calibration was done with glandular and adipose tissue equivalent phantoms of uniform thicknesses and iodine disk phantoms of various concentrations. A secondary calibration was carried out using the iodine signal obtained from the dual-energy decomposed images and the known background phantom thicknesses and densities. The iodinemore » signal quantification method was validated using phantoms composed of a mixture of glandular and adipose materials, for various breast thicknesses and densities. Finally, the traditional dual-energy weighted subtraction method was also studied as a comparison. The measured iodine signal from both methods was compared to the known iodine concentrations of the disk phantoms to characterize the quantification accuracy. Results: There was good agreement between the iodine mass thicknesses measured using the proposed method and the known values. The root-mean-square (RMS) error was estimated to be 0.2 mg/cm2. The traditional weighted subtraction method also predicted a linear correlation between the measured signal and the known iodine mass thickness. However, the correlation slope and offset values were strongly dependent on the total breast thickness and density. Conclusion: The results of the current study suggest that iodine mass thickness can be accurately quantified with contrast-enhanced spectral mammography. The quantitative information can potentially improve the differentiation between benign and malignant legions. Grant funding from Philips Medical Systems.« less

Understanding density functional theory (DFT) and completing it in practice

DOE Office of Scientific and Technical Information (OSTI.GOV)

Bagayoko, Diola

2014-12-15

We review some salient points in the derivation of density functional theory (DFT) and of the local density approximation (LDA) of it. We then articulate an understanding of DFT and LDA that seems to be ignored in the literature. We note the well-established failures of many DFT and LDA calculations to reproduce the measured energy gaps of finite systems and band gaps of semiconductors and insulators. We then illustrate significant differences between the results from self consistent calculations using single trial basis sets and those from computations following the Bagayoko, Zhao, and Williams (BZW) method, as enhanced by Ekuma andmore » Franklin (BZW-EF). Unlike the former, the latter calculations verifiably attain the absolute minima of the occupied energies, as required by DFT. These minima are one of the reasons for the agreement between their results and corresponding, experimental ones for the band gap and a host of other properties. Further, we note predictions of DFT BZW-EF calculations that have been confirmed by experiment. Our subsequent description of the BZW-EF method ends with the application of the Rayleigh theorem in the selection, among the several calculations the method requires, of the one whose results have a full, physics content ascribed to DFT. This application of the Rayleigh theorem adds to or completes DFT, in practice, to preserve the physical content of unoccupied, low energy levels. Discussions, including implications of the method, and a short conclusion follow the description of the method. The successive augmentation of the basis set in the BZW-EF method, needed for the application of the Rayleigh theorem, is also necessary in the search for the absolute minima of the occupied energies, in practice.« less

The QTP family of consistent functionals and potentials in Kohn-Sham density functional theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jin, Yifan; Bartlett, Rodney J., E-mail: bartlett@qtp.ufl.edu

This manuscript presents the second, consistent density functional in the QTP (Quantum Theory Project) family, that is, the CAM-QTP(01). It is a new range-separated exchange-correlation functional in which the non-local exchange contribution is 100% at large separation. It follows the same basic principles of this family that the Kohn-Sham eigenvalues of the occupied orbitals approximately equal the vertical ionization energies, which is not fulfilled by most of the traditional density functional methods. This new CAM-QTP(01) functional significantly improves the accuracy of the vertical excitation energies especially for the Rydberg states in the test set. It also reproduces many other propertiesmore » such as geometries, reaction barrier heights, and atomization energies.« less

Variational second order density matrix study of F3-: importance of subspace constraints for size-consistency.

PubMed

van Aggelen, Helen; Verstichel, Brecht; Bultinck, Patrick; Van Neck, Dimitri; Ayers, Paul W; Cooper, David L

2011-02-07

Variational second order density matrix theory under "two-positivity" constraints tends to dissociate molecules into unphysical fractionally charged products with too low energies. We aim to construct a qualitatively correct potential energy surface for F(3)(-) by applying subspace energy constraints on mono- and diatomic subspaces of the molecular basis space. Monoatomic subspace constraints do not guarantee correct dissociation: the constraints are thus geometry dependent. Furthermore, the number of subspace constraints needed for correct dissociation does not grow linearly with the number of atoms. The subspace constraints do impose correct chemical properties in the dissociation limit and size-consistency, but the structure of the resulting second order density matrix method does not exactly correspond to a system of noninteracting units.

Obtaining source current density related to irregularly structured electromagnetic target field inside human body using hybrid inverse/FDTD method.

PubMed

Han, Jijun; Yang, Deqiang; Sun, Houjun; Xin, Sherman Xuegang

2017-01-01

Inverse method is inherently suitable for calculating the distribution of source current density related with an irregularly structured electromagnetic target field. However, the present form of inverse method cannot calculate complex field-tissue interactions. A novel hybrid inverse/finite-difference time domain (FDTD) method that can calculate the complex field-tissue interactions for the inverse design of source current density related with an irregularly structured electromagnetic target field is proposed. A Huygens' equivalent surface is established as a bridge to combine the inverse and FDTD method. Distribution of the radiofrequency (RF) magnetic field on the Huygens' equivalent surface is obtained using the FDTD method by considering the complex field-tissue interactions within the human body model. The obtained magnetic field distributed on the Huygens' equivalent surface is regarded as the next target. The current density on the designated source surface is derived using the inverse method. The homogeneity of target magnetic field and specific energy absorption rate are calculated to verify the proposed method.

Antiproton powered propulsion with magnetically confined plasma engines

NASA Technical Reports Server (NTRS)

Lapointe, Michael R.

1989-01-01

Matter-antimatter annihilation releases more energy per unit mass than any other method of energy production, making it an attractive energy source for spacecraft propulsion. In the magnetically confined plasma engine, antiproton beams are injected axially into a pulsed magnetic mirror system, where they annihilate with an initially neutral hydrogen gas. The resulting charged annihilation products transfer energy to the hydrogen propellant, which is then exhausted through one end of the pulsed mirror system to provide thrust. The calculated energy transfer efficiencies for a low number density (10(14)/cu cm) hydrogen propellant are insufficient to warrant operating the engine in this mode. Efficiencies are improved using moderate propellant number densities (10(16)/cu cm), but the energy transferred to the plasma in a realistic magnetic mirror system is generally limited to less than 2 percent of the initial proton-antiproton annihilation energy. The energy transfer efficiencies are highest for high number density (10(18)/cu cm) propellants, but plasma temperatures are reduced by excessive radiation losses. Low to moderate thrust over a wide range of specific impulse can be generated with moderate propellant number densities, while higher thrust but lower specific impulse may be generated using high propellant number densities. Significant mass will be required to shield the superconducting magnet coils from the high energy gamma radiation emitted by neutral pion decay. The mass of such a radiation shield may dominate the total engine mass, and could severely diminish the performance of antiproton powered engines which utilize magnetic confinement. The problem is compounded in the antiproton powered plasma engine, where lower energy plasma bremsstrahlung radiation may cause shield surface ablation and degradation.

Low-Density Nozzle Flow by the Direct Simulation Monte Carlo and Continuum Methods

NASA Technical Reports Server (NTRS)

Chung, Chang-Hong; Kim, Sku C.; Stubbs, Robert M.; Dewitt, Kenneth J.

1994-01-01

Two different approaches, the direct simulation Monte Carlo (DSMC) method based on molecular gasdynamics, and a finite-volume approximation of the Navier-Stokes equations, which are based on continuum gasdynamics, are employed in the analysis of a low-density gas flow in a small converging-diverging nozzle. The fluid experiences various kinds of flow regimes including continuum, slip, transition, and free-molecular. Results from the two numerical methods are compared with Rothe's experimental data, in which density and rotational temperature variations along the centerline and at various locations inside a low-density nozzle were measured by the electron-beam fluorescence technique. The continuum approach showed good agreement with the experimental data as far as density is concerned. The results from the DSMC method showed good agreement with the experimental data, both in the density and the rotational temperature. It is also shown that the simulation parameters, such as the gas/surface interaction model, the energy exchange model between rotational and translational modes, and the viscosity-temperature exponent, have substantial effects on the results of the DSMC method.

Collision cross sections of N2 by H+ impact at keV energies within time-dependent density-functional theory

NASA Astrophysics Data System (ADS)

Yu, W.; Gao, C.-Z.; Zhang, Y.; Zhang, F. S.; Hutton, R.; Zou, Y.; Wei, B.

2018-03-01

We calculate electron capture and ionization cross sections of N2 impacted by the H+ projectile at keV energies. To this end, we employ the time-dependent density-functional theory coupled nonadiabatically to molecular dynamics. To avoid the explicit treatment of the complex density matrix in the calculation of cross sections, we propose an approximate method based on the assumption of constant ionization rate over the period of the projectile passing the absorbing boundary. Our results agree reasonably well with experimental data and semi-empirical results within the measurement uncertainties in the considered energy range. The discrepancies are mainly attributed to the inadequate description of exchange-correlation functional and the crude approximation for constant ionization rate. Although the present approach does not predict the experiments quantitatively for collision energies below 10 keV, it is still helpful to calculate total cross sections of ion-molecule collisions within a certain energy range.

Development of Fast and Reliable Free-Energy Density Functional Methods for Simulations of Dense Plasmas from Cold- to Hot-Temperature Regimes

NASA Astrophysics Data System (ADS)

Karasiev, V. V.

2017-10-01

Free-energy density functional theory (DFT) is one of the standard tools in high-energy-density physics used to determine the fundamental properties of dense plasmas, especially in cold and warm regimes when quantum effects are essential. DFT is usually implemented via the orbital-dependent Kohn-Sham (KS) procedure. There are two challenges of conventional implementation: (1) KS computational cost becomes prohibitively expensive at high temperatures; and (2) ground-state exchange-correlation (XC) functionals do not take into account the XC thermal effects. This talk will address both challenges and report details of the formal development of new generalized gradient approximation (GGA) XC free-energy functional which bridges low-temperature (ground state) and high-temperature (plasma) limits. Recent progress on development of functionals for orbital-free DFT as a way to address the second challenge will also be discussed. This material is based upon work supported by the Department of Energy National Nuclear Security Administration under Award Number DE-NA0001944.

Large Energy Storage Density and High Thermal Stability in a Highly Textured (111)-Oriented Pb0.8Ba0.2ZrO3 Relaxor Thin Film with the Coexistence of Antiferroelectric and Ferroelectric Phases.

PubMed

Peng, Biaolin; Zhang, Qi; Li, Xing; Sun, Tieyu; Fan, Huiqing; Ke, Shanming; Ye, Mao; Wang, Yu; Lu, Wei; Niu, Hanben; Zeng, Xierong; Huang, Haitao

2015-06-24

A highly textured (111)-oriented Pb0.8Ba0.2ZrO3 (PBZ) relaxor thin film with the coexistence of antiferroelectric (AFE) and ferroelectric (FE) phases was prepared on a Pt/TiOx/SiO2/Si(100) substrate by using a sol-gel method. A large recoverable energy storage density of 40.18 J/cm(3) along with an efficiency of 64.1% was achieved at room temperature. Over a wide temperature range of 250 K (from room temperature to 523 K), the variation of the energy density is within 5%, indicating a high thermal stability. The high energy storage performance was endowed by a large dielectric breakdown strength, great relaxor dispersion, highly textured orientation, and the coexistence of FE and AFE phases. The PBZ thin film is believed to be an attractive material for applications in energy storage systems over a wide temperature range.

Experimental and DFT studies on the vibrational spectra of 1H-indene-2-boronic acid

NASA Astrophysics Data System (ADS)

Alver, Özgur; Kaya, Mehmet Fatih

2014-11-01

Stable conformers and geometrical molecular structures of 1H-indene-2-boronic acid (I-2B(OH)2) were studied experimentally and theoretically using FT-IR and FT-Raman spectroscopic methods. FT-IR and FT-Raman spectra were recorded in the region of 4000-400 cm-1, and 3700-400 cm-1, respectively. The optimized geometric structures were searched by Becke-3-Lee-Yang-Parr (B3LYP) hybrid density functional theory method with 6-31++G(d,p) basis set. Vibrational wavenumbers of I-2B(OH)2 were calculated using B3LYP density functional methods including 6-31++G(d,p) basis set. Experimental and theoretical results show that density functional B3LYP method gives satisfactory results for predicting vibrational wavenumbers except OH stretching modes which is probably due to increasing unharmonicity in the high wave number region and possible intra and inter molecular interaction at OH edges. To support the assigned vibrational wavenumbers, the potential energy distribution (PED) values were also calculated using VEDA 4 (Vibrational Energy Distribution Analysis) program.

Preliminary investigation of a sealed, remotely activated silver-zinc battery

NASA Technical Reports Server (NTRS)

Wheat, C. G.

1977-01-01

Methods necessary to provide a remotely activated, silver zinc battery capable of an extended activated stand while in a sealed condition were investigated. These requirements were to be accomplished in a battery package demonstrating an energy density of at least 35 watt hours per pound. Several methods of gas suppression were considered in view of the primary nature of this unit and utilized the electroplated dendritic zinc electrode. Amalgamation of the electrode provided the greatest suppression of gas at the zinc electrode. The approach to extending the activated stand capability of the remotely activated battery was through evaluation of three basic methods of remote, multi-cell activation; 1) the electrolyte manifold, 2) the gas manifold and 3) the individual cell. All three methods of activation can be incorporated into units which will meet the minimum energy density requirement.

Fruits and Vegetables Displace, But Do Not Decrease, Total Energy in School Lunches

PubMed Central

Schoeller, Dale A.

2014-01-01

Abstract Background: The high overweight and obesity prevalence among US children is a well-established public health concern. Diet is known to play a causal role in obesity. Increasing fruit and vegetable (FV) consumption to recommended levels is proposed to help reduce obesity, because their bulk and low energy density are believed to reduce energy-dense food consumption (volume displacement hypothesis). This study tests this hypothesis at the lunch meal among upper-elementary students participating in a Farm to School (F2S) program. Methods: Digital photographs of students' school lunch trays were visually analyzed to identify the food items and amounts that were present and consumed before and after the meal. Using the USDA Nutrient Database, total and FV-only energy were calculated for each tray. Analysis of total- and non-FV energy intake was performed according to (1) levels of FV energy intake, (2) FV energy density, and (3) previous years of Farm to School programming. Results: Higher intake of FV energy displaced non-FV energy, but total energy did not decrease across FV energy intake groups. High-FV-energy-density trays showed lower non-FV energy intake than low-FV-energy-density trays (470±179 vs. 534±219 kcal; p<0.0001). Trays from schools with more previous years of F2S programming decreased total and non-FV energy intake from school lunches (p for trend<0.0001, both). Conclusions: Increased FV consumption reduces non-FV energy intake, but does not reduce total energy intake. Therefore, this study does not support the volume displacement hypothesis and suggests calorie displacement instead. PMID:24988122

Battery technologies for large-scale stationary energy storage.

PubMed

Soloveichik, Grigorii L

2011-01-01

In recent years, with the deployment of renewable energy sources, advances in electrified transportation, and development in smart grids, the markets for large-scale stationary energy storage have grown rapidly. Electrochemical energy storage methods are strong candidate solutions due to their high energy density, flexibility, and scalability. This review provides an overview of mature and emerging technologies for secondary and redox flow batteries. New developments in the chemistry of secondary and flow batteries as well as regenerative fuel cells are also considered. Advantages and disadvantages of current and prospective electrochemical energy storage options are discussed. The most promising technologies in the short term are high-temperature sodium batteries with β″-alumina electrolyte, lithium-ion batteries, and flow batteries. Regenerative fuel cells and lithium metal batteries with high energy density require further research to become practical.

Neutron densities from a global analysis of medium-energy proton-nucleus elastic scattering

NASA Astrophysics Data System (ADS)

Clark, B. C.; Kerr, L. J.; Hama, S.

2003-05-01

A new method for extracting neutron densities from intermediate-energy elastic proton-nucleus scattering observables uses a global Dirac phenomenological approach based on the relativistic impulse approximation. Datasets for 40Ca, 48Ca, and 208Pb in the energy range from 500 MeV to 1040 MeV are considered. The global fits are successful in reproducing the data and in predicting datasets not included in the analysis. Using this global approach, energy-independent neutron densities are obtained. The vector point proton density distribution ρpv is determined from the empirical charge density after unfolding the proton form factor. The other densities, ρnv, ρps, ρns, are parametrized. This work provides energy-independent values for the rms neutron radius Rn and the neutron skin thickness Sn, in contrast to the energy-dependent values obtained by previous studies. In addition, the results presented in this paper show that the expected rms neutron radius and the skin thickness for 40Ca are accurately reproduced. The values of Rn and Sn obtained from the global fits that we consider to be the most reliable are given as follows: for 40Ca, 3.314>Rn>3.310 fm and -0.063>Sn >-0.067 fm; for 48Ca, 3.459>Rn>3.413 fm and 0.102>Sn>0.056 fm; and for 208Pb, 5.550>Rn>5.522 fm and 0.111>Sn>0.083 fm. These values are in reasonable agreement with nonrelativistic Skyrme-Hartree-Fock models and with relativistic Hartree-Bogoliubov models with density-dependent meson-nucleon couplings. The results from the global fits for 48Ca and 208Pb are generally not in agreement with the usual relativistic mean-field models.

Ratio of shear viscosity to entropy density in multifragmentation of Au + Au

NASA Astrophysics Data System (ADS)

Zhou, C. L.; Ma, Y. G.; Fang, D. Q.; Li, S. X.; Zhang, G. Q.

2012-06-01

The ratio of the shear viscosity (η) to entropy density (s) for the intermediate energy heavy-ion collisions has been calculated by using the Green-Kubo method in the framework of the quantum molecular dynamics model. The theoretical curve of η/s as a function of the incident energy for the head-on Au + Au collisions displays that a minimum region of η/s has been approached at higher incident energies, where the minimum η/s value is about 7 times Kovtun-Son-Starinets (KSS) bound (1/4π). We argue that the onset of minimum η/s region at higher incident energies corresponds to the nuclear liquid gas phase transition in nuclear multifragmentation.

Correlation Among the Variant Group, Effective Grain Size, and Elastic Strain Energy During the Phase Transformation in 9Ni Steels

NASA Astrophysics Data System (ADS)

Terasaki, Hidenori; Moriguchi, Koji; Tomio, Yusaku; Yamagishi, Hideki; Morito, Shigekazu

2017-12-01

The effect of carbon content on the density of variant-pair boundaries was investigated in 9Ni steel using an electron backscatter diffraction patterns method. The changes in the density of variant-pair boundaries were correlated with the nondestructive measured values of shear modulus of the austenite phase at the phase transformation point. Furthermore, the effective grain size was correlated with the shear modulus and the density of variant-pair boundaries. These relations are discussed from the viewpoint of self-accommodation of elastic strain energy and the nucleation event in the bainite and martensitic transformations.

Multi-Paradigm Multi-Scale Simulations for Fuel Cell Catalysts and Membranes

DTIC Science & Technology

2006-01-01

transfer studies on model systems. . Applying newly developed density functionals QM ( X3LYP ) for estimating the thermodynamics and kinetic energy...Density functional theory methods We have used many QM methods to probe chemical reaction mechanisms and find that the B3LYP and X3LYP [6] flavors of DFT...carried out QM calculations on the surface reactivity of the Pt and PtRu anode catalysts. This QM uses a new ab initio DFT-GGA method ( X3LYP ) [6

Lead-free 0.5Ba(Zr0.2Ti0.8)O3-0.5(Ba0.7Ca0.3)TiO3 nanowires for energy harvesting.

PubMed

Zhou, Zhi; Bowland, Christopher C; Malakooti, Mohammad H; Tang, Haixiong; Sodano, Henry A

2016-03-07

Lead-free piezoelectric nanowires (NWs) show strong potential in sensing and energy harvesting applications due to their flexibility and ability to convert mechanical energy to electric energy. Currently, most lead-free piezoelectric NWs are produced through low yield synthesis methods and result in low electromechanical coupling, which limit their efficiency as energy harvesters. In order to alleviate these issues, a scalable method is developed to synthesize perovskite type 0.5Ba(Zr0.2Ti0.8)O3-0.5(Ba0.7Ca0.3)TiO3 (BZT-BCT) NWs with high piezoelectric coupling coefficient. The piezoelectric coupling coefficient of the BZT-BCT NWs is measured by a refined piezoresponse force microscopy (PFM) testing method and shows the highest reported coupling coefficient for lead-free piezoelectric nanowires of 90 ± 5 pm V(-1). Flexible nanocomposites utilizing dispersed BZT-BCT NWs are fabricated to demonstrate an energy harvesting application with an open circuit voltage of up to 6.25 V and a power density of up to 2.25 μW cm(-3). The high electromechanical coupling coefficient and high power density demonstrated with these lead-free NWs produced via a scalable synthesis method shows the potential for high performance NW-based devices.

Density Functional Study of Structures and Electron Affinities of BrO4F/BrO4F−

PubMed Central

Gong, Liangfa; Xiong, Jieming; Wu, Xinmin; Qi, Chuansong; Li, Wei; Guo, Wenli

2009-01-01

The structures, electron affinities and bond dissociation energies of BrO4F/BrO4F− species have been investigated with five density functional theory (DFT) methods with DZP++ basis sets. The planar F-Br…O2…O2 complexes possess 3A′ electronic state for neutral molecule and 4A′ state for the corresponding anion. Three types of the neutral-anion energy separations are the adiabatic electron affinity (EAad), the vertical electron affinity (EAvert), and the vertical detachment energy (VDE). The EAad value predicted by B3LYP method is 4.52 eV. The bond dissociation energies De (BrO4F → BrO4-mF + Om) (m = 1–4) and De− (BrO4F− → BrO4-mF− + Om and BrO4F− → BrO4-mF + Om−) are predicted. The adiabatic electron affinities (EAad) were predicted to be 4.52 eV for F-Br…O2…O2 (3A′←4A′) (B3LYP method). PMID:19742128

A new quasi-relativistic approach for density functional theory based on the normalized elimination of the small component

NASA Astrophysics Data System (ADS)

Filatov, Michael; Cremer, Dieter

2002-01-01

A recently developed variationally stable quasi-relativistic method, which is based on the low-order approximation to the method of normalized elimination of the small component, was incorporated into density functional theory (DFT). The new method was tested for diatomic molecules involving Ag, Cd, Au, and Hg by calculating equilibrium bond lengths, vibrational frequencies, and dissociation energies. The method is easy to implement into standard quantum chemical programs and leads to accurate results for the benchmark systems studied.

Periodic subsystem density-functional theory

NASA Astrophysics Data System (ADS)

Genova, Alessandro; Ceresoli, Davide; Pavanello, Michele

2014-11-01

By partitioning the electron density into subsystem contributions, the Frozen Density Embedding (FDE) formulation of subsystem Density Functional Theory (DFT) has recently emerged as a powerful tool for reducing the computational scaling of Kohn-Sham DFT. To date, however, FDE has been employed to molecular systems only. Periodic systems, such as metals, semiconductors, and other crystalline solids have been outside the applicability of FDE, mostly because of the lack of a periodic FDE implementation. To fill this gap, in this work we aim at extending FDE to treat subsystems of molecular and periodic character. This goal is achieved by a dual approach. On one side, the development of a theoretical framework for periodic subsystem DFT. On the other, the realization of the method into a parallel computer code. We find that periodic FDE is capable of reproducing total electron densities and (to a lesser extent) also interaction energies of molecular systems weakly interacting with metallic surfaces. In the pilot calculations considered, we find that FDE fails in those cases where there is appreciable density overlap between the subsystems. Conversely, we find FDE to be in semiquantitative agreement with Kohn-Sham DFT when the inter-subsystem density overlap is low. We also conclude that to make FDE a suitable method for describing molecular adsorption at surfaces, kinetic energy density functionals that go beyond the GGA level must be employed.

Periodic subsystem density-functional theory.

PubMed

Genova, Alessandro; Ceresoli, Davide; Pavanello, Michele

2014-11-07

By partitioning the electron density into subsystem contributions, the Frozen Density Embedding (FDE) formulation of subsystem Density Functional Theory (DFT) has recently emerged as a powerful tool for reducing the computational scaling of Kohn-Sham DFT. To date, however, FDE has been employed to molecular systems only. Periodic systems, such as metals, semiconductors, and other crystalline solids have been outside the applicability of FDE, mostly because of the lack of a periodic FDE implementation. To fill this gap, in this work we aim at extending FDE to treat subsystems of molecular and periodic character. This goal is achieved by a dual approach. On one side, the development of a theoretical framework for periodic subsystem DFT. On the other, the realization of the method into a parallel computer code. We find that periodic FDE is capable of reproducing total electron densities and (to a lesser extent) also interaction energies of molecular systems weakly interacting with metallic surfaces. In the pilot calculations considered, we find that FDE fails in those cases where there is appreciable density overlap between the subsystems. Conversely, we find FDE to be in semiquantitative agreement with Kohn-Sham DFT when the inter-subsystem density overlap is low. We also conclude that to make FDE a suitable method for describing molecular adsorption at surfaces, kinetic energy density functionals that go beyond the GGA level must be employed.

Periodic subsystem density-functional theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Genova, Alessandro; Pavanello, Michele, E-mail: m.pavanello@rutgers.edu; Ceresoli, Davide

2014-11-07

By partitioning the electron density into subsystem contributions, the Frozen Density Embedding (FDE) formulation of subsystem Density Functional Theory (DFT) has recently emerged as a powerful tool for reducing the computational scaling of Kohn–Sham DFT. To date, however, FDE has been employed to molecular systems only. Periodic systems, such as metals, semiconductors, and other crystalline solids have been outside the applicability of FDE, mostly because of the lack of a periodic FDE implementation. To fill this gap, in this work we aim at extending FDE to treat subsystems of molecular and periodic character. This goal is achieved by a dualmore » approach. On one side, the development of a theoretical framework for periodic subsystem DFT. On the other, the realization of the method into a parallel computer code. We find that periodic FDE is capable of reproducing total electron densities and (to a lesser extent) also interaction energies of molecular systems weakly interacting with metallic surfaces. In the pilot calculations considered, we find that FDE fails in those cases where there is appreciable density overlap between the subsystems. Conversely, we find FDE to be in semiquantitative agreement with Kohn–Sham DFT when the inter-subsystem density overlap is low. We also conclude that to make FDE a suitable method for describing molecular adsorption at surfaces, kinetic energy density functionals that go beyond the GGA level must be employed.« less

Ab-initio study of electronic structure and elastic properties of ZrC

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mund, H. S., E-mail: hmoond@gmail.com; Ahuja, B. L.

2016-05-23

The electronic and elastic properties of ZrC have been investigated using the linear combination of atomic orbitals method within the framework of density functional theory. Different exchange-correlation functionals are taken into account within generalized gradient approximation. We have computed energy bands, density of states, elastic constants, bulk modulus, shear modulus, Young’s modulus, Poisson’s ratio, lattice parameters and pressure derivative of the bulk modulus by calculating ground state energy of the rock salt structure type ZrC.

High energy density aluminum battery

DOEpatents

Brown, Gilbert M.; Paranthaman, Mariappan Parans; Dai, Sheng; Dudney, Nancy J.; Manthiram, Arumugan; McIntyre, Timothy J.; Sun, Xiao-Guang; Liu, Hansan

2016-10-11

Compositions and methods of making are provided for a high energy density aluminum battery. The battery comprises an anode comprising aluminum metal. The battery further comprises a cathode comprising a material capable of intercalating aluminum or lithium ions during a discharge cycle and deintercalating the aluminum or lithium ions during a charge cycle. The battery further comprises an electrolyte capable of supporting reversible deposition and stripping of aluminum at the anode, and reversible intercalation and deintercalation of aluminum or lithium at the cathode.

One-step electrodeposited nickel cobalt sulfide nanosheet arrays for high-performance asymmetric supercapacitors.

PubMed

Chen, Wei; Xia, Chuan; Alshareef, Husam N

2014-09-23

A facile one-step electrodeposition method is developed to prepare ternary nickel cobalt sulfide interconnected nanosheet arrays on conductive carbon substrates as electrodes for supercapacitors, resulting in exceptional energy storage performance. Taking advantages of the highly conductive, mesoporous nature of the nanosheets and open framework of the three-dimensional nanoarchitectures, the ternary sulfide electrodes exhibit high specific capacitance (1418 F g(-1) at 5 A g(-1) and 1285 F g(-1) at 100 A g(-1)) with excellent rate capability. An asymmetric supercapacitor fabricated by the ternary sulfide nanosheet arrays as positive electrode and porous graphene film as negative electrode demonstrates outstanding electrochemical performance for practical energy storage applications. Our asymmetric supercapacitors show a high energy density of 60 Wh kg(-1) at a power density of 1.8 kW kg(-1). Even when charging the cell within 4.5 s, the energy density is still as high as 33 Wh kg(-1) at an outstanding power density of 28.8 kW kg(-1) with robust long-term cycling stability up to 50,000 cycles.

Symmetry Energy and Its Components in Finite Nuclei

NASA Astrophysics Data System (ADS)

Antonov, A. N.; Gaidarov, M. K.; Kadrev, D. N.; Sarriguren, P.; Moya de Guerra, E.

2018-05-01

We derive the volume and surface components of the nuclear symmetry energy (NSE) and their ratio within the coherent density fluctuation model. The estimations use the results of the model for the NSE in finite nuclei based on the Brueckner and Skyrme energy-density functionals for nuclear matter. The obtained values of the volume and surface contributions to the NSE and their ratio for the Ni, Sn, and Pb isotopic chains are compared with estimations of other approaches which have used available experimental data on binding energies, neutron-skin thicknesses, and excitation energies to isobaric analog states (IAS). Apart from the density dependence investigated in our previous works, we study also the temperature dependence of the symmetry energy in finite nuclei in the framework of the local density approximation combining it with the self-consistent Skyrme-HFB method using the cylindrical transformed deformed harmonic-oscillator basis. The results for the thermal evolution of the NSE in the interval T = 0–4 MeV show that its values decrease with temperature. The investigations of the T-dependence of the neutron and proton root-mean-square radii and the corresponding neutron skin thickness point out that the effect of temperature leads mainly to a substantial increase of the neutron radii and skins, especially in nuclei which are more rich of neutrons.

Determination of thermal physical properties of alkali fluoride/carbonate eutectic molten salt

NASA Astrophysics Data System (ADS)

An, Xue-Hui; Cheng, Jin-Hui; Su, Tao; Zhang, Peng

2017-06-01

Molten salts used in high temperatures are more and more interested in the CSP for higher energy conversion efficiency. Thermal physical properties are the basic engineering data of thermal hydraulic calculation and safety analysis. Therefore, the thermophysical performances involving density, specific heat capacity, viscosity and thermal conductivity of FLiNaK, (LiNaK)2CO3 and LiF(NaK)2CO3 molten salts are experimentally determined and through comparison the general rules can be summarized. Density measurement was performed on the basis of Archimedes theory; specific heat capacity was measured using the DSC technique; viscosity was tested based on the rotating method; and the thermal conductivity was gained by laser flash method with combination of the density, specific heat capacity and thermal diffusivity through a formula. Finally, the energy storage capacity and figures of merit are calculated to evaluate their feasibility as TES and HFT media. The results show that FLiNaK has the largest energy storage capacity and best heat transfer performance, LiF(NaK)2CO3 is secondary, and (LiNaK)2CO3 has the smallest.

Self-consistent description of the SHFB equations for 112Sn

NASA Astrophysics Data System (ADS)

Ghafouri, M.; Sadeghi, H.; Torkiha, M.

2018-03-01

The Hartree-Fock (HF) method is an excellent approximation of the closed shell magic nuclei. Pair correlation is essential for the description of open shell nuclei and has been derived for even-even, odd-odd and even-odd nuclei. These effects are reported by Hartree-Fock with BCS (HFBCS) or Hartree-Fock-Bogolyubov (HFB). These issues have been investigated, especially in the nuclear charts, and such studies have been compared with the observed information. We compute observations such as total binding energy, charge radius, densities, separation energies, pairing gaps and potential energy surfaces for neutrons and protons, and compare them with experimental data and the result of the spherical codes. In spherical even-even neutron-rich nuclei are considered in the Skyrme-Hartree-Fock-Bogolyubov (SHFB) method with density-dependent pairing interaction. Zero-range density-dependent interactions is used in the pairing channel. We solve SHF or SHFB equations in the spatial coordinates with spherical symmetry for tin isotopes such as 112Sn. The numerical accuracy of solving equations in the coordinate space is much greater than the fundamental extensions, which yields almost precise results.

Multiconfiguration Pair-Density Functional Theory: A New Way To Treat Strongly Correlated Systems.

PubMed

Gagliardi, Laura; Truhlar, Donald G; Li Manni, Giovanni; Carlson, Rebecca K; Hoyer, Chad E; Bao, Junwei Lucas

2017-01-17

The electronic energy of a system provides the Born-Oppenheimer potential energy for internuclear motion and thus determines molecular structure and spectra, bond energies, conformational energies, reaction barrier heights, and vibrational frequencies. The development of more efficient and more accurate ways to calculate the electronic energy of systems with inherently multiconfigurational electronic structure is essential for many applications, including transition metal and actinide chemistry, systems with partially broken bonds, many transition states, and most electronically excited states. Inherently multiconfigurational systems are called strongly correlated systems or multireference systems, where the latter name refers to the need for using more than one ("multiple") configuration state function to provide a good zero-order reference wave function. This Account describes multiconfiguration pair-density functional theory (MC-PDFT), which was developed as a way to combine the advantages of wave function theory (WFT) and density functional theory (DFT) to provide a better treatment of strongly correlated systems. First we review background material: the widely used Kohn-Sham DFT (which uses only a single Slater determinant as reference wave function), multiconfiguration WFT methods that treat inherently multiconfigurational systems based on an active space, and previous attempts to combine multiconfiguration WFT with DFT. Then we review the formulation of MC-PDFT. It is a generalization of Kohn-Sham DFT in that the electron kinetic energy and classical electrostatic energy are calculated from a reference wave function, while the rest of the energy is obtained from a density functional. However, there are two main differences with respent to Kohn-Sham DFT: (i) The reference wave function is multiconfigurational rather than being a single Slater determinant. (ii) The density functional is a function of the total density and the on-top pair density rather than being a function of the spin-up and spin-down densities. In work carried out so far, the multiconfigurational wave function is a multiconfiguration self-consistent-field wave function. The new formulation has the advantage that the reference wave function has the correct spatial and spin symmetry and can describe bond dissociation (of both single and multiple bonds) and electronic excitations in a formally and physically correct way. We then review the formulation of density functionals in terms of the on-top pair density. Finally we review successful applications of the theory to bond energies and bond dissociation potential energy curves of main-group and transition metal bonds, to barrier heights (including pericyclic reactions), to proton affinities, to the hydrogen bond energy of water dimer, to ground- and excited-state charge transfer, to valence and Rydberg excitations of molecules, and to singlet-triplet splittings of radicals. We find that that MC-PDFT can give accurate results not only with complete-active-space multiconfiguration wave functions but also with generalized-active-space multiconfiguration wave functions, which are practical for larger numbers of active electrons and active orbitals than are complete-active-space wave functions. The separated-pair approximation, which is a special case of generalized active space self-consistent-field theory, is especially promising. MC-PDFT, because it requires much less computer time and storage than pure WFT methods, has the potential to open larger and more complex strongly correlated systems to accurate simulation.

Simulation of electron energy loss spectra of nanomaterials with linear-scaling density functional theory

DOE PAGES

Tait, E. W.; Ratcliff, L. E.; Payne, M. C.; ...

2016-04-20

Experimental techniques for electron energy loss spectroscopy (EELS) combine high energy resolution with high spatial resolution. They are therefore powerful tools for investigating the local electronic structure of complex systems such as nanostructures, interfaces and even individual defects. Interpretation of experimental electron energy loss spectra is often challenging and can require theoretical modelling of candidate structures, which themselves may be large and complex, beyond the capabilities of traditional cubic-scaling density functional theory. In this work, we present functionality to compute electron energy loss spectra within the onetep linear-scaling density functional theory code. We first demonstrate that simulated spectra agree withmore » those computed using conventional plane wave pseudopotential methods to a high degree of precision. The ability of onetep to tackle large problems is then exploited to investigate convergence of spectra with respect to supercell size. As a result, we apply the novel functionality to a study of the electron energy loss spectra of defects on the (1 0 1) surface of an anatase slab and determine concentrations of defects which might be experimentally detectable.« less

A benchmark study of electronic excitation energies, transition moments, and excited-state energy gradients on the nicotine molecule

NASA Astrophysics Data System (ADS)

Egidi, Franco; Segado, Mireia; Koch, Henrik; Cappelli, Chiara; Barone, Vincenzo

2014-12-01

In this work, we report a comparative study of computed excitation energies, oscillator strengths, and excited-state energy gradients of (S)-nicotine, chosen as a test case, using multireference methods, coupled cluster singles and doubles, and methods based on time-dependent density functional theory. This system was chosen because its apparent simplicity hides a complex electronic structure, as several different types of valence excitations are possible, including n-π*, π-π*, and charge-transfer states, and in order to simulate its spectrum it is necessary to describe all of them consistently well by the chosen method.

A benchmark study of electronic excitation energies, transition moments, and excited-state energy gradients on the nicotine molecule

DOE Office of Scientific and Technical Information (OSTI.GOV)

Egidi, Franco, E-mail: franco.egidi@sns.it; Segado, Mireia; Barone, Vincenzo, E-mail: vincenzo.barone@sns.it

In this work, we report a comparative study of computed excitation energies, oscillator strengths, and excited-state energy gradients of (S)-nicotine, chosen as a test case, using multireference methods, coupled cluster singles and doubles, and methods based on time-dependent density functional theory. This system was chosen because its apparent simplicity hides a complex electronic structure, as several different types of valence excitations are possible, including n-π{sup *}, π-π{sup *}, and charge-transfer states, and in order to simulate its spectrum it is necessary to describe all of them consistently well by the chosen method.

Structure determination and characterization of two rare-earth molybdenum borate compounds: LnMoBO(6) (Ln = La, Ce).

PubMed

Zhao, Dan; Cheng, Wen-Dan; Zhang, Hao; Hang, Shu-Ping; Fang, Ming

2008-07-28

The structural, optical, and electronic properties of two rare-earth molybdenum borate compounds, LnMoBO(6) (Ln = La, Ce), have been investigated by means of single-crystal X-ray diffraction, elemental analyses, and spectral measurements, as well as calculations of energy band structures, density of states, and optical response functions by the density functional method. The title compounds, which crystallize in monoclinic space group P2(1)/c, possess a similar network of interconnected [Ce(2)(MoO(4))(2)](2+) chains and [BO(2)](-) wavy chains. Novel 1D molybdenum oxide chains are contained in their three-dimensional (3D) networks. The calculated results of crystal energy band structure by the density functional theory (DFT) method show that the solid-state compound LaMoBO(6) is a semiconductor with indirect band gaps.

Correlations between emission timescale of fragments and isospin dynamics in 124Sn+64Ni and 112Sn+58Ni reactions at 35A MeV

NASA Astrophysics Data System (ADS)

De Filippo, E.; Pagano, A.; Russotto, P.; Amorini, F.; Anzalone, A.; Auditore, L.; Baran, V.; Berceanu, I.; Borderie, B.; Bougault, R.; Bruno, M.; Cap, T.; Cardella, G.; Cavallaro, S.; Chatterjee, M. B.; Chbihi, A.; Colonna, M.; D'Agostino, M.; Dayras, R.; Di Toro, M.; Frankland, J.; Galichet, E.; Gawlikowicz, W.; Geraci, E.; Grzeszczuk, A.; Guazzoni, P.; Kowalski, S.; La Guidara, E.; Lanzalone, G.; Lanzanò, G.; Le Neindre, N.; Lombardo, I.; Maiolino, C.; Papa, M.; Piasecki, E.; Pirrone, S.; Płaneta, R.; Politi, G.; Pop, A.; Porto, F.; Rivet, M. F.; Rizzo, F.; Rosato, E.; Schmidt, K.; Siwek-Wilczyńska, K.; Skwira-Chalot, I.; Trifirò, A.; Trimarchi, M.; Verde, G.; Vigilante, M.; Wieleczko, J. P.; Wilczyński, J.; Zetta, L.; Zipper, W.

2012-07-01

We present a new experimental method to correlate the isotopic composition of intermediate mass fragments (IMF) emitted at midrapidity in semiperipheral collisions with the emission timescale: IMFs emitted in the early stage of the reaction show larger values of isospin asymmetry, stronger angular anisotropies, and reduced odd-even staggering effects in neutron to proton ratio distributions than those produced in sequential statistical emission. All these effects support the concept of isospin “migration”, that is sensitive to the density gradient between participant and quasispectator nuclear matter, in the so called neck fragmentation mechanism. By comparing the data to a stochastic mean field (SMF) simulation we show that this method gives valuable constraints on the symmetry energy term of nuclear equation of state at subsaturation densities. An indication emerges for a linear density dependence of the symmetry energy.

Tight-binding approximations to time-dependent density functional theory — A fast approach for the calculation of electronically excited states

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rüger, Robert, E-mail: rueger@scm.com; Department of Theoretical Chemistry, Vrije Universiteit Amsterdam, De Boelelaan 1083, 1081 HV Amsterdam; Wilhelm-Ostwald-Institut für Physikalische und Theoretische Chemie, Linnéstr. 2, 04103 Leipzig

2016-05-14

We propose a new method of calculating electronically excited states that combines a density functional theory based ground state calculation with a linear response treatment that employs approximations used in the time-dependent density functional based tight binding (TD-DFTB) approach. The new method termed time-dependent density functional theory TD-DFT+TB does not rely on the DFTB parametrization and is therefore applicable to systems involving all combinations of elements. We show that the new method yields UV/Vis absorption spectra that are in excellent agreement with computationally much more expensive TD-DFT calculations. Errors in vertical excitation energies are reduced by a factor of twomore » compared to TD-DFTB.« less

Fusion reaction cross-sections using the Wong model within Skyrme energy density based semiclassical extended Thomas Fermi approach

NASA Astrophysics Data System (ADS)

Kumar, Raj; Sharma, Manoj K.; Gupta, Raj K.

2011-11-01

First, the nuclear proximity potential, obtained by using the semiclassical extended Thomas Fermi (ETF) approach in Skyrme energy density formalism (SEDF), is shown to give more realistic barriers in frozen density approximation, as compared to the sudden approximation. Then, taking advantage of the fact that, in ETF method, different Skyrme forces give different barriers (height, position and curvature), we use the ℓ-summed extended-Wong model of Gupta and collaborators (2009) [1] under frozen densities approximation for calculating the cross-sections, where the Skyrme force is chosen with proper barrier characteristics, not-requiring additional "barrier modification" effects (lowering or narrowing, etc.), for a best fit to data at sub-barrier energies. The method is applied to capture cross-section data from 48Ca + 238U, 244Pu, and 248Cm reactions and to fusion-evaporation cross-sections from 58Ni + 58Ni, 64Ni + 64Ni, and 64Ni + 100Mo reactions, with effects of deformations and orientations of nuclei included, wherever required. Interestingly, whereas the capture cross-sections in Ca-induced reactions could be fitted to any force, such as SIII, SV and GSkI, by allowing a small change of couple of units in deduced ℓ-values at below-barrier energies, the near-barrier data point of 48Ca + 248Cm reaction could not be fitted to ℓ-values deduced for below-barrier energies, calling for a check of data. On the other hand, the fusion-evaporation cross-sections in Ni-induced reactions at sub-barrier energies required different Skyrme forces, representing "modifications of the barrier", for the best fit to data at all incident center-of-mass energies E's, displaying a kind of fusion hindrance at sub-barrier energies. This barrier modification effect is taken into care here by using different Skyrme forces for reactions belonging to different regions of the periodic table. Note that more than one Skyrme force (with identical barrier characteristics) could equally well fit the same data.

High energy density asymmetric supercapacitors with a nickel oxide nanoflake cathode and a 3D reduced graphene oxide anode

NASA Astrophysics Data System (ADS)

Luan, Feng; Wang, Gongming; Ling, Yichuan; Lu, Xihong; Wang, Hanyu; Tong, Yexiang; Liu, Xiao-Xia; Li, Yat

2013-08-01

Here we demonstrate a high energy density asymmetric supercapacitor with nickel oxide nanoflake arrays as the cathode and reduced graphene oxide as the anode. Nickel oxide nanoflake arrays were synthesized on a flexible carbon cloth substrate using a seed-mediated hydrothermal method. The reduced graphene oxide sheets were deposited on three-dimensional (3D) nickel foam by hydrothermal treatment of nickel foam in graphene oxide solution. The nanostructured electrodes provide a large effective surface area. The asymmetric supercapacitor device operates with a voltage of 1.7 V and achieved a remarkable areal capacitance of 248 mF cm-2 (specific capacitance of 50 F g-1) at a charge/discharge current density of 1 mA cm-2 and a maximum energy density of 39.9 W h kg-1 (based on the total mass of active materials of 5.0 mg). Furthermore, the device showed an excellent charge/discharge cycling performance in 1.0 M KOH electrolyte at a current density of 5 mA cm-2, with a capacitance retention of 95% after 3000 cycles.

Efficient algorithm for multiconfiguration pair-density functional theory with application to the heterolytic dissociation energy of ferrocene

NASA Astrophysics Data System (ADS)

Sand, Andrew M.; Truhlar, Donald G.; Gagliardi, Laura

2017-01-01

The recently developed multiconfiguration pair-density functional theory (MC-PDFT) combines multiconfiguration wave function theory with a density functional that depends on the on-top pair density of an electronic system. In an MC-PDFT calculation, there are two steps: a conventional multiconfiguration self-consistent-field (MCSCF) calculation and a post-MCSCF evaluation of the energy with an on-top density functional. In this work, we present the details of the MC-PDFT algorithm that avoids steeply scaling steps that are present in other post-self-consistent-field multireference calculations of dynamic correlation energy. We demonstrate the favorable scaling by considering systems of H2 molecules with active spaces of several different sizes. We then apply the MC-PDFT method to calculate the heterolytic dissociation enthalpy of ferrocene. We find that MC-PDFT yields results that are at least as accurate as complete active space second-order perturbation theory and are more stable with respect to basis set, but at a fraction of the cost in both time and memory.

Efficient algorithm for multiconfiguration pair-density functional theory with application to the heterolytic dissociation energy of ferrocene.

PubMed

Sand, Andrew M; Truhlar, Donald G; Gagliardi, Laura

2017-01-21

The recently developed multiconfiguration pair-density functional theory (MC-PDFT) combines multiconfiguration wave function theory with a density functional that depends on the on-top pair density of an electronic system. In an MC-PDFT calculation, there are two steps: a conventional multiconfiguration self-consistent-field (MCSCF) calculation and a post-MCSCF evaluation of the energy with an on-top density functional. In this work, we present the details of the MC-PDFT algorithm that avoids steeply scaling steps that are present in other post-self-consistent-field multireference calculations of dynamic correlation energy. We demonstrate the favorable scaling by considering systems of H 2 molecules with active spaces of several different sizes. We then apply the MC-PDFT method to calculate the heterolytic dissociation enthalpy of ferrocene. We find that MC-PDFT yields results that are at least as accurate as complete active space second-order perturbation theory and are more stable with respect to basis set, but at a fraction of the cost in both time and memory.

High energy density asymmetric supercapacitors with a nickel oxide nanoflake cathode and a 3D reduced graphene oxide anode.

PubMed

Luan, Feng; Wang, Gongming; Ling, Yichuan; Lu, Xihong; Wang, Hanyu; Tong, Yexiang; Liu, Xiao-Xia; Li, Yat

2013-09-07

Here we demonstrate a high energy density asymmetric supercapacitor with nickel oxide nanoflake arrays as the cathode and reduced graphene oxide as the anode. Nickel oxide nanoflake arrays were synthesized on a flexible carbon cloth substrate using a seed-mediated hydrothermal method. The reduced graphene oxide sheets were deposited on three-dimensional (3D) nickel foam by hydrothermal treatment of nickel foam in graphene oxide solution. The nanostructured electrodes provide a large effective surface area. The asymmetric supercapacitor device operates with a voltage of 1.7 V and achieved a remarkable areal capacitance of 248 mF cm(-2) (specific capacitance of 50 F g(-1)) at a charge/discharge current density of 1 mA cm(-2) and a maximum energy density of 39.9 W h kg(-1) (based on the total mass of active materials of 5.0 mg). Furthermore, the device showed an excellent charge/discharge cycling performance in 1.0 M KOH electrolyte at a current density of 5 mA cm(-2), with a capacitance retention of 95% after 3000 cycles.

Effects of an electric field on interaction of aromatic systems.

PubMed

Youn, Il Seung; Cho, Woo Jong; Kim, Kwang S

2016-04-30

The effect of uniform external electric field on the interactions between small aromatic compounds and an argon atom is investigated using post-HF (MP2, SCS-MP2, and CCSD(T)) and density functional (PBE0-D3, PBE0-TS, and vdW-DF2) methods. The electric field effect is quantified by the difference of interaction energy calculated in the presence and absence of the electric field. All the post-HF methods describe electric field effects accurately although the interaction energy itself is overestimated by MP2. The electric field effect is explained by classical electrostatic models, where the permanent dipole moment from mutual polarization mainly determines its sign. The size of π-conjugated system does not have significant effect on the electric field dependence. We found out that PBE0-based methods give reasonable interaction energies and electric field response in every case, while vdW-DF2 sometimes shows spurious artifact owing to its sensitivity toward the real space electron density. © 2015 Wiley Periodicals, Inc.

Effective scheme for partitioning covalent bonds in density-functional embedding theory: From molecules to extended covalent systems.

PubMed

Huang, Chen; Muñoz-García, Ana Belén; Pavone, Michele

2016-12-28

Density-functional embedding theory provides a general way to perform multi-physics quantum mechanics simulations of large-scale materials by dividing the total system's electron density into a cluster's density and its environment's density. It is then possible to compute the accurate local electronic structures and energetics of the embedded cluster with high-level methods, meanwhile retaining a low-level description of the environment. The prerequisite step in the density-functional embedding theory is the cluster definition. In covalent systems, cutting across the covalent bonds that connect the cluster and its environment leads to dangling bonds (unpaired electrons). These represent a major obstacle for the application of density-functional embedding theory to study extended covalent systems. In this work, we developed a simple scheme to define the cluster in covalent systems. Instead of cutting covalent bonds, we directly split the boundary atoms for maintaining the valency of the cluster. With this new covalent embedding scheme, we compute the dehydrogenation energies of several different molecules, as well as the binding energy of a cobalt atom on graphene. Well localized cluster densities are observed, which can facilitate the use of localized basis sets in high-level calculations. The results are found to converge faster with the embedding method than the other multi-physics approach ONIOM. This work paves the way to perform the density-functional embedding simulations of heterogeneous systems in which different types of chemical bonds are present.

Non-pairwise additivity of the leading-order dispersion energy

DOE Office of Scientific and Technical Information (OSTI.GOV)

Hollett, Joshua W., E-mail: j.hollett@uwinnipeg.ca

2015-02-28

The leading-order (i.e., dipole-dipole) dispersion energy is calculated for one-dimensional (1D) and two-dimensional (2D) infinite lattices, and an infinite 1D array of infinitely long lines, of doubly occupied locally harmonic wells. The dispersion energy is decomposed into pairwise and non-pairwise additive components. By varying the force constant and separation of the wells, the non-pairwise additive contribution to the dispersion energy is shown to depend on the overlap of density between neighboring wells. As well separation is increased, the non-pairwise additivity of the dispersion energy decays. The different rates of decay for 1D and 2D lattices of wells is explained inmore » terms of a Jacobian effect that influences the number of nearest neighbors. For an array of infinitely long lines of wells spaced 5 bohrs apart, and an inter-well spacing of 3 bohrs within a line, the non-pairwise additive component of the leading-order dispersion energy is −0.11 kJ mol{sup −1} well{sup −1}, which is 7% of the total. The polarizability of the wells and the density overlap between them are small in comparison to that of the atomic densities that arise from the molecular density partitioning used in post-density-functional theory (DFT) damped dispersion corrections, or DFT-D methods. Therefore, the nonadditivity of the leading-order dispersion observed here is a conservative estimate of that in molecular clusters.« less

Isovector dipole resonance and shear viscosity in low energy heavy-ion collisions

NASA Astrophysics Data System (ADS)

Guo, C. Q.; Ma, Y. G.; He, W. B.; Cao, X. G.; Fang, D. Q.; Deng, X. G.; Zhou, C. L.

2017-05-01

The ratio of shear viscosity over entropy density in low energy heavy-ion collision has been calculated by using the Green-Kubo method in the framework of an extended quantum molecular dynamics model. After the system almost reaches a local equilibration for a head-on 40Ca+100Mo collision, thermodynamic and transport properties are extracted. Meanwhile, the isovector giant dipole resonance (IVGDR) of the collision system also is studied. By the Gaussian fits to the IVGDR photon spectra, the peak energies of the IVGDR are extracted at different incident energies. The result shows that the IVGDR peak energy has a positive correlation with the ratio of shear viscosity over entropy density. This is a quantum effect and indicates a difference between nuclear matter and classical fluid.

Water 16-mers and hexamers: assessment of the three-body and electrostatically embedded many-body approximations of the correlation energy or the nonlocal energy as ways to include cooperative effects.

PubMed

Qi, Helena W; Leverentz, Hannah R; Truhlar, Donald G

2013-05-30

This work presents a new fragment method, the electrostatically embedded many-body expansion of the nonlocal energy (EE-MB-NE), and shows that it, along with the previously proposed electrostatically embedded many-body expansion of the correlation energy (EE-MB-CE), produces accurate results for large systems at the level of CCSD(T) coupled cluster theory. We primarily study water 16-mers, but we also test the EE-MB-CE method on water hexamers. We analyze the distributions of two-body and three-body terms to show why the many-body expansion of the electrostatically embedded correlation energy converges faster than the many-body expansion of the entire electrostatically embedded interaction potential. The average magnitude of the dimer contributions to the pairwise additive (PA) term of the correlation energy (which neglects cooperative effects) is only one-half of that of the average dimer contribution to the PA term of the expansion of the total energy; this explains why the mean unsigned error (MUE) of the EE-PA-CE approximation is only one-half of that of the EE-PA approximation. Similarly, the average magnitude of the trimer contributions to the three-body (3B) term of the EE-3B-CE approximation is only one-fourth of that of the EE-3B approximation, and the MUE of the EE-3B-CE approximation is one-fourth that of the EE-3B approximation. Finally, we test the efficacy of two- and three-body density functional corrections. One such density functional correction method, the new EE-PA-NE method, with the OLYP or the OHLYP density functional (where the OHLYP functional is the OptX exchange functional combined with the LYP correlation functional multiplied by 0.5), has the best performance-to-price ratio of any method whose computational cost scales as the third power of the number of monomers and is competitive in accuracy in the tests presented here with even the electrostatically embedded three-body approximation.

Quantification of the Relationship between Surrogate Fuel Structure and Performance

DTIC Science & Technology

2012-07-31

order to account for know deficiencies [18]. The frequencies are then used to calculate the zero point energy ( ZPE ). In the G3 theory HF/6-31G* was used...for the ZPE and the new procedure is likely to be more reliable. Also in contrast to previous G series composite methods, the Hartree–Fock energy...The total energy is obtained by adding the previously calculated ZPE . Durant and Rohlfing [38] reported that B3LYP density functional methods provide

Prediction of Excitation Energies for Conjugated Oligomers and Polymers from Time-Dependent Density Functional Theory

PubMed Central

Tao, Jianmin; Tretiak, Sergei; Zhu, Jian-Xin

2010-01-01

With technological advances, light-emitting conjugated oligomers and polymers have become competitive candidates in the commercial market of light-emitting diodes for display and other technologies, due to the ultralow cost, light weight, and flexibility. Prediction of excitation energies of these systems plays a crucial role in the understanding of their optical properties and device design. In this review article, we discuss the calculation of excitation energies with time-dependent density functional theory, which is one of the most successful methods in the investigation of the dynamical response of molecular systems to external perturbation, owing to its high computational efficiency.

Optical properties of B12P2 crystals: Ab initio calculation and EELS

NASA Astrophysics Data System (ADS)

Reshetniak, V. V.; Mavrin, B. N.; Medvedev, V. V.; Perezhogin, I. A.; Kulnitskiy, B. A.

2018-05-01

We report an experimental and theoretical investigation of the electronic structure and optical properties of B12P2 crystals in the energy range up to 60 eV. Experimental studies are performed by the method of electron energy loss spectroscopy, and theoretical studies are carried out using density functional theory and the GW approximation. The calculated dependence of the energy loss function is in agreement with the experiment. Based on the results of the calculations, we determine the optical properties of B12P2 crystals and investigate their anisotropy. The dispersion and density of electronic states are calculated and analyzed.

Roll-to-roll production of spray coated N-doped carbon nanotube electrodes for supercapacitors

NASA Astrophysics Data System (ADS)

Karakaya, Mehmet; Zhu, Jingyi; Raghavendra, Achyut J.; Podila, Ramakrishna; Parler, Samuel G.; Kaplan, James P.; Rao, Apparao M.

2014-12-01

Although carbon nanomaterials are being increasingly used in energy storage, there has been a lack of inexpensive, continuous, and scalable synthesis methods. Here, we present a scalable roll-to-roll (R2R) spray coating process for synthesizing randomly oriented multi-walled carbon nanotubes electrodes on Al foils. The coin and jellyroll type supercapacitors comprised such electrodes yield high power densities (˜700 mW/cm3) and energy densities (1 mW h/cm3) on par with Li-ion thin film batteries. These devices exhibit excellent cycle stability with no loss in performance over more than a thousand cycles. Our cost analysis shows that the R2R spray coating process can produce supercapacitors with 10 times the energy density of conventional activated carbon devices at ˜17% lower cost.

Surface energy and radiation balance systems - General description and improvements

NASA Technical Reports Server (NTRS)

Fritschen, Leo J.; Simpson, James R.

1989-01-01

Surface evaluation of sensible and latent heat flux densities and the components of the radiation balance were desired for various vegetative surfaces during the ASCOT84 experiment to compare with modeled results and to relate these values to drainage winds. Five battery operated data systems equipped with sensors to determine the above values were operated for 105 station days during the ASCOT84 experiment. The Bowen ratio energy balance technique was used to partition the available energy into the sensible and latent heat flux densities. A description of the sensors and battery operated equipment used to collect and process the data is presented. In addition, improvements and modifications made since the 1984 experiment are given. Details of calculations of soil heat flow at the surface and an alternate method to calculate sensible and latent heat flux densities are provided.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Azadi, Sam, E-mail: s.azadi@ucl.ac.uk; Cohen, R. E.; Department of Earth- and Environmental Sciences, Ludwig Maximilians Universität, Munich 80333

We studied the low-pressure (0–10 GPa) phase diagram of crystalline benzene using quantum Monte Carlo and density functional theory (DFT) methods. We performed diffusion quantum Monte Carlo (DMC) calculations to obtain accurate static phase diagrams as benchmarks for modern van der Waals density functionals. Using density functional perturbation theory, we computed the phonon contributions to the free energies. Our DFT enthalpy-pressure phase diagrams indicate that the Pbca and P2{sub 1}/c structures are the most stable phases within the studied pressure range. The DMC Gibbs free-energy calculations predict that the room temperature Pbca to P2{sub 1}/c phase transition occurs at 2.1(1)more » GPa. This prediction is consistent with available experimental results at room temperature. Our DMC calculations give 50.6 ± 0.5 kJ/mol for crystalline benzene lattice energy.« less

Advanced Sulfur-Silicon Full Cell Architecture for Lithium Ion Batteries.

PubMed

Ye, Rachel; Bell, Jeffrey; Patino, Daisy; Ahmed, Kazi; Ozkan, Mihri; Ozkan, Cengiz S

2017-12-08

Lithium-ion batteries are crucial to the future of energy storage. However, the energy density of current lithium-ion batteries is insufficient for future applications. Sulfur cathodes and silicon anodes have garnered a lot of attention in the field due their high capacity potential. Although recent developments in sulfur and silicon electrodes show exciting results in half cell formats, neither electrode can act as a lithium source when put together into a full cell format. Current methods toward incorporating lithium in sulfur-silicon full cells involves prelithiating silicon or using lithium sulfide. These methods however, complicate material processing and creates safety hazards. Herein, we present a novel full cell battery architecture that bypasses the issues associated with current methods. This battery architecture gradually integrates controlled amounts of pure lithium into the system by allowing lithium the access to external circuit. A high specific energy density of 350 Wh/kg after 250 cycles at C/10 was achieved using this method. This work should pave the way for future researches into sulfur-silicon full cells.

Local thermodynamic equilibrium in rapidly heated high energy density plasmas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Aslanyan, V.; Tallents, G. J.

Emission spectra and the dynamics of high energy density plasmas created by optical and Free Electron Lasers (FELs) depend on the populations of atomic levels. Calculations of plasma emission and ionization may be simplified by assuming Local Thermodynamic Equilibrium (LTE), where populations are given by the Saha-Boltzmann equation. LTE can be achieved at high densities when collisional processes are much more significant than radiative processes, but may not be valid if plasma conditions change rapidly. A collisional-radiative model has been used to calculate the times taken by carbon and iron plasmas to reach LTE at varying densities and heating rates.more » The effect of different energy deposition methods, as well as Ionization Potential Depression are explored. This work shows regimes in rapidly changing plasmas, such as those created by optical lasers and FELs, where the use of LTE is justified, because timescales for plasma changes are significantly longer than the times needed to achieve an LTE ionization balance.« less

Dependence of Mobility on Density of Gap States in Organics by GAMEaS - Gate Modulated Activation Energy Spectroscopy

NASA Astrophysics Data System (ADS)

So, Woo-Young; Lang, David; Ramirez, Arthur

2008-03-01

We develop a spectroscopic method for determining the density of states (DOS) in the energy gap - GAte Modulated activation Energy Spectroscopy (GAMEaS), We also report the relationship of these gap states to the mobility of organic field-effect-transistors (FETs). We find that the field-effect mobility is parameterized by two factors: (1) the free-carrier mobility and (2) the ratio of the free carrier density to the total carrier density induced by the gate bias. We show that the highest mobility FETs have shallow exponential band tails of localized states with characteristic slope of 1/kT at 300K. Most remarkably, state-of-the-art crystalline FETs fabricated from rubrene, pentacene, and tetracene all have a very high free-carrier mobility, up to 200cm2/Vsec at 300K, with the somewhat lower effective mobilities dominated by localized gap states. This strongly suggests that further improvements in device performance could be possible with enhanced material quality.

Studies on effective atomic numbers for photon energy absorption and electron density of some narcotic drugs in the energy range 1 keV-20 MeV

NASA Astrophysics Data System (ADS)

Gounhalli, Shivraj G.; Shantappa, Anil; Hanagodimath, S. M.

2013-04-01

Effective atomic numbers for photon energy absorption ZPEA,eff, photon interaction ZPI,eff and for electron density Nel, have been calculated by a direct method in the photon-energy region from 1 keV to 20 MeV for narcotic drugs, such as Heroin (H), Cocaine (CO), Caffeine (CA), Tetrahydrocannabinol (THC), Cannabinol (CBD), Tetrahydrocannabivarin (THCV). The ZPEA,eff, ZPI,eff and Nel values have been found to change with energy and composition of the narcotic drugs. The energy dependence ZPEA,eff, ZPI,eff and Nel is shown graphically. The maximum difference between the values of ZPEA,eff, and ZPI,eff occurs at 30 keV and the significant difference of 2 to 33% for the energy region 5-100 keV for all drugs. The reason for these differences is discussed.

Structure and Electronic Properties of Neutral and Negatively Charged RhBn Clusters (n = 3-10): A Density Functional Theory Study.

PubMed

Li, Peifang; Mei, Tingting; Lv, Linxia; Lu, Cheng; Wang, Weihua; Bao, Gang; Gutsev, Gennady L

2017-08-31

The geometrical structure and electronic properties of the neutral RhB n and singly negatively charged RhB n - clusters are obtained in the range of 3 ≤ n ≤ 10 using the unbiased CALYPSO structure search method and density functional theory (DFT). A combination of the PBE0 functional and the def2-TZVP basis set is used for determining global minima on potential energy surfaces of the Rh-doped B n clusters. The photoelectron spectra of the anions are simulated using the time-dependent density functional theory (TD-DFT) method. Good agreement between our simulated and experimentally obtained photoelectron spectra for RhB 9 - provides support to the validity of our theoretical method. The relative stabilities of the ground-state RhB n and RhB n - clusters are estimated using the calculated binding energies, second-order total energy differences, and HOMO-LUMO gaps. It is found that RhB 7 and RhB 8 - are the most stable species in the neutral and anionic series, respectively. The chemical bonding analysis reveals that the RhB 8 - cluster possesses two sets of delocalized σ and π bonds. In both cases, the Hückel 4N + 2 rule is fulfilled and this cluster possesses both σ and π aromaticities.

All-solid state symmetric supercapacitors based on compressible and flexible free-standing 3D carbon nanotubes (CNTs)/poly(3,4-ethylenedioxythiophene) (PEDOT) sponge electrodes

NASA Astrophysics Data System (ADS)

He, Xin; Yang, Wenyao; Mao, Xiling; Xu, Lu; Zhou, Yujiu; Chen, Yan; Zhao, Yuetao; Yang, Yajie; Xu, Jianhua

2018-02-01

Flexible supercapacitors that maintain electrochemical performance under deformation have attracted much attention for the potential application in the flexible electronics market. A compressible and flexible free-standing electrodes sponge and all-solid-state symmetric supercapacitors based on as-prepared electrodes are presented. The carbon nanotubes (CNTs) framework is synthesized by chemical vapor deposition (CVD) method, and then composited with poly (3,4-ethylenedioxythiophene) PEDOT by the electrodeposition. This CNTs/PEDOT sponge electrode shows highest mass-specific capacitance of 147 Fg-1 at 0.5 A g-1, tuned by the PEDOT mass loading, and exhibits good cyclic stability with the evidence that more than 95% of capacitance is remained after 3000 cycles. Furthermore, the symmetric supercapacitor shows the highest energy density of 12.6 Wh kg-1 under the power density of 1 kW kg-1 and highest power density of 10.2 kW kg-1 with energy density of 8 Wh kg-1, which exhibits both high energy density and power density. The electrochemical performance of composite electrode also indicates that the operate voltage of device could be extend to 1.4 V by the n-doping and p-doping process in different potential of PEDOT component. This flexible supercapacitor maintains stable electrochemical performance working on different bending condition, which shows promising prospect for wearable energy storage applications.

Light-front representation of chiral dynamics in peripheral transverse densities

DOE PAGES

Granados, Carlos G.; Weiss, Christian

2015-07-31

The nucleon's electromagnetic form factors are expressed in terms of the transverse densities of charge and magnetization at fixed light-front time. At peripheral transverse distances b = O(M_pi^{-1}) the densities are governed by chiral dynamics and can be calculated model-independently using chiral effective field theory (EFT). We represent the leading-order chiral EFT results for the peripheral transverse densities as overlap integrals of chiral light-front wave functions, describing the transition of the initial nucleon to soft pion-nucleon intermediate states and back. The new representation (a) explains the parametric order of the peripheral transverse densities; (b) establishes an inequality between the spin-independentmore » and -dependent densities; (c) exposes the role of pion orbital angular momentum in chiral dynamics; (d) reveals a large left-right asymmetry of the current in a transversely polarized nucleon and suggests a simple interpretation. The light-front representation enables a first-quantized, quantum-mechanical view of chiral dynamics that is fully relativistic and exactly equivalent to the second-quantized, field-theoretical formulation. It relates the charge and magnetization densities measured in low-energy elastic scattering to the generalized parton distributions probed in peripheral high-energy scattering processes. The method can be applied to nucleon form factors of other operators, e.g. the energy-momentum tensor.« less

SC-CO2-assisted process for a high energy density aerogel supercapacitor: the effect of GO loading

NASA Astrophysics Data System (ADS)

Sarno, Maria; Baldino, Lucia; Scudieri, Carmela; Cardea, Stefano; Ciambelli, Paolo; Reverchon, Ernesto

2017-05-01

Energy density, safety, and simple and environmentally friendly preparation methods are very significant aspects in the realization of a compact supercapacitor. Herein we report the use of a supercritical CO2-assisted gel drying process (SC-CO2) for the preparation of porous electrodes containing dispersed graphene in a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) binder membrane to sandwich in a new portable supercapacitor based on graphene oxide (GO). A GO loading of 60 wt.% was found to give the best combination of factors (porosity, wettability, mechanical and electrochemical properties). Cycling voltammetry and charge/discharge studies showed an excellent capacitance behaviour and stability in an ionic liquid electrolyte, suggesting SC-CO2 processing as a promising platform to produce highly bulky and porous films for supercapacitors. The supercapacitor device delivers a very high energy density of 79.2 Wh kg-1 at a power density of 0.23 KW kg-1 (current density 0.5 A g-1, specific capacitance 36.2 F g-1) while that of steel remains at 50.3 Wh kg-1 at a power density of 2.8 KW kg-1 (current density 6 A g-1, specific capacitance 23.5 F g-1).

SC-CO2-assisted process for a high energy density aerogel supercapacitor: the effect of GO loading.

PubMed

Sarno, Maria; Baldino, Lucia; Scudieri, Carmela; Cardea, Stefano; Ciambelli, Paolo; Reverchon, Ernesto

2017-05-19

Energy density, safety, and simple and environmentally friendly preparation methods are very significant aspects in the realization of a compact supercapacitor. Herein we report the use of a supercritical CO 2 -assisted gel drying process (SC-CO 2 ) for the preparation of porous electrodes containing dispersed graphene in a poly(vinylidene fluoride-co-hexafluoropropylene) (PVDF-HFP) binder membrane to sandwich in a new portable supercapacitor based on graphene oxide (GO). A GO loading of 60 wt.% was found to give the best combination of factors (porosity, wettability, mechanical and electrochemical properties). Cycling voltammetry and charge/discharge studies showed an excellent capacitance behaviour and stability in an ionic liquid electrolyte, suggesting SC-CO 2 processing as a promising platform to produce highly bulky and porous films for supercapacitors. The supercapacitor device delivers a very high energy density of 79.2 Wh kg -1 at a power density of 0.23 KW kg -1 (current density 0.5 A g -1 , specific capacitance 36.2 F g -1 ) while that of steel remains at 50.3 Wh kg -1 at a power density of 2.8 KW kg -1 (current density 6 A g -1 , specific capacitance 23.5 F g -1 ).

Modern Possibilities for Calculating Some Properties of Molecules and Crystals from the Experimental Electron Density

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stash, A.I.; Tsirelson, V.G.

2005-03-01

Methods for calculating some properties of molecules and crystals from the electron density reconstructed from a precise X-ray diffraction experiment using the multipole model are considered. These properties include, on the one hand, the characteristics of the electron density and the inner-crystal electrostatic field and, on the other hand, the local electronic energies (kinetic, potential, total), the exchange energy density, the electron-pair localization function, the localized-orbital locator, the effective crystal potential, and others. It is shown that the integration of these characteristics over pseudoatomic volumes bounded by the surfaces of the zero flux of the electron density gradient makes itmore » possible to characterize directly from an experiment the properties of molecules and crystals in terms of the atomic contributions. The computer program WinXPRO2004, realizing these possibilities, is briefly described.« less

Isochoric Heating of Solid-Density Matter with an Ultrafast Proton Beam

DOE Office of Scientific and Technical Information (OSTI.GOV)

Key, M H; Mackinnon, A J; Patel, P K

A new technique is described for the isochoric heating (i.e., heating at constant volume) of matter to high energy-density plasma states (>10{sup 5} J/g) on a picosecond timescale (10{sup -12} sec). An intense, collimated, ultrashort-pulse beam of protons--generated by a high-intensity laser pulse--is used to isochorically heat a solid density material to a temperature of several eV. The duration of heating is shorter than the timescale for significant hydrodynamic expansion to occur, hence the material is heated to a solid density warm dense plasma state. Using spherically-shaped laser targets a focused proton beam is produced and used to heat amore » smaller volume to over 20 eV. The technique described of ultrafast proton heating provides a unique method for creating isochorically heated high-energy density plasma states.« less

Continuum Level Density of a Coupled-Channel System in the Complex Scaling Method

NASA Astrophysics Data System (ADS)

Suzuki, R.; Kruppa, A. T.; Giraud, B. G.; Katō, K.

2008-06-01

We study the continuum level density (CLD) in the formalism of the complex scaling method (CSM) for coupled-channel systems. We apply the formalism to the ^{4}He = [^{3}H + p] + [^3{He} + n] coupled-channel cluster model where there are resonances at low energy. Numerical calculations of the CLD in the CSM with a finite number of L^{2} basis functions are consistent with the exact result calculated from the S-matrix by solving coupled-channel equations. We also study channel densities. In this framework, the extended completeness relation (ECR) plays an important role.

Squeeze strengthening of magnetorheological fluids using mixed mode operation

NASA Astrophysics Data System (ADS)

Becnel, A. C.; Sherman, S. G.; Hu, W.; Wereley, N. M.

2015-05-01

This research details a novel method of increasing the shear yield stress of magnetorheological fluids by combining shear and squeeze modes of operation to manipulate particle chain structures, so-called squeeze strengthening. Using a custom built Searle cell magnetorheometer, which is a model device emulating a rotary magnetorheological energy absorber (MREA), the contribution of squeeze strengthening to the total controllable yield force is experimentally investigated. Using an eccentric rotating inner cylinder, characterization data from large (1 mm) and small (0.25 mm) nominal gap geometries are compared to investigate the squeeze strengthening effect. Details of the experimental setup and method are presented, and a hybrid model is used to explain experimental trends. This study demonstrates that it is feasible, utilizing squeeze strengthening to increase yield stress, to either (1) design a rotary MREA of a given volume to achieve higher energy absorption density (energy absorbed normalized by active fluid volume), or (2) reduce the volume of a given rotary MREA to achieve the same energy absorption density.

High power density yeast catalyzed microbial fuel cells

NASA Astrophysics Data System (ADS)

Ganguli, Rahul

Microbial fuel cells leverage whole cell biocatalysis to convert the energy stored in energy-rich renewable biomolecules such as sugar, directly to electrical energy at high efficiencies. Advantages of the process include ambient temperature operation, operation in natural streams such as wastewater without the need to clean electrodes, minimal balance-of-plant requirements compared to conventional fuel cells, and environmentally friendly operation. These make the technology very attractive as portable power sources and waste-to-energy converters. The principal problem facing the technology is the low power densities compared to other conventional portable power sources such as batteries and traditional fuel cells. In this work we examined the yeast catalyzed microbial fuel cell and developed methods to increase the power density from such fuel cells. A combination of cyclic voltammetry and optical absorption measurements were used to establish significant adsorption of electron mediators by the microbes. Mediator adsorption was demonstrated to be an important limitation in achieving high power densities in yeast-catalyzed microbial fuel cells. Specifically, the power densities are low for the length of time mediator adsorption continues to occur. Once the mediator adsorption stops, the power densities increase. Rotating disk chronoamperometry was used to extract reaction rate information, and a simple kinetic expression was developed for the current observed in the anodic half-cell. Since the rate expression showed that the current was directly related to microbe concentration close to the electrode, methods to increase cell mass attached to the anode was investigated. Electrically biased electrodes were demonstrated to develop biofilm-like layers of the Baker's yeast with a high concentration of cells directly connected to the electrode. The increased cell mass did increase the power density 2 times compared to a non biofilm fuel cell, but the power density increase was shown to quickly saturate with cell mass attached on the electrode. Based on recent modelling data that suggested that the electrode currents might be limited by the poor electrical conductivity of the anode, the power density versus electrical conductivity of a yeast-immobilized anode was investigated. Introduction of high aspect ratio carbon fiber filaments to the immobilization matrix increased the electrical conductivity of the anode. Although a higher electrical conductivity clearly led to an increase in power densities, it was shown that the principal limitation to power density increase was coming from proton transfer limitations in the immobilized anode. Partial overcoming of the gradients lead a power density of ca. 250 microW cm-2, which is the highest reported for yeast powered MFCs. A yeast-catalyzed microbial fuel cell was investigated as a power source for low power sensors using raw tree sap. It was shown that yeast can efficiently utilize the sucrose present in the raw tree sap to produce electricity when excess salt is added to the medium. Therefore the salinity of a potential energy source is an important consideration when MFCs are being considered for energy harvesting from natural sources.

Solutions of the two-dimensional Hubbard model: Benchmarks and results from a wide range of numerical algorithms

DOE PAGES

LeBlanc, J. P. F.; Antipov, Andrey E.; Becca, Federico; ...

2015-12-14

Numerical results for ground-state and excited-state properties (energies, double occupancies, and Matsubara-axis self-energies) of the single-orbital Hubbard model on a two-dimensional square lattice are presented, in order to provide an assessment of our ability to compute accurate results in the thermodynamic limit. Many methods are employed, including auxiliary-field quantum Monte Carlo, bare and bold-line diagrammatic Monte Carlo, method of dual fermions, density matrix embedding theory, density matrix renormalization group, dynamical cluster approximation, diffusion Monte Carlo within a fixed-node approximation, unrestricted coupled cluster theory, and multireference projected Hartree-Fock methods. Comparison of results obtained by different methods allows for the identification ofmore » uncertainties and systematic errors. The importance of extrapolation to converged thermodynamic-limit values is emphasized. Furthermore, cases where agreement between different methods is obtained establish benchmark results that may be useful in the validation of new approaches and the improvement of existing methods.« less

Transport properties in mixtures involving carbon dioxide at low and moderate density: test of several intermolecular potential energies and comparison with experiment

NASA Astrophysics Data System (ADS)

Moghadasi, Jalil; Yousefi, Fakhri; Papari, Mohammad Mehdi; Faghihi, Mohammad Ali; Mohsenipour, Ali Asghar

2009-09-01

It is the purpose of this paper to extract unlike intermolecular potential energies of five carbon dioxide-based binary gas mixtures including CO2-He, CO2-Ne, CO2-Ar, CO2-Kr, and CO2-Xe from viscosity data and compare the calculated potentials with other models potential energy reported in literature. Then, dilute transport properties consisting of viscosity, diffusion coefficient, thermal diffusion factor, and thermal conductivity of aforementioned mixtures are calculated from the calculated potential energies and compared with literature data. Rather accurate correlations for the viscosity coefficient of afore-cited mixtures embracing the temperature range 200 K < T < 3273.15 K is reproduced from the present unlike intermolecular potentials energy. Our estimated accuracies for the viscosity are to within ±2%. In addition, the calculated potential energies are used to present smooth correlations for other transport properties. The accuracies of the binary diffusion coefficients are of the order of ±3%. Finally, the unlike interaction energy and the calculated low density viscosity have been employed to calculate high density viscosities using Vesovic-Wakeham method.

Density Functional Methods for Shock Physics and High Energy Density Science

NASA Astrophysics Data System (ADS)

Desjarlais, Michael

2017-06-01

Molecular dynamics with density functional theory has emerged over the last two decades as a powerful and accurate framework for calculating thermodynamic and transport properties with broad application to dynamic compression, high energy density science, and warm dense matter. These calculations have been extensively validated against shock and ramp wave experiments, are a principal component of high-fidelity equation of state generation, and are having wide-ranging impacts on inertial confinement fusion, planetary science, and shock physics research. In addition to thermodynamic properties, phase boundaries, and the equation of state, one also has access to electrical conductivity, thermal conductivity, and lower energy optical properties. Importantly, all these properties are obtained within the same theoretical framework and are manifestly consistent. In this talk I will give a brief history and overview of molecular dynamics with density functional theory and its use in calculating a wide variety of thermodynamic and transport properties for materials ranging from ambient to extreme conditions and with comparisons to experimental data. I will also discuss some of the limitations and difficulties, as well as active research areas. Sandia is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

Effects of ultrasound energy density on the non-thermal pasteurization of chocolate milk beverage.

PubMed

Monteiro, Sara H M C; Silva, Eric Keven; Alvarenga, Verônica O; Moraes, Jeremias; Freitas, Mônica Q; Silva, Márcia C; Raices, Renata S L; Sant'Ana, Anderson S; Meireles, M Angela A; Cruz, Adriano G

2018-04-01

This study presents the emerging high-intensity ultrasound (HIUS) processing as a non-thermal alternative to high-temperature short-time pasteurization (HTST). Chocolate milk beverage (CMB) was subjected to different ultrasound energy densities (0.3-3.0 kJ/cm 3 ), as compared to HTST pasteurization (72 °C/15 s) aimed to verify the effect of the HIUS processing on the microbiological and physicochemical characteristics of the beverage. The application of HIUS at an energy density of 3.0 kJ/cm 3 was able to reduce 3.56 ± 0.02 logarithmic cycles in the total aerobic counts. In addition, the ultrasound energy density affected the physical properties of the beverage as the size distribution of fat globule and rheological behavior, as well as the chemical properties such as antioxidant activity, ACE inhibitory activity, fatty acid profile, and volatile profile. In general, the different energetic densities used as a non-thermal method of pasteurization of CMB were more effective when compared to the conventional pasteurization by HTST, since they improved the microbiological and physicochemical quality, besides preserving the bioactive compounds and the nutritional quality of the product. Copyright © 2017 Elsevier B.V. All rights reserved.

Chapman Enskog-maximum entropy method on time-dependent neutron transport equation

NASA Astrophysics Data System (ADS)

Abdou, M. A.

2006-09-01

The time-dependent neutron transport equation in semi and infinite medium with linear anisotropic and Rayleigh scattering is proposed. The problem is solved by means of the flux-limited, Chapman Enskog-maximum entropy for obtaining the solution of the time-dependent neutron transport. The solution gives the neutron distribution density function which is used to compute numerically the radiant energy density E(x,t), net flux F(x,t) and reflectivity Rf. The behaviour of the approximate flux-limited maximum entropy neutron density function are compared with those found by other theories. Numerical calculations for the radiant energy, net flux and reflectivity of the proposed medium are calculated at different time and space.

Quantification of breast density with dual energy mammography: A simulation study

PubMed Central

Ducote, Justin L.; Molloi, Sabee

2008-01-01

Breast density, the percentage of glandular breast tissue, has been identified as an important yet underutilized risk factor in the development of breast cancer. A quantitative method to measure breast density with dual energy imaging was investigated using a computer simulation model. Two configurations to measure breast density were evaluated: the usage of monoenergetic beams and an ideal detector, and the usage of polyenergetic beams with spectra from a tungsten anode x-ray tube with a detector modeled after a digital mammography system. The simulation model calculated the mean glandular dose necessary to quantify the variability of breast density to within 1∕3%. The breast was modeled as a semicircle 10 cm in radius with equal homogenous thicknesses of adipose and glandular tissues. Breast thicknesses were considered in the range of 2–10 cm and energies in the range of 10–150 keV for the two monoenergetic beams, and 20–150 kVp for spectra with a tungsten anode x-ray tube. For a 4.2 cm breast thickness, the required mean glandular doses were 0.183 μGy for two monoenergetic beams at 19 and 71 keV, and 9.85 μGy for two polyenergetic spectra from a tungsten anode at 32 and 96 kVp with beam filtrations of 50 μm Rh and 300 μm Cu for the low and high energy beams, respectively. The results suggest that for either configuration, breast density can be precisely measured with dual energy imaging requiring only a small amount of additional dose to the breast. The possibility of using a standard screening mammogram as the low energy image is also discussed. PMID:19175100

ERP Energy and Cognitive Activity Correlates

NASA Astrophysics Data System (ADS)

Schillaci, Michael Jay; Vendemia, Jennifer M. C.

2014-03-01

We propose a novel analysis approach for high-density event related scalp potential (ERP) data where the integrated channel-power is used to attain an energy density functional state for channel-clusters of neurophysiological significance. The method is applied to data recorded during a two-stimulus, directed lie paradigm and shows that deceptive responses emit between 8% and 10% less power. A time course analysis of these cognitive activity measures over posterior and anterior regions of the cortex suggests that neocortical interactions, reflecting the differing workload demands during executive and semantic processes, take about 50% longer for the case of deception. These results suggest that the proposed method may provide a useful tool for the analysis of ERP correlates of high-order cognitive functioning. We also report on a possible equivalence between the energy functional distribution and near-infrared signatures that have been measured with other modalities.

Globally optimal superconducting magnets part II: symmetric MSE coil arrangement.

PubMed

Tieng, Quang M; Vegh, Viktor; Brereton, Ian M

2009-01-01

A globally optimal superconducting magnet coil design procedure based on the Minimum Stored Energy (MSE) current density map is outlined. The method has the ability to arrange coils in a manner that generates a strong and homogeneous axial magnetic field over a predefined region, and ensures the stray field external to the assembly and peak magnetic field at the wires are in acceptable ranges. The outlined strategy of allocating coils within a given domain suggests that coils should be placed around the perimeter of the domain with adjacent coils possessing alternating winding directions for optimum performance. The underlying current density maps from which the coils themselves are derived are unique, and optimized to possess minimal stored energy. Therefore, the method produces magnet designs with the lowest possible overall stored energy. Optimal coil layouts are provided for unshielded and shielded short bore symmetric superconducting magnets.

Molecular Excitation Energies from Time-Dependent Density Functional Theory Employing Random-Phase Approximation Hessians with Exact Exchange.

PubMed

Heßelmann, Andreas

2015-04-14

Molecular excitation energies have been calculated with time-dependent density-functional theory (TDDFT) using random-phase approximation Hessians augmented with exact exchange contributions in various orders. It has been observed that this approach yields fairly accurate local valence excitations if combined with accurate asymptotically corrected exchange-correlation potentials used in the ground-state Kohn-Sham calculations. The inclusion of long-range particle-particle with hole-hole interactions in the kernel leads to errors of 0.14 eV only for the lowest excitations of a selection of three alkene, three carbonyl, and five azabenzene molecules, thus surpassing the accuracy of a number of common TDDFT and even some wave function correlation methods. In the case of long-range charge-transfer excitations, the method typically underestimates accurate reference excitation energies by 8% on average, which is better than with standard hybrid-GGA functionals but worse compared to range-separated functional approximations.

The instantaneous frequency rate spectrogram

NASA Astrophysics Data System (ADS)

Czarnecki, Krzysztof

2016-01-01

An accelerogram of the instantaneous phase of signal components referred to as an instantaneous frequency rate spectrogram (IFRS) is presented as a joint time-frequency distribution. The distribution is directly obtained by processing the short-time Fourier transform (STFT) locally. A novel approach to amplitude demodulation based upon the reassignment method is introduced as a useful by-product. Additionally, an estimator of energy density versus the instantaneous frequency rate (IFR) is proposed and referred to as the IFR profile. The energy density is estimated based upon both the classical energy spectrogram and the IFRS smoothened by the median filter. Moreover, the impact of an analyzing window width, additive white Gaussian noise and observation time is tested. Finally, the introduced method is used for the analysis of the acoustic emission of an automotive engine. The recording of the engine of a Lamborghini Gallardo is analyzed as an example.

Energy density of bloaters in the upper Great Lakes

USGS Publications Warehouse

Pothoven, Steven A.; Bunnell, David B.; Madenjian, Charles P.; Gorman, Owen T.; Roseman, Edward F.

2012-01-01

We evaluated the energy density of bloaters Coregonus hoyi as a function of fish size across Lakes Michigan, Huron, and Superior in 2008–2009 and assessed how differences in energy density are related to factors such as biomass density of bloaters and availability of prey. Additional objectives were to compare energy density between sexes and to compare energy densities of bloaters in Lake Michigan between two time periods (1998–2001 and 2008–2009). For the cross-lake comparisons in 2008, energy density increased with fish total length (TL) only in Lake Michigan. Mean energy density adjusted for fish size was 8% higher in bloaters from Lake Superior than in bloaters from Lake Huron. Relative to fish in these two lakes, small (175 mm TL) bloaters had higher energy density. In 2009, energy density increased with bloater size, and mean energy density adjusted for fish size was about 9% higher in Lake Michigan than in Lake Huron (Lake Superior was not sampled during 2009). Energy density of bloaters in Lake Huron was generally the lowest among lakes, reflecting the relatively low densities of opossum shrimp Mysis diluviana and the relatively high biomass of bloaters reported for that lake. Other factors, such as energy content of prey, growing season, or ontogenetic differences in energy use strategies, may also influence cross-lake variation in energy density. Mean energy density adjusted for length was 7% higher for female bloaters than for male bloaters in Lakes Michigan and Huron. In Lake Superior, energy density did not differ between males and females. Finally, energy density of bloaters in Lake Michigan was similar between the periods 2008–2009 and 1998–2001, possibly due to a low population abundance of bloaters, which could offset food availability changes linked to the loss of prey such as the amphipods Diporeia spp.

Ab-initio study on electronic properties of rocksalt SnAs

NASA Astrophysics Data System (ADS)

Babariya, Bindiya; Vaghela, M. V.; Gajjar, P. N.

2018-05-01

Within the frame work of Local Density Approximation of Exchange and Correlation, ab-initio method of density functional theory with Abinit code is used to compute electronic energy band structure, density of States and charge density of SnAs in rocksalt phase. Our result after optimization for lattice constant agrees with experimental value within 0.59% deviation. The computed electronic energy bands in high symmetry directions Γ→K→X→Γ→L→X→W→L→U shown metallic nature. The lowest band in the electronic band structure is showing band-gap approximately 1.70 eV from next higher band and no crossing between lowest two bands are seen. The density of states revels p-p orbit hybridization between Sn and As atoms. The spherical contour around Sn and As in the charge density plot represent partly ionic and partly covalent bonding. Fermi surface topology is the resultant effect of the single band crossing along L direction at Ef.

Study of local currents in low dimension materials using complex injecting potentials

NASA Astrophysics Data System (ADS)

He, Shenglai; Covington, Cody; Varga, Kálmán

2018-04-01

A complex potential is constructed to inject electrons into the conduction band, mimicking electron currents in nanoscale systems. The injected electrons are time propagated until a steady state is reached. The local current density can then be calculated to show the path of the conducting electrons on an atomistic level. The method allows for the calculation of the current density vectors within the medium as a function of energy of the conducting electron. Using this method, we investigate the electron pathway of graphene nanoribbons in various structures, molecular junctions, and black phosphorus nanoribbons. By analyzing the current flow through the structures, we find strong dependence on the structural geometry and the energy of the injected electrons. This method may be of general use in the study of nano-electronic materials and interfaces.

Electron-Ion Dynamics with Time-Dependent Density Functional Theory: Towards Predictive Solar Cell Modeling: Final Technical Report

DOE Office of Scientific and Technical Information (OSTI.GOV)

Maitra, Neepa

2016-07-14

This project investigates the accuracy of currently-used functionals in time-dependent density functional theory, which is today routinely used to predict and design materials and computationally model processes in solar energy conversion. The rigorously-based electron-ion dynamics method developed here sheds light on traditional methods and overcomes challenges those methods have. The fundamental research undertaken here is important for building reliable and practical methods for materials discovery. The ultimate goal is to use these tools for the computational design of new materials for solar cell devices of high efficiency.

Density functional Gaussian-type-orbital approach to theoretical study of nitric oxide dimers

DOE Office of Scientific and Technical Information (OSTI.GOV)

Jursic, B.S.; Zdravkovski, Z.

Structure and total energies of the cis NO dimer, the trans NO dimer, and the NO monomer were calculated by ab initio methods (UHF, UMP2, and MP3) and density functional theory methods (LSDA and BLYP) with different basis sets [from 3-21G* to 6-311++(3df,3pd)]. The system is especially hard to model because two NO molecules are weakly associated in a dimer that has very long N-N bond. The results obtained by different methods are compared and the necessity of correlational methods for studying these systems is discussed.

Direct Density Functional Energy Minimization using an Tetrahedral Finite Element Grid

NASA Astrophysics Data System (ADS)

Vaught, A.; Schmidt, K. E.; Chizmeshya, A. V. G.

1998-03-01

We describe an O(N) (N proportional to volume) technique for solving electronic structure problems using the finite element method (FEM). A real--space tetrahedral grid is used as a basis to represent the electronic density, of a free or periodic system and Poisson's equation is solved as a boundary value problem. Nuclear cusps are treated using a local grid consisting of radial elements. These features facilitate the implementation of complicated energy functionals and permit a direct (constrained) energy minimization with respect to the density. We demonstrate the usefulness of the scheme by calculating the binding trends and polarizabilities of a number of atoms and molecules using a number of recently proposed non--local, orbital--free kinetic energy functionals^1,2. Scaling behavior, computational efficiency and the generalization to band--structure will also be discussed. indent 0 pt øbeylines øbeyspaces skip 0 pt ^1 P. Garcia-Gonzalez, J.E. Alvarellos and E. Chacon, Phys. Rev. B 54, 1897 (1996). ^2 A. J. Thakkar, Phys.Rev.B 46, 6920 (1992).

One-step electroplating porous graphene oxide electrodes of supercapacitors for ultrahigh capacitance and energy density.

PubMed

Wang, Yongjie; Zhu, Jiaqi

2015-02-06

An electroplating method was used for the first time to synthesize 3D porous graphene oxide (PGO) architectures, exhibiting ultrahigh capacitance and energy density as electrodes of supercapacitors. Scanning electron microscopy illustrated the porous structures which promoted the stability and alleviated the stacking of the graphene oxide layers. As investigated in a three-electrode supercapacitor cell, PGO electrodes exhibited the maximum capacitance and energy of 973 F · g(-1) and 98.4 Wh · Kg(-1), which are better than current reports and comparable to batteries. At 4 A · g(-1) for high-power applications, PGO electrodes reached a capacitance, energy, and power density of 493 F · g(-1), 49.9 Wh · Kg(-1), and 1700 W · Kg(-1), and they retained ∼97.83% of capacitance after 10 000 charge/discharge processes. Furthermore, when the PGO was bent exaggeratedly, it still displayed identical properties, which is of important significance for supporting wearable devices.

Density-matrix based determination of low-energy model Hamiltonians from ab initio wavefunctions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Changlani, Hitesh J.; Zheng, Huihuo; Wagner, Lucas K.

2015-09-14

We propose a way of obtaining effective low energy Hubbard-like model Hamiltonians from ab initio quantum Monte Carlo calculations for molecular and extended systems. The Hamiltonian parameters are fit to best match the ab initio two-body density matrices and energies of the ground and excited states, and thus we refer to the method as ab initio density matrix based downfolding. For benzene (a finite system), we find good agreement with experimentally available energy gaps without using any experimental inputs. For graphene, a two dimensional solid (extended system) with periodic boundary conditions, we find the effective on-site Hubbard U{sup ∗}/t tomore » be 1.3 ± 0.2, comparable to a recent estimate based on the constrained random phase approximation. For molecules, such parameterizations enable calculation of excited states that are usually not accessible within ground state approaches. For solids, the effective Hamiltonian enables large-scale calculations using techniques designed for lattice models.« less

Density Measurement for MORB Melts by X-ray Absorption Method

NASA Astrophysics Data System (ADS)

Sakamaki, T.; Urakawa, S.; Suzuki, A.; Ohtani, E.; Katayama, Y.

2006-12-01

Density of silicate melts at high pressure is one of the most important properties to understand magma migration in the planetary interior and the differentiation of the terrestrial planets. The density measurements of silicate melts have been carried out by several methods (shock compression experiments and sink-float method in static experiments, etc.). However, since these methods have difficulties in acquisition of data at a desired pressure and temperature, the density of the silicate melt have been measured under only a few conditions. Recently a new density measurement was developed by the X-ray absorption method. Advantage of this method is to measure density of liquids at a desired pressure and temperature. In the present study we measured the density of MORB melt by X-ray absorption method. Experiments were carried out at the BL22XU beamline at SPring-8. A DIA-type cubic anvil apparatus was used for generation of high pressure and temperature. We used tungsten carbide anvils with the top anvil sizes of 6 mm and 4 mm. The energy of monochromateized X-ray beam was 23 keV. The intensities of incident and transmitted X-ray were measured by ion chambers. The density of the melt was calculated on the basis of Beer-Lambert law. The starting material was a glass with the MORB composition. Experiments were made from 1 atm to 5 GPa, from 300 to 2000 K. We compared the density of MORB melt with the compression curve of the melt in previous works. The density measured by this study is lower than that expected from the compression curve determined at higher pressures by the sink-float method. Structural change of the MORB melt with increasing pressure might be attributed to this discrepancy.

Density Measurement for MORB Melts by X-ray Absorption Method

NASA Astrophysics Data System (ADS)

Sakamaki, T.; Urakawa, S.; Ohtani, E.; Suzuki, A.; Katayama, Y.

2005-12-01

Density of silicate melts at high pressure is one of the most important properties to understand magma migration in the planetary interior and the differentiation of the terrestrial planets. The density measurements of silicate melts have been carried out by several methods (shock compression experiments and sink-float method in static experiments, etc.). However, since these methods have difficulties in acquisition of data at a desired pressure and temperature, the density of the silicate melt have been measured under only a few conditions. Recently a new density measurement was developed by the X-ray absorption method. Advantage of this method is to measure density of liquids at a desired pressure and temperature. In the present study we measured the density of MORB melt by X-ray absorption method. Experiments were carried out at the BL22XU beamline at SPring-8. A DIA-type cubic anvil apparatus was used for generation of high pressure and temperature. We used tungsten carbide anvils with the edge-length of 6 mm. The energy of monochromateized X-ray beam was 23 keV. The intensities of incident and transmitted X-ray were measured by ion chambers. The density of the melt was calculated on the basis of Beer-Lambert law. The starting material was a glass with the MORB composition. Experiments were made from 1 atm to 4 GPa, from 300 to 2200 K. We compared the density of MORB melt with the compression curve of the melt in previous works. The density measured by this study is lower than that expected from the compression curve determined at higher pressures by the sink-float method. Structural change of the MORB melt with increasing pressure might be attributed to this discrepancy.

Multiple-energy Techniques in Industrial Computerized Tomography

DOE R&D Accomplishments Database

Schneberk, D.; Martz, H.; Azevedo, S.

1990-08-01

Considerable effort is being applied to develop multiple-energy industrial CT techniques for materials characterization. Multiple-energy CT can provide reliable estimates of effective Z (Z{sub eff}), weight fraction, and rigorous calculations of absolute density, all at the spatial resolution of the scanner. Currently, a wide variety of techniques exist for CT scanners, but each has certain problems and limitations. Ultimately, the best multi-energy CT technique would combine the qualities of accuracy, reliability, and wide range of application, and would require the smallest number of additional measurements. We have developed techniques for calculating material properties of industrial objects that differ somewhat from currently used methods. In this paper, we present our methods for calculating Z{sub eff}, weight fraction, and density. We begin with the simplest case -- methods for multiple-energy CT using isotopic sources -- and proceed to multiple-energy work with x-ray machine sources. The methods discussed here are illustrated on CT scans of PBX-9502 high explosives, a lexan-aluminum phantom, and a cylinder of glass beads used in a preliminary study to determine if CT can resolve three phases: air, water, and a high-Z oil. In the CT project at LLNL, we have constructed several CT scanners of varying scanning geometries using {gamma}- and x-ray sources. In our research, we employed two of these scanners: pencil-beam CAT for CT data using isotopic sources and video-CAT equipped with an IRT micro-focal x-ray machine source.

Solution synthesis of metal oxides for electrochemical energy storage applications.

PubMed

Xia, Xinhui; Zhang, Yongqi; Chao, Dongliang; Guan, Cao; Zhang, Yijun; Li, Lu; Ge, Xiang; Bacho, Ignacio Mínguez; Tu, Jiangping; Fan, Hong Jin

2014-05-21

This article provides an overview of solution-based methods for the controllable synthesis of metal oxides and their applications for electrochemical energy storage. Typical solution synthesis strategies are summarized and the detailed chemical reactions are elaborated for several common nanostructured transition metal oxides and their composites. The merits and demerits of these synthesis methods and some important considerations are discussed in association with their electrochemical performance. We also propose the basic guideline for designing advanced nanostructure electrode materials, and the future research trend in the development of high power and energy density electrochemical energy storage devices.

Method of sintering ceramic materials

DOEpatents

Holcombe, Cressie E.; Dykes, Norman L.

1992-01-01

A method for sintering ceramic materials is described. A ceramic article is coated with layers of protective coatings such as boron nitride, graphite foil, and niobium. The coated ceramic article is embedded in a container containing refractory metal oxide granules and placed within a microwave oven. The ceramic article is heated by microwave energy to a temperature sufficient to sinter the ceramic article to form a densified ceramic article having a density equal to or greater than 90% of theoretical density.

Linear response coupled cluster theory with the polarizable continuum model within the singles approximation for the solvent response.

PubMed

Caricato, Marco

2018-04-07

We report the theory and the implementation of the linear response function of the coupled cluster (CC) with the single and double excitations method combined with the polarizable continuum model of solvation, where the correlation solvent response is approximated with the perturbation theory with energy and singles density (PTES) scheme. The singles name is derived from retaining only the contribution of the CC single excitation amplitudes to the correlation density. We compare the PTES working equations with those of the full-density (PTED) method. We then test the PTES scheme on the evaluation of excitation energies and transition dipoles of solvated molecules, as well as of the isotropic polarizability and specific rotation. Our results show a negligible difference between the PTED and PTES schemes, while the latter affords a significantly reduced computational cost. This scheme is general and can be applied to any solvation model that includes mutual solute-solvent polarization, including explicit models. Therefore, the PTES scheme is a competitive approach to compute response properties of solvated systems using CC methods.

Linear response coupled cluster theory with the polarizable continuum model within the singles approximation for the solvent response

NASA Astrophysics Data System (ADS)

Caricato, Marco

2018-04-01

We report the theory and the implementation of the linear response function of the coupled cluster (CC) with the single and double excitations method combined with the polarizable continuum model of solvation, where the correlation solvent response is approximated with the perturbation theory with energy and singles density (PTES) scheme. The singles name is derived from retaining only the contribution of the CC single excitation amplitudes to the correlation density. We compare the PTES working equations with those of the full-density (PTED) method. We then test the PTES scheme on the evaluation of excitation energies and transition dipoles of solvated molecules, as well as of the isotropic polarizability and specific rotation. Our results show a negligible difference between the PTED and PTES schemes, while the latter affords a significantly reduced computational cost. This scheme is general and can be applied to any solvation model that includes mutual solute-solvent polarization, including explicit models. Therefore, the PTES scheme is a competitive approach to compute response properties of solvated systems using CC methods.

Theoretical investigations on the structures and properties of CL-20/TNT cocrystal and its defective models by molecular dynamics simulation.

PubMed

Hang, Gui-Yun; Yu, Wen-Li; Wang, Tao; Wang, Jin-Tao

2018-06-09

"Perfect" and defective models of CL-20/TNT cocrystal explosive were established. Molecular dynamics methods were introduced to determine the structures and predict the comprehensive performances, including stabilities, sensitivity, energy density and mechanical properties, of the different models. The influences of crystal defects on the properties of these explosives were investigated and evaluated. The results show that, compared with the "perfect" model, the rigidity and toughness of defective models are decreased, while the ductility, tenacity and plastic properties are enhanced. The binding energies, interaction energy of the trigger bond, and the cohesive energy density of defective crystals declined, thus implying that stabilities are weakened, the explosive molecule is activated, trigger bond strength is diminished and safety is worsened. Detonation performance showed that, owing to the influence of crystal defects, the density is lessened, detonation pressure and detonation velocity are also declined, i.e., the power of defective explosive is decreased. In a word, the crystal defects may have a favorable effect on the mechanical properties, but have a disadvantageous influence on sensitivity, stability and energy density of CL-20/TNT cocrystal explosive. The results could provide theoretical guidance and practical instructions to estimate the properties of defective crystal models.

Note: The performance of new density functionals for a recent blind test of non-covalent interactions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Mardirossian, Narbe; Head-Gordon, Martin

Benchmark datasets of non-covalent interactions are essential for assessing the performance of density functionals and other quantum chemistry approaches. In a recent blind test, Taylor et al. benchmarked 14 methods on a new dataset consisting of 10 dimer potential energy curves calculated using coupled cluster with singles, doubles, and perturbative triples (CCSD(T)) at the complete basis set (CBS) limit (80 data points in total). Finally, the dataset is particularly interesting because compressed, near-equilibrium, and stretched regions of the potential energy surface are extensively sampled.

Note: The performance of new density functionals for a recent blind test of non-covalent interactions

DOE PAGES

Mardirossian, Narbe; Head-Gordon, Martin

2016-11-09

Benchmark datasets of non-covalent interactions are essential for assessing the performance of density functionals and other quantum chemistry approaches. In a recent blind test, Taylor et al. benchmarked 14 methods on a new dataset consisting of 10 dimer potential energy curves calculated using coupled cluster with singles, doubles, and perturbative triples (CCSD(T)) at the complete basis set (CBS) limit (80 data points in total). Finally, the dataset is particularly interesting because compressed, near-equilibrium, and stretched regions of the potential energy surface are extensively sampled.

Segmentation-free statistical image reconstruction for polyenergetic x-ray computed tomography with experimental validation.

PubMed

Idris A, Elbakri; Fessler, Jeffrey A

2003-08-07

This paper describes a statistical image reconstruction method for x-ray CT that is based on a physical model that accounts for the polyenergetic x-ray source spectrum and the measurement nonlinearities caused by energy-dependent attenuation. Unlike our earlier work, the proposed algorithm does not require pre-segmentation of the object into the various tissue classes (e.g., bone and soft tissue) and allows mixed pixels. The attenuation coefficient of each voxel is modelled as the product of its unknown density and a weighted sum of energy-dependent mass attenuation coefficients. We formulate a penalized-likelihood function for this polyenergetic model and develop an iterative algorithm for estimating the unknown density of each voxel. Applying this method to simulated x-ray CT measurements of objects containing both bone and soft tissue yields images with significantly reduced beam hardening artefacts relative to conventional beam hardening correction methods. We also apply the method to real data acquired from a phantom containing various concentrations of potassium phosphate solution. The algorithm reconstructs an image with accurate density values for the different concentrations, demonstrating its potential for quantitative CT applications.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wang, Weizhou, E-mail: wzw@lynu.edu.cn, E-mail: ybw@gzu.edu.cn; Zhang, Yu; Sun, Tao

High-level coupled cluster singles, doubles, and perturbative triples [CCSD(T)] computations with up to the aug-cc-pVQZ basis set (1924 basis functions) and various extrapolations toward the complete basis set (CBS) limit are presented for the sandwich, T-shaped, and parallel-displaced benzene⋯naphthalene complex. Using the CCSD(T)/CBS interaction energies as a benchmark, the performance of some newly developed wave function and density functional theory methods has been evaluated. The best performing methods were found to be the dispersion-corrected PBE0 functional (PBE0-D3) and spin-component scaled zeroth-order symmetry-adapted perturbation theory (SCS-SAPT0). The success of SCS-SAPT0 is very encouraging because it provides one method for energy componentmore » analysis of π-stacked complexes with 200 atoms or more. Most newly developed methods do, however, overestimate the interaction energies. The results of energy component analysis show that interaction energies are overestimated mainly due to the overestimation of dispersion energy.« less

Plasma Modification of Graphite Fibers and Its Effect on Composite Properties.

DTIC Science & Technology

1983-08-01

liquids have been difficult to measure with adequate accuracy. As a result, critical surface energy data are not readily available. A flotation method...tension of the fiber surface. However, the fiber density must always exceed the density of the flotation liquid. Although this is a very useful...technioue, it is inanplicable to graphite fiber due to its irregular surface structure, small filament diameter and small difference in density with flotation

Technical note: optimization for improved tube-loading efficiency in the dual-energy computed tomography coupled with balanced filter method.

PubMed

Saito, Masatoshi

2010-08-01

This article describes the spectral optimization of dual-energy computed tomography using balanced filters (bf-DECT) to reduce the tube loadings and dose by dedicating to the acquisition of electron density information, which is essential for treatment planning in radiotherapy. For the spectral optimization of bf-DECT, the author calculated the beam-hardening error and air kerma required to achieve a desired noise level in an electron density image of a 50-cm-diameter cylindrical water phantom. The calculation enables the selection of beam parameters such as tube voltage, balanced filter material, and its thickness. The optimal combination of tube voltages was 80 kV/140 kV in conjunction with Tb/Hf and Bi/Mo filter pairs; this combination agrees with that obtained in a previous study [M. Saito, "Spectral optimization for measuring electron density by the dual-energy computed tomography coupled with balanced filter method," Med. Phys. 36, 3631-3642 (2009)], although the thicknesses of the filters that yielded a minimum tube output were slightly different from those obtained in the previous study. The resultant tube loading of a low-energy scan of the present bf-DECT significantly decreased from 57.5 to 4.5 times that of a high-energy scan for conventional DECT. Furthermore, the air kerma of bf-DECT could be reduced to less than that of conventional DECT, while obtaining the same figure of merit for the measurement of electron density and effective atomic number. The tube-loading and dose efficiencies of bf-DECT were considerably improved by sacrificing the quality of the noise level in the images of effective atomic number.

Post occupancy evaluation of energy-efficient behavior in informal housing of high density area

NASA Astrophysics Data System (ADS)

Aulia, D. N.; Marpaung, B. O. Y.

2018-02-01

The concept of energy-efficient building emphasizes the critical of efficiency in the use of water, electrical energy, and building materials, beginning with design, construction, to the maintenance of the building in the future. This study was conducted to observe the behavior of Energy Saving of the residents in performing everyday activities in the building. The observed variables are the consumption of natural resources (energy, material, water, and land) and the emissions of air, water, and land related to the environment and health. This research is a descriptive qualitative research with the method of data collection is the distribution of questionnaires and observation. The method of analyzing data is posted occupancy evaluation undertaken to obtain patterns of community-based behavior in urban areas. The informal high-density housing area is a typology of population settlements that found in many big cities in Indonesia. This community represents various community groups regarding occupation, education, income, and race. The results of the study concluded that there are five components of energy-saving behavioral formers in housing namely: residential building components, environmental components in occupancy, external occupancy components, components of social activities and elements of business

Absorption and resonance Raman study of the pyromellitic diahydride anion via density functional theory

NASA Astrophysics Data System (ADS)

Andruniow, T.; Pawlikowski, M.

2000-05-01

The electronic structure of the low-energy states of the pyromellitic diahydride (PMDA) anion is investigated in terms of the VWN (Vosco-Wilk-Nusair) the BP (Becke-Perdew) and the B3LYP density functional (DF) methods employed with 6-31G * basis sets. All the methods are shown to reproduce correctly the absorption and resonance Raman spectra in the region corresponding to the low-energy 1 2Au→1 2B3g transition. The discrepancies between the theory and experiment are attributed to a (weak) Dushinsky effect predominately due to a mixing of the ν3=1593 cm -1 and ν4=1342 cm -1 vibrations in the 1 2B3 g state of the PMDA radical.

Conjugate-gradient optimization method for orbital-free density functional calculations.

PubMed

Jiang, Hong; Yang, Weitao

2004-08-01

Orbital-free density functional theory as an extension of traditional Thomas-Fermi theory has attracted a lot of interest in the past decade because of developments in both more accurate kinetic energy functionals and highly efficient numerical methodology. In this paper, we developed a conjugate-gradient method for the numerical solution of spin-dependent extended Thomas-Fermi equation by incorporating techniques previously used in Kohn-Sham calculations. The key ingredient of the method is an approximate line-search scheme and a collective treatment of two spin densities in the case of spin-dependent extended Thomas-Fermi problem. Test calculations for a quartic two-dimensional quantum dot system and a three-dimensional sodium cluster Na216 with a local pseudopotential demonstrate that the method is accurate and efficient. (c) 2004 American Institute of Physics.

Assessing the Accuracy of Density Functional and Semiempirical Wave Function Methods for Water Nanoparticles: Comparing Binding and Relative Energies of (H2O)16 and (H2O)17 to CCSD(T) Results.

PubMed

Leverentz, Hannah R; Qi, Helena W; Truhlar, Donald G

2013-02-12

The binding energies and relative conformational energies of five configurations of the water 16-mer are computed using 61 levels of density functional (DF) theory, 12 methods combining DF theory with molecular mechanics damped dispersion (DF-MM), seven semiempirical-wave function (SWF) methods, and five methods combining SWF theory with molecular mechanics damped dispersion (SWF-MM). The accuracies of the computed energies are assessed by comparing them to recent high-level ab initio results; this assessment is more relevant to bulk water than previous tests on small clusters because a 16-mer is large enough to have water molecules that participate in more than three hydrogen bonds. We find that for water 16-mer binding energies the best DF, DF-MM, SWF, and SWF-MM methods (and their mean unsigned errors in kcal/mol) are respectively M06-2X (1.6), ωB97X-D (2.3), SCC-DFTB-γ(h) (35.2), and PM3-D (3.2). We also mention the good performance of CAM-B3LYP (1.8), M05-2X (1.9), and TPSSLYP (3.0). In contrast, for relative energies of various water nanoparticle 16-mer structures, the best methods (and mean unsigned errors in kcal/mol), in the same order of classes of methods, are SOGGA11-X (0.3), ωB97X-D (0.2), PM6 (0.4), and PMOv1 (0.6). We also mention the good performance of LC-ωPBE-D3 (0.3) and ωB97X (0.4). When both relative and binding energies are taken into consideration, the best methods overall (out of the 85 tested) are M05-2X without molecular mechanics and ωB97X-D when molecular mechanics corrections are included; with considerably higher average errors and considerably lower cost, the best SWF or SWF-MM method is PMOv1. We use six of the best methods for binding energies of the water 16-mers to calculate the binding energies of water hexamers and water 17-mers to test whether these methods are also reliable for binding energy calculations on other types of water clusters.

Density Imaging of Puy de Dôme Volcano by Joint Inversion of Muographic and Gravimetric Data

NASA Astrophysics Data System (ADS)

Barnoud, A.; Niess, V.; Le Ménédeu, E.; Cayol, V.; Carloganu, C.

2016-12-01

We aim at jointly inverting high density muographic and gravimetric data to robustly infer the density structure of volcanoes. We use the puy de Dôme volcano in France as a proof of principle since high quality data sets are available for both muography and gravimetry. Gravimetric inversion and muography are independent methods that provide an estimation of density distributions. On the one hand, gravimetry allows to reconstruct 3D density variations by inversion. This process is well known to be ill-posed and intrinsically non unique, thus it requires additional constraints (eg. a priori density model). On the other hand, muography provides a direct measurement of 2D mean densities (radiographic images) from the detection of high energy atmospheric muons crossing the volcanic edifice. 3D density distributions can be computed from several radiographic images, but the number of images is generally limited by field constraints and by the limited number of available telescopes. Thus, muon tomography is also ill-posed in practice.In the case of the puy de Dôme volcano, the density structures inferred from gravimetric data (Portal et al. 2016) and from muographic data (Le Ménédeu et al. 2016) show a qualitative agreement but cannot be compared quantitatively. Because each method has different intrinsic resolutions due to the physics (Jourde et al., 2015), the joint inversion is expected to improve the robustness of the inversion. Such joint inversion has already been applied in a volcanic context (Nishiyama et al., 2013).Volcano muography requires state-of-art, high-resolution and large-scale muon detectors (Ambrosino et al., 2015). Instrumental uncertainties and systematic errors may constitute an important limitation for muography and should not be overlooked. For instance, low-energy muons are detected together with ballistic high-energy muons, decreasing the measured value of the mean density closed to the topography.Here, we jointly invert the gravimetric and muographic data to characterize the 3D density distribution of the puy de Dôme volcano. We attempt to precisely identify and estimate the different uncertainties and systematic errors so that they can be accounted for in the inversion scheme.

Primary Energy Reconstruction from the Charged Particle Densities Recorded with the KASCADE-Grande Detector at 500 m Distance from Shower Core

NASA Astrophysics Data System (ADS)

Toma, G.; Apel, W. D.; Arteaga, J. C.; Bekk, K.; Bertaina, M.; Blümer, J.; Bozdog, H.; Brancus, I. M.; Buchholz, P.; Cantoni, E.; Chiavassa, A.; Cossavella, F.; Daumiller, K.; de Souza, V.; di Pierro, F.; Doll, P.; Engel, R.; Engler, J.; Finger, M.; Fuhrmann, D.; Ghia, P. L.; Gils, H. J.; Glasstetter, R.; Grupen, C.; Haungs, A.; Heck, D.; Hörandel, J. R.; Huege, T.; Isar, P. G.; Kampert, K.-H.; Kang, D.; Kickelbick, D.; Klages, H. O.; Link, K.; Łuczak, P.; Ludwig, M.; Mathes, H. J.; Mayer, H. J.; Melissas, M.; Milke, J.; Mitrica, B.; Morello, C.; Navarra, G.; Nehls, S.; Oehlschläger, J.; Ostapchenko, S.; Over, S.; Palmieri, N.; Petcu, M.; Pierog, T.; Rebel, H.; Roth, M.; Schieler, H.; Schröder, F.; Sima, O.; Trinchero, G. C.; Ulrich, H.; Weindl, A.; Wochele, J.; Wommer, M.; Zabierowski, J.

2010-11-01

Previous EAS investigations have shown that for a fixed primary energy the charged particle density becomes independent of the primary mass at certain (fixed) distances from the shower core. This feature can be used as an estimator for the primary energy. We present results on the reconstruction of the primary energy spectrum of cosmic rays from the experimentally recorded S(500) observable (the density of charged particles at 500 m distance to the shower core) using the KASCADE-Grande detector array. The KASCADE-Grande experiment is hosted by the Karlsruhe Institute for Technology-Campus North, Karlsruhe, Germany, and operated by an international collaboration. The constant intensity cut (CIC) method is applied to evaluate the attenuation of the S(500) observable with the zenith angle and is corrected for. A calibration of S(500) values with the primary energy has been worked out by simulations and was applied to the data to obtain the primary energy spectrum (in the energy range log10[E0/GeV]∈[7.5,9]). The systematic uncertainties induced by different sources are considered. In addition, a correction based on a response matrix is applied to account for the effects of shower-to-shower fluctuations on the spectral index of the reconstructed energy spectrum.

Octupole correlations in the 144Ba nucleus described with symmetry-conserving configuration-mixing calculations

NASA Astrophysics Data System (ADS)

Bernard, Rémi N.; Robledo, Luis M.; Rodríguez, Tomás R.

2016-06-01

We study the interplay of quadrupole and octupole degrees of freedom in the structure of the isotope 144Ba. A symmetry-conserving configuration-mixing method (SCCM) based on a Gogny energy density functional (EDF) has been used. The method includes particle number, parity, and angular momentum restoration as well as axial quadrupole and octupole shape mixing within the generator coordinate method. Predictions both for excitation energies and electromagnetic transition probabilities are in good agreement with the most recent experimental data.

Understanding and controlling the rest potential of carbon nanotube-based supercapacitors for energy density enhancement

NASA Astrophysics Data System (ADS)

Yoo, Young-Eun; Park, Jinwoo; Kim, Woong

2018-03-01

We present a novel method for enhancing the energy density of an electrical double layer capacitor (EDLC). Surface modification of single-walled carbon nanotube (SWNT) electrodes significantly affects the rest potential (E0) of EDLCs; acid treatment and polyethyleneimine (PEI) coating of SWNTs shift E0 toward more positive and more negative values, respectively. Adjusting E0 towards the center of the electrolyte stability window can increase the cell voltage and hence the energy density. PEI coating on SWNTs increases the cell voltage from 0.8 V to 1.7 V in tetrabutylammonium perchlorate (TBAP)/tetrahydrofuran (THF) electrolyte, and from 2.5 V to 3.1 V in tetraethylammonium tetrafluoroborate (TEABF4)/3-cyanopropionic acid methyl ester (CPAME), respectively. Moreover, PEI-SWNT EDLCs exhibit excellent cycling stability (92% of capacitance retention over 10000 cycles). We attribute the shift in E0 to a change in the Fermi level of SWNTs owing to the surface charge modification. Injection of electrical charge into PEI-SWNTs consistently yielded similar trends and thus validated our hypothesis. Our results may help to push various electrolytes that have been overlooked so far to new frontiers for obtaining high energy-density supercapacitors.

Multiconfiguration Pair-Density Functional Theory Spectral Calculations Are Stable to Adding Diffuse Basis Functions.

PubMed

Hoyer, Chad E; Gagliardi, Laura; Truhlar, Donald G

2015-11-05

Time-dependent Kohn-Sham density functional theory (TD-KS-DFT) is useful for calculating electronic excitation spectra of large systems, but the low-energy spectra are often complicated by artificially lowered higher-energy states. This affects even the lowest energy excited states. Here, by calculating the lowest energy spin-conserving excited state for atoms from H to K and for formaldehyde, we show that this problem does not occur in multiconfiguration pair-density functional theory (MC-PDFT). We use the tPBE on-top density functional, which is a translation of the PBE exchange-correlation functional. We compare to a robust multireference method, namely, complete active space second-order perturbation theory (CASPT2), and to TD-KS-DFT with two popular exchange-correlation functionals, PBE and PBE0. We find for atoms that the mean unsigned error (MUE) of MC-PDFT with the tPBE functional improves from 0.42 to 0.40 eV with a double set of diffuse functions, whereas the MUEs for PBE and PBE0 drastically increase from 0.74 to 2.49 eV and from 0.45 to 1.47 eV, respectively.

Application of a Modular Particle-Continuum Method to Partially Rarefied, Hypersonic Flow

NASA Astrophysics Data System (ADS)

Deschenes, Timothy R.; Boyd, Iain D.

2011-05-01

The Modular Particle-Continuum (MPC) method is used to simulate partially-rarefied, hypersonic flow over a sting-mounted planetary probe configuration. This hybrid method uses computational fluid dynamics (CFD) to solve the Navier-Stokes equations in regions that are continuum, while using direct simulation Monte Carlo (DSMC) in portions of the flow that are rarefied. The MPC method uses state-based coupling to pass information between the two flow solvers and decouples both time-step and mesh densities required by each solver. It is parallelized for distributed memory systems using dynamic domain decomposition and internal energy modes can be consistently modeled to be out of equilibrium with the translational mode in both solvers. The MPC results are compared to both full DSMC and CFD predictions and available experimental measurements. By using DSMC in only regions where the flow is nonequilibrium, the MPC method is able to reproduce full DSMC results down to the level of velocity and rotational energy probability density functions while requiring a fraction of the computational time.

Computational Investigation of the Geometrical and Electronic Structures of VGen-/0 (n = 1-4) Clusters by Density Functional Theory and Multiconfigurational CASSCF/CASPT2 Method.

PubMed

Tran, Van Tan; Nguyen, Minh Thao; Tran, Quoc Tri

2017-10-12

Density functional theory and the multiconfigurational CASSCF/CASPT2 method have been employed to study the low-lying states of VGe n -/0 (n = 1-4) clusters. For VGe -/0 and VGe 2 -/0 clusters, the relative energies and geometrical structures of the low-lying states are reported at the CASSCF/CASPT2 level. For the VGe 3 -/0 and VGe 4 -/0 clusters, the computational results show that due to the large contribution of the Hartree-Fock exact exchange, the hybrid B3LYP, B3PW91, and PBE0 functionals overestimate the energies of the high-spin states as compared to the pure GGA BP86 and PBE functionals and the CASPT2 method. On the basis of the pure GGA BP86 and PBE functionals and the CASSCF/CASPT2 results, the ground states of anionic and neutral clusters are defined, the relative energies of the excited states are computed, and the electron detachment energies of the anionic clusters are evaluated. The computational results are employed to give new assignments for all features in the photoelectron spectra of VGe 3 - and VGe 4 - clusters.

Spectral optimization for measuring electron density by the dual-energy computed tomography coupled with balanced filter method.

PubMed

Saito, Masatoshi

2009-08-01

Dual-energy computed tomography (DECT) has the potential for measuring electron density distribution in a human body to predict the range of particle beams for treatment planning in proton or heavy-ion radiotherapy. However, thus far, a practical dual-energy method that can be used to precisely determine electron density for treatment planning in particle radiotherapy has not been developed. In this article, another DECT technique involving a balanced filter method using a conventional x-ray tube is described. For the spectral optimization of DECT using balanced filters, the author calculates beam-hardening error and air kerma required to achieve a desired noise level in electron density and effective atomic number images of a cylindrical water phantom with 50 cm diameter. The calculation enables the selection of beam parameters such as tube voltage, balanced filter material, and its thickness. The optimized parameters were applied to cases with different phantom diameters ranging from 5 to 50 cm for the calculations. The author predicts that the optimal combination of tube voltages would be 80 and 140 kV with Tb/Hf and Bi/Mo filter pairs for the 50-cm-diameter water phantom. When a single phantom calibration at a diameter of 25 cm was employed to cover all phantom sizes, maximum absolute beam-hardening errors were 0.3% and 0.03% for electron density and effective atomic number, respectively, over a range of diameters of the water phantom. The beam-hardening errors were 1/10 or less as compared to those obtained by conventional DECT, although the dose was twice that of the conventional DECT case. From the viewpoint of beam hardening and the tube-loading efficiency, the present DECT using balanced filters would be significantly more effective in measuring the electron density than the conventional DECT. Nevertheless, further developments of low-exposure imaging technology should be necessary as well as x-ray tubes with higher outputs to apply DECT coupled with the balanced filter method for clinical use.

Free-energy-based lattice Boltzmann model for the simulation of multiphase flows with density contrast.

PubMed

Shao, J Y; Shu, C; Huang, H B; Chew, Y T

2014-03-01

A free-energy-based phase-field lattice Boltzmann method is proposed in this work to simulate multiphase flows with density contrast. The present method is to improve the Zheng-Shu-Chew (ZSC) model [Zheng, Shu, and Chew, J. Comput. Phys. 218, 353 (2006)] for correct consideration of density contrast in the momentum equation. The original ZSC model uses the particle distribution function in the lattice Boltzmann equation (LBE) for the mean density and momentum, which cannot properly consider the effect of local density variation in the momentum equation. To correctly consider it, the particle distribution function in the LBE must be for the local density and momentum. However, when the LBE of such distribution function is solved, it will encounter a severe numerical instability. To overcome this difficulty, a transformation, which is similar to the one used in the Lee-Lin (LL) model [Lee and Lin, J. Comput. Phys. 206, 16 (2005)] is introduced in this work to change the particle distribution function for the local density and momentum into that for the mean density and momentum. As a result, the present model still uses the particle distribution function for the mean density and momentum, and in the meantime, considers the effect of local density variation in the LBE as a forcing term. Numerical examples demonstrate that both the present model and the LL model can correctly simulate multiphase flows with density contrast, and the present model has an obvious improvement over the ZSC model in terms of solution accuracy. In terms of computational time, the present model is less efficient than the ZSC model, but is much more efficient than the LL model.

Solid-State High Performance Flexible Supercapacitors Based on Polypyrrole-MnO2-Carbon Fiber Hybrid Structure

NASA Astrophysics Data System (ADS)

Tao, Jiayou; Liu, Nishuang; Ma, Wenzhen; Ding, Longwei; Li, Luying; Su, Jun; Gao, Yihua

2013-07-01

A solid-state flexible supercapacitor (SC) based on organic-inorganic composite structure was fabricated through an ``in situ growth for conductive wrapping'' and an electrode material of polypyrrole (PPy)-MnO2 nanoflakes-carbon fiber (CF) hybrid structure was obtained. The conductive organic material of PPy greatly improved the electrochemical performance of the device. With a high specific capacitance of 69.3 F cm-3 at a discharge current density of 0.1 A cm-3 and an energy density of 6.16 × 10-3 Wh cm-3 at a power density of 0.04 W cm-3, the device can drive a commercial liquid crystal display (LCD) after being charged. The organic-inorganic composite active materials have enormous potential in energy management and the ``in situ growth for conductive wrapping'' method might be generalized to open up new strategies for designing next-generation energy storage devices.

Lithium-Based High Energy Density Flow Batteries

NASA Technical Reports Server (NTRS)

Bugga, Ratnakumar V. (Inventor); West, William C. (Inventor); Kindler, Andrew (Inventor); Smart, Marshall C. (Inventor)

2014-01-01

Systems and methods in accordance with embodiments of the invention implement a lithium-based high energy density flow battery. In one embodiment, a lithium-based high energy density flow battery includes a first anodic conductive solution that includes a lithium polyaromatic hydrocarbon complex dissolved in a solvent, a second cathodic conductive solution that includes a cathodic complex dissolved in a solvent, a solid lithium ion conductor disposed so as to separate the first solution from the second solution, such that the first conductive solution, the second conductive solution, and the solid lithium ionic conductor define a circuit, where when the circuit is closed, lithium from the lithium polyaromatic hydrocarbon complex in the first conductive solution dissociates from the lithium polyaromatic hydrocarbon complex, migrates through the solid lithium ionic conductor, and associates with the cathodic complex of the second conductive solution, and a current is generated.

Implicit solvation model for density-functional study of nanocrystal surfaces and reaction pathways

NASA Astrophysics Data System (ADS)

Mathew, Kiran; Sundararaman, Ravishankar; Letchworth-Weaver, Kendra; Arias, T. A.; Hennig, Richard G.

2014-02-01

Solid-liquid interfaces are at the heart of many modern-day technologies and provide a challenge to many materials simulation methods. A realistic first-principles computational study of such systems entails the inclusion of solvent effects. In this work, we implement an implicit solvation model that has a firm theoretical foundation into the widely used density-functional code Vienna ab initio Software Package. The implicit solvation model follows the framework of joint density functional theory. We describe the framework, our algorithm and implementation, and benchmarks for small molecular systems. We apply the solvation model to study the surface energies of different facets of semiconducting and metallic nanocrystals and the SN2 reaction pathway. We find that solvation reduces the surface energies of the nanocrystals, especially for the semiconducting ones and increases the energy barrier of the SN2 reaction.

Orbital relaxation effects on Kohn–Sham frontier orbital energies in density functional theory

DOE Office of Scientific and Technical Information (OSTI.GOV)

Zhang, DaDi; Zheng, Xiao, E-mail: xz58@ustc.edu.cn; Synergetic Innovation Center of Quantum Information and Quantum Physics, University of Science and Technology of China, Hefei, Anhui 230026

2015-04-21

We explore effects of orbital relaxation on Kohn–Sham frontier orbital energies in density functional theory by using a nonempirical scaling correction approach developed in Zheng et al. [J. Chem. Phys. 138, 174105 (2013)]. Relaxation of Kohn–Sham orbitals upon addition/removal of a fractional number of electrons to/from a finite system is determined by a systematic perturbative treatment. The information of orbital relaxation is then used to improve the accuracy of predicted Kohn–Sham frontier orbital energies by Hartree–Fock, local density approximation, and generalized gradient approximation methods. The results clearly highlight the significance of capturing the orbital relaxation effects. Moreover, the proposed scalingmore » correction approach provides a useful way of computing derivative gaps and Fukui quantities of N-electron finite systems (N is an integer), without the need to perform self-consistent-field calculations for (N ± 1)-electron systems.« less

Optimization of gas-filled quartz capillary discharge waveguide for high-energy laser wakefield acceleration

NASA Astrophysics Data System (ADS)

Qin, Zhiyong; Li, Wentao; Liu, Jiansheng; Liu, Jiaqi; Yu, Changhai; Wang, Wentao; Qi, Rong; Zhang, Zhijun; Fang, Ming; Feng, Ke; Wu, Ying; Ke, Lintong; Chen, Yu; Wang, Cheng; Li, Ruxin; Xu, Zhizhan

2018-04-01

A hydrogen-filled capillary discharge waveguide made of quartz is presented for high-energy laser wakefield acceleration (LWFA). The experimental parameters (discharge current and gas pressure) were optimized to mitigate ablation by a quantitative analysis of the ablation plasma density inside the hydrogen-filled quartz capillary. The ablation plasma density was obtained by combining a spectroscopic measurement method with a calibrated gas transducer. In order to obtain a controllable plasma density and mitigate the ablation as much as possible, the range of suitable parameters was investigated. The experimental results demonstrated that the ablation in the quartz capillary could be mitigated by increasing the gas pressure to ˜7.5-14.7 Torr and decreasing the discharge current to ˜70-100 A. These optimized parameters are promising for future high-energy LWFA experiments based on the quartz capillary discharge waveguide.

Nonadiabatic Molecular Dynamics and Orthogonality Constrained Density Functional Theory

NASA Astrophysics Data System (ADS)

Shushkov, Philip Georgiev

The exact quantum dynamics of realistic, multidimensional systems remains a formidable computational challenge. In many chemical processes, however, quantum effects such as tunneling, zero-point energy quantization, and nonadiabatic transitions play an important role. Therefore, approximate approaches that improve on the classical mechanical framework are of special practical interest. We propose a novel ring polymer surface hopping method for the calculation of chemical rate constants. The method blends two approaches, namely ring polymer molecular dynamics that accounts for tunneling and zero-point energy quantization, and surface hopping that incorporates nonadiabatic transitions. We test the method against exact quantum mechanical calculations for a one-dimensional, two-state model system. The method reproduces quite accurately the tunneling contribution to the rate and the distribution of reactants between the electronic states for this model system. Semiclassical instanton theory, an approach related to ring polymer molecular dynamics, accounts for tunneling by the use of periodic classical trajectories on the inverted potential energy surface. We study a model of electron transfer in solution, a chemical process where nonadiabatic events are prominent. By representing the tunneling electron with a ring polymer, we derive Marcus theory of electron transfer from semiclassical instanton theory after a careful analysis of the tunneling mode. We demonstrate that semiclassical instanton theory can recover the limit of Fermi's Golden Rule rate in a low-temperature, deep-tunneling regime. Mixed quantum-classical dynamics treats a few important degrees of freedom quantum mechanically, while classical mechanics describes affordably the rest of the system. But the interface of quantum and classical description is a challenging theoretical problem, especially for low-energy chemical processes. We therefore focus on the semiclassical limit of the coupled nuclear-electronic dynamics. We show that the time-dependent Schrodinger equation for the electrons employed in the widely used fewest switches surface hopping method is applicable only in the limit of nearly identical classical trajectories on the different potential energy surfaces. We propose a short-time decoupling algorithm that restricts the use of the Schrodinger equation only to the interaction regions. We test the short-time approximation on three model systems against exact quantum-mechanical calculations. The approximation improves the performance of the surface hopping approach. Nonadiabatic molecular dynamics simulations require the efficient and accurate computation of ground and excited state potential energy surfaces. Unlike the ground state calculations where standard methods exist, the computation of excited state properties is a challenging task. We employ time-independent density functional theory, in which the excited state energy is represented as a functional of the total density. We suggest an adiabatic-like approximation that simplifies the excited state exchange-correlation functional. We also derive a set of minimal conditions to impose exactly the orthogonality of the excited state Kohn-Sham determinant to the ground state determinant. This leads to an efficient, variational algorithm for the self-consistent optimization of the excited state energy. Finally, we assess the quality of the excitation energies obtained by the new method on a set of 28 organic molecules. The new approach provides results of similar accuracy to time-dependent density functional theory.

Redox potentials and pKa for benzoquinone from density functional theory based molecular dynamics.

PubMed

Cheng, Jun; Sulpizi, Marialore; Sprik, Michiel

2009-10-21

The density functional theory based molecular dynamics (DFTMD) method for the computation of redox free energies presented in previous publications and the more recent modification for computation of acidity constants are reviewed. The method uses a half reaction scheme based on reversible insertion/removal of electrons and protons. The proton insertion is assisted by restraining potentials acting as chaperones. The procedure for relating the calculated deprotonation free energies to Brønsted acidities (pK(a)) and the oxidation free energies to electrode potentials with respect to the normal hydrogen electrode is discussed in some detail. The method is validated in an application to the reduction of aqueous 1,4-benzoquinone. The conversion of hydroquinone to quinone can take place via a number of alternative pathways consisting of combinations of acid dissociations, oxidations, or dehydrogenations. The free energy changes of all elementary steps (ten in total) are computed. The accuracy of the calculations is assessed by comparing the energies of different pathways for the same reaction (Hess's law) and by comparison to experiment. This two-sided test enables us to separate the errors related with the restrictions on length and time scales accessible to DFTMD from the errors introduced by the DFT approximation. It is found that the DFT approximation is the main source of error for oxidation free energies.

High power and high energy electrodes using carbon nanotubes

DOEpatents

Martini, Fabrizio; Brambilla, Nicolo Michele; Signorelli, Riccardo

2015-04-07

An electrode useful in an energy storage system, such as a capacitor, includes an electrode that includes at least one to a plurality of layers of compressed carbon nanotube aggregate. Methods of fabrication are provided. The resulting electrode exhibits superior electrical performance in terms of gravimetric and volumetric power density.

The Hubble diagram for a system within dark energy: influence of some relevant quantities

NASA Astrophysics Data System (ADS)

Saarinen, J.; Teerikorpi, P.

2014-08-01

Aims: We study the influence of relevant quantities, including the density of dark energy (DE), to the predicted Hubble outflow around a system of galaxies. In particular, we are interested in the difference between two models: 1) the standard ΛCDM model, with the everywhere constant DE density, and 2) the "Swiss cheese model", where the Universe is as old as the standard model and the DE density is zero on short scales, including the environment of the system. Methods: We calculated the current predicted outflow patterns of dwarf galaxies around the Local Group-like system, using different values for the mass of the group, the local DE density, and the time of ejection of the dwarf galaxies, which are treated as test particles. These results are compared with the observed Hubble flow around the Local Group. Results: The predicted distance-velocity relations around galaxy groups are not very sensitive indicators of the DE density, owing to the observational scatter and the uncertainties caused by the mass used for the group and a range in the ejection times. In general, the Local Group outflow data agree with the local DE density being equal to the global one, if the Local Group mass is about 4 × 1012 M⊙; a lower mass ≲ 2 × 1012 M⊙ could suggest a zero local DE density. The dependence of the inferred DE density on the mass is a handicap in this and other common dynamical methods. This emphasizes the need to use different approaches together, for constraining the local DE density.

Diffusion quantum Monte Carlo calculations of SrFeO 3 and LaFeO 3

DOE PAGES

Santana, Juan A.; Krogel, Jaron T.; Kent, Paul R. C.; ...

2017-07-18

The equations of state, formation energy, and migration energy barrier of the oxygen vacancy in SrFeO 3 and LaFeO 3 were calculated in this paper with the diffusion quantum Monte Carlo (DMC) method. Calculations were also performed with various Density Functional Theory (DFT) approximations for comparison. DMC reproduces the measured cohesive energies of these materials with errors below 0.23(5) eV and the structural properties within 1% of the experimental values. The DMC formation energies of the oxygen vacancy in SrFeO 3 and LaFeO 3 under oxygen-rich conditions are 1.3(1) and 6.24(7) eV, respectively. Similar calculations with semi-local DFT approximations formore » LaFeO 3 yielded vacancy formation energies 1.5 eV lower. Comparison of charge density evaluated with DMC and DFT approximations shows that DFT tends to overdelocalize the electrons in defected SrFeO 3 and LaFeO 3. Finally, calculations with DMC and local density approximation yield similar vacancy migration energy barriers, indicating that steric/electrostatic effects mainly determine migration barriers in these materials.« less

Study on composite flywheels for energy storage

NASA Astrophysics Data System (ADS)

Kogai, K.; Inutake, T.; Hamamoto, A.; Tadaishi, Y.; Kawamura, K.

1982-09-01

In order to investigate the feasibility of composite flywheels as a means of storing energy, flywheels consisting of carbon fiber epoxy rims and aluminum or carbon fabric composite hubs were designed, fabricated, and tested. The carbon fiber epoxy composite rims fabricated by the filament winding method were 380 mm in outer diameter and 300 mm in inner diameter with a thickness of 25 mm. The test rotor with an aluminum hub was spun to a maximum peripheral speed of 982 m/s on burst tests. This corresponds to an energy density, based upon the total rotor weight, of approximately 71 W h/kg. Another rotor with two aluminum hubs using a four-rim configuration was successfully tested to 800 m/s without any damage or dynamic problems. The stored energy in the rotor is more than 500 W h, and the energy density is about 55 W h/kg at 800 m/s. The rotor with a composite hub was tested to a peripheral speed of 820 m/s. It was restricted by dynamic problems in the rotor, but the energy density was about 66 W h/kg at 800 m/s due to the light weight of the hub.

Anti-Ferroelectric Ceramics for High Energy Density Capacitors.

PubMed

Chauhan, Aditya; Patel, Satyanarayan; Vaish, Rahul; Bowen, Chris R

2015-11-25

With an ever increasing dependence on electrical energy for powering modern equipment and electronics, research is focused on the development of efficient methods for the generation, storage and distribution of electrical power. In this regard, the development of suitable dielectric based solid-state capacitors will play a key role in revolutionizing modern day electronic and electrical devices. Among the popular dielectric materials, anti-ferroelectrics (AFE) display evidence of being a strong contender for future ceramic capacitors. AFE materials possess low dielectric loss, low coercive field, low remnant polarization, high energy density, high material efficiency, and fast discharge rates; all of these characteristics makes AFE materials a lucrative research direction. However, despite the evident advantages, there have only been limited attempts to develop this area. This article attempts to provide a focus to this area by presenting a timely review on the topic, on the relevant scientific advancements that have been made with respect to utilization and development of anti-ferroelectric materials for electric energy storage applications. The article begins with a general introduction discussing the need for high energy density capacitors, the present solutions being used to address this problem, and a brief discussion of various advantages of anti-ferroelectric materials for high energy storage applications. This is followed by a general description of anti-ferroelectricity and important anti-ferroelectric materials. The remainder of the paper is divided into two subsections, the first of which presents various physical routes for enhancing the energy storage density while the latter section describes chemical routes for enhanced storage density. This is followed by conclusions and future prospects and challenges which need to be addressed in this particular field.

Anti-Ferroelectric Ceramics for High Energy Density Capacitors

PubMed Central

Chauhan, Aditya; Patel, Satyanarayan; Vaish, Rahul; Bowen, Chris R.

2015-01-01

With an ever increasing dependence on electrical energy for powering modern equipment and electronics, research is focused on the development of efficient methods for the generation, storage and distribution of electrical power. In this regard, the development of suitable dielectric based solid-state capacitors will play a key role in revolutionizing modern day electronic and electrical devices. Among the popular dielectric materials, anti-ferroelectrics (AFE) display evidence of being a strong contender for future ceramic capacitors. AFE materials possess low dielectric loss, low coercive field, low remnant polarization, high energy density, high material efficiency, and fast discharge rates; all of these characteristics makes AFE materials a lucrative research direction. However, despite the evident advantages, there have only been limited attempts to develop this area. This article attempts to provide a focus to this area by presenting a timely review on the topic, on the relevant scientific advancements that have been made with respect to utilization and development of anti-ferroelectric materials for electric energy storage applications. The article begins with a general introduction discussing the need for high energy density capacitors, the present solutions being used to address this problem, and a brief discussion of various advantages of anti-ferroelectric materials for high energy storage applications. This is followed by a general description of anti-ferroelectricity and important anti-ferroelectric materials. The remainder of the paper is divided into two subsections, the first of which presents various physical routes for enhancing the energy storage density while the latter section describes chemical routes for enhanced storage density. This is followed by conclusions and future prospects and challenges which need to be addressed in this particular field. PMID:28793694

Reconstructing f(R) modified gravity with dark energy parametrization

NASA Astrophysics Data System (ADS)

Morita, Masaaki; Takahashi, Hirotaka

2014-03-01

We demonstrate the reconstruction of f(R) modified gravity theory with late-time accelerated cosmic expansion. A second-order differential equation for Lagrangian density is obtained from the field equation, and is solved as a function of the cosmic scale factor in two cases. First we begin with the case of a wCDM cosmological model, in which a dark-energy equation-of-state parameter w is constant, for simplicity. Next we extend the method to a case in which the parameter w is epoch-dependent and is expressed as the Chevallier-Polarski-Linder parametrization. Thus we can represent Lagrangian density of f(R) modified gravity theory in terms of dark energy parameters.

Structure of 8Li from a reaction cross-section measurement

NASA Astrophysics Data System (ADS)

Fan, G. W.; Fukuda, M.; Nishimura, D.; Cai, X. L.; Fukuda, S.; Hachiuma, I.; Ichikawa, C.; Izumikawa, T.; Kanazawa, M.; Kitagawa, A.; Kuboki, T.; Lantz, M.; Mihara, M.; Nagashima, M.; Namihira, K.; Ohkuma, Y.; Ohtsubo, T.; Ren, Zhongzhou; Sato, S.; Shen, Z. Q.; Sugiyama, M.; Suzuki, S.; Suzuki, T.; Takechi, M.; Yamaguchi, T.; Xu, B. J.; Xu, W.

2014-10-01

We have precisely measured reaction cross sections (σR) for 8Li using 9Be, 12C , 27Al, and proton targets at intermediate energies by the transmission method. From the energy dependence of the σR including the high energy data, the density distribution of 8Li was deduced through a modified Glauber model. It is shown that 8Li has a shorter tail structure in the density as compared with that of 8B and the matter radius of 8Li is similar to those of the other nonhalo Li isotopes. The result is consistent with the previous experiments that there is a tendency for 8Li to be a skin nucleus.

Dark energy in the environments of the Local Group, the M 81 group, and the CenA group: the normalized Hubble diagram

NASA Astrophysics Data System (ADS)

Teerikorpi, P.; Chernin, A. D.; Karachentsev, I. D.; Valtonen, M. J.

2008-05-01

Context: Type Ia supernova observations on scales of thousands of Mpc show that the global expansion of the universe is accelerated by antigravity produced by the enigmatic dark energy contributing 3/4 of the total energy of the universe. Aims: Does antigravity act on small scales as well as large? As a continuation of our efforts to answer this crucial question we combine high accuracy observations of the galaxy flows around the Local Group and the nearby M 81 and CenA groups to observe the effect of the dark energy density on local scales of a few Mpc. Methods: We use an analytical model to describe non-uniform static space-time regions around galaxy groups. In this context it is useful to present the Hubble flow in a normalized Hubble diagram V/Hv Rv vs. r/R_v, where the vacuum Hubble constant Hv depends only on the cosmological vacuum density and the zero-gravity distance Rv depends on the vacuum density and on the mass of the galaxy group. We have prepared the normalized Hubble diagrams for the LG, M 81 and CenA group environments for different values of the assumed vacuum energy density, using a total of about 150 galaxies, for almost all of which the distances have been measured by the HST. Results: The normalized Hubble diagram, where we identify dynamically different regions, is in agreement with the standard vacuum density (Ωv = 0.77~h_70-2), the out-flow of galaxies clearly being controlled by the minimum energy condition imposed by the central mass plus the vacuum density. A high vacuum density 1.6~h_70-2 violates the minimum energy limit, while a low density 0.1~h_70-2 leaves the start of the Hubble flow around 1-2 Mpc with the slope close to the global value obscure. We also consider the subtle relation of the zero-gravity radius Rv to the zero-velocity distance R0 appearing in the usual retarded expansion around a mass M: in a vacuum-dominated flat universe R0 ≈ 0.76 R_v. Conclusions: The normalized Hubble diagram appears to be a good way to present and analyze physically different regions around mass clumps embedded in cosmological vacuum. The most natural interpretation of the diagram is that the local density of the dark energy is approximately equal to the density known from studies on global scales.

Exact analytical solutions of continuity equation for electron beams precipitating in Coulomb collisions

DOE Office of Scientific and Technical Information (OSTI.GOV)

Dobranskis, R. R.; Zharkova, V. V., E-mail: valentina.zharkova@northumbria.ac.uk

2014-06-10

The original continuity equation (CE) used for the interpretation of the power law energy spectra of beam electrons in flares was written and solved for an electron beam flux while ignoring an additional free term with an electron density. In order to remedy this omission, the original CE for electron flux, considering beam's energy losses in Coulomb collisions, was first differentiated by the two independent variables: depth and energy leading to partial differential equation for an electron beam density instead of flux with the additional free term. The analytical solution of this partial differential continuity equation (PDCE) is obtained bymore » using the method of characteristics. This solution is further used to derive analytical expressions for mean electron spectra for Coulomb collisions and to carry out numeric calculations of hard X-ray (HXR) photon spectra for beams with different parameters. The solutions revealed a significant departure of electron densities at lower energies from the original results derived from the CE for the flux obtained for Coulomb collisions. This departure is caused by the additional exponential term that appeared in the updated solutions for electron differential density leading to its faster decrease at lower energies (below 100 keV) with every precipitation depth similar to the results obtained with numerical Fokker-Planck solutions. The effects of these updated solutions for electron densities on mean electron spectra and HXR photon spectra are also discussed.« less

Fission dynamics with microscopic level densities

NASA Astrophysics Data System (ADS)

Randrup, Jørgen; Ward, Daniel; Carlsson, Gillis; Døssing, Thomas; Möller, Peter; Åberg, Sven

2018-03-01

Working within the Langevin framework of nuclear shape dynamics, we study the dependence of the evolution on the degree of excitation. As the excitation energy of the fissioning system is increased, the pairing correlations and the shell effects diminish and the effective potential-energy surface becomes ever more liquid-drop like. This feature can be included in the treatment in a formally well-founded manner by using the local level densities as a basis for the shape evolution. This is particularly easy to understand and implement in the Metropolis treatment where the evolution is simulated by means of a random walk on the five-dimensional lattice of shapes for which the potential energy has been tabulated. Because the individual steps between two neighboring lattice sites are decided on the basis of the ratio of the statistical weights, what is needed is the ratio of the local level densities for those shapes, evaluated at the associated local excitation energies. For this purpose, we adapt a recently developed combinatorial method for calculating level densities which employs the same single-particle levels as those that were used for the calculation of the pairing and shell contributions to the macroscopic-microscopic deformation-energy surface. For each nucleus under consideration, the level density (for a fixed total angular momentum) is calculated microscopically for each of the over five million shapes given in the three-quadratic-surface parametrization. This novel treatment, which introduces no new parameters, is illustrated for the fission fragment mass distributions for selected uranium and plutonium cases.

Multiconfiguration Pair-Density Functional Theory and Complete Active Space Second Order Perturbation Theory. Bond Dissociation Energies of FeC, NiC, FeS, NiS, FeSe, and NiSe.

PubMed

Sharkas, Kamal; Gagliardi, Laura; Truhlar, Donald G

2017-12-07

We investigate the performance of multiconfiguration pair-density functional theory (MC-PDFT) and complete active space second-order perturbation theory for computing the bond dissociation energies of the diatomic molecules FeC, NiC, FeS, NiS, FeSe, and NiSe, for which accurate experimental data have become recently available [Matthew, D. J.; Tieu, E.; Morse, M. D. J. Chem. Phys. 2017, 146, 144310-144320]. We use three correlated participating orbital (CPO) schemes (nominal, moderate, and extended) to define the active spaces, and we consider both the complete active space (CAS) and the separated-pair (SP) schemes to specify the configurations included for a given active space. We found that the moderate SP-PDFT scheme with the tPBE on-top density functional has the smallest mean unsigned error (MUE) of the methods considered. This level of theory provides a balanced treatment of the static and dynamic correlation energies for the studied systems. This is encouraging because the method is low in cost even for much more complicated systems.

Theoretical studies on the crystal structure, thermodynamic properties, detonation performance and thermal stability of cage-tetranitrotetraazabicyclooctane as a novel high energy density compound.

PubMed

Zhao, Guo-zheng; Lu, Ming

2013-01-01

The B3LYP/6-31G (d) method of density functional theory (DFT) was used to study molecular geometry, electronic structure, infrared spectrum (IR) and thermodynamic properties. The heat of formation (HOF) and calculated density were estimated to evaluate the detonation properties using Kamlet-Jacobs equations. Thermal stability of 3,5,7,10,12,14,15,16-octanitro- 3,5,7,10,12,14,15,16-octaaza-heptacyclo[7.5.1.1(2,8).0(1,11).0(2,6).0(4,13).0(6,11)]hexadecane (cage-tetranitrotetraazabicyclooctane) was investigated by calculating the bond dissociation energy (BDE) at unrestricted B3LYP/6-31G (d) level. The calculated results show that the N-NO2 bond is a trigger bond during thermolysis initiation process. The crystal structure obtained by molecular mechanics (MM) methods belongs to Pna2(1) space group, with cell parameters a=12.840 Å, b=9.129 Å, c=14.346 Å, Z=6 and ρ=2.292 g·cm(-3). Both the detonation velocity of 9.96 km·s(-1) and the detonation pressure of 47.47 GPa are better than those of CL-20. According to the quantitative standard of energetics and stability, as a high energy density compound (HEDC), cage-tetranitrotetraazabicyclooctane essentially satisfies this requirement.

Nanowire Na0.35MnO2 from a hydrothermal method as a cathode material for aqueous asymmetric supercapacitors

NASA Astrophysics Data System (ADS)

Zhang, B. H.; Liu, Y.; Chang, Z.; Yang, Y. Q.; Wen, Z. B.; Wu, Y. P.; Holze, R.

2014-05-01

Nanowire Na0.35MnO2 was prepared by a simple and low energy consumption hydrothermal method; its electrochemical performance as a cathode material for aqueous asymmetric supercapacitors in Na2SO4 solution was investigated. Due to the nanowire structure its capacitance (157 F g-1) is much higher than that of the rod-like Na0.95MnO2 (92 F g-1) from solid phase reaction although its sodium content is lower. When it is assembled into an asymmetric aqueous supercapacitor using activated carbon as the counter electrode and aqueous 0.5 mol L-1 Na2SO4 electrolyte solution, the nanowire Na0.35MnO2 shows an energy density of 42.6 Wh kg-1 at a power density of 129.8 W kg-1 based on the total weight of the two electrode material, higher than those for the rod-like Na0.95MnO2, with an energy density of 27.3 Wh kg-1 at a power density of 74.8 W kg-1, and that of LiMn2O4. The new material presents excellent cycling behavior even when dissolved oxygen is not removed from the electrolyte solution. The results hold great promise for practical applications of this cathode material since sodium is much cheaper than lithium and its natural resources are rich.

Combining Density Functional Theory and Green's Function Theory: Range-Separated, Nonlocal, Dynamic, and Orbital-Dependent Hybrid Functional.

PubMed

Kananenka, Alexei A; Zgid, Dominika

2017-11-14

We present a rigorous framework which combines single-particle Green's function theory with density functional theory based on a separation of electron-electron interactions into short- and long-range components. Short-range contribution to the total energy and exchange-correlation potential is provided by a density functional approximation, while the long-range contribution is calculated using an explicit many-body Green's function method. Such a hybrid results in a nonlocal, dynamic, and orbital-dependent exchange-correlation functional of a single-particle Green's function. In particular, we present a range-separated hybrid functional called srSVWN5-lrGF2 which combines the local-density approximation and the second-order Green's function theory. We illustrate that similarly to density functional approximations, the new functional is weakly basis-set dependent. Furthermore, it offers an improved description of the short-range dynamic correlation. The many-body contribution to the functional mitigates the many-electron self-interaction error present in many density functional approximations and provides a better description of molecular properties. Additionally, we illustrate that the new functional can be used to scale down the self-energy and, therefore, introduce an additional sparsity to the self-energy matrix that in the future can be exploited in calculations for large molecules or periodic systems.

Efficient grid-based techniques for density functional theory

NASA Astrophysics Data System (ADS)

Rodriguez-Hernandez, Juan Ignacio

Understanding the chemical and physical properties of molecules and materials at a fundamental level often requires quantum-mechanical models for these substance's electronic structure. This type of many body quantum mechanics calculation is computationally demanding, hindering its application to substances with more than a few hundreds atoms. The supreme goal of many researches in quantum chemistry---and the topic of this dissertation---is to develop more efficient computational algorithms for electronic structure calculations. In particular, this dissertation develops two new numerical integration techniques for computing molecular and atomic properties within conventional Kohn-Sham-Density Functional Theory (KS-DFT) of molecular electronic structure. The first of these grid-based techniques is based on the transformed sparse grid construction. In this construction, a sparse grid is generated in the unit cube and then mapped to real space according to the pro-molecular density using the conditional distribution transformation. The transformed sparse grid was implemented in program deMon2k, where it is used as the numerical integrator for the exchange-correlation energy and potential in the KS-DFT procedure. We tested our grid by computing ground state energies, equilibrium geometries, and atomization energies. The accuracy on these test calculations shows that our grid is more efficient than some previous integration methods: our grids use fewer points to obtain the same accuracy. The transformed sparse grids were also tested for integrating, interpolating and differentiating in different dimensions (n = 1,2,3,6). The second technique is a grid-based method for computing atomic properties within QTAIM. It was also implemented in deMon2k. The performance of the method was tested by computing QTAIM atomic energies, charges, dipole moments, and quadrupole moments. For medium accuracy, our method is the fastest one we know of.

On the accuracy of density functional theory and wave function methods for calculating vertical ionization energies

DOE Office of Scientific and Technical Information (OSTI.GOV)

McKechnie, Scott; Booth, George H.; Cohen, Aron J.

The best practice in computational methods for determining vertical ionization energies (VIEs) is assessed, via reference to experimentally determined VIEs that are corroborated by highly accurate coupled-cluster calculations. These reference values are used to benchmark the performance of density-functional theory (DFT) and wave function methods: Hartree-Fock theory (HF), second-order Møller-Plesset perturbation theory (MP2) and Electron Propagator Theory (EPT). The core test set consists of 147 small molecules. An extended set of six larger molecules, from benzene to hexacene, is also considered to investigate the dependence of the results on molecule size. The closest agreement with experiment is found for ionizationmore » energies obtained from total energy diff calculations. In particular, DFT calculations using exchange-correlation functionals with either a large amount of exact exchange or long-range correction perform best. The results from these functionals are also the least sensitive to an increase in molecule size. In general, ionization energies calculated directly from the orbital energies of the neutral species are less accurate and more sensitive to an increase in molecule size. For the single-calculation approach, the EPT calculations are in closest agreement for both sets of molecules. For the orbital energies from DFT functionals, only those with long-range correction give quantitative agreement with dramatic failing for all other functionals considered. The results offer a practical hierarchy of approximations for the calculation of vertical ionization energies. In addition, the experimental and computational reference values can be used as a standardized set of benchmarks, against which other approximate methods can be compared.« less

The rising disparity in the price of healthful foods: 2004–2008

PubMed Central

Monsivais, Pablo; McLain, Julia; Drewnowski, Adam

2014-01-01

Nutrient dense foods that are associated with better health outcomes tend to cost more per kilocalorie (kcal) than do refined grains, sweets and fats. The price disparity between healthful and less healthful foods appears to be growing. This study demonstrates a new method for linking longitudinal retail price data with objective, nutrient-based ratings of the nutritional quality of foods and beverages. Retail prices for 378 foods and beverages were obtained from major supermarket chains in the Seattle, WA for 2004-8. Nutritional quality was based on energy density (kcal/g) and two measures of nutrient density, calculated using the Naturally Nutrient Rich (NNR) score and the Nutrient Rich Foods index (NRF9.3). Food prices were expressed as $/100g edible portion and as $/1,000 kcal. Foods were stratified by quintiles of energy and nutrient density for analyses. Both measures of nutrient density were negatively associated with energy density and positively associated with cost per 1,000 kcal. The mean cost of foods in the top quintile of nutrient density was $27.20/1,000 kcal and the 4 y price increase was 29.2%. Foods in the bottom quintile cost a mean of $3.32/1000 kcal and the 4 y price increase was 16.1%. There is a growing price disparity between nutrient-dense foods and less nutritious options. Cost may pose a barrier to the adoption of healthier diets and so limit the impact of dietary guidance. Nutrient profiling methods provide objective criteria for tracking retail prices of foods in relation to their nutritional quality and for guiding food and nutrition policy. PMID:25411518

Computational studies on the crystal structure, thermodynamic properties, detonation performance, and pyrolysis mechanism of 2,4,6,8-tetranitro-1,3,5,7-tetraazacubane as a novel high energy density material.

PubMed

Wang, Fang; Du, Hongchen; Zhang, Jianying; Gong, Xuedong

2011-10-27

Studies have suggested that octanitrocubane (ONC) is one of the most powerful non-nuclear high energy density material (HEDM) currently known. 2,4,6,8-Tetranitro-1,3,5,7-tetraazacubane (TNTAC) studied in this work may also be a novel HEDM due to its high nitrogen content and crystal density. Density functional theory and molecular mechanics methods have been employed to study the crystal structure, IR spectrum, electronic structure, thermodynamic properties, gas-phase and condensed-phase heat of formation, detonation performance, and pyrolysis mechanism of TNTAC. The TNTAC has a predicted density of about 2.12 g/cm(3), and its detonation velocity (10.42 km/s) and detonation pressure (52.82 GPa) are higher than that of ONC. The crystalline packing is P2(1)2(1)2(1), and the corresponding cell parameters are Z = 4, a = 8.87 Å, b = 8.87 Å, and c = 11.47 Å. Both the density of states of the predicted crystal and the bond dissociation energy of the molecule in gas phase show that the cage C-N bond is the trigger bond during thermolysis. The activation energy of the pyrolysis initiation reaction obtained from the B3LYP/6-311++G(2df,2p) level is 125.98 kJ/mol, which indicates that TNTAC meets the thermal stability request as an exploitable HEDM.

The use of salinity contrast for density difference compensation to improve the thermal recovery efficiency in high-temperature aquifer thermal energy storage systems

NASA Astrophysics Data System (ADS)

van Lopik, Jan H.; Hartog, Niels; Zaadnoordijk, Willem Jan

2016-08-01

The efficiency of heat recovery in high-temperature (>60 °C) aquifer thermal energy storage (HT-ATES) systems is limited due to the buoyancy of the injected hot water. This study investigates the potential to improve the efficiency through compensation of the density difference by increased salinity of the injected hot water for a single injection-recovery well scheme. The proposed method was tested through numerical modeling with SEAWATv4, considering seasonal HT-ATES with four consecutive injection-storage-recovery cycles. Recovery efficiencies for the consecutive cycles were investigated for six cases with three simulated scenarios: (a) regular HT-ATES, (b) HT-ATES with density difference compensation using saline water, and (c) theoretical regular HT-ATES without free thermal convection. For the reference case, in which 80 °C water was injected into a high-permeability aquifer, regular HT-ATES had an efficiency of 0.40 after four consecutive recovery cycles. The density difference compensation method resulted in an efficiency of 0.69, approximating the theoretical case (0.76). Sensitivity analysis showed that the net efficiency increase by using the density difference compensation method instead of regular HT-ATES is greater for higher aquifer hydraulic conductivity, larger temperature difference between injection water and ambient groundwater, smaller injection volume, and larger aquifer thickness. This means that density difference compensation allows the application of HT-ATES in thicker, more permeable aquifers and with larger temperatures than would be considered for regular HT-ATES systems.

An updated Lagrangian discontinuous Galerkin hydrodynamic method for gas dynamics

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wu, Tong; Shashkov, Mikhail Jurievich; Morgan, Nathaniel Ray

Here, we present a new Lagrangian discontinuous Galerkin (DG) hydrodynamic method for gas dynamics. The new method evolves conserved unknowns in the current configuration, which obviates the Jacobi matrix that maps the element in a reference coordinate system or the initial coordinate system to the current configuration. The density, momentum, and total energy (ρ, ρu, E) are approximated with conservative higher-order Taylor expansions over the element and are limited toward a piecewise constant field near discontinuities using a limiter. Two new limiting methods are presented for enforcing the bounds on the primitive variables of density, velocity, and specific internal energymore » (ρ, u, e). The nodal velocity, and the corresponding forces, are calculated by solving an approximate Riemann problem at the element nodes. An explicit second-order method is used to temporally advance the solution. This new Lagrangian DG hydrodynamic method conserves mass, momentum, and total energy. 1D Cartesian coordinates test problem results are presented to demonstrate the accuracy and convergence order of the new DG method with the new limiters.« less

An updated Lagrangian discontinuous Galerkin hydrodynamic method for gas dynamics

DOE PAGES

Wu, Tong; Shashkov, Mikhail Jurievich; Morgan, Nathaniel Ray; ...

2018-04-09

Here, we present a new Lagrangian discontinuous Galerkin (DG) hydrodynamic method for gas dynamics. The new method evolves conserved unknowns in the current configuration, which obviates the Jacobi matrix that maps the element in a reference coordinate system or the initial coordinate system to the current configuration. The density, momentum, and total energy (ρ, ρu, E) are approximated with conservative higher-order Taylor expansions over the element and are limited toward a piecewise constant field near discontinuities using a limiter. Two new limiting methods are presented for enforcing the bounds on the primitive variables of density, velocity, and specific internal energymore » (ρ, u, e). The nodal velocity, and the corresponding forces, are calculated by solving an approximate Riemann problem at the element nodes. An explicit second-order method is used to temporally advance the solution. This new Lagrangian DG hydrodynamic method conserves mass, momentum, and total energy. 1D Cartesian coordinates test problem results are presented to demonstrate the accuracy and convergence order of the new DG method with the new limiters.« less

Dynamical mean-field theory, density-matrix embedding theory, and rotationally invariant slave bosons: A unified perspective

NASA Astrophysics Data System (ADS)

Ayral, Thomas; Lee, Tsung-Han; Kotliar, Gabriel

2017-12-01

We present a unified perspective on dynamical mean-field theory (DMFT), density-matrix embedding theory (DMET), and rotationally invariant slave bosons (RISB). We show that DMET can be regarded as a simplification of the RISB method where the quasiparticle weight is set to unity. This relation makes it easy to transpose extensions of a given method to another: For instance, a temperature-dependent version of RISB can be used to derive a temperature-dependent free-energy formula for DMET.

Method of sintering ceramic materials

DOEpatents

Holcombe, C.E.; Dykes, N.L.

1992-11-17

A method for sintering ceramic materials is described. A ceramic article is coated with layers of protective coatings such as boron nitride, graphite foil, and niobium. The coated ceramic article is embedded in a container containing refractory metal oxide granules and placed within a microwave oven. The ceramic article is heated by microwave energy to a temperature sufficient to sinter the ceramic article to form a densified ceramic article having a density equal to or greater than 90% of theoretical density. 2 figs.

Methods for converging correlation energies within the dielectric matrix formalism

NASA Astrophysics Data System (ADS)

Dixit, Anant; Claudot, Julien; Gould, Tim; Lebègue, Sébastien; Rocca, Dario

2018-03-01

Within the dielectric matrix formalism, the random-phase approximation (RPA) and analogous methods that include exchange effects are promising approaches to overcome some of the limitations of traditional density functional theory approximations. The RPA-type methods however have a significantly higher computational cost, and, similarly to correlated quantum-chemical methods, are characterized by a slow basis set convergence. In this work we analyzed two different schemes to converge the correlation energy, one based on a more traditional complete basis set extrapolation and one that converges energy differences by accounting for the size-consistency property. These two approaches have been systematically tested on the A24 test set, for six points on the potential-energy surface of the methane-formaldehyde complex, and for reaction energies involving the breaking and formation of covalent bonds. While both methods converge to similar results at similar rates, the computation of size-consistent energy differences has the advantage of not relying on the choice of a specific extrapolation model.

Suprathermal plasma analyzer for the measurement of low-energy electron distribution in the ionosphere.

PubMed

Shimoyama, M; Oyama, K-I; Abe, T; Yau, A W

2011-07-01

It is commonly believed that an energy transfer from thermal to suprathermal electrons (

Complex-energy approach to sum rules within nuclear density functional theory

DOE PAGES

Hinohara, Nobuo; Kortelainen, Markus; Nazarewicz, Witold; ...

2015-04-27

The linear response of the nucleus to an external field contains unique information about the effective interaction, correlations governing the behavior of the many-body system, and properties of its excited states. To characterize the response, it is useful to use its energy-weighted moments, or sum rules. By comparing computed sum rules with experimental values, the information content of the response can be utilized in the optimization process of the nuclear Hamiltonian or nuclear energy density functional (EDF). But the additional information comes at a price: compared to the ground state, computation of excited states is more demanding. To establish anmore » efficient framework to compute energy-weighted sum rules of the response that is adaptable to the optimization of the nuclear EDF and large-scale surveys of collective strength, we have developed a new technique within the complex-energy finite-amplitude method (FAM) based on the quasiparticle random- phase approximation. The proposed sum-rule technique based on the complex-energy FAM is a tool of choice when optimizing effective interactions or energy functionals. The method is very efficient and well-adaptable to parallel computing. As a result, the FAM formulation is especially useful when standard theorems based on commutation relations involving the nuclear Hamiltonian and external field cannot be used.« less

Investigation of radiological properties of some shielding materials on charged and uncharged radiation interaction for neutron generator

NASA Astrophysics Data System (ADS)

Büyükyıldız, Mehmet

2017-04-01

Radiation interaction parameters such as total stopping power, projected range (longitudinal and lateral) straggling, mass attenuation coefficient, effective atomic number (Zeff) and electron density (Neff) of some shielding materials were investigated for photon and heavy charged particle interactions. The ranges, stragglings and mass attenuation coefficients were calculated for the high-density polyethylene(HDPE), borated polyethylene (BPE), brick (common silica), concrete (regular), wood, water, stainless steel (304), aluminum (alloy 6061-O), lead and bismuth using SRIM Monte Carlo software and WinXCom program. In addition, effective atomic numbers (Zeff) and electron densities (Neff) of HDPE, BPE, brick (common silica), concrete (regular), wood, water, stainless steel (304) and aluminum (alloy 6061-O) were calculated in the energy region 10 keV-100 MeV using mass stopping powers and mass attenuation coefficients. Two different methods namely direct and interpolation procedures were used to calculate Zeff for comparison and significant differences were determined between the methods. Variations of the ranges, longitudinal and lateral stragglings of water, concrete and stainless steel (304) were compared with each other in the continuous kinetic energy region and discussed with respect to their Zeffs. Moreover, energy absorption buildup factors (EABF) and exposure buildup factors (EBF) of the materials were determined for gamma rays as well and were compared with each other for different photon energies and different mfps in the photon energy region 0.015-15 MeV.

Intuitive Density Functional Theory-Based Energy Decomposition Analysis for Protein-Ligand Interactions.

PubMed

Phipps, M J S; Fox, T; Tautermann, C S; Skylaris, C-K

2017-04-11

First-principles quantum mechanical calculations with methods such as density functional theory (DFT) allow the accurate calculation of interaction energies between molecules. These interaction energies can be dissected into chemically relevant components such as electrostatics, polarization, and charge transfer using energy decomposition analysis (EDA) approaches. Typically EDA has been used to study interactions between small molecules; however, it has great potential to be applied to large biomolecular assemblies such as protein-protein and protein-ligand interactions. We present an application of EDA calculations to the study of ligands that bind to the thrombin protein, using the ONETEP program for linear-scaling DFT calculations. Our approach goes beyond simply providing the components of the interaction energy; we are also able to provide visual representations of the changes in density that happen as a result of polarization and charge transfer, thus pinpointing the functional groups between the ligand and protein that participate in each kind of interaction. We also demonstrate with this approach that we can focus on studying parts (fragments) of ligands. The method is relatively insensitive to the protocol that is used to prepare the structures, and the results obtained are therefore robust. This is an application to a real protein drug target of a whole new capability where accurate DFT calculations can produce both energetic and visual descriptors of interactions. These descriptors can be used to provide insights for tailoring interactions, as needed for example in drug design.

Material engineering to fabricate rare earth erbium thin films for exploring nuclear energy sources

NASA Astrophysics Data System (ADS)

Banerjee, A.; Abhilash, S. R.; Umapathy, G. R.; Kabiraj, D.; Ojha, S.; Mandal, S.

2018-04-01

High vacuum evaporation and cold-rolling techniques to fabricate thin films of the rare earth lanthanide-erbium have been discussed in this communication. Cold rolling has been used for the first time to successfully fabricate films of enriched and highly expensive erbium metal with areal density in the range of 0.5-1.0 mg/cm2. The fabricated films were used as target materials in an advanced nuclear physics experiment. The experiment was designed to investigate isomeric states in the heavy nuclei mass region for exploring physics related to nuclear energy sources. The films fabricated using different techniques varied in thickness as well as purity. Methods to fabricate films with thickness of the order of 0.9 mg/cm2 were different than those of 0.4 mg/cm2 areal density. All the thin films were characterized using multiple advanced techniques to accurately ascertain levels of contamination as well as to determine their exact surface density. Detailed fabrication methods as well as characterization techniques have been discussed.

Recent progress in density functional theory

NASA Astrophysics Data System (ADS)

Truhlar, Donald

2014-03-01

Ongoing work involves several areas of density functional theory: new methods for computing electronic excitation energies, including a new way to remove spin contamination in the spin-flip Tamm-Dancoff approximation and a configuration-interaction-corrected Tamm-Dancoff Approximation for treating conical intersections; new ways to treat open-shell states, including a reinterpreted broken-symmetry method and multi-configuration Kohn-Sham theory; a new exchange-correlation functional; new tests of density functional theory against databases for electronic transition energies and molecules and solids containing metal atoms; and applications. A selection of results will be presented. I am grateful to the following collaborators for contributions to the ongoing work: Boris Averkiev, Rebecca Carlson, Laura Fernandez, Laura Gagliardi, Chad Hoyer, Francesc Illas, Miho Isegawa, Shaohong Li, Giovanni Li Manni, Sijie Luo, Dongxia Ma, Remi Maurice, Rubén Means-Pañeda, Roberto Peverati, Nora Planas, Prasenjit Seal, Pragya Verma, Bo Wang, Xuefei Xu, Ke R. Yang, Haoyu Yu, Wenjing Zhang, and Jingjing Zheng. Supported in part by the AFOSR and U.S. DOE.

Modifying Current Collectors to Produce High Volumetric Energy Density and Power Density Storage Devices.

PubMed

Khani, Hadi; Dowell, Timothy J; Wipf, David O

2018-06-27

We develop zirconium-templated NiO/NiOOH nanosheets on nickel foam and polypyrrole-embedded in exfoliated carbon fiber cloth as complementary electrodes for an asymmetric battery-type supercapacitor device. We achieve high volumetric energy and power density by the modification of commercially available current collectors (CCs). The modified CCs provide the source of active material, actively participate in the charge storage process, provide a larger surface area for active material loading, need no additional binders or conductive additives, and retain the ability to act as the CC. Nickel foam (NF) CCs are modified by use of a soft-templating/solvothermal treatment to generate NiO/NiOOH nanosheets, where the NF is the source of Ni for the synthesis. Carbon-fiber cloth (CFC) CCs are modified by an electrochemical oxidation/reduction process to generate exfoliated core-shell structures (ECFC). Electropolymerization of pyrrole into the shell structure produces polypyrrole embedded in exfoliated core-shell material (PPy@rECFC). Battery-type supercapacitor devices are produced with NiO/NiOOH@NF and PPy@rECFC as positive and negative electrodes, respectively, to demonstrate the utility of this approach. Volumetric energy densities for the full-cell device are in the range of 2.60-4.12 mWh cm -3 with corresponding power densities in the range of 9.17-425.58 mW cm -3 . This is comparable to thin-film lithium-ion batteries (0.3-10 mWh cm -3 ) and better than some commercial supercapacitors (<1 mWh cm -3 ). 1 The energy and power density is impressive considering that it was calculated using the entire cell volume (active materials, separator, and both CCs). The full-cell device is highly stable, retaining 96% and 88% of capacity after 2000 and 5000 cycles, respectively. These results demonstrate the utility of directly modifying the CCs and suggest a new method to produce high volumetric energy density and power density storage devices.

Short-range density functional correlation within the restricted active space CI method

NASA Astrophysics Data System (ADS)

Casanova, David

2018-03-01

In the present work, I introduce a hybrid wave function-density functional theory electronic structure method based on the range separation of the electron-electron Coulomb operator in order to recover dynamic electron correlations missed in the restricted active space configuration interaction (RASCI) methodology. The working equations and the computational algorithm for the implementation of the new approach, i.e., RAS-srDFT, are presented, and the method is tested in the calculation of excitation energies of organic molecules. The good performance of the RASCI wave function in combination with different short-range exchange-correlation functionals in the computation of relative energies represents a quantitative improvement with respect to the RASCI results and paves the path for the development of RAS-srDFT as a promising scheme in the computation of the ground and excited states where nondynamic and dynamic electron correlations are important.

Method for adhesion of metal films to ceramics

DOEpatents

Lowndes, Douglas H.; Pedraza, Anthony J.; DeSilva, Melvin J.; Kumar, Rajagopalan A.

1997-01-01

Methods for making strongly bonded metal-ceramic materials. The methods include irradiating a portion of the surface of the ceramic material with a pulsed ultraviolet laser having an energy density sufficient to effect activation of the irradiated surface of the ceramic material so that adhesion of metals subsequently deposited onto the irradiated surface is substantially increased. Advantages of the invention include (i) the need for only a small number of laser pulses at relatively low focused energy density, (ii) a smoother substrate surface, (iii) activation of the laser-treated surface which provides a chemical bond between the surface and a metal deposited thereon, (iv) only low temperature annealing is required to produce the strong metal-ceramic bond; (v) the ability to obtain strong adhesion between ceramic materials and oxidation resistant metals; (vi) ability to store the laser treated ceramic materials for later deposition of metals thereon.

Method for adhesion of metal films to ceramics

DOEpatents

Lowndes, D.H.; Pedraza, A.J.; DeSilva, M.J.; Kumar, R.A.

1997-12-30

Methods for making strongly bonded metal-ceramic materials are disclosed. The methods include irradiating a portion of the surface of the ceramic material with a pulsed ultraviolet laser having an energy density sufficient to effect activation of the irradiated surface of the ceramic material so that adhesion of metals subsequently deposited onto the irradiated surface is substantially increased. Advantages of the invention include (i) the need for only a small number of laser pulses at relatively low focused energy density, (ii) a smoother substrate surface, (iii) activation of the laser-treated surface which provides a chemical bond between the surface and a metal deposited thereon, (iv) only low temperature annealing is required to produce the strong metal-ceramic bond; (v) the ability to obtain strong adhesion between ceramic materials and oxidation resistant metals; (vi) ability to store the laser treated ceramic materials for later deposition of metals thereon. 7 figs.

Energy Density, Nutrient Adequacy, and Cost per Serving Can Provide Insight into Food Choices in the Lower Mississippi Delta

ERIC Educational Resources Information Center

Connell, Carol L.; Zoellner, Jamie M.; Yadrick, M. Kathleen; Chekuri, Srinivasa C.; Crook, Lashaundrea B.; Bogle, Margaret L.

2012-01-01

Objective: To compare differences across food groups for food cost, energy, and nutrient profiles of 100 items from a cross-sectional survey of 225 stores in 18 counties across the Lower Mississippi Delta of Arkansas, Louisiana, and Mississippi. Methods: Energy, nutrient, and cost profiles for food items were calculated by using Naturally Nutrient…

Characterizing Bonding Patterns in Diradicals and Triradicals by Density-Based Wave Function Analysis: A Uniform Approach.

PubMed

Orms, Natalie; Rehn, Dirk R; Dreuw, Andreas; Krylov, Anna I

2018-02-13

Density-based wave function analysis enables unambiguous comparisons of the electronic structure computed by different methods and removes ambiguity of orbital choices. We use this tool to investigate the performance of different spin-flip methods for several prototypical diradicals and triradicals. In contrast to previous calibration studies that focused on energy gaps between high- and low spin-states, we focus on the properties of the underlying wave functions, such as the number of effectively unpaired electrons. Comparison of different density functional and wave function theory results provides insight into the performance of the different methods when applied to strongly correlated systems such as polyradicals. We show that canonical molecular orbitals for species like large copper-containing diradicals fail to correctly represent the underlying electronic structure due to highly non-Koopmans character, while density-based analysis of the same wave function delivers a clear picture of the bonding pattern.

Silicon-Based Lithium-Ion Capacitor for High Energy and High Power Application

NASA Technical Reports Server (NTRS)

Wu, James J.; Demattia, Brianne; Loyselle, Patricia; Reid, Concha; Kohout, Lisa

2017-01-01

Si-based Li-ion capacitor has been developed and demonstrated. The results show it is feasible to improve both power density and energy density in this configuration. The applied current density impacts the power and energy density: low current favors energy density while high current favors power density. Active carbon has a better rate capability than Si. Next StepsFuture Directions. Si electrode needs to be further studied and improved. Further optimization of SiAC ratio and evaluation of its impact on energy density and power density.

Ionic Liquid Directed Mesoporous Carbon Nanoflakes as an Effiencient Electrode material

NASA Astrophysics Data System (ADS)

Kong, Lirong; Chen, Wei

2015-12-01

Supercapacitors are considered to be the most promising approach to meet the pressing requirements for energy storage devices. The electrode materials for supercapacitors have close relationship with their electrochemical properties and thus become the key point to improve their energy storage efficiency. Herein, by using poly (vinylidene fluoride-co-hexafluoropropylene) and ionic liquid as the dual templates, polyacrylonitrile as the carbon precursor, a flake-like carbon material was prepared by a direct carbonization method. In this method, poly (vinylidene fluoride-co-hexafluoropropylene) worked as the separator for the formation of isolated carbon flakes while aggregated ionic liquid worked as the pore template. The obtained carbon flakes exhibited a specific capacitance of 170 F/g at 0.1 A/g, a high energy density of 12.2 Wh/kg and a high power density of 5 kW/kg at the current of 10 A/g. It also maintained a high capacitance retention capability with almost no declination after 500 charge-discharge cycles. The ionic liquid directed method developed here also provided a new idea for the preparation of hierarchically porous carbon nanomaterials.

Molecular structure and spectroscopic characterization of Carbamazepine with experimental techniques and DFT quantum chemical calculations

NASA Astrophysics Data System (ADS)

Suhasini, M.; Sailatha, E.; Gunasekaran, S.; Ramkumaar, G. R.

2015-04-01

A systematic vibrational spectroscopic assignment and analysis of Carbamazepine has been carried out by using FT-IR, FT-Raman and UV spectral data. The vibrational analysis were aided by electronic structure calculations - ab initio (RHF) and hybrid density functional methods (B3LYP) performed with standard basis set 6-31G(d,p). Molecular equilibrium geometries, electronic energies, natural bond order analysis, harmonic vibrational frequencies and IR intensities have been computed. A detailed interpretation of the vibrational spectra of the molecule has been made on the basis of the calculated Potential Energy Distribution (PED) by VEDA program. UV-visible spectrum of the compound was also recorded and the electronic properties, such as HOMO and LUMO energies and λmax were determined by HF/6-311++G(d,p) Time-Dependent method. The thermodynamic functions of the title molecule were also performed using the RHF and DFT methods. The restricted Hartree-Fock and density functional theory-based nuclear magnetic resonance (NMR) calculation procedure was also performed, and it was used for assigning the 13C and 1H NMR chemical shifts of Carbamazepine.

Sensitivity analysis of a coupled hydrodynamic-vegetation model using the effectively subsampled quadratures method

USGS Publications Warehouse

Kalra, Tarandeep S.; Aretxabaleta, Alfredo; Seshadri, Pranay; Ganju, Neil K.; Beudin, Alexis

2017-01-01

Coastal hydrodynamics can be greatly affected by the presence of submerged aquatic vegetation. The effect of vegetation has been incorporated into the Coupled-Ocean-Atmosphere-Wave-Sediment Transport (COAWST) Modeling System. The vegetation implementation includes the plant-induced three-dimensional drag, in-canopy wave-induced streaming, and the production of turbulent kinetic energy by the presence of vegetation. In this study, we evaluate the sensitivity of the flow and wave dynamics to vegetation parameters using Sobol' indices and a least squares polynomial approach referred to as Effective Quadratures method. This method reduces the number of simulations needed for evaluating Sobol' indices and provides a robust, practical, and efficient approach for the parameter sensitivity analysis. The evaluation of Sobol' indices shows that kinetic energy, turbulent kinetic energy, and water level changes are affected by plant density, height, and to a certain degree, diameter. Wave dissipation is mostly dependent on the variation in plant density. Performing sensitivity analyses for the vegetation module in COAWST provides guidance for future observational and modeling work to optimize efforts and reduce exploration of parameter space.

The size effect to O2- -Ce4+ charge transfer emission and band gap structure of Sr2 CeO4.

PubMed

Wang, Wenjun; Pan, Yu; Zhang, Wenying; Liu, Xiaoguang; Li, Ling

2018-04-24

Sr 2 CeO 4 phosphors with different crystalline sizes were synthesized by the sol-gel method or the solid-state reaction. Their crystalline size, luminescence intensity of O 2- -Ce 4+ charge transfer and energy gaps were obtained through the characterization by X-ray diffraction, photoluminescence spectra, as well as UV-visible diffuse reflectance measurements. An inverse relationship between photoluminescence (PL) spectra and crystalline size was observed when the heating temperature was from 1000°C to 1300°C. In addition, band energy calculated for all samples showed that a reaction temperature of 1200°C for the solid-state method and 1100°C for sol-gel method gave the largest values, which corresponded with the smallest crystalline size. Correlation between PL intensity and crystalline size showed an inverse relationship. Band structure, density of states and partial density of states of the crystal were calculated to analyze the mechanism using the cambrige sequential total energy package (CASTEP) module integrated with Materials Studio software. Copyright © 2018 John Wiley & Sons, Ltd.

Basis convergence of range-separated density-functional theory.

PubMed

Franck, Odile; Mussard, Bastien; Luppi, Eleonora; Toulouse, Julien

2015-02-21

Range-separated density-functional theory (DFT) is an alternative approach to Kohn-Sham density-functional theory. The strategy of range-separated density-functional theory consists in separating the Coulomb electron-electron interaction into long-range and short-range components and treating the long-range part by an explicit many-body wave-function method and the short-range part by a density-functional approximation. Among the advantages of using many-body methods for the long-range part of the electron-electron interaction is that they are much less sensitive to the one-electron atomic basis compared to the case of the standard Coulomb interaction. Here, we provide a detailed study of the basis convergence of range-separated density-functional theory. We study the convergence of the partial-wave expansion of the long-range wave function near the electron-electron coalescence. We show that the rate of convergence is exponential with respect to the maximal angular momentum L for the long-range wave function, whereas it is polynomial for the case of the Coulomb interaction. We also study the convergence of the long-range second-order Møller-Plesset correlation energy of four systems (He, Ne, N2, and H2O) with cardinal number X of the Dunning basis sets cc - p(C)V XZ and find that the error in the correlation energy is best fitted by an exponential in X. This leads us to propose a three-point complete-basis-set extrapolation scheme for range-separated density-functional theory based on an exponential formula.

Non-aqueous hybrid supercapacitors fabricated with mesoporous TiO2 microspheres and activated carbon electrodes with superior performance

NASA Astrophysics Data System (ADS)

Cai, Yong; Zhao, Bote; Wang, Jie; Shao, Zongping

2014-05-01

Mesoporous TiO2 microspheres, synthesized by a facile template-free solvothermal method and subsequent heat treatment, are exploited as the electrode for hybrid supercapacitors. The effects of the calcination temperature on the phase composition, particulate microstructure and morphology are characterized by XRD, Raman, FE-SEM and N2 adsorption/desorption measurements. Hybrid supercapacitors utilizing the as-prepared TiO2 mesoporous microspheres as the negative electrode and activated carbon (AC) as the positive electrode in a non-aqueous electrolyte are fabricated. The electrochemical performance of these hybrid supercapacitors is studied by galvanostatic charge-discharge and cyclic voltammetry (CV). The hybrid supercapacitor built from TiO2 microspheres calcined at 400 °C shows the best performance, delivering an energy density of 79.3 Wh kg-1 at a power density of 178.1 W kg-1. Even at a power density of 9.45 kW kg-1, an energy density of 31.5 Wh kg-1 is reached. These values are much higher than the AC-AC symmetric supercapacitor. In addition, the hybrid supercapacitor exhibits excellent cycling performance, retaining 98% of the initial energy density after 1000 cycles. Such outstanding electrochemical performance of the hybrid supercapacitor is attributed to the matched reaction kinetics between the two electrodes with different energy storage mechanisms.

Effects of thermal treatment on energy density and hardness of torrefied wood pellets

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peng, Jianghong; Wang, Jingsong; Bi, Xiaotao T.

Here, three types of wood pellets samples, including two types of commercial pellets and one type of lab-made control pellets were torrefied in a fixed bed unit to study the effect of thermal pretreatment on the quality of wood pellets. The quality of wood pellets was mainly characterized by the pellet density, bulk density, higher heating value, Meyer hardness, saturated moisture uptake, volumetric energy density, and energy yield. Results showed that torrefaction significantly decreased the pellet density, hardness, volumetric energy density, and energy yield. The higher heating value increased and the saturated moisture content decreased after torrefaction. In view ofmore » the lower density, lower hardness, lower volumetric energy density, and energy yield of torrefied pellets, it is recommended that biomass should be torrefied and then compressed to make strong pellets of high hydrophobicity and volumetric energy density.« less

Effects of thermal treatment on energy density and hardness of torrefied wood pellets

DOE PAGES

Peng, Jianghong; Wang, Jingsong; Bi, Xiaotao T.; ...

2014-09-27

Here, three types of wood pellets samples, including two types of commercial pellets and one type of lab-made control pellets were torrefied in a fixed bed unit to study the effect of thermal pretreatment on the quality of wood pellets. The quality of wood pellets was mainly characterized by the pellet density, bulk density, higher heating value, Meyer hardness, saturated moisture uptake, volumetric energy density, and energy yield. Results showed that torrefaction significantly decreased the pellet density, hardness, volumetric energy density, and energy yield. The higher heating value increased and the saturated moisture content decreased after torrefaction. In view ofmore » the lower density, lower hardness, lower volumetric energy density, and energy yield of torrefied pellets, it is recommended that biomass should be torrefied and then compressed to make strong pellets of high hydrophobicity and volumetric energy density.« less

Thermodynamic neutral density: A new physically-based, energy-constrained, materially conserved neutral density variable for quantifying mixing and tracking water masses in the ocean

NASA Astrophysics Data System (ADS)

Tailleux, R.

2016-02-01

A new materially-conserved quasi-neutral density variable has been constructed, called thermodynamic neutral density. It is composed of two parts. The first part is the Lorenz reference density entering Lorenz theory of available potential energy, which can be interpreted as the potential density of a fluid parcel referenced to the pressure it would have in Lorenz reference state of minimum potential energy. The second part is an empirical correction for pressure, which can be suitably chosen to make thermodynamic neutral density a very good approximation of Jackett and McDougall (1997) neutral density over most of the ocean water masses for which the latter is defined. Thermodynamic neutral density possesses many advantages over the empirically constructed Jackett and McDougall (1997) neutral density: 1) it is physically-based; 2) it is easily computed using fast and efficient methods for arbitrary states of the ocean, not just the present state, using the recently developed methodology by Saenz et al. (2015); 3) it is exactly neutral in a state of rest, and approximately neutral in the present ocean; 4) it is exactly materially conserved (it is a function of salinity and potential temperature only) and not plagued by unphysical nonmaterial effects, so can be used unambiguously to define and diagnose diapycnal and isopycnal mixing; 5) it is based on available potential energy, and therefore is the most suitable variable to discuss the energy cost of adiabatic stirring; 6) it is the variable that should be used to define the isopycnal and diapycnal directions in rotated diffusion tensor, as it can be shown that using the directions defined by the local neutral tangent plane as currently done causes spurious destruction of water masses. References: J. A. Saenz, R. Tailleux, E.D. Butler, G.O. Hughes, and K.I.C. Oliver, 2015: Estimating Lorenz's reference state in an ocean with a nonlinear equation of state for seawater. J. Phys. Oceanogr., 45, 1242—1257

Asymptotics of the monomer-dimer model on two-dimensional semi-infinite lattices

NASA Astrophysics Data System (ADS)

Kong, Yong

2007-05-01

By using the asymptotic theory of Pemantle and Wilson [R. Pemantle and M. C. Wilson, J. Comb. Theory, Ser. AJCBTA70097-316510.1006/jcta.2001.3201 97, 129 (2002)], asymptotic expansions of the free energy of the monomer-dimer model on two-dimensional semi-infinite ∞×n lattices in terms of dimer density are obtained for small values of n , at both high- and low-dimer-density limits. In the high-dimer-density limit, the theoretical results confirm the dependence of the free energy on the parity of n , a result obtained previously by computational methods by Y. Kong [Y. Kong, Phys. Rev. EPLEEE81063-651X10.1103/PhysRevE.74.061102 74, 061102 (2006); Phys. Rev. EPLEEE81063-651X10.1103/PhysRevE.73.016106 73, 016106 (2006);Phys. Rev. EPLEEE81063-651X10.1103/PhysRevE.74.011102 74, 011102 (2006)]. In the low-dimer-density limit, the free energy on a cylinder ∞×n lattice strip has exactly the same first n terms in the series expansion as that of an infinite ∞×∞ lattice.

Stochastic Optimally Tuned Range-Separated Hybrid Density Functional Theory.

PubMed

Neuhauser, Daniel; Rabani, Eran; Cytter, Yael; Baer, Roi

2016-05-19

We develop a stochastic formulation of the optimally tuned range-separated hybrid density functional theory that enables significant reduction of the computational effort and scaling of the nonlocal exchange operator at the price of introducing a controllable statistical error. Our method is based on stochastic representations of the Coulomb convolution integral and of the generalized Kohn-Sham density matrix. The computational cost of the approach is similar to that of usual Kohn-Sham density functional theory, yet it provides a much more accurate description of the quasiparticle energies for the frontier orbitals. This is illustrated for a series of silicon nanocrystals up to sizes exceeding 3000 electrons. Comparison with the stochastic GW many-body perturbation technique indicates excellent agreement for the fundamental band gap energies, good agreement for the band edge quasiparticle excitations, and very low statistical errors in the total energy for large systems. The present approach has a major advantage over one-shot GW by providing a self-consistent Hamiltonian that is central for additional postprocessing, for example, in the stochastic Bethe-Salpeter approach.

Influence of sample preparation on the transformation of low-density to high-density amorphous ice: An explanation based on the potential energy landscape

NASA Astrophysics Data System (ADS)

Giovambattista, Nicolas; Starr, Francis W.; Poole, Peter H.

2017-07-01

Experiments and computer simulations of the transformations of amorphous ices display different behaviors depending on sample preparation methods and on the rates of change of temperature and pressure to which samples are subjected. In addition to these factors, simulation results also depend strongly on the chosen water model. Using computer simulations of the ST2 water model, we study how the sharpness of the compression-induced transition from low-density amorphous ice (LDA) to high-density amorphous ice (HDA) is influenced by the preparation of LDA. By studying LDA samples prepared using widely different procedures, we find that the sharpness of the LDA-to-HDA transformation is correlated with the depth of the initial LDA sample in the potential energy landscape (PEL), as characterized by the inherent structure energy. Our results show that the complex phenomenology of the amorphous ices reported in experiments and computer simulations can be understood and predicted in a unified way from knowledge of the PEL of the system.

A method to estimate statistical errors of properties derived from charge-density modelling

PubMed Central

Lecomte, Claude

2018-01-01

Estimating uncertainties of property values derived from a charge-density model is not straightforward. A methodology, based on calculation of sample standard deviations (SSD) of properties using randomly deviating charge-density models, is proposed with the MoPro software. The parameter shifts applied in the deviating models are generated in order to respect the variance–covariance matrix issued from the least-squares refinement. This ‘SSD methodology’ procedure can be applied to estimate uncertainties of any property related to a charge-density model obtained by least-squares fitting. This includes topological properties such as critical point coordinates, electron density, Laplacian and ellipticity at critical points and charges integrated over atomic basins. Errors on electrostatic potentials and interaction energies are also available now through this procedure. The method is exemplified with the charge density of compound (E)-5-phenylpent-1-enylboronic acid, refined at 0.45 Å resolution. The procedure is implemented in the freely available MoPro program dedicated to charge-density refinement and modelling. PMID:29724964

Solar energy in the context of energy use, energy transportation and energy storage.

PubMed

MacKay, David J C

2013-08-13

Taking the UK as a case study, this paper describes current energy use and a range of sustainable energy options for the future, including solar power and other renewables. I focus on the area involved in collecting, converting and delivering sustainable energy, looking in particular detail at the potential role of solar power. Britain consumes energy at a rate of about 5000 watts per person, and its population density is about 250 people per square kilometre. If we multiply the per capita energy consumption by the population density, then we obtain the average primary energy consumption per unit area, which for the UK is 1.25 watts per square metre. This areal power density is uncomfortably similar to the average power density that could be supplied by many renewables: the gravitational potential energy of rainfall in the Scottish highlands has a raw power per unit area of roughly 0.24 watts per square metre; energy crops in Europe deliver about 0.5 watts per square metre; wind farms deliver roughly 2.5 watts per square metre; solar photovoltaic farms in Bavaria, Germany, and Vermont, USA, deliver 4 watts per square metre; in sunnier locations, solar photovoltaic farms can deliver 10 watts per square metre; concentrating solar power stations in deserts might deliver 20 watts per square metre. In a decarbonized world that is renewable-powered, the land area required to maintain today's British energy consumption would have to be similar to the area of Britain. Several other high-density, high-consuming countries are in the same boat as Britain, and many other countries are rushing to join us. Decarbonizing such countries will only be possible through some combination of the following options: the embracing of country-sized renewable power-generation facilities; large-scale energy imports from country-sized renewable facilities in other countries; population reduction; radical efficiency improvements and lifestyle changes; and the growth of non-renewable low-carbon sources, namely 'clean' coal, 'clean' gas and nuclear power. If solar is to play a large role in the future energy system, then we need new methods for energy storage; very-large-scale solar either would need to be combined with electricity stores or it would need to serve a large flexible demand for energy that effectively stores useful energy in the form of chemicals, heat, or cold.

Communication: Charge-population based dispersion interactions for molecules and materials

DOE Office of Scientific and Technical Information (OSTI.GOV)

Stöhr, Martin; Department Chemie, Technische Universität München, Lichtenbergstr. 4, D-85748 Garching; Michelitsch, Georg S.

2016-04-21

We introduce a system-independent method to derive effective atomic C{sub 6} coefficients and polarizabilities in molecules and materials purely from charge population analysis. This enables the use of dispersion-correction schemes in electronic structure calculations without recourse to electron-density partitioning schemes and expands their applicability to semi-empirical methods and tight-binding Hamiltonians. We show that the accuracy of our method is en par with established electron-density partitioning based approaches in describing intermolecular C{sub 6} coefficients as well as dispersion energies of weakly bound molecular dimers, organic crystals, and supramolecular complexes. We showcase the utility of our approach by incorporation of the recentlymore » developed many-body dispersion method [Tkatchenko et al., Phys. Rev. Lett. 108, 236402 (2012)] into the semi-empirical density functional tight-binding method and propose the latter as a viable technique to study hybrid organic-inorganic interfaces.« less

A Kernel-Free Particle-Finite Element Method for Hypervelocity Impact Simulation. Chapter 4

NASA Technical Reports Server (NTRS)

Park, Young-Keun; Fahrenthold, Eric P.

2004-01-01

An improved hybrid particle-finite element method has been developed for the simulation of hypervelocity impact problems. Unlike alternative methods, the revised formulation computes the density without reference to any kernel or interpolation functions, for either the density or the rate of dilatation. This simplifies the state space model and leads to a significant reduction in computational cost. The improved method introduces internal energy variables as generalized coordinates in a new formulation of the thermomechanical Lagrange equations. Example problems show good agreement with exact solutions in one dimension and good agreement with experimental data in a three dimensional simulation.

Properties of Augmented Kohn-Sham Potential for Energy as Simple Sum of Orbital Energies.

PubMed

Zahariev, Federico; Levy, Mel

2017-01-12

A recent modification to the traditional Kohn-Sham method ( Levy , M. ; Zahariev , F. Phys. Rev. Lett. 2014 , 113 , 113002 ; Levy , M. ; Zahariev , F. Mol. Phys. 2016 , 114 , 1162 - 1164 ), which gives the ground-state energy as a direct sum of the occupied orbital energies, is discussed and its properties are numerically illustrated on representative atoms and ions. It is observed that current approximate density functionals tend to give surprisingly small errors for the highest occupied orbital energies that are obtained with the augmented potential. The appropriately shifted Kohn-Sham potential is the basic object within this direct-energy Kohn-Sham method and needs to be approximated. To facilitate approximations, several constraints to the augmented Kohn-Sham potential are presented.

A real-space stochastic density matrix approach for density functional electronic structure.

PubMed

Beck, Thomas L

2015-12-21

The recent development of real-space grid methods has led to more efficient, accurate, and adaptable approaches for large-scale electrostatics and density functional electronic structure modeling. With the incorporation of multiscale techniques, linear-scaling real-space solvers are possible for density functional problems if localized orbitals are used to represent the Kohn-Sham energy functional. These methods still suffer from high computational and storage overheads, however, due to extensive matrix operations related to the underlying wave function grid representation. In this paper, an alternative stochastic method is outlined that aims to solve directly for the one-electron density matrix in real space. In order to illustrate aspects of the method, model calculations are performed for simple one-dimensional problems that display some features of the more general problem, such as spatial nodes in the density matrix. This orbital-free approach may prove helpful considering a future involving increasingly parallel computing architectures. Its primary advantage is the near-locality of the random walks, allowing for simultaneous updates of the density matrix in different regions of space partitioned across the processors. In addition, it allows for testing and enforcement of the particle number and idempotency constraints through stabilization of a Feynman-Kac functional integral as opposed to the extensive matrix operations in traditional approaches.

Fast Computation of Solvation Free Energies with Molecular Density Functional Theory: Thermodynamic-Ensemble Partial Molar Volume Corrections.

PubMed

Sergiievskyi, Volodymyr P; Jeanmairet, Guillaume; Levesque, Maximilien; Borgis, Daniel

2014-06-05

Molecular density functional theory (MDFT) offers an efficient implicit-solvent method to estimate molecule solvation free-energies, whereas conserving a fully molecular representation of the solvent. Even within a second-order approximation for the free-energy functional, the so-called homogeneous reference fluid approximation, we show that the hydration free-energies computed for a data set of 500 organic compounds are of similar quality as those obtained from molecular dynamics free-energy perturbation simulations, with a computer cost reduced by 2-3 orders of magnitude. This requires to introduce the proper partial volume correction to transform the results from the grand canonical to the isobaric-isotherm ensemble that is pertinent to experiments. We show that this correction can be extended to 3D-RISM calculations, giving a sound theoretical justification to empirical partial molar volume corrections that have been proposed recently.

Dodging the dark matter degeneracy while determining the dynamics of dark energy

NASA Astrophysics Data System (ADS)

Busti, Vinicius C.; Clarkson, Chris

2016-05-01

One of the key issues in cosmology is to establish the nature of dark energy, and to determine whether the equation of state evolves with time. When estimating this from distance measurements there is a degeneracy with the matter density. We show that there exists a simple function of the dark energy equation of state and its first derivative which is independent of this degeneracy at all redshifts, and so is a much more robust determinant of the evolution of dark energy than just its derivative. We show that this function can be well determined at low redshift from supernovae using Gaussian Processes, and that this method is far superior to a variety of parameterisations which are also subject to priors on the matter density. This shows that parametrised models give very biased constraints on the evolution of dark energy.

Significantly Enhanced Energy Density in Nanocomposite Capacitors Combining the TiO2 Nanorod Array with Poly(vinylidene fluoride).

PubMed

Yao, Lingmin; Pan, Zhongbin; Liu, Shaohui; Zhai, Jiwei; Chen, Haydn H D

2016-10-05

A novel inorganic/polymer nanocomposite, using 1-dimensional TiO 2 nanorod array as fillers (TNA) and poly(vinylidene fluoride) (PVDF) as matrix, has been successfully synthesized for the first time. A carefully designed process sequence includes several steps with the initial epitaxial growth of highly oriented TNA on the fluorine-doped tin oxide (FTO) conductive glass. Subsequently, PVDF is embedded into the nanorods by the spin-coating method followed by annealing and quenching processes. This novel structure with dispersive fillers demonstrates a successful compromise between the electric displacement and breakdown strength, resulting in a dramatic increase in the electric polarization which leads to a significant improvement on the energy density and discharge efficiency. The nanocomposites with various height ratios of fillers between the TNA and total film thickness were investigated by us. The results show that nanocomposite with 18% height ratio fillers obtains maximum increase in the energy density (10.62 J cm -3 ) at a lower applied electric field of 340 MV m -1 , and it also illustrates a higher efficiency (>85%) under the electric field less than 100 MV m -1 . Even when the electric field reached 340 MV m -1 , the efficiency of nanocomposites can still maintained at ∼70%. This energy density exceeds most of the previously reported TiO 2 -based nanocomposite values at such a breakdown strength, which provides another promising design for the next generation of dielectric nanocomposite material, by using the highly oriented nanorod array as fillers for the higher energy density capacitors. Additionally, the finite element simulation has been employed to analyze the distribution of electric fields and electric flux density to explore the inherent mechanism of the higher performance of the TNA/PVDF nanocomposites.

Solar Illumination Control of the Polar Wind

NASA Astrophysics Data System (ADS)

Maes, L.; Maggiolo, R.; De Keyser, J.; André, M.; Eriksson, A. I.; Haaland, S.; Li, K.; Poedts, S.

2017-11-01

Polar wind outflow is an important process through which the ionosphere supplies plasma to the magnetosphere. The main source of energy driving the polar wind is solar illumination of the ionosphere. As a result, many studies have found a relation between polar wind flux densities and solar EUV intensity, but less is known about their relation to the solar zenith angle at the ionospheric origin, certainly at higher altitudes. The low energy of the outflowing particles and spacecraft charging means it is very difficult to measure the polar wind at high altitudes. We take advantage of an alternative method that allows estimations of the polar wind flux densities far in the lobes. We analyze measurements made by the Cluster spacecraft at altitudes from 4 up to 20 RE. We observe a strong dependence on the solar zenith angle in the ion flux density and see that both the ion velocity and density exhibit a solar zenith angle dependence as well. We also find a seasonal variation of the flux density.

Method for Predicting the Energy Characteristics of Li-Ion Cells Designed for High Specific Energy

NASA Technical Reports Server (NTRS)

Bennett, William, R.

2012-01-01

Novel electrode materials with increased specific capacity and voltage performance are critical to the NASA goals for developing Li-ion batteries with increased specific energy and energy density. Although performance metrics of the individual electrodes are critically important, a fundamental understanding of the interactions of electrodes in a full cell is essential to achieving the desired performance, and for establishing meaningful goals for electrode performance in the first place. This paper presents design considerations for matching positive and negative electrodes in a viable design. Methods for predicting cell-level performance, based on laboratory data for individual electrodes, are presented and discussed.

Communication: Biological applications of coupled-cluster frozen-density embedding

NASA Astrophysics Data System (ADS)

Heuser, Johannes; Höfener, Sebastian

2018-04-01

We report the implementation of the Laplace-transform scaled opposite-spin (LT-SOS) resolution-of-the-identity second-order approximate coupled-cluster singles and doubles (RICC2) combined with frozen-density embedding for excitation energies and molecular properties. In the present work, we furthermore employ the Hartree-Fock density for the interaction energy leading to a simplified Lagrangian which is linear in the Lagrangian multipliers. This approximation has the key advantage of a decoupling of the coupled-cluster amplitude and multipliers, leading also to a significant reduction in computation time. Using the new simplified Lagrangian in combination with efficient wavefunction models such as RICC2 or LT-SOS-RICC2 and density-functional theory (DFT) for the environment molecules (CC2-in-DFT) enables the efficient study of biological applications such as the rhodopsin and visual cone pigments using ab initio methods as routine applications.

A Density Functional Study of Atomic Hydrogen and Oxygen Chemisorptions on the (0001) Surface of Double Hexagonal Close Packed Americium

NASA Astrophysics Data System (ADS)

Dholabhai, Pratik; Atta-Fynn, Raymond; Ray, Asok

2008-03-01

Ab initio total energy calculations within the framework of density functional theory have been performed for atomic hydrogen and oxygen chemisorptions on the (0001) surface of double hexagonal packed americium using a full-potential all-electron linearized augmented plane wave plus local orbitals (FLAPW+lo) method. The three-fold hollow hcp site was found to be the most stable site for H adsorption, while the two-fold bridge adsorption site was found to be the most stable site for O adsorption. Chemisorption energies and adsorption geometries for different adsorption sites will be discussed. The change in work functions, magnetic moments, partial charges inside muffin-tins, difference charge density distributions and density of states for the bare Am slab and the Am slab after adsorption of the adatom will be discussed. The implications of chemisorption on Am 5f electron localization-delocalization will also be discussed.

Screened exchange hybrid density functional for accurate and efficient structures and interaction energies.

PubMed

Brandenburg, Jan Gerit; Caldeweyher, Eike; Grimme, Stefan

2016-06-21

We extend the recently introduced PBEh-3c global hybrid density functional [S. Grimme et al., J. Chem. Phys., 2015, 143, 054107] by a screened Fock exchange variant based on the Henderson-Janesko-Scuseria exchange hole model. While the excellent performance of the global hybrid is maintained for small covalently bound molecules, its performance for computed condensed phase mass densities is further improved. Most importantly, a speed up of 30 to 50% can be achieved and especially for small orbital energy gap cases, the method is numerically much more robust. The latter point is important for many applications, e.g., for metal-organic frameworks, organic semiconductors, or protein structures. This enables an accurate density functional based electronic structure calculation of a full DNA helix structure on a single core desktop computer which is presented as an example in addition to comprehensive benchmark results.

Low RMRratio as a Surrogate Marker for Energy Deficiency, the Choice of Predictive Equation Vital for Correctly Identifying Male and Female Ballet Dancers at Risk.

PubMed

Staal, Sarah; Sjödin, Anders; Fahrenholtz, Ida; Bonnesen, Karen; Melin, Anna Katarina

2018-06-22

Ballet dancers are reported to have an increased risk for energy deficiency with or without disordered eating behavior. A low ratio between measured ( m ) and predicted ( p ) resting metabolic rate (RMR ratio  < 0.90) is a recognized surrogate marker for energy deficiency. We aimed to evaluate the prevalence of suppressed RMR using different methods to calculate p RMR and to explore associations with additional markers of energy deficiency. Female (n = 20) and male (n = 20) professional ballet dancers, 19-35 years of age, were enrolled. m RMR was assessed by respiratory calorimetry (ventilated open hood). p RMR was determined using the Cunningham and Harris-Benedict equations, and different tissue compartments derived from whole-body dual-energy X-ray absorptiometry assessment. The protocol further included assessment of body composition and bone mineral density, blood pressure, disordered eating (Eating Disorder Inventory-3), and for females, the Low Energy Availability in Females Questionnaire. The prevalence of suppressed RMR was generally high but also clearly dependent on the method used to calculate p RMR, ranging from 25% to 80% in males and 35% to 100% in females. Five percent had low bone mineral density, whereas 10% had disordered eating and 25% had hypotension. Forty percent of females had elevated Low Energy Availability in Females Questionnaire score and 50% were underweight. Suppressed RMR was associated with elevated Low Energy Availability in Females Questionnaire score in females and with higher training volume in males. In conclusion, professional ballet dancers are at risk for energy deficiency. The number of identified dancers at risk varies greatly depending on the method used to predict RMR when using RMR ratio as a marker for energy deficiency.

Synthesis and characterization of RuO(2)/poly(3,4-ethylenedioxythiophene) composite nanotubes for supercapacitors.

PubMed

Liu, Ran; Duay, Jonathon; Lane, Timothy; Bok Lee, Sang

2010-05-07

We report the synthesis of composite RuO(2)/poly(3,4-ethylenedioxythiophene) (PEDOT) nanotubes with high specific capacitance and fast charging/discharging capability as well as their potential application as electrode materials for a high-energy and high-power supercapacitor. RuO(2)/PEDOT nanotubes were synthesized in a porous alumina membrane by a step-wise electrochemical deposition method, and their structures were characterized using electron microscopy. Cyclic voltammetry was used to qualitatively characterize the capacitive properties of the composite RuO(2)/PEDOT nanotubes. Their specific capacitance, energy density and power density were evaluated by galvanostatic charge/discharge cycles at various current densities. The pseudocapacitance behavior of these composite nanotubes originates from ion diffusion during the simultaneous and parallel redox processes of RuO(2) and PEDOT. We show that the energy density (specific capacitance) of PEDOT nanotubes can be remarkably enhanced by electrodepositing RuO(2) into their porous walls and onto their rough internal surfaces. The flexible PEDOT prevents the RuO(2) from breaking and detaching from the current collector while the rigid RuO(2) keeps the PEDOT nanotubes from collapsing and aggregating. The composite RuO(2)/PEDOT nanotube can reach a high power density of 20 kW kg(-1) while maintaining 80% energy density (28 Wh kg(-1)) of its maximum value. This high power capability is attributed to the fast charge/discharge of nanotubular structures: hollow nanotubes allow counter-ions to readily penetrate into the composite material and access their internal surfaces, while a thin wall provides a short diffusion distance to facilitate ion transport. The high energy density originates from the RuO(2), which can store high electrical/electrochemical energy intrinsically. The high specific capacitance (1217 F g(-1)) which is contributed by the RuO(2) in the composite RuO(2)/PEDOT nanotube is realized because of the high specific surface area of the nanotubular structures. Such PEDOT/RuO(2) composite nanotube materials are an ideal candidate for the development of high-energy and high-power supercapacitors.

SU-F-J-213: Feasibility Study of Using a Dual-Energy Cone Beam CT (DECBCT) in Proton Therapy Treatment Planning

DOE Office of Scientific and Technical Information (OSTI.GOV)

Peng, H; Xing, L; Kanehira, T

2016-06-15

Purpose: The aim of this study is to evaluate the feasibility of using a dual-energy CBCT (DECBCT) in proton therapy treatment planning to allow for accurate electron density estimation. Methods: For direct comparison, two scenarios were selected: a dual-energy fan-beam CT (high: 140 kVp, low: 80 kVp) and a DECBCT (high: 125 kVp, low: 80 kVp). A Gammex 467 tissue characterization phantom was used, including the rods of air, water, bone (B2–30% mineral), cortical bone (SB3), lung (LN-300), brain, liver and adipose. For the CBCT, Hounsfield Unit (HU) numbers were first obtained from the reconstructed images after a calibration wasmore » made based on water (=0) and air materials (=−1000). For each tissue surrogate, region-of-interest (ROI) analyses were made to derive high-energy and low-energy HU values (HUhigh and HUlow), which were subsequently used to estimate electron density based on the algorithm as previously described by Hunemohr N., et al. Parameters k1 and k2 are energy dependent and can be derived from calibration materials. Results: While for the dual-energy FBCT, the electron density is found be within +/−3% error relative to the values provided by the phantom vendor: −1.8% (water), 0.03% (lung), 1.1% (brain), −2.82% (adipose), −0.49% (liver) and −1.89% (cortical bones). While for the DECBCT, the estimation of electron density exhibits a relatively larger variation: −1.76% (water), −36.7% (lung), −1.92% (brain), −3.43% (adipose), 8.1% (liver) and 9.5% (cortical bones). Conclusion: For DECBCT, the accuracy of electron density estimation is inferior to that of a FBCT, especially for materials of either low-density (lung) or high density (cortical bone) compared to water. Such limitation arises from inaccurate HU number derivation in a CBCT. Advanced scatter-correction and HU calibration routines, as well as the deployment of photon counting CT detectors need be investigated to minimize the difference between FBCT and CBCT.« less

Microstress, strain, band gap tuning and photocatalytic properties of thermally annealed and Cu-doped ZnO nanoparticles

NASA Astrophysics Data System (ADS)

Prasad, Neena; V. M. M, Saipavitra; Swaminathan, Hariharan; Thangaraj, Pandiyarajan; Ramalinga Viswanathan, Mangalaraja; Balasubramanian, Karthikeyan

2016-06-01

ZnO nanoparticles and Cu-doped ZnO nanoparticles were prepared by co-precipitation method. Also, a part of the pure ZnO nanoparticles were annealed at 750 °C for 3, 6, and 9 h. X-ray diffraction studies were carried out and the lattice parameters, unit cell volume, interplanar spacing, and Young's modulus were calculated for all the samples, and also the crystallite size was found using the Scherrer method. X-ray peak broadening analysis was used to estimate the crystallite sizes and the strain using the Williamson-Hall (W-H) method and the size-strain plot (SSP) method. Stress and the energy density were calculated using the W-H method assuming different models such as uniform deformation model, uniform strain deformation model, uniform deformation energy density model, and the SSP method. Optical absorption properties of the samples were understood from their UV-visible spectra. Photocatalytic activities of ZnO and 5 % Cu-doped ZnO were observed by the degradation of methylene blue dye in aqueous medium under the irradiation of 20-W compact fluorescent lamp for an hour.

Are energy-dense foods really cheaper? Reexamining the relation between food price and energy density.

PubMed

Lipsky, Leah M

2009-11-01

The inverse relation between energy density (kcal/g) and energy cost (price/kcal) has been interpreted to suggest that produce (fruit, vegetables) is more expensive than snacks (cookies, chips). The objective of this study was to show the methodologic weakness of comparing energy density with energy cost. The relation between energy density and energy cost was replicated in a random-number data set. Additionally, observational data were collected for produce and snacks from an online supermarket. Variables included total energy (kcal), total weight (g), total number of servings, serving size (g/serving), and energy density (kcal/g). Price measures included energy cost ($/kcal), total price ($), unit price ($/g), and serving price ($/serving). Two-tailed t tests were used to compare price measures by food category. Relations between energy density and price measures within food categories were examined with the use of Spearman rank correlation analysis. The relation between energy density and energy cost was shown to be driven by the algebraic properties of these variables. Food category was strongly correlated with both energy density and food price measures. Energy cost was higher for produce than for snacks. However, total price and unit price were lower for produce. Serving price and serving size were greater for produce than for snacks. Within food categories, energy density was uncorrelated with most measures of food price, except for a weak positive correlation with serving price within the produce category. The findings suggest the relation between energy density and food price is confounded by food category and depends on which measure of price is used.

A quantitative relationship for the shock sensitivities of energetic compounds based on X-NO(2) (X=C, N, O) bond dissociation energy.

PubMed

Li, Jinshan

2010-08-15

The ZPE-corrected X-NO(2) (X=C, N, O) bond dissociation energies (BDEs(ZPE)) of 11 energetic nitrocompounds of different types have been calculated employing density functional theory methods. Computed results show that using the 6-31G** basis set the UB3LYP calculated BDE(ZPE) is less than the UB3P86. For these typical energetic nitrocompounds the shock-initiated pressure (P(98)) is strongly related to the BDE(ZPE) indeed, and a polynomial correlation of ln(P(98)) with the BDE(ZPE) has been established successfully at different density functional theory levels, which provides a method to address the shock sensitivity problem. Copyright 2010 Elsevier B.V. All rights reserved.

Microhartree precision in density functional theory calculations

NASA Astrophysics Data System (ADS)

Gulans, Andris; Kozhevnikov, Anton; Draxl, Claudia

2018-04-01

To address ultimate precision in density functional theory calculations we employ the full-potential linearized augmented plane-wave + local-orbital (LAPW + lo) method and justify its usage as a benchmark method. LAPW + lo and two completely unrelated numerical approaches, the multiresolution analysis (MRA) and the linear combination of atomic orbitals, yield total energies of atoms with mean deviations of 0.9 and 0.2 μ Ha , respectively. Spectacular agreement with the MRA is reached also for total and atomization energies of the G2-1 set consisting of 55 molecules. With the example of α iron we demonstrate the capability of LAPW + lo to reach μ Ha /atom precision also for periodic systems, which allows also for the distinction between the numerical precision and the accuracy of a given functional.

DOE Office of Scientific and Technical Information (OSTI.GOV)

Wojciech, Blachucki

This work treats of the high energy resolution off-resonant X-ray spectroscopy (HEROS) method of determining the density of unoccupied electronic states in the vicinity of the absorption edge. HEROS is an alternative to the existing X-ray absorption spectroscopy (XAS) methods and opens the way for new studies not achievable before.

Estimation of lattice strain in nanocrystalline RuO2 by Williamson-Hall and size-strain plot methods

NASA Astrophysics Data System (ADS)

Sivakami, R.; Dhanuskodi, S.; Karvembu, R.

2016-01-01

RuO2 nanoparticles (RuO2 NPs) have been successfully synthesized by the hydrothermal method. Structure and the particle size have been determined by X-ray diffraction (XRD), scanning electron microscopy (SEM), atomic force microscopy (AFM) and transmission electron microscopy (TEM). UV-Vis spectra reveal that the optical band gap of RuO2 nanoparticles is red shifted from 3.95 to 3.55 eV. BET measurements show a high specific surface area (SSA) of 118-133 m2/g and pore diameter (10-25 nm) has been estimated by Barret-Joyner-Halenda (BJH) method. The crystallite size and lattice strain in the samples have been investigated by Williamson-Hall (W-H) analysis assuming uniform deformation, deformation stress and deformation energy density, and the size-strain plot method. All other relevant physical parameters including stress, strain and energy density have been calculated. The average crystallite size and the lattice strain evaluated from XRD measurements are in good agreement with the results of TEM.

The vibrational spectroscopic studies and molecular property analysis of L-Phenylalanine using quantum chemical method

NASA Astrophysics Data System (ADS)

Borah, Mukunda Madhab; Devi, Th. Gomti

2017-05-01

In the present work, L-phenylalanine is studied using the experimental and theoretical methods. The spectral characterization of the molecule has been done using Raman, FTIR, Hartee-Fock(HF), density functional theory (DFT) and vibrational energy distribution analysis (VEDA) calculation. The optimization of the molecule has been studied using basis set HF/6-31G(d,p) and B3LYP/6-31G(d,p) for Hartree Fock and density functional theory calculation. The complete vibrational assignment of the molecule in monomer and dimer states have been attempted. The potential energy distribution and normal mode analysis are also carried out to determine the contributions of bond oscillators in each normal mode. The molecular geometry, HOMO-LUMO energy gap, molecular hardness (η), ionization energy (IE), electron affinity (EA), total energy and dipole moment were determined from the calculated data. The observed experimental and the scaled theoretical results are compared and found to be in good agreement. The vibrational assignment of molecule in different dimer states has also been done using SERS data and better correlated Raman peaks are observed as compare to normal Raman technique.

Systematic implementation of spectral CT with a photon counting detector for liquid security inspection

NASA Astrophysics Data System (ADS)

Xu, Xiaofei; Xing, Yuxiang; Wang, Sen; Zhang, Li

2018-06-01

X-ray liquid security inspection system plays an important role in homeland security, while the conventional dual-energy CT (DECT) system may have a big deviation in extracting the atomic number and the electron density of materials in various conditions. Photon counting detectors (PCDs) have the capability of discriminating the incident photons of different energy. The technique becomes more and more mature in nowadays. In this work, we explore the performance of a multi-energy CT imaging system with a PCD for liquid security inspection in material discrimination. We used a maximum-likelihood (ML) decomposition method with scatter correction based on a cross-energy response model (CERM) for PCDs so that to improve the accuracy of atomic number and electronic density imaging. Experimental study was carried to examine the effectiveness and robustness of the proposed system. Our results show that the concentration of different solutions in physical phantoms can be reconstructed accurately, which could improve the material identification compared to current available dual-energy liquid security inspection systems. The CERM-base decomposition and reconstruction method can be easily used to different applications such as medical diagnosis.

Simple vertex correction improves G W band energies of bulk and two-dimensional crystals

NASA Astrophysics Data System (ADS)

Schmidt, Per S.; Patrick, Christopher E.; Thygesen, Kristian S.

2017-11-01

The G W self-energy method has long been recognized as the gold standard for quasiparticle (QP) calculations of solids in spite of the fact that the neglect of vertex corrections and the use of a density-functional theory starting point lack rigorous justification. In this work we remedy this situation by including a simple vertex correction that is consistent with a local-density approximation starting point. We analyze the effect of the self-energy by splitting it into short-range and long-range terms which are shown to govern, respectively, the center and size of the band gap. The vertex mainly improves the short-range correlations and therefore has a small effect on the band gap, while it shifts the band gap center up in energy by around 0.5 eV, in good agreement with experiments. Our analysis also explains how the relative importance of short- and long-range interactions in structures of different dimensionality is reflected in their QP energies. Inclusion of the vertex comes at practically no extra computational cost and even improves the basis set convergence compared to G W . Taken together, the method provides an efficient and rigorous improvement over the G W approximation.

High density harp or wire scanner for particle beam diagnostics

DOEpatents

Fritsche, C.T.; Krogh, M.L.

1996-05-21

Disclosed is a diagnostic detector head harp used to detect and characterize high energy particle beams using an array of closely spaced detector wires, typically carbon wires, spaced less than 0.1 cm (0.040 inch) connected to a hybrid microcircuit formed on a ceramic substrate. A method to fabricate harps to obtain carbon wire spacing and density not previously available utilizing hybrid microcircuit technology. The hybrid microcircuit disposed on the ceramic substrate connects electrically between the detector wires and diagnostic equipment which analyzes pulses generated in the detector wires by the high energy particle beams. 6 figs.

Molecular structure, vibrational spectra, NBO analysis, first hyperpolarizability, and HOMO-LUMO studies of 2-amino-4-hydroxypyrimidine by density functional method

NASA Astrophysics Data System (ADS)

Jeyavijayan, S.

2015-04-01

This study is a comparative analysis of FTIR and FT-Raman spectra of 2-amino-4-hydroxypyrimidine. The total energies of different conformations have been obtained from DFT (B3LYP) method with 6-31+G(d,p) and 6-311++G(d,p) basis sets. The barrier of planarity between the most stable and planar form is also predicted. The molecular structure, vibrational wavenumbers, infrared intensities, Raman scattering activities were calculated for the molecule using the B3LYP density functional theory (DFT) method. The computed values of frequencies are scaled using multiple scaling factors to yield good coherence with the observed values. Reliable vibrational assignments were made on the basis of total energy distribution (TED) along with scaled quantum mechanical (SQM) method. The stability of the molecule arising from hyperconjugative interactions, charge delocalization has been analyzed using natural bond orbital (NBO) analysis. Non-linear properties such as electric dipole moment (μ), polarizability (α), and hyperpolarizability (β) values of the investigated molecule have been computed using B3LYP quantum chemical calculation. The calculated HOMO and LUMO energies show that charge transfer occurs within the molecule. Besides, molecular electrostatic potential (MEP), Mulliken's charges analysis, and several thermodynamic properties were performed by the DFT method.

Radiation source

DOEpatents

Thode, Lester E.

1981-01-01

A device and method for relativistic electron beam heating of a high-density plasma in a small localized region. A relativistic electron beam generator or accelerator produces a high-voltage electron beam which propagates along a vacuum drift tube and is modulated to initiate electron bunching within the beam. The beam is then directed through a low-density gas chamber which provides isolation between the vacuum modulator and the relativistic electron beam target. The relativistic beam is then applied to a high-density target plasma which typically comprises DT, DD, or similar thermonuclear gas at a density of 10.sup.17 to 10.sup.20 electrons per cubic centimeter. The target gas is ionized prior to application of the relativistic electron beam by means of a laser or other preionization source to form a plasma. Utilizing a relativistic electron beam with an individual particle energy exceeding 3 MeV, classical scattering by relativistic electrons passing through isolation foils is negligible. As a result, relativistic streaming instabilities are initiated within the high-density target plasma causing the relativistic electron beam to efficiently deposit its energy into a small localized region of the high-density plasma target.

Orbital-free bond breaking via machine learning

NASA Astrophysics Data System (ADS)

Snyder, John C.; Rupp, Matthias; Hansen, Katja; Blooston, Leo; Müller, Klaus-Robert; Burke, Kieron

2013-12-01

Using a one-dimensional model, we explore the ability of machine learning to approximate the non-interacting kinetic energy density functional of diatomics. This nonlinear interpolation between Kohn-Sham reference calculations can (i) accurately dissociate a diatomic, (ii) be systematically improved with increased reference data and (iii) generate accurate self-consistent densities via a projection method that avoids directions with no data. With relatively few densities, the error due to the interpolation is smaller than typical errors in standard exchange-correlation functionals.

Density functional study of double ionization energies

NASA Astrophysics Data System (ADS)

Chong, D. P.

2008-02-01

In this paper, double ionization energies (DIEs) of gas-phase atoms and molecules are calculated by energy difference method with density functional theory. To determine the best functional for double ionization energies, we first study 24 main group atoms in the second, third, and fourth periods. An approximation is used in which the electron density is first obtained from a density functional computation with the exchange-correlation potential Vxc known as statistical average of orbital potentials, after which the energy is computed from that density with 59 different exchange-correlation energy functionals Exc. For the 24 atoms, the two best Exc functional providing DIEs with average absolute deviation (AAD) of only 0.25eV are the Perdew-Burke-Ernzerhof functional modified by Hammer et al. [Phys. Rev. B 59, 6413 (1999)] and one known as the Krieger-Chen-Iafrate-Savin functional modified by Krieger et al. (unpublished). Surprisingly, none of the 20 available hybrid functionals is among the top 15 functionals for the DIEs of the 24 atoms. A similar procedure is then applied to molecules, with opposite results: Only hybrid functionals are among the top 15 functionals for a selection of 29molecules. The best Exc functional for the 29molecules is found to be the Becke 1997 functional modified by Wilson et al. [J. Chem. Phys. 115, 9233 (2001)]. With that functional, the AAD from experiment for DIEs of 29molecules is just under 0.5eV. If the two suspected values for C2H2 and Fe(CO)5 are excluded, the AAD improves to 0.32eV. Many other hybrid functionals perform almost as well.

Bio-inspired spider-web-like membranes with a hierarchical structure for high performance lithium/sodium ion battery electrodes: the case of 3D freestanding and binder-free bismuth/CNF anodes.

PubMed

Jin, Yuqiang; Yuan, Haocheng; Lan, Jin-Le; Yu, Yunhua; Lin, Yuan-Hua; Yang, Xiaoping

2017-09-14

High gravimetric energy density and volumetric energy density energy storage devices are highly desirable due to the rapid development of electric vehicles, and portable and wearable electronic equipment. Electrospinning is a promising technology for preparing freestanding electrodes with high gravimetric and volumetric energy density. However, the energy density of the traditional electrospun electrodes is restricted by the low mass loading of active materials (e.g. 20%-30 wt%). Herein, a biomimetic strategy inspired by the phenomenon of the sticky spider web is demonstrated as a high performance anode, which simultaneously improves the gravimetric and volumetric energy density. Freestanding carbon nanofiber (CNF) membranes containing over 50 wt% of bismuth were prepared by electrospinning and subsequent thermal treatment. Membranes consisting of CNF network structures bonded tightly with active Bi cluster materials, resulting in excellent mechanical protection and a fast charge transport path, which are difficult to achieve simultaneously. The composite membrane delivers high reversible capacity (483 mA h g -1 at 100 mA g -1 after 200 cycles) and high rate performance (242 mA h g -1 at 1 A g -1 ) as a lithium-ion battery anode. For use as a sodium ion battery, the composite membrane also shows a high reversible specific capacity of 346 mA h g -1 and outstanding cycling performance (186 mA h g -1 at 50 mA g -1 after 100 cycles). This work offers a simple, low cost and eco-friendly method for fabricating free-standing and binder-free composite electrodes with high loading used in LIBs and SIBs.

Short-term overeating results in incomplete energy intake compensation regardless of energy density or macronutrient composition

PubMed Central

Apolzan, John W.; Bray, George A.; Hamilton, Marc T.; Zderic, Theodore W.; Han, Hongmei; Champagne, Catherine M.; Shepard, Desti; Martin, Corby K.

2013-01-01

Objective To evaluate the effects of overeating (140% of energy requirements) a high-fat low-energy density diet (HF/LED, 1.05kcal/g), high-fat high-energy density diet (HF/HED, 1.60kcal/g), and high-carbohydrate (HC) LED (1.05kcal/g) for 2-days on subsequent 4-day energy intake (EI), activity levels, appetite, and mood. Design and Methods Using a randomized cross-over design, energy expenditure and EI were standardized during overeating. Results In 20 adults with a mean±SD BMI of 30.7±4.6kg/m2, EI was not suppressed until the second day after overeating and accounted for ~30% of the excess EI. Reductions in EI did not differ among the 3 diets or across days. Overeating had no effect on subsequent energy expenditure but steps/day decreased after the HC/LED and HF/HED. Sleep time was increased after the HF/HED compared to both LEDs. After overeating a HF/HED vs. HF/LED, carbohydrate cravings, hunger, prospective food consumption, and sadness increased and satisfaction, relaxation, and tranquility decreased. Conclusions Diet type, time, or their interaction had no impact on compensation over 4 days. No adaptive thermogenesis was observed. The HF/HED vs. HF/LED had detrimental effects on food cravings, appetite, and mood. These results suggest short-term overeating is associated with incomplete compensation. PMID:23913807

Explicit polarization (X-Pol) potential using ab initio molecular orbital theory and density functional theory.

PubMed

Song, Lingchun; Han, Jaebeom; Lin, Yen-lin; Xie, Wangshen; Gao, Jiali

2009-10-29

The explicit polarization (X-Pol) method has been examined using ab initio molecular orbital theory and density functional theory. The X-Pol potential was designed to provide a novel theoretical framework for developing next-generation force fields for biomolecular simulations. Importantly, the X-Pol potential is a general method, which can be employed with any level of electronic structure theory. The present study illustrates the implementation of the X-Pol method using ab initio Hartree-Fock theory and hybrid density functional theory. The computational results are illustrated by considering a set of bimolecular complexes of small organic molecules and ions with water. The computed interaction energies and hydrogen bond geometries are in good accord with CCSD(T) calculations and B3LYP/aug-cc-pVDZ optimizations.

Kinetic energy partition method applied to ground state helium-like atoms.

PubMed

Chen, Yu-Hsin; Chao, Sheng D

2017-03-28

We have used the recently developed kinetic energy partition (KEP) method to solve the quantum eigenvalue problems for helium-like atoms and obtain precise ground state energies and wave-functions. The key to treating properly the electron-electron (repulsive) Coulomb potential energies for the KEP method to be applied is to introduce a "negative mass" term into the partitioned kinetic energy. A Hartree-like product wave-function from the subsystem wave-functions is used to form the initial trial function, and the variational search for the optimized adiabatic parameters leads to a precise ground state energy. This new approach sheds new light on the all-important problem of solving many-electron Schrödinger equations and hopefully opens a new way to predictive quantum chemistry. The results presented here give very promising evidence that an effective one-electron model can be used to represent a many-electron system, in the spirit of density functional theory.

Molecular dynamics calculation on structures, stabilities, mechanical properties, and energy density of CL-20/FOX-7 cocrystal explosives.

PubMed

Hang, Gui-Yun; Yu, Wen-Li; Wang, Tao; Wang, Jin-Tao; Li, Zhen

2017-11-30

In this article, different CL-20/FOX-7 cocrystal models were established by the substitution method based on the molar ratios of CL-20:FOX-7. The structures and comprehensive properties, including mechanical properties, stabilities, and energy density, of different cocrystal models were obtained and compared with each other. The main aim was to estimate the influence of molar ratios on properties of cocrystal explosives. The molecular dynamics (MD) simulation results show that the cocrystal model with molar ratio 1:1 has the best mechanical properties and highest binding energy, so the CL-20/FOX-7 cocrystal model is more likely to form in 1:1 M ratio. The detonation parameters show that the cocrystal explosive exhibited preferable energy density and excellent detonation performance. In a word, the 1:1 cocrystal model has the best comprehensive properties, is very promising, and worth more theoretical investigations and experimental tests. This paper gives some original theories to better understand the cocrystal mechanism and provides some helpful guidance and useful instructions to help design CL-20 cocrystal explosives.

The Mechanical Properties of Energetically Deposited Non-Crystalline Carbon Thin Films

DOE PAGES

Kracica, M.; Kocer, C.; Lau, D.; ...

2015-11-05

The mechanical behaviour of carbon films prepared with a variety of densities and microstructures was investigated using nanoindentation. Deposition energies between 25 and 600 eV and temperatures in the range 25-600 °C were used. Films prepared at low temperatures and moderate energy were amorphous with a high density. Finite element methods were used to model the stress fields, reproduce the indentation behaviour and evaluate elastic properties. Young s moduli up to 670 GPa and a low Poisson s ratio of ~ 0.17 were found, comparable to polycrystalline cubic boron nitride, one of the hardest materials known. Films with the samemore » density did not always show the same behaviour, emphasising the role of microstructure in determining mechanical response. Extended graphite- like regions within the films grown at high energy and high temperature observed in transmission electron microscopy caused plastic deformation and failure to recover after a complete indentation cycle. At low deposition energies, the graphite-like regions were smaller in size causing plastic deformation but with complete recovery after indentation.« less

Reducing the energy density of an entrée decreases children's energy intake at lunch.

PubMed

Leahy, Kathleen E; Birch, Leann L; Rolls, Barbara J

2008-01-01

Strategies need to be developed to reduce preschool children's energy intake. To test the effect of reducing the energy density of an entrée on children's ad libitum energy intake. Subjects were 2- to 5-year-old children (37 boys and 40 girls) in a university day-care facility. In this within-subjects crossover study, children were served a test lunch once per week for 6 weeks. Two versions of a macaroni and cheese entrée were formulated to differ in energy density while maintaining similar palatability. Each version was served to children three times. The higher-energy-density entrée had 2.0 kcal/g and the other entrée was 30% lower in energy density. Lunch, consumed ad libitum, also included broccoli, applesauce, and milk. Food intake and energy intake were measured. A mixed linear model tested effect of energy density of the entrée on food intake and energy intake. Results are reported as mean+/-standard error. Decreasing the energy density of the entrée by 30% significantly (P<0.0001) reduced children's energy intake from the entrée by 25% (72.3+/-8.3 kcal) and total lunch energy intake by 18% (71.8+/-7.9 kcal). Children consumed significantly more of the lower-energy-density entrée (10.1+/-4.2 g; P<0.05). Children's sex-specific body mass index-for-age percentiles did not affect the relationship between energy density of the entrée and children's intakes. Decreasing the energy density of a lunch entrée resulted in a reduction in children's energy intake from the entrée and from the total meal. Reducing the energy density of foods may be an effective strategy to moderate children's energy intake.

2.097μ Cth:YAG flashlamp pumped high energy high efficiency laser operation (patent pending)

NASA Astrophysics Data System (ADS)

Bar-Joseph, Dan

2018-02-01

Flashlamp pumped Cth:YAG lasers are mainly used in medical applications (urology). The main laser transition is at 2.13μ and is called a quasi-three level having an emission cross-section of 7x10-21 cm2 and a ground state absorption of approximately 5%/cm. Because of the relatively low absorption, combined with a modest emission cross-section, the laser requires high reflectivity output coupling, and therefore high intra-cavity energy density which limits the output to approximately 4J/pulse for reliable operation. This paper will describe a method of efficiently generating high output energy at low intra-cavity energy density by using an alternative 2.097μ transition having an emission cross-section of 5x10-21 cm2 and a ground level absorption of approximately 14%/cm.

Ground state energy of electrons in a static point-ion lattice

NASA Technical Reports Server (NTRS)

Styer, D. F.; Ashcroft, N. W.

1983-01-01

The ground state energy of a neutral collection of protons and electrons was investigated under the assumption that in the ground state configuration, static protons occupy the sites of a rigid Bravais lattice. The Wigner-Seitz method was used in conjunction with three postulated potentials: bare Coulomb, Thomas-Fermi screening, and screening by a uniform bare background charge. Within these approximations, the exact band-minimum energy and wave functions are derived. For each of the three potentials, the approximate minimum ground state energy per proton (relative to isolated electrons and protons) is, respectively, -1.078 Ry, -1.038 Ry, and -1.052 Ry. These three minima all fall at a density of about 0.60 gm/cu cm, which is thus an approximate lower bound on the density of metallic hydrogen at its transition pressure.

Entropy and density of states from isoenergetic nonequilibrium processes

NASA Astrophysics Data System (ADS)

Adib, Artur B.

2005-05-01

Two identities in statistical mechanics involving entropy differences (or ratios of densities of states) at constant energy are derived. The first provides a nontrivial extension of the Jarzynski equality to the microcanonical ensemble [C. Jarzynski, Phys. Rev. Lett. 78, 2690 (1997)], which can be seen as a “fast-switching” version of the adiabatic switching method for computing entropies [M. Watanabe and W. P. Reinhardt, Phys. Rev. Lett. 65, 3301 (1990)]. The second is a thermodynamic integration formula analogous to a well-known expression for free energies, and follows after taking the quasistatic limit of the first. Both identities can be conveniently used in conjunction with a scaling relation (herein derived) that allows one to extrapolate measurements taken at a single energy to a wide range of energy values. Practical aspects of these identities in the context of numerical simulations are discussed.

Theoretical insights into effects of molar ratios on stabilities, mechanical properties and detonation performance of CL-20/RDX cocrystal explosives by molecular dynamics simulation

NASA Astrophysics Data System (ADS)

Hang, Gui-yun; Yu, Wen-li; Wang, Tao; Wang, Jin-tao; Li, Zhen

2017-08-01

The CL-20/RDX cocrystal models with different molar ratios were established by substitution method and molecular dynamics (MD) simulation method was applied to investigate the influences of molar ratios on mechanical properties, stabilities and detonation performance of cocrystal explosives. The crystal parameters, structures, binding energies, mechanical properties and some detonation parameters of different cocrystal explosives were got and compared. The results illustrate that the molar ratio has a direct influence on properties of cocrystal explosive and each of the cocrystal model holds different mechanical properties, binding energies and detonation parameters. The mechanical properties of CL-20/RDX cocrystal explosive can be effectively improved and the cocrystal model with molar ratio in 1:1 has the best mechanical properties. Besides, it has the highest binding energy, so the stability and compatibility is the best. The detonation parameters show that the cocrystal explosive has better detonation performance than RDX. In a word, the cocrystal explosive with molar ratio in 1:1 has the best mechanical properties, highest binding energy and excellent energy density and detonation performance, it is quite promising and can satisfy the requirements of high energy density compounds (HEDC). This paper could offer some theoretical instructions and novel insights for the CL-20 cocrystal explosive designing.

Transition metal sulfides grown on graphene fibers for wearable asymmetric supercapacitors with high volumetric capacitance and high energy density

NASA Astrophysics Data System (ADS)

Cai, Weihua; Lai, Ting; Lai, Jianwei; Xie, Haoting; Ouyang, Liuzhang; Ye, Jianshan; Yu, Chengzhong

2016-06-01

Fiber shaped supercapacitors are promising candidates for wearable electronics because they are flexible and light-weight. However, a critical challenge of the widespread application of these energy storage devices is their low cell voltages and low energy densities, resulting in limited run-time of the electronics. Here, we demonstrate a 1.5 V high cell voltage and high volumetric energy density asymmetric fiber supercapacitor in aqueous electrolyte. The lightweight (0.24 g cm-3), highly conductive (39 S cm-1), and mechanically robust (221 MPa) graphene fibers were firstly fabricated and then coated by NiCo2S4 nanoparticles (GF/NiCo2S4) via the solvothermal deposition method. The GF/NiCo2S4 display high volumetric capacitance up to 388 F cm-3 at 2 mV s-1 in a three-electrode cell and 300 F cm-3 at 175.7 mA cm-3 (568 mF cm-2 at 0.5 mA cm-2) in a two-electrode cell. The electrochemical characterizations show 1000% higher capacitance of the GF/NiCo2S4 as compared to that of neat graphene fibers. The fabricated device achieves high energy density up to 12.3 mWh cm-3 with a maximum power density of 1600 mW cm-3, outperforming the thin-film lithium battery. Therefore, these supercapacitors are promising for the next generation flexible and wearable electronic devices.

Transition metal sulfides grown on graphene fibers for wearable asymmetric supercapacitors with high volumetric capacitance and high energy density

PubMed Central

Cai, Weihua; Lai, Ting; Lai, Jianwei; Xie, Haoting; Ouyang, Liuzhang; Ye, Jianshan; Yu, Chengzhong

2016-01-01

Fiber shaped supercapacitors are promising candidates for wearable electronics because they are flexible and light-weight. However, a critical challenge of the widespread application of these energy storage devices is their low cell voltages and low energy densities, resulting in limited run-time of the electronics. Here, we demonstrate a 1.5 V high cell voltage and high volumetric energy density asymmetric fiber supercapacitor in aqueous electrolyte. The lightweight (0.24 g cm−3), highly conductive (39 S cm−1), and mechanically robust (221 MPa) graphene fibers were firstly fabricated and then coated by NiCo2S4 nanoparticles (GF/NiCo2S4) via the solvothermal deposition method. The GF/NiCo2S4 display high volumetric capacitance up to 388 F cm−3 at 2 mV s−1 in a three-electrode cell and 300 F cm−3 at 175.7 mA cm−3 (568 mF cm−2 at 0.5 mA cm−2) in a two-electrode cell. The electrochemical characterizations show 1000% higher capacitance of the GF/NiCo2S4 as compared to that of neat graphene fibers. The fabricated device achieves high energy density up to 12.3 mWh cm−3 with a maximum power density of 1600 mW cm−3, outperforming the thin-film lithium battery. Therefore, these supercapacitors are promising for the next generation flexible and wearable electronic devices. PMID:27248510

Ab-initio Computation of the Electronic, transport, and Bulk Properties of Calcium Oxide.

NASA Astrophysics Data System (ADS)

Mbolle, Augustine; Banjara, Dipendra; Malozovsky, Yuriy; Franklin, Lashounda; Bagayoko, Diola

We report results from ab-initio, self-consistent, local Density approximation (LDA) calculations of electronic and related properties of calcium oxide (CaO) in the rock salt structure. We employed the Ceperley and Alder LDA potential and the linear combination of atomic orbitals (LCAO) formalism. Our calculations are non-relativistic. We implemented the LCAO formalism following the Bagayoko, Zhao, and Williams (BZW) method, as enhanced by Ekuma and Franklin (BZW-EF). The BZW-EF method involves a methodical search for the optimal basis set that yields the absolute minima of the occupied energies, as required by density functional theory (DFT). Our calculated, indirect band gap of 6.91eV, from towards the L point, is in excellent agreement with experimental value of 6.93-7.7eV, at room temperature (RT). We have also calculated the total (DOS) and partial (pDOS) densities of states as well as the bulk modulus. Our calculated bulk modulus is in excellent agreement with experiment. Work funded in part by the US Department of Energy (DOE), National Nuclear Security Administration (NNSA) (Award No.DE-NA0002630), the National Science Foundation (NSF) (Award No, 1503226), LaSPACE, and LONI-SUBR.

Solid H2 in the interstellar medium

NASA Astrophysics Data System (ADS)

Füglistaler, A.; Pfenniger, D.

2018-06-01

Context. Condensation of H2 in the interstellar medium (ISM) has long been seen as a possibility, either by deposition on dust grains or thanks to a phase transition combined with self-gravity. H2 condensation might explain the observed low efficiency of star formation and might help to hide baryons in spiral galaxies. Aims: Our aim is to quantify the solid fraction of H2 in the ISM due to a phase transition including self-gravity for different densities and temperatures in order to use the results in more complex simulations of the ISM as subgrid physics. Methods: We used molecular dynamics simulations of fluids at different temperatures and densities to study the formation of solids. Once the simulations reached a steady state, we calculated the solid mass fraction, energy increase, and timescales. By determining the power laws measured over several orders of magnitude, we extrapolated to lower densities the higher density fluids that can be simulated with current computers. Results: The solid fraction and energy increase of fluids in a phase transition are above 0.1 and do not follow a power law. Fluids out of a phase transition are still forming a small amount of solids due to chance encounters of molecules. The solid mass fraction and energy increase of these fluids are linearly dependent on density and can easily be extrapolated. The timescale is below one second, the condensation can be considered instantaneous. Conclusions: The presence of solid H2 grains has important dynamic implications on the ISM as they may be the building blocks for larger solid bodies when gravity is included. We provide the solid mass fraction, energy increase, and timescales for high density fluids and extrapolation laws for lower densities.

Darkness without dark matter and energy - generalized unimodular gravity

NASA Astrophysics Data System (ADS)

Barvinsky, A. O.; Kamenshchik, A. Yu.

2017-11-01

We suggest a Lorentz non-invariant generalization of the unimodular gravity theory, which is classically equivalent to general relativity with a locally inert (devoid of local degrees of freedom) perfect fluid having an equation of state with a constant parameter w. For the range of w near -1 this dark fluid can play the role of dark energy, while for w = 0 this dark dust admits spatial inhomogeneities and can be interpreted as dark matter. We discuss possible implications of this model in the cosmological initial conditions problem. In particular, this is the extension of known microcanonical density matrix predictions for the initial quantum state of the closed cosmology to the case of spatially open Universe, based on the imitation of the spatial curvature by the dark fluid density. We also briefly discuss quantization of this model necessarily involving the method of gauge systems with reducible constraints and the effect of this method on the treatment of recently! suggested mechanism of vacuum energy sequestering.

Efficient Determination of Free Energy Landscapes in Multiple Dimensions from Biased Umbrella Sampling Simulations Using Linear Regression.

PubMed

Meng, Yilin; Roux, Benoît

2015-08-11

The weighted histogram analysis method (WHAM) is a standard protocol for postprocessing the information from biased umbrella sampling simulations to construct the potential of mean force with respect to a set of order parameters. By virtue of the WHAM equations, the unbiased density of state is determined by satisfying a self-consistent condition through an iterative procedure. While the method works very effectively when the number of order parameters is small, its computational cost grows rapidly in higher dimension. Here, we present a simple and efficient alternative strategy, which avoids solving the self-consistent WHAM equations iteratively. An efficient multivariate linear regression framework is utilized to link the biased probability densities of individual umbrella windows and yield an unbiased global free energy landscape in the space of order parameters. It is demonstrated with practical examples that free energy landscapes that are comparable in accuracy to WHAM can be generated at a small fraction of the cost.

Formation of Triboelectric Series via Atomic-Level Surface Functionalization for Triboelectric Energy Harvesting.

PubMed

Shin, Sung-Ho; Bae, Young Eun; Moon, Hyun Kyung; Kim, Jungkil; Choi, Suk-Ho; Kim, Yongho; Yoon, Hyo Jae; Lee, Min Hyung; Nah, Junghyo

2017-06-27

Triboelectric charging involves frictional contact of two different materials, and their contact electrification usually relies on polarity difference in the triboelectric series. This limits the choices of materials for triboelectric contact pairs, hindering research and development of energy harvest devices utilizing triboelectric effect. A progressive approach to resolve this issue involves modification of chemical structures of materials for effectively engineering their triboelectric properties. Here, we describe a facile method to change triboelectric property of a polymeric surface via atomic-level chemical functionalizations using a series of halogens and amines, which allows a wide spectrum of triboelectric series over single material. Using this method, tunable triboelectric output power density is demonstrated in triboelectric generators. Furthermore, molecular-scale calculation using density functional theory unveils that electrons transferred through electrification are occupying the PET group rather than the surface functional group. The work introduced here would open the ability to tune triboelectric property of materials by chemical modification of surface and facilitate the development of energy harvesting devices and sensors exploiting triboelectric effect.

Efficient Determination of Free Energy Landscapes in Multiple Dimensions from Biased Umbrella Sampling Simulations Using Linear Regression

PubMed Central

2015-01-01

The weighted histogram analysis method (WHAM) is a standard protocol for postprocessing the information from biased umbrella sampling simulations to construct the potential of mean force with respect to a set of order parameters. By virtue of the WHAM equations, the unbiased density of state is determined by satisfying a self-consistent condition through an iterative procedure. While the method works very effectively when the number of order parameters is small, its computational cost grows rapidly in higher dimension. Here, we present a simple and efficient alternative strategy, which avoids solving the self-consistent WHAM equations iteratively. An efficient multivariate linear regression framework is utilized to link the biased probability densities of individual umbrella windows and yield an unbiased global free energy landscape in the space of order parameters. It is demonstrated with practical examples that free energy landscapes that are comparable in accuracy to WHAM can be generated at a small fraction of the cost. PMID:26574437

Analytical modeling of electron energy loss spectroscopy of graphene: Ab initio study versus extended hydrodynamic model.

PubMed

Djordjević, Tijana; Radović, Ivan; Despoja, Vito; Lyon, Keenan; Borka, Duško; Mišković, Zoran L

2018-01-01

We present an analytical modeling of the electron energy loss (EEL) spectroscopy data for free-standing graphene obtained by scanning transmission electron microscope. The probability density for energy loss of fast electrons traversing graphene under normal incidence is evaluated using an optical approximation based on the conductivity of graphene given in the local, i.e., frequency-dependent form derived by both a two-dimensional, two-fluid extended hydrodynamic (eHD) model and an ab initio method. We compare the results for the real and imaginary parts of the optical conductivity in graphene obtained by these two methods. The calculated probability density is directly compared with the EEL spectra from three independent experiments and we find very good agreement, especially in the case of the eHD model. Furthermore, we point out that the subtraction of the zero-loss peak from the experimental EEL spectra has a strong influence on the analytical model for the EEL spectroscopy data. Copyright © 2017 Elsevier B.V. All rights reserved.

Current density characteristics in the studies of electromagnetically induced transparency in a GaAs/GaAlAs quantum well

NASA Astrophysics Data System (ADS)

Jayarubi, J.; Peter, A. John

2017-05-01

Confinement potential profiles due to conduction and valence bands are obtained in a Ga0.7Al0.3As/ GaAs/ Ga0.7Al0.3As using variation formulism. The free electron distribution is carried out. The confined energy eigenvalue and its corresponding wavefunctions of charge carriers are found using self-consistent method. The confined energies with the geometrical confinement are computed. The potentials due to charges are done by Poisson equation. The effects of dielectric mismatch between the GaAs and GaAlAs semiconductors are introduced in the effective potential expressions. Transfer matrix method is employed to obtain the respective energies. The transmission probability is obtained for a constant well size. The high current density characteristics as a function of applied voltage is investigated. This investigation on the electromagnetically induced transparency in the photonic material will exploit in fabricating novel nonlinear optical devices in future.

QM/QM approach to model energy disorder in amorphous organic semiconductors.

PubMed

Friederich, Pascal; Meded, Velimir; Symalla, Franz; Elstner, Marcus; Wenzel, Wolfgang

2015-02-10

It is an outstanding challenge to model the electronic properties of organic amorphous materials utilized in organic electronics. Computation of the charge carrier mobility is a challenging problem as it requires integration of morphological and electronic degrees of freedom in a coherent methodology and depends strongly on the distribution of polaron energies in the system. Here we represent a QM/QM model to compute the polaron energies combining density functional methods for molecules in the vicinity of the polaron with computationally efficient density functional based tight binding methods in the rest of the environment. For seven widely used amorphous organic semiconductor materials, we show that the calculations are accelerated up to 1 order of magnitude without any loss in accuracy. Considering that the quantum chemical step is the efficiency bottleneck of a workflow to model the carrier mobility, these results are an important step toward accurate and efficient disordered organic semiconductors simulations, a prerequisite for accelerated materials screening and consequent component optimization in the organic electronics industry.

Fission fragment charge and mass distributions in 239Pu(n ,f ) in the adiabatic nuclear energy density functional theory

NASA Astrophysics Data System (ADS)

Regnier, D.; Dubray, N.; Schunck, N.; Verrière, M.

2016-05-01

Background: Accurate knowledge of fission fragment yields is an essential ingredient of numerous applications ranging from the formation of elements in the r process to fuel cycle optimization for nuclear energy. The need for a predictive theory applicable where no data are available, together with the variety of potential applications, is an incentive to develop a fully microscopic approach to fission dynamics. Purpose: In this work, we calculate the pre-neutron emission charge and mass distributions of the fission fragments formed in the neutron-induced fission of 239Pu using a microscopic method based on nuclear density functional theory (DFT). Methods: Our theoretical framework is the nuclear energy density functional (EDF) method, where large-amplitude collective motion is treated adiabatically by using the time-dependent generator coordinate method (TDGCM) under the Gaussian overlap approximation (GOA). In practice, the TDGCM is implemented in two steps. First, a series of constrained EDF calculations map the configuration and potential-energy landscape of the fissioning system for a small set of collective variables (in this work, the axial quadrupole and octupole moments of the nucleus). Then, nuclear dynamics is modeled by propagating a collective wave packet on the potential-energy surface. Fission fragment distributions are extracted from the flux of the collective wave packet through the scission line. Results: We find that the main characteristics of the fission charge and mass distributions can be well reproduced by existing energy functionals even in two-dimensional collective spaces. Theory and experiment agree typically within two mass units for the position of the asymmetric peak. As expected, calculations are sensitive to the structure of the initial state and the prescription for the collective inertia. We emphasize that results are also sensitive to the continuity of the collective landscape near scission. Conclusions: Our analysis confirms that the adiabatic approximation provides an effective scheme to compute fission fragment yields. It also suggests that, at least in the framework of nuclear DFT, three-dimensional collective spaces may be a prerequisite to reach 10% accuracy in predicting pre-neutron emission fission fragment yields.

An energy-stable method for solving the incompressible Navier-Stokes equations with non-slip boundary condition

NASA Astrophysics Data System (ADS)

Lee, Byungjoon; Min, Chohong

2018-05-01

We introduce a stable method for solving the incompressible Navier-Stokes equations with variable density and viscosity. Our method is stable in the sense that it does not increase the total energy of dynamics that is the sum of kinetic energy and potential energy. Instead of velocity, a new state variable is taken so that the kinetic energy is formulated by the L2 norm of the new variable. Navier-Stokes equations are rephrased with respect to the new variable, and a stable time discretization for the rephrased equations is presented. Taking into consideration the incompressibility in the Marker-And-Cell (MAC) grid, we present a modified Lax-Friedrich method that is L2 stable. Utilizing the discrete integration-by-parts in MAC grid and the modified Lax-Friedrich method, the time discretization is fully discretized. An explicit CFL condition for the stability of the full discretization is given and mathematically proved.

Growth Method-Dependent and Defect Density-Oriented Structural, Optical, Conductive, and Physical Properties of Solution-Grown ZnO Nanostructures.

PubMed

Rana, Abu Ul Hassan Sarwar; Lee, Ji Young; Shahid, Areej; Kim, Hyun-Seok

2017-09-10

It is time for industry to pay a serious heed to the application and quality-dependent research on the most important solution growth methods for ZnO, namely, aqueous chemical growth (ACG) and microwave-assisted growth (MAG) methods. This study proffers a critical analysis on how the defect density and formation behavior of ZnO nanostructures (ZNSs) are growth method-dependent. Both antithetical and facile methods are exploited to control the ZnO defect density and the growth mechanism. In this context, the growth of ZnO nanorods (ZNRs), nanoflowers, and nanotubes (ZNTs) are considered. The aforementioned growth methods directly stimulate the nanostructure crystal growth and, depending upon the defect density, ZNSs show different trends in structural, optical, etching, and conductive properties. The defect density of MAG ZNRs is the least because of an ample amount of thermal energy catered by high-power microwaves to the atoms to grow on appropriate crystallographic planes, which is not the case in faulty convective ACG ZNSs. Defect-centric etching of ZNRs into ZNTs is also probed and methodological constraints are proposed. ZNS optical properties are different in the visible region, which are quite peculiar, but outstanding for ZNRs. Hall effect measurements illustrate incongruent conductive trends in both samples.

Accelerating large scale Kohn-Sham density functional theory calculations with semi-local functionals and hybrid functionals

NASA Astrophysics Data System (ADS)

Lin, Lin

The computational cost of standard Kohn-Sham density functional theory (KSDFT) calculations scale cubically with respect to the system size, which limits its use in large scale applications. In recent years, we have developed an alternative procedure called the pole expansion and selected inversion (PEXSI) method. The PEXSI method solves KSDFT without solving any eigenvalue and eigenvector, and directly evaluates physical quantities including electron density, energy, atomic force, density of states, and local density of states. The overall algorithm scales as at most quadratically for all materials including insulators, semiconductors and the difficult metallic systems. The PEXSI method can be efficiently parallelized over 10,000 - 100,000 processors on high performance machines. The PEXSI method has been integrated into a number of community electronic structure software packages such as ATK, BigDFT, CP2K, DGDFT, FHI-aims and SIESTA, and has been used in a number of applications with 2D materials beyond 10,000 atoms. The PEXSI method works for LDA, GGA and meta-GGA functionals. The mathematical structure for hybrid functional KSDFT calculations is significantly different. I will also discuss recent progress on using adaptive compressed exchange method for accelerating hybrid functional calculations. DOE SciDAC Program, DOE CAMERA Program, LBNL LDRD, Sloan Fellowship.

Extracting electron transfer coupling elements from constrained density functional theory

NASA Astrophysics Data System (ADS)

Wu, Qin; Van Voorhis, Troy

2006-10-01

Constrained density functional theory (DFT) is a useful tool for studying electron transfer (ET) reactions. It can straightforwardly construct the charge-localized diabatic states and give a direct measure of the inner-sphere reorganization energy. In this work, a method is presented for calculating the electronic coupling matrix element (Hab) based on constrained DFT. This method completely avoids the use of ground-state DFT energies because they are known to irrationally predict fractional electron transfer in many cases. Instead it makes use of the constrained DFT energies and the Kohn-Sham wave functions for the diabatic states in a careful way. Test calculations on the Zn2+ and the benzene-Cl atom systems show that the new prescription yields reasonable agreement with the standard generalized Mulliken-Hush method. We then proceed to produce the diabatic and adiabatic potential energy curves along the reaction pathway for intervalence ET in the tetrathiafulvalene-diquinone (Q-TTF-Q) anion. While the unconstrained DFT curve has no reaction barrier and gives Hab≈17kcal /mol, which qualitatively disagrees with experimental results, the Hab calculated from constrained DFT is about 3kcal /mol and the generated ground state has a barrier height of 1.70kcal/mol, successfully predicting (Q-TTF-Q)- to be a class II mixed-valence compound.

Frontiers of controlling energy levels at interfaces

NASA Astrophysics Data System (ADS)

Koch, Norbert

The alignment of electron energy levels at interfaces between semiconductors, dielectrics, and electrodes determines the function and efficiency of all electronic and optoelectronic devices. Reliable guidelines for predicting the level alignment for a given material combination and methods to adjust the intrinsic energy landscape are needed to enable efficient engineering approaches. These are sufficiently understood for established electronic materials, e.g., Si, but for the increasing number of emerging materials, e.g., organic and 2D semiconductors, perovskites, this is work in progress. The intrinsic level alignment and the underlying mechanisms at interfaces between organic and inorganic semiconductors are discussed first. Next, methods to alter the level alignment are introduced, which all base on proper charge density rearrangement at a heterojunction. As interface modification agents we use molecular electron acceptors and donors, as well as molecular photochromic switches that add a dynamic aspect and allow device multifunctionality. For 2D semiconductors surface transfer doping with molecular acceptors/donors transpires as viable method to locally tune the Fermi-level position in the energy gap. The fundamental electronic properties of a prototypical 1D interface between intrinsic and p-doped 2D semiconductor regions are derived from local (scanning probe) and area-averaged (photoemission) spectroscopy experiments. Future research opportunities for attaining unsurpassed interface control through charge density management are discussed.

The energy density distribution of an ideal gas and Bernoulli’s equations

NASA Astrophysics Data System (ADS)

Santos, Leonardo S. F.

2018-05-01

This work discusses the energy density distribution in an ideal gas and the consequences of Bernoulli’s equation and the corresponding relation for compressible fluids. The aim of this work is to study how Bernoulli’s equation determines the energy flow in a fluid, although Bernoulli’s equation does not describe the energy density itself. The model from molecular dynamic considerations that describes an ideal gas at rest with uniform density is modified to explore the gas in motion with non-uniform density and gravitational effects. The difference between the component of the speed of a particle that is parallel to the gas speed and the gas speed itself is called ‘parallel random speed’. The pressure from the ‘parallel random speed’ is denominated as parallel pressure. The modified model predicts that the energy density is the sum of kinetic and potential gravitational energy densities plus two terms with static and parallel pressures. The application of Bernoulli’s equation and the corresponding relation for compressible fluids in the energy density expression has resulted in two new formulations. For incompressible and compressible gas, the energy density expressions are written as a function of stagnation, static and parallel pressures, without any dependence on kinetic or gravitational potential energy densities. These expressions of the energy density are the main contributions of this work. When the parallel pressure was uniform, the energy density distribution for incompressible approximation and compressible gas did not converge to zero for the limit of null static pressure. This result is rather unusual because the temperature tends to zero for null pressure. When the gas was considered incompressible and the parallel pressure was equal to static pressure, the energy density maintained this unusual behaviour with small pressures. If the parallel pressure was equal to static pressure, the energy density converged to zero for the limit of the null pressure only if the gas was compressible. Only the last situation describes an intuitive behaviour for an ideal gas.

Study of Volumetrically Heated Ultra-High Energy Density Plasmas

DOE Office of Scientific and Technical Information (OSTI.GOV)

Rocca, Jorge J.

2016-10-27

Heating dense matter to millions of degrees is important for applications, but requires complex and expensive methods. The major goal of the project was to demonstrate using a compact laser the creation of a new ultra-high energy density plasma regime characterized by simultaneous extremely high temperature and high density, and to study it combining experimental measurements and advanced simulations. We have demonstrated that trapping of intense femtosecond laser pulses deep within ordered nanowire arrays can heat near solid density matter into a new ultra hot plasma regime. Extreme electron densities, and temperatures of several tens of million degrees were achievedmore » using laser pulses of only 0.5 J energy from a compact laser. Our x-ray spectra and simulations showed that extremely highly ionized plasma volumes several micrometers in depth are generated by irradiation of gold and Nickel nanowire arrays with femtosecond laser pulses of relativistic intensities. We obtained extraordinarily high degrees of ionization (e.g. we peeled 52 electrons from gold atoms, and up to 26 electrons from nickel atoms). In the process we generated Gigabar pressures only exceeded in the central hot spot of highly compressed thermonuclear fusion plasmas.. The plasma created after the dissolved wires expand, collide, and thermalize, is computed to have a thermal energy density of 0.3 GJ cm -3 and a pressure of 1-2 Gigabar. These are pressures only exceeded in highly compressed thermonuclear fusion plasmas. Scaling these results to higher laser intensities promises to create plasmas with temperatures and pressures exceeding those in the center of the sun.« less

Coupled-cluster, Möller Plesset (MP2), Density Fitted Local MP2, and Density Functional Theory Examination of the Energetic and Structural Features of Hydrophobic Solvation: Water and Pentane

DOE Office of Scientific and Technical Information (OSTI.GOV)

Ghadar, Yasaman; Clark, Aurora E.

2012-02-02

The interaction potentials between immiscible polar and non-polar solvents are a major driving force behind the formation of liquid:liquid interfaces. In this work, the interaction energy of water–pentane dimer has been determined using coupled-cluster theory with single double (triple) excitations [CCSD(T)], 2nd order Möller Plesset perturbation theory (MP2), density fitted local MP2 (DF-LMP2), as well as density functional theory using a wide variety of density functionals and several different basis sets. The M05-2X exchange correlation functionals exhibit excellent agreement with CCSD(T) and DF-LMP2 after taking into account basis set superposition error. The gas phase water–pentane interaction energy is found tomore » be quite sensitive to the specific pentane isomer (2,2- dimethylpropane vs. n-pentane) and relative orientation of the monomeric constituents. Subsequent solution phase cluster calculations of 2,2-dimethylpropane and n-pentane solvated by water indicate a positive free energy of solvation that is in good agreement with available experimental data. Structural parameters are quite sensitive to the density functional employed and reflect differences in the two-body interaction energy calculated by each method. In contrast, cluster calculations of pentane solvation of H2O solute are found to be inadequate for describing the organic solvent, likely due to limitations associated with the functionals employed (B3LYP, BHandH, and M05-2X).« less

Electrodeposited nickel-cobalt sulfide nanosheet on polyacrylonitrile nanofibers: a binder-free electrode for flexible supercapacitors

NASA Astrophysics Data System (ADS)

Kamran Sami, Syed; Siddiqui, Saqib; Tajmeel Feroze, Muhammad; Chung, Chan-Hwa

2017-11-01

To pursue high-performance energy storage devices with both high energy density and power density, one-dimensional (1D) nanostructures play a key role in the development of functional devices including energy conversion, energy storage, and environmental devices. The polyacrylonitrile (PAN) nanofibers were obtained by the versatile electrospinning method. An ultra-thin nickel-cobalt sulfide (NiCoS) layer was conformably electrodeposited on a self-standing PAN nanofibers by cyclic voltammetry to fabricate the light-weighted porous electrodes for supercapacitors. The porous web of PAN nanofibers acts as a high-surface-area scaffold with significant electrochemical performance, while the electrodeposition of metal sulfide nanosheet further enhances the specific capacitance. The fabricated NiCoS on PAN (NiCoS/PAN) nanofibers exhibits a very high capacitance of 1513 F g-1 at 5 A g-1 in 1 M potassium chloride (KCl) aqueous electrolyte with superior rate capability and excellent electrochemical stability as a hybrid electrode. The high capacitance of the NiCoS is attributed to the large surface area of the electrospun PAN nanofibers scaffold, which has offered a large number of active sites for possible redox reaction of ultra-thin NiCoS layer. Benefiting from the compositional features and electrode architectures, the hybrid electrode of NiCoS/PAN nanofibers shows greatly improved electrochemical performance with an ultra-high capacitance (1124 F g-1 at 50 A g-1). Moreover, a binder-free asymmetric supercapacitor device is also fabricated by using NiCoS/PAN nanofibers as the positive electrode and activated carbon (MSP-20) on PAN nanofibers as the negative electrode; this demonstrates high energy density of 56.904 W h kg-1 at a power density of 1.445 kW kg-1, and it still delivers the energy density of 33.3923 W h kg-1 even at higher power density of 16.5013 kW kg-1.

Investigation of various energy deposition kernel refinements for the convolution/superposition method

PubMed Central

Huang, Jessie Y.; Eklund, David; Childress, Nathan L.; Howell, Rebecca M.; Mirkovic, Dragan; Followill, David S.; Kry, Stephen F.

2013-01-01

Purpose: Several simplifications used in clinical implementations of the convolution/superposition (C/S) method, specifically, density scaling of water kernels for heterogeneous media and use of a single polyenergetic kernel, lead to dose calculation inaccuracies. Although these weaknesses of the C/S method are known, it is not well known which of these simplifications has the largest effect on dose calculation accuracy in clinical situations. The purpose of this study was to generate and characterize high-resolution, polyenergetic, and material-specific energy deposition kernels (EDKs), as well as to investigate the dosimetric impact of implementing spatially variant polyenergetic and material-specific kernels in a collapsed cone C/S algorithm. Methods: High-resolution, monoenergetic water EDKs and various material-specific EDKs were simulated using the EGSnrc Monte Carlo code. Polyenergetic kernels, reflecting the primary spectrum of a clinical 6 MV photon beam at different locations in a water phantom, were calculated for different depths, field sizes, and off-axis distances. To investigate the dosimetric impact of implementing spatially variant polyenergetic kernels, depth dose curves in water were calculated using two different implementations of the collapsed cone C/S method. The first method uses a single polyenergetic kernel, while the second method fully takes into account spectral changes in the convolution calculation. To investigate the dosimetric impact of implementing material-specific kernels, depth dose curves were calculated for a simplified titanium implant geometry using both a traditional C/S implementation that performs density scaling of water kernels and a novel implementation using material-specific kernels. Results: For our high-resolution kernels, we found good agreement with the Mackie et al. kernels, with some differences near the interaction site for low photon energies (<500 keV). For our spatially variant polyenergetic kernels, we found that depth was the most dominant factor affecting the pattern of energy deposition; however, the effects of field size and off-axis distance were not negligible. For the material-specific kernels, we found that as the density of the material increased, more energy was deposited laterally by charged particles, as opposed to in the forward direction. Thus, density scaling of water kernels becomes a worse approximation as the density and the effective atomic number of the material differ more from water. Implementation of spatially variant, polyenergetic kernels increased the percent depth dose value at 25 cm depth by 2.1%–5.8% depending on the field size, while implementation of titanium kernels gave 4.9% higher dose upstream of the metal cavity (i.e., higher backscatter dose) and 8.2% lower dose downstream of the cavity. Conclusions: Of the various kernel refinements investigated, inclusion of depth-dependent and metal-specific kernels into the C/S method has the greatest potential to improve dose calculation accuracy. Implementation of spatially variant polyenergetic kernels resulted in a harder depth dose curve and thus has the potential to affect beam modeling parameters obtained in the commissioning process. For metal implants, the C/S algorithms generally underestimate the dose upstream and overestimate the dose downstream of the implant. Implementation of a metal-specific kernel mitigated both of these errors. PMID:24320507

High energy storage density over a broad temperature range in sodium bismuth titanate-based lead-free ceramics.

PubMed

Yang, Haibo; Yan, Fei; Lin, Ying; Wang, Tong; Wang, Fen

2017-08-18

A series of (1-x)Bi 0.48 La 0.02 Na 0.48 Li 0.02 Ti 0.98 Zr 0.02 O 3 -xNa 0.73 Bi 0.09 NbO 3 ((1-x)LLBNTZ-xNBN) (x = 0-0.14) ceramics were designed and fabricated using the conventional solid-state sintering method. The phase structure, microstructure, dielectric, ferroelectric and energy storage properties of the ceramics were systematically investigated. The results indicate that the addition of Na 0.73 Bi 0.09 NbO 3 (NBN) could decrease the remnant polarization (P r ) and improve the temperature stability of dielectric constant obviously. The working temperature range satisfying TCC 150  °C  ≤±15% of this work spans over 400 °C with the compositions of x ≥ 0.06. The maximum energy storage density can be obtained for the sample with x = 0.10 at room temperature, with an energy storage density of 2.04 J/cm 3 at 178 kV/cm. In addition, the (1-x)LLBNTZ-xNBN ceramics exhibit excellent energy storage properties over a wide temperature range from room temperature to 90 °C. The values of energy storage density and energy storage efficiency is 0.91 J/cm 3 and 79.51%, respectively, for the 0.90LLBNTZ-0.10NBN ceramic at the condition of 100 kV/cm and 90 °C. It can be concluded that the (1-x)LLBNTZ-xNBN ceramics are promising lead-free candidate materials for energy storage devices over a broad temperature range.

High Energy Density Li-ion Cells for EV’s Based on Novel, High Voltage Cathode Material Systems

DOE Office of Scientific and Technical Information (OSTI.GOV)

Kepler, Keith D.; Slater, Michael

This Li-ion cell technology development project had three objectives: to develop advanced electrode materials and cell components to enable stable high-voltage operation; to design and demonstrate a Li-ion cell using these materials that meets the PHEV40 performance targets; and to design and demonstrate a Li-ion cell using these materials that meets the EV performance targets. The major challenge to creating stable high energy cells with long cycle life is system integration. Although materials that can give high energy cells are known, stabilizing them towards long-term cycling in the presence of other novel cell components is a major challenge. The majormore » technical barriers addressed by this work include low cathode specific energy, poor electrolyte stability during high voltage operation, and insufficient capacity retention during deep discharge for Si-containing anodes. Through the course of this project, Farasis was able to improve capacity retention of NCM materials for 4.4+ V operation, through both surface treatment and bulk-doping approaches. Other material advances include increased rate capability and of HE-NCM materials through novel synthesis approach, doubling the relative capacity at 1C over materials synthesized using standard methods. Silicon active materials proved challenging throughout the project and ultimately were the limiting factor in the energy density vs. cycle life trade off. By avoiding silicon anodes for the lower energy PHEV design, we manufactured cells with intermediate energy density and long cycle life under high voltage operation for PHEV applications. Cells with high energy density for EV applications were manufactured targeting a 300 Wh/kg design and were able to achieve > 200 cycles.« less

Singularity analysis: theory and further developments

NASA Astrophysics Data System (ADS)

Cheng, Qiuming

2015-04-01

Since the concept of singularity and local singularity analysis method (LSA) were originally proposed by the author for characterizing the nonlinear property of hydrothermal mineralization processes, the local singularity analysis technique has been successfully applied for identification of geochemical and geophysical anomalies related to various types of mineral deposits. It has also been shown that the singularity is the generic property of singular geo-processes which result in anomalous amounts of energy release or material accumulation within a narrow spatial-temporal interval. In the current paper we introduce several new developments about singularity analysis. First is a new concept of 'fractal density' which describes the singularity of complex phenomena of fractal nature. While the ordinary density possesses a unit of ratio of mass and volume (e.g. g/cm3, kg/m3) or ratio of energy over volume or time (e.g. J/cm3, w/L3, w/s), the fractal density has a unit of ratio of mass over fractal set or energy over fractal set (e.g. g/cmα, kg/mα, J/ mα, w/Lα, where α can be a non-integer). For the matter with fractal density (a non-integer α), the ordinary density of the phenomena (mass or energy) no longer exists and depicts singularity. We demonstrate that most of extreme geo-processes occurred in the earth crust originated from cascade earth dynamics (mental convection, plate tectonics, orogeny and weathering etc) may cause fractal density of mass accumulation or energy release. The examples to be used to demonstrate the concepts of fractal density and singularity are earthquakes, floods, volcanos, hurricanes, heat flow over oceanic ridge, hydrothermal mineralization in orogenic belt, and anomalies in regolith over mine caused by ore and toxic elements vertical migration. Other developments of singularity theory and methodologies including singular Kriging and singularity weights of evidence model for information integration will also be introduced.

Diffusion quantum Monte Carlo and density functional calculations of the structural stability of bilayer arsenene

NASA Astrophysics Data System (ADS)

Kadioglu, Yelda; Santana, Juan A.; Özaydin, H. Duygu; Ersan, Fatih; Aktürk, O. Üzengi; Aktürk, Ethem; Reboredo, Fernando A.

2018-06-01

We have studied the structural stability of monolayer and bilayer arsenene (As) in the buckled (b) and washboard (w) phases with diffusion quantum Monte Carlo (DMC) and density functional theory (DFT) calculations. DMC yields cohesive energies of 2.826(2) eV/atom for monolayer b-As and 2.792(3) eV/atom for w-As. In the case of bilayer As, DMC and DFT predict that AA-stacking is the more stable form of b-As, while AB is the most stable form of w-As. The DMC layer-layer binding energies for b-As-AA and w-As-AB are 30(1) and 53(1) meV/atom, respectively. The interlayer separations were estimated with DMC at 3.521(1) Å for b-As-AA and 3.145(1) Å for w-As-AB. A comparison of DMC and DFT results shows that the van der Waals density functional method yields energetic properties of arsenene close to DMC, while the DFT + D3 method closely reproduced the geometric properties from DMC. The electronic properties of monolayer and bilayer arsenene were explored with various DFT methods. The bandgap values vary significantly with the DFT method, but the results are generally qualitatively consistent. We expect the present work to be useful for future experiments attempting to prepare multilayer arsenene and for further development of DFT methods for weakly bonded systems.

Controlling the formation of rodlike V2O5 nanocrystals on reduced graphene oxide for high-performance supercapacitors.

PubMed

Li, Meili; Sun, Guoying; Yin, Pingping; Ruan, Changping; Ai, Kelong

2013-11-13

Vanadium pentoxide (V2O5) has attracted much attention for energy storage application because of its high Faradaic activity and stable crystal structure, which make it a promising electrode material for supercapacitors. However, the low electronic conductivity and small lithium-ion diffusion coefficient of V2O5 limit its practical applications. To overcome these limitations, a facile and efficient method is here demonstrated for the fabrication of V2O5/reduced graphene oxide (rGO) nanocomposites as electrode materials for supercapacitors. With this method, the reduction of graphene oxide can be achieved in a cost-effective and environmentally friendly solvent, without the addition of any other toxic reducing agent. Importantly, this solvent can control the formation of the uniform rodlike V2O5 nanocrystals on the surface of rGO. Compared to pure V2O5 microspheres, the V2O5/rGO nanocomposites exhibited a higher specific capacitance of 537 F g(-1) at a current density of 1 A g(-1) in neutral aqueous electrolytes, a higher energy density of 74.58 Wh kg(-1) at a power density of 500 W kg(-1), and better stability even after 1000 charge/discharge cycles. Their excellent performances can be attributed to the synergistic effect of rGO and rodlike V2O5 nanocrystals. Such impressive results may promote new opportunities for these electrode materials in high-energy-density storage systems.

Soft- to network hard-material for constructing both ion- and electron-conductive hierarchical porous structure to significantly boost energy density of a supercapacitor.

PubMed

Yang, Pingping; Xie, Jiale; Guo, Chunxian; Li, Chang Ming

2017-01-01

Soft-material PEDOT is used to network hard Co 3 O 4 nanowires for constructing both ion- and electron-conductive hierarchical porous structure Co 3 O 4 /PEDOT to greatly boost the capacitor energy density than sum of that of plain Co 3 O 4 nanowires and PEDOT film. Specifically, the networked hierarchical porous structure of Co 3 O 4 /PEDOT is synthesized and tailored through hydrothermal method and post-electrochemical polymerization method for the PEDOT coating onto Co 3 O 4 nanowires. Typically, Co 3 O 4 /PEDOT supercapacitor gets a highest areal capacitance of 160mFcm -2 at a current density of 0.2mAcm -2 , which is about 2.2 times larger than the sum of that of plain Co 3 O 4 NWs (0.92mFcm -2 ) and PEDOT film (69.88mFcm -2 ). Besides, if only PEDOT as active mass is counted, Co 3 O 4 /PEDOT cell can achieve a highest capacitance of 567.21Fg -1 , this is the highest capacitance value obtained by PEDOT-based supercapacitors. Furthermore, this soft-hard network porous structure also achieves a high cycling stability of 93% capacitance retention after the 20,000th cycle. This work demonstrates a new approach to constructing both ion and electron conductive hierarchical porous structure to significantly boost energy density of a supercapacitor. Copyright © 2016 Elsevier Inc. All rights reserved.

Electron correlation in the interacting quantum atoms partition via coupled-cluster lagrangian densities.

PubMed

Holguín-Gallego, Fernando José; Chávez-Calvillo, Rodrigo; García-Revilla, Marco; Francisco, Evelio; Pendás, Ángel Martín; Rocha-Rinza, Tomás

2016-07-15

The electronic energy partition established by the Interacting Quantum Atoms (IQA) approach is an important method of wavefunction analyses which has yielded valuable insights about different phenomena in physical chemistry. Most of the IQA applications have relied upon approximations, which do not include either dynamical correlation (DC) such as Hartree-Fock (HF) or external DC like CASSCF theory. Recently, DC was included in the IQA method by means of HF/Coupled-Cluster (CC) transition densities (Chávez-Calvillo et al., Comput. Theory Chem. 2015, 1053, 90). Despite the potential utility of this approach, it has a few drawbacks, for example, it is not consistent with the calculation of CC properties different from the total electronic energy. To improve this situation, we have implemented the IQA energy partition based on CC Lagrangian one- and two-electron orbital density matrices. The development presented in this article is tested and illustrated with the H2 , LiH, H2 O, H2 S, N2 , and CO molecules for which the IQA results obtained under the consideration of (i) the CC Lagrangian, (ii) HF/CC transition densities, and (iii) HF are critically analyzed and compared. Additionally, the effect of the DC in the different components of the electronic energy in the formation of the T-shaped (H2 )2 van der Waals cluster and the bimolecular nucleophilic substitution between F(-) and CH3 F is examined. We anticipate that the approach put forward in this article will provide new understandings on subjects in physical chemistry wherein DC plays a crucial role like molecular interactions along with chemical bonding and reactivity. © 2016 Wiley Periodicals, Inc. © 2016 Wiley Periodicals, Inc.

A moving mesh finite difference method for equilibrium radiation diffusion equations

DOE Office of Scientific and Technical Information (OSTI.GOV)

Yang, Xiaobo, E-mail: xwindyb@126.com; Huang, Weizhang, E-mail: whuang@ku.edu; Qiu, Jianxian, E-mail: jxqiu@xmu.edu.cn

2015-10-01

An efficient moving mesh finite difference method is developed for the numerical solution of equilibrium radiation diffusion equations in two dimensions. The method is based on the moving mesh partial differential equation approach and moves the mesh continuously in time using a system of meshing partial differential equations. The mesh adaptation is controlled through a Hessian-based monitor function and the so-called equidistribution and alignment principles. Several challenging issues in the numerical solution are addressed. Particularly, the radiation diffusion coefficient depends on the energy density highly nonlinearly. This nonlinearity is treated using a predictor–corrector and lagged diffusion strategy. Moreover, the nonnegativitymore » of the energy density is maintained using a cutoff method which has been known in literature to retain the accuracy and convergence order of finite difference approximation for parabolic equations. Numerical examples with multi-material, multiple spot concentration situations are presented. Numerical results show that the method works well for radiation diffusion equations and can produce numerical solutions of good accuracy. It is also shown that a two-level mesh movement strategy can significantly improve the efficiency of the computation.« less

Fully-relativistic full-potential multiple scattering theory: A pathology-free scheme

NASA Astrophysics Data System (ADS)

Liu, Xianglin; Wang, Yang; Eisenbach, Markus; Stocks, G. Malcolm

2018-03-01

The Green function plays an essential role in the Korringa-Kohn-Rostoker(KKR) multiple scattering method. In practice, it is constructed from the regular and irregular solutions of the local Kohn-Sham equation and robust methods exist for spherical potentials. However, when applied to a non-spherical potential, numerical errors from the irregular solutions give rise to pathological behaviors of the charge density at small radius. Here we present a full-potential implementation of the fully-relativistic KKR method to perform ab initio self-consistent calculation by directly solving the Dirac differential equations using the generalized variable phase (sine and cosine matrices) formalism Liu et al. (2016). The pathology around the origin is completely eliminated by carrying out the energy integration of the single-site Green function along the real axis. By using an efficient pole-searching technique to identify the zeros of the well-behaved Jost matrices, we demonstrated that this scheme is numerically stable and computationally efficient, with speed comparable to the conventional contour energy integration method, while free of the pathology problem of the charge density. As an application, this method is utilized to investigate the crystal structures of polonium and their bulk properties, which is challenging for a conventional real-energy scheme. The noble metals are also calculated, both as a test of our method and to study the relativistic effects.

Fully-relativistic full-potential multiple scattering theory: A pathology-free scheme

DOE Office of Scientific and Technical Information (OSTI.GOV)

Liu, Xianglin; Wang, Yang; Eisenbach, Markus

The Green function plays an essential role in the Korringa–Kohn–Rostoker(KKR) multiple scattering method. In practice, it is constructed from the regular and irregular solutions of the local Kohn–Sham equation and robust methods exist for spherical potentials. However, when applied to a non-spherical potential, numerical errors from the irregular solutions give rise to pathological behaviors of the charge density at small radius. Here we present a full-potential implementation of the fully-relativistic KKR method to perform ab initio self-consistent calculation by directly solving the Dirac differential equations using the generalized variable phase (sine and cosine matrices) formalism Liu et al. (2016). Themore » pathology around the origin is completely eliminated by carrying out the energy integration of the single-site Green function along the real axis. Here, by using an efficient pole-searching technique to identify the zeros of the well-behaved Jost matrices, we demonstrated that this scheme is numerically stable and computationally efficient, with speed comparable to the conventional contour energy integration method, while free of the pathology problem of the charge density. As an application, this method is utilized to investigate the crystal structures of polonium and their bulk properties, which is challenging for a conventional real-energy scheme. The noble metals are also calculated, both as a test of our method and to study the relativistic effects.« less

Exploiting the spatial locality of electron correlation within the parametric two-electron reduced-density-matrix method

NASA Astrophysics Data System (ADS)

DePrince, A. Eugene; Mazziotti, David A.

2010-01-01

The parametric variational two-electron reduced-density-matrix (2-RDM) method is applied to computing electronic correlation energies of medium-to-large molecular systems by exploiting the spatial locality of electron correlation within the framework of the cluster-in-molecule (CIM) approximation [S. Li et al., J. Comput. Chem. 23, 238 (2002); J. Chem. Phys. 125, 074109 (2006)]. The 2-RDMs of individual molecular fragments within a molecule are determined, and selected portions of these 2-RDMs are recombined to yield an accurate approximation to the correlation energy of the entire molecule. In addition to extending CIM to the parametric 2-RDM method, we (i) suggest a more systematic selection of atomic-orbital domains than that presented in previous CIM studies and (ii) generalize the CIM method for open-shell quantum systems. The resulting method is tested with a series of polyacetylene molecules, water clusters, and diazobenzene derivatives in minimal and nonminimal basis sets. Calculations show that the computational cost of the method scales linearly with system size. We also compute hydrogen-abstraction energies for a series of hydroxyurea derivatives. Abstraction of hydrogen from hydroxyurea is thought to be a key step in its treatment of sickle cell anemia; the design of hydroxyurea derivatives that oxidize more rapidly is one approach to devising more effective treatments.

Fully-relativistic full-potential multiple scattering theory: A pathology-free scheme

DOE PAGES

Liu, Xianglin; Wang, Yang; Eisenbach, Markus; ...

2017-10-28

The Green function plays an essential role in the Korringa–Kohn–Rostoker(KKR) multiple scattering method. In practice, it is constructed from the regular and irregular solutions of the local Kohn–Sham equation and robust methods exist for spherical potentials. However, when applied to a non-spherical potential, numerical errors from the irregular solutions give rise to pathological behaviors of the charge density at small radius. Here we present a full-potential implementation of the fully-relativistic KKR method to perform ab initio self-consistent calculation by directly solving the Dirac differential equations using the generalized variable phase (sine and cosine matrices) formalism Liu et al. (2016). Themore » pathology around the origin is completely eliminated by carrying out the energy integration of the single-site Green function along the real axis. Here, by using an efficient pole-searching technique to identify the zeros of the well-behaved Jost matrices, we demonstrated that this scheme is numerically stable and computationally efficient, with speed comparable to the conventional contour energy integration method, while free of the pathology problem of the charge density. As an application, this method is utilized to investigate the crystal structures of polonium and their bulk properties, which is challenging for a conventional real-energy scheme. The noble metals are also calculated, both as a test of our method and to study the relativistic effects.« less