Monte Carlo study of four dimensional binary hard hypersphere mixtures

NASA Astrophysics Data System (ADS)

Bishop, Marvin; Whitlock, Paula A.

2012-01-01

A multithreaded Monte Carlo code was used to study the properties of binary mixtures of hard hyperspheres in four dimensions. The ratios of the diameters of the hyperspheres examined were 0.4, 0.5, 0.6, and 0.8. Many total densities of the binary mixtures were investigated. The pair correlation functions and the equations of state were determined and compared with other simulation results and theoretical predictions. At lower diameter ratios the pair correlation functions of the mixture agree with the pair correlation function of a one component fluid at an appropriately scaled density. The theoretical results for the equation of state compare well to the Monte Carlo calculations for all but the highest densities studied.

Gradient corrections to the exchange-correlation free energy

DOE PAGES

Sjostrom, Travis; Daligault, Jerome

2014-10-07

We develop the first-order gradient correction to the exchange-correlation free energy of the homogeneous electron gas for use in finite-temperature density functional calculations. Based on this, we propose and implement a simple temperature-dependent extension for functionals beyond the local density approximation. These finite-temperature functionals show improvement over zero-temperature functionals, as compared to path-integral Monte Carlo calculations for deuterium equations of state, and perform without computational cost increase compared to zero-temperature functionals and so should be used for finite-temperature calculations. Furthermore, while the present functionals are valid at all temperatures including zero, non-negligible difference with zero-temperature functionals begins at temperatures abovemore » 10 000 K.« less

Multiconfiguration pair-density functional theory investigation of the electronic spectrum of MnO4-

NASA Astrophysics Data System (ADS)

Sharma, Prachi; Truhlar, Donald G.; Gagliardi, Laura

2018-03-01

The electronic spectrum of permanganate ions contains various highly multiconfigurational ligand-to-metal charge transfer states and is notorious for being one of the most challenging systems to be treated by quantum-chemical methods. Here we studied the lowest nine vertical excitation energies using restricted active space second-order perturbation theory (RASPT2) and multiconfiguration pair-density functional theory (MC-PDFT) to test and compare these two theories in computing such a challenging spectrum. The results are compared to literature data, including time-dependent density functional theory, completely renormalized equation-of-motion couple-cluster theory with single and double excitations, symmetry-adapted-cluster configuration interaction, and experimental spectra in the gas phase and solution. Our results show that MC-PDFT accurately predicts the spectrum at a significantly reduced cost as compared to RASPT2.

Multiconfiguration pair-density functional theory investigation of the electronic spectrum of MnO4.

PubMed

Sharma, Prachi; Truhlar, Donald G; Gagliardi, Laura

2018-03-28

The electronic spectrum of permanganate ions contains various highly multiconfigurational ligand-to-metal charge transfer states and is notorious for being one of the most challenging systems to be treated by quantum-chemical methods. Here we studied the lowest nine vertical excitation energies using restricted active space second-order perturbation theory (RASPT2) and multiconfiguration pair-density functional theory (MC-PDFT) to test and compare these two theories in computing such a challenging spectrum. The results are compared to literature data, including time-dependent density functional theory, completely renormalized equation-of-motion couple-cluster theory with single and double excitations, symmetry-adapted-cluster configuration interaction, and experimental spectra in the gas phase and solution. Our results show that MC-PDFT accurately predicts the spectrum at a significantly reduced cost as compared to RASPT2.

Accuracy of electron densities obtained via Koopmans-compliant hybrid functionals

NASA Astrophysics Data System (ADS)

Elmaslmane, A. R.; Wetherell, J.; Hodgson, M. J. P.; McKenna, K. P.; Godby, R. W.

2018-04-01

We evaluate the accuracy of electron densities and quasiparticle energy gaps given by hybrid functionals by directly comparing these to the exact quantities obtained from solving the many-electron Schrödinger equation. We determine the admixture of Hartree-Fock exchange to approximate exchange-correlation in our hybrid functional via one of several physically justified constraints, including the generalized Koopmans' theorem. We find that hybrid functionals yield strikingly accurate electron densities and gaps in both exchange-dominated and correlated systems. We also discuss the role of the screened Fock operator in the success of hybrid functionals.

A long-range-corrected density functional that performs well for both ground-state properties and time-dependent density functional theory excitation energies, including charge-transfer excited states.

PubMed

Rohrdanz, Mary A; Martins, Katie M; Herbert, John M

2009-02-07

We introduce a hybrid density functional that asymptotically incorporates full Hartree-Fock exchange, based on the long-range-corrected exchange-hole model of Henderson et al. [J. Chem. Phys. 128, 194105 (2008)]. The performance of this functional, for ground-state properties and for vertical excitation energies within time-dependent density functional theory, is systematically evaluated, and optimal values are determined for the range-separation parameter, omega, and for the fraction of short-range Hartree-Fock exchange. We denote the new functional as LRC-omegaPBEh, since it reduces to the standard PBEh hybrid functional (also known as PBE0 or PBE1PBE) for a certain choice of its two parameters. Upon optimization of these parameters against a set of ground- and excited-state benchmarks, the LRC-omegaPBEh functional fulfills three important requirements: (i) It outperforms the PBEh hybrid functional for ground-state atomization energies and reaction barrier heights; (ii) it yields statistical errors comparable to PBEh for valence excitation energies in both small and medium-sized molecules; and (iii) its performance for charge-transfer excitations is comparable to its performance for valence excitations. LRC-omegaPBEh, with the parameters determined herein, is the first density functional that satisfies all three criteria. Notably, short-range Hartree-Fock exchange appears to be necessary in order to obtain accurate ground-state properties and vertical excitation energies using the same value of omega.

Equilibrium Structures and Absorption Spectra for SixOy-nH2O Molecular Clusters using Density Functional Theory

DTIC Science & Technology

2017-05-04

Naval Research Laboratory Washington, DC 20375-5320 NRL/MR/6390--17-9723 Equilibrium Structures and Absorption Spectra for SixOy-nH2O Molecular...Absorption Spectra for SixOy-nH2O Molecular Clusters using Density Functional Theory L. Huang, S.G. Lambrakos, and L. Massa1 Naval Research Laboratory, Code...and time-dependent density functional theory (TD-DFT). The size of the clusters considered is relatively large compared to those considered in

In vitro cell-mediated immunity after thermal injury is not impaired. Density gradient purification of mononuclear cells is associated with spurious (artifactual) immunosuppression.

PubMed Central

Xu, D Z; Deitch, E A; Sittig, K; Qi, L; McDonald, J C

1988-01-01

Mononuclear cells isolated by density gradient centrifugation from the peripheral blood of burn patients, but not healthy volunteers, are contaminated with large numbers of nonmononuclear cells. These contaminating leukocytes could cause artifactual alterations in standard in vitro tests of lymphocyte function. Thus, we compared the in vitro blastogenic response of density gradient purified leukocytes and T-cell purified lymphocytes from 13 burn patients to mitogenic (PHA) and antigenic stimuli. The mitogenic and antigenic response of the patients' density gradient purified leukocytes were impaired compared to healthy volunteers (p less than 0.01). However, when the contaminating nonlymphocytes were removed, the patients' cells responded normally to both stimuli. Thus, density gradient purified mononuclear cells from burn patients are contaminated by leukocytes that are not phenotypically or functionally lymphocytes. Since the lymphocytes from burn patients respond normally to PHA and alloantigens after the contaminating nonlymphocyte cell population has been removed, it appears that in vitro assays of lymphocyte function using density gradient purified leukocytes may give spurious results. PMID:2973771

Importance of finite-temperature exchange correlation for warm dense matter calculations.

PubMed

Karasiev, Valentin V; Calderín, Lázaro; Trickey, S B

2016-06-01

The effects of an explicit temperature dependence in the exchange correlation (XC) free-energy functional upon calculated properties of matter in the warm dense regime are investigated. The comparison is between the Karasiev-Sjostrom-Dufty-Trickey (KSDT) finite-temperature local-density approximation (TLDA) XC functional [Karasiev et al., Phys. Rev. Lett. 112, 076403 (2014)PRLTAO0031-900710.1103/PhysRevLett.112.076403] parametrized from restricted path-integral Monte Carlo data on the homogeneous electron gas (HEG) and the conventional Monte Carlo parametrization ground-state LDA XC [Perdew-Zunger (PZ)] functional evaluated with T-dependent densities. Both Kohn-Sham (KS) and orbital-free density-functional theories are used, depending upon computational resource demands. Compared to the PZ functional, the KSDT functional generally lowers the dc electrical conductivity of low-density Al, yielding improved agreement with experiment. The greatest lowering is about 15% for T=15 kK. Correspondingly, the KS band structure of low-density fcc Al from the KSDT functional exhibits a clear increase in interband separation above the Fermi level compared to the PZ bands. In some density-temperature regimes, the deuterium equations of state obtained from the two XC functionals exhibit pressure differences as large as 4% and a 6% range of differences. However, the hydrogen principal Hugoniot is insensitive to the explicit XC T dependence because of cancellation between the energy and pressure-volume work difference terms in the Rankine-Hugoniot equation. Finally, the temperature at which the HEG becomes unstable is T≥7200 K for the T-dependent XC, a result that the ground-state XC underestimates by about 1000 K.

Excited-state absorption in tetrapyridyl porphyrins: comparing real-time and quadratic-response time-dependent density functional theory

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

Bowman, David N.; Asher, Jason C.; Fischer, Sean A.

2017-01-01

Threemeso-substituted tetrapyridyl porphyrins (free base, Ni(ii), and Cu(ii)) were investigated for their optical limiting (OL) capabilities using real-time (RT-), linear-response (LR-), and quadratic-response (QR-) time-dependent density functional theory (TDDFT) methods.

Performance of exchange-correlation functionals in density functional theory calculations for liquid metal: A benchmark test for sodium.

PubMed

Han, Jeong-Hwan; Oda, Takuji

2018-04-14

The performance of exchange-correlation functionals in density-functional theory (DFT) calculations for liquid metal has not been sufficiently examined. In the present study, benchmark tests of Perdew-Burke-Ernzerhof (PBE), Armiento-Mattsson 2005 (AM05), PBE re-parameterized for solids, and local density approximation (LDA) functionals are conducted for liquid sodium. The pair correlation function, equilibrium atomic volume, bulk modulus, and relative enthalpy are evaluated at 600 K and 1000 K. Compared with the available experimental data, the errors range from -11.2% to 0.0% for the atomic volume, from -5.2% to 22.0% for the bulk modulus, and from -3.5% to 2.5% for the relative enthalpy depending on the DFT functional. The generalized gradient approximation functionals are superior to the LDA functional, and the PBE and AM05 functionals exhibit the best performance. In addition, we assess whether the error tendency in liquid simulations is comparable to that in solid simulations, which would suggest that the atomic volume and relative enthalpy performances are comparable between solid and liquid states but that the bulk modulus performance is not. These benchmark test results indicate that the results of liquid simulations are significantly dependent on the exchange-correlation functional and that the DFT functional performance in solid simulations can be used to roughly estimate the performance in liquid simulations.

Performance of exchange-correlation functionals in density functional theory calculations for liquid metal: A benchmark test for sodium

NASA Astrophysics Data System (ADS)

Han, Jeong-Hwan; Oda, Takuji

2018-04-01

The performance of exchange-correlation functionals in density-functional theory (DFT) calculations for liquid metal has not been sufficiently examined. In the present study, benchmark tests of Perdew-Burke-Ernzerhof (PBE), Armiento-Mattsson 2005 (AM05), PBE re-parameterized for solids, and local density approximation (LDA) functionals are conducted for liquid sodium. The pair correlation function, equilibrium atomic volume, bulk modulus, and relative enthalpy are evaluated at 600 K and 1000 K. Compared with the available experimental data, the errors range from -11.2% to 0.0% for the atomic volume, from -5.2% to 22.0% for the bulk modulus, and from -3.5% to 2.5% for the relative enthalpy depending on the DFT functional. The generalized gradient approximation functionals are superior to the LDA functional, and the PBE and AM05 functionals exhibit the best performance. In addition, we assess whether the error tendency in liquid simulations is comparable to that in solid simulations, which would suggest that the atomic volume and relative enthalpy performances are comparable between solid and liquid states but that the bulk modulus performance is not. These benchmark test results indicate that the results of liquid simulations are significantly dependent on the exchange-correlation functional and that the DFT functional performance in solid simulations can be used to roughly estimate the performance in liquid simulations.

Interconfigurational energies in transition-metal atoms using gradient-corrected density-functional theory

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

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

1991-03-15

The rapid variation of charge and spin densities in atoms and molecules provides a severe test for local-density-functional theory and for the use of gradient corrections. In the study reported in this paper, we use the Langreth, Mehl, and Hu (LMH) functional and the generalized gradient approximation (GGA) of Perdew and Yue to calculate {ital s}-{ital d} transition energies, 4{ital s} ionization energies, and 3{ital d} ionization energies for the 3{ital d} transition-metal atoms. These calculations are compared with results from the local-density functional of Vosko, Wilk, and Nusair. By comparison with experimental energies, we find that the gradient functionalsmore » are only marginally more successful than the local-density approximation in calculating energy differences between states in transition-metal atoms. The GGA approximation is somewhat better than the LMH functional for most of the atoms studied, although there are several exceptions.« less

Derivative discontinuity and exchange-correlation potential of meta-GGAs in density-functional theory.

PubMed

Eich, F G; Hellgren, Maria

2014-12-14

We investigate fundamental properties of meta-generalized-gradient approximations (meta-GGAs) to the exchange-correlation energy functional, which have an implicit density dependence via the Kohn-Sham kinetic-energy density. To this purpose, we construct the most simple meta-GGA by expressing the local exchange-correlation energy per particle as a function of a fictitious density, which is obtained by inverting the Thomas-Fermi kinetic-energy functional. This simple functional considerably improves the total energy of atoms as compared to the standard local density approximation. The corresponding exchange-correlation potentials are then determined exactly through a solution of the optimized effective potential equation. These potentials support an additional bound state and exhibit a derivative discontinuity at integer particle numbers. We further demonstrate that through the kinetic-energy density any meta-GGA incorporates a derivative discontinuity. However, we also find that for commonly used meta-GGAs the discontinuity is largely underestimated and in some cases even negative.

Derivative discontinuity and exchange-correlation potential of meta-GGAs in density-functional theory

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

Eich, F. G., E-mail: eichf@missouri.edu; Hellgren, Maria

2014-12-14

We investigate fundamental properties of meta-generalized-gradient approximations (meta-GGAs) to the exchange-correlation energy functional, which have an implicit density dependence via the Kohn-Sham kinetic-energy density. To this purpose, we construct the most simple meta-GGA by expressing the local exchange-correlation energy per particle as a function of a fictitious density, which is obtained by inverting the Thomas-Fermi kinetic-energy functional. This simple functional considerably improves the total energy of atoms as compared to the standard local density approximation. The corresponding exchange-correlation potentials are then determined exactly through a solution of the optimized effective potential equation. These potentials support an additional bound state andmore » exhibit a derivative discontinuity at integer particle numbers. We further demonstrate that through the kinetic-energy density any meta-GGA incorporates a derivative discontinuity. However, we also find that for commonly used meta-GGAs the discontinuity is largely underestimated and in some cases even negative.« less

Force Density Function Relationships in 2-D Granular Media

NASA Technical Reports Server (NTRS)

Youngquist, Robert C.; Metzger, Philip T.; Kilts, Kelly N.

2004-01-01

An integral transform relationship is developed to convert between two important probability density functions (distributions) used in the study of contact forces in granular physics. Developing this transform has now made it possible to compare and relate various theoretical approaches with one another and with the experimental data despite the fact that one may predict the Cartesian probability density and another the force magnitude probability density. Also, the transforms identify which functional forms are relevant to describe the probability density observed in nature, and so the modified Bessel function of the second kind has been identified as the relevant form for the Cartesian probability density corresponding to exponential forms in the force magnitude distribution. Furthermore, it is shown that this transform pair supplies a sufficient mathematical framework to describe the evolution of the force magnitude distribution under shearing. Apart from the choice of several coefficients, whose evolution of values must be explained in the physics, this framework successfully reproduces the features of the distribution that are taken to be an indicator of jamming and unjamming in a granular packing. Key words. Granular Physics, Probability Density Functions, Fourier Transforms

The non-Gaussian joint probability density function of slope and elevation for a nonlinear gravity wave field. [in ocean surface

NASA Technical Reports Server (NTRS)

Huang, N. E.; Long, S. R.; Bliven, L. F.; Tung, C.-C.

1984-01-01

On the basis of the mapping method developed by Huang et al. (1983), an analytic expression for the non-Gaussian joint probability density function of slope and elevation for nonlinear gravity waves is derived. Various conditional and marginal density functions are also obtained through the joint density function. The analytic results are compared with a series of carefully controlled laboratory observations, and good agreement is noted. Furthermore, the laboratory wind wave field observations indicate that the capillary or capillary-gravity waves may not be the dominant components in determining the total roughness of the wave field. Thus, the analytic results, though derived specifically for the gravity waves, may have more general applications.

A density functional theory for colloids with two multiple bonding associating sites.

PubMed

Haghmoradi, Amin; Wang, Le; Chapman, Walter G

2016-06-22

Wertheim's multi-density formalism is extended for patchy colloidal fluids with two multiple bonding patches. The theory is developed as a density functional theory to predict the properties of an associating inhomogeneous fluid. The equation of state developed for this fluid depends on the size of the patch, and includes formation of cyclic, branched and linear clusters of associated species. The theory predicts the density profile and the fractions of colloids in different bonding states versus the distance from one wall as a function of bulk density and temperature. The predictions from our theory are compared with previous results for a confined fluid with four single bonding association sites. Also, comparison between the present theory and Monte Carlo simulation indicates a good agreement.

Exchange-correlation approximations for reduced-density-matrix-functional theory at finite temperature: Capturing magnetic phase transitions in the homogeneous electron gas

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

Baldsiefen, Tim; Cangi, Attila; Eich, F. G.

Here, we derive an intrinsically temperature-dependent approximation to the correlation grand potential for many-electron systems in thermodynamical equilibrium in the context of finite-temperature reduced-density-matrix-functional theory (FT-RDMFT). We demonstrate its accuracy by calculating the magnetic phase diagram of the homogeneous electron gas. We compare it to known limits from highly accurate quantum Monte Carlo calculations as well as to phase diagrams obtained within existing exchange-correlation approximations from density functional theory and zero-temperature RDMFT.

Application of information theory to the design of line-scan imaging systems

NASA Technical Reports Server (NTRS)

Huck, F. O.; Park, S. K.; Halyo, N.; Stallman, S.

1981-01-01

Information theory is used to formulate a single figure of merit for assessing the performance of line scan imaging systems as a function of their spatial response (point spread function or modulation transfer function), sensitivity, sampling and quantization intervals, and the statistical properties of a random radiance field. Computational results for the information density and efficiency (i.e., the ratio of information density to data density) are intuitively satisfying and compare well with experimental and theoretical results obtained by earlier investigators concerned with the performance of TV systems.

Exchange-correlation approximations for reduced-density-matrix-functional theory at finite temperature: Capturing magnetic phase transitions in the homogeneous electron gas

DOE PAGES

Baldsiefen, Tim; Cangi, Attila; Eich, F. G.; ...

2017-12-18

Here, we derive an intrinsically temperature-dependent approximation to the correlation grand potential for many-electron systems in thermodynamical equilibrium in the context of finite-temperature reduced-density-matrix-functional theory (FT-RDMFT). We demonstrate its accuracy by calculating the magnetic phase diagram of the homogeneous electron gas. We compare it to known limits from highly accurate quantum Monte Carlo calculations as well as to phase diagrams obtained within existing exchange-correlation approximations from density functional theory and zero-temperature RDMFT.

Multiconfiguration Pair-Density Functional Theory Predicts Spin-State Ordering in Iron Complexes with the Same Accuracy as Complete Active Space Second-Order Perturbation Theory at a Significantly Reduced Computational Cost.

PubMed

Wilbraham, Liam; Verma, Pragya; Truhlar, Donald G; Gagliardi, Laura; Ciofini, Ilaria

2017-05-04

The spin-state orderings in nine Fe(II) and Fe(III) complexes with ligands of diverse ligand-field strength were investigated with multiconfiguration pair-density functional theory (MC-PDFT). The performance of this method was compared to that of complete active space second-order perturbation theory (CASPT2) and Kohn-Sham density functional theory. We also investigated the dependence of CASPT2 and MC-PDFT results on the size of the active-space. MC-PDFT reproduces the CASPT2 spin-state ordering, the dependence on the ligand field strength, and the dependence on active space at a computational cost that is significantly reduced as compared to CASPT2.

Relative binding affinity of carboxylate-, phosphonate-, and bisphosphonate-functionalized gold nanoparticles targeted to damaged bone tissue

NASA Astrophysics Data System (ADS)

Ross, Ryan D.; Cole, Lisa E.; Roeder, Ryan K.

2012-10-01

Functionalized Au NPs have received considerable recent interest for targeting and labeling cells and tissues. Damaged bone tissue can be targeted by functionalizing Au NPs with molecules exhibiting affinity for calcium. Therefore, the relative binding affinity of Au NPs surface functionalized with either carboxylate ( l-glutamic acid), phosphonate (2-aminoethylphosphonic acid), or bisphosphonate (alendronate) was investigated for targeted labeling of damaged bone tissue in vitro. Targeted labeling of damaged bone tissue was qualitatively verified by visual observation and backscattered electron microscopy, and quantitatively measured by the surface density of Au NPs using field-emission scanning electron microscopy. The surface density of functionalized Au NPs was significantly greater within damaged tissue compared to undamaged tissue for each functional group. Bisphosphonate-functionalized Au NPs exhibited a greater surface density labeling damaged tissue compared to glutamic acid- and phosphonic acid-functionalized Au NPs, which was consistent with the results of previous work comparing the binding affinity of the same functionalized Au NPs to synthetic hydroxyapatite crystals. Targeted labeling was enabled not only by the functional groups but also by the colloidal stability in solution. Functionalized Au NPs were stabilized by the presence of the functional groups, and were shown to remain well dispersed in ionic (phosphate buffered saline) and serum (fetal bovine serum) solutions for up to 1 week. Therefore, the results of this study suggest that bisphosphonate-functionalized Au NPs have potential for targeted delivery to damaged bone tissue in vitro and provide motivation for in vivo investigation.

Electronic structure and normal vibrations of the 1-ethyl-3-methylimidazolium ethyl sulfate ion pair.

PubMed

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

2011-04-21

Electronic and structural properties of the ion pair 1-ethyl-3-methylimidazolium ethyl sulfate are studied using density functional methods. Three locally stable conformers of the ion pair complex are considered to analyze molecular interactions between its cation and anion. Manifestations of these interactions in the vibrational spectra are discussed and compared with experimental IR and Raman spectroscopy data. NBO analysis and difference electron density coupled with molecular electron density topography are used to interpret the frequency shifts of the normal vibrations of the ion pair, compared to the free anion and cation. Excitation energies of low-lying singlet excited states of the conformers are also studied. The density functional theory results are found to be in a reasonable agreement with experimental UV/vis absorption spectra.

New approach to canonical partition functions computation in Nf=2 lattice QCD at finite baryon density

NASA Astrophysics Data System (ADS)

Bornyakov, V. G.; Boyda, D. L.; Goy, V. A.; Molochkov, A. V.; Nakamura, Atsushi; Nikolaev, A. A.; Zakharov, V. I.

2017-05-01

We propose and test a new approach to computation of canonical partition functions in lattice QCD at finite density. We suggest a few steps procedure. We first compute numerically the quark number density for imaginary chemical potential i μq I . Then we restore the grand canonical partition function for imaginary chemical potential using the fitting procedure for the quark number density. Finally we compute the canonical partition functions using high precision numerical Fourier transformation. Additionally we compute the canonical partition functions using the known method of the hopping parameter expansion and compare results obtained by two methods in the deconfining as well as in the confining phases. The agreement between two methods indicates the validity of the new method. Our numerical results are obtained in two flavor lattice QCD with clover improved Wilson fermions.

Two-component hybrid time-dependent density functional theory within the Tamm-Dancoff approximation.

PubMed

Kühn, Michael; Weigend, Florian

2015-01-21

We report the implementation of a two-component variant of time-dependent density functional theory (TDDFT) for hybrid functionals that accounts for spin-orbit effects within the Tamm-Dancoff approximation (TDA) for closed-shell systems. The influence of the admixture of Hartree-Fock exchange on excitation energies is investigated for several atoms and diatomic molecules by comparison to numbers for pure density functionals obtained previously [M. Kühn and F. Weigend, J. Chem. Theory Comput. 9, 5341 (2013)]. It is further related to changes upon switching to the local density approximation or using the full TDDFT formalism instead of TDA. Efficiency is demonstrated for a comparably large system, Ir(ppy)3 (61 atoms, 1501 basis functions, lowest 10 excited states), which is a prototype molecule for organic light-emitting diodes, due to its "spin-forbidden" triplet-singlet transition.

Ensemble density variational methods with self- and ghost-interaction-corrected functionals

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

Pastorczak, Ewa; Pernal, Katarzyna, E-mail: pernalk@gmail.com

2014-05-14

Ensemble density functional theory (DFT) offers a way of predicting excited-states energies of atomic and molecular systems without referring to a density response function. Despite a significant theoretical work, practical applications of the proposed approximations have been scarce and they do not allow for a fair judgement of the potential usefulness of ensemble DFT with available functionals. In the paper, we investigate two forms of ensemble density functionals formulated within ensemble DFT framework: the Gross, Oliveira, and Kohn (GOK) functional proposed by Gross et al. [Phys. Rev. A 37, 2809 (1988)] alongside the orbital-dependent eDFT form of the functional introducedmore » by Nagy [J. Phys. B 34, 2363 (2001)] (the acronym eDFT proposed in analogy to eHF – ensemble Hartree-Fock method). Local and semi-local ground-state density functionals are employed in both approaches. Approximate ensemble density functionals contain not only spurious self-interaction but also the so-called ghost-interaction which has no counterpart in the ground-state DFT. We propose how to correct the GOK functional for both kinds of interactions in approximations that go beyond the exact-exchange functional. Numerical applications lead to a conclusion that functionals free of the ghost-interaction by construction, i.e., eDFT, yield much more reliable results than approximate self- and ghost-interaction-corrected GOK functional. Additionally, local density functional corrected for self-interaction employed in the eDFT framework yields excitations energies of the accuracy comparable to that of the uncorrected semi-local eDFT functional.« less

A density functional theory study of the influence of exchange-correlation functionals on the properties of FeAs.

PubMed

Griffin, Sinéad M; Spaldin, Nicola A

2017-06-01

We use density functional theory within the local density approximation (LDA), LDA  +  U, generalised gradient approximation (GGA), GGA  +  U, and hybrid-functional methods to calculate the properties of iron monoarsenide. FeAs, which forms in the MnP structure, is of current interest for potential spintronic applications as well as being the parent compound for the pnictide superconductors. We compare the calculated structural, magnetic and electronic properties obtained using the different functionals to each other and to experiment, and investigate the origin of a recently reported magnetic spiral. Our results indicate the appropriateness or otherwise of the various functionals for describing FeAs and the related Fe-pnictide superconductors.

The large-scale gravitational bias from the quasi-linear regime.

NASA Astrophysics Data System (ADS)

Bernardeau, F.

1996-08-01

It is known that in gravitational instability scenarios the nonlinear dynamics induces non-Gaussian features in cosmological density fields that can be investigated with perturbation theory. Here, I derive the expression of the joint moments of cosmological density fields taken at two different locations. The results are valid when the density fields are filtered with a top-hat filter window function, and when the distance between the two cells is large compared to the smoothing length. In particular I show that it is possible to get the generating function of the coefficients C_p,q_ defined by <δ^p^({vec}(x)_1_)δ^q^({vec}(x)_2_)>_c_=C_p,q_ <δ^2^({vec}(x))>^p+q-2^ <δ({vec}(x)_1_)δ({vec}(x)_2_)> where δ({vec}(x)) is the local smoothed density field. It is then possible to reconstruct the joint density probability distribution function (PDF), generalizing for two points what has been obtained previously for the one-point density PDF. I discuss the validity of the large separation approximation in an explicit numerical Monte Carlo integration of the C_2,1_ parameter as a function of |{vec}(x)_1_-{vec}(x)_2_|. A straightforward application is the calculation of the large-scale ``bias'' properties of the over-dense (or under-dense) regions. The properties and the shape of the bias function are presented in details and successfully compared with numerical results obtained in an N-body simulation with CDM initial conditions.

The large-scale correlations of multicell densities and profiles: implications for cosmic variance estimates

NASA Astrophysics Data System (ADS)

Codis, Sandrine; Bernardeau, Francis; Pichon, Christophe

2016-08-01

In order to quantify the error budget in the measured probability distribution functions of cell densities, the two-point statistics of cosmic densities in concentric spheres is investigated. Bias functions are introduced as the ratio of their two-point correlation function to the two-point correlation of the underlying dark matter distribution. They describe how cell densities are spatially correlated. They are computed here via the so-called large deviation principle in the quasi-linear regime. Their large-separation limit is presented and successfully compared to simulations for density and density slopes: this regime is shown to be rapidly reached allowing to get sub-percent precision for a wide range of densities and variances. The corresponding asymptotic limit provides an estimate of the cosmic variance of standard concentric cell statistics applied to finite surveys. More generally, no assumption on the separation is required for some specific moments of the two-point statistics, for instance when predicting the generating function of cumulants containing any powers of concentric densities in one location and one power of density at some arbitrary distance from the rest. This exact `one external leg' cumulant generating function is used in particular to probe the rate of convergence of the large-separation approximation.

Fractional Wigner Crystal in the Helical Luttinger Liquid.

PubMed

Traverso Ziani, N; Crépin, F; Trauzettel, B

2015-11-13

The properties of the strongly interacting edge states of two dimensional topological insulators in the presence of two-particle backscattering are investigated. We find an anomalous behavior of the density-density correlation functions, which show oscillations that are neither of Friedel nor of Wigner type: they, instead, represent a Wigner crystal of fermions of fractional charge e/2, with e the electron charge. By studying the Fermi operator, we demonstrate that the state characterized by such fractional oscillations still bears the signatures of spin-momentum locking. Finally, we compare the spin-spin correlation functions and the density-density correlation functions to argue that the fractional Wigner crystal is characterized by a nontrivial spin texture.

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

A physical model study of scattering of waves by aligned cracks: Comparison between experiment and theory

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

Ass'ad, J.M.; McDonald, J.A.; Kusky, T.M.

1993-04-01

An approximation to plane-wave propagation through a composite material is examined using a physical model with oriented but randomly distributed penny-shaped rubber inclusions within an isotropic epoxy resin matrix. A pulse transmission method is used to determine velocities of shear and compressional waves as a function of angle of incidence and crack density. The experimental and theoretical results of Hudson were compared and limitations within the crack parameters used in this study have been determined. Results from both polarized shear waves (S1, S2) compare favorably with the theory for a composite with up to 7% crack density, but theory andmore » experiment diverge at higher crack densities. On the other hand, compressional-wave velocities at low crack densities (1% and 3%) compare favorably with the theory. It is also shown that the velocity ratio V[sub p]/V[sub s] for two extreme cases, i.e. propagation normal and parallel to the cracks, as a function of crack density and porosity, has a strong directional dependence.« less

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.

Density functional theory study of the concerted pyrolysis mechanism for lignin models

Treesearch

Thomas Elder; Ariana Beste

2014-01-01

ABSTRACT: Studies on the pyrolysis mechanisms of lignin model compounds have largely focused on initial homolytic cleavage reactions. It has been noted, however, that concerted mechanisms may also account for observed product formation. In the current work, the latter processes are examined and compared to the former, by the application of density functional theory...

Nucleon localization and fragment formation in nuclear fission

DOE PAGES

Zhang, C. L.; Schuetrumpf, B.; Nazarewicz, W.

2016-12-27

An electron localization measure was originally introduced to characterize chemical bond structures in molecules. Recently, a nucleon localization based on Hartree-Fock densities has been introduced to investigate α-cluster structures in light nuclei. Compared to the local nucleonic densities, the nucleon localization function has been shown to be an excellent indicator of shell effects and cluster correlations. In this work, using the spatial nucleon localization measure, we investigated the emergence of fragments in fissioning heavy nuclei using the self-consistent energy density functional method with a quantified energy density functional optimized for fission studies. We studied the particle densities and spatial nucleonmore » localization distributions along the fission pathways of 264Fm, 232Th, and 240Pu. We demonstrated that the fission fragments were formed fairly early in the evolution, well before scission. To illustrate the usefulness of the localization measure, we showed how the hyperdeformed state of 232Th could be understood in terms of a quasimolecular state made of 132Sn and 100Zr fragments. Compared to nucleonic distributions, the nucleon localization function more effectively quantifies nucleonic clustering: its characteristic oscillating pattern, traced back to shell effects, is a clear fingerprint of cluster/fragment configurations. This is of particular interest for studies of fragment formation and fragment identification in fissioning nuclei.« less

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

Zhang, C. L.; Schuetrumpf, B.; Nazarewicz, W.

An electron localization measure was originally introduced to characterize chemical bond structures in molecules. Recently, a nucleon localization based on Hartree-Fock densities has been introduced to investigate α-cluster structures in light nuclei. Compared to the local nucleonic densities, the nucleon localization function has been shown to be an excellent indicator of shell effects and cluster correlations. In this work, using the spatial nucleon localization measure, we investigated the emergence of fragments in fissioning heavy nuclei using the self-consistent energy density functional method with a quantified energy density functional optimized for fission studies. We studied the particle densities and spatial nucleonmore » localization distributions along the fission pathways of 264Fm, 232Th, and 240Pu. We demonstrated that the fission fragments were formed fairly early in the evolution, well before scission. To illustrate the usefulness of the localization measure, we showed how the hyperdeformed state of 232Th could be understood in terms of a quasimolecular state made of 132Sn and 100Zr fragments. Compared to nucleonic distributions, the nucleon localization function more effectively quantifies nucleonic clustering: its characteristic oscillating pattern, traced back to shell effects, is a clear fingerprint of cluster/fragment configurations. This is of particular interest for studies of fragment formation and fragment identification in fissioning nuclei.« less

Density functional theory for polymeric systems in 2D.

PubMed

Słyk, Edyta; Roth, Roland; Bryk, Paweł

2016-06-22

We propose density functional theory for polymeric fluids in two dimensions. The approach is based on Wertheim's first order thermodynamic perturbation theory (TPT) and closely follows density functional theory for polymers proposed by Yu and Wu (2002 J. Chem. Phys. 117 2368). As a simple application we evaluate the density profiles of tangent hard-disk polymers at hard walls. The theoretical predictions are compared against the results of the Monte Carlo simulations. We find that for short chain lengths the theoretical density profiles are in an excellent agreement with the Monte Carlo data. The agreement is less satisfactory for longer chains. The performance of the theory can be improved by recasting the approach using the self-consistent field theory formalism. When the self-avoiding chain statistics is used, the theory yields a marked improvement in the low density limit. Further improvements for long chains could be reached by going beyond the first order of TPT.

Use of the rVV10 Nonlocal Correlation Functional in the B97M-V Density Functional: Defining B97M-rV and Related Functionals [On the Use of the rVV10 Nonlocal Correlation Functional in the B97M-V Density Functional: Defining B97M-rV and Related Functionals

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

Mardirossian, Narbe; Ruiz Pestana, Luis; Womack, James C.

The VV10 and rVV10 nonlocal correlation functionals are consistently implemented and assessed, with the goal of determining if the rVV10 nonlocal correlation functional can replace the VV10 nonlocal correlation functional in the recently developed B97M-V density functional, to give the B97M-rV density functional. Along the way, four density functionals are simultaneously tested: VV10, rVV10, B97M-V, and B97M-rV. An initial assessment is carried out across the S22 data set, and the short-range damping variable, b, is varied for all four density functionals in order to determine the sensitivity of the functionals to the empirical parameter. The results of this test indicatemore » that a value of b = 6 (fortuitously the same as that in B97M-V) is suitable for B97M-rV. The functionals are then compared across an extensive database of interaction energies, and it is demonstrated that B97M-rV either matches or outperforms B97M-V for all of the tests considered. Finally, the optimization of b across the S22 data set is extended to two range-separated hybrid density functionals, ωB97X-V and ωB97M-V, and a value of b = 6.2 is recommended for both ωB97X-rV and ωB97M-rV.« less

Use of the rVV10 Nonlocal Correlation Functional in the B97M-V Density Functional: Defining B97M-rV and Related Functionals [On the Use of the rVV10 Nonlocal Correlation Functional in the B97M-V Density Functional: Defining B97M-rV and Related Functionals

DOE PAGES

Mardirossian, Narbe; Ruiz Pestana, Luis; Womack, James C.; ...

2016-12-06

The VV10 and rVV10 nonlocal correlation functionals are consistently implemented and assessed, with the goal of determining if the rVV10 nonlocal correlation functional can replace the VV10 nonlocal correlation functional in the recently developed B97M-V density functional, to give the B97M-rV density functional. Along the way, four density functionals are simultaneously tested: VV10, rVV10, B97M-V, and B97M-rV. An initial assessment is carried out across the S22 data set, and the short-range damping variable, b, is varied for all four density functionals in order to determine the sensitivity of the functionals to the empirical parameter. The results of this test indicatemore » that a value of b = 6 (fortuitously the same as that in B97M-V) is suitable for B97M-rV. The functionals are then compared across an extensive database of interaction energies, and it is demonstrated that B97M-rV either matches or outperforms B97M-V for all of the tests considered. Finally, the optimization of b across the S22 data set is extended to two range-separated hybrid density functionals, ωB97X-V and ωB97M-V, and a value of b = 6.2 is recommended for both ωB97X-rV and ωB97M-rV.« less

Microscopically based energy density functionals for nuclei using the density matrix expansion: Implementation and pre-optimization

NASA Astrophysics Data System (ADS)

Stoitsov, M.; Kortelainen, M.; Bogner, S. K.; Duguet, T.; Furnstahl, R. J.; Gebremariam, B.; Schunck, N.

2010-11-01

In a recent series of articles, Gebremariam, Bogner, and Duguet derived a microscopically based nuclear energy density functional by applying the density matrix expansion (DME) to the Hartree-Fock energy obtained from chiral effective field theory two- and three-nucleon interactions. Owing to the structure of the chiral interactions, each coupling in the DME functional is given as the sum of a coupling constant arising from zero-range contact interactions and a coupling function of the density arising from the finite-range pion exchanges. Because the contact contributions have essentially the same structure as those entering empirical Skyrme functionals, a microscopically guided Skyrme phenomenology has been suggested in which the contact terms in the DME functional are released for optimization to finite-density observables to capture short-range correlation energy contributions from beyond Hartree-Fock. The present article is the first attempt to assess the ability of the newly suggested DME functional, which has a much richer set of density dependencies than traditional Skyrme functionals, to generate sensible and stable results for nuclear applications. The results of the first proof-of-principle calculations are given, and numerous practical issues related to the implementation of the new functional in existing Skyrme codes are discussed. Using a restricted singular value decomposition optimization procedure, it is found that the new DME functional gives numerically stable results and exhibits a small but systematic reduction of our test χ2 function compared to standard Skyrme functionals, thus justifying its suitability for future global optimizations and large-scale calculations.

Development and application of a 2-electron reduced density matrix approach to electron transport via molecular junctions

NASA Astrophysics Data System (ADS)

Hoy, Erik P.; Mazziotti, David A.; Seideman, Tamar

2017-11-01

Can an electronic device be constructed using only a single molecule? Since this question was first asked by Aviram and Ratner in the 1970s [Chem. Phys. Lett. 29, 277 (1974)], the field of molecular electronics has exploded with significant experimental advancements in the understanding of the charge transport properties of single molecule devices. Efforts to explain the results of these experiments and identify promising new candidate molecules for molecular devices have led to the development of numerous new theoretical methods including the current standard theoretical approach for studying single molecule charge transport, i.e., the non-equilibrium Green's function formalism (NEGF). By pairing this formalism with density functional theory (DFT), a wide variety of transport problems in molecular junctions have been successfully treated. For some systems though, the conductance and current-voltage curves predicted by common DFT functionals can be several orders of magnitude above experimental results. In addition, since density functional theory relies on approximations to the exact exchange-correlation functional, the predicted transport properties can show significant variation depending on the functional chosen. As a first step to addressing this issue, the authors have replaced density functional theory in the NEGF formalism with a 2-electron reduced density matrix (2-RDM) method, creating a new approach known as the NEGF-RDM method. 2-RDM methods provide a more accurate description of electron correlation compared to density functional theory, and they have lower computational scaling compared to wavefunction based methods of similar accuracy. Additionally, 2-RDM methods are capable of capturing static electron correlation which is untreatable by existing NEGF-DFT methods. When studying dithiol alkane chains and dithiol benzene in model junctions, the authors found that the NEGF-RDM predicts conductances and currents that are 1-2 orders of magnitude below those of B3LYP and M06 DFT functionals. This suggests that the NEGF-RDM method could be a viable alternative to NEGF-DFT for molecular junction calculations.

Density-Decomposed Orbital-Free Density Functional Theory for Covalent Systems and Application to Li-Si alloys

NASA Astrophysics Data System (ADS)

Xia, Junchao; Carter, Emily

2014-03-01

We propose a density decomposition scheme using a Wang-Govind-Carter (WGC)-based kinetic energy density functional (KEDF) to accurately and efficiently simulate covalent systems within orbital-free (OF) density functional theory (DFT). By using a local, density-dependent scale function, the total density is decomposed into a localized density within covalent bond regions and a flattened delocalized density, with the former described by semilocal KEDFs and the latter treated by the WGC KEDF. The new model predicts reasonable equilibrium volumes, bulk moduli, and phase ordering energies for various semiconductors compared to Kohn-Sham (KS) DFT benchmarks. The surface energy of Si(100) also agrees well with KSDFT. We further apply the model to study mechanical properties of Li-Si alloys, which have been recently recognized as a promising candidate for next-generation anodes of Li-ion batteries with outstanding capacity. We study multiple crystalline Li-Si alloys. The WGCD KEDF predicts accurate cell lattice vectors, equilibrium volumes, elastic moduli, electron densities, alloy formation and Li adsorption energies. Because of its quasilinear scaling, coupled with the level of accuracy shown here, OFDFT appears quite promising for large-scale simulation of such materials phenomena. Office of Naval Research, National Science Foundation, Tigress High Performance Computing Center.

A classical density-functional theory for describing water interfaces.

PubMed

Hughes, Jessica; Krebs, Eric J; Roundy, David

2013-01-14

We develop a classical density functional for water which combines the White Bear fundamental-measure theory (FMT) functional for the hard sphere fluid with attractive interactions based on the statistical associating fluid theory variable range (SAFT-VR). This functional reproduces the properties of water at both long and short length scales over a wide range of temperatures and is computationally efficient, comparable to the cost of FMT itself. We demonstrate our functional by applying it to systems composed of two hard rods, four hard rods arranged in a square, and hard spheres in water.

Charge transport calculations by a wave-packet dynamical approach using maximally localized Wannier functions based on density functional theory: Application to high-mobility organic semiconductors

NASA Astrophysics Data System (ADS)

Ishii, Hiroyuki; Kobayashi, Nobuhiko; Hirose, Kenji

2017-01-01

We present a wave-packet dynamical approach to charge transport using maximally localized Wannier functions based on density functional theory including van der Waals interactions. We apply it to the transport properties of pentacene and rubrene single crystals and show the temperature-dependent natures from bandlike to thermally activated behaviors as a function of the magnitude of external static disorder. We compare the results with those obtained by the conventional band and hopping models and experiments.

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

Antolin, J.; Instituto Carlos I de Fisica Teorica y Computacional, Universidad de Granada, ES-18071 Granada; Bouvrie, P. A.

An alternative one-parameter measure of divergence is proposed, quantifying the discrepancy among general probability densities. Its main mathematical properties include (i) comparison among an arbitrary number of functions, (ii) the possibility of assigning different weights to each function according to its relevance on the comparative procedure, and (iii) ability to modify the relative contribution of different regions within the domain. Applications to the study of atomic density functions, in both conjugated spaces, show the versatility and universality of this divergence.

A well-scaling natural orbital theory

DOE PAGES

Gebauer, Ralph; Cohen, Morrel H.; Car, Roberto

2016-11-01

Here, we introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled approximations to the two-particle density matrix that yield algebraic scaling in general, and Hartree–Fock scaling in its seniority-zero version. Results from the latter version for small molecular systems are compared with those of highly accurate quantum-chemical computations. The energies lie above full configuration interaction calculations, close to doubly occupied configuration interaction calculations. Their accuracy is considerably greater than that obtained from current density-functional theory approximations and from current functionals ofmore » the oneparticle density matrix.« less

A well-scaling natural orbital theory

PubMed Central

Gebauer, Ralph; Cohen, Morrel H.; Car, Roberto

2016-01-01

We introduce an energy functional for ground-state electronic structure calculations. Its variables are the natural spin-orbitals of singlet many-body wave functions and their joint occupation probabilities deriving from controlled approximations to the two-particle density matrix that yield algebraic scaling in general, and Hartree–Fock scaling in its seniority-zero version. Results from the latter version for small molecular systems are compared with those of highly accurate quantum-chemical computations. The energies lie above full configuration interaction calculations, close to doubly occupied configuration interaction calculations. Their accuracy is considerably greater than that obtained from current density-functional theory approximations and from current functionals of the one-particle density matrix. PMID:27803328

Course 4: Density Functional Theory, Methods, Techniques, and Applications

NASA Astrophysics Data System (ADS)

Chrétien, S.; Salahub, D. R.

Contents 1 Introduction 2 Density functional theory 2.1 Hohenberg and Kohn theorems 2.2 Levy's constrained search 2.3 Kohn-Sham method 3 Density matrices and pair correlation functions 4 Adiabatic connection or coupling strength integration 5 Comparing and constrasting KS-DFT and HF-CI 6 Preparing new functionals 7 Approximate exchange and correlation functionals 7.1 The Local Spin Density Approximation (LSDA) 7.2 Gradient Expansion Approximation (GEA) 7.3 Generalized Gradient Approximation (GGA) 7.4 meta-Generalized Gradient Approximation (meta-GGA) 7.5 Hybrid functionals 7.6 The Optimized Effective Potential method (OEP) 7.7 Comparison between various approximate functionals 8 LAP correlation functional 9 Solving the Kohn-Sham equations 9.1 The Kohn-Sham orbitals 9.2 Coulomb potential 9.3 Exchange-correlation potential 9.4 Core potential 9.5 Other choices and sources of error 9.6 Functionality 10 Applications 10.1 Ab initio molecular dynamics for an alanine dipeptide model 10.2 Transition metal clusters: The ecstasy, and the agony... 10.3 The conversion of acetylene to benzene on Fe clusters 11 Conclusions

Dynamic Density: An Air Traffic Management Metric

NASA Technical Reports Server (NTRS)

Laudeman, I. V.; Shelden, S. G.; Branstrom, R.; Brasil, C. L.

1998-01-01

The definition of a metric of air traffic controller workload based on air traffic characteristics is essential to the development of both air traffic management automation and air traffic procedures. Dynamic density is a proposed concept for a metric that includes both traffic density (a count of aircraft in a volume of airspace) and traffic complexity (a measure of the complexity of the air traffic in a volume of airspace). It was hypothesized that a metric that includes terms that capture air traffic complexity will be a better measure of air traffic controller workload than current measures based only on traffic density. A weighted linear dynamic density function was developed and validated operationally. The proposed dynamic density function includes a traffic density term and eight traffic complexity terms. A unit-weighted dynamic density function was able to account for an average of 22% of the variance in observed controller activity not accounted for by traffic density alone. A comparative analysis of unit weights, subjective weights, and regression weights for the terms in the dynamic density equation was conducted. The best predictor of controller activity was the dynamic density equation with regression-weighted complexity terms.

Molecular simulation of disjoining-pressure isotherms for free liquid , Lennard-Jones thin films

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

Bhatt, Divesh; Newman, John; Radke, C.J.

2001-10-01

We present canonical-ensemble molecular-dynamics simulations of disjoining-pressure isotherms in Lennard-Jones free liquid films. Thermodynamics demands that the disjoining pressure is determined uniquely as a function of the chemical potential purely from the phase diagram of the fluid. Our results from molecular dynamics validate this argument. The inverse-sixth-power distance term in the Lennard-Jones intermolecular potential represents van der Waals dispersion forces. Hence, we compare our results with classical Hamaker theory that is based on dispersion forces but assumes a slab geometry for the density profile and completely neglects fluid structure and entropy. We find that the Hamaker constant obtained from ourmore » simulations is about an order of magnitude larger than that from classical theory. To investigate the origin of this discrepancy, we calculate the disjoining-pressure isotherm using a density-functional theory relaxing the inherent assumptions in the Hamaker theory and imparting to the fluid an approximate structure. For disjoining pressure as a function of chemical potential, the results of density-functional theory and molecular dynamics are very close. Even for disjoining-pressure isotherms, and the subsequently calculated Hamaker constant, results of the density-functional theory are closer to the molecular-dynamics simulations by about a factor of 4 compared to Hamaker theory. [References: 44]« less

Density-functional theory based on the electron distribution on the energy coordinate

NASA Astrophysics Data System (ADS)

Takahashi, Hideaki

2018-03-01

We developed an electronic density functional theory utilizing a novel electron distribution n(ɛ) as a basic variable to compute ground state energy of a system. n(ɛ) is obtained by projecting the electron density n({\\boldsymbol{r}}) defined on the space coordinate {\\boldsymbol{r}} onto the energy coordinate ɛ specified with the external potential {\\upsilon }ext}({\\boldsymbol{r}}) of interest. It was demonstrated that the Kohn-Sham equation can also be formulated with the exchange-correlation functional E xc[n(ɛ)] that employs the density n(ɛ) as an argument. It turned out an exchange functional proposed in our preliminary development suffices to describe properly the potential energies of several types of chemical bonds with comparable accuracies to the corresponding functional based on local density approximation. As a remarkable feature of the distribution n(ɛ) it inherently involves the spatially non-local information of the exchange hole at the bond dissociation limit in contrast to conventional approximate functionals. By taking advantage of this property we also developed a prototype of the static correlation functional E sc including no empirical parameters, which showed marked improvements in describing the dissociations of covalent bonds in {{{H}}}2,{{{C}}}2{{{H}}}4 and {CH}}4 molecules.

Basis convergence of range-separated density-functional theory

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

Franck, Odile, E-mail: odile.franck@etu.upmc.fr; Mussard, Bastien, E-mail: bastien.mussard@upmc.fr; CNRS, UMR 7616, Laboratoire de Chimie Théorique, F-75005 Paris

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. Wemore » 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, N{sub 2}, and H{sub 2}O) 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.« less

A conceptual DFT study of the molecular properties of glycating carbonyl compounds.

PubMed

Frau, Juan; Glossman-Mitnik, Daniel

2017-01-01

Several glycating carbonyl compounds have been studied by resorting to the latest Minnesota family of density functional with the objective of determinating their molecular properties. In particular, the chemical reactivity descriptors that arise from conceptual density functional theory and chemical reactivity theory have been calculated through a [Formula: see text]SCF protocol. The validity of the KID (Koopmans' in DFT) procedure has been checked by comparing the reactivity descriptors obtained from the values of the HOMO and LUMO with those calculated through vertical energy values. The reactivity sites have been determined by means of the calculation of the Fukui function indices, the condensed dual descriptor [Formula: see text] and the electrophilic and nucleophilic Parr functions. The glycating power of the studied compounds have been compared with the same property for simple carbohydrates.Graphical abstractSeveral glycating carbonyl compounds have been studied by resorting to the latest Minnesota family of density functional with the objective of determinating their molecular properties, the chemical reactivity descriptors and the validity of the KID (Koopmans' in DFT) procedure.

Continuous time random walk model with asymptotical probability density of waiting times via inverse Mittag-Leffler function

NASA Astrophysics Data System (ADS)

Liang, Yingjie; Chen, Wen

2018-04-01

The mean squared displacement (MSD) of the traditional ultraslow diffusion is a logarithmic function of time. Recently, the continuous time random walk model is employed to characterize this ultraslow diffusion dynamics by connecting the heavy-tailed logarithmic function and its variation as the asymptotical waiting time density. In this study we investigate the limiting waiting time density of a general ultraslow diffusion model via the inverse Mittag-Leffler function, whose special case includes the traditional logarithmic ultraslow diffusion model. The MSD of the general ultraslow diffusion model is analytically derived as an inverse Mittag-Leffler function, and is observed to increase even more slowly than that of the logarithmic function model. The occurrence of very long waiting time in the case of the inverse Mittag-Leffler function has the largest probability compared with the power law model and the logarithmic function model. The Monte Carlo simulations of one dimensional sample path of a single particle are also performed. The results show that the inverse Mittag-Leffler waiting time density is effective in depicting the general ultraslow random motion.

The harmonic frequencies of benzene

NASA Astrophysics Data System (ADS)

Handy, Nicholas C.; Maslen, Paul E.; Amos, Roger D.; Andrews, Jamie S.; Murray, Christopher W.; Laming, Gregory J.

1992-09-01

We report calculations for the harmonic frequencies of C 6H 6 and C 6D 6. Our most sophisticated quantum chemistry values are obtained with the MP2 method and a TZ2P+f basis set (288 basis functions), which are the largest such calculations reported on benzene to date. Using the SCF density, we also calculate the frequencies using the exchange and correlation expressions of density functional theory. We compare our calculated harmonic frequencies with those deduced from experiment by Goodman, Ozkabak and Thakur. The density functional frequencies appear to be more reliable predictions than the MP2 frequencies and they are obtained at significantly less cost.

Nonlocal kinetic energy functionals by functional integration.

PubMed

Mi, Wenhui; Genova, Alessandro; Pavanello, Michele

2018-05-14

Since the seminal studies of Thomas and Fermi, researchers in the Density-Functional Theory (DFT) community are searching for accurate electron density functionals. Arguably, the toughest functional to approximate is the noninteracting kinetic energy, T s [ρ], the subject of this work. The typical paradigm is to first approximate the energy functional and then take its functional derivative, δT s [ρ]δρ(r), yielding a potential that can be used in orbital-free DFT or subsystem DFT simulations. Here, this paradigm is challenged by constructing the potential from the second-functional derivative via functional integration. A new nonlocal functional for T s [ρ] is prescribed [which we dub Mi-Genova-Pavanello (MGP)] having a density independent kernel. MGP is constructed to satisfy three exact conditions: (1) a nonzero "Kinetic electron" arising from a nonzero exchange hole; (2) the second functional derivative must reduce to the inverse Lindhard function in the limit of homogenous densities; (3) the potential is derived from functional integration of the second functional derivative. Pilot calculations show that MGP is capable of reproducing accurate equilibrium volumes, bulk moduli, total energy, and electron densities for metallic (body-centered cubic, face-centered cubic) and semiconducting (crystal diamond) phases of silicon as well as of III-V semiconductors. The MGP functional is found to be numerically stable typically reaching self-consistency within 12 iterations of a truncated Newton minimization algorithm. MGP's computational cost and memory requirements are low and comparable to the Wang-Teter nonlocal functional or any generalized gradient approximation functional.

Nonlocal kinetic energy functionals by functional integration

NASA Astrophysics Data System (ADS)

Mi, Wenhui; Genova, Alessandro; Pavanello, Michele

2018-05-01

Since the seminal studies of Thomas and Fermi, researchers in the Density-Functional Theory (DFT) community are searching for accurate electron density functionals. Arguably, the toughest functional to approximate is the noninteracting kinetic energy, Ts[ρ], the subject of this work. The typical paradigm is to first approximate the energy functional and then take its functional derivative, δ/Ts[ρ ] δ ρ (r ) , yielding a potential that can be used in orbital-free DFT or subsystem DFT simulations. Here, this paradigm is challenged by constructing the potential from the second-functional derivative via functional integration. A new nonlocal functional for Ts[ρ] is prescribed [which we dub Mi-Genova-Pavanello (MGP)] having a density independent kernel. MGP is constructed to satisfy three exact conditions: (1) a nonzero "Kinetic electron" arising from a nonzero exchange hole; (2) the second functional derivative must reduce to the inverse Lindhard function in the limit of homogenous densities; (3) the potential is derived from functional integration of the second functional derivative. Pilot calculations show that MGP is capable of reproducing accurate equilibrium volumes, bulk moduli, total energy, and electron densities for metallic (body-centered cubic, face-centered cubic) and semiconducting (crystal diamond) phases of silicon as well as of III-V semiconductors. The MGP functional is found to be numerically stable typically reaching self-consistency within 12 iterations of a truncated Newton minimization algorithm. MGP's computational cost and memory requirements are low and comparable to the Wang-Teter nonlocal functional or any generalized gradient approximation functional.

Estimation of option-implied risk-neutral into real-world density by using calibration function

NASA Astrophysics Data System (ADS)

Bahaludin, Hafizah; Abdullah, Mimi Hafizah

2017-04-01

Option prices contain crucial information that can be used as a reflection of future development of an underlying assets' price. The main objective of this study is to extract the risk-neutral density (RND) and the risk-world density (RWD) of option prices. A volatility function technique is applied by using a fourth order polynomial interpolation to obtain the RNDs. Then, a calibration function is used to convert the RNDs into RWDs. There are two types of calibration function which are parametric and non-parametric calibrations. The density is extracted from the Dow Jones Industrial Average (DJIA) index options with a one month constant maturity from January 2009 until December 2015. The performance of RNDs and RWDs extracted are evaluated by using a density forecasting test. This study found out that the RWDs obtain can provide an accurate information regarding the price of the underlying asset in future compared to that of the RNDs. In addition, empirical evidence suggests that RWDs from a non-parametric calibration has a better accuracy than other densities.

Comparative atmosphere structure experiment

NASA Technical Reports Server (NTRS)

Sommer, S.

1974-01-01

Atmospheric structure of outer planets as determined by pressure, temperature, and accelerometers is reviewed and results obtained from the PAET earth entry are given. In order to describe atmospheric structure, entry is divided into two regimes, high and low speed. Acceleration is then measured: from these measurements density is determined as a function of time. The equations of motion are integrated to determine velocity, flight path angle, and altitude as a function of time. Density is then determined as a function of altitude from the previous determinations of density and altitude as a function of time. Hydrostatic equilibrium was assumed to determine pressure as a function of altitude. Finally the equation of space applied to determine temperature as a function of altitude, if the mean molecular weight is known. The mean molecular weight is obtained independently from either the low speed experiment or from the composition experiments.

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.

Density functional theory study of structural, electronic, and thermal properties of Pt, Pd, Rh, Ir, Os and PtPd X (X = Ir, Os, and Rh) alloys

NASA Astrophysics Data System (ADS)

Shabbir, Ahmed; Muhammad, Zafar; M, Shakil; M, A. Choudhary

2016-03-01

The structural, electronic, mechanical, and thermal properties of Pt, Pd, Rh, Ir, Os metals and their alloys PtPdX (X = Ir, Os and Rh) are studied systematically using ab initio density functional theory. The groundstate properties such as lattice constant and bulk modulus are calculated to find the equilibrium atomic position for stable alloys. The electronic band structure and density of states are calculated to study the electronic behavior of metals on making their alloys. The electronic properties substantiate the metallic behavior for all studied materials. The firstprinciples density functional perturbation theory as implemented in quasi-harmonic approximation is used for the calculations of thermal properties. We have calculated the thermal properties such as the Debye temperature, vibrational energy, entropy and constant-volume specific heat. The calculated properties are compared with the previously reported experimental and theoretical data for metals and are found to be in good agreement. Calculated results for alloys could not be compared because there is no data available in the literature with such alloy composition.

Electronic structure of LiCoO2 thin films: A combined photoemission spectroscopy and density functional theory study

NASA Astrophysics Data System (ADS)

Ensling, David; Thissen, Andreas; Laubach, Stefan; Schmidt, Peter C.; Jaegermann, Wolfram

2010-11-01

The electronic properties of LiCoO2 have been studied by theoretical band-structure calculations (using density functional theory) and experimental methods (photoemission). Synchrotron-induced photoelectron spectroscopy, resonant photoemission spectroscopy (ResPES), and soft x-ray absorption (XAS) have been applied to investigate the electronic structure of both occupied and unoccupied states. High-quality PES spectra were obtained from stoichiometric and highly crystalline LiCoO2 thin films deposited “in situ” by rf magnetron sputtering. An experimental approach of separating oxygen- and cobalt-derived (final) states by ResPES in the valence-band region is presented. The procedure takes advantage of an antiresonant behavior of cobalt-derived states at the 3p-3d excitation threshold. Information about the unoccupied density of states has been obtained by OK XAS. The structure of the CoL absorption edge is compared to semiempirical charge-transfer multiplet calculations. The experimental results are furthermore compared with band-structure calculations considering three different exchange potentials [generalized gradient approximation (GGA), using a nonlocal Hubbard U (GGA+U) and using a hybrid functional (Becke, three-parameter, Lee-Yang-Parr [B3LYP])]. For these different approaches total density of states and partial valence-band density of states have been investigated. The best qualitative agreement with experimental results has been obtained by using a GGA+U functional with U=2.9eV .

CPB-K mice a mouse model of schizophrenia? Differences in dopaminergic, serotonergic and behavioral markers compared to BALB/cJ mice.

PubMed

Panther, P; Nullmeier, S; Dobrowolny, H; Schwegler, H; Wolf, R

2012-04-21

Schizophrenia is characterized by disturbances in social behavior, sensorimotor gating and cognitive function, that are discussed to be caused by a termination of different transmitter systems. Beside morphological alterations in cortical and subcortical areas reduced AMPA- NMDA-, 5-HT2-receptor densities and increased 5-HT1-receptor densities are found in the hippocampus.The two inbred mouse strains CPB-K and BALB/cJ are known to display considerable differences in cognitive function and prepulse inhibition, a stable marker of sensorimotor gating. Furthermore, CPB-K mice exhibit lower NMDA-, AMPA- and increased 5-HT-receptor densities in the hippocampus as compared to BALB/cJ mice. We investigated both mouse strains in social interaction test for differences in social behavior and with immuncytochemical approaches for alterations of dopaminergic and serotonergic parameters. Our results can be summarized as follows: compared to BALB/cJ, CPB-K mice showed:(1) significantly reduced traveling distance and number of contacts in social interaction test, (2) differences in the number of serotonin transporter-immunoreactive neurons and volume of raphe nuclei and a lower serotonergic fiber density in the ventral and dorsal hippocampal subfields CA1 and CA3, (3) no alterations of dopaminergic markers like neuron number, neuron density and volume in subregions of substantia nigra and ventral tegmental area, but a significantly higher dopaminergic fiber density in the dorsal hippocampus, the ventral hippocampus of CA1 and gyrus dentatus, (4) no significant differences in serotonergic and dopaminergic fiber densities in the amygdala.Based on our results and previous studies, CPB-K mice compared to BALB/cJ may serve as an important model to understand the interaction of the serotonergic and dopaminergic system and their impact on sensorimotor gating and cognitive function as related to neuropsychiatric disorders like schizophrenia. 2012 Elsevier B.V. All rights reserved.

Semi-local machine-learned kinetic energy density functional with third-order gradients of electron density

NASA Astrophysics Data System (ADS)

Seino, Junji; Kageyama, Ryo; Fujinami, Mikito; Ikabata, Yasuhiro; Nakai, Hiromi

2018-06-01

A semi-local kinetic energy density functional (KEDF) was constructed based on machine learning (ML). The present scheme adopts electron densities and their gradients up to third-order as the explanatory variables for ML and the Kohn-Sham (KS) kinetic energy density as the response variable in atoms and molecules. Numerical assessments of the present scheme were performed in atomic and molecular systems, including first- and second-period elements. The results of 37 conventional KEDFs with explicit formulae were also compared with those of the ML KEDF with an implicit formula. The inclusion of the higher order gradients reduces the deviation of the total kinetic energies from the KS calculations in a stepwise manner. Furthermore, our scheme with the third-order gradient resulted in the closest kinetic energies to the KS calculations out of the presented functionals.

Communication: Density functional theory model for multi-reference systems based on the exact-exchange hole normalization

NASA Astrophysics Data System (ADS)

Laqua, Henryk; Kussmann, Jörg; Ochsenfeld, Christian

2018-03-01

The correct description of multi-reference electronic ground states within Kohn-Sham density functional theory (DFT) requires an ensemble-state representation, employing fractionally occupied orbitals. However, the use of fractional orbital occupation leads to non-normalized exact-exchange holes, resulting in large fractional-spin errors for conventional approximative density functionals. In this communication, we present a simple approach to directly include the exact-exchange-hole normalization into DFT. Compared to conventional functionals, our model strongly improves the description for multi-reference systems, while preserving the accuracy in the single-reference case. We analyze the performance of our proposed method at the example of spin-averaged atoms and spin-restricted bond dissociation energy surfaces.

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.

Communication: Density functional theory model for multi-reference systems based on the exact-exchange hole normalization.

PubMed

Laqua, Henryk; Kussmann, Jörg; Ochsenfeld, Christian

2018-03-28

The correct description of multi-reference electronic ground states within Kohn-Sham density functional theory (DFT) requires an ensemble-state representation, employing fractionally occupied orbitals. However, the use of fractional orbital occupation leads to non-normalized exact-exchange holes, resulting in large fractional-spin errors for conventional approximative density functionals. In this communication, we present a simple approach to directly include the exact-exchange-hole normalization into DFT. Compared to conventional functionals, our model strongly improves the description for multi-reference systems, while preserving the accuracy in the single-reference case. We analyze the performance of our proposed method at the example of spin-averaged atoms and spin-restricted bond dissociation energy surfaces.

Habitat suitability criteria via parametric distributions: estimation, model selection and uncertainty

USGS Publications Warehouse

Som, Nicholas A.; Goodman, Damon H.; Perry, Russell W.; Hardy, Thomas B.

2016-01-01

Previous methods for constructing univariate habitat suitability criteria (HSC) curves have ranged from professional judgement to kernel-smoothed density functions or combinations thereof. We present a new method of generating HSC curves that applies probability density functions as the mathematical representation of the curves. Compared with previous approaches, benefits of our method include (1) estimation of probability density function parameters directly from raw data, (2) quantitative methods for selecting among several candidate probability density functions, and (3) concise methods for expressing estimation uncertainty in the HSC curves. We demonstrate our method with a thorough example using data collected on the depth of water used by juvenile Chinook salmon (Oncorhynchus tschawytscha) in the Klamath River of northern California and southern Oregon. All R code needed to implement our example is provided in the appendix. Published 2015. This article is a U.S. Government work and is in the public domain in the USA.

Comparative study of DFT+U functionals for non-collinear magnetism

NASA Astrophysics Data System (ADS)

Ryee, Siheon; Han, Myung Joon

2018-07-01

We performed comparative analysis for DFT+U functionals to better understand their applicability to non-collinear magnetism. Taking LiNiPO4 and Sr2IrO4 as examples, we investigated the results out of two formalisms based on charge-only density and spin density functional plus U calculations. Our results show that the ground state spin order in terms of tilting angle is strongly dependent on Hund J. In particular, the opposite behavior of canting angles as a function of J is found for LiNiPO4. The dependence on the other physical parameters such as Hubbard U and Slater parameterization is investigated. We also discuss the formal aspects of these functional dependences as well as parameter dependences. The current study provides useful information and important intuition for the first-principles calculation of non-collinear magnetic materials.

KIDS Nuclear Energy Density Functional: 1st Application in Nuclei

NASA Astrophysics Data System (ADS)

Gil, Hana; Papakonstantinou, Panagiota; Hyun, Chang Ho; Oh, Yongseok

We apply the KIDS (Korea: IBS-Daegu-Sungkyunkwan) nuclear energy density functional model, which is based on the Fermi momentum expansion, to the study of properties of lj-closed nuclei. The parameters of the model are determined by the nuclear properties at the saturation density and theoretical calculations on pure neutron matter. For applying the model to the study of nuclei, we rely on the Skyrme force model, where the Skyrme force parameters are determined through the KIDS energy density functional. Solving Hartree-Fock equations, we obtain the energies per particle and charge radii of closed magic nuclei, namely, 16O, 28O, 40Ca, 48Ca, 60Ca, 90Zr, 132Sn, and 208Pb. The results are compared with the observed data and further improvement of the model is shortly mentioned.

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

Sim, Eunji; Kim, Min-Cheol; Burke, Kieron

We investigate dissociation of diatomic molecules using standard density functional theory (DFT) and density-corrected density functional theory (DC-DFT) compared with CCSD(T) results as reference. The results show the difference between the HOMO values of dissociated atomic species often can be used as an indicator whether DFT would predict the correct dissociation limit. DFT predicts incorrect dissociation limits and charge distribution in molecules or molecular ions when the fragments have large HOMO differences, while DC-DFT and CCSD(T) do not. The criteria for large HOMO difference is about 2 ∼ 4 eV.

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 density functional theory for association of fluid molecules with a functionalized surface: fluid-wall single and double bonding.

PubMed

Haghmoradi, Amin; Wang, Le; Chapman, Walter G

2017-02-01

In this manuscript we extend Wertheim's two-density formalism beyond its first order to model a system of fluid molecules with a single association site close to a planar hard wall with association sites on its surface in a density functional theory framework. The association sites of the fluid molecules are small enough that they can form only one bond, while the wall association sites are large enough to bond with more than one fluid molecule. The effects of temperature and of bulk fluid and wall site densities on the fluid density profile, extent of association, and competition between single and double bonding of fluid segments at the wall sites versus distance from the wall are presented. The theory predictions are compared with new Monte Carlo simulation results and they are in good agreement. The theory captures the surface coverage over wide ranges of temperature and bulk density by introducing the effect of steric hindrance in fluid association at a wall site.

On the logistic equation subject to uncertainties in the environmental carrying capacity and initial population density

NASA Astrophysics Data System (ADS)

Dorini, F. A.; Cecconello, M. S.; Dorini, L. B.

2016-04-01

It is recognized that handling uncertainty is essential to obtain more reliable results in modeling and computer simulation. This paper aims to discuss the logistic equation subject to uncertainties in two parameters: the environmental carrying capacity, K, and the initial population density, N0. We first provide the closed-form results for the first probability density function of time-population density, N(t), and its inflection point, t*. We then use the Maximum Entropy Principle to determine both K and N0 density functions, treating such parameters as independent random variables and considering fluctuations of their values for a situation that commonly occurs in practice. Finally, closed-form results for the density functions and statistical moments of N(t), for a fixed t > 0, and of t* are provided, considering the uniform distribution case. We carried out numerical experiments to validate the theoretical results and compared them against that obtained using Monte Carlo simulation.

A Tomographic Method for the Reconstruction of Local Probability Density Functions

NASA Technical Reports Server (NTRS)

Sivathanu, Y. R.; Gore, J. P.

1993-01-01

A method of obtaining the probability density function (PDF) of local properties from path integrated measurements is described. The approach uses a discrete probability function (DPF) method to infer the PDF of the local extinction coefficient from measurements of the PDFs of the path integrated transmittance. The local PDFs obtained using the method are compared with those obtained from direct intrusive measurements in propylene/air and ethylene/air diffusion flames. The results of this comparison are good.

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.

Functional response of ungulate browsers in disturbed eastern hemlock forests

USGS Publications Warehouse

DeStefano, Stephen

2015-01-01

Ungulate browsing in predator depleted North American landscapes is believed to be causing widespread tree recruitment failures. However, canopy disturbances and variations in ungulate densities are sources of heterogeneity that can buffer ecosystems against herbivory. Relatively little is known about the functional response (the rate of consumption in relation to food availability) of ungulates in eastern temperate forests, and therefore how “top down” control of vegetation may vary with disturbance type, intensity, and timing. This knowledge gap is relevant in the Northeastern United States today with the recent arrival of hemlock woolly adelgid (HWA; Adelges tsugae) that is killing eastern hemlocks (Tsuga canadensis) and initiating salvage logging as a management response. We used an existing experiment in central New England begun in 2005, which simulated severe adelgid infestation and intensive logging of intact hemlock forest, to examine the functional response of combined moose (Alces americanus) and white-tailed deer (Odocoileus virginianus) foraging in two different time periods after disturbance (3 and 7 years). We predicted that browsing impacts would be linear or accelerating (Type I or Type III response) in year 3 when regenerating stem densities were relatively low and decelerating (Type II response) in year 7 when stem densities increased. We sampled and compared woody regeneration and browsing among logged and simulated insect attack treatments and two intact controls (hemlock and hardwood forest) in 2008 and again in 2012. We then used AIC model selection to compare the three major functional response models (Types I, II, and III) of ungulate browsing in relation to forage density. We also examined relative use of the different stand types by comparing pellet group density and remote camera images. In 2008, total and proportional browse consumption increased with stem density, and peaked in logged plots, revealing a Type I response. In 2012, stem densities were greatest in girdled plots, but proportional browse consumption was highest at intermediate stem densities in logged plots, exhibiting a Type III (rather than a Type II) functional response. Our results revealed shifting top–down control by herbivores at different stages of stand recovery after disturbance and in different understory conditions resulting from logging vs. simulated adelgid attack. If forest managers wish to promote tree regeneration in hemlock stands that is more resistant to ungulate browsers, leaving HWA-infested stands unmanaged may be a better option than preemptively logging them.

Two-component scattering model and the electron density spectrum

NASA Astrophysics Data System (ADS)

Zhou, A. Z.; Tan, J. Y.; Esamdin, A.; Wu, X. J.

2010-02-01

In this paper, we discuss a rigorous treatment of the refractive scintillation caused by a two-component interstellar scattering medium and a Kolmogorov form of density spectrum. It is assumed that the interstellar scattering medium is composed of a thin-screen interstellar medium (ISM) and an extended interstellar medium. We consider the case that the scattering of the thin screen concentrates in a thin layer represented by a δ function distribution and that the scattering density of the extended irregular medium satisfies the Gaussian distribution. We investigate and develop equations for the flux density structure function corresponding to this two-component ISM geometry in the scattering density distribution and compare our result with the observations. We conclude that the refractive scintillation caused by this two-component ISM scattering gives a more satisfactory explanation for the observed flux density variation than does the single extended medium model. The level of refractive scintillation is strongly sensitive to the distribution of scattering material along the line of sight (LOS). The theoretical modulation indices are comparatively less sensitive to the scattering strength of the thin-screen medium, but they critically depend on the distance from the observer to the thin screen. The logarithmic slope of the structure function is sensitive to the scattering strength of the thin-screen medium, but is relatively insensitive to the thin-screen location. Therefore, the proposed model can be applied to interpret the structure functions of flux density observed in pulsar PSR B2111 + 46 and PSR B0136 + 57. The result suggests that the medium consists of a discontinuous distribution of plasma turbulence embedded in the interstellar medium. Thus our work provides some insight into the distribution of the scattering along the LOS to the pulsar PSR B2111 + 46 and PSR B0136 + 57.

Current Density Functional Theory Using Meta-Generalized Gradient Exchange-Correlation Functionals.

PubMed

Furness, James W; Verbeke, Joachim; Tellgren, Erik I; Stopkowicz, Stella; Ekström, Ulf; Helgaker, Trygve; Teale, Andrew M

2015-09-08

We present the self-consistent implementation of current-dependent (hybrid) meta-generalized gradient approximation (mGGA) density functionals using London atomic orbitals. A previously proposed generalized kinetic energy density is utilized to implement mGGAs in the framework of Kohn-Sham current density functional theory (KS-CDFT). A unique feature of the nonperturbative implementation of these functionals is the ability to seamlessly explore a wide range of magnetic fields up to 1 au (∼235 kT) in strength. CDFT functionals based on the TPSS and B98 forms are investigated, and their performance is assessed by comparison with accurate coupled-cluster singles, doubles, and perturbative triples (CCSD(T)) data. In the weak field regime, magnetic properties such as magnetizabilities and nuclear magnetic resonance shielding constants show modest but systematic improvements over generalized gradient approximations (GGA). However, in the strong field regime, the mGGA-based forms lead to a significantly improved description of the recently proposed perpendicular paramagnetic bonding mechanism, comparing well with CCSD(T) data. In contrast to functionals based on the vorticity, these forms are found to be numerically stable, and their accuracy at high field suggests that the extension of mGGAs to CDFT via the generalized kinetic energy density should provide a useful starting point for further development of CDFT approximations.

DFT benchmark study for the oxidative addition of CH 4 to Pd. Performance of various density functionals

NASA Astrophysics Data System (ADS)

de Jong, G. Theodoor; Geerke, Daan P.; Diefenbach, Axel; Matthias Bickelhaupt, F.

2005-06-01

We have evaluated the performance of 24 popular density functionals for describing the potential energy surface (PES) of the archetypal oxidative addition reaction of the methane C-H bond to the palladium atom by comparing the results with our recent ab initio [CCSD(T)] benchmark study of this reaction. The density functionals examined cover the local density approximation (LDA), the generalized gradient approximation (GGA), meta-GGAs as well as hybrid density functional theory. Relativistic effects are accounted for through the zeroth-order regular approximation (ZORA). The basis-set dependence of the density-functional-theory (DFT) results is assessed for the Becke-Lee-Yang-Parr (BLYP) functional using a hierarchical series of Slater-type orbital (STO) basis sets ranging from unpolarized double-ζ (DZ) to quadruply polarized quadruple-ζ quality (QZ4P). Stationary points on the reaction surface have been optimized using various GGA functionals, all of which yield geometries that differ only marginally. Counterpoise-corrected relative energies of stationary points are converged to within a few tenths of a kcal/mol if one uses the doubly polarized triple-ζ (TZ2P) basis set and the basis-set superposition error (BSSE) drops to 0.0 kcal/mol for our largest basis set (QZ4P). Best overall agreement with the ab initio benchmark PES is achieved by functionals of the GGA, meta-GGA, and hybrid-DFT type, with mean absolute errors of 1.3-1.4 kcal/mol and errors in activation energies ranging from +0.8 to -1.4 kcal/mol. Interestingly, the well-known BLYP functional compares very reasonably with an only slightly larger mean absolute error of 2.5 kcal/mol and an underestimation by -1.9 kcal/mol of the overall barrier (i.e., the difference in energy between the TS and the separate reactants). For comparison, with B3LYP we arrive at a mean absolute error of 3.8 kcal/mol and an overestimation of the overall barrier by 4.5 kcal/mol.

Molecular adsorption on metal surfaces with van der Waals density functionals

NASA Astrophysics Data System (ADS)

Li, Guo; Tamblyn, Isaac; Cooper, Valentino R.; Gao, Hong-Jun; Neaton, Jeffrey B.

2012-03-01

The adsorption of 1,4-benzenediamine (BDA) on Au(111) and azobenzene on Ag(111) is investigated using density functional theory (DFT) with the nonlocal van der Waals density functional (vdW-DF) and the semilocal Perdew-Burke-Ernzerhof functional. For BDA on Au(111), the inclusion of London dispersion interactions not only dramatically enhances the molecule-substrate binding, resulting in adsorption energies consistent with experimental results, but also significantly alters the BDA binding geometry. For azobenzene on Ag(111), vdW-DFs produce superior adsorption energies compared to those obtained with other dispersion-corrected DFT approaches. These results provide evidence for the applicability of the vdW-DF approach and serve as practical benchmarks for the investigation of molecules adsorbed on noble-metal surfaces.

Binary collision approximations for the memory function for density fluctuations in equilibrium atomic liquids

NASA Astrophysics Data System (ADS)

Noah, Joyce E.

Time correlation functions of density fluctuations of liquids at equilibrium can be used to relate the microscopic dynamics of a liquid to its macroscopic transport properties. Time correlation functions are especially useful since they can be generated in a variety of ways, from scattering experiments to computer simulation to analytic theory. The kinetic theory of fluctuations in equilibrium liquids is an analytic theory for calculating correlation functions using memory functions. In this work, we use a diagrammatic formulation of the kinetic theory to develop a series of binary collision approximations for the collisional part of the memory function. We define binary collisions as collisions between two distinct density fluctuations whose identities are fixed during the duration of a collsion. R approximations are for the short time part of the memory function, and build upon the work of Ranganathan and Andersen. These approximations have purely repulsive interactions between the fluctuations. The second type of approximation, RA approximations, is for the longer time part of the memory function, where the density fluctuations now interact via repulsive and attractive forces. Although RA approximations are a natural extension of R approximations, they permit two density fluctuations to become trapped in the wells of the interaction potential, leading to long-lived oscillatory behavior, which is unphysical. Therefore we consider S approximations which describe binary particles which experience the random effect of the surroundings while interacting via repulsive or repulsive and attractive interactions. For each of these approximations for the memory function we numerically solve the kinetic equation to generate correlation functions. These results are compared to molecular dynamics results for the correlation functions. Comparing the successes and failures of the different approximations, we conclude that R approximations give more accurate intermediate and long time results while RA and S approximations do particularly well at predicting the short time behavior. Lastly, we also develop a series of non-graphically derived approximations and use an optimization procedure to determine the underlying memory function from the simulation data. These approaches provide valuable information about the memory function that will be used in the development of future kinetic theories.

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.

Mapping the genome of meta-generalized gradient approximation density functionals: The search for B97M-V

NASA Astrophysics Data System (ADS)

Mardirossian, Narbe; Head-Gordon, Martin

2015-02-01

A meta-generalized gradient approximation density functional paired with the VV10 nonlocal correlation functional is presented. The functional form is selected from more than 1010 choices carved out of a functional space of almost 1040 possibilities. Raw data come from training a vast number of candidate functional forms on a comprehensive training set of 1095 data points and testing the resulting fits on a comprehensive primary test set of 1153 data points. Functional forms are ranked based on their ability to reproduce the data in both the training and primary test sets with minimum empiricism, and filtered based on a set of physical constraints and an often-overlooked condition of satisfactory numerical precision with medium-sized integration grids. The resulting optimal functional form has 4 linear exchange parameters, 4 linear same-spin correlation parameters, and 4 linear opposite-spin correlation parameters, for a total of 12 fitted parameters. The final density functional, B97M-V, is further assessed on a secondary test set of 212 data points, applied to several large systems including the coronene dimer and water clusters, tested for the accurate prediction of intramolecular and intermolecular geometries, verified to have a readily attainable basis set limit, and checked for grid sensitivity. Compared to existing density functionals, B97M-V is remarkably accurate for non-bonded interactions and very satisfactory for thermochemical quantities such as atomization energies, but inherits the demonstrable limitations of existing local density functionals for barrier heights.

A comparative study of nonparametric methods for pattern recognition

NASA Technical Reports Server (NTRS)

Hahn, S. F.; Nelson, G. D.

1972-01-01

The applied research discussed in this report determines and compares the correct classification percentage of the nonparametric sign test, Wilcoxon's signed rank test, and K-class classifier with the performance of the Bayes classifier. The performance is determined for data which have Gaussian, Laplacian and Rayleigh probability density functions. The correct classification percentage is shown graphically for differences in modes and/or means of the probability density functions for four, eight and sixteen samples. The K-class classifier performed very well with respect to the other classifiers used. Since the K-class classifier is a nonparametric technique, it usually performed better than the Bayes classifier which assumes the data to be Gaussian even though it may not be. The K-class classifier has the advantage over the Bayes in that it works well with non-Gaussian data without having to determine the probability density function of the data. It should be noted that the data in this experiment was always unimodal.

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.

Statistics of cosmic density profiles from perturbation theory

NASA Astrophysics Data System (ADS)

Bernardeau, Francis; Pichon, Christophe; Codis, Sandrine

2014-11-01

The joint probability distribution function (PDF) of the density within multiple concentric spherical cells is considered. It is shown how its cumulant generating function can be obtained at tree order in perturbation theory as the Legendre transform of a function directly built in terms of the initial moments. In the context of the upcoming generation of large-scale structure surveys, it is conjectured that this result correctly models such a function for finite values of the variance. Detailed consequences of this assumption are explored. In particular the corresponding one-cell density probability distribution at finite variance is computed for realistic power spectra, taking into account its scale variation. It is found to be in agreement with Λ -cold dark matter simulations at the few percent level for a wide range of density values and parameters. Related explicit analytic expansions at the low and high density tails are given. The conditional (at fixed density) and marginal probability of the slope—the density difference between adjacent cells—and its fluctuations is also computed from the two-cell joint PDF; it also compares very well to simulations. It is emphasized that this could prove useful when studying the statistical properties of voids as it can serve as a statistical indicator to test gravity models and/or probe key cosmological parameters.

Invited Paper - Density functional theory: coverage of dynamic and non-dynamic electron correlation effects

NASA Astrophysics Data System (ADS)

Cremer, Dieter

The electron correlation effects covered by density functional theory (DFT) can be assessed qualitatively by comparing DFT densities ρ(r) with suitable reference densities obtained with wavefunction theory (WFT) methods that cover typical electron correlation effects. The analysis of difference densities ρ(DFT)-ρ(WFT) reveals that LDA and GGA exchange (X) functionals mimic non-dynamic correlation effects in an unspecified way. It is shown that these long range correlation effects are caused by the self-interaction error (SIE) of standard X functionals. Self-interaction corrected (SIC) DFT exchange gives, similar to exact exchange, for the bonding region a delocalized exchange hole, and does not cover any correlation effects. Hence, the exchange SIE is responsible for the fact that DFT densities often resemble MP4 or MP2 densities. The correlation functional changes X-only DFT densities in a manner observed when higher order coupling effects between lower order N-electron correlation effects are included. Hybrid functionals lead to changes in the density similar to those caused by SICDFT, which simply reflects the fact that hybrid functionals have been developed to cover part of the SIE and its long range correlation effects in a balanced manner. In the case of spin-unrestricted DFT (UDFT), non-dynamic electron correlation effects enter the calculation both via the X functional and via the wavefunction, which may cause a double-counting of correlation effects. The use of UDFT in the form of permuted orbital and broken-symmetry DFT (PO-UDFT, BS-UDFT) can lead to reasonable descriptions of multireference systems provided certain conditions are fulfilled. More reliable, however, is a combination of DFT and WFT methods, which makes the routine description of multireference systems possible. The development of such methods implies a separation of dynamic and non-dynamic correlation effects. Strategies for accomplishing this goal are discussed in general and tested in practice for CAS (complete active space)-DFT.

Coherent nonlinear optical studies of elementary processes in biological complexes: diagrammatic techniques based on the wave function versus the density matrix

PubMed Central

Biggs, Jason D.; Voll, Judith A.; Mukamel, Shaul

2012-01-01

Two types of diagrammatic approaches for the design and simulation of nonlinear optical experiments (closed-time path loops based on the wave function and double-sided Feynman diagrams for the density matrix) are presented and compared. We give guidelines for the assignment of relevant pathways and provide rules for the interpretation of existing nonlinear experiments in carotenoids. PMID:22753822

On the feasibility of p-type Ga2O3

NASA Astrophysics Data System (ADS)

Kyrtsos, Alexandros; Matsubara, Masahiko; Bellotti, Enrico

2018-01-01

We investigate the various cation substitutional dopants in Ga2O3 for the possibility of p-type conductivity using density functional theory. Our calculations include both standard density functional theory and hybrid functional calculations. We demonstrate that all the investigated dopants result in deep acceptor levels, not able to contribute to the p-type conductivity of Ga2O3. In light of these results, we compare our findings with other wide bandgap oxides and reexamine previous experiments on zinc doping in Ga2O3.

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

Megala, M.; Rajkumar, Beulah J. M., E-mail: beulah-rajkumar@yahoo.co.in

The electronic and optical transfer properties of Benzene, Benzoic Acid (BA), Nitrobenzene (NB) and Para Nitro Benzoic Acid (PNBA) at ground and first excited state has been investigated by the Density functional theory (DFT)and Time Dependent Density Functional Theory (TDDFT) using SVWN functional/3-21G basis set respectively. Possible intra-molecular charge transfer and n to π* transitions in the ground and the first excitation states have been predicted by the molecular orbitals and the Natural Bond Orbital (NBO) analysis. The simulated absorption spectra have been generated and the result compared with existing experimental results.

Compton profiles of NiO and TiO2 obtained from first principles GWA spectral function

NASA Astrophysics Data System (ADS)

S, M. Khidzir; M, F. M. Halid; W, A. T. Wan Abdullah

2016-06-01

In this work, we first use momentum density studies to understand strongly correlated electron behavior, which is typically seen in transition metal oxides. We observe that correlated electron behavior as seen in bulk NiO is due to the Fermi break located in the middle of overlapping spectral functions obtained from a GW (G is Green’s function and W is the screened Coulomb interaction) approximation (GWA) calculation while in the case of TiO2 we can see that the origin of the constant momentum distribution in lower momenta is due to a pile up of spectra before the Fermi energy. These observations are then used to compare our calculated Compton profiles with previous experimental studies of Fukamachi and Limandri. Our calculations for NiO are observed to follow the same trend as the experimental profile but it is seen to have a wide difference in the case of TiO2before the Fermi break. The ground state momentum densities differ significantly from the quasiparticle momentum density, thus stressing the importance of the quasiparticle wave function as the input for the study of charge density and the electron localization function. Finally we perform a calculation of the quasiparticle renormalization function, giving a quantitative description of the discontinuity of the GWA momentum density.

Generalized Pauli constraints in reduced density matrix functional theory.

PubMed

Theophilou, Iris; Lathiotakis, Nektarios N; Marques, Miguel A L; Helbig, Nicole

2015-04-21

Functionals of the one-body reduced density matrix (1-RDM) are routinely minimized under Coleman's ensemble N-representability conditions. Recently, the topic of pure-state N-representability conditions, also known as generalized Pauli constraints, received increased attention following the discovery of a systematic way to derive them for any number of electrons and any finite dimensionality of the Hilbert space. The target of this work is to assess the potential impact of the enforcement of the pure-state conditions on the results of reduced density-matrix functional theory calculations. In particular, we examine whether the standard minimization of typical 1-RDM functionals under the ensemble N-representability conditions violates the pure-state conditions for prototype 3-electron systems. We also enforce the pure-state conditions, in addition to the ensemble ones, for the same systems and functionals and compare the correlation energies and optimal occupation numbers with those obtained by the enforcement of the ensemble conditions alone.

Assessing Hubbard-corrected AM05+ U and PBEsol+ U density functionals for strongly correlated oxides CeO 2 and Ce 2O 3

DOE PAGES

Weck, Philippe F.; Kim, Eunja

2016-09-12

The structure–property relationships of bulk CeO 2 and Ce 2O 3 have been investigated using AM05 and PBEsol exchange–correlation functionals within the frameworks of Hubbard-corrected density functional theory (DFT+ U) and density functional perturbation theory (DFPT+ U). Compared with conventional PBE+ U, RPBE+ U, PW91+ U and LDA+ U functionals, AM05+ U and PBEsol+ U describe experimental crystalline parameters and properties of CeO 2 and Ce 2O 3 with superior accuracy, especially when + U is chosen close to its value derived by the linear-response approach. Lastly, the present findings call for a reexamination of some of the problematic oxidemore » materials featuring strong f- and d-electron correlation using AM05+ U and PBEsol+ U.« less

Assessing Hubbard-corrected AM05+ U and PBEsol+ U density functionals for strongly correlated oxides CeO 2 and Ce 2O 3

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

Weck, Philippe F.; Kim, Eunja

The structure–property relationships of bulk CeO 2 and Ce 2O 3 have been investigated using AM05 and PBEsol exchange–correlation functionals within the frameworks of Hubbard-corrected density functional theory (DFT+ U) and density functional perturbation theory (DFPT+ U). Compared with conventional PBE+ U, RPBE+ U, PW91+ U and LDA+ U functionals, AM05+ U and PBEsol+ U describe experimental crystalline parameters and properties of CeO 2 and Ce 2O 3 with superior accuracy, especially when + U is chosen close to its value derived by the linear-response approach. Lastly, the present findings call for a reexamination of some of the problematic oxidemore » materials featuring strong f- and d-electron correlation using AM05+ U and PBEsol+ U.« less

Effects of molecular elongation on liquid crystalline phase behaviour: isotropic-nematic transition

NASA Astrophysics Data System (ADS)

Singh, Ram Chandra; Ram, Jokhan

2003-08-01

We present the density-functional approach to study the isotropic-nematic transitions and calculate the values of freezing parameters of the Gay-Berne liquid crystal model, concentrating on the effects of varying the molecular elongation, x0. For this, we have solved the Percus-Yevick integral equation theory to calculate the pair-correlation functions of a fluid the molecules of which interact via a Gay-Berne pair potential. These results have been used in the density-functional theory as an input to locate the isotropic-nematic transition and calculate freezing parameters for a range of length-to-width parameters 3.0⩽ x0⩽4.0 at reduced temperatures 0.95 and 1.25. We observed that as x0 is increased, the isotropic-nematic transition is seen to move to lower density at a given temperature. We find that the density-functional theory is good to study the freezing transitions in such fluids. We have also compared our results with computer simulation results wherever they are available.

Functional connectivity analysis of the neural bases of emotion regulation: A comparison of independent component method with density-based k-means clustering method.

PubMed

Zou, Ling; Guo, Qian; Xu, Yi; Yang, Biao; Jiao, Zhuqing; Xiang, Jianbo

2016-04-29

Functional magnetic resonance imaging (fMRI) is an important tool in neuroscience for assessing connectivity and interactions between distant areas of the brain. To find and characterize the coherent patterns of brain activity as a means of identifying brain systems for the cognitive reappraisal of the emotion task, both density-based k-means clustering and independent component analysis (ICA) methods can be applied to characterize the interactions between brain regions involved in cognitive reappraisal of emotion. Our results reveal that compared with the ICA method, the density-based k-means clustering method provides a higher sensitivity of polymerization. In addition, it is more sensitive to those relatively weak functional connection regions. Thus, the study concludes that in the process of receiving emotional stimuli, the relatively obvious activation areas are mainly distributed in the frontal lobe, cingulum and near the hypothalamus. Furthermore, density-based k-means clustering method creates a more reliable method for follow-up studies of brain functional connectivity.

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.

Theory of melting at high pressures: Amending density functional theory with quantum Monte Carlo

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

Shulenburger, L.; Desjarlais, M. P.; Mattsson, T. R.

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

Theory of melting at high pressures: Amending density functional theory with quantum Monte Carlo

DOE PAGES

Shulenburger, L.; Desjarlais, M. P.; Mattsson, T. R.

2014-10-01

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

Computing thermal Wigner densities with the phase integration method

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

Beutier, J.; Borgis, D.; Vuilleumier, R.

2014-08-28

We discuss how the Phase Integration Method (PIM), recently developed to compute symmetrized time correlation functions [M. Monteferrante, S. Bonella, and G. Ciccotti, Mol. Phys. 109, 3015 (2011)], can be adapted to sampling/generating the thermal Wigner density, a key ingredient, for example, in many approximate schemes for simulating quantum time dependent properties. PIM combines a path integral representation of the density with a cumulant expansion to represent the Wigner function in a form calculable via existing Monte Carlo algorithms for sampling noisy probability densities. The method is able to capture highly non-classical effects such as correlation among the momenta andmore » coordinates parts of the density, or correlations among the momenta themselves. By using alternatives to cumulants, it can also indicate the presence of negative parts of the Wigner density. Both properties are demonstrated by comparing PIM results to those of reference quantum calculations on a set of model problems.« less

Computing thermal Wigner densities with the phase integration method.

PubMed

Beutier, J; Borgis, D; Vuilleumier, R; Bonella, S

2014-08-28

We discuss how the Phase Integration Method (PIM), recently developed to compute symmetrized time correlation functions [M. Monteferrante, S. Bonella, and G. Ciccotti, Mol. Phys. 109, 3015 (2011)], can be adapted to sampling/generating the thermal Wigner density, a key ingredient, for example, in many approximate schemes for simulating quantum time dependent properties. PIM combines a path integral representation of the density with a cumulant expansion to represent the Wigner function in a form calculable via existing Monte Carlo algorithms for sampling noisy probability densities. The method is able to capture highly non-classical effects such as correlation among the momenta and coordinates parts of the density, or correlations among the momenta themselves. By using alternatives to cumulants, it can also indicate the presence of negative parts of the Wigner density. Both properties are demonstrated by comparing PIM results to those of reference quantum calculations on a set of model problems.

Evolution of HI from Z=5 to the present

NASA Technical Reports Server (NTRS)

Storrie-Lombardi, L. J.

2002-01-01

Studies of damped Lya systems provide us with a good measure of the evolution of the HI column density distribution function and the contribution to the comoving mass density in neutral gas out to redshifts of z = 5 . The column density distribution function at high redshift steepens for the highest column density HI absorbers, though the contribution to the comoving mass density of neutral gas remains fiat from 2 < z < 5 . Results from studies at z < 2 are finding substantial numbers of damped absorbers identified from MgII absorption, compared to previous blind surveys. These results indicate that the contribution to the comoving mass density in neutral gas may be constant from z 0 to z 5. Details of recent work in the redshift range z < 2 work is covered elsewhere in this volume (see D. Nestor). We review here recent results for the redshift range 2 < z < 5.

Calculation of the dielectric properties of semiconductors

NASA Astrophysics Data System (ADS)

Engel, G. E.; Farid, Behnam

1992-12-01

We report on numerical calculations of the dynamical dielectric function in silicon, using a continued-fraction expansion of the polarizability and a recently proposed representation of the inverse dielectric function in terms of plasmonlike excitations. A number of important technical refinements to further improve the computational efficiency of the method are introduced, making the ab initio calculation of the full energy dependence of the dielectric function comparable in cost to calculation of its static value. Physical results include the observation of previously unresolved features in the random-phase approximated dielectric function and its inverse within the framework of density-functional theory in the local-density approximation, which may be accessible to experiment. We discuss the dispersion of plasmon energies in silicon along the Λ and Δ directions and find improved agreement with experiment compared to earlier calculations. We also present quantitative evidence indicating the degree of violation of the Johnson f-sum rule for the dielectric function due to the nonlocality of the one-electron potential used in the underlying band-structure calculations.

On the design of random metasurface based devices.

PubMed

Dupré, Matthieu; Hsu, Liyi; Kanté, Boubacar

2018-05-08

Metasurfaces are generally designed by placing scatterers in periodic or pseudo-periodic grids. We propose and discuss design rules for functional metasurfaces with randomly placed anisotropic elements that randomly sample a well-defined phase function. By analyzing the focusing performance of random metasurface lenses as a function of their density and the density of the phase-maps used to design them, we find that the performance of 1D metasurfaces is mostly governed by their density while 2D metasurfaces strongly depend on both the density and the near-field coupling configuration of the surface. The proposed approach is used to design all-polarization random metalenses at near infrared frequencies. Challenges, as well as opportunities of random metasurfaces compared to periodic ones are discussed. Our results pave the way to new approaches in the design of nanophotonic structures and devices from lenses to solar energy concentrators.

Validating density-functional theory simulations at high energy-density conditions with liquid krypton shock experiments to 850 GPa on Sandia's Z machine

DOE PAGES

Mattsson, Thomas R.; Root, Seth; Mattsson, Ann E.; ...

2014-11-11

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

Bulk dynamics of Brownian hard disks: Dynamical density functional theory versus experiments on two-dimensional colloidal hard spheres

NASA Astrophysics Data System (ADS)

Stopper, Daniel; Thorneywork, Alice L.; Dullens, Roel P. A.; Roth, Roland

2018-03-01

Using dynamical density functional theory (DDFT), we theoretically study Brownian self-diffusion and structural relaxation of hard disks and compare to experimental results on quasi two-dimensional colloidal hard spheres. To this end, we calculate the self-van Hove correlation function and distinct van Hove correlation function by extending a recently proposed DDFT-approach for three-dimensional systems to two dimensions. We find that the theoretical results for both self-part and distinct part of the van Hove function are in very good quantitative agreement with the experiments up to relatively high fluid packing fractions of roughly 0.60. However, at even higher densities, deviations between the experiment and the theoretical approach become clearly visible. Upon increasing packing fraction, in experiments, the short-time self-diffusive behavior is strongly affected by hydrodynamic effects and leads to a significant decrease in the respective mean-squared displacement. By contrast, and in accordance with previous simulation studies, the present DDFT, which neglects hydrodynamic effects, shows no dependence on the particle density for this quantity.

The van Hove distribution function for Brownian hard spheres: Dynamical test particle theory and computer simulations for bulk dynamics

NASA Astrophysics Data System (ADS)

Hopkins, Paul; Fortini, Andrea; Archer, Andrew J.; Schmidt, Matthias

2010-12-01

We describe a test particle approach based on dynamical density functional theory (DDFT) for studying the correlated time evolution of the particles that constitute a fluid. Our theory provides a means of calculating the van Hove distribution function by treating its self and distinct parts as the two components of a binary fluid mixture, with the "self " component having only one particle, the "distinct" component consisting of all the other particles, and using DDFT to calculate the time evolution of the density profiles for the two components. We apply this approach to a bulk fluid of Brownian hard spheres and compare to results for the van Hove function and the intermediate scattering function from Brownian dynamics computer simulations. We find good agreement at low and intermediate densities using the very simple Ramakrishnan-Yussouff [Phys. Rev. B 19, 2775 (1979)] approximation for the excess free energy functional. Since the DDFT is based on the equilibrium Helmholtz free energy functional, we can probe a free energy landscape that underlies the dynamics. Within the mean-field approximation we find that as the particle density increases, this landscape develops a minimum, while an exact treatment of a model confined situation shows that for an ergodic fluid this landscape should be monotonic. We discuss possible implications for slow, glassy, and arrested dynamics at high densities.

Modeling ecological traps for the control of feral pigs

PubMed Central

Dexter, Nick; McLeod, Steven R

2015-01-01

Ecological traps are habitat sinks that are preferred by dispersing animals but have higher mortality or reduced fecundity compared to source habitats. Theory suggests that if mortality rates are sufficiently high, then ecological traps can result in extinction. An ecological trap may be created when pest animals are controlled in one area, but not in another area of equal habitat quality, and when there is density-dependent immigration from the high-density uncontrolled area to the low-density controlled area. We used a logistic population model to explore how varying the proportion of habitat controlled, control mortality rate, and strength of density-dependent immigration for feral pigs could affect the long-term population abundance and time to extinction. Increasing control mortality, the proportion of habitat controlled and the strength of density-dependent immigration decreased abundance both within and outside the area controlled. At higher levels of these parameters, extinction was achieved for feral pigs. We extended the analysis with a more complex stochastic, interactive model of feral pig dynamics in the Australian rangelands to examine how the same variables as the logistic model affected long-term abundance in the controlled and uncontrolled area and time to extinction. Compared to the logistic model of feral pig dynamics, the stochastic interactive model predicted lower abundances and extinction at lower control mortalities and proportions of habitat controlled. To improve the realism of the stochastic interactive model, we substituted fixed mortality rates with a density-dependent control mortality function, empirically derived from helicopter shooting exercises in Australia. Compared to the stochastic interactive model with fixed mortality rates, the model with the density-dependent control mortality function did not predict as substantial decline in abundance in controlled or uncontrolled areas or extinction for any combination of variables. These models demonstrate that pest eradication is theoretically possible without the pest being controlled throughout its range because of density-dependent immigration into the area controlled. The stronger the density-dependent immigration, the better the overall control in controlled and uncontrolled habitat combined. However, the stronger the density-dependent immigration, the poorer the control in the area controlled. For feral pigs, incorporating environmental stochasticity improves the prospects for eradication, but adding a realistic density-dependent control function eliminates these prospects. PMID:26045954

Mapping the genome of meta-generalized gradient approximation density functionals: The search for B97M-V

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

Mardirossian, Narbe; Head-Gordon, Martin, E-mail: mhg@cchem.berkeley.edu; Chemical Sciences Division, Lawrence Berkeley National Laboratory, Berkeley, California 94720

2015-02-21

A meta-generalized gradient approximation density functional paired with the VV10 nonlocal correlation functional is presented. The functional form is selected from more than 10{sup 10} choices carved out of a functional space of almost 10{sup 40} possibilities. Raw data come from training a vast number of candidate functional forms on a comprehensive training set of 1095 data points and testing the resulting fits on a comprehensive primary test set of 1153 data points. Functional forms are ranked based on their ability to reproduce the data in both the training and primary test sets with minimum empiricism, and filtered based onmore » a set of physical constraints and an often-overlooked condition of satisfactory numerical precision with medium-sized integration grids. The resulting optimal functional form has 4 linear exchange parameters, 4 linear same-spin correlation parameters, and 4 linear opposite-spin correlation parameters, for a total of 12 fitted parameters. The final density functional, B97M-V, is further assessed on a secondary test set of 212 data points, applied to several large systems including the coronene dimer and water clusters, tested for the accurate prediction of intramolecular and intermolecular geometries, verified to have a readily attainable basis set limit, and checked for grid sensitivity. Compared to existing density functionals, B97M-V is remarkably accurate for non-bonded interactions and very satisfactory for thermochemical quantities such as atomization energies, but inherits the demonstrable limitations of existing local density functionals for barrier heights.« less

Mapping the genome of meta-generalized gradient approximation density functionals: The search for B97M-V

DOE PAGES

Mardirossian, Narbe; Head-Gordon, Martin

2015-02-20

We present a meta-generalized gradient approximation density functional paired with the VV10 nonlocal correlation functional. The functional form is selected from more than 10 10 choices carved out of a functional space of almost 10 40 possibilities. This raw data comes from training a vast number of candidate functional forms on a comprehensive training set of 1095 data points and testing the resulting fits on a comprehensive primary test set of 1153 data points. Functional forms are ranked based on their ability to reproduce the data in both the training and primary test sets with minimum empiricism, and filteredmore » based on a set of physical constraints and an often-overlooked condition of satisfactory numerical precision with medium-sized integration grids. The resulting optimal functional form has 4 linear exchange parameters, 4 linear same-spin correlation parameters, and 4 linear opposite-spin correlation parameters, for a total of 12 fitted parameters. The final density functional, B97M-V, is further assessed on a secondary test set of 212 data points, applied to several large systems including the coronene dimer and water clusters, tested for the accurate prediction of intramolecular and intermolecular geometries, verified to have a readily attainable basis set limit, and checked for grid sensitivity. Compared to existing density functionals, B97M-V is remarkably accurate for non-bonded interactions and very satisfactory for thermochemical quantities such as atomization energies, but inherits the demonstrable limitations of existing local density functionals for barrier heights.« less

Surface modification of carbon nanotubes using 3-aminopropyltriethoxysilane to improve mechanical properties of nanocomposite based polymer matrix: Experimental and Density functional theory study

NASA Astrophysics Data System (ADS)

Hamed Mashhadzadeh, A.; Fereidoon, Ab.; Ghorbanzadeh Ahangari, M.

2017-10-01

In current study we combined theoretical and experimental studies to evaluate the effect of functionalization and silanization on mechanical behavior of polymer-based/CNT nanocomposites. Epoxy was selected as thermoset polymer, polypropylene and poly vinyl chloride were selected as thermoplastic polymers. The whole procedure is divided to two sections . At first we applied density functional theory (DFT) to analyze the effect of functionalization on equilibrium distance and adsorption energy of unmodified, functionalized by sbnd OH group and silanized epoxy/CNT, PP/CNT and PVC/CNT nanocomposites and the results showed that functionalization increased adsorption energy and reduced the equilibrium distance in all studied nanocomposites and silanization had higher effect comparing to OH functionalizing. Then we prepared experimental samples of all mentioned nanocomposites and tested their tensile and flexural strength properties. The obtained results showed that functionalization increased the studied mechanical properties in all evaluated nanocomposites. Finally we compared the results of experimental and theoretical sections with each other and estimated a suitable agreement between these parts.

Use of a priori statistics to minimize acquisition time for RFI immune spread spectrum systems

NASA Technical Reports Server (NTRS)

Holmes, J. K.; Woo, K. T.

1978-01-01

The optimum acquisition sweep strategy was determined for a PN code despreader when the a priori probability density function was not uniform. A psuedo noise spread spectrum system was considered which could be utilized in the DSN to combat radio frequency interference. In a sample case, when the a priori probability density function was Gaussian, the acquisition time was reduced by about 41% compared to a uniform sweep approach.

Density of Key-Species Determines Efficiency of Macroalgae Detritus Uptake by Intertidal Benthic Communities

PubMed Central

Karlson, Agnes M. L.; Niemand, Clarisse; Savage, Candida; Pilditch, Conrad A

2016-01-01

Accumulating evidence shows that increased biodiversity has a positive effect on ecosystem functioning, but the mechanisms that underpin this positive relationship are contentious. Complete extinctions of regional species pools are comparatively rare whereas compositional changes and reductions in abundance and biomass are common, although seldom the focus of biodiversity-ecosystem functioning studies. We use natural, small-scale patchiness in the density of two species of large bivalves with contrasting feeding modes (the suspension-feeding Austrovenus stutchburyi and deposit-feeding Macomona liliana) to examine their influence on the uptake of nitrogen from macroalgae detritus (i.e. measure of ecosystem function and food web efficiency) by other infauna in a 10-d laboratory isotope-tracer experiment. We predicted that densities of these key bivalve species and functional group diversity (calculated as Shannons H, a density-independent measure of community composition) of the intact infaunal community will be critical factors explaining variance in macroalgal per capita uptake rates by the community members and hence determine total uptake by the community. Results show that only two species, M. liliana and a large orbiniid polychaete (Scoloplos cylindrifer) dominated macroalgal nitrogen taken up by the whole community due to their large biomass. However, their densities were mostly not important or negatively influenced per capita uptake by other species. Instead, the density of a head-down deposit-feeder (the capitellid Heteromastus filiformis), scavengers (mainly nemertines and nereids) and species and functional group diversity, best explained per capita uptake rates in community members. Our results demonstrate the importance of species identity, density and large body size for ecosystem functioning and highlight the complex interactions underlying loss of ecological functions with declining biodiversity and compositional changes. PMID:27414032

Molecular density functional theory of water describing hydrophobicity at short and long length scales

NASA Astrophysics Data System (ADS)

Jeanmairet, Guillaume; Levesque, Maximilien; Borgis, Daniel

2013-10-01

We present an extension of our recently introduced molecular density functional theory of water [G. Jeanmairet et al., J. Phys. Chem. Lett. 4, 619 (2013)] to the solvation of hydrophobic solutes of various sizes, going from angstroms to nanometers. The theory is based on the quadratic expansion of the excess free energy in terms of two classical density fields: the particle density and the multipolar polarization density. Its implementation requires as input a molecular model of water and three measurable bulk properties, namely, the structure factor and the k-dependent longitudinal and transverse dielectric susceptibilities. The fine three-dimensional water structure around small hydrophobic molecules is found to be well reproduced. In contrast, the computed solvation free-energies appear overestimated and do not exhibit the correct qualitative behavior when the hydrophobic solute is grown in size. These shortcomings are corrected, in the spirit of the Lum-Chandler-Weeks theory, by complementing the functional with a truncated hard-sphere functional acting beyond quadratic order in density, and making the resulting functional compatible with the Van-der-Waals theory of liquid-vapor coexistence at long range. Compared to available molecular simulations, the approach yields reasonable solvation structure and free energy of hard or soft spheres of increasing size, with a correct qualitative transition from a volume-driven to a surface-driven regime at the nanometer scale.

Analysis of the proton longitudinal structure function from the gluon distribution function

NASA Astrophysics Data System (ADS)

Boroun, G. R.; Rezaei, B.

2012-11-01

We make a critical, next-to-leading order, study of the relationship between the longitudinal structure function F L and the gluon distribution proposed in Cooper-Sarkar et al. (Z. Phys. C 39:281, 1988; Acta Phys. Pol. B 34:2911 2003), which is frequently used to extract the gluon distribution from the proton longitudinal structure function at small x. The gluon density is obtained by expanding at particular choices of the point of expansion and compared with the hard Pomeron behavior for the gluon density. Comparisons with H1 data are made and predictions for the proposed best approach are also provided.

Comparing fluorescence-based cell-free assays for the assessment of antioxidative capacity of high-density lipoproteins

USDA-ARS?s Scientific Manuscript database

Background: Population studies have shown an inverse association between high-density lipoprotein (HDL) cholesterol levels and risk of coronary heart disease (CHD). HDL has different functions, including the ability to protect biological molecules from oxidation. Our aim was to evaluate the performa...

Two-dimensional molecular line transfer for a cometary coma

NASA Astrophysics Data System (ADS)

Szutowicz, S.

2017-09-01

In the proposed axisymmetric model of the cometary coma the gas density profile is described by an angular density function. Three methods for treating two-dimensional radiative transfer are compared: the Large Velocity Gradient (LVG) (the Sobolev method), Accelerated Lambda Iteration (ALI) and accelerated Monte Carlo (MC).

Trunk density profile estimates from dual X-ray absorptiometry.

PubMed

Wicke, Jason; Dumas, Geneviève A; Costigan, Patrick A

2008-01-01

Accurate body segment parameters are necessary to estimate joint loads when using biomechanical models. Geometric methods can provide individualized data for these models but the accuracy of the geometric methods depends on accurate segment density estimates. The trunk, which is important in many biomechanical models, has the largest variability in density along its length. Therefore, the objectives of this study were to: (1) develop a new method for modeling trunk density profiles based on dual X-ray absorptiometry (DXA) and (2) develop a trunk density function for college-aged females and males that can be used in geometric methods. To this end, the density profiles of 25 females and 24 males were determined by combining the measurements from a photogrammetric method and DXA readings. A discrete Fourier transformation was then used to develop the density functions for each sex. The individual density and average density profiles compare well with the literature. There were distinct differences between the profiles of two of participants (one female and one male), and the average for their sex. It is believed that the variations in these two participants' density profiles were a result of the amount and distribution of fat they possessed. Further studies are needed to support this possibility. The new density functions eliminate the uniform density assumption associated with some geometric models thus providing more accurate trunk segment parameter estimates. In turn, more accurate moments and forces can be estimated for the kinetic analyses of certain human movements.

Universal analytical scattering form factor for shell-, core-shell, or homogeneous particles with continuously variable density profile shape.

PubMed

Foster, Tobias

2011-09-01

A novel analytical and continuous density distribution function with a widely variable shape is reported and used to derive an analytical scattering form factor that allows us to universally describe the scattering from particles with the radial density profile of homogeneous spheres, shells, or core-shell particles. Composed by the sum of two Fermi-Dirac distribution functions, the shape of the density profile can be altered continuously from step-like via Gaussian-like or parabolic to asymptotically hyperbolic by varying a single "shape parameter", d. Using this density profile, the scattering form factor can be calculated numerically. An analytical form factor can be derived using an approximate expression for the original Fermi-Dirac distribution function. This approximation is accurate for sufficiently small rescaled shape parameters, d/R (R being the particle radius), up to values of d/R ≈ 0.1, and thus captures step-like, Gaussian-like, and parabolic as well as asymptotically hyperbolic profile shapes. It is expected that this form factor is particularly useful in a model-dependent analysis of small-angle scattering data since the applied continuous and analytical function for the particle density profile can be compared directly with the density profile extracted from the data by model-free approaches like the generalized inverse Fourier transform method. © 2011 American Chemical Society

Equilibrium finite-frequency noise of an interacting mesoscopic capacitor studied in time-dependent density functional theory

NASA Astrophysics Data System (ADS)

Dittmann, Niklas; Splettstoesser, Janine; Helbig, Nicole

2018-03-01

We calculate the frequency-dependent equilibrium noise of a mesoscopic capacitor in time-dependent density functional theory (TDDFT). The capacitor is modeled as a single-level quantum dot with on-site Coulomb interaction and tunnel coupling to a nearby reservoir. The noise spectra are derived from linear-response conductances via the fluctuation-dissipation theorem. Thereby, we analyze the performance of a recently derived exchange-correlation potential with time-nonlocal density dependence in the finite-frequency linear-response regime. We compare our TDDFT noise spectra with real-time perturbation theory and find excellent agreement for noise frequencies below the reservoir temperature.

Implementation and benchmark of a long-range corrected functional in the density functional based tight-binding method

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

Lutsker, V.; Niehaus, T. A., E-mail: thomas.niehaus@physik.uni-regensburg.de; Aradi, B.

2015-11-14

Bridging the gap between first principles methods and empirical schemes, the density functional based tight-binding method (DFTB) has become a versatile tool in predictive atomistic simulations over the past years. One of the major restrictions of this method is the limitation to local or gradient corrected exchange-correlation functionals. This excludes the important class of hybrid or long-range corrected functionals, which are advantageous in thermochemistry, as well as in the computation of vibrational, photoelectron, and optical spectra. The present work provides a detailed account of the implementation of DFTB for a long-range corrected functional in generalized Kohn-Sham theory. We apply themore » method to a set of organic molecules and compare ionization potentials and electron affinities with the original DFTB method and higher level theory. The new scheme cures the significant overpolarization in electric fields found for local DFTB, which parallels the functional dependence in first principles density functional theory (DFT). At the same time, the computational savings with respect to full DFT calculations are not compromised as evidenced by numerical benchmark data.« less

Probability density function approach for compressible turbulent reacting flows

NASA Technical Reports Server (NTRS)

Hsu, A. T.; Tsai, Y.-L. P.; Raju, M. S.

1994-01-01

The objective of the present work is to extend the probability density function (PDF) tubulence model to compressible reacting flows. The proability density function of the species mass fractions and enthalpy are obtained by solving a PDF evolution equation using a Monte Carlo scheme. The PDF solution procedure is coupled with a compression finite-volume flow solver which provides the velocity and pressure fields. A modeled PDF equation for compressible flows, capable of treating flows with shock waves and suitable to the present coupling scheme, is proposed and tested. Convergence of the combined finite-volume Monte Carlo solution procedure is discussed. Two super sonic diffusion flames are studied using the proposed PDF model and the results are compared with experimental data; marked improvements over solutions without PDF are observed.

Capillary electrophoresis of covalently functionalized single-chirality carbon nanotubes.

PubMed

He, Pingli; Meany, Brendan; Wang, Chunyan; Piao, Yanmei; Kwon, Hyejin; Deng, Shunliu; Wang, YuHuang

2017-07-01

We demonstrate the separation of chirality-enriched single-walled carbon nanotubes (SWCNTs) by degree of surface functionalization using high-performance CE. Controlled amounts of negatively charged and positively charged functional groups were attached to the sidewall of chirality-enriched SWCNTs through covalent functionalization using 4-carboxybenzenediazonium tetrafluoroborate or 4-diazo-N,N-diethylaniline tetrafluoroborate, respectively. Surfactant- and pH-dependent studies confirmed that under conditions that minimized ionic screening effects, separation of these functionalized SWCNTs was strongly dependent on the surface charge density introduced through covalent surface chemistry. For both heterogeneous mixtures and single-chirality-enriched samples, covalently functionalized SWCNTs showed substantially increased peak width in electropherogram spectra compared to nonfunctionalized SWCNTs, which can be attributed to a distribution of surface charges along the functionalized nanotubes. Successful separation of functionalized single-chirality SWCNTs by functional density was confirmed with UV-Vis-NIR absorption and Raman scattering spectroscopies of fraction collected samples. These results suggest a high degree of structural heterogeneity in covalently functionalized SWCNTs, even for chirality-enriched samples, and show the feasibility of applying CE for high-performance separation of nanomaterials based on differences in surface functional density. © 2017 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Orbital-Dependent Density Functionals for Chemical Catalysis

DTIC Science & Technology

2014-10-17

noncollinear density functional theory to show that the low-spin state of Mn3 in a model of the oxygen -evolving complex of photosystem II avoids...DK, which denotes the cc-pV5Z-DK basis set for 3d metals and hydrogen and the ma-cc- pV5Z-DK basis set for oxygen ) and to nonrelativistic all...cc-pV5Z basis set for oxygen ). As compared to NCBS-DK results, all ECP calculations perform worse than def2-TZVP all-electron relativistic

Analysis of Different Cost Functions in the Geosect Airspace Partitioning Tool

NASA Technical Reports Server (NTRS)

Wong, Gregory L.

2010-01-01

A new cost function representing air traffic controller workload is implemented in the Geosect airspace partitioning tool. Geosect currently uses a combination of aircraft count and dwell time to select optimal airspace partitions that balance controller workload. This is referred to as the aircraft count/dwell time hybrid cost function. The new cost function is based on Simplified Dynamic Density, a measure of different aspects of air traffic controller workload. Three sectorizations are compared. These are the current sectorization, Geosect's sectorization based on the aircraft count/dwell time hybrid cost function, and Geosect s sectorization based on the Simplified Dynamic Density cost function. Each sectorization is evaluated for maximum and average workload along with workload balance using the Simplified Dynamic Density as the workload measure. In addition, the Airspace Concept Evaluation System, a nationwide air traffic simulator, is used to determine the capacity and delay incurred by each sectorization. The sectorization resulting from the Simplified Dynamic Density cost function had a lower maximum workload measure than the other sectorizations, and the sectorization based on the combination of aircraft count and dwell time did a better job of balancing workload and balancing capacity. However, the current sectorization had the lowest average workload, highest sector capacity, and the least system delay.

Ecological and evolutionary consequences of tri-trophic interactions: Spatial variation and effects of plant density.

PubMed

Abdala-Roberts, Luis; Parra-Tabla, Víctor; Moreira, Xoaquín; Ramos-Zapata, José

2017-02-01

The factors driving variation in species interactions are often unknown, and few studies have made a link between changes in interactions and the strength of selection. We report on spatial variation in functional responses by a seed predator (SP) and its parasitic wasps associated with the herb Ruellia nudiflora . We assessed the influence of plant density on consumer responses and determined whether density effects and spatial variation in functional responses altered natural selection by these consumers on the plant. We established common gardens at two sites in Yucatan, Mexico, and planted R. nudiflora at two densities in each garden. We recorded fruit output and SP and parasitoid attack; calculated relative fitness (seed number) under scenarios of three trophic levels (accounting for SP and parasitoid effects), two trophic levels (accounting for SP but not parasitoid effects), and one trophic level (no consumer effects); and compared selection strength on fruit number under these scenarios across sites and densities. There was spatial variation in SP recruitment, whereby the SP functional response was negatively density-dependent at one site but density-independent at the other; parasitoid responses were density-independent and invariant across sites. Site variation in SP attack led, in turn, to differences in SP selection on fruit output, and parasitoids did not alter SP selection. There were no significant effects of density at either site. Our results provide a link between consumer functional responses and consumer selection on plants, which deepens our understanding of geographic variation in the evolutionary outcomes of multitrophic interactions. © 2017 Botanical Society of America.

Disrupted resting brain graph measures in individuals at high risk for alcoholism.

PubMed

Holla, Bharath; Panda, Rajanikant; Venkatasubramanian, Ganesan; Biswal, Bharat; Bharath, Rose Dawn; Benegal, Vivek

2017-07-30

Familial susceptibility to alcoholism is likely to be linked to the externalizing diathesis seen in high-risk offspring from high-density alcohol use disorder (AUD) families. The present study aimed at comparing resting brain functional connectivity and their association with externalizing symptoms and alcoholism familial density in 40 substance-naive high-risk (HR) male offspring from high-density AUD families and 30 matched healthy low-risk (LR) males without a family history of substance dependence using graph theory-based network analysis. The HR subjects from high-density AUD families compared with LR, showed significantly reduced clustering, small-worldness, and local network efficiency. The frontoparietal, cingulo-opercular, sensorimotor and cerebellar networks exhibited significantly reduced functional segregation. These disruptions exhibited independent incremental value in predicting the externalizing symptoms over and above the demographic variables. The reduction of functional segregation in HR subjects was significant across both the younger and older age groups and was proportional to the family loading of AUDs. Detection and estimation of these developmentally relevant disruptions in small-world architecture at critical brain regions sub-serving cognitive, affective, and sensorimotor processes are vital for understanding the familial risk for early onset alcoholism as well as for understanding the pathophysiological mechanism of externalizing behaviors. Copyright © 2017 Elsevier Ireland Ltd. All rights reserved.

Determination of atomic sodium in coal combustion using laser-induced fluorescence

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

Sweeny, P.G.; Abrahamson, H.B.; Radonovich, L.J.

1987-01-01

A laser-induced fluorescence spectrometer (LIFS) was assembled and sodium atom densities produced from the aspiration of solutions and direct introduction of a lignite into a flame were determined from fluorescence measurements. The average flame volume observed was 0.4mm/sup 3/. This small volume allowed the measurement of sodium concentrations as a function of vertical and horizontal flame position. Temperature profiles of the flames employed were also obtained and compared with the sodium atom densities. The sodium atom densities calculated from the fluorescence measurements (N/sub tt/) are compared with the sodium atom densities calculated from thermodynamic considerations (N/sub tt/) and sodium concentrationsmore » derived from aspiration/introduction rates (N/sub ta/).« less

Investigations on Cs-free alternatives for negative ion formation in a low pressure hydrogen discharge at ion source relevant parameters

NASA Astrophysics Data System (ADS)

Kurutz, U.; Friedl, R.; Fantz, U.

2017-07-01

Caesium (Cs) is applied in high power negative hydrogen ion sources to reduce a converter surface’s work function and thus enabling an efficient negative ion surface formation. Inherent drawbacks with the usage of this reactive alkali metal motivate the search for Cs-free alternative materials for neutral beam injection systems in fusion research. In view of a future DEMOnstration power plant, a suitable material should provide a high negative ion formation efficiency and comply with the RAMI issues of the system: reliability, availability, maintainability, inspectability. Promising candidates, like low work function materials (molybdenum doped with lanthanum (MoLa) and LaB6), as well as different non-doped and boron-doped diamond samples were investigated in this context at identical and ion source relevant parameters at the laboratory experiment HOMER. Negative ion densities were measured above the samples by means of laser photodetachment and compared with two reference cases: pure negative ion volume formation with negative ion densities of about 1× {10}15 {{{m}}}-3 and the effect of H- surface production using an in situ caesiated stainless steel sample which yields 2.5 times higher densities. Compared to pure volume production, none of the diamond samples did exhibit a measurable increase in H- densities, while showing clear indications of plasma-induced erosion. In contrast, both MoLa and LaB6 produced systematically higher densities (MoLa: ×1.60 LaB6: ×1.43). The difference to caesiation can be attributed to the higher work functions of MoLa and LaB6 which are expected to be about 3 eV for both compared to 2.1 eV of a caesiated surface.

Improved first-pass spiral myocardial perfusion imaging with variable density trajectories.

PubMed

Salerno, Michael; Sica, Christopher; Kramer, Christopher M; Meyer, Craig H

2013-11-01

To develop and evaluate variable-density spiral first-pass perfusion pulse sequences for improved efficiency and off-resonance performance and to demonstrate the utility of an apodizing density compensation function (DCF) to improve signal-to-noise ratio (SNR) and reduce dark-rim artifact caused by cardiac motion and Gibbs Ringing. Three variable density spiral trajectories were designed, simulated, and evaluated in 18 normal subjects, and in eight patients with cardiac pathology on a 1.5T scanner. By using a DCF, which intentionally apodizes the k-space data, the sidelobe amplitude of the theoretical point spread function (PSF) is reduced by 68%, with only a 13% increase in the full-width at half-maximum of the main-lobe when compared with the same data corrected with a conventional variable-density DCF, and has an 8% higher resolution than a uniform density spiral with the same number of interleaves and readout duration. Furthermore, this strategy results in a greater than 60% increase in measured SNR when compared with the same variable-density spiral data corrected with a conventional DCF (P < 0.01). Perfusion defects could be clearly visualized with minimal off-resonance and dark-rim artifacts. Variable-density spiral pulse sequences using an apodized DCF produce high-quality first-pass perfusion images with minimal dark-rim and off-resonance artifacts, high SNR and contrast-to-noise ratio, and good delineation of resting perfusion abnormalities. Copyright © 2012 Wiley Periodicals, Inc.

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.

Back in the saddle: large-deviation statistics of the cosmic log-density field

NASA Astrophysics Data System (ADS)

Uhlemann, C.; Codis, S.; Pichon, C.; Bernardeau, F.; Reimberg, P.

2016-08-01

We present a first principle approach to obtain analytical predictions for spherically averaged cosmic densities in the mildly non-linear regime that go well beyond what is usually achieved by standard perturbation theory. A large deviation principle allows us to compute the leading order cumulants of average densities in concentric cells. In this symmetry, the spherical collapse model leads to cumulant generating functions that are robust for finite variances and free of critical points when logarithmic density transformations are implemented. They yield in turn accurate density probability distribution functions (PDFs) from a straightforward saddle-point approximation valid for all density values. Based on this easy-to-implement modification, explicit analytic formulas for the evaluation of the one- and two-cell PDF are provided. The theoretical predictions obtained for the PDFs are accurate to a few per cent compared to the numerical integration, regardless of the density under consideration and in excellent agreement with N-body simulations for a wide range of densities. This formalism should prove valuable for accurately probing the quasi-linear scales of low-redshift surveys for arbitrary primordial power spectra.

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

Sherlock, M.; Brodrick, J. P.; Ridgers, C. P.

Here, we compare the reduced non-local electron transport model developed to Vlasov-Fokker-Planck simulations. Two new test cases are considered: the propagation of a heat wave through a high density region into a lower density gas, and a one-dimensional hohlraum ablation problem. We find that the reduced model reproduces the peak heat flux well in the ablation region but significantly over-predicts the coronal preheat. The suitability of the reduced model for computing non-local transport effects other than thermal conductivity is considered by comparing the computed distribution function to the Vlasov-Fokker-Planck distribution function. It is shown that even when the reduced modelmore » reproduces the correct heat flux, the distribution function is significantly different to the Vlasov-Fokker-Planck prediction. Two simple modifications are considered which improve agreement between models in the coronal region.« less

Underscreening in ionic liquids: a first principles analysis.

PubMed

Rotenberg, Benjamin; Bernard, Olivier; Hansen, Jean-Pierre

2018-02-07

An attempt is made to understand the underscreening effect, observed in concentrated electrolyte solutions or melts, on the basis of simple, admittedly crude models involving charged (for the ions) and neutral (for the solvent molecules) hard spheres. The thermodynamic and structural properties of these 'primitive' and 'semi-primitive' models are calculated within mean spherical approximation, which provides the basic input required to determine the partial density response functions. The screening length [Formula: see text], which is unambiguously defined in terms of the wave-number-dependent response functions, exhibits a cross-over from a low density, Debye-like regime, to a regime where [Formula: see text] increases with density beyond a critical density at which the Debye length [Formula: see text] becomes comparable to the ion diameter. In this high density regime the ratio [Formula: see text] increases according to a power law, in qualitative agreement with experimental measurements, albeit at a much slower rate.

Underscreening in ionic liquids: a first principles analysis

NASA Astrophysics Data System (ADS)

Rotenberg, Benjamin; Bernard, Olivier; Hansen, Jean-Pierre

2018-02-01

An attempt is made to understand the underscreening effect, observed in concentrated electrolyte solutions or melts, on the basis of simple, admittedly crude models involving charged (for the ions) and neutral (for the solvent molecules) hard spheres. The thermodynamic and structural properties of these ‘primitive’ and ‘semi-primitive’ models are calculated within mean spherical approximation, which provides the basic input required to determine the partial density response functions. The screening length λS , which is unambiguously defined in terms of the wave-number-dependent response functions, exhibits a cross-over from a low density, Debye-like regime, to a regime where λS increases with density beyond a critical density at which the Debye length λD becomes comparable to the ion diameter. In this high density regime the ratio λ_S/λD increases according to a power law, in qualitative agreement with experimental measurements, albeit at a much slower rate.

Quantitative computed tomography of lung parenchyma in patients with emphysema: analysis of higher-density lung regions

NASA Astrophysics Data System (ADS)

Lederman, Dror; Leader, Joseph K.; Zheng, Bin; Sciurba, Frank C.; Tan, Jun; Gur, David

2011-03-01

Quantitative computed tomography (CT) has been widely used to detect and evaluate the presence (or absence) of emphysema applying the density masks at specific thresholds, e.g., -910 or -950 Hounsfield Unit (HU). However, it has also been observed that subjects with similar density-mask based emphysema scores could have varying lung function, possibly indicating differences of disease severity. To assess this possible discrepancy, we investigated whether density distribution of "viable" lung parenchyma regions with pixel values > -910 HU correlates with lung function. A dataset of 38 subjects, who underwent both pulmonary function testing and CT examinations in a COPD SCCOR study, was assembled. After the lung regions depicted on CT images were automatically segmented by a computerized scheme, we systematically divided the lung parenchyma into different density groups (bins) and computed a number of statistical features (i.e., mean, standard deviation (STD), skewness of the pixel value distributions) in these density bins. We then analyzed the correlations between each feature and lung function. The correlation between diffusion lung capacity (DLCO) and STD of pixel values in the bin of -910HU <= PV < -750HU was -0.43, as compared with a correlation of -0.49 obtained between the post-bronchodilator ratio (FEV1/FVC) measured by the forced expiratory volume in 1 second (FEV1) dividing the forced vital capacity (FVC) and the STD of pixel values in the bin of -1024HU <= PV < -910HU. The results showed an association between the distribution of pixel values in "viable" lung parenchyma and lung function, which indicates that similar to the conventional density mask method, the pixel value distribution features in "viable" lung parenchyma areas may also provide clinically useful information to improve assessments of lung disease severity as measured by lung functional tests.

Experimental Investigation of Ultrafast Hydration Structure and Dynamics at Sub-Angstrom Lengthscales

ERIC Educational Resources Information Center

Coridan, Robert Henry

2009-01-01

This thesis outlines how meV-resolution inelastic x-ray scattering and causality-enforcing mathematics can be used to measure the dynamical density-density linear response function for liquid water with Angstrom spatial resolution and 50fs temporal resolution. The results are compared to high-resolution spectroscopic and scattering experiments and…

Adaptive Dynamics, Control, and Extinction in Networked Populations

DTIC Science & Technology

2015-07-09

network geometries. From the pre-history of paths that go extinct, a density function is created from the prehistory of these paths, and a clear local...density plots of Fig. 3b. Using the IAMM to compute the most probable path and comparing it to the prehistory of extinction events on stochastic networks

Fermi liquid, clustering, and structure factor in dilute warm nuclear matter

NASA Astrophysics Data System (ADS)

Röpke, G.; Voskresensky, D. N.; Kryukov, I. A.; Blaschke, D.

2018-02-01

Properties of nuclear systems at subsaturation densities can be obtained from different approaches. We demonstrate the use of the density autocorrelation function which is related to the isothermal compressibility and, after integration, to the equation of state. This way we connect the Landau Fermi liquid theory well elaborated in nuclear physics with the approaches to dilute nuclear matter describing cluster formation. A quantum statistical approach is presented, based on the cluster decomposition of the polarization function. The fundamental quantity to be calculated is the dynamic structure factor. Comparing with the Landau Fermi liquid theory which is reproduced in lowest approximation, the account of bound state formation and continuum correlations gives the correct low-density result as described by the second virial coefficient and by the mass action law (nuclear statistical equilibrium). Going to higher densities, the inclusion of medium effects is more involved compared with other quantum statistical approaches, but the relation to the Landau Fermi liquid theory gives a promising approach to describe not only thermodynamic but also collective excitations and non-equilibrium properties of nuclear systems in a wide region of the phase diagram.

Comparative studies of the spectroscopy of CuCl2: DFT versus standard ab initio approaches

NASA Astrophysics Data System (ADS)

Ramírez-Solís, A.; Poteau, R.; Vela, A.; Daudey, J. P.

2005-04-01

The XΠg2-Σg +2, XΠg2-Δg2, XΠg2-Σu +2, XΠg2-Πu2 transitions on CuCl2 have been studied using several exchange-correlation functionals from the various types of density functional theory (DFT) approaches like local density approximation (LDA), generalized gradient approximation (GGA), hybrid and meta-GGA. The results are compared with the experience and with those coming from the most sophisticated nondynamic and dynamic electronic correlation treatments using the same relativistic effective core potentials and especially developed basis sets to study the electronic structure of the five lowest states and the corresponding vertical and adiabatic transition energies. The calculated transition energies for three of the hybrid functionals (B3LYP, B97-2, and PBE0) are in very good agreement with the benchmark ab initio results and experimental figures. All of the other functionals largely overestimate the XΠg2-Σg +2 and XΠg2-Δg2 transition energies, many of them even placing the Δg2 ligand field state above the charge transfer Πu2 and Σu +2 states. The relative weight of the Hartree-Fock exchange in the definition of the functional used appears to play a key role in the accurate description of the ΛSΣ density defined by the orientation of the 3d hole (σ, π, or δ) on Cu in the field of both chlorine atoms, but no simple connection of this weight with the quality of the spectra has been found. Mulliken charges and spin densities are carefully analyzed; a possible link between the extent of spin density on the metal for the XΠg2 state and the performance of the various functionals was observed, suggesting that those that lead to the largest values (close to 0.65) are the ones that best reproduce these four transitions. Most functionals lead to a remarkably low ionicity for the three ligand field states even for the best performing functionals, compared to the complete active space (SCF) (21, 14) ab initio values. These findings show that not only large variational ab initio calculations can produce reliable spectroscopic results for extremely complex systems where delicate electronic correlation effects have to be carefully dealt with. However, those functionals that were recently shown to perform best for a series of molecular properties [J. Chem. Phys. 121 3405 (2004)] are not the ones that produce the best transition energies for this complex case.

Statistical properties of a filtered Poisson process with additive random noise: distributions, correlations and moment estimation

NASA Astrophysics Data System (ADS)

Theodorsen, A.; E Garcia, O.; Rypdal, M.

2017-05-01

Filtered Poisson processes are often used as reference models for intermittent fluctuations in physical systems. Such a process is here extended by adding a noise term, either as a purely additive term to the process or as a dynamical term in a stochastic differential equation. The lowest order moments, probability density function, auto-correlation function and power spectral density are derived and used to identify and compare the effects of the two different noise terms. Monte-Carlo studies of synthetic time series are used to investigate the accuracy of model parameter estimation and to identify methods for distinguishing the noise types. It is shown that the probability density function and the three lowest order moments provide accurate estimations of the model parameters, but are unable to separate the noise types. The auto-correlation function and the power spectral density also provide methods for estimating the model parameters, as well as being capable of identifying the noise type. The number of times the signal crosses a prescribed threshold level in the positive direction also promises to be able to differentiate the noise type.

Performance of the density matrix functional theory in the quantum theory of atoms in molecules.

PubMed

García-Revilla, Marco; Francisco, E; Costales, A; Martín Pendás, A

2012-02-02

The generalization to arbitrary molecular geometries of the energetic partitioning provided by the atomic virial theorem of the quantum theory of atoms in molecules (QTAIM) leads to an exact and chemically intuitive energy partitioning scheme, the interacting quantum atoms (IQA) approach, that depends on the availability of second-order reduced density matrices (2-RDMs). This work explores the performance of this approach in particular and of the QTAIM in general with approximate 2-RDMs obtained from the density matrix functional theory (DMFT), which rests on the natural expansion (natural orbitals and their corresponding occupation numbers) of the first-order reduced density matrix (1-RDM). A number of these functionals have been implemented in the promolden code and used to perform QTAIM and IQA analyses on several representative molecules and model chemical reactions. Total energies, covalent intra- and interbasin exchange-correlation interactions, as well as localization and delocalization indices have been determined with these functionals from 1-RDMs obtained at different levels of theory. Results are compared to the values computed from the exact 2-RDMs, whenever possible.

Electronic Excitations in Solution: The Interplay between State Specific Approaches and a Time-Dependent Density Functional Theory Description.

PubMed

Guido, Ciro A; Jacquemin, Denis; Adamo, Carlo; Mennucci, Benedetta

2015-12-08

We critically analyze the performances of continuum solvation models when coupled to time-dependent density functional theory (TD-DFT) to predict solvent effects on both absorption and emission energies of chromophores in solution. Different polarization schemes of the polarizable continuum model (PCM), such as linear response (LR) and three different state specific (SS) approaches, are considered and compared. We show the necessity of introducing a SS model in cases where large electron density rearrangements are involved in the excitations, such as charge-transfer transitions in both twisted and quadrupolar compounds, and underline the very delicate interplay between the selected polarization method and the chosen exchange-correlation functional. This interplay originates in the different descriptions of the transition and ground/excited state multipolar moments by the different functionals. As a result, the choice of both the DFT functional and the solvent polarization scheme has to be consistent with the nature of the studied electronic excitation.

Systematic theoretical investigation of the zero-field splitting in Gd(III) complexes: Wave function and density functional approaches

NASA Astrophysics Data System (ADS)

Khan, Shehryar; Kubica-Misztal, Aleksandra; Kruk, Danuta; Kowalewski, Jozef; Odelius, Michael

2015-01-01

The zero-field splitting (ZFS) of the electronic ground state in paramagnetic ions is a sensitive probe of the variations in the electronic and molecular structure with an impact on fields ranging from fundamental physical chemistry to medical applications. A detailed analysis of the ZFS in a series of symmetric Gd(III) complexes is presented in order to establish the applicability and accuracy of computational methods using multiconfigurational complete-active-space self-consistent field wave functions and of density functional theory calculations. The various computational schemes are then applied to larger complexes Gd(III)DOTA(H2O)-, Gd(III)DTPA(H2O)2-, and Gd(III)(H2O)83+ in order to analyze how the theoretical results compare to experimentally derived parameters. In contrast to approximations based on density functional theory, the multiconfigurational methods produce results for the ZFS of Gd(III) complexes on the correct order of magnitude.

Band structure calculations of CuAlO2, CuGaO2, CuInO2, and CuCrO2 by screened exchange

NASA Astrophysics Data System (ADS)

Gillen, Roland; Robertson, John

2011-07-01

We report density functional theory band structure calculations on the transparent conducting oxides CuAlO2, CuGaO2, CuInO2, and CuCrO2. The use of the hybrid functional screened-exchange local density approximation (sX-LDA) leads to considerably improved electronic properties compared to standard LDA and generalized gradient approximation (GGA) approaches. We show that the resulting electronic band gaps compare well with experimental values and previous quasiparticle calculations, and show the correct trends with respect to the atomic number of the cation (Al, Ga, In). The resulting energetic depths of Cu d and O p levels and the valence-band widths are considerable improvements compared to LDA and GGA and are in good agreement with available x-ray photoelectron spectroscopy data. Lastly, we show the calculated imaginary part of the dielectric function for all four systems.

Macroscopic dielectric function within time-dependent density functional theory—Real time evolution versus the Casida approach

NASA Astrophysics Data System (ADS)

Sander, Tobias; Kresse, Georg

2017-02-01

Linear optical properties can be calculated by solving the time-dependent density functional theory equations. Linearization of the equation of motion around the ground state orbitals results in the so-called Casida equation, which is formally very similar to the Bethe-Salpeter equation. Alternatively one can determine the spectral functions by applying an infinitely short electric field in time and then following the evolution of the electron orbitals and the evolution of the dipole moments. The long wavelength response function is then given by the Fourier transformation of the evolution of the dipole moments in time. In this work, we compare the results and performance of these two approaches for the projector augmented wave method. To allow for large time steps and still rely on a simple difference scheme to solve the differential equation, we correct for the errors in the frequency domain, using a simple analytic equation. In general, we find that both approaches yield virtually indistinguishable results. For standard density functionals, the time evolution approach is, with respect to the computational performance, clearly superior compared to the solution of the Casida equation. However, for functionals including nonlocal exchange, the direct solution of the Casida equation is usually much more efficient, even though it scales less beneficial with the system size. We relate this to the large computational prefactors in evaluating the nonlocal exchange, which renders the time evolution algorithm fairly inefficient.

A cumulant functional for static and dynamic correlation

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

Hollett, Joshua W., E-mail: j.hollett@uwinnipeg.ca; Department of Chemistry, University of Manitoba, Winnipeg, Manitoba R3T 2N2; Hosseini, Hessam

A functional for the cumulant energy is introduced. The functional is composed of a pair-correction and static and dynamic correlation energy components. The pair-correction and static correlation energies are functionals of the natural orbitals and the occupancy transferred between near-degenerate orbital pairs, rather than the orbital occupancies themselves. The dynamic correlation energy is a functional of the statically correlated on-top two-electron density. The on-top density functional used in this study is the well-known Colle-Salvetti functional. Using the cc-pVTZ basis set, the functional effectively models the bond dissociation of H{sub 2}, LiH, and N{sub 2} with equilibrium bond lengths and dissociationmore » energies comparable to those provided by multireference second-order perturbation theory. The performance of the cumulant functional is less impressive for HF and F{sub 2}, mainly due to an underestimation of the dynamic correlation energy by the Colle-Salvetti functional.« less

Electrostatics of DNA-Functionalized Nanoparticles

NASA Astrophysics Data System (ADS)

Hoffmann, Kyle; Krishnamoorthy, Kurinji; Kewalramani, Sumit; Bedzyk, Michael; Olvera de La Cruz, Monica

DNA-functionalized nanoparticles have applications in directed self-assembly and targeted cellular delivery of therapeutic proteins. In order to design specific systems, it is necessary to understand their self-assembly properties, of which the long-range electrostatic interactions are a critical component. We iteratively solved equations derived from classical density functional theory in order to predict the distribution of ions around DNA-functionalized Cg Catalase. We then compared estimates of the resonant intensity to those from SAXS measurements to estimate key features of DNA-functionalized proteins, such as the size of the region linking the protein and DNA and the extension of the single-stranded DNA. Using classical density functional theory and coarse-grained simulations, we are able to predict and understand these fundamental properties in order to rationally design new biomaterials.

[Effects of canopy density on the functional group of soil macro fauna in Pinus massoniana plantations].

PubMed

Zhou, Hong Yang; Zhang, Dan Ju; Zhang, Jie; Zhao, Yan Bo; Zhao, Bo; Wei, Da Ping; Zhang, Jian

2017-06-18

In order to understand the effects of canopy density on the functional group characteristics of soil macrofauna in Pinus massoniana plantations, we divided the captured soil fauna into five types including xylophages, predators, saprophages, omnivores and fungal feeders. The results showed that 1) Saprozoic feeders had the highest percentage of total individuals, and the omnivores and xylophages occupied higher percentages of total taxa. 2) The individual and group number of the predators, and the group number of xylophages did not change significantly under 0.5-0.6 and then decreased significantly under 0.6-0.9 canopy density. 3) With the increasing canopy density, the individual an dgroup number of predators in litter layer decreased significantly, the saprozoic individual number in 5-10 cm soil layer represented irregular trends. The individual number of xylophage increased with the depth of soil, and the group number in litter layer, the individual and group number in 5-10 cm soil layer decreased significantly. 4) Pielou evenness of xylophage had no significant changes with the canopy density, all the other diversity index of xylophage and saprophage were various with the increasing canopy density. The predatory Simpson index was stable under 0.5-0.8, and then decreased significantly under 0.8-0.9 canopy density. 5) The CCA (canonical correlation analysis) indicated that soil bulk density and moisture content were the main environmental factors affecting functional groups of soil macro fauna. Moisture content greatly impacted on the number of saprophagous individuals. But xylophage and predators were mostly affected by soil bulk density, and the predatory Simpson index was mainly affected by soil pH value and total phosphorus. Our research indicated that the structure of soil macro faunal functional group under 0.7 canopy density was comparatively stable, which would facilitate the maintenance of soil fertility and ecological function in Pinus massoniana plantation.

The effect of different π-bridge configuration on bi-anchored triphenylamine and phenyl modified triphenylamine based dyes for dye sensitized solar cell (DSSC) application: A theoretical approach.

PubMed

Pounraj, P; Mohankumar, V; Pandian, M Senthil; Ramasamy, P

2018-01-01

Twenty eight bi-anchored triphenylamine (TH-1 to TH-14) and phenyl modified triphenylamine (PH-TH-1 to PH-TH-14) based metal free organic dyes are designed for DSSC application. The electronic effect of different π-bridge configurations in donor-π-bridge-acceptor (D-π-A) 2 structure was theoretically simulated and verified using density functional theory (DFT) and time dependent density functional theory (TD-DFT). The triphenylamine and phenyl modified triphenylamine groups are used as donor and cyanoacrylic acid group is used as acceptor. Thiophene and cyanovinyl groups are used as π-bridge. The ground state molecular structure was optimized by density functional theory and the electronic absorption spectra were calculated by time dependent density functional theory. The light harvesting efficiency (LHE), dye regeneration energy (ΔG reg ) and electron injection energy (ΔG inject ) are determined by computational examination. It is observed that, when the number of π-bridge increases, the band gap of the dye decreases. Also the absorption maximum and molar extinction coefficient of the dyes are increased. Theoretical result shows that the thiophene-cyanovinyl and thiophene-thiophene-cyanovinyl-cyanovinyl configurations give broader and red shifted absorption spectrum compared to other configurations. Also the results of phenyl modified triphenylamine (PH-TH) dyes clearly show better absorption and dye regeneration energy compared to TH dyes. Copyright © 2017 Elsevier Inc. All rights reserved.

Angle-dependent strong-field molecular ionization rates with tuned range-separated time-dependent density functional theory.

PubMed

Sissay, Adonay; Abanador, Paul; Mauger, François; Gaarde, Mette; Schafer, Kenneth J; Lopata, Kenneth

2016-09-07

Strong-field ionization and the resulting electronic dynamics are important for a range of processes such as high harmonic generation, photodamage, charge resonance enhanced ionization, and ionization-triggered charge migration. Modeling ionization dynamics in molecular systems from first-principles can be challenging due to the large spatial extent of the wavefunction which stresses the accuracy of basis sets, and the intense fields which require non-perturbative time-dependent electronic structure methods. In this paper, we develop a time-dependent density functional theory approach which uses a Gaussian-type orbital (GTO) basis set to capture strong-field ionization rates and dynamics in atoms and small molecules. This involves propagating the electronic density matrix in time with a time-dependent laser potential and a spatial non-Hermitian complex absorbing potential which is projected onto an atom-centered basis set to remove ionized charge from the simulation. For the density functional theory (DFT) functional we use a tuned range-separated functional LC-PBE*, which has the correct asymptotic 1/r form of the potential and a reduced delocalization error compared to traditional DFT functionals. Ionization rates are computed for hydrogen, molecular nitrogen, and iodoacetylene under various field frequencies, intensities, and polarizations (angle-dependent ionization), and the results are shown to quantitatively agree with time-dependent Schrödinger equation and strong-field approximation calculations. This tuned DFT with GTO method opens the door to predictive all-electron time-dependent density functional theory simulations of ionization and ionization-triggered dynamics in molecular systems using tuned range-separated hybrid functionals.

Angle-dependent strong-field molecular ionization rates with tuned range-separated time-dependent density functional theory

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

Sissay, Adonay; Abanador, Paul; Mauger, François

2016-09-07

Strong-field ionization and the resulting electronic dynamics are important for a range of processes such as high harmonic generation, photodamage, charge resonance enhanced ionization, and ionization-triggered charge migration. Modeling ionization dynamics in molecular systems from first-principles can be challenging due to the large spatial extent of the wavefunction which stresses the accuracy of basis sets, and the intense fields which require non-perturbative time-dependent electronic structure methods. In this paper, we develop a time-dependent density functional theory approach which uses a Gaussian-type orbital (GTO) basis set to capture strong-field ionization rates and dynamics in atoms and small molecules. This involves propagatingmore » the electronic density matrix in time with a time-dependent laser potential and a spatial non-Hermitian complex absorbing potential which is projected onto an atom-centered basis set to remove ionized charge from the simulation. For the density functional theory (DFT) functional we use a tuned range-separated functional LC-PBE*, which has the correct asymptotic 1/r form of the potential and a reduced delocalization error compared to traditional DFT functionals. Ionization rates are computed for hydrogen, molecular nitrogen, and iodoacetylene under various field frequencies, intensities, and polarizations (angle-dependent ionization), and the results are shown to quantitatively agree with time-dependent Schrödinger equation and strong-field approximation calculations. This tuned DFT with GTO method opens the door to predictive all-electron time-dependent density functional theory simulations of ionization and ionization-triggered dynamics in molecular systems using tuned range-separated hybrid functionals.« less

Calculation of phonon dispersion relation using new correlation functional

NASA Astrophysics Data System (ADS)

Jitropas, Ukrit; Hsu, Chung-Hao

2017-06-01

To extend the use of Local Density Approximation (LDA), a new analytical correlation functional is introduced. Correlation energy is an essential ingredient within density functional theory and used to determine ground state energy and other properties including phonon dispersion relation. Except for high and low density limit, the general expression of correlation energy is unknown. The approximation approach is therefore required. The accuracy of the modelling system depends on the quality of correlation energy approximation. Typical correlation functionals used in LDA such as Vosko-Wilk-Nusair (VWN) and Perdew-Wang (PW) were obtained from parameterizing the near-exact quantum Monte Carlo data of Ceperley and Alder. These functionals are presented in complex form and inconvenient to implement. Alternatively, the latest published formula of Chachiyo correlation functional provides a comparable result for those much more complicated functionals. In addition, it provides more predictive power based on the first principle approach, not fitting functionals. Nevertheless, the performance of Chachiyo formula for calculating phonon dispersion relation (a key to the thermal properties of materials) has not been tested yet. Here, the implementation of new correlation functional to calculate phonon dispersion relation is initiated. The accuracy and its validity will be explored.

Determination of the nuclear level densities and radiative strength function for 43 nuclei in the mass interval 28≤A≤200

NASA Astrophysics Data System (ADS)

Knezevic, David; Jovancevic, Nikola; Sukhovoj, Anatoly M.; Mitsyna, Ludmila V.; Krmar, Miodrag; Cong, Vu D.; Hambsch, Franz-Josef; Oberstedt, Stephan; Revay, Zsolt; Stieghorst, Christian; Dragic, Aleksandar

2018-03-01

The determination of nuclear level densities and radiative strength functions is one of the most important tasks in low-energy nuclear physics. Accurate experimental values of these parameters are critical for the study of the fundamental properties of nuclear structure. The step-like structure in the dependence of the level densities p on the excitation energy of nuclei Eex is observed in the two-step gamma cascade measurements for nuclei in the 28 ≤ A ≤ 200 mass region. This characteristic structure can be explained only if a co-existence of quasi-particles and phonons, as well as their interaction in a nucleus, are taken into account in the process of gamma-decay. Here we present a new improvement to the Dubna practical model for the determination of nuclear level densities and radiative strength functions. The new practical model guarantees a good description of the available intensities of the two step gamma cascades, comparable to the experimental data accuracy.

Atomic density functional and diagram of structures in the phase field crystal model

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

Ankudinov, V. E., E-mail: vladimir@ankudinov.org; Galenko, P. K.; Kropotin, N. V.

2016-02-15

The phase field crystal model provides a continual description of the atomic density over the diffusion time of reactions. We consider a homogeneous structure (liquid) and a perfect periodic crystal, which are constructed from the one-mode approximation of the phase field crystal model. A diagram of 2D structures is constructed from the analytic solutions of the model using atomic density functionals. The diagram predicts equilibrium atomic configurations for transitions from the metastable state and includes the domains of existence of homogeneous, triangular, and striped structures corresponding to a liquid, a body-centered cubic crystal, and a longitudinal cross section of cylindricalmore » tubes. The method developed here is employed for constructing the diagram for the homogeneous liquid phase and the body-centered iron lattice. The expression for the free energy is derived analytically from density functional theory. The specific features of approximating the phase field crystal model are compared with the approximations and conclusions of the weak crystallization and 2D melting theories.« less

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.

The Radial Distribution Function (RDF) of Amorphous Selenium Obtained through the Vacuum Evaporator

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

Guda, Bardhyl; Dede, Marie

2010-01-21

After the amorphous selenium obtained through the vacuum evaporator, the relevant diffraction intensity is taken and its processing is made. Further on the interferential function is calculated and the radial density function is defined. For determining these functions are used two methods, which were compared with each other and finally are received results for amorphous selenium RDF.

Differences in ecological structure, function, and native species abundance between native and invaded Hawaiian streams.

PubMed

Holitzki, Tara M; MacKenzie, Richard A; Wiegner, Tracy N; McDermid, Karla J

2013-09-01

Poeciliids, one of the most invasive species worldwide, are found on almost every continent and have been identified as an "invasive species of concern" in the United States, New Zealand, and Australia. Despite their global prevalence, few studies have quantified their impacts on tropical stream ecosystem structure, function, and biodiversity. Utilizing Hawaiian streams as model ecosystems, we documented how ecological structure, function, and native species abundance differed between poeciliid-free and poeciliid-invaded tropical streams. Stream nutrient yields, benthic biofilm biomass, densities of macroinvertebrates and fish, and community structures of benthic algae, macroinvertebrates, and fish were compared between streams with and without established poeciliid populations on the island of Hawai'i, Hawaii, USA. Sum nitrate (sigmaNO3(-) = NO3(-) + NO2(-)), total nitrogen, and total organic carbon yields were eight times, six times, and five times higher, respectively, in poeciliid streams than in poeciliid-free streams. Benthic biofilm ash-free dry mass was 1.5x higher in poeciliid streams than in poeciliid-free streams. Percentage contributions of chironomids and hydroptilid caddisflies to macroinvertebrate densities were lower in poeciliid streams compared to poeciliid-free streams, while percentage contributions of Cheumatopsyche analis caddisflies, Dugesia sp. flatworms, and oligochaetes were higher. Additionally, mean densities of native gobies were two times lower in poeciliid streams than in poeciliid-free ones, with poeciliid densities being approximately eight times higher than native fish densities. Our results, coupled with the wide distribution of invasive poeciliids across Hawaii and elsewhere in the tropics, suggest that poeciliids may negatively impact the ecosystem structure, function, and native species abundance of tropical streams they invade. This underscores the need for increased public awareness to prevent future introductions and for developing and implementing effective eradication and restoration strategies.

Efficiency of Cs-free materials for negative ion production in H2 and D2 plasmas

NASA Astrophysics Data System (ADS)

Friedl, R.; Kurutz, U.; Fantz, U.

2017-08-01

High power negative ion sources use caesium to reduce the work function of the converter surface which significantly increases the negative ion yield. Caesium, however, is a very reactive alkali-metal and shows complex redistribution dynamics in consequence of plasma-surface-interaction. Thus, maintaining a stable and homogenous low work function surface is a demanding task, which is not easily compatible with the RAMI issues (reliability, availability, maintainability, inspectability) for a future DEMO fusion reactor. Hence, Cs-free alternative materials for efficient negative ion formation are desirable. At the laboratory experiment HOMER materials which are referred to as promising are investigated under identical and ion source relevant parameters: the refractory metals Ta and W, non-doped and boron-doped diamond as well as materials with inherent low work function (lanthanum-doped molybdenum, MoLa and lanthanum hexaboride, LaB6). The results are compared to the effect of in-situ caesiation, which at HOMER leads to a maximal increase of the negative ion density by a factor of 2.5. Among the examined samples low work function materials are most efficient. In particular, MoLa leads to an increase of almost 50 % compared to pure volume formation. The difference to a caesiated surface can be attributed to the still higher work function of MoLa, which is expected to be slightly below 3 eV. Using deuterium instead of hydrogen leads to increased atomic and positive ion densities, while comparable negative ion densities are achieved. In contrast to the low work function materials, bulk samples of the refractory metals as well as carbon based materials have no enhancing effect on H-, where the latter materials furthermore show severe erosion due to the hydrogen plasma.

Effect of whole body vibration training on quadriceps strength, bone mineral density, and functional capacity in children with hemophilia: a randomized clinical trial.

PubMed

El-Shamy, S

2017-06-01

The objective was to evaluate the effects of whole body vibration training on quadriceps strength, bone mineral density, and functional capacity in children with hemophilia. Thirty children with hemophilia with age ranging from 9 to 13 years were selected and randomly assigned to either the study group that received whole body vibration training (30-40 Hz, 2-4 mm of peak-to-peak vertical plate displacement for 15 minutes/day, 3 days/week/ 12 weeks) plus the conventional physical therapy program or the control group that performed a conventional physical therapy program only. Outcomes included quadriceps strength, bone mineral density, and the functional capacity. Children in the study group showed a significant improvement in all outcomes compared with the control group. The quadriceps peak torque after treatment was 70.26 and 56.46 Nm for the study and control group, respectively (p⟨0.001). The lumbar spine bone mineral density after treatment was 0.85 and 0.72 g/cm 2 for the study and control group, respectively (p⟨0.001). The functional capacity after treatment was 325 and 290 m for the study and control group, respectively (p=0.006). Whole body vibration training is an effective modality in increasing quadriceps strength, bone mineral density, and functional capacity in children with hemophilia.

The role of relativity in the optical response of gold within the time-dependent current-density-functional theory.

PubMed

Romaniello, P; de Boeij, P L

2005-04-22

We included relativistic effects in the formulation of the time-dependent current-density-functional theory for the calculation of linear response properties of metals [P. Romaniello and P. L. de Boeij, Phys. Rev. B (to be published)]. We treat the dominant scalar-relativistic effects using the zeroth-order regular approximation in the ground-state density-functional theory calculations, as well as in the time-dependent response calculations. The results for the dielectric function of gold calculated in the spectral range of 0-10 eV are compared with experimental data reported in literature and recent ellipsometric measurements. As well known, relativistic effects strongly influence the color of gold. We find that the onset of interband transitions is shifted from around 3.5 eV, obtained in a nonrelativistic calculation, to around 1.9 eV when relativity is included. With the inclusion of the scalar-relativistic effects there is an overall improvement of both real and imaginary parts of the dielectric function over the nonrelativistic ones. Nevertheless some important features in the absorption spectrum are not well reproduced, but can be explained in terms of spin-orbit coupling effects. The remaining deviations are attributed to the underestimation of the interband gap (5d-6sp band gap) in the local-density approximation and to the use of the adiabatic local-density approximation in the response calculation.

Applications of Density Functional Theory in Soft Condensed Matter

NASA Astrophysics Data System (ADS)

Löwen, Hartmut

Applications of classical density functional theory (DFT) to soft matter systems like colloids, liquid crystals and polymer solutions are discussed with a focus on the freezing transition and on nonequilibrium Brownian dynamics. First, after a brief reminder of equilibrium density functional theory, DFT is applied to the freezing transition of liquids into crystalline lattices. In particular, spherical particles with radially symmetric pair potentials will be treated (like hard spheres, the classical one-component plasma or Gaussian-core particles). Second, the DFT will be generalized towards Brownian dynamics in order to tackle nonequilibrium problems. After a general introduction to Brownian dynamics using the complementary Smoluchowski and Langevin pictures appropriate for the dynamics of colloidal suspensions, the dynamical density functional theory (DDFT) will be derived from the Smoluchowski equation. This will be done first for spherical particles (e.g. hard spheres or Gaussian-cores) without hydrodynamic interactions. Then we show how to incorporate hydrodynamic interactions between the colloidal particles into the DDFT framework and compare to Brownian dynamics computer simulations. Third orientational degrees of freedom (rod-like particles) will be considered as well. In the latter case, the stability of intermediate liquid crystalline phases (isotropic, nematic, smectic-A, plastic crystals etc) can be predicted. Finally, the corresponding dynamical extension of density functional theory towards orientational degrees of freedom is proposed and the collective behaviour of "active" (self-propelled) Brownian particles is briefly discussed.

Effect of whole body vibration training on quadriceps strength, bone mineral density, and functional capacity in children with hemophilia: a randomized clinical trial

PubMed Central

El-Shamy, S.

2017-01-01

Objectives: The objective was to evaluate the effects of whole body vibration training on quadriceps strength, bone mineral density, and functional capacity in children with hemophilia. Methods: Thirty children with hemophilia with age ranging from 9 to 13 years were selected and randomly assigned to either the study group that received whole body vibration training (30-40 Hz, 2-4 mm of peak-to-peak vertical plate displacement for 15 minutes/day, 3 days/week/ 12 weeks) plus the conventional physical therapy program or the control group that performed a conventional physical therapy program only. Outcomes included quadriceps strength, bone mineral density, and the functional capacity. Results: Children in the study group showed a significant improvement in all outcomes compared with the control group. The quadriceps peak torque after treatment was 70.26 and 56.46 Nm for the study and control group, respectively (p<0.001). The lumbar spine bone mineral density after treatment was 0.85 and 0.72 g/cm2 for the study and control group, respectively (p<0.001). The functional capacity after treatment was 325 and 290 m for the study and control group, respectively (p=0.006). Conclusions: Whole body vibration training is an effective modality in increasing quadriceps strength, bone mineral density, and functional capacity in children with hemophilia. PMID:28574408

HIGH STAR FORMATION RATES IN TURBULENT ATOMIC-DOMINATED GAS IN THE INTERACTING GALAXIES IC 2163 AND NGC 2207

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

Elmegreen, Bruce G.; Kaufman, Michele; Bournaud, Frédéric

CO observations of the interacting galaxies IC 2163 and NGC 2207 are combined with HI, H α , and 24 μ m observations to study the star formation rate (SFR) surface density as a function of the gas surface density. More than half of the high-SFR regions are HI dominated. When compared to other galaxies, these HI-dominated regions have excess SFRs relative to their molecular gas surface densities but normal SFRs relative to their total gas surface densities. The HI-dominated regions are mostly located in the outer part of NGC 2207 where the HI velocity dispersion is high, 40–50 kmmore » s{sup −1}. We suggest that the star-forming clouds in these regions have envelopes at lower densities than normal, making them predominantly atomic, and cores at higher densities than normal because of the high turbulent Mach numbers. This is consistent with theoretical predictions of a flattening in the density probability distribution function for compressive, high Mach number turbulence.« less

Bragg-cell receiver study

NASA Technical Reports Server (NTRS)

Wilson, Lonnie A.

1987-01-01

Bragg-cell receivers are employed in specialized Electronic Warfare (EW) applications for the measurement of frequency. Bragg-cell receiver characteristics are fully characterized for simple RF emitter signals. This receiver is early in its development cycle when compared to the IFM receiver. Functional mathematical models are derived and presented in this report for the Bragg-cell receiver. Theoretical analysis is presented and digital computer signal processing results are presented for the Bragg-cell receiver. Probability density function analysis are performed for output frequency. Probability density function distributions are observed to depart from assumed distributions for wideband and complex RF signals. This analysis is significant for high resolution and fine grain EW Bragg-cell receiver systems.

Nonrelativistic approaches derived from point-coupling relativistic models

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

Lourenco, O.; Dutra, M.; Delfino, A.

2010-03-15

We construct nonrelativistic versions of relativistic nonlinear hadronic point-coupling models, based on new normalized spinor wave functions after small component reduction. These expansions give us energy density functionals that can be compared to their relativistic counterparts. We show that the agreement between the nonrelativistic limit approach and the Skyrme parametrizations becomes strongly dependent on the incompressibility of each model. We also show that the particular case A=B=0 (Walecka model) leads to the same energy density functional of the Skyrme parametrizations SV and ZR2, while the truncation scheme, up to order {rho}{sup 3}, leads to parametrizations for which {sigma}=1.

Improved First Pass Spiral Myocardial Perfusion Imaging with Variable Density Trajectories

PubMed Central

Salerno, Michael; Sica, Christopher; Kramer, Christopher M.; Meyer, Craig H.

2013-01-01

Purpose To develop and evaluate variable-density (VD) spiral first-pass perfusion pulse sequences for improved efficiency and off-resonance performance and to demonstrate the utility of an apodizing density compensation function (DCF) to improve SNR and reduce dark-rim artifact caused by cardiac motion and Gibbs Ringing. Methods Three variable density spiral trajectories were designed, simulated, and evaluated in 18 normal subjects, and in 8 patients with cardiac pathology on a 1.5T scanner. Results By utilizing a density compensation function (DCF) which intentionally apodizes the k-space data, the side-lobe amplitude of the theoretical PSF is reduced by 68%, with only a 13% increase in the FWHM of the main-lobe as compared to the same data corrected with a conventional VD DCF, and has an 8% higher resolution than a uniform density spiral with the same number of interleaves and readout duration. Furthermore, this strategy results in a greater than 60% increase in measured SNR as compared to the same VD spiral data corrected with a conventional DCF (p<0.01). Perfusion defects could be clearly visualized with minimal off-resonance and dark-rim artifacts. Conclusion VD spiral pulse sequences using an apodized DCF produce high-quality first-pass perfusion images with minimal dark-rim and off-resonance artifacts, high SNR and CNR and good delineation of resting perfusion abnormalities. PMID:23280884

The exact solution of the monoenergetic transport equation for critical cylinders

NASA Technical Reports Server (NTRS)

Westfall, R. M.; Metcalf, D. R.

1972-01-01

An analytic solution for the critical, monoenergetic, bare, infinite cylinder is presented. The solution is obtained by modifying a previous development based on a neutron density transform and Case's singular eigenfunction method. Numerical results for critical radii and the neutron density as a function of position are included and compared with the results of other methods.

Influence of the Level Density Parametrization on the Effective GDR Width at High Spins

NASA Astrophysics Data System (ADS)

Mazurek, K.; Matejska, M.; Kmiecik, M.; Maj, A.; Dudek, J.

Parameterizations of the nucleonic level densities are tested by computing the effective GDR strength-functions and GDR widths at high spins. Calculations are based on the thermal shape fluctuation method with the Lublin-Strasbourg Drop (LSD) model. Results for 106Sn, 147Eu, 176W, 194Hg are compared to the experimental data.

Association between nailfold capillaroscopy findings and pulmonary function tests in patients with systemic sclerosis.

PubMed

Castellví, Ivan; Simeón-Aznar, Carmen Pilar; Sarmiento, Mónica; Fortuna, Ana; Mayos, Mercedes; Geli, Carme; Diaz-Torné, César; Moya, Patricia; De Llobet, Josep Maria; Casademont, Jordi

2015-02-01

To determine whether there is an association between different capillaroscopic findings and pulmonary function tests in systemic sclerosis (SSc). We did a retrospective observational study in a cohort of patients with SSc and early SSc. Patients with at least 1 nailfold videocapillaroscopy (NVC) magnified 120× were included. Pathological findings were giant capillaries, angiogenesis, and density loss. Findings were compared with lung function values: percent expected value of forced vital capacity (FVC), DLCO, and FVC/DLCO ratio. Other variables collected were sex and SSc type, and the presence of digital ulcers (DU), interstitial lung disease (ILD), scleroderma renal crisis, and/or pulmonary hypertension (PH). Of 136 patients with SSc, 85 had undergone an NVC. The frequency of ILD, DU, and PH was 24.1%, 28.7%, and 17.2%, respectively. Data analysis showed that patients with density loss had worse FVC% (86.91 ± 19.42 vs 101.13 ± 16.06, p < 0.01) and DLCO% (71.43 ± 21.19 vs 85.9 ± 19.81, p < 0.01) compared to those without. Patients with loss of density present worse FVC and DLCO values. Prospective studies are warranted to determine whether NVC is useful for studying pulmonary function in SSc.

Comparative Analysis of the Clinical Significance of Oscillatory Components in the Rhythmic Structure of Pulse Signal in the Diagnostics of Psychosomatic Disorders in School Age Children.

PubMed

Desova, A A; Dorofeyuk, A A; Anokhin, A M

2017-01-01

We performed a comparative analysis of the types of spectral density typical of various parameters of pulse signal. The experimental material was obtained during the examination of school age children with various psychosomatic disorders. We also performed a typological analysis of the spectral density functions corresponding to the time series of different parameters of a single oscillation of pulse signals; the results of their comparative analysis are presented. We determined the most significant spectral components for two disordersin children: arterial hypertension and mitral valve prolapse.

Effect of stretching on the ballistic conductance of Au nanocontacts in presence of CO: A density functional study

NASA Astrophysics Data System (ADS)

Sclauzero, Gabriele; Dal Corso, Andrea; Smogunov, Alexander

2012-04-01

CO adsorption on an Au monatomic chain is studied within density functional theory in nanocontact geometries as a function of the contact stretching. We compare the bridge and atop adsorption sites of CO, finding that the bridge site is energetically favored at all strains studied here. Atop adsorption gives rise to an almost complete suppression of the ballistic conductance of the nanocontact, while adsorption at the bridge site results in a conductance value close to 0.6G0, in agreement with previous experimental data. We show that only the bridge site can qualitatively account for the evolution of the conductance as a function of the contact stretching observed in the experimental conductance traces. The numerical discrepancy between the theoretical and experimental conductance slopes is rationalized through a simple model for the elastic response of the metallic leads. We also verify that our conductance values are not affected by the specific choice of the nanocontact geometry by comparing two different atomistic models for the tips.

A comparison of non-local electron transport models for laser-plasmas relevant to inertial confinement fusion

DOE PAGES

Sherlock, M.; Brodrick, J. P.; Ridgers, C. P.

2017-08-08

Here, we compare the reduced non-local electron transport model developed to Vlasov-Fokker-Planck simulations. Two new test cases are considered: the propagation of a heat wave through a high density region into a lower density gas, and a one-dimensional hohlraum ablation problem. We find that the reduced model reproduces the peak heat flux well in the ablation region but significantly over-predicts the coronal preheat. The suitability of the reduced model for computing non-local transport effects other than thermal conductivity is considered by comparing the computed distribution function to the Vlasov-Fokker-Planck distribution function. It is shown that even when the reduced modelmore » reproduces the correct heat flux, the distribution function is significantly different to the Vlasov-Fokker-Planck prediction. Two simple modifications are considered which improve agreement between models in the coronal region.« less

On the equilibrium charge density at tilt grain boundaries

NASA Astrophysics Data System (ADS)

Srikant, V.; Clarke, D. R.

1998-05-01

The equilibrium charge density and free energy of tilt grain boundaries as a function of their misorientation is computed using a Monte Carlo simulation that takes into account both the electrostatic and configurational energies associated with charges at the grain boundary. The computed equilibrium charge density increases with the grain-boundary angle and approaches a saturation value. The equilibrium charge density at large-angle grain boundaries compares well with experimental values for large-angle tilt boundaries in GaAs. The computed grain-boundary electrostatic energy is in agreement with the analytical solution to a one-dimensional Poisson equation at high donor densities but indicates that the analytical solution overestimates the electrostatic energy at lower donor densities.

The Role of Resource Density on Energy Allocation in the Neotropical Termite Nasutitermes aff. coxipoensis (Termitidae: Nasutitermitinae).

PubMed

Cristaldo, P F; Almeida, C S; Cruz, N G; Ribeiro, E J M; Rocha, M L C; Santos, A A; Santana, A S; Araújo, A P A

2018-06-01

Organisms acquire energy from environment and must allocate it among different life traits (growth, maintenance and reproduction). Social insects must manage the energy allocation to various levels such as colony growth and caste functions. Here, we addressed the question of whether resource density affects the energy allocation to the number of individuals and caste functions as well as nest's growth rate in the Neotropical termite Nasutitermes aff. coxipoensis (Homgren) (Termitidae: Nasutitermitinae). In a manipulative field experiment, colonies of N. aff. coxipoensis, with known volume, were maintained in plots with three different resource's density (0.32, 0.64 and 1.92 baits/m 2 ) over 3 months. After this period, the number of individuals as well as the caste identity and nest volume were measured. Surprisingly, our results showed that colonies reared in the extremes of resource's density (0.32 and 1.92 baits/m 2 ) produced a higher number of individuals compared with colonies reared with intermediate resource density (0. 64 baits/m 2 ). The mean number of workers increased linearly with resource density; however, the average number of immature was higher in colonies reared with 0.32 baits/m 2 compared with colonies reared with 0.64 and 1.92 baits/m 2 . No significant differences of resource density were observed in the mean number of soldiers, worker/soldier ratio as well as in the nest's growth rate. In conclusion, the resource's density seems to play an important role in determining the investment of energy in the number of individuals and caste in N. aff. coxipoensis colonies.

Changes in Structure and Functioning of Protist (Testate Amoebae) Communities Due to Conversion of Lowland Rainforest into Rubber and Oil Palm Plantations.

PubMed

Krashevska, Valentyna; Klarner, Bernhard; Widyastuti, Rahayu; Maraun, Mark; Scheu, Stefan

2016-01-01

Large areas of tropical rainforest are being converted to agricultural and plantation land uses, but little is known of biodiversity and ecological functioning under these replacement land uses. We investigated the effects of conversion of rainforest into jungle rubber, intensive rubber and oil palm plantations on testate amoebae, diverse and functionally important protists in litter and soil. Living testate amoebae species richness, density and biomass were all lower in replacement land uses than in rainforest, with the impact being more pronounced in litter than in soil. Similar abundances of species of high and low trophic level in rainforest suggest that trophic interactions are more balanced, with a high number of functionally redundant species, than in rubber and oil palm. In contrast, plantations had a low density of high trophic level species indicating losses of functions. This was particularly so in oil palm plantations. In addition, the relative density of species with siliceous shells was >50% lower in the litter layer of oil palm and rubber compared to rainforest and jungle rubber. This difference suggests that rainforest conversion changes biogenic silicon pools and increases silicon losses. Overall, the lower species richness, density and biomass in plantations than in rainforest, and the changes in the functional composition of the testate amoebae community, indicate detrimental effects of rainforest conversion on the structure and functioning of microbial food webs.

Spectral Discrete Probability Density Function of Measured Wind Turbine Noise in the Far Field

PubMed Central

Ashtiani, Payam; Denison, Adelaide

2015-01-01

Of interest is the spectral character of wind turbine noise at typical residential set-back distances. In this paper, a spectral statistical analysis has been applied to immission measurements conducted at three locations. This method provides discrete probability density functions for the Turbine ONLY component of the measured noise. This analysis is completed for one-third octave sound levels, at integer wind speeds, and is compared to existing metrics for measuring acoustic comfort as well as previous discussions on low-frequency noise sources. PMID:25905097

Germanium multiphase equation of state

DOE PAGES

Crockett, Scott D.; Lorenzi-Venneri, Giulia De; Kress, Joel D.; ...

2014-05-07

A new SESAME multiphase germanium equation of state (EOS) has been developed using the best available experimental data and density functional theory (DFT) calculations. The equilibrium EOS includes the Ge I (diamond), the Ge II (β-Sn) and the liquid phases. The foundation of the EOS is based on density functional theory calculations which are used to determine the cold curve and the Debye temperature. Results are compared to Hugoniot data through the solid-solid and solid-liquid transitions. We propose some experiments to better understand the dynamics of this element

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.

In Search of Sleep Biomarkers of Alzheimer’s Disease: K-Complexes Do Not Discriminate between Patients with Mild Cognitive Impairment and Healthy Controls

PubMed Central

Reda, Flaminia; Gorgoni, Maurizio; Lauri, Giulia; Truglia, Ilaria; Cordone, Susanna; Scarpelli, Serena; Mangiaruga, Anastasia; D’Atri, Aurora; Ferrara, Michele; Lacidogna, Giordano; Marra, Camillo; Rossini, Paolo Maria; De Gennaro, Luigi

2017-01-01

The K-complex (KC) is one of the hallmarks of Non-Rapid Eye Movement (NREM) sleep. Recent observations point to a drastic decrease of spontaneous KCs in Alzheimer’s disease (AD). However, no study has investigated when, in the development of AD, this phenomenon starts. The assessment of KC density in mild cognitive impairment (MCI), a clinical condition considered a possible transitional stage between normal cognitive function and probable AD, is still lacking. The aim of the present study was to compare KC density in AD/MCI patients and healthy controls (HCs), also assessing the relationship between KC density and cognitive decline. Twenty amnesic MCI patients underwent a polysomnographic recording of a nocturnal sleep. Their data were compared to those of previously recorded 20 HCs and 20 AD patients. KCs during stage 2 NREM sleep were visually identified and KC densities of the three groups were compared. AD patients showed a significant KC density decrease compared with MCI patients and HCs, while no differences were observed between MCI patients and HCs. KC density was positively correlated with Mini-Mental State Examination (MMSE) scores. Our results point to the existence of an alteration of KC density only in a full-blown phase of AD, which was not observable in the early stage of the pathology (MCI), but linked with cognitive deterioration. PMID:28468235

Density- and luminosity-functions for UBV-photometric discand halo-stars in SA 54, compared with earlier RGU-results in this field

NASA Astrophysics Data System (ADS)

Fenkart, R.; Esin-Yilmaz, F.

1983-12-01

Space density- and luminosity-functions for the photometric halo- and disc-populations in the test-field SA 54 of the Basle Halo Program have been derived on the basis of UBV observations of the same 1377 stars used already for the corresponding RGU investigation by Fenkart (1968). The statistical method for separating the photometrically defined populations and for attributing absolute magnitudes to their members developed, described and first applied to SA 51 in RGU by Becker (1965) has been adapted for use in the UBV system. The (U-B, B- V) diagrams for consecutive intervals in apparent V-magnitude of figures 2a to f contain, contrary to what was first expected in this system, substantial numbers of stars in the < blanketing-region above and to the right of the late branch of the two-colour diagram main-sequence. The density-functions for different MVintervals within the overall interval < 3m, 7m> covered by this investigation for halo and disc are given in tables IIa and b, and plotted in figures 3 and 4, respectively. The corresponding luminosity-functions within the partial volume up to 1 kpc from the sun over the same overall MVinterval are given together with Glieses (1969) solar values for population I, in table III, and plotted in figure 5. The overall density-functions (3m ≦ MV ≦ 7m) for both populations can be and are compared with the corresponding ones (3m ≦ MG ≦ 8m) in RGU (last column in table II) in figures 6 and 7, for halo and disc, respectively. The coincidence of the density results between UBV and RGU is much better for both populations than the mean misidentification rate per system derived in section 5 would let us expect, suggesting a statistically fairly repartition of the misidentifications with respect to absolute magnitudes and distances.

Density Functional Theory Calculations of the Quantum Capacitance of Graphene Oxide as a Supercapacitor Electrode.

PubMed

Song, Ce; Wang, Jinyan; Meng, Zhaoliang; Hu, Fangyuan; Jian, Xigao

2018-03-31

Graphene oxide has become an attractive electrode-material candidate for supercapacitors thanks to its higher specific capacitance compared to graphene. The quantum capacitance makes relative contributions to the specific capacitance, which is considered as the major limitation of graphene electrodes, while the quantum capacitance of graphene oxide is rarely concerned. This study explores the quantum capacitance of graphene oxide, which bears epoxy and hydroxyl groups on its basal plane, by employing density functional theory (DFT) calculations. The results demonstrate that the total density of states near the Fermi level is significantly enhanced by introducing oxygen-containing groups, which is beneficial for the improvement of the quantum capacitance. Moreover, the quantum capacitances of the graphene oxide with different concentrations of these two oxygen-containing groups are compared, revealing that more epoxy and hydroxyl groups result in a higher quantum capacitance. Notably, the hydroxyl concentration has a considerable effect on the capacitive behavior. © 2018 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

Theoretical calculations of Electron Paramagnetic Resonance parameters of liquid phase Orotic acid radical

NASA Astrophysics Data System (ADS)

Sarikaya, Ebru Karakaş; Dereli, Ömer

2017-02-01

To obtain liquid phase molecular structure, conformational analysis of Orotic acid was performed and six conformers were determined. For these conformations, eight possible radicals were modelled by using Density Functional Theory computations with respect to molecular structure. Electron Paramagnetic Resonance parameters of these model radicals were calculated and then they were compared with the experimental ones. Geometry optimizations of the molecule and modeled radicals were performed using Becke's three-parameter hybrid-exchange functional combined with the Lee-Yang-Parr correlation functional of Density Functional Theory and 6-311++G(d,p) basis sets in p-dioxane solution. Because Orotic acid can be mutagenic in mammalian somatic cells and it is also mutagenic for bacteria and yeast, it has been studied.

12-h abstinence-induced functional connectivity density changes and craving in young smokers: a resting-state study.

PubMed

Zhao, Shuzhi; Li, Yangding; Li, Min; Wang, Ruonan; Bi, Yanzhi; Zhang, Yajuan; Lu, Xiaoqi; Yu, Dahua; Yang, Likun; Yuan, Kai

2018-06-20

Studying the neural correlates of craving to smoke is of great importance to improve treatment outcomes in smoking addiction. According to previous studies, the critical roles of striatum and frontal brain regions had been revealed in addiction. However, few studies focused on the hub of brain regions in the 12 h abstinence induced craving in young smokers. Thirty-one young male smokers were enrolled in the present study. A within-subject experiment design was carried out to compare functional connectivity density between 12-h smoking abstinence and smoking satiety conditions during resting state in young adult smokers by using functional connectivity density mapping (FCDM). Then, the functional connectivity density changes during smoking abstinence versus satiety were further used to examine correlations with abstinence-induced changes in subjective craving. We found young adult smokers in abstinence state (vs satiety) had higher local functional connectivity density (lFCD) and global functional connectivity density (gFCD) in brain regions including striatal subregions (i.e., bilateral caudate and putamen), frontal regions (i.e., anterior cingulate cortex (ACC) and orbital frontal cortex (OFC)) and bilateral insula. We also found higher lFCD during smoking abstinence (vs satiety) in bilateral thalamus. Additionally, the lFCD changes of the left ACC, bilateral caudate and right OFC were positively correlated with the changes in craving induced by abstinence (i.e., abstinence minus satiety) in young adult smokers. The present findings improve the understanding of the effects of acute smoking abstinence on the hubs of brain gray matter in the abstinence-induces craving and may contribute new insights into the neural mechanism of abstinence-induced craving in young smokers in smoking addiction.

Theoretical prediction of nuclear magnetic shieldings and indirect spin-spin coupling constants in 1,1-, cis-, and trans-1,2-difluoroethylenes

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

Nozirov, Farhod, E-mail: teobaldk@gmail.com, E-mail: farhod.nozirov@gmail.com; Stachów, Michał, E-mail: michal.stachow@gmail.com; Kupka, Teobald, E-mail: teobaldk@gmail.com, E-mail: farhod.nozirov@gmail.com

2014-04-14

A theoretical prediction of nuclear magnetic shieldings and indirect spin-spin coupling constants in 1,1-, cis- and trans-1,2-difluoroethylenes is reported. The results obtained using density functional theory (DFT) combined with large basis sets and gauge-independent atomic orbital calculations were critically compared with experiment and conventional, higher level correlated electronic structure methods. Accurate structural, vibrational, and NMR parameters of difluoroethylenes were obtained using several density functionals combined with dedicated basis sets. B3LYP/6-311++G(3df,2pd) optimized structures of difluoroethylenes closely reproduced experimental geometries and earlier reported benchmark coupled cluster results, while BLYP/6-311++G(3df,2pd) produced accurate harmonic vibrational frequencies. The most accurate vibrations were obtained using B3LYP/6-311++G(3df,2pd)more » with correction for anharmonicity. Becke half and half (BHandH) density functional predicted more accurate {sup 19}F isotropic shieldings and van Voorhis and Scuseria's τ-dependent gradient-corrected correlation functional yielded better carbon shieldings than B3LYP. A surprisingly good performance of Hartree-Fock (HF) method in predicting nuclear shieldings in these molecules was observed. Inclusion of zero-point vibrational correction markedly improved agreement with experiment for nuclear shieldings calculated by HF, MP2, CCSD, and CCSD(T) methods but worsened the DFT results. The threefold improvement in accuracy when predicting {sup 2}J(FF) in 1,1-difluoroethylene for BHandH density functional compared to B3LYP was observed (the deviations from experiment were −46 vs. −115 Hz)« less

Few-particle quantum dynamics-comparing nonequilibrium Green functions with the generalized Kadanoff-Baym ansatz to density operator theory

NASA Astrophysics Data System (ADS)

Hermanns, S.; Balzer, K.; Bonitz, M.

2013-03-01

The nonequilibrium description of quantum systems requires, for more than two or three particles, the use of a reduced description to be numerically tractable. Two possible approaches are based on either reduced density matrices or nonequilibrium Green functions (NEGF). Both concepts are formulated in terms of hierarchies of coupled equations—the Bogoliubov-Born-Green-Kirkwood-Yvon (BBGKY) hierarchy for the reduced density operators and the Martin-Schwinger-hierarchy (MS) for the Green functions, respectively. In both cases, similar approximations are introduced to decouple the hierarchy, yet still many questions regarding the correspondence of both approaches remain open. Here we analyze this correspondence by studying the generalized Kadanoff-Baym ansatz (GKBA) that reduces the NEGF to a single-time theory. Starting from the BBGKY-hierarchy we present the approximations that are necessary to recover the GKBA result both, with Hartree-Fock propagators (HF-GKBA) and propagators in second Born approximation. To test the quality of the HF-GKBA, we study the dynamics of a 4-electron Hubbard nanocluster starting from a strong nonequilibrium initial state and compare to exact results and the Wang-Cassing approximation to the BBGKY hierarchy presented recently by Akbari et al. [1].

The risks and returns of stock investment in a financial market

NASA Astrophysics Data System (ADS)

Li, Jiang-Cheng; Mei, Dong-Cheng

2013-03-01

The risks and returns of stock investment are discussed via numerically simulating the mean escape time and the probability density function of stock price returns in the modified Heston model with time delay. Through analyzing the effects of delay time and initial position on the risks and returns of stock investment, the results indicate that: (i) There is an optimal delay time matching minimal risks of stock investment, maximal average stock price returns and strongest stability of stock price returns for strong elasticity of demand of stocks (EDS), but the opposite results for weak EDS; (ii) The increment of initial position recedes the risks of stock investment, strengthens the average stock price returns and enhances stability of stock price returns. Finally, the probability density function of stock price returns and the probability density function of volatility and the correlation function of stock price returns are compared with other literatures. In addition, good agreements are found between them.

Densities and temperatures in the polar thermosphere

NASA Technical Reports Server (NTRS)

Gardner, L. J.

1977-01-01

The atomic oxygen density at 120 km, the 630 nm airglow temperature, the helium density at 300 km and the molecular nitrogen density near 400 km were examined as functions of geomagnetic latitude, geomagnetic time, season and magnetic activity level. The long-term averages of these quantities were examined so as to provide a baseline of these thermospheric parameters from which future studies may be made for comparison. The hours around magnetic noon are characterized by low temperatures, high 0 and He densities, and median nitrogen densities. The pre-midnight hours exhibit high temperatures, high He density, low nitrogen density and median 0 densities. The post-midnight sector shows low 0 and He densities, median temperatures and high nitrogen densities. These results are compared to recent models and observations and are discussed with respect to their causes due to divergence of the wind field and energy deposition in the thermosphere.

Controlled functionalization of carbonaceous fibers for asymmetric solid-state micro-supercapacitors with high volumetric energy density.

PubMed

Yu, Dingshan; Goh, Kunli; Zhang, Qiang; Wei, Li; Wang, Hong; Jiang, Wenchao; Chen, Yuan

2014-10-22

A 1.8 V asymmetric solid-state flexible micro-supercapacitor is designed with one MnO2 -coated reduced graphene oxide/single-walled carbon nanotube (rGO/SWCNT) composite fiber as positive electrode and one nitrogen-doped rGO/SWCNT fiber as negative electrode, which demonstrates ultrahigh volumetric energy density, comparable to some thin-film lithium batteries, along with high power density, long cycle life, and good flexibility. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

The gluon density of the proton at low x from a QCD analysis of F2

NASA Astrophysics Data System (ADS)

Aid, S.; Andreev, V.; Andrieu, B.; Appuhn, R.-D.; Arpagaus, M.; Babaev, A.; Baehr, J.; Bán, J.; Ban, Y.; Baranov, P.; Barrelet, E.; Barschke, R.; Bartel, W.; Barth, M.; Bassler, U.; Beck, H. P.; Behrend, H.-J.; Belousov, A.; Berger, Ch.; Bernardi, G.; Bernet, R.; Bertrand-Coremans, G.; Besançon, M.; Beyer, R.; Biddulph, P.; Bispham, P.; Bizot, J. C.; Blobel, V.; Borras, K.; Botterweck, F.; Boudry, V.; Braemer, A.; Brasse, F.; Braunschweig, W.; Brisson, V.; Bruncko, D.; Brune, C.; Buchholz, R.; Büngener, L.; Bürger, J.; Büsser, F. W.; Buniatian, A.; Burke, S.; Burton, M.; Buschhorn, G.; Campbell, A. J.; Carli, T.; Charles, F.; Charlet, M.; Clarke, D.; Clegg, A. B.; Clerbaux, B.; Colombo, M.; Contreras, J. G.; Cormack, C.; Coughlan, J. A.; Courau, A.; Coutures, Ch.; Cozzika, G.; Criegee, L.; Cussans, D. G.; Cvach, J.; Dagoret, S.; Dainton, J. B.; Dau, W. D.; Daum, K.; David, M.; Delcourt, B.; Del Buono, L.; De Roeck, A.; De Wolf, E. A.; Di Nezza, P.; Dollfus, C.; Dowell, J. D.; Dreis, H. B.; Droutskoi, A.; Duboc, J.; Düllmann, D.; Dünger, O.; Duhm, H.; Ebert, J.; Ebert, T. R.; Eckerlin, G.; Efremenko, V.; Egli, S.; Ehrlichmann, H.; Eichenberger, S.; Eichler, R.; Eisele, F.; Eisenhandler, E.; Ellison, R. J.; Elsen, E.; Erdmann, M.; Erdmann, W.; Evrard, E.; Favart, L.; Fedotov, A.; Feeken, D.; Felst, R.; Feltesse, J.; Ferencei, J.; Ferrarotto, F.; Flamm, K.; Fleischer, M.; Flieser, M.; Flügge, G.; Fomenko, A.; Fominykh, B.; Forbush, M.; Formánek, J.; Foster, J. M.; Franke, G.; Fretwurst, E.; Gabathuler, E.; Gabathuler, K.; Gamerdinger, K.; Garvey, J.; Gayler, J.; Gebauer, M.; Gellrich, A.; Genzel, H.; Gerhards, R.; Goerlach, U.; Goerlich, L.; Gogitidze, N.; Goldberg, M.; Goldner, D.; Gonzalez-Pineiro, B.; Gorelov, I.; Goritchev, P.; Grab, C.; Grässler, H.; Grässler, R.; Greenshaw, T.; Grindhammer, G.; Gruber, A.; Gruber, C.; Haack, J.; Haidt, D.; Hajduk, L.; Hamon, O.; Hampel, M.; Hanlon, E. M.; Hapke, M.; Haynes, W. J.; Heatherington, J.; Heinzelmann, G.; Henderson, R. C. W.; Henschel, H.; Herynek, I.; Hess, M. F.; Hildesheim, W.; Hill, P.; Hiller, K. H.; Hilton, C. D.; Hladký, J.; Hoeger, K. C.; Höppner, M.; Horisberger, R.; Hudgson, V. L.; Huet, Ph.; Hütte, M.; Hufnagel, H.; Ibbotson, M.; Itterbeck, H.; Jabiol, M.-A.; Jacholkowska, A.; Jacobsson, C.; Jaffre, M.; Janoth, J.; Jansen, T.; Jönsson, L.; Johnson, D. P.; Johnson, L.; Jung, H.; Kalmus, P. I. P.; Kant, D.; Kaschowitz, R.; Kasselmann, P.; Kathage, U.; Katzy, J.; Kaufmann, H. H.; Kazarian, S.; Kenyon, I. R.; Kermiche, S.; Keuker, C.; Kiesling, C.; Klein, M.; Kleinwort, C.; Knies, G.; Ko, W.; Köhler, T.; Köhne, J. H.; Kolanoski, H.; Kole, F.; Kolya, S. D.; Korbel, V.; Korn, M.; Kostka, P.; Kotelnikov, S. K.; Krämerkämper, T.; Krasny, M. W.; Krehbiel, H.; Krücker, D.; Krüger, U.; Krüner-Marquis, U.; Kubenka, J. P.; Küster, H.; Kuhlen, M.; Kurča, T.; Kurzhöfer, J.; Kuznik, B.; Lacour, D.; Lamarche, F.; Lander, R.; Landon, M. P. J.; Lange, W.; Lanius, P.; Laporte, J.-F.; Lebedev, A.; Leverenz, C.; Levonian, S.; Ley, Ch.; Lindner, A.; Lindström, G.; Link, J.; Linsel, F.; Lipinski, J.; List, B.; Lobo, G.; Loch, P.; Lohmander, H.; Lomas, J.; Lopez, G. C.; Lubimov, V.; Lüke, D.; Magnussen, N.; Malinovski, E.; Mani, S.; Maraček, R.; Marage, P.; Marks, J.; Marshall, R.; Martens, J.; Martin, R.; Martyn, H.-U.; Martyniak, J.; Masson, S.; Mavroidis, T.; Maxfield, S. J.; McMahon, S. J.; Mehta, A.; Meier, K.; Mercer, D.; Merz, T.; Meyer, C. A.; Meyer, H.; Meyer, J.; Migliori, A.; Mikocki, S.; Milstead, D.; Moreau, F.; Morris, J. V.; Mroczko, E.; Müller, G.; Müller, K.; Murín, P.; Nagovizin, V.; Nahnhauer, R.; Naroska, B.; Naumann, Th.; Newman, P. R.; Newton, D.; Neyret, D.; Nguyen, H. K.; Nicholls, T. C.; Niebergall, F.; Niebuhr, C.; Niedzballa, Ch.; Nisius, R.; Nowak, G.; Noyes, G. W.; Nyberg-Werther, M.; Oakden, M.; Oberlack, H.; Obrock, U.; Olsson, J. E.; Ozerov, D.; Panaro, E.; Panitch, A.; Pascaud, C.; Patel, G. D.; Peppel, E.; Perez, E.; Phillips, J. P.; Pichler, Ch.; Pieuchot, A.; Pitzl, D.; Pope, G.; Prell, S.; Prosi, R.; Rabbertz, K.; Rädel, G.; Raupach, F.; Reimer, P.; Reinshagen, S.; Ribarics, P.; Rick, H.; Riech, V.; Riedlberger, J.; Riess, S.; Rietz, M.; Rizvi, E.; Robertson, S. M.; Robmann, P.; Roloff, H. E.; Roosen, R.; Rosenbauer, K.; Rostovtsev, A.; Rouse, F.; Royon, C.; Rüter, K.; Rusakov, S.; Rybicki, K.; Rylko, R.; Sahlmann, N.; Sanchez, E.; Sankey, D. P. C.; Schacht, P.; Schiek, S.; Schleper, P.; von Schlippe, W.; Schmidt, C.; Schmidt, D.; Schmidt, G.; Schöning, A.; Schröder, V.; Schuhmann, E.; Schwab, B.; Schwind, A.; Sefkow, F.; Seidel, M.; Sell, R.; Semenov, A.; Shekelyan, V.; Sheviakov, I.; Shooshtari, H.; Shtarkov, L. N.; Siegmon, G.; Siewert, U.; Sirois, Y.; Skillicorn, I. O.; Smirnov, P.; Smith, J. R.; Solochenko, V.; Soloviev, Y.; Spiekermann, J.; Spielman, S.; Spitzer, H.; Starosta, R.; Steenbock, M.; Steffen, P.; Steinberg, R.; Stella, B.; Stephens, K.; Stier, J.; Stiewe, J.; Stösslein, U.; Stolze, K.; Strachota, J.; Straumann, U.; Struczinski, W.; Sutton, J. P.; Tapprogge, S.; Tchernyshov, V.; Thiebaux, C.; Thompson, G.; Truöl, P.; Turnau, J.; Tutas, J.; Uelkes, P.; Usik, A.; Valkár, S.; Valkárová, A.; Vallée, C.; Van Esch, P.; Van Mechelen, P.; Vartapetian, A.; Vazdik, Y.; Verrecchia, P.; Villet, G.; Wacker, K.; Wagener, A.; Wagener, M.; Walker, I. W.; Walther, A.; Weber, G.; Weber, M.; Wegener, D.; Wegner, A.; Wellisch, H. P.; West, L. R.; Willard, S.; Willard, S.; Winde, M.; Winter, G.-G.; Wittek, C.; Wright, A. E.; Wünsch, E.; Wulff, N.; Yiou, T. P.; Žáček, J.; Zarbock, D.; Zhang, Z.; Zhokin, A.; Zimmer, M.; Zimmermann, W.; Zomer, F.; Zuber, K.; H1 Collaboration

1995-02-01

We present a QCD analysis of the proton structure function F2 measured by the H1 experiment at HERA, combined with data from previous fixed target experiments. The gluon density is extracted from the scaling violations of F2 in the range 2 · 10 -4 < x < 3 · 10 -2 and compared with an approximate solution of the QCD evolution equations. The gluon density is found to rise steeply with decreasing x.

Coarse-grained density functional theories for metallic alloys: Generalized coherent-potential approximations and charge-excess functional theory

NASA Astrophysics Data System (ADS)

Bruno, Ezio; Mammano, Francesco; Fiorino, Antonino; Morabito, Emanuela V.

2008-04-01

The class of the generalized coherent-potential approximations (GCPAs) to the density functional theory (DFT) is introduced within the multiple scattering theory formalism with the aim of dealing with ordered or disordered metallic alloys. All GCPA theories are based on a common ansatz for the kinetic part of the Hohenberg-Kohn functional and each theory of the class is specified by an external model concerning the potential reconstruction. Most existing DFT implementations of CPA-based theories belong to the GCPA class. The analysis of the formal properties of the density functional defined by GCPA theories shows that it consists of marginally coupled local contributions. Furthermore, it is shown that the GCPA functional does not depend on the details of the charge density and that it can be exactly rewritten as a function of the appropriate charge multipole moments to be associated with each lattice site. A general procedure based on the integration of the qV laws is described that allows for the explicit construction of the same function. The coarse-grained nature of the GCPA density functional implies a great deal of computational advantages and is connected with the O(N) scalability of GCPA algorithms. Moreover, it is shown that a convenient truncated series expansion of the GCPA functional leads to the charge-excess functional (CEF) theory [E. Bruno , Phys. Rev. Lett. 91, 166401 (2003)], which here is offered in a generalized version that includes multipolar interactions. CEF and the GCPA numerical results are compared with status of art linearized augmented plane wave (LAPW) full-potential density functional calculations for 62 bcc- and fcc-based ordered CuZn alloys, in all the range of concentrations. Two facts clearly emerge from these extensive tests. In the first place, the discrepancies between GCPA and CEF results are always within the numerical accuracy of the calculations, both for the site charges and the total energies. In the second place, the GCPA (or the CEF) is able to very carefully reproduce the LAPW site charges and a good agreement is obtained also about the total energies.

Vibrational, spectroscopic, molecular docking and density functional theory studies on N-(5-aminopyridin-2-yl)acetamide

NASA Astrophysics Data System (ADS)

Asath, R. Mohamed; Rekha, T. N.; Premkumar, S.; Mathavan, T.; Benial, A. Milton Franklin

2016-12-01

Conformational analysis was carried out for N-(5-aminopyridin-2-yl)acetamide (APA) molecule. The most stable, optimized structure was predicted by the density functional theory calculations using the B3LYP functional with cc-pVQZ basis set. The optimized structural parameters and vibrational frequencies were calculated. The experimental and theoretical vibrational frequencies were assigned and compared. Ultraviolet-visible spectrum was simulated and validated experimentally. The molecular electrostatic potential surface was simulated. Frontier molecular orbitals and related molecular properties were computed, which reveals that the higher molecular reactivity and stability of the APA molecule and further density of states spectrum was simulated. The natural bond orbital analysis was also performed to confirm the bioactivity of the APA molecule. Antidiabetic activity was studied based on the molecular docking analysis and the APA molecule was identified that it can act as a good inhibitor against diabetic nephropathy.

On the phase diagram of water with density functional theory potentials: the melting temperature of Ice I-h with the Perdew-Burke-Ernzerhof and Becke-Lee-Yang-Parr functionals

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

Yoo, Soohaeng; Zeng, Xiao Cheng; Xantheas, Sotiris S.

2009-06-11

The melting temperature (Tm) of ice Ih was determined from constant enthalphy (NPH) Born-Oppenheimer Molecular Dynamics (BOMD) simulations to be 417±3 K for the Perdew-Burke-Ernzerhof (PBE) and 411±4 K for the Becke-Lee-Yang-Parr (BLYP) density functionals using a coexisting ice (Ih)-liquid phase at constant pressures of P = 2,500 and 10,000 bar and a density ρ = 1 g/cm3, respectively. This suggests that ambient condition simulations at ρ = 1 g/cm3 will rather describe a supercooled state that is overstructured when compared to liquid water. This work was supported by the US Department of Energy Office of Basic Energy Sciences' Chemicalmore » Sciences program. Pacific Northwest National Laboratory is operated by Battelle for the US Department of Energy.« less

Analyzing the financial crisis using the entropy density function

NASA Astrophysics Data System (ADS)

Oh, Gabjin; Kim, Ho-yong; Ahn, Seok-Won; Kwak, Wooseop

2015-02-01

The risk that is created by nonlinear interactions among subjects in economic systems is assumed to increase during an abnormal state of a financial market. Nevertheless, investigating the systemic risk in financial markets following the global financial crisis is not sufficient. In this paper, we analyze the entropy density function in the return time series for several financial markets, such as the S&P500, KOSPI, and DAX indices, from October 2002 to December 2011 and analyze the variability in the entropy value over time. We find that the entropy density function of the S&P500 index during the subprime crisis exhibits a significant decrease compared to that in other periods, whereas the other markets, such as those in Germany and Korea, exhibit no significant decrease during the market crisis. These findings demonstrate that the S&P500 index generated a regular pattern in the return time series during the financial crisis.

Thermal and active fluctuations of a compressible bilayer vesicle

NASA Astrophysics Data System (ADS)

Sachin Krishnan, T. V.; Yasuda, Kento; Okamoto, Ryuichi; Komura, Shigeyuki

2018-05-01

We discuss thermal and active fluctuations of a compressible bilayer vesicle by using the results of hydrodynamic theory for vesicles. Coupled Langevin equations for the membrane deformation and the density fields are employed to calculate the power spectral density matrix of membrane fluctuations. Thermal contribution is obtained by means of the fluctuation dissipation theorem, whereas active contribution is calculated from exponentially decaying time correlation functions of active random forces. We obtain the total power spectral density as a sum of thermal and active contributions. An apparent response function is further calculated in order to compare with the recent microrheology experiment on red blood cells. An enhanced response is predicted in the low-frequency regime for non-thermal active fluctuations.

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.

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.

The molecular, electronic structures and vibrational spectra of metal-free, N,N'-dideuterio and magnesium tetra-2,3-pyridino-porphyrazines: Density functional calculations.

PubMed

Liu, Zhongqiang; Zhang, Xianxi; Zhang, Yuexing; Li, Renjie; Jiang, Jianzhuang

2006-10-01

A theoretical investigation of the fully optimized geometries and electronic structures of the metal-free (TPdPzH(2)), N,N'-dideuterio (TPdPzD(2)), and magnesium (TPdPzMg) tetra-2,3-pyridino-porphyrazine has been conducted based on density functional theory. The optimized geometries at density functional theory level for these compounds are reported here for the first time. A comparison between the different molecules for the geometry, molecular orbital, and atomic charge is made. The substituent effect of the N atoms on the molecular structures of these compounds is discussed. The IR and Raman spectra for these three compounds have also been calculated at density functional B3LYP level using the 6-31G(d) basis set. Detailed assignments of the NH, NM, and pyridine ring vibrational bands in the IR and Raman spectra have been made based on assistance of animated pictures. The simulated IR spectra of TPdPzH(2) are compared with the experimental absorption spectra, and very good consistency has been found. The isotope effect on the IR and Raman spectra is also discussed.

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.

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

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 Bottomside Ionospheric Electron Density Specification using Passive High Frequency Signals

NASA Astrophysics Data System (ADS)

Kaeppler, S. R.; Cosgrove, R. B.; Mackay, C.; Varney, R. H.; Kendall, E. A.; Nicolls, M. J.

2016-12-01

The vertical bottomside electron density profile is influenced by a variety of natural sources, most especially traveling ionospheric disturbances (TIDs). These disturbances cause plasma to be moved up or down along the local geomagnetic field and can strongly impact the propagation of high frequency radio waves. While the basic physics of these perturbations has been well studied, practical bottomside models are not well developed. We present initial results from an assimilative bottomside ionosphere model. This model uses empirical orthogonal functions based on the International Reference Ionosphere (IRI) to develop a vertical electron density profile, and features a builtin HF ray tracing function. This parameterized model is then perturbed to model electron density perturbations associated with TIDs or ionospheric gradients. Using the ray tracing feature, the model assimilates angle of arrival measurements from passive HF transmitters. We demonstrate the effectiveness of the model using angle of arrival data. Modeling results of bottomside electron density specification are compared against suitable ancillary observations to quantify accuracy of our model.

Evolution of the Blue and Far-Infrared Galaxy Luminosity Functions

NASA Technical Reports Server (NTRS)

Lonsdale, Carol J.; Chokshi, Arati

1993-01-01

The space density of blue-selected galaxies at moderate redshifts is determined here directly by deriving the luminosity function. Evidence is found for density evolution for moderate luminosity galaxies at a rate of (1+z) exp delta, with a best fit of delta + 4 +/- 2, between the current epoch and Z greater than about 0.1. At M(b) less than -22 evidence is found for about 0.5-1.5 mag of luminosity evolution in addition to the density evolution, corresponding to an evolutionary rate of about (1+z) exp gamma, with gamma = 0.5-2.5, but a redshift of about 0.4. Assuming a steeper faint end slope of alpha = -1.3 similar to that observed in the Virgo cluster, could explain the data with a luminosity evolution rate of gamma = 1-2, without need for any density evolution. Acceptable fits are found by comparing composite density and luminosity evolution models to faint IRAS 60 micron source counts, implying that the blue and far-IR evolutionary rates may be similar.

Density functional studies of the defect-induced electronic structure modifications in bilayer boronitrene

NASA Astrophysics Data System (ADS)

Ukpong, A. M.; Chetty, N.

2012-05-01

The van der Waals interaction-corrected density functional theory is used in this study to investigate the formation, energetic stability, and inter-layer cohesion in bilayer hexagonal boronitrene. The effect of inter-layer separation on the electronic structure is systematically investigated. The formation and energetic stability of intrinsic defects are also investigated at the equilibrium inter-layer separation. It is found that nonstoichiometric defects, and their complexes, that induce excess nitrogen or excess boron, in each case, are relatively more stable in the atmosphere that corresponds to the excess atomic species. The modifications of the electronic structure due to formation of complexes are also investigated. It is shown that van der Waals density functional theory gives an improved description of the cohesive properties but not the electronic structure in bilayer boronitrene compared to other functionals. We identify energetically favourable topological defects that retain the energy gap in the electronic structure, and discuss their implications for band gap engineering in low-n layer boronitrene insulators. The relative strengths and weaknesses of the functionals in predicting the properties of bilayer boronitrene are also discussed.

Density functional theory calculations of III-N based semiconductors with mBJLDA

NASA Astrophysics Data System (ADS)

Gürel, Hikmet Hakan; Akıncı, Özden; Ünlü, Hilmi

2017-02-01

In this work, we present first principles calculations based on a full potential linear augmented plane-wave method (FP-LAPW) to calculate structural and electronic properties of III-V based nitrides such as GaN, AlN, InN in a zinc-blende cubic structure. First principles calculation using the local density approximation (LDA) and generalized gradient approximation (GGA) underestimate the band gap. We proposed a new potential called modified Becke-Johnson local density approximation (MBJLDA) that combines modified Becke-Johnson exchange potential and the LDA correlation potential to get better band gap results compared to experiment. We compared various exchange-correlation potentials (LSDA, GGA, HSE, and MBJLDA) to determine band gaps and structural properties of semiconductors. We show that using MBJLDA density potential gives a better agreement with experimental data for band gaps III-V nitrides based semiconductors.

Deconvolution of Stark broadened spectra for multi-point density measurements in a flow Z-pinch

DOE PAGES

Vogman, G. V.; Shumlak, U.

2011-10-13

Stark broadened emission spectra, once separated from other broadening effects, provide a convenient non-perturbing means of making plasma density measurements. A deconvolution technique has been developed to measure plasma densities in the ZaP flow Z-pinch experiment. The ZaP experiment uses sheared flow to mitigate MHD instabilities. The pinches exhibit Stark broadened emission spectra, which are captured at 20 locations using a multi-chord spectroscopic system. Spectra that are time- and chord-integrated are well approximated by a Voigt function. The proposed method simultaneously resolves plasma electron density and ion temperature by deconvolving the spectral Voigt profile into constituent functions: a Gaussian functionmore » associated with instrument effects and Doppler broadening by temperature; and a Lorentzian function associated with Stark broadening by electron density. The method uses analytic Fourier transforms of the constituent functions to fit the Voigt profile in the Fourier domain. The method is discussed and compared to a basic least-squares fit. The Fourier transform fitting routine requires fewer fitting parameters and shows promise in being less susceptible to instrumental noise and to contamination from neighboring spectral lines. The method is evaluated and tested using simulated lines and is applied to experimental data for the 229.69 nm C III line from multiple chords to determine plasma density and temperature across the diameter of the pinch. As a result, these measurements are used to gain a better understanding of Z-pinch equilibria.« less

Deconvolution of Stark broadened spectra for multi-point density measurements in a flow Z-pinch

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

Vogman, G. V.; Shumlak, U.

2011-10-15

Stark broadened emission spectra, once separated from other broadening effects, provide a convenient non-perturbing means of making plasma density measurements. A deconvolution technique has been developed to measure plasma densities in the ZaP flow Z-pinch experiment. The ZaP experiment uses sheared flow to mitigate MHD instabilities. The pinches exhibit Stark broadened emission spectra, which are captured at 20 locations using a multi-chord spectroscopic system. Spectra that are time- and chord-integrated are well approximated by a Voigt function. The proposed method simultaneously resolves plasma electron density and ion temperature by deconvolving the spectral Voigt profile into constituent functions: a Gaussian functionmore » associated with instrument effects and Doppler broadening by temperature; and a Lorentzian function associated with Stark broadening by electron density. The method uses analytic Fourier transforms of the constituent functions to fit the Voigt profile in the Fourier domain. The method is discussed and compared to a basic least-squares fit. The Fourier transform fitting routine requires fewer fitting parameters and shows promise in being less susceptible to instrumental noise and to contamination from neighboring spectral lines. The method is evaluated and tested using simulated lines and is applied to experimental data for the 229.69 nm C III line from multiple chords to determine plasma density and temperature across the diameter of the pinch. These measurements are used to gain a better understanding of Z-pinch equilibria.« less

Low-memory iterative density fitting.

PubMed

Grajciar, Lukáš

2015-07-30

A new low-memory modification of the density fitting approximation based on a combination of a continuous fast multipole method (CFMM) and a preconditioned conjugate gradient solver is presented. Iterative conjugate gradient solver uses preconditioners formed from blocks of the Coulomb metric matrix that decrease the number of iterations needed for convergence by up to one order of magnitude. The matrix-vector products needed within the iterative algorithm are calculated using CFMM, which evaluates them with the linear scaling memory requirements only. Compared with the standard density fitting implementation, up to 15-fold reduction of the memory requirements is achieved for the most efficient preconditioner at a cost of only 25% increase in computational time. The potential of the method is demonstrated by performing density functional theory calculations for zeolite fragment with 2592 atoms and 121,248 auxiliary basis functions on a single 12-core CPU workstation. © 2015 Wiley Periodicals, Inc.

Transverse Densities of Octet Baryons from Chiral Effective Field Theory

DOE PAGES

Alarcón, Jose Manuel; Hiller Blin, Astrid N.; Weiss, Christian

2017-03-24

Transverse densities describe the distribution of charge and current at fixed light-front time and provide a frame-independent spatial representation of hadrons as relativistic systems. In this paper, we calculate the transverse densities of the octet baryons at peripheral distances b=O(M π -1) in an approach that combines chiral effective field theory (χχEFT) and dispersion analysis. The densities are represented as dispersive integrals of the imaginary parts of the baryon electromagnetic form factors in the timelike region (spectral functions). The spectral functions on the two-pion cut at t>4Mmore » $$2\\atop{π}$$ are computed using relativistic χEFT with octet and decuplet baryons in the extended on-mass-shell renormalization scheme. The calculations are extended into the ρ-meson mass region using a dispersive method that incorporates the timelike pion form-factor data. The approach allows us to construct densities at distances b>1 fm with controlled uncertainties. Finally, our results provide insight into the peripheral structure of nucleons and hyperons and can be compared with empirical densities and lattice-QCD calculations.« less

Is there a generalized anomeric effect? Analyses from energy components and information-theoretic quantities from density functional reactivity theory

NASA Astrophysics Data System (ADS)

Cao, Xiaofang; Liu, Shaoqian; Rong, Chunying; Lu, Tian; Liu, Shubin

2017-11-01

The nature and origin of the generalized anomeric effect is investigated with energy components and information-theoretic quantities from density functional reactivity theory. Forty-five systems with the general formula of R1-X-CH2-Y-R2 were examined, where R1 and R2 are functional groups and X and Y as electronegative heteroatoms. Our results show that in most cases the effect is valid, and the dominant contribution for the validity of the effect is from the electrostatic interaction. Other contributions such as steric and hyperconjugation play minor but indispensable roles. Its relationship with the conventional anomeric effect is compared and discussed.

Collagen Matrix Density Drives the Metabolic Shift in Breast Cancer Cells.

PubMed

Morris, Brett A; Burkel, Brian; Ponik, Suzanne M; Fan, Jing; Condeelis, John S; Aguirre-Ghiso, Julio A; Castracane, James; Denu, John M; Keely, Patricia J

2016-11-01

Increased breast density attributed to collagen I deposition is associated with a 4-6 fold increased risk of developing breast cancer. Here, we assessed cellular metabolic reprogramming of mammary carcinoma cells in response to increased collagen matrix density using an in vitro 3D model. Our initial observations demonstrated changes in functional metabolism in both normal mammary epithelial cells and mammary carcinoma cells in response to changes in matrix density. Further, mammary carcinoma cells grown in high density collagen matrices displayed decreased oxygen consumption and glucose metabolism via the tricarboxylic acid (TCA) cycle compared to cells cultured in low density matrices. Despite decreased glucose entry into the TCA cycle, levels of glucose uptake, cell viability, and ROS were not different between high and low density matrices. Interestingly, under high density conditions the contribution of glutamine as a fuel source to drive the TCA cycle was significantly enhanced. These alterations in functional metabolism mirrored significant changes in the expression of metabolic genes involved in glycolysis, oxidative phosphorylation, and the serine synthesis pathway. This study highlights the broad importance of the collagen microenvironment to cellular expression profiles, and shows that changes in density of the collagen microenvironment can modulate metabolic shifts of cancer cells. Copyright © 2016 The Authors. Published by Elsevier B.V. All rights reserved.

Excitons in Potassium Bromide: A Study using Embedded Time-dependent Density Functional Theory and Equation-of-Motion Coupled Cluster Methods

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

Govind, Niranjan; Sushko, Petr V.; Hess, Wayne P.

2009-03-05

We present a study of the electronic excitations in insulating materials using an embedded- cluster method. The excited states of the embedded cluster are studied systematically using time-dependent density functional theory (TDDFT) and high-level equation-of-motion coupled cluster (EOMCC) methods. In particular, we have used EOMCC models with singles and doubles (EOMCCSD) and two approaches which account for the e®ect of triply excited con¯gurations in non-iterative and iterative fashions. We present calculations of the lowest surface excitations of the well-studied potassium bromide (KBr) system and compare our results with experiment. The bulk-surface exciton shift is also calculated at the TDDFT levelmore » and compared with experiment.« less

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.

Benchmark study of ionization potentials and electron affinities of armchair single-walled carbon nanotubes using density functional theory

NASA Astrophysics Data System (ADS)

Zhou, Bin; Hu, Zhubin; Jiang, Yanrong; He, Xiao; Sun, Zhenrong; Sun, Haitao

2018-05-01

The intrinsic parameters of carbon nanotubes (CNTs) such as ionization potential (IP) and electron affinity (EA) are closely related to their unique properties and associated applications. In this work, we demonstrated the success of optimal tuning method based on range-separated (RS) density functionals for both accurate and efficient prediction of vertical IPs and electron affinities (EAs) of a series of armchair single-walled carbon nanotubes C20n H20 (n  =  2–6) compared to the high-level IP/EA equation-of-motion coupled-cluster method with single and double substitutions (IP/EA-EOM-CCSD). Notably, the resulting frontier orbital energies (–ε HOMO and –ε LUMO) from the tuning method exhibit an excellent approximation to the corresponding IPs and EAs, that significantly outperform other conventional density functionals. In addition, it is suggested that the RS density functionals that possess both a fixed amount of exact exchange in the short-range and a correct long-range asymptotic behavior are suitable for calculating electronic structures of finite-sized CNTs. Next the performance of density functionals for description of various molecular properties such as chemical potential, hardness and electrophilicity are assessed as a function of tube length. Thanks to the efficiency and accuracy of this tuning method, the related behaviors of much longer armchair single-walled CNTs until C200H20 were studied. Lastly, the present work is proved to provide an efficient theoretical tool for future materials design and reliable characterization of other interesting properties of CNT-based systems.

Development of a Multicenter Density Functional Tight Binding Model for Plutonium Surface Hydriding.

PubMed

Goldman, Nir; Aradi, Bálint; Lindsey, Rebecca K; Fried, Laurence E

2018-05-08

We detail the creation of a multicenter density functional tight binding (DFTB) model for hydrogen on δ-plutonium, using a framework of new Slater-Koster interaction parameters and a repulsive energy based on the Chebyshev Interaction Model for Efficient Simulation (ChIMES), where two- and three-center atomic interactions are represented by linear combinations of Chebyshev polynomials. We find that our DFTB/ChIMES model yields a total electron density of states for bulk δ-Pu that compares well to that from Density Functional Theory, as well as to a grid of energy calculations representing approximate H 2 dissociation paths on the δ-Pu (100) surface. We then perform molecular dynamics simulations and minimum energy pathway calculations to determine the energetics of surface dissociation and subsurface diffusion on the (100) and (111) surfaces. Our approach allows for the efficient creation of multicenter repulsive energies with a relatively small investment in initial DFT calculations. Our efforts are particularly pertinent to studies that rely on quantum calculations for interpretation and validation, such as experimental determination of chemical reactivity both on surfaces and in condensed phases.

Compliance with dietary guidelines affects capillary recruitment in healthy middle-aged men and women.

PubMed

Govoni, Virginia; Sanders, Thomas A B; Reidlinger, Dianne P; Darzi, Julia; Berry, Sarah E E; Goff, Louise M; Seed, Paul T; Chowienczyk, Philip J; Hall, Wendy L

2017-04-01

Healthy microcirculation is important to maintain the health of tissues and organs, most notably the heart, kidney and retina. Single components of the diet such as salt, lipids and polyphenols may influence microcirculation, but the effects of dietary patterns that are consistent with current dietary guidelines are uncertain. It was hypothesized that compliance to UK dietary guidelines would have a favourable effect on skin capillary density/recruitment compared with a traditional British diet (control diet). A 12-week randomized controlled trial in men and women aged 40-70 years was used to test whether skin microcirculation, measured by skin video-capillaroscopy on the dorsum of the finger, influenced functional capillary density (number of capillaries perfused under basal conditions), structural capillary density (number of anatomical capillaries perfused during finger cuff inflation) and capillary recruitment (percentage difference between structural and functional capillary density). Microvascular measures were available for 137 subjects out of the 165 participants randomized to treatment. There was evidence of compliance to the dietary intervention, and participants randomized to follow dietary guidelines showed significant falls in resting supine systolic, diastolic and mean arterial pressure of 3.5, 2.6 and 2.9 mmHg compared to the control diet. There was no evidence of differences in capillary density, but capillary recruitment was 3.5 % (95 % CI 0.2, 6.9) greater (P = 0.04) on dietary guidelines compared with control. Adherence to dietary guidelines may help maintain a healthy microcirculation in middle-aged men and women. This study is registered at www.isrctn.com as ISRCTN92382106.

Calculation of spin-densities within the context of density functional theory. The crucial role of the correlation functional

NASA Astrophysics Data System (ADS)

Filatov, Michael; Cremer, Dieter

2005-09-01

It is demonstrated that the LYP correlation functional is not suited to be used for the calculation of electron spin resonance hyperfine structure (HFS) constants, nuclear magnetic resonance spin-spin coupling constants, magnetic, shieldings and other properties that require a balanced account of opposite- and equal-spin correlation, especially in the core region. In the case of the HFS constants of alkali atoms, LYP exaggerates opposite-spin correlation effects thus invoking too strong in-out correlation effects, an exaggerated spin-polarization pattern in the core shells of the atoms, and, consequently, too large HFS constants. Any correlation functional that provides a balanced account of opposite- and equal-spin correlation leads to improved HFS constants, which is proven by comparing results obtained with the LYP and the PW91 correlation functional. It is suggested that specific response properties are calculated with the PW91 rather than the LYP correlation functional.

Composite polarizability and the construction of an invariant function of refraction and mass density for solutions.

PubMed

Szymański, Krzysztof; Petrache, Horia I

2011-04-14

Re-examination of dynamical ionic polarizabilities in water solutions leads to the formulation of a solution function r(c), which combines the indices of refraction and mass densities of solutions. We show that this function should be independent of ionic concentration if the composite polarizabilities of hydrated solute clusters are constant. Using existing experimental data for a number of aqueous salt and organic solutions, we find that the r(c) function is either constant or varies linearly with concentration, in most cases with negligible slope. We use this function to compare ionic polarizabilities of crystals and aqueous solutions and to highlight how solute polarizabilities at infinite dilution scale with the electronic valence shell of cations and anions. The proposed r(c) function can be used generally to verify the consistency of experimental measurements and of simulation results, and it provides a test of assumptions in current theories of ionic polarizabilities.

Quantitative Tomography for Continuous Variable Quantum Systems

NASA Astrophysics Data System (ADS)

Landon-Cardinal, Olivier; Govia, Luke C. G.; Clerk, Aashish A.

2018-03-01

We present a continuous variable tomography scheme that reconstructs the Husimi Q function (Wigner function) by Lagrange interpolation, using measurements of the Q function (Wigner function) at the Padua points, conjectured to be optimal sampling points for two dimensional reconstruction. Our approach drastically reduces the number of measurements required compared to using equidistant points on a regular grid, although reanalysis of such experiments is possible. The reconstruction algorithm produces a reconstructed function with exponentially decreasing error and quasilinear runtime in the number of Padua points. Moreover, using the interpolating polynomial of the Q function, we present a technique to directly estimate the density matrix elements of the continuous variable state, with only a linear propagation of input measurement error. Furthermore, we derive a state-independent analytical bound on this error, such that our estimate of the density matrix is accompanied by a measure of its uncertainty.

Charge Transfer Enhancement in the D-π-A Type Porphyrin Dyes: A Density Functional Theory (DFT) and Time-Dependent Density Functional Theory (TD-DFT) Study.

PubMed

Kang, Guo-Jun; Song, Chao; Ren, Xue-Feng

2016-11-25

The electronic geometries and optical properties of two D-π-A type zinc porphyrin dyes (NCH₃-YD2 and TPhe-YD) were systematically investigated by density functional theory (DFT) and time-dependent density functional theory (TD-DFT) to reveal the origin of significantly altered charge transfer enhancement by changing the electron donor of the famous porphyrin-based sensitizer YD2-o-C8. The molecular geometries and photophysical properties of dyes before and after binding to the TiO₂ cluster were fully investigated. From the analyses of natural bond orbital (NBO), extended charge decomposition analysis (ECDA), and electron density variations (Δρ) between the excited state and ground state, it was found that the introduction of N(CH₃)₂ and 1,1,2-triphenylethene groups enhanced the intramolecular charge-transfer (ICT) character compared to YD2-o-C8. The absorption wavelength and transition possess character were significantly influenced by N(CH₃)₂ and 1,1,2-triphenylethene groups. NCH₃-YD2 with N(CH₃)₂ groups in the donor part is an effective way to improve the interactions between the dyes and TiO₂ surface, light having efficiency (LHE), and free energy change (ΔG inject ), which is expected to be an efficient dye for use in dye-sensitized solar cells (DSSCs).

Approaching the basis set limit for DFT calculations using an environment-adapted minimal basis with perturbation theory: Formulation, proof of concept, and a pilot implementation

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

Mao, Yuezhi; Horn, Paul R.; Mardirossian, Narbe

2016-07-28

Recently developed density functionals have good accuracy for both thermochemistry (TC) and non-covalent interactions (NC) if very large atomic orbital basis sets are used. To approach the basis set limit with potentially lower computational cost, a new self-consistent field (SCF) scheme is presented that employs minimal adaptive basis (MAB) functions. The MAB functions are optimized on each atomic site by minimizing a surrogate function. High accuracy is obtained by applying a perturbative correction (PC) to the MAB calculation, similar to dual basis approaches. Compared to exact SCF results, using this MAB-SCF (PC) approach with the same large target basis set producesmore » <0.15 kcal/mol root-mean-square deviations for most of the tested TC datasets, and <0.1 kcal/mol for most of the NC datasets. The performance of density functionals near the basis set limit can be even better reproduced. With further improvement to its implementation, MAB-SCF (PC) is a promising lower-cost substitute for conventional large-basis calculations as a method to approach the basis set limit of modern density functionals.« less

Numerical Optimization of Density Functional Tight Binding Models: Application to Molecules Containing Carbon, Hydrogen, Nitrogen, and Oxygen

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

Krishnapriyan, A.; Yang, P.; Niklasson, A. M. N.

New parametrizations for semiempirical density functional tight binding (DFTB) theory have been developed by the numerical optimization of adjustable parameters to minimize errors in the atomization energy and interatomic forces with respect to ab initio calculated data. Initial guesses for the radial dependences of the Slater- Koster bond integrals and overlap integrals were obtained from minimum basis density functional theory calculations. The radial dependences of the pair potentials and the bond and overlap integrals were represented by simple analytic functions. The adjustable parameters in these functions were optimized by simulated annealing and steepest descent algorithms to minimize the value ofmore » an objective function that quantifies the error between the DFTB model and ab initio calculated data. The accuracy and transferability of the resulting DFTB models for the C, H, N, and O system were assessed by comparing the predicted atomization energies and equilibrium molecular geometries of small molecules that were not included in the training data from DFTB to ab initio data. The DFTB models provide accurate predictions of the properties of hydrocarbons and more complex molecules containing C, H, N, and O.« less

Numerical Optimization of Density Functional Tight Binding Models: Application to Molecules Containing Carbon, Hydrogen, Nitrogen, and Oxygen

DOE PAGES

Krishnapriyan, A.; Yang, P.; Niklasson, A. M. N.; ...

2017-10-17

New parametrizations for semiempirical density functional tight binding (DFTB) theory have been developed by the numerical optimization of adjustable parameters to minimize errors in the atomization energy and interatomic forces with respect to ab initio calculated data. Initial guesses for the radial dependences of the Slater- Koster bond integrals and overlap integrals were obtained from minimum basis density functional theory calculations. The radial dependences of the pair potentials and the bond and overlap integrals were represented by simple analytic functions. The adjustable parameters in these functions were optimized by simulated annealing and steepest descent algorithms to minimize the value ofmore » an objective function that quantifies the error between the DFTB model and ab initio calculated data. The accuracy and transferability of the resulting DFTB models for the C, H, N, and O system were assessed by comparing the predicted atomization energies and equilibrium molecular geometries of small molecules that were not included in the training data from DFTB to ab initio data. The DFTB models provide accurate predictions of the properties of hydrocarbons and more complex molecules containing C, H, N, and O.« less

Changes in Structure and Functioning of Protist (Testate Amoebae) Communities Due to Conversion of Lowland Rainforest into Rubber and Oil Palm Plantations

PubMed Central

Krashevska, Valentyna; Klarner, Bernhard; Widyastuti, Rahayu; Maraun, Mark; Scheu, Stefan

2016-01-01

Large areas of tropical rainforest are being converted to agricultural and plantation land uses, but little is known of biodiversity and ecological functioning under these replacement land uses. We investigated the effects of conversion of rainforest into jungle rubber, intensive rubber and oil palm plantations on testate amoebae, diverse and functionally important protists in litter and soil. Living testate amoebae species richness, density and biomass were all lower in replacement land uses than in rainforest, with the impact being more pronounced in litter than in soil. Similar abundances of species of high and low trophic level in rainforest suggest that trophic interactions are more balanced, with a high number of functionally redundant species, than in rubber and oil palm. In contrast, plantations had a low density of high trophic level species indicating losses of functions. This was particularly so in oil palm plantations. In addition, the relative density of species with siliceous shells was >50% lower in the litter layer of oil palm and rubber compared to rainforest and jungle rubber. This difference suggests that rainforest conversion changes biogenic silicon pools and increases silicon losses. Overall, the lower species richness, density and biomass in plantations than in rainforest, and the changes in the functional composition of the testate amoebae community, indicate detrimental effects of rainforest conversion on the structure and functioning of microbial food webs. PMID:27463805

The ugrizYJHK luminosity distributions and densities from the combined MGC, SDSS and UKIDSS LAS data sets

NASA Astrophysics Data System (ADS)

Hill, David T.; Driver, Simon P.; Cameron, Ewan; Cross, Nicholas; Liske, Jochen; Robotham, Aaron

2010-05-01

We combine data from the Millennium Galaxy Catalogue, Sloan Digital Sky Survey and UKIRT Infrared Deep Sky Survey Large Area Survey to produce ugrizYJHK luminosity functions and densities from within a common, low-redshift volume (z < 0.1, ~ 71000h-31 Mpc3 for L* systems) with 100 per cent spectroscopic completeness. In the optical the fitted Schechter functions are comparable in shape to those previously reported values but with higher normalizations (typically 0, 30, 20, 15, 5 per cent higher φ* values in u, g, r, i, z, respectively, over those reported by the SDSS team). We attribute these to differences in the redshift ranges probed, incompleteness and adopted normalization methods. In the near-IR (NIR) we find significantly different Schechter function parameters (mainly in the M* values) to those previously reported and attribute this to the improvement in the quality of the imaging data over previous studies. This is the first homogeneous measurement of the extragalactic luminosity density which fully samples both the optical and NIR regimes. Unlike previous compilations that have noted a discontinuity between the optical and NIR regimes our homogeneous data set shows a smooth cosmic spectral energy distribution (CSED). After correcting for dust attenuation we compare our CSED to the expected values based on recent constraints on the cosmic star formation history and the initial mass function.

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.

Virial Coefficients for the Liquid Argon

NASA Astrophysics Data System (ADS)

Korth, Micheal; Kim, Saesun

2014-03-01

We begin with a geometric model of hard colliding spheres and calculate probability densities in an iterative sequence of calculations that lead to the pair correlation function. The model is based on a kinetic theory approach developed by Shinomoto, to which we added an interatomic potential for argon based on the model from Aziz. From values of the pair correlation function at various values of density, we were able to find viral coefficients of liquid argon. The low order coefficients are in good agreement with theoretical hard sphere coefficients, but appropriate data for argon to which these results might be compared is difficult to find.

Time-dependent density functional theory description of total photoabsorption cross sections

NASA Astrophysics Data System (ADS)

Tenorio, Bruno Nunes Cabral; Nascimento, Marco Antonio Chaer; Rocha, Alexandre Braga

2018-02-01

The time-dependent version of the density functional theory (TDDFT) has been used to calculate the total photoabsorption cross section of a number of molecules, namely, benzene, pyridine, furan, pyrrole, thiophene, phenol, naphthalene, and anthracene. The discrete electronic pseudo-spectra, obtained in a L2 basis set calculation were used in an analytic continuation procedure to obtain the photoabsorption cross sections. The ammonia molecule was chosen as a model system to compare the results obtained with TDDFT to those obtained with the linear response coupled cluster approach in order to make a link with our previous work and establish benchmarks.

Molecular docking and spectroscopic investigations aided by density functional theory of Parkinson's drug 2-(3,4-dihydroxyphenyl)ethylamine

NASA Astrophysics Data System (ADS)

Sherlin, Y. Sheeba; Vijayakumar, T.; Roy, S. D. D.; Jayakumar, V. S.

2018-05-01

Molecular geometry of Parkinson's drug 2-(3,4-Dihydroxyphenyl)ethylamine hydrochloride (Dopamine, DA) has been evaluated and compared with experimental XRD data. Molecular docking and vibrational spectral analysis of DA have been carried out using FT-Raman and FT-IR spectra aided by Density Functional Theory at B3LYP/6-311++G(d,p). The present investigation deals with the analysis of structural and spectral features responsible for drug activities, nature of hydrogen bonding interactions of the molecule and the correlation of Parkinson's nature with its molecular structural features.

First-principles calculation of the reflectance of shock-compressed xenon

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

Norman, G. E.; Saitov, I. M., E-mail: saitovilnur@gmail.com; Stegailov, V. V.

2015-05-15

Within electron density functional theory (DFT), the reflectance of radiation from shock-compressed xenon plasma is calculated. The dependence of the reflectance on the frequency of the incident radiation and on the plasma density is considered. The Fresnel formula is used. The expression for the longitudinal dielectric tensor in the long-wavelength limit is used to calculate the imaginary part of the dielectric function (DF). The real part of the DF is determined by the Kramers-Kronig transformation. The results are compared with experimental data. An approach is proposed to estimate the plasma frequency in shock-compressed xenon.

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.

Three-dimensional culture of rat calvarial osteoblasts in porous biodegradable polymers

NASA Technical Reports Server (NTRS)

Ishaug-Riley, S. L.; Crane-Kruger, G. M.; Yaszemski, M. J.; Mikos, A. G.

1998-01-01

Neonatal rat calvarial osteoblasts were cultured in 90% porous, 75:25 poly(DL-lactic-co-glycolic acid) (PLGA) foam scaffolds for up to 56 days to examine the effects of the cell seeding density, scaffold pore size, and foam thickness on the proliferation and function of the cells in this three-dimensional environment. Osteoblasts were seeded at either 11.1 x 10(5) or 22.1 x 10(5) cells per cm2 onto PLGA scaffolds having pore sizes in the range of 150-300 or 500-710 microm with a thickness of either 1.9 or 3.2 mm. After 1 day in culture, 75.6 and 68.6% of the seeded cells attached and proliferated on the 1.9 mm thick scaffolds of 150-300 microm pore size for the low and high seeding densities, respectively. The number of osteoblasts continued to increase throughout the study and eventually leveled off near 56 days, as indicated by a quantitative DNA assay. Osteoblast/foam constructs with a low cell seeding density achieved comparable DNA content and alkaline phosphatase (ALPase) activity after 14 days, and mineralization results after 56 days to those with a high cell seeding density. A maximum penetration depth of osseous tissue of 220+/-40 microm was reached after 56 days in the osteoblast/foam constructs of 150-300 microm pore size initially seeded with a high cell density. For constructs of 500-710 microm pore size, the penetration depth was 190+/-40 microm under the same conditions. Scaffold pore size and thickness did not significantly affect the proliferation or function of osteoblasts as demonstrated by DNA content, ALPase activity, and mineralized tissue formation. These data show that comparable bone-like tissues can be engineered in vitro over a 56 day period using different rat calvarial osteoblast seeding densities onto biodegradable polymer scaffolds with pore sizes in the range of 150-710 microm. When compared with the results of a previous study where similar polymer scaffolds were seeded and cultured with marrow stromal cells, this study demonstrates that PLGA foams are suitable substrates for osteoblast growth and differentiated function independent of cell source.

Abnormalities in cortical gray matter density in borderline personality disorder

PubMed Central

Rossi, Roberta; Lanfredi, Mariangela; Pievani, Michela; Boccardi, Marina; Rasser, Paul E; Thompson, Paul M; Cavedo, Enrica; Cotelli, Maria; Rosini, Sandra; Beneduce, Rossella; Bignotti, Stefano; Magni, Laura R; Rillosi, Luciana; Magnaldi, Silvia; Cobelli, Milena; Rossi, Giuseppe; Frisoni, Giovanni B

2015-01-01

Background Borderline personality disorder (BPD) is a chronic condition with a strong impact on patients‘ affective,cognitive and social functioning. Neuroimaging techniques offer invaluable tools to understand the biological substrate of the disease. We aimed to investigate gray matter alterations over the whole cortex in a group of Borderline Personality Disorder (BPD) patients compared to healthy controls (HC). Methods Magnetic resonance-based cortical pattern matching was used to assess cortical gray matter density (GMD) in 26 BPD patients and in their age- and sex-matched HC (age: 38±11; females: 16, 61%). Results BPD patients showed widespread lower cortical GMD compared to HC (4% difference) with peaks of lower density located in the dorsal frontal cortex, in the orbitofrontal cortex, the anterior and posterior cingulate, the right parietal lobe, the temporal lobe (medial temporal cortex and fusiform gyrus) and in the visual cortex (p<0.005). Our BPD subjects displayed a symmetric distribution of anomalies in the dorsal aspect of the cortical mantle, but a wider involvement of the left hemisphere in the mesial aspect in terms of lower density. A few restricted regions of higher density were detected in the right hemisphere. All regions remained significant after correction for multiple comparisons via permutation testing. Conclusions BPD patients feature specific morphology of the cerebral structures involved in cognitive and emotional processing and social cognition/mentalization, consistent with clinical and functional data. PMID:25561291

Dielectric properties of organic solvents from non-polarizable molecular dynamics simulation with electronic continuum model and density functional theory.

PubMed

Lee, Sanghun; Park, Sung Soo

2011-11-03

Dielectric constants of electrolytic organic solvents are calculated employing nonpolarizable Molecular Dynamics simulation with Electronic Continuum (MDEC) model and Density Functional Theory. The molecular polarizabilities are obtained by the B3LYP/6-311++G(d,p) level of theory to estimate high-frequency refractive indices while the densities and dipole moment fluctuations are computed using nonpolarizable MD simulations. The dielectric constants reproduced from these procedures are evaluated to provide a reliable approach for estimating the experimental data. An additional feature, two representative solvents which have similar molecular weights but are different dielectric properties, i.e., ethyl methyl carbonate and propylene carbonate, are compared using MD simulations and the distinctly different dielectric behaviors are observed at short times as well as at long times.

Gamma Strength Functions and Level Densities from 300 MeV Proton Scatttering at 0°

NASA Astrophysics Data System (ADS)

von Neumann-Cosel, Peter; Bassauer, Sergej; Martin, Dirk

The gamma strength function (GSF) as well as total level densities (LDs) in 208Pb and 96Mo were extracted from high-resolution forward angle inelastic proton scattering data taken at RCNP, Osaka, Japan, and compared to experimental results obtained with the Oslo method in order to test the validity of the Brink-Axel (BA) hypothesis in the energy region of the pygmy dipole resonance. The case of 208Pb is inconclusive because of strong fluctuations of the GSF due to the small level density in a doubly closed-shell nucleus. In 96Mo the data are consistent with the BA hypothesis. The good agreement of LDs provides an independent confirmation of the approach underlying the decomposition of GSF and LDs in Oslo-type experiments.

Characterization of Thin Film Materials using SCAN meta-GGA, an Accurate Nonempirical Density Functional

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

Buda, I. G.; Lane, C.; Barbiellini, B.

We discuss self-consistently obtained ground-state electronic properties of monolayers of graphene and a number of ’beyond graphene’ compounds, including films of transition-metal dichalcogenides (TMDs), using the recently proposed strongly constrained and appropriately normed (SCAN) meta-generalized gradient approximation (meta-GGA) to the density functional theory. The SCAN meta-GGA results are compared with those based on the local density approximation (LDA) as well as the generalized gradient approximation (GGA). As expected, the GGA yields expanded lattices and softened bonds in relation to the LDA, but the SCAN meta-GGA systematically improves the agreement with experiment. Our study suggests the efficacy of the SCAN functionalmore » for accurate modeling of electronic structures of layered materials in high-throughput calculations more generally.« less

Band-gap corrected density functional theory calculations for InAs/GaSb type II superlattices

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

Wang, Jianwei; Zhang, Yong

2014-12-07

We performed pseudopotential based density functional theory (DFT) calculations for GaSb/InAs type II superlattices (T2SLs), with bandgap errors from the local density approximation mitigated by applying an empirical method to correct the bulk bandgaps. Specifically, this work (1) compared the calculated bandgaps with experimental data and non-self-consistent atomistic methods; (2) calculated the T2SL band structures with varying structural parameters; (3) investigated the interfacial effects associated with the no-common-atom heterostructure; and (4) studied the strain effect due to lattice mismatch between the two components. This work demonstrates the feasibility of applying the DFT method to more exotic heterostructures and defect problemsmore » related to this material system.« less

Characterization of Thin Film Materials using SCAN meta-GGA, an Accurate Nonempirical Density Functional

DOE PAGES

Buda, I. G.; Lane, C.; Barbiellini, B.; ...

2017-03-23

We discuss self-consistently obtained ground-state electronic properties of monolayers of graphene and a number of ’beyond graphene’ compounds, including films of transition-metal dichalcogenides (TMDs), using the recently proposed strongly constrained and appropriately normed (SCAN) meta-generalized gradient approximation (meta-GGA) to the density functional theory. The SCAN meta-GGA results are compared with those based on the local density approximation (LDA) as well as the generalized gradient approximation (GGA). As expected, the GGA yields expanded lattices and softened bonds in relation to the LDA, but the SCAN meta-GGA systematically improves the agreement with experiment. Our study suggests the efficacy of the SCAN functionalmore » for accurate modeling of electronic structures of layered materials in high-throughput calculations more generally.« less

Enhanced von Weizsäcker Wang-Govind-Carter kinetic energy density functional for semiconductors

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

Shin, Ilgyou; Carter, Emily A., E-mail: eac@princeton.edu

2014-05-14

We propose a new form of orbital-free (OF) kinetic energy density functional (KEDF) for semiconductors that is based on the Wang-Govind-Carter (WGC99) nonlocal KEDF. We enhance within the latter the semi-local von Weizsäcker KEDF term, which is exact for a single orbital. The enhancement factor we introduce is related to the extent to which the electron density is localized. The accuracy of the new KEDF is benchmarked against Kohn-Sham density functional theory (KSDFT) by comparing predicted energy differences between phases, equilibrium volumes, and bulk moduli for various semiconductors, along with metal-insulator phase transition pressures. We also compare point defect andmore » (100) surface energies in silicon for a broad test of its applicability. This new KEDF accurately reproduces the exact non-interacting kinetic energy of KSDFT with only one additional adjustable parameter beyond the three parameters in the WGC99 KEDF; it exhibits good transferability between semiconducting to metallic silicon phases and between various III-V semiconductors without parameter adjustment. Overall, this KEDF is more accurate than previously proposed OF KEDFs (e.g., the Huang-Carter (HC) KEDF) for semiconductors, while the computational efficiency remains at the level of the WGC99 KEDF (several hundred times faster than the HC KEDF). This accurate, fast, and transferable new KEDF holds considerable promise for large-scale OFDFT simulations of metallic through semiconducting materials.« less

Ground-state densities from the Rayleigh-Ritz variation principle and from density-functional theory.

PubMed

Kvaal, Simen; Helgaker, Trygve

2015-11-14

The relationship between the densities of ground-state wave functions (i.e., the minimizers of the Rayleigh-Ritz variation principle) and the ground-state densities in density-functional theory (i.e., the minimizers of the Hohenberg-Kohn variation principle) is studied within the framework of convex conjugation, in a generic setting covering molecular systems, solid-state systems, and more. Having introduced admissible density functionals as functionals that produce the exact ground-state energy for a given external potential by minimizing over densities in the Hohenberg-Kohn variation principle, necessary and sufficient conditions on such functionals are established to ensure that the Rayleigh-Ritz ground-state densities and the Hohenberg-Kohn ground-state densities are identical. We apply the results to molecular systems in the Born-Oppenheimer approximation. For any given potential v ∈ L(3/2)(ℝ(3)) + L(∞)(ℝ(3)), we establish a one-to-one correspondence between the mixed ground-state densities of the Rayleigh-Ritz variation principle and the mixed ground-state densities of the Hohenberg-Kohn variation principle when the Lieb density-matrix constrained-search universal density functional is taken as the admissible functional. A similar one-to-one correspondence is established between the pure ground-state densities of the Rayleigh-Ritz variation principle and the pure ground-state densities obtained using the Hohenberg-Kohn variation principle with the Levy-Lieb pure-state constrained-search functional. In other words, all physical ground-state densities (pure or mixed) are recovered with these functionals and no false densities (i.e., minimizing densities that are not physical) exist. The importance of topology (i.e., choice of Banach space of densities and potentials) is emphasized and illustrated. The relevance of these results for current-density-functional theory is examined.

Involvement of mast cells and microvessels density in reactive lesions of oral cavity: A comparative immunohistochemical study.

PubMed

Ferreira, Stephany Vasco; Xavier, Flávia Caló Aquino; Freitas, Maria da Conceição Andrade de; Nunes, Fábio Daumas; Gurgel, Clarissa Araújo; Cangussu, Maria Cristina Teixeira; Martins, Manoela Domingues; Freitas, Valéria Souza; Dos Santos, Jean Nunes

2016-09-01

In view of the similarity of clinicopathological features between reactive lesions of the oral cavity, the objective of the present study was to investigate the density of MCs (mast cells) and microvessels in a series of these lesions. Thirty-seven cases of reactive lesions including fibrous hyperplasia (FH, n=10), inflammatory fibrous hyperplasia (IFH, n=10), peripheral giant cell lesion (PGCL, n=10) and lobular capillary hemangioma (LCH, n=7) were investigated using immunohistochemistry for mast cell tryptase and CD34. For comparative purposes, central giant cell lesions (CGCL, n=5) were included. A higher MC density was observed in LCH (37.01), while CGCL exhibited the lowest density (n=8.14). There was a significant difference in MC density when all reactive lesions were compared to CGCL (p=0.001). The largest mean density of microvessels was observed in LCH (n=21.69). The smallest number was observed in CGCL (n=6.24). There was a significant difference in microvessel density when the reactive lesions were compared to CGCL (p=0.003). There was a significant and direct correlation between the density of MCs and microvessels only for IFH (p=0.048) and CGCL (p=0.005). A significant and direct correlation between the mean density of MCs and microvessels was observed when the reactive lesions were analyzed as a whole (p=0.005). Our results suggest that mast cells contribute to the connective tissue framework and angiogenic function, as well as the development, of reactive lesions of the oral cavity, including FH, IFH, LCH and PGCL. Copyright © 2016 Elsevier GmbH. All rights reserved.

The virialization density of peaks with general density profiles under spherical collapse

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

Rubin, Douglas; Loeb, Abraham, E-mail: dsrubin@physics.harvard.edu, E-mail: aloeb@cfa.harvard.edu

2013-12-01

We calculate the non-linear virialization density, Δ{sub c}, of halos under spherical collapse from peaks with an arbitrary initial and final density profile. This is in contrast to the standard calculation of Δ{sub c} which assumes top-hat profiles. Given our formalism, the non-linear halo density can be calculated once the shape of the initial peak's density profile and the shape of the virialized halo's profile are provided. We solve for Δ{sub c} for halos in an Einstein de-Sitter and a ΛCDM universe. As examples, we consider power-law initial profiles as well as spherically averaged peak profiles calculated from the statisticsmore » of a Gaussian random field. We find that, depending on the profiles used, Δ{sub c} is smaller by a factor of a few to as much as a factor of 10 as compared to the density given by the standard calculation ( ≈ 200). Using our results, we show that, for halo finding algorithms that identify halos through an over-density threshold, the halo mass function measured from cosmological simulations can be enhanced at all halo masses by a factor of a few. This difference could be important when using numerical simulations to assess the validity of analytic models of the halo mass function.« less

Comparative studies of efficiency droop in polar and non-polar InGaN quantum wells

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

Davies, M. J.; Dawson, P.; Hammersley, S.

We report on a comparative study of efficiency droop in polar and non-polar InGaN quantum well structures at T = 10 K. To ensure that the experiments were carried out with identical carrier densities for any particular excitation power density, we used laser pulses of duration ∼100 fs at a repetition rate of 400 kHz. For both types of structures, efficiency droop was observed to occur for carrier densities of above 7 × 10{sup 11 }cm{sup −2 }pulse{sup −1} per quantum well; also both structures exhibited similar spectral broadening in the droop regime. These results show that efficiency droop is intrinsic in InGaN quantum wells, whether polar or non-polar,more » and is a function, specifically, of carrier density.« less

The Surface Density Distribution in the Solar Nebula

NASA Technical Reports Server (NTRS)

Davis, Sanford S.

2004-01-01

The commonly used minimum mass power law representation of the pre-solar nebula is reanalyzed using a new cumulative-mass-model. This model predicts a smoother surface density approximation compared with methods based on direct computation of surface density. The density is quantified using two independent analytical formulations. First, a best-fit transcendental function is applied directly to the basic planetary data. Next a solution to the time-dependent disk evolution equation is parametrically adapted to the solar nebula data. The latter model is shown to be a good approximation to the finite-size early Solar Nebula, and by extension to other extra solar protoplanetary disks.

Nonstationary Dynamics Data Analysis with Wavelet-SVD Filtering

NASA Technical Reports Server (NTRS)

Brenner, Marty; Groutage, Dale; Bessette, Denis (Technical Monitor)

2001-01-01

Nonstationary time-frequency analysis is used for identification and classification of aeroelastic and aeroservoelastic dynamics. Time-frequency multiscale wavelet processing generates discrete energy density distributions. The distributions are processed using the singular value decomposition (SVD). Discrete density functions derived from the SVD generate moments that detect the principal features in the data. The SVD standard basis vectors are applied and then compared with a transformed-SVD, or TSVD, which reduces the number of features into more compact energy density concentrations. Finally, from the feature extraction, wavelet-based modal parameter estimation is applied.

A comparison of non-local electron transport models relevant to inertial confinement fusion

NASA Astrophysics Data System (ADS)

Sherlock, Mark; Brodrick, Jonathan; Ridgers, Christopher

2017-10-01

We compare the reduced non-local electron transport model developed by Schurtz et al. to Vlasov-Fokker-Planck simulations. Two new test cases are considered: the propagation of a heat wave through a high density region into a lower density gas, and a 1-dimensional hohlraum ablation problem. We find the reduced model reproduces the peak heat flux well in the ablation region but significantly over-predicts the coronal preheat. The suitability of the reduced model for computing non-local transport effects other than thermal conductivity is considered by comparing the computed distribution function to the Vlasov-Fokker-Planck distribution function. It is shown that even when the reduced model reproduces the correct heat flux, the distribution function is significantly different to the Vlasov-Fokker-Planck prediction. Two simple modifications are considered which improve agreement between models in the coronal region. This work was performed under the auspices of the U.S. Department of Energy by Lawrence Livermore National Laboratory under Contract DE-AC52-07NA27344.

Properties of real metallic surfaces: Effects of density functional semilocality and van der Waals nonlocality

PubMed Central

Patra, Abhirup; Bates, Jefferson E.; Sun, Jianwei; Perdew, John P.

2017-01-01

We have computed the surface energies, work functions, and interlayer surface relaxations of clean (111), (100), and (110) surfaces of Al, Cu, Ru, Rh, Pd, Ag, Pt, and Au. We interpret the surface energy from liquid metal measurements as the mean of the solid-state surface energies over these three lowest-index crystal faces. We compare experimental (and random phase approximation) reference values to those of a family of nonempirical semilocal density functionals, from the basic local density approximation (LDA) to our most advanced general purpose meta-generalized gradient approximation, strongly constrained and appropriately normed (SCAN). The closest agreement is achieved by the simplest density functional LDA, and by the most sophisticated one, SCAN+rVV10 (Vydrov–Van Voorhis 2010). The long-range van der Waals interaction, incorporated through rVV10, increases the surface energies by about 10%, and increases the work functions by about 3%. LDA works for metal surfaces through two known error cancellations. The Perdew–Burke–Ernzerhof generalized gradient approximation tends to underestimate both surface energies (by about 24%) and work functions (by about 4%), yielding the least-accurate results. The amount by which a functional underestimates these surface properties correlates with the extent to which it neglects van der Waals attraction at intermediate and long range. Qualitative arguments are given for the signs of the van der Waals contributions to the surface energy and work function. A standard expression for the work function in Kohn–Sham (KS) theory is shown to be valid in generalized KS theory. Interlayer relaxations from different functionals are in reasonable agreement with one another, and usually with experiment. PMID:29042509

Morphometric analysis of primary graft non-function in liver transplantation.

PubMed

Vertemati, M; Sabatella, G; Minola, E; Gambacorta, M; Goffredi, M; Vizzotto, L

2005-04-01

Primary graft non-function (PNF) is a life-threatening condition that is thought to be the consequence of microcirculation injury. The aim of the present study was to assess, with a computerized morphometric model, the morphological changes at reperfusion in liver biopsy specimens from patients who developed PNF after liver transplantation. Biopsy specimens were obtained at maximum ischaemia and at the end of reperfusion. Morphology included many stereological parameters, such as volumes of all parenchymal components, surface density, size distribution and mean diameter of hepatocytes. Other variables examined were intensive care unit stay, degree of steatosis, serum liver function tests and ischaemic time. In the postoperative period, the PNF group showed elevated serum levels of alanine transferase, decreased daily rate of bile production and prothrombin activity. Blood lactates were significantly higher in the PNF group than in a control group. When comparing groups, the volumetric parameters related to hepatocytes and sinusoids and the surface densities of the hepatic cells showed an inverse relationship. At the end of reperfusion, in PNF group the volume fraction of hepatocyte cytoplasm was decreased; in contrast, the volume fraction of sinusoidal lumen was markedly increased. The cell profiles showed the same inverse trend: the surface density of the parenchymal border of hepatocytes was decreased in PNF when compared with the control group, while the surface density of the vascular border was increased. In the PNF group, the surface density of the sinusoidal bed was directly correlated with alanine transferase, daily rate of bile production, prothrombin activity and cold ischaemic time. The alterations in hepatic architecture, as demonstrated by morphometric analysis in liver transplant recipients that developed PNF, provide additional information that may represent useful viability markers of the graft to complement conventional histological analysis.

[Effects of land use changes on soil water conservation in Hainan Island, China].

PubMed

Wen, Zhi; Zhao, He; Liu, Lei; OuYang, Zhi Yun; Zheng, Hua; Mi, Hong Xu; Li, Yan Min

2017-12-01

In tropical areas, a large number of natural forests have been transformed into other plantations, which affected the water conservation function of terrestrial ecosystems. In order to clari-fy the effects of land use changes on soil water conservation function, we selected four typical land use types in the central mountainous region of Hainan Island, i.e., natural forests with stand age greater than 100 years (VF), secondary forests with stand age of 10 years (SF), areca plantations with stand age of 12 years (AF) and rubber plantations with stand age of 35 years (RF). The effects of land use change on soil water holding capacity and water conservation (presented by soil water index, SWI) were assessed. The results showed that, compared with VF, the soil water holding capacity index of other land types decreased in the top soil layer (0-10 cm). AF had the lowest soil water holding capacity in all soil layers. Soil water content and maximum water holding capacity were significantly related to canopy density, soil organic matter and soil bulk density, which indicated that canopy density, soil organic matter and compactness were important factors influencing soil water holding capacity. Compared to VF, soil water conservation of SF, AF and RF were reduced by 27.7%, 54.3% and 11.5%, respectively. The change of soil water conservation was inconsistent in different soil layers. Vegetation canopy density, soil organic matter and soil bulk density explained 83.3% of the variance of soil water conservation. It was suggested that land use conversion had significantly altered soil water holding capacity and water conservation function. RF could keep the soil water better than AF in the research area. Increasing soil organic matter and reducing soil compaction would be helpful to improve soil water holding capacity and water conservation function in land management.

An electron momentum spectroscopy and density functional theory study of the outer valence electronic structure of stella-2,6-dione

NASA Astrophysics Data System (ADS)

Nixon, K. L.; Wang, F.; Campbell, L.; Maddern, T.; Winkler, D.; Gleiter, R.; Loeb, P.; Weigold, E.; Brunger, M. J.

2003-07-01

We report on the first electron momentum spectroscopy (EMS) study into the outer valence electronic structure of the ground electronic state for the organic molecule stella-2,6-dione (C8H8O2). Experimentally measured binding-energy spectra are compared against a He(Ialpha) photoelectron spectroscopy result, while our derived momentum distributions (MDs) are compared against corresponding results from the plane wave impulse approximation (PWIA) level calculations. These computations employed density functional theory (DFT) basis states at the triple zeta valence polarization (TZVP) level, with a range of exchange-correlation (XC) functionals. A detailed comparison between the experimental and PWIA DFT-XC/TZVP calculated MDs enabled us to evaluate the accuracy of the various functionals, the Becke-Perdew (BP) XC functional being found to provide the most accurate description here. The importance of the through-bond interaction to the molecular orbitals (MOs) of stella-2,6-dione is demonstrated using the orbital imaging capability of EMS. Finally we show that the molecular geometry of this molecule, as derived from BP/TZVP, is in quite good agreement with corresponding independent experimental data.

Isobaric first-principles molecular dynamics of liquid water with nonlocal van der Waals interactions

NASA Astrophysics Data System (ADS)

Miceli, Giacomo; de Gironcoli, Stefano; Pasquarello, Alfredo

2015-01-01

We investigate the structural properties of liquid water at near ambient conditions using first-principles molecular dynamics simulations based on a semilocal density functional augmented with nonlocal van der Waals interactions. The adopted scheme offers the advantage of simulating liquid water at essentially the same computational cost of standard semilocal functionals. Applied to the water dimer and to ice Ih, we find that the hydrogen-bond energy is only slightly enhanced compared to a standard semilocal functional. We simulate liquid water through molecular dynamics in the NpH statistical ensemble allowing for fluctuations of the system density. The structure of the liquid departs from that found with a semilocal functional leading to more compact structural arrangements. This indicates that the directionality of the hydrogen-bond interaction has a diminished role as compared to the overall attractions, as expected when dispersion interactions are accounted for. This is substantiated through a detailed analysis comprising the study of the partial radial distribution functions, various local order indices, the hydrogen-bond network, and the selfdiffusion coefficient. The explicit treatment of the van der Waals interactions leads to an overall improved description of liquid water.

Comparative Study of Exchange-Correlation Functional and Potential for Evaluating Thermoelectric Transport Properties in d0 Perovskite Oxides

NASA Astrophysics Data System (ADS)

Ohkubo, Isao; Mori, Takao

2017-07-01

The influence of two different types of exchange-correlation functional/potential, namely, the generalized gradient approximation Perdew-Burke-Ernzerhof (GGA-PBE) functional and the modified Becke-Johnson (mBJ) potential, on the thermoelectric transport properties of d0 perovskite oxides (SrTiO3 and KTaO3) was investigated. The reduction of band dispersion induced by the mBJ scheme allows the improved prediction of band gap values by thelocal density approximation (LDA) and GGA, which increases the resolution of the increases in the density of states (DOS), carrier concentration, and effective mass near the conduction band edge. A comparison of the experimental effective mass values of d0 perovskite oxides shows that the effective mass values provided by the mBJ potential are similar to those provided by the GGA-PBE functional. Comparative analysis of the data obtained from Boltzmann theory calculations using the electronic structures determined with the GGA-PBE functional and the mBJ potential shows a difference in the transport coefficients owing to the increases in the DOS, carrier concentration, and effective mass induced by the mBJ scheme.

When Anatase Nanoparticles Become Bulklike: Properties of Realistic TiO2 Nanoparticles in the 1-6 nm Size Range from All Electron Relativistic Density Functional Theory Based Calculations.

PubMed

Lamiel-Garcia, Oriol; Ko, Kyoung Chul; Lee, Jin Yong; Bromley, Stefan T; Illas, Francesc

2017-04-11

All electron relativistic density functional theory (DFT) based calculations using numerical atom-centered orbitals have been carried out to explore the relative stability, atomic, and electronic structure of a series of stoichiometric TiO 2 anatase nanoparticles explicitly containing up to 1365 atoms as a function of size and morphology. The nanoparticles under scrutiny exhibit octahedral or truncated octahedral structures and span the 1-6 nm diameter size range. Initial structures were obtained using the Wulff construction, thus exhibiting the most stable (101) and (001) anatase surfaces. Final structures were obtained from geometry optimization with full relaxation of all structural parameters using both generalized gradient approximation (GGA) and hybrid density functionals. Results show that, for nanoparticles of a similar size, octahedral and truncated octahedral morphologies have comparable energetic stabilities. The electronic structure properties exhibit a clear trend converging to the bulk values as the size of the nanoparticles increases but with a marked influence of the density functional employed. Our results suggest that electronic structure properties, and hence reactivity, for the largest anatase nanoparticles considered in this study will be similar to those exhibited by even larger mesoscale particles or by bulk systems. Finally, we present compelling evidence that anatase nanoparticles become effectively bulklike when reaching a size of ∼20 nm diameter.

Clogging and depinning of ballistic active matter systems in disordered media

NASA Astrophysics Data System (ADS)

Reichhardt, C.; Reichhardt, C. J. O.

2018-05-01

We numerically examine ballistic active disks driven through a random obstacle array. Formation of a pinned or clogged state occurs at much lower obstacle densities for the active disks than for passive disks. As a function of obstacle density, we identify several distinct phases including a depinned fluctuating cluster state, a pinned single-cluster or jammed state, a pinned multicluster state, a pinned gel state, and a pinned disordered state. At lower active disk densities, a drifting uniform liquid forms in the absence of obstacles, but when even a small number of obstacles are introduced, the disks organize into a pinned phase-separated cluster state in which clusters nucleate around the obstacles, similar to a wetting phenomenon. We examine how the depinning threshold changes as a function of disk or obstacle density and find a crossover from a collectively pinned cluster state to a disordered plastic depinning transition as a function of increasing obstacle density. We compare this to the behavior of nonballistic active particles and show that as we vary the activity from completely passive to completely ballistic, a clogged phase-separated state appears in both the active and passive limits, while for intermediate activity, a readily flowing liquid state appears and there is an optimal activity level that maximizes the flux through the sample.

Properties of nuclei in the nobelium region studied within the covariant, Skyrme, and Gogny energy density functionals

DOE PAGES

Dobaczewski, J.; Afanasjev, A. V.; Bender, M.; ...

2015-07-29

In this study, we calculate properties of the ground and excited states of nuclei in the nobelium region for proton and neutron numbers of 92 ≤ Z ≤ 104 and 144 ≤ N ≤ 156, respectively. We use three different energy-density-functional (EDF) approaches, based on covariant, Skyrme, and Gogny functionals, each with two different parameter sets. A comparative analysis of the results obtained for quasiparticle spectra, odd–even and two-particle mass staggering, and moments of inertia allows us to identify single-particle and shell effects that are characteristic to these different models and to illustrate possible systematic uncertainties related to using themore » EDF modelling.« less

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.

Structure and orientational ordering in a fluid of elongated quadrupolar molecules

NASA Astrophysics Data System (ADS)

Singh, Ram Chandra

2013-01-01

A second-order density-functional theory is used to study the effect of quadrupolar interactions on the isotropic-nematic transition in a system of fluids of elongated molecules interacting via the Gay-Berne potential. The direct pair-correlation functions of the coexisting isotropic fluid that enter in the theory as input information are obtained by solving the Ornstein-Zernike equation using the Percus-Yevick integral equation theory in the (reduced) temperature range of 1.6≤T∗≤3.0 for different densities, temperatures and quadrupole moments. Using the harmonic coefficients of the direct pair-correlation functions, isotropic-nematic phase coexistence and thermodynamic parameters have been calculated. The theoretical results have been compared with the available computer simulation results.

Using Density Functional Theory (DFT) for the Calculation of Atomization Energies

NASA Technical Reports Server (NTRS)

Bauschlicher, Charles W., Jr.; Partridge, Harry; Langhoff, Stephen R. (Technical Monitor)

1995-01-01

The calculation of atomization energies using density functional theory (DFT), using the B3LYP hybrid functional, is reported. The sensitivity of the atomization energy to basis set is studied and compared with the coupled cluster singles and doubles approach with a perturbational estimate of the triples (CCSD(T)). Merging the B3LYP results with the G2(MP2) approach is also considered. It is found that replacing the geometry optimization and calculation of the zero-point energy by the analogous quantities computed using the B3LYP approach reduces the maximum error in the G2(MP2) approach. In addition to the 55 G2 atomization energies, some results for transition metal containing systems will also be presented.

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

Vibrational and thermal properties of β-HMX and TATB from dispersion corrected density functional theory

NASA Astrophysics Data System (ADS)

Landerville, Aaron C.; Oleynik, Ivan I.

2017-01-01

Dispersion Corrected Density Functional Theory (DFT+vdW) calculations are performed to predict vibrational and thermal properties of the bulk energetic materials (EMs) β-octahydrocyclotetramethylene-tetranitramine (β-HMX) and triaminotrinitrobenzene (TATB). DFT+vdW calculations of pressure-dependent crystal structure and the hydrostatic equation of state are followed by frozen-phonon calculations of their respective vibration spectra at each pressure. These are then used under the quasi-harmonic approximation to obtain zero-point and thermal free energy contributions to the pressure, resulting in pressure-volume-temperature (PVT) EOS for each material that are in excellent agreement with experiment. Heat capacities, and coefficients of thermal expansion as functions of temperature are also calculated and compared with experiment.

Electromagnetic Scattering From a Polygonal Thin Metallic Plate Using Quadrilateral Meshing

NASA Technical Reports Server (NTRS)

Deshpande, Manohar D.

2003-01-01

The problem of electromagnetic (EM) scattering from irregularly shaped, thin, metallic flat plates in free space is solved using the electric field integral equation (EFIE) approach in conjunction with the method of moments (MoM) with quadrilateral meshing. An irregularly shaped thin plate is discretized into quadrilateral patches and the unknown electric surface current over the plate is expressed in terms of proper basis functions over these patches. The basis functions for the electric surface current density that satisfy the proper boundary conditions on these quadrilateral patches are derived. The unknown surface current density on these quadrilateral patches is determined by setting up and solving the electric field integral equation by the application of the MoM. From the knowledge of the surface current density, the EM scattering from various irregularly shaped plates is determined and compared with the earlier published results. The novelty in the present approach is the use of quadrilateral patches instead of well known and often used triangular patches. The numerical results obtained using the quadrilateral patches compare favorably with measured results.

Comparison of volatility function technique for risk-neutral densities estimation

NASA Astrophysics Data System (ADS)

Bahaludin, Hafizah; Abdullah, Mimi Hafizah

2017-08-01

Volatility function technique by using interpolation approach plays an important role in extracting the risk-neutral density (RND) of options. The aim of this study is to compare the performances of two interpolation approaches namely smoothing spline and fourth order polynomial in extracting the RND. The implied volatility of options with respect to strike prices/delta are interpolated to obtain a well behaved density. The statistical analysis and forecast accuracy are tested using moments of distribution. The difference between the first moment of distribution and the price of underlying asset at maturity is used as an input to analyze forecast accuracy. RNDs are extracted from the Dow Jones Industrial Average (DJIA) index options with a one month constant maturity for the period from January 2011 until December 2015. The empirical results suggest that the estimation of RND using a fourth order polynomial is more appropriate to be used compared to a smoothing spline in which the fourth order polynomial gives the lowest mean square error (MSE). The results can be used to help market participants capture market expectations of the future developments of the underlying asset.

Optimization lighting layout based on gene density improved genetic algorithm for indoor visible light communications

NASA Astrophysics Data System (ADS)

Liu, Huanlin; Wang, Xin; Chen, Yong; Kong, Deqian; Xia, Peijie

2017-05-01

For indoor visible light communication system, the layout of LED lamps affects the uniformity of the received power on communication plane. In order to find an optimized lighting layout that meets both the lighting needs and communication needs, a gene density genetic algorithm (GDGA) is proposed. In GDGA, a gene indicates a pair of abscissa and ordinate of a LED, and an individual represents a LED layout in the room. The segmented crossover operation and gene mutation strategy based on gene density are put forward to make the received power on communication plane more uniform and increase the population's diversity. A weighted differences function between individuals is designed as the fitness function of GDGA for reserving the population having the useful LED layout genetic information and ensuring the global convergence of GDGA. Comparing square layout and circular layout, with the optimized layout achieved by the GDGA, the power uniformity increases by 83.3%, 83.1% and 55.4%, respectively. Furthermore, the convergence of GDGA is verified compared with evolutionary algorithm (EA). Experimental results show that GDGA can quickly find an approximation of optimal layout.

Quantitative analysis of the renal aging in rats. Stereological study.

PubMed

Melchioretto, Eduardo Felippe; Zeni, Marcelo; Veronez, Djanira Aparecida da Luz; Martins, Eduardo Lopes; Fraga, Rogério de

2016-05-01

To evaluate the renal function and the renal histological alterations through the stereology and morphometrics in rats submitted to the natural process of aging. Seventy two Wistar rats, divided in six groups. Each group was sacrificed in a different age: 3, 6, 9, 12, 18 and 24 months. It was performed right nephrectomy, stereological and morphometric analysis of the renal tissue (renal volume and weight, density of volume (Vv[glom]) and numerical density (Nv[glom]) of the renal glomeruli and average glomerular volume (Vol[glom])) and also it was evaluated the renal function for the dosage of serum creatinine and urea. There was significant decrease of the renal function in the oldest rats. The renal volume presented gradual increase during the development of the rats with the biggest values registered in the group of animals at 12 months of age and significant progressive decrease in older animals. Vv[glom] presented statistically significant gradual reduction between the groups and the Nv[glom] also decreased significantly. The renal function proved to be inferior in senile rats when compared to the young rats. The morphometric and stereological analysis evidenced renal atrophy, gradual reduction of the volume density and numerical density of the renal glomeruli associated to the aging process.

Calculation of the exchange coupling constants of copper binuclear systems based on spin-flip constricted variational density functional theory.

PubMed

Zhekova, Hristina R; Seth, Michael; Ziegler, Tom

2011-11-14

We have recently developed a methodology for the calculation of exchange coupling constants J in weakly interacting polynuclear metal clusters. The method is based on unrestricted and restricted second order spin-flip constricted variational density functional theory (SF-CV(2)-DFT) and is here applied to eight binuclear copper systems. Comparison of the SF-CV(2)-DFT results with experiment and with results obtained from other DFT and wave function based methods has been made. Restricted SF-CV(2)-DFT with the BH&HLYP functional yields consistently J values in excellent agreement with experiment. The results acquired from this scheme are comparable in quality to those obtained by accurate multi-reference wave function methodologies such as difference dedicated configuration interaction and the complete active space with second-order perturbation theory. © 2011 American Institute of Physics

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.

Identifying the distinct features of geometric structures for hole trapping to generate radicals on rutile TiO₂(110) in photooxidation using density functional theory calculations with hybrid functional.

PubMed

Wang, Dong; Wang, Haifeng; Hu, P

2015-01-21

Using density functional theory calculations with HSE 06 functional, we obtained the structures of spin-polarized radicals on rutile TiO2(110), which is crucial to understand the photooxidation at the atomic level, and further calculate the thermodynamic stabilities of these radicals. By analyzing the results, we identify the structural features for hole trapping in the system, and reveal the mutual effects among the geometric structures, the energy levels of trapped hole states and their hole trapping capacities. Furthermore, the results from HSE 06 functional are compared to those from DFT + U and the stability trend of radicals against the number of slabs is tested. The effect of trapped holes on two important steps of the oxygen evolution reaction, i.e. water dissociation and the oxygen removal, is investigated and discussed.

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.

Dispersion- and Exchange-Corrected Density Functional Theory for Sodium Ion Hydration.

PubMed

Soniat, Marielle; Rogers, David M; Rempe, Susan B

2015-07-14

A challenge in density functional theory is developing functionals that simultaneously describe intermolecular electron correlation and electron delocalization. Recent exchange-correlation functionals address those two issues by adding corrections important at long ranges: an atom-centered pairwise dispersion term to account for correlation and a modified long-range component of the electron exchange term to correct for delocalization. Here we investigate how those corrections influence the accuracy of binding free energy predictions for sodium-water clusters. We find that the dual-corrected ωB97X-D functional gives cluster binding energies closest to high-level ab initio methods (CCSD(T)). Binding energy decomposition shows that the ωB97X-D functional predicts the smallest ion-water (pairwise) interaction energy and larger multibody contributions for a four-water cluster than most other functionals - a trend consistent with CCSD(T) results. Also, ωB97X-D produces the smallest amounts of charge transfer and the least polarizable waters of the density functionals studied, which mimics the lower polarizability of CCSD. When compared with experimental binding free energies, however, the exchange-corrected CAM-B3LYP functional performs best (error <1 kcal/mol), possibly because of its parametrization to experimental formation enthalpies. For clusters containing more than four waters, "split-shell" coordination must be considered to obtain accurate free energies in comparison with experiment.

Lung function reductions associated with motor vehicle density in chronic obstructive pulmonary disease: a cross-sectional study.

PubMed

Nitschke, Monika; Appleton, Sarah L; Li, Qiaoyu; Tucker, Graeme R; Shah, Pushan; Bi, Peng; Pisaniello, Dino L; Adams, Robert J

2016-10-24

Motor vehicle-related air pollution can potentially impair lung function. The effect of pollution in people with compromised pulmonary function such as in COPD has not been previously investigated. To examine the association of lung function with motor vehicle density in people with spirometrically determined COPD in a cross-sectional study. In 2004-06, The North West Adelaide Health Study (NWAHS), a biomedical cohort of adults assessed pre and post-bronchodilator spirometry (n = 3,103). Traffic density, obtained from the motor vehicle inventory maintained by the South Australian Environment Protection Authority, was expressed as the daily numbers of vehicles travelling within a 200 m diameter zone around participants' geocoded residences. In subjects with COPD (FEV 1 /FVC <0.7, n = 221, 7.1 %), increasing daily vehicle density was associated with statistically significant decreases in lung function parameters after adjustment for smoking and socio-economic variables. Mean (95 % CI) post-bronchodilator % predicted FEV 1 was 81 % (76-87) in the low (≤7179/day) compared with 71 % (67-75) in the high (≥15,270/day) vehicle exposure group (p < 0.05). Linear regression analysis in all subjects with COPD showed significant decrements in post-bronchodilator FEV 1 /FVC ratio and % predicted FEV 1 of 0.03 and 0.05 % respectively per daily increase in 1000 vehicles. In men with COPD (n = 150), the corresponding reductions were 0.03 and 0.06 %. Smaller, non-significant decrements were seen in females. No difference was seen in those without COPD. Vehicle traffic density was associated with significant reductions in lung function in people with COPD. Urban planning should consider the health impacts for those with pre-existing respiratory conditions.

Prediction of three sigma maximum dispersed density for aerospace applications

NASA Technical Reports Server (NTRS)

Charles, Terri L.; Nitschke, Michael D.

1993-01-01

Free molecular heating (FMH) is caused by the transfer of energy during collisions between the upper atmosphere molecules and a space vehicle. The dispersed free molecular heating on a surface is an important constraint for space vehicle thermal analyses since it can be a significant source of heating. To reduce FMH to a spacecraft, the parking orbit is often designed to a higher altitude at the expense of payload capability. Dispersed FMH is a function of both space vehicle velocity and atmospheric density, however, the space vehicle velocity variations are insignificant when compared to the atmospheric density variations. The density of the upper atmosphere molecules is a function of altitude, but also varies with other environmental factors, such as solar activity, geomagnetic activity, location, and time. A method has been developed to predict three sigma maximum dispersed density for up to 15 years into the future. This method uses a state-of-the-art atmospheric density code, MSIS 86, along with 50 years of solar data, NASA and NOAA solar activity predictions for the next 15 years, and an Aerospace Corporation correlation to account for density code inaccuracies to generate dispersed maximum density ratios denoted as 'K-factors'. The calculated K-factors can be used on a mission unique basis to calculate dispersed density, and hence dispersed free molecular heating rates. These more accurate K-factors can allow lower parking orbit altitudes, resulting in increased payload capability.

Gold nanoparticles with different capping systems: an electronic and structural XAS analysis.

PubMed

López-Cartes, C; Rojas, T C; Litrán, R; Martínez-Martínez, D; de la Fuente, J M; Penadés, S; Fernández, A

2005-05-12

Gold nanoparticles (NPs) have been prepared with three different capping systems: a tetralkylammonium salt, an alkanethiol, and a thiol-derivatized neoglycoconjugate. Also gold NPs supported on a porous TiO(2) substrate have been investigated. X-ray absorption spectroscopy (XAS) has been used to determine the electronic behavior of the different capped/supported systems regarding the electron/hole density of d states. Surface and size effects, as well as the role of the microstructure, have been also studied through an exhaustive analysis of the EXAFS (extended X-ray absorption fine structure) data. Very small gold NPs functionalized with thiol-derivatized molecules show an increase in d-hole density at the gold site due to Au-S charge transfer. This effect is overcoming size effects (which lead to a slightly increase of the d-electron density) for high S:Au atomic ratios and core-shell microstructures where an atomically abrupt Au-S interface likely does not exist. It has been also shown that thiol functionalization of very small gold NPs is introducing a strong distortion as compared to fcc order. To the contrary, electron transfer from reduced support oxides to gold NPs can produce a higher increase in d-electron density at the gold site, as compared to naked gold clusters.

The phonon-coupling model for Skyrme forces

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

Lyutorovich, N.; Tselyaev, V.; Speth, J., E-mail: J.Speth@fz-juelich.de

2016-11-15

A short review on the self-consistent RPA based on the energy-density functional of the Skyrme type is given. We also present an extension of the RPA where the coupling of phonons to the single-particle states is considered. Within this approach we present numerical results which are compared with data. The self-consistent approach is compared with the Landau–Migdal theory. Here we derive from the self-consistent ph interaction, the Landau–Migdal parameters as well as their density dependence. In the Appendix a new derivation of the reduced matrix elements of the ph interaction is presented.

Self-consistent DFT +U method for real-space time-dependent density functional theory calculations

NASA Astrophysics Data System (ADS)

Tancogne-Dejean, Nicolas; Oliveira, Micael J. T.; Rubio, Angel

2017-12-01

We implemented various DFT+U schemes, including the Agapito, Curtarolo, and Buongiorno Nardelli functional (ACBN0) self-consistent density-functional version of the DFT +U method [Phys. Rev. X 5, 011006 (2015), 10.1103/PhysRevX.5.011006] within the massively parallel real-space time-dependent density functional theory (TDDFT) code octopus. We further extended the method to the case of the calculation of response functions with real-time TDDFT+U and to the description of noncollinear spin systems. The implementation is tested by investigating the ground-state and optical properties of various transition-metal oxides, bulk topological insulators, and molecules. Our results are found to be in good agreement with previously published results for both the electronic band structure and structural properties. The self-consistent calculated values of U and J are also in good agreement with the values commonly used in the literature. We found that the time-dependent extension of the self-consistent DFT+U method yields improved optical properties when compared to the empirical TDDFT+U scheme. This work thus opens a different theoretical framework to address the nonequilibrium properties of correlated systems.

A study of isotropic-nematic transition of quadrupolar Gay-Berne fluid using density-functional theory approach

NASA Astrophysics Data System (ADS)

Singh, Ram Chandra; Ram, Jokhan

2011-11-01

The effects of quadrupole moments on the isotropic-nematic (IN) phase transitions are studied using the density-functional theory (DFT) for a Gay-Berne (GB) fluid for a range of length-to-breadth parameters ? in the reduced temperature range ? . The pair-correlation functions of the isotropic phase, which enter into the DFT as input parameters are found by solving the Percus-Yevick integral equation theory. The method used involves an expansion of angle-dependent functions appearing in the integral equations in terms of spherical harmonics and the harmonic coefficients are obtained by an iterative algorithm. All the terms of harmonic coefficients which involve l indices up to less than or equal to 6 are considered. The numerical accuracy of the results depends on the number of spherical harmonic coefficients considered for each orientation-dependent function. As the length-to-breadth ratio of quadrupolar GB molecules is increased, the IN transition is seen to move to lower density (and pressure) at a given temperature. It has been observed that the DFT is good to study the IN transitions in such fluids. The theoretical results have also been compared with the computer simulation results wherever they are available.

Co-altered functional networks and brain structure in unmedicated patients with bipolar and major depressive disorders.

PubMed

He, Hao; Sui, Jing; Du, Yuhui; Yu, Qingbao; Lin, Dongdong; Drevets, Wayne C; Savitz, Jonathan B; Yang, Jian; Victor, Teresa A; Calhoun, Vince D

2017-12-01

Bipolar disorder (BD) and major depressive disorder (MDD) share similar clinical characteristics that often obscure the diagnostic distinctions between their depressive conditions. Both functional and structural brain abnormalities have been reported in these two disorders. However, the direct link between altered functioning and structure in these two diseases is unknown. To elucidate this relationship, we conducted a multimodal fusion analysis on the functional network connectivity (FNC) and gray matter density from MRI data from 13 BD, 40 MDD, and 33 matched healthy controls (HC). A data-driven fusion method called mCCA+jICA was used to identify the co-altered FNC and gray matter components. Comparing to HC, BD exhibited reduced gray matter density in the parietal and occipital cortices, which correlated with attenuated functional connectivity within sensory and motor networks, as well as hyper-connectivity in regions that are putatively engaged in cognitive control. In addition, lower gray matter density was found in MDD in the amygdala and cerebellum. High accuracy in discriminating across groups was also achieved by trained classification models, implying that features extracted from the fusion analysis hold the potential to ultimately serve as diagnostic biomarkers for mood disorders.

Relationship between PPARα mRNA expression and mitochondrial respiratory function and ultrastructure of the skeletal muscle of patients with COPD.

PubMed

Zhang, Jian-Qing; Long, Xiang-Yu; Xie, Yu; Zhao, Zhi-Huan; Fang, Li-Zhou; Liu, Ling; Fu, Wei-Ping; Shu, Jing-Kui; Wu, Jiang-Hai; Dai, Lu-Ming

2017-11-02

Peripheral muscle dysfunction is an important complication in patients with chronic obstructive pulmonary disease (COPD). The objective of this study was to explore the relationship between the levels of peroxisome proliferator-activated receptor α (PPARα) mRNA expression and the respiratory function and ultrastructure of mitochondria in the vastus lateralis of patients with COPD. Vastus lateralis biopsies were performed on 14 patients with COPD and 6 control subjects with normal lung function. PPARα mRNA levels in the muscle tissue were detected by real-time PCR. A Clark oxygen electrode was used to assess mitochondrial respiratory function. Mitochondrial number, fractional area in skeletal muscle cross-sections, and Z-line width were observed via transmission electron microscopy. The PPARα mRNA expression was significantly lower in COPD patients with low body mass index (BMIL) than in both COPD patients with normal body mass index (BMIN) and controls. Mitochondrial respiratory function (assessed by respiratory control ratio) was impaired in COPD patients, particularly in BMIL. Compared with that in the control group, mitochondrial number and fractional area were lower in the BMIL group, but were maintained in the BMIN group. Further, the Z-line became narrow in the BMIL group. PPARα mRNA expression was positively related to mitochondrial respiratory function and volume density. In COPD patients with BMIN, mitochondria volume density was maintained, while respiratory function decreased, whereas both volume density and respiratory function decreased in COPD patients with BMIL. PPARα mRNA expression levels are associated with decreased mitochondrial respiratory function and volume density, which may contribute to muscle dysfunction in COPD patients.

Density functional theory studies on the structures and electronic communication of meso-ferrocenylporphyrins: long range orbital coupling via porphyrin core.

PubMed

Zhang, Lijuan; Qi, Dongdong; Zhang, Yuexing; Bian, Yongzhong; Jiang, Jianzhuang

2011-02-01

The molecular and electronic structures together with the electronic absorption spectra of a series of metal free meso-ferrocenylporphyrins, namely 5-ferrocenylporphyrin (1), 5,10-diferrocenylporphyrin (2), 5,15-diferrocenylporphyrin (3), 5,10,15-triferrocenylporphyrin (4), and 5,10,15,20-tetraferrocenylporphyrin (5) have been studied with the density functional theory (DFT) and time-dependent density functional theory (TD-DFT) methods. For the purpose of comparative studies, metal free porphyrin without any ferrocenyl group (0) and isolated ferrocene (6) were also calculated. The effects of the number and position of meso-attached ferrocenyl substituents on their molecular and electronic structures, atomic charges, molecular orbitals, and electronic absorption spectra of 1-5 were systematically investigated. The orbital coupling is investigated in detail, explaining well the long range coupling of ferrocenyl substituents connected via porphyrin core and the systematic change in the electronic absorption spectra of porphyrin compounds. Copyright © 2010 Elsevier Inc. All rights reserved.

A general range-separated double-hybrid density-functional theory

NASA Astrophysics Data System (ADS)

Kalai, Cairedine; Toulouse, Julien

2018-04-01

A range-separated double-hybrid (RSDH) scheme which generalizes the usual range-separated hybrids and double hybrids is developed. This scheme consistently uses a two-parameter Coulomb-attenuating-method (CAM)-like decomposition of the electron-electron interaction for both exchange and correlation in order to combine Hartree-Fock exchange and second-order Møller-Plesset (MP2) correlation with a density functional. The RSDH scheme relies on an exact theory which is presented in some detail. Several semi-local approximations are developed for the short-range exchange-correlation density functional involved in this scheme. After finding optimal values for the two parameters of the CAM-like decomposition, the RSDH scheme is shown to have a relatively small basis dependence and to provide atomization energies, reaction barrier heights, and weak intermolecular interactions globally more accurate or comparable to range-separated MP2 or standard MP2. The RSDH scheme represents a new family of double hybrids with minimal empiricism which could be useful for general chemical applications.

Electric Field Induced Spectra of H sub 2 and D sub 2

NASA Technical Reports Server (NTRS)

Boyd, William Joseph

1974-01-01

The frequencies of four Q-branch lines of H2 and five Q-branch lines of D2 were measured as a function of density, and their shifts were observed to be in the linear region. The individual slopes and extrapolated zero density frequency of each line was determined. Hydrogen was measured for polarizability using the integrated intensity of the Q1(0) and S1(1), H2 absorption line. A highly automated technique for determining the response function of the spectrometer using digitally recorded data is presented. For the Q1(0) and Q1(1) lines of H2 the halfwidths were measured as a function of electric field intensity at constant pressure, and again at several densities and compared to previously measured widths. Technical and operational details of equipment built for this experiment, and for the five-meter Littrow spectrometer used, are described. Modifications of the spectrometer optics to accept the Stark cell are discussed.

Adaptive frozen orbital treatment for the fragment molecular orbital method combined with density-functional tight-binding

NASA Astrophysics Data System (ADS)

Nishimoto, Yoshio; Fedorov, Dmitri G.

2018-02-01

The exactly analytic gradient is derived and implemented for the fragment molecular orbital (FMO) method combined with density-functional tight-binding (DFTB) using adaptive frozen orbitals. The response contributions which arise from freezing detached molecular orbitals on the border between fragments are computed by solving Z-vector equations. The accuracy of the energy, its gradient, and optimized structures is verified on a set of representative inorganic materials and polypeptides. FMO-DFTB is applied to optimize the structure of a silicon nano-wire, and the results are compared to those of density functional theory and experiment. FMO accelerates the DFTB calculation of a boron nitride nano-ring with 7872 atoms by a factor of 406. Molecular dynamics simulations using FMO-DFTB applied to a 10.7 μm chain of boron nitride nano-rings, consisting of about 1.2 × 106 atoms, reveal the rippling and twisting of nano-rings at room temperature.

Phonon and magnetic structure in δ-plutonium from density-functional theory

DOE PAGES

Söderlind, Per; Zhou, F.; Landa, A.; ...

2015-10-30

We present phonon properties of plutonium metal obtained from a combination of density-functional-theory (DFT) electronic structure and the recently developed compressive sensing lattice dynamics (CSLD). The CSLD model is here trained on DFT total energies of several hundreds of quasi-random atomic configurations for best possible accuracy of the phonon properties. The calculated phonon dispersions compare better with experiment than earlier results obtained from dynamical mean-field theory. The density-functional model of the electronic structure consists of disordered magnetic moments with all relativistic effects and explicit orbital-orbital correlations. The magnetic disorder is approximated in two ways: (i) a special quasi-random structure andmore » (ii) the disordered-local-moment (DLM) method within the coherent potential approximation. Magnetism in plutonium has been debated intensely, However, the present magnetic approach for plutonium is validated by the close agreement between the predicted magnetic form factor and that of recent neutron-scattering experiments.« less

Analytic derivation of the next-to-leading order proton structure function F2p(x ,Q2) based on the Laplace transformation

NASA Astrophysics Data System (ADS)

Khanpour, Hamzeh; Mirjalili, Abolfazl; Tehrani, S. Atashbar

2017-03-01

An analytical solution based on the Laplace transformation technique for the Dokshitzer-Gribov-Lipatov-Altarelli-Parisi (DGLAP) evolution equations is presented at next-to-leading order accuracy in perturbative QCD. This technique is also applied to extract the analytical solution for the proton structure function, F2p(x ,Q2) , in the Laplace s space. We present the results for the separate parton distributions of all parton species, including valence quark densities, the antiquark and strange sea parton distribution functions (PDFs), and the gluon distribution. We successfully compare the obtained parton distribution functions and the proton structure function with the results from GJR08 [Gluck, Jimenez-Delgado, and Reya, Eur. Phys. J. C 53, 355 (2008)], 10.1140/epjc/s10052-007-0462-9 and KKT12 [Khanpour, Khorramian, and Tehrani, J. Phys. G 40, 045002 (2013)], 10.1088/0954-3899/40/4/045002 parametrization models as well as the x -space results using QCDnum code. Our calculations show a very good agreement with the available theoretical models as well as the deep inelastic scattering (DIS) experimental data throughout the small and large values of x . The use of our analytical solution to extract the parton densities and the proton structure function is discussed in detail to justify the analysis method, considering the accuracy and speed of calculations. Overall, the accuracy we obtain from the analytical solution using the inverse Laplace transform technique is found to be better than 1 part in 104 to 105. We also present a detailed QCD analysis of nonsinglet structure functions using all available DIS data to perform global QCD fits. In this regard we employ the Jacobi polynomial approach to convert the results from Laplace s space to Bjorken x space. The extracted valence quark densities are also presented and compared to the JR14, MMHT14, NNPDF, and CJ15 PDFs sets. We evaluate the numerical effects of target mass corrections (TMCs) and higher twist (HT) terms on various structure functions, and compare fits to data with and without these corrections.

Comparative studies on molecular structure, vibrational spectra and hyperpolarizabilies of NLO chromophore Ethyl 4-Dimethylaminobenzoate

NASA Astrophysics Data System (ADS)

Amalanathan, M.; Jasmine, G. Femina; Roy, S. Dawn Dharma

2017-08-01

The molecular structure, vibrational spectra and polarizabilities of Ethyl 4-Dimethylaminobenzoate (EDAB) was investigated by density functional theory employing Becke's three parameter hybrid exchange functional with Lee-Yang-Parr (B3LYP) co-relational functional involving 6-311++G(d,p) basis set and compared with some other levels. A detailed interpretation of the IR and Raman spectra of EDBA have been reported and analyzed. Complete vibrational assignments of the vibrational modes have been done on the basis of the potential energy distribution (TED) using VEDA software. The molecular electrostatic potential mapped onto total density surface has been obtained. A study on the electronic properties, such as absorption wavelength, and frontier molecular orbitals energy, was performed using DFT approach. The stability of the molecule arising from hyper conjugative interactions and accompanying charge delocalization has been analyzed using natural bond orbital (NBO) analysis. The natural and Mulliken charge also calculated and compared with different level of calculation. The dipole moment, polarizability and first, second order hyperpolarizabilities of the title molecule were calculated and compared with the experimental values. The energy gap between frontier orbitals has been used along with electric moments and first order hyperpolarizability, to understand the non linear optical (NLO) activity of the molecule. The NLO activity of molecule was confirmed by SHG analysis.

A density functional theory (DFT) and time-dependent density functional theory (TDDFT) study on optical transitions in oligo(p-phenylenevinylene)-fullerene dyads and the applicability to resonant energy transfer.

PubMed

Toivonen, Teemu L J; Hukka, Terttu I

2007-06-07

The optical transitions of three different size oligo(p-phenylenevinylene)-fullerene dyads (OPV(n)-MPC(60); n = 2-4) and of the corresponding separate molecules are studied using density functional theory (DFT) and time-dependent density functional theory. The DFT is used to determine the geometries and the electronic structures of the ground states. Transition energies and excited-state structures are obtained from the TDDFT calculations. Resonant energy transfer from OPV(n) to MPC(60) is also studied and the Fermi golden rule is used, along with two simple models to describe the electronic coupling to calculate the energy transfer rates. The hybrid-type PBE0 functional is used with a split-valence basis set augmented with a polarization function (SV(P)) in calculations and the calculated results are compared to the corresponding experimental results. The calculated PBE0 spectra of the OPV(n)-MPC(60) dyads correspond to the experimental spectra very well and are approximately sums of the absorption spectra of the separate OPV(n) and MPC(60) molecules. Also, the absorption energies of OPV(n) and MPC(60) and the emission energies of OPV(n) are predicted well with the PBE0 functional. The PBE0 calculated resonant energy transfer rates are in a good agreement with the experimental rates and show the existence of many possible pathways for energy transfer from the first excited singlet states of the OPV(n) molecules to the MPC(60) molecule.

Simultaneous measurements of work function and H‒ density including caesiation of a converter surface

NASA Astrophysics Data System (ADS)

Cristofaro, S.; Friedl, R.; Fantz, U.

2017-08-01

Negative hydrogen ion sources rely on the surface conversion of neutral atomic hydrogen and positive hydrogen ions to H-. The efficiency of this process depends on the actual work function of the converter surface. By introducing caesium into the source the work function decreases, enhancing the negative ion yield. In order to study the impact of the work function on the H- surface production at similar conditions to the ones in ion sources for fusion devices like ITER and DEMO, fundamental investigations are performed in a flexible laboratory experiment. The work function of the converter surface can be absolutely measured by photoelectric effect, while a newly installed cavity ring-down spectroscopy system (CRDS) measures the H- density. The CRDS is firstly tested and characterized by investigations on H- volume production. Caesiation of a stainless steel sample is then performed in vacuum and the plasma effect on the Cs layer is investigated also for long plasma-on times. A minimum work function of (1.9±0.1) eV is reached after some minutes of plasma treatment, resulting in a reduction by a value of 0.8 eV compared to vacuum measurements. The H- density above the surface is (2.1±0.5)×1015 m-3. With further plasma exposure of the caesiated surface, the work function increases up to 3.75 eV, due to the impinging plasma particles which gradually remove the Cs layer. As a result, the H- density decreases by a factor of at least 2.

Variational Optimization of the Second-Order Density Matrix Corresponding to a Seniority-Zero Configuration Interaction Wave Function.

PubMed

Poelmans, Ward; Van Raemdonck, Mario; Verstichel, Brecht; De Baerdemacker, Stijn; Torre, Alicia; Lain, Luis; Massaccesi, Gustavo E; Alcoba, Diego R; Bultinck, Patrick; Van Neck, Dimitri

2015-09-08

We perform a direct variational determination of the second-order (two-particle) density matrix corresponding to a many-electron system, under a restricted set of the two-index N-representability P-, Q-, and G-conditions. In addition, we impose a set of necessary constraints that the two-particle density matrix must be derivable from a doubly occupied many-electron wave function, i.e., a singlet wave function for which the Slater determinant decomposition only contains determinants in which spatial orbitals are doubly occupied. We rederive the two-index N-representability conditions first found by Weinhold and Wilson and apply them to various benchmark systems (linear hydrogen chains, He, N2, and CN(-)). This work is motivated by the fact that a doubly occupied many-electron wave function captures in many cases the bulk of the static correlation. Compared to the general case, the structure of doubly occupied two-particle density matrices causes the associate semidefinite program to have a very favorable scaling as L(3), where L is the number of spatial orbitals. Since the doubly occupied Hilbert space depends on the choice of the orbitals, variational calculation steps of the two-particle density matrix are interspersed with orbital-optimization steps (based on Jacobi rotations in the space of the spatial orbitals). We also point to the importance of symmetry breaking of the orbitals when performing calculations in a doubly occupied framework.

Evaluation of atmospheric density models and preliminary functional specifications for the Langley Atmospheric Information Retrieval System (LAIRS)

NASA Technical Reports Server (NTRS)

Lee, T.; Boland, D. F., Jr.

1980-01-01

This document presents the results of an extensive survey and comparative evaluation of current atmosphere and wind models for inclusion in the Langley Atmospheric Information Retrieval System (LAIRS). It includes recommended models for use in LAIRS, estimated accuracies for the recommended models, and functional specifications for the development of LAIRS.

Numerical methods for the inverse problem of density functional theory

DOE PAGES

Jensen, Daniel S.; Wasserman, Adam

2017-07-17

Here, the inverse problem of Kohn–Sham density functional theory (DFT) is often solved in an effort to benchmark and design approximate exchange-correlation potentials. The forward and inverse problems of DFT rely on the same equations but the numerical methods for solving each problem are substantially different. We examine both problems in this tutorial with a special emphasis on the algorithms and error analysis needed for solving the inverse problem. Two inversion methods based on partial differential equation constrained optimization and constrained variational ideas are introduced. We compare and contrast several different inversion methods applied to one-dimensional finite and periodic modelmore » systems.« less

Estimation of the four-wave mixing noise probability-density function by the multicanonical Monte Carlo method.

PubMed

Neokosmidis, Ioannis; Kamalakis, Thomas; Chipouras, Aristides; Sphicopoulos, Thomas

2005-01-01

The performance of high-powered wavelength-division multiplexed (WDM) optical networks can be severely degraded by four-wave-mixing- (FWM-) induced distortion. The multicanonical Monte Carlo method (MCMC) is used to calculate the probability-density function (PDF) of the decision variable of a receiver, limited by FWM noise. Compared with the conventional Monte Carlo method previously used to estimate this PDF, the MCMC method is much faster and can accurately estimate smaller error probabilities. The method takes into account the correlation between the components of the FWM noise, unlike the Gaussian model, which is shown not to provide accurate results.

The use of copulas to practical estimation of multivariate stochastic differential equation mixed effects models

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

Rupšys, P.

A system of stochastic differential equations (SDE) with mixed-effects parameters and multivariate normal copula density function were used to develop tree height model for Scots pine trees in Lithuania. A two-step maximum likelihood parameter estimation method is used and computational guidelines are given. After fitting the conditional probability density functions to outside bark diameter at breast height, and total tree height, a bivariate normal copula distribution model was constructed. Predictions from the mixed-effects parameters SDE tree height model calculated during this research were compared to the regression tree height equations. The results are implemented in the symbolic computational language MAPLE.

Measurements of surface-pressure fluctuations on the XB-70 airplane at local Mach numbers up to 2.45

NASA Technical Reports Server (NTRS)

Lewis, T. L.; Dods, J. B., Jr.; Hanly, R. D.

1973-01-01

Measurements of surface-pressure fluctuations were made at two locations on the XB-70 airplane for nine flight-test conditions encompassing a local Mach number range from 0.35 to 2.45. These measurements are presented in the form of estimated power spectral densities, coherence functions, and narrow-band-convection velocities. The estimated power spectral densities compared favorably with wind-tunnel data obtained by other experimenters. The coherence function and convection velocity data supported conclusions by other experimenters that low-frequency surface-pressure fluctuations consist of small-scale turbulence components with low convection velocity.

Time-dependent spin-density-functional-theory description of He+-He collisions

NASA Astrophysics Data System (ADS)

Baxter, Matthew; Kirchner, Tom; Engel, Eberhard

2017-09-01

Theoretical total cross-section results for all ionization and capture processes in the He+-He collision system are presented in the approximate impact energy range of 10-1000 keV/amu. Calculations were performed within the framework of time-dependent spin-density functional theory. The Krieger-Li-Iafrate approximation was used to determine an accurate exchange-correlation potential in the exchange-only limit. The results of two models, one where electron translation factors in the orbitals used to calculate the potential are ignored and another where partial electron translation factors are included, are compared with available experimental data as well as a selection of previous theoretical calculations.

Application of Density Functional Theory to Systems Containing Metal Atoms

NASA Technical Reports Server (NTRS)

Bauschlicher, Charles W., Jr.

2006-01-01

The accuracy of density functional theory (DFT) for problems involving metal atoms is considered. The DFT results are compared with experiment as well as results obtained using the coupled cluster approach. The comparisons include geometries, frequencies, and bond energies. The systems considered include MO2, M(OH)+n, MNO+, and MCO+2. The DFT works well for frequencies and geometries, even in case with symmetry breaking; however, some examples have been found where the symmetry breaking is quite severe and the DFT methods do not work well. The calculation of bond energies is more difficult and examples of successes as well as failures of DFT will be given.

Spacing distribution functions for the one-dimensional point-island model with irreversible attachment

NASA Astrophysics Data System (ADS)

González, Diego Luis; Pimpinelli, Alberto; Einstein, T. L.

2011-07-01

We study the configurational structure of the point-island model for epitaxial growth in one dimension. In particular, we calculate the island gap and capture zone distributions. Our model is based on an approximate description of nucleation inside the gaps. Nucleation is described by the joint probability density pnXY(x,y), which represents the probability density to have nucleation at position x within a gap of size y. Our proposed functional form for pnXY(x,y) describes excellently the statistical behavior of the system. We compare our analytical model with extensive numerical simulations. Our model retains the most relevant physical properties of the system.

Numerical methods for the inverse problem of density functional theory

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

Jensen, Daniel S.; Wasserman, Adam

Here, the inverse problem of Kohn–Sham density functional theory (DFT) is often solved in an effort to benchmark and design approximate exchange-correlation potentials. The forward and inverse problems of DFT rely on the same equations but the numerical methods for solving each problem are substantially different. We examine both problems in this tutorial with a special emphasis on the algorithms and error analysis needed for solving the inverse problem. Two inversion methods based on partial differential equation constrained optimization and constrained variational ideas are introduced. We compare and contrast several different inversion methods applied to one-dimensional finite and periodic modelmore » systems.« less

Correlation techniques and measurements of wave-height statistics

NASA Technical Reports Server (NTRS)

Guthart, H.; Taylor, W. C.; Graf, K. A.; Douglas, D. G.

1972-01-01

Statistical measurements of wave height fluctuations have been made in a wind wave tank. The power spectral density function of temporal wave height fluctuations evidenced second-harmonic components and an f to the minus 5th power law decay beyond the second harmonic. The observations of second harmonic effects agreed very well with a theoretical prediction. From the wave statistics, surface drift currents were inferred and compared to experimental measurements with satisfactory agreement. Measurements were made of the two dimensional correlation coefficient at 15 deg increments in angle with respect to the wind vector. An estimate of the two-dimensional spatial power spectral density function was also made.

A statistical analysis of the elastic distortion and dislocation density fields in deformed crystals

DOE PAGES

Mohamed, Mamdouh S.; Larson, Bennett C.; Tischler, Jonathan Z.; ...

2015-05-18

The statistical properties of the elastic distortion fields of dislocations in deforming crystals are investigated using the method of discrete dislocation dynamics to simulate dislocation structures and dislocation density evolution under tensile loading. Probability distribution functions (PDF) and pair correlation functions (PCF) of the simulated internal elastic strains and lattice rotations are generated for tensile strain levels up to 0.85%. The PDFs of simulated lattice rotation are compared with sub-micrometer resolution three-dimensional X-ray microscopy measurements of rotation magnitudes and deformation length scales in 1.0% and 2.3% compression strained Cu single crystals to explore the linkage between experiment and the theoreticalmore » analysis. The statistical properties of the deformation simulations are analyzed through determinations of the Nye and Kr ner dislocation density tensors. The significance of the magnitudes and the length scales of the elastic strain and the rotation parts of dislocation density tensors are demonstrated, and their relevance to understanding the fundamental aspects of deformation is discussed.« less

Coupling of ab initio density functional theory and molecular dynamics for the multiscale modeling of carbon nanotubes

NASA Astrophysics Data System (ADS)

Ng, T. Y.; Yeak, S. H.; Liew, K. M.

2008-02-01

A multiscale technique is developed that couples empirical molecular dynamics (MD) and ab initio density functional theory (DFT). An overlap handshaking region between the empirical MD and ab initio DFT regions is formulated and the interaction forces between the carbon atoms are calculated based on the second-generation reactive empirical bond order potential, the long-range Lennard-Jones potential as well as the quantum-mechanical DFT derived forces. A density of point algorithm is also developed to track all interatomic distances in the system, and to activate and establish the DFT and handshaking regions. Through parallel computing, this multiscale method is used here to study the dynamic behavior of single-walled carbon nanotubes (SWCNTs) under asymmetrical axial compression. The detection of sideways buckling due to the asymmetrical axial compression is reported and discussed. It is noted from this study on SWCNTs that the MD results may be stiffer compared to those with electron density considerations, i.e. first-principle ab initio methods.

Solvatochromic shifts from coupled-cluster theory embedded in density functional theory

NASA Astrophysics Data System (ADS)

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

2013-09-01

Building on the framework recently reported for determining general response properties for frozen-density embedding [S. Höfener, A. S. P. Gomes, and L. Visscher, J. Chem. Phys. 136, 044104 (2012)], 10.1063/1.3675845, in this work we report a first implementation of an embedded coupled-cluster in density-functional theory (CC-in-DFT) scheme for electronic excitations, where only the response of the active subsystem is taken into account. The formalism is applied to the calculation of coupled-cluster excitation energies of water and uracil in aqueous solution. We find that the CC-in-DFT results are in good agreement with reference calculations and experimental results. The accuracy of calculations is mainly sensitive to factors influencing the correlation treatment (basis set quality, truncation of the cluster operator) and to the embedding treatment of the ground-state (choice of density functionals). This allows for efficient approximations at the excited state calculation step without compromising the accuracy. This approximate scheme makes it possible to use a first principles approach to investigate environment effects with specific interactions at coupled-cluster level of theory at a cost comparable to that of calculations of the individual subsystems in vacuum.

The correlation function for density perturbations in an expanding universe. I - Linear theory

NASA Technical Reports Server (NTRS)

Mcclelland, J.; Silk, J.

1977-01-01

The evolution of the two-point correlation function for adiabatic density perturbations in the early universe is studied. Analytical solutions are obtained for the evolution of linearized spherically symmetric adiabatic density perturbations and the two-point correlation function for these perturbations in the radiation-dominated portion of the early universe. The results are then extended to the regime after decoupling. It is found that: (1) adiabatic spherically symmetric perturbations comparable in scale with the maximum Jeans length would survive the radiation-dominated regime; (2) irregular fluctuations are smoothed out up to the scale of the maximum Jeans length in the radiation era, but regular fluctuations might survive on smaller scales; (3) in general, the only surviving structures for irregularly shaped adiabatic density perturbations of arbitrary but finite scale in the radiation regime are the size of or larger than the maximum Jeans length in that regime; (4) infinite plane waves with a wavelength smaller than the maximum Jeans length but larger than the critical dissipative damping scale could survive the radiation regime; and (5) black holes would also survive the radiation regime and might accrete sufficient mass after decoupling to nucleate the formation of galaxies.

Does low bone density influence symptoms and functional status in patients with fibromyalgia? Observations from rural South India.

PubMed

Babu, Abraham Samuel; Ikbal, Faizal M; Noone, Manjula Sukumari; Joseph, Anupama Naomi; Danda, Debashish

2015-11-01

The presence of more than one musculoskeletal disease has been found to impair quality of life (QoL). The influence of low bone mineral density (BMD) on symptoms and function in those with fibromyalgia syndrome (FMS) is unknown. A cross sectional study was carried out on 158 patients attending camps in rural South India. BMD was determined using quantitative ultrasound of the distal radius. Symptoms and function were assessed using a visual analogue scale (VAS) and the Fibromyalgia Impact Questionnaire (FIQ). Low BMD was seen in 81.6% (129/158) of the persons screened. FMS was seen in 37/158 persons, of which 31/37 (83.7%) had low BMD. FMS with low bone density leads to higher levels of pain and a poorer QoL compared to those without FMS. Coexisting musculoskeletal problems could also contribute to this. Therefore, medical practitioners and rehabilitation specialists should consider screening for bone density among those with FMS and should use this information to decide appropriate therapies to reduce pain and improve QoL. © 2015 Asia Pacific League of Associations for Rheumatology and Wiley Publishing Asia Pty Ltd.

Dielectric function and plasmons in graphene: A self-consistent-field calculation within a Markovian master equation formalism

DOE PAGES

Karimi, F.; Davoody, A. H.; Knezevic, I.

2016-05-12

We introduce a method for calculating the dielectric function of nanostructures with an arbitrary band dispersion and Bloch wave functions. The linear response of a dissipative electronic system to an external electromagnetic field is calculated by a self-consistent-field approach within a Markovian master equation formalism (SCF-MMEF) coupled with full-wave electromagnetic equations. The SCF-MMEF accurately accounts for several concurrent scattering mechanisms. The method captures interband electron-hole-pair generation, as well as the interband and intraband electron scattering with phonons and impurities. We employ the SCF-MMEF to calculate the dielectric function, complex conductivity, and loss function for supported graphene. From the loss-function maximum,more » we obtain plasmon dispersion and propagation length for different substrate types [nonpolar diamondlike carbon (DLC) and polar SiO 2 and hBN], impurity densities, carrier densities, and temperatures. Plasmons on the two polar substrates are suppressed below the highest surface phonon energy, while the spectrum is broad on the nonpolar DLC. Plasmon propagation lengths are comparable on polar and nonpolar substrates and are on the order of tens of nanometers, considerably shorter than previously reported. As a result, they improve with fewer impurities, at lower temperatures, and at higher carrier densities.« less

Reformulation of Density Functional Theory for N-Representable Densities and the Resolution of the v-Representability Problem

DOE PAGES

Gonis, A.; Zhang, X. G.; Stocks, G. M.; ...

2015-10-23

Density functional theory for the case of general, N-representable densities is reformulated in terms of density functional derivatives of expectation values of operators evaluated with wave functions leading to a density, making no reference to the concept of potential. The developments provide a complete solution of the v-representability problem by establishing a mathematical procedure that determines whether a density is v-representable and in the case of an affirmative answer determines the potential (within an additive constant) as a derivative with respect to the density of a constrained search functional. It also establishes the existence of an energy functional of themore » density that, for v-representable densities, assumes its minimum value at the density describing the ground state of an interacting many-particle system. The theorems of Hohenberg and Kohn emerge as special cases of the formalism.« less

No difference in long-term trunk muscle strength, cross-sectional area, and density in patients with chronic low back pain 7 to 11 years after lumbar fusion versus cognitive intervention and exercises.

PubMed

Froholdt, Anne; Holm, Inger; Keller, Anne; Gunderson, Ragnhild B; Reikeraas, Olav; Brox, Jens I

2011-08-01

Reduced muscle strength and density observed at 1 year after lumbar fusion may deteriorate more in the long term. To compare the long-term effect of lumbar fusion and cognitive intervention and exercises on muscle strength, cross-sectional area, density, and self-rated function in patients with chronic low back pain (CLBP) and disc degeneration. Randomized controlled study with a follow-up examination at 8.5 years (range, 7-11 years). Patients with CLBP and disc degeneration randomized to either instrumented posterolateral fusion of one or both of the two lower lumbar levels or a 3-week cognitive intervention and exercise program were included. Isokinetic muscle strength was measured by a Cybex 6000 (Cybex-Lumex, Inc., Ronkonkoma, NY, USA). All patients had previous experience with the test procedure. The back extension (E) flexion (F) muscles were tested, and the E/F ratios were calculated. Cross-sectional area and density of the back muscles were measured at the L3-L4 segment by computed tomography. Patients rated their function by the General Function Score. Trunk muscle strength, cross-sectional area, density, and self-rated function. Fifty-five patients (90%) were included at long-term follow-up. There were no significant differences in cross-sectional area, density, muscle strength, or self-rated function between the two groups. The cognitive intervention and exercise group increased trunk muscle extension significantly (p<.05), and both groups performed significantly better on trunk muscle flexion tests (p<.01) at long-term follow-up. On average, self-rated function improved by 56%, cross-sectional area was reduced by 8.5%, and muscle density was reduced by 27%. Although this study did not assess the morphology of muscles likely damaged by surgery, trunk muscle strength and cross-sectional area above the surgical levels are not different between those who had lumbar fusion or cognitive intervention and exercises at 7- to 11-year follow-up. Copyright © 2011 Elsevier Inc. All rights reserved.

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.

Molecular mechanics and structure of the fluid-solid interface in simple fluids

NASA Astrophysics Data System (ADS)

Wang, Gerald J.; Hadjiconstantinou, Nicolas G.

2017-09-01

Near a fluid-solid interface, the fluid spatial density profile is highly nonuniform at the molecular scale. This nonuniformity can have profound effects on the dynamical behavior of the fluid and has been shown to play an especially important role when modeling a wide variety of nanoscale heat and momentum transfer phenomena. We use molecular-mechanics arguments and molecular-dynamics (MD) simulations to develop a better understanding of the structure of the first fluid layer directly adjacent to the solid in the layering regime, as delineated by a nondimensional number that compares the effects of wall-fluid interaction to thermal energy. Using asymptotic analysis of the Nernst-Planck equation, we show that features of the fluid density profile close to the wall, such as the areal density of the first layer ΣFL (defined as the number of atoms in this layer per unit of fluid-solid interfacial area), can be expressed as polynomial functions of the fluid average density ρave. This is found to be in agreement with MD simulations, which also show that the width of the first layer hFL is a linear function of the average density and only a weak function of the temperature T . These results can be combined to show that, for system average densities corresponding to a dense fluid (ρave≥0.7 ), the ratio C ≡ΣFLρavehFL, representing a density enhancement with respect to the bulk fluid, depends only weakly on temperature and is essentially independent of density. Further MD simulations suggest that the above results, nominally valid for large systems (solid in contact with semi-infinite fluid), also describe fluid-solid interfaces under considerable nanoconfinement, provided ρave is appropriately defined.

Effects of plasmon pole models on the G0W0 electronic structure of various oxides

NASA Astrophysics Data System (ADS)

Miglio, A.; Waroquiers, D.; Antonius, G.; Giantomassi, M.; Stankovski, M.; Côté, M.; Gonze, X.; Rignanese, G.-M.

2012-09-01

The electronic properties of three different oxides (ZnO, SnO2 and SiO2) are investigated within many-body perturbation theory in the G 0 W 0 approximation. The frequency dependence of the dielectric function is either approximated using two different well-established plasmon-pole models (one of which enforces the fulfillment of the f-sum rule) or treated explicitly by means of the contour-deformation approach. Comparing these results, it is found that the plasmon-pole model enforcing the f-sum rule gives less accurate results for all three oxides. The calculated electronic properties are also compared with the available experimental data and previous ab initio results, focusing on the d state binding energies. The G 0 W 0 approach leads to significantly improved band gaps with respect to calculations based on the density functional theory in the local density approximation.

Very large scale wavefunction orthogonalization in Density Functional Theory electronic structure calculations

NASA Astrophysics Data System (ADS)

Bekas, C.; Curioni, A.

2010-06-01

Enforcing the orthogonality of approximate wavefunctions becomes one of the dominant computational kernels in planewave based Density Functional Theory electronic structure calculations that involve thousands of atoms. In this context, algorithms that enjoy both excellent scalability and single processor performance properties are much needed. In this paper we present block versions of the Gram-Schmidt method and we show that they are excellent candidates for our purposes. We compare the new approach with the state of the art practice in planewave based calculations and find that it has much to offer, especially when applied on massively parallel supercomputers such as the IBM Blue Gene/P Supercomputer. The new method achieves excellent sustained performance that surpasses 73 TFLOPS (67% of peak) on 8 Blue Gene/P racks (32 768 compute cores), while it enables more than a two fold decrease in run time when compared with the best competing methodology.

Density functional study on the mechanism for the highly active palladium monolayer supported on titanium carbide for the oxygen reduction reaction

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

Mao, Jianjun; Zhang, Yanxing; Chu, Xingli

2016-05-28

The adsorption, diffusion, and dissociation of O{sub 2} on the palladium monolayer supported on TiC(001) surface, MLPd/TiC(001), are investigated using ab initio density functional theory calculations. Strong adhesion of palladium monolayer to the TiC(001) support, accompanied by a modification of electronic structure of the supported palladium, is evidenced. Compared with Pt(111) surface, the MLPd/TiC(001) can enhance the adsorption of O{sub 2}, leading to comparable dissociation barrier and a smaller diffusion barrier of O{sub 2}. Whilst the adsorption strength of atomic O (the dissociation product of O{sub 2}) on MLPd/TiC(001) is similar to that on the Pt(111) surface, possessing high mobility,more » our theoretical results indicate that MLPd/TiC(001) may serve as a good catalyst for the oxygen reduction reaction.« less

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

Pair potentials for warm dense matter and their application to x-ray Thomson scattering in aluminum and beryllium.

PubMed

Harbour, L; Dharma-Wardana, M W C; Klug, D D; Lewis, L J

2016-11-01

Ultrafast laser experiments yield increasingly reliable data on warm dense matter, but their interpretation requires theoretical models. We employ an efficient density functional neutral-pseudoatom hypernetted-chain (NPA-HNC) model with accuracy comparable to ab initio simulations and which provides first-principles pseudopotentials and pair potentials for warm-dense matter. It avoids the use of (i) ad hoc core-repulsion models and (ii) "Yukawa screening" and (iii) need not assume ion-electron thermal equilibrium. Computations of the x-ray Thomson scattering (XRTS) spectra of aluminum and beryllium are compared with recent experiments and with density-functional-theory molecular-dynamics (DFT-MD) simulations. The NPA-HNC structure factors, compressibilities, phonons, and conductivities agree closely with DFT-MD results, while Yukawa screening gives misleading results. The analysis of the XRTS data for two of the experiments, using two-temperature quasi-equilibrium models, is supported by calculations of their temperature relaxation times.

Density-based clustering analyses to identify heterogeneous cellular sub-populations

NASA Astrophysics Data System (ADS)

Heaster, Tiffany M.; Walsh, Alex J.; Landman, Bennett A.; Skala, Melissa C.

2017-02-01

Autofluorescence microscopy of NAD(P)H and FAD provides functional metabolic measurements at the single-cell level. Here, density-based clustering algorithms were applied to metabolic autofluorescence measurements to identify cell-level heterogeneity in tumor cell cultures. The performance of the density-based clustering algorithm, DENCLUE, was tested in samples with known heterogeneity (co-cultures of breast carcinoma lines). DENCLUE was found to better represent the distribution of cell clusters compared to Gaussian mixture modeling. Overall, DENCLUE is a promising approach to quantify cell-level heterogeneity, and could be used to understand single cell population dynamics in cancer progression and treatment.

On the asymptotic improvement of supervised learning by utilizing additional unlabeled samples - Normal mixture density case

NASA Technical Reports Server (NTRS)

Shahshahani, Behzad M.; Landgrebe, David A.

1992-01-01

The effect of additional unlabeled samples in improving the supervised learning process is studied in this paper. Three learning processes. supervised, unsupervised, and combined supervised-unsupervised, are compared by studying the asymptotic behavior of the estimates obtained under each process. Upper and lower bounds on the asymptotic covariance matrices are derived. It is shown that under a normal mixture density assumption for the probability density function of the feature space, the combined supervised-unsupervised learning is always superior to the supervised learning in achieving better estimates. Experimental results are provided to verify the theoretical concepts.

Quantitative analysis of the guest-concentration dependence of the mobility in a disordered fluorene-arylamine host-guest system in the guest-to-guest regime

NASA Astrophysics Data System (ADS)

Nicolai, H. T.; Hof, A. J.; Lu, M.; Blom, P. W. M.; de Vries, R. J.; Coehoorn, R.

2011-11-01

The charge transport in a polyspirobifluorene derivative with copolymerized N,N,N',N'-tetraaryldiamino biphenyl (TAD) hole transport units is investigated as a function of the TAD content. For TAD concentrations larger than 5%, guest-to-guest transport is observed. It is demonstrated that in this regime the charge carrier density dependent mobility can be described consistently with the extended Gaussian disorder model, with a density of hopping sites which is proportional to the TAD concentration and comparable to the molecular density.

MC-PDFT can calculate singlet-triplet splittings of organic diradicals

NASA Astrophysics Data System (ADS)

Stoneburner, Samuel J.; Truhlar, Donald G.; Gagliardi, Laura

2018-02-01

The singlet-triplet splittings of a set of diradical organic molecules are calculated using multiconfiguration pair-density functional theory (MC-PDFT), and the results are compared with those obtained by Kohn-Sham density functional theory (KS-DFT) and complete active space second-order perturbation theory (CASPT2) calculations. We found that MC-PDFT, even with small and systematically defined active spaces, is competitive in accuracy with CASPT2, and it yields results with greater accuracy and precision than Kohn-Sham DFT with the parent functional. MC-PDFT also avoids the challenges associated with spin contamination in KS-DFT. It is also shown that MC-PDFT is much less computationally expensive than CASPT2 when applied to larger active spaces, and this illustrates the promise of this method for larger diradical organic systems.

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.

The density structure and star formation rate of non-isothermal polytropic turbulence

NASA Astrophysics Data System (ADS)

Federrath, Christoph; Banerjee, Supratik

2015-04-01

The interstellar medium of galaxies is governed by supersonic turbulence, which likely controls the star formation rate (SFR) and the initial mass function (IMF). Interstellar turbulence is non-universal, with a wide range of Mach numbers, magnetic fields strengths and driving mechanisms. Although some of these parameters were explored, most previous works assumed that the gas is isothermal. However, we know that cold molecular clouds form out of the warm atomic medium, with the gas passing through chemical and thermodynamic phases that are not isothermal. Here we determine the role of temperature variations by modelling non-isothermal turbulence with a polytropic equation of state (EOS), where pressure and temperature are functions of gas density, P˜ ρ ^Γ, T ˜ ρΓ - 1. We use grid resolutions of 20483 cells and compare polytropic exponents Γ = 0.7 (soft EOS), Γ = 1 (isothermal EOS) and Γ = 5/3 (stiff EOS). We find a complex network of non-isothermal filaments with more small-scale fragmentation occurring for Γ < 1, while Γ > 1 smoothes out density contrasts. The density probability distribution function (PDF) is significantly affected by temperature variations, with a power-law tail developing at low densities for Γ > 1. In contrast, the PDF becomes closer to a lognormal distribution for Γ ≲ 1. We derive and test a new density variance-Mach number relation that takes Γ into account. This new relation is relevant for theoretical models of the SFR and IMF, because it determines the dense gas mass fraction of a cloud, from which stars form. We derive the SFR as a function of Γ and find that it decreases by a factor of ˜5 from Γ = 0.7 to 5/3.

Altered Right Ventricular Kinetic Energy Work Density and Viscous Energy Dissipation in Patients with Pulmonary Arterial Hypertension: A Pilot Study Using 4D Flow MRI.

PubMed

Han, Q Joyce; Witschey, Walter R T; Fang-Yen, Christopher M; Arkles, Jeffrey S; Barker, Alex J; Forfia, Paul R; Han, Yuchi

2015-01-01

Right ventricular (RV) function has increasingly being recognized as an important predictor for morbidity and mortality in patients with pulmonary arterial hypertension (PAH). The increased RV after-load increase RV work in PAH. We used time-resolved 3D phase contrast MRI (4D flow MRI) to derive RV kinetic energy (KE) work density and energy loss in the pulmonary artery (PA) to better characterize RV work in PAH patients. 4D flow and standard cardiac cine images were obtained in ten functional class I/II patients with PAH and nine healthy subjects. For each individual, we calculated the RV KE work density and the amount of viscous dissipation in the PA. PAH patients had alterations in flow patterns in both the RV and the PA compared to healthy subjects. PAH subjects had significantly higher RV KE work density than healthy subjects (94.7±33.7 mJ/mL vs. 61.7±14.8 mJ/mL, p = 0.007) as well as a much greater percent PA energy loss (21.1±6.4% vs. 2.2±1.3%, p = 0.0001) throughout the cardiac cycle. RV KE work density and percent PA energy loss had mild and moderate correlations with RV ejection fraction. This study has quantified two kinetic energy metrics to assess RV function using 4D flow. RV KE work density and PA viscous energy loss not only distinguished healthy subjects from patients, but also provided distinction amongst PAH patients. These metrics hold promise as imaging markers for RV function.

Density and viscosity of some partially carbonated aqueous alkanolamine solutions and their blends

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

Weiland, R.H.; Dingman, J.C.; Cronin, D.B.

1998-05-01

Very little information is available concerning the effect of acid gas loading on the physical properties of amine-treating solutions flowing through the absorption and regeneration columns used in gas processing. The densities and viscosities of partially carbonated monoethanolamine (MEA), diethanolamine (DEA), and N-methyldiethanolamine (MDEA) solutions were measured at 298 K. With increasing carbon dioxide loadings, significant increases in both density and viscosity were observed. These results were combined with literature data to produce correlations for alkanolamine solution density and viscosity as a function of amine concentration, carbon dioxide loading, and temperature. The resulting single-amine correlations were used to predict themore » densities and viscosities of DEA + MDEA and MEA + MDEA blends. Predictions are compared with data measured for these blends.« less

Four-Component Relativistic Density-Functional Theory Calculations of Nuclear Spin-Rotation Constants: Relativistic Effects in p-Block Hydrides.

PubMed

Komorovsky, Stanislav; Repisky, Michal; Malkin, Elena; Demissie, Taye B; Ruud, Kenneth

2015-08-11

We present an implementation of the nuclear spin-rotation (SR) constants based on the relativistic four-component Dirac-Coulomb Hamiltonian. This formalism has been implemented in the framework of the Hartree-Fock and Kohn-Sham theory, allowing assessment of both pure and hybrid exchange-correlation functionals. In the density-functional theory (DFT) implementation of the response equations, a noncollinear generalized gradient approximation (GGA) has been used. The present approach enforces a restricted kinetic balance condition for the small-component basis at the integral level, leading to very efficient calculations of the property. We apply the methodology to study relativistic effects on the spin-rotation constants by performing calculations on XHn (n = 1-4) for all elements X in the p-block of the periodic table and comparing the effects of relativity on the nuclear SR tensors to that observed for the nuclear magnetic shielding tensors. Correlation effects as described by the density-functional theory are shown to be significant for the spin-rotation constants, whereas the differences between the use of GGA and hybrid density functionals are much smaller. Our calculated relativistic spin-rotation constants at the DFT level of theory are only in fair agreement with available experimental data. It is shown that the scaling of the relativistic effects for the spin-rotation constants (varying between Z(3.8) and Z(4.5)) is as strong as for the chemical shieldings but with a much smaller prefactor.

Resolution-of-identity stochastic time-dependent configuration interaction for dissipative electron dynamics in strong fields.

PubMed

Klinkusch, Stefan; Tremblay, Jean Christophe

2016-05-14

In this contribution, we introduce a method for simulating dissipative, ultrafast many-electron dynamics in intense laser fields. The method is based on the norm-conserving stochastic unraveling of the dissipative Liouville-von Neumann equation in its Lindblad form. The N-electron wave functions sampling the density matrix are represented in the basis of singly excited configuration state functions. The interaction with an external laser field is treated variationally and the response of the electronic density is included to all orders in this basis. The coupling to an external environment is included via relaxation operators inducing transition between the configuration state functions. Single electron ionization is represented by irreversible transition operators from the ionizing states to an auxiliary continuum state. The method finds its efficiency in the representation of the operators in the interaction picture, where the resolution-of-identity is used to reduce the size of the Hamiltonian eigenstate basis. The zeroth-order eigenstates can be obtained either at the configuration interaction singles level or from a time-dependent density functional theory reference calculation. The latter offers an alternative to explicitly time-dependent density functional theory which has the advantage of remaining strictly valid for strong field excitations while improving the description of the correlation as compared to configuration interaction singles. The method is tested on a well-characterized toy system, the excitation of the low-lying charge transfer state in LiCN.

Final Technical Report for DE-SC0001878 [Theory and Simulation of Defects in Oxide Materials

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

Chelikowsky, James R.

2014-04-14

We explored a wide variety of oxide materials and related problems, including materials at the nanoscale and generic problems associated with oxide materials such as the development of more efficient computational tools to examine these materials. We developed and implemented methods to understand the optical and structural properties of oxides. For ground state properties, our work is predominantly based on pseudopotentials and density functional theory (DFT), including new functionals and going beyond the local density approximation (LDA): LDA+U. To study excited state properties (quasiparticle and optical excitations), we use time dependent density functional theory, the GW approach, and GW plusmore » Bethe-Salpeter equation (GW-BSE) methods based on a many-body Green function approaches. Our work focused on the structural, electronic, optical and magnetic properties of defects (such as oxygen vacancies) in hafnium oxide, titanium oxide (both bulk and clusters) and related materials. We calculated the quasiparticle defect states and charge transition levels of oxygen vacancies in monoclinic hafnia. we presented a milestone G0W0 study of two of the crystalline phases of dye-sensitized TiO{sub 2} clusters. We employed hybrid density functional theory to examine the electronic structure of sexithiophene/ZnO interfaces. To identify the possible effect of epitaxial strain on stabilization of the ferromagnetic state of LaCoO{sub 3} (LCO), we compare the total energy of the magnetic and nonmagnetic states of the strained theoretical bulk structure.« less

Resolution-of-identity stochastic time-dependent configuration interaction for dissipative electron dynamics in strong fields

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

Klinkusch, Stefan; Tremblay, Jean Christophe

In this contribution, we introduce a method for simulating dissipative, ultrafast many-electron dynamics in intense laser fields. The method is based on the norm-conserving stochastic unraveling of the dissipative Liouville-von Neumann equation in its Lindblad form. The N-electron wave functions sampling the density matrix are represented in the basis of singly excited configuration state functions. The interaction with an external laser field is treated variationally and the response of the electronic density is included to all orders in this basis. The coupling to an external environment is included via relaxation operators inducing transition between the configuration state functions. Single electronmore » ionization is represented by irreversible transition operators from the ionizing states to an auxiliary continuum state. The method finds its efficiency in the representation of the operators in the interaction picture, where the resolution-of-identity is used to reduce the size of the Hamiltonian eigenstate basis. The zeroth-order eigenstates can be obtained either at the configuration interaction singles level or from a time-dependent density functional theory reference calculation. The latter offers an alternative to explicitly time-dependent density functional theory which has the advantage of remaining strictly valid for strong field excitations while improving the description of the correlation as compared to configuration interaction singles. The method is tested on a well-characterized toy system, the excitation of the low-lying charge transfer state in LiCN.« less

Long-range-corrected Rung 3.5 density functional approximations

NASA Astrophysics Data System (ADS)

Janesko, Benjamin G.; Proynov, Emil; Scalmani, Giovanni; Frisch, Michael J.

2018-03-01

Rung 3.5 functionals are a new class of approximations for density functional theory. They provide a flexible intermediate between exact (Hartree-Fock, HF) exchange and semilocal approximations for exchange. Existing Rung 3.5 functionals inherit semilocal functionals' limitations in atomic cores and density tails. Here we address those limitations using range-separated admixture of HF exchange. We present three new functionals. LRC-ωΠLDA combines long-range HF exchange with short-range Rung 3.5 ΠLDA exchange. SLC-ΠLDA combines short- and long-range HF exchange with middle-range ΠLDA exchange. LRC-ωΠLDA-AC incorporates a combination of HF, semilocal, and Rung 3.5 exchange in the short range, based on an adiabatic connection. We test these in a new Rung 3.5 implementation including up to analytic fourth derivatives. LRC-ωΠLDA and SLC-ΠLDA improve atomization energies and reaction barriers by a factor of 8 compared to the full-range ΠLDA. LRC-ωΠLDA-AC brings further improvement approaching the accuracy of standard long-range corrected schemes LC-ωPBE and SLC-PBE. The new functionals yield highest occupied orbital energies closer to experimental ionization potentials and describe correctly the weak charge-transfer complex of ethylene and dichlorine and the hole-spin distribution created by an Al defect in quartz. This study provides a framework for more flexible range-separated Rung 3.5 approximations.

Nuclear magnetic resonance spin-spin coupling constants from coupled perturbed density functional theory

NASA Astrophysics Data System (ADS)

Sychrovský, Vladimír; Gräfenstein, Jürgen; Cremer, Dieter

2000-09-01

For the first time, a complete implementation of coupled perturbed density functional theory (CPDFT) for the calculation of NMR spin-spin coupling constants (SSCCs) with pure and hybrid DFT is presented. By applying this method to several hydrides, hydrocarbons, and molecules with multiple bonds, the performance of DFT for the calculation of SSCCs is analyzed in dependence of the XC functional used. The importance of electron correlation effects is demonstrated and it is shown that the hybrid functional B3LYP leads to the best accuracy of calculated SSCCs. Also, CPDFT is compared with sum-over-states (SOS) DFT where it turns out that the former method is superior to the latter because it explicitly considers the dependence of the Kohn-Sham operator on the perturbed orbitals in DFT when calculating SSCCs. The four different coupling mechanisms contributing to the SSCC are discussed in connection with the electronic structure of the molecule.

How well do static electronic dipole polarizabilities from gas-phase experiments compare with density functional and MP2 computations?

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

Thakkar, Ajit J., E-mail: ajit@unb.ca; Wu, Taozhe

2015-10-14

Static electronic dipole polarizabilities for 135 molecules are calculated using second-order Møller-Plesset perturbation theory and six density functionals recently recommended for polarizabilities. Comparison is made with the best gas-phase experimental data. The lowest mean absolute percent deviations from the best experimental values for all 135 molecules are 3.03% and 3.08% for the LC-τHCTH and M11 functionals, respectively. Excluding the eight extreme outliers for which the experimental values are almost certainly in error, the mean absolute percent deviation for the remaining 127 molecules drops to 2.42% and 2.48% for the LC-τHCTH and M11 functionals, respectively. Detailed comparison enables us to identifymore » 32 molecules for which the discrepancy between the calculated and experimental values warrants further investigation.« less

Local structure analysis on (La,Ba)(Ga,Mg)O3-δ by the pair distribution function method using a neutron source and density functional theory calculations

NASA Astrophysics Data System (ADS)

Kitamura, Naoto; Vogel, Sven C.; Idemoto, Yasushi

2013-06-01

In this work, we focused on La0.95Ba0.05Ga0.8Mg0.2O3-δ with the perovskite structure, and investigated the local structure around the oxygen vacancy by pair distribution function (PDF) method and density functional theory (DFT) calculation. By comparing the G(r) simulated based on the DFT calculation and the experimentally-observed G(r), it was suggested that the oxygen vacancy was trapped by Ba2+ at the La3+ site at least at room temperature. Such a defect association may be one of the reasons why the La0.95Ba0.05Ga0.8Mg0.2O3-δ showed lower oxide-ion conductivity than (La,Sr)(Ga,Mg)O3-δ which was widely-used as an electrolyte of the solid oxide fuel cell.

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

Theophilou, Iris; Helbig, Nicole; Lathiotakis, Nektarios N.

Functionals of the one-body reduced density matrix (1-RDM) are routinely minimized under Coleman’s ensemble N-representability conditions. Recently, the topic of pure-state N-representability conditions, also known as generalized Pauli constraints, received increased attention following the discovery of a systematic way to derive them for any number of electrons and any finite dimensionality of the Hilbert space. The target of this work is to assess the potential impact of the enforcement of the pure-state conditions on the results of reduced density-matrix functional theory calculations. In particular, we examine whether the standard minimization of typical 1-RDM functionals under the ensemble N-representability conditions violatesmore » the pure-state conditions for prototype 3-electron systems. We also enforce the pure-state conditions, in addition to the ensemble ones, for the same systems and functionals and compare the correlation energies and optimal occupation numbers with those obtained by the enforcement of the ensemble conditions alone.« less

Do muscle mass, muscle density, strength, and physical function similarly influence risk of hospitalization in older adults?

PubMed

Cawthon, Peggy Mannen; Fox, Kathleen M; Gandra, Shravanthi R; Delmonico, Matthew J; Chiou, Chiun-Fang; Anthony, Mary S; Sewall, Ase; Goodpaster, Bret; Satterfield, Suzanne; Cummings, Steven R; Harris, Tamara B

2009-08-01

To examine the association between strength, function, lean mass, muscle density, and risk of hospitalization. Prospective cohort study. Two U.S. clinical centers. Adults aged 70 to 80 (N=3,011) from the Health, Aging and Body Composition Study. Measurements were of grip strength, knee extension strength, lean mass, walking speed, and chair stand pace. Thigh computed tomography scans assessed muscle area and density (a proxy for muscle fat infiltration). Hospitalizations were confirmed by local review of medical records. Negative binomial regression models estimated incident rate ratios (IRRs) of hospitalization for race- and sex-specific quartiles of each muscle and function parameter separately. Multivariate models adjusted for age, body mass index, health status, and coexisting medical conditions. During an average 4.7 years of follow-up, 1,678 (55.7%) participants experienced one or more hospitalizations. Participants in the lowest quartile of muscle density were more likely to be subsequently hospitalized (multivariate IRR=1.47, 95% confidence interval (CI)=1.24-1.73) than those in the highest quartile. Similarly, participants with the weakest grip strength were at greater risk of hospitalization (multivariate IRR=1.52, 95% CI=1.30-1.78, Q1 vs. Q4). Comparable results were seen for knee strength, walking pace, and chair stands pace. Lean mass and muscle area were not associated with risk of hospitalization. Weak strength, poor function, and low muscle density, but not muscle size or lean mass, were associated with greater risk of hospitalization. Interventions to reduce the disease burden associated with sarcopenia should focus on increasing muscle strength and improving physical function rather than simply increasing lean mass.

Interpretation of monoclinic hafnia valence electron energy-loss spectra by time-dependent density functional theory

NASA Astrophysics Data System (ADS)

Hung, L.; Guedj, C.; Bernier, N.; Blaise, P.; Olevano, V.; Sottile, F.

2016-04-01

We present the valence electron energy-loss spectrum and the dielectric function of monoclinic hafnia (m -HfO2) obtained from time-dependent density-functional theory (TDDFT) predictions and compared to energy-filtered spectroscopic imaging measurements in a high-resolution transmission-electron microscope. Fermi's golden rule density-functional theory (DFT) calculations can capture the qualitative features of the energy-loss spectrum, but we find that TDDFT, which accounts for local-field effects, provides nearly quantitative agreement with experiment. Using the DFT density of states and TDDFT dielectric functions, we characterize the excitations that result in the m -HfO2 energy-loss spectrum. The sole plasmon occurs between 13 and 16 eV, although the peaks ˜28 and above 40 eV are also due to collective excitations. We furthermore elaborate on the first-principles techniques used, their accuracy, and remaining discrepancies among spectra. More specifically, we assess the influence of Hf semicore electrons (5 p and 4 f ) on the energy-loss spectrum, and find that the inclusion of transitions from the 4 f band damps the energy-loss intensity in the region above 13 eV. We study the impact of many-body effects in a DFT framework using the adiabatic local-density approximation (ALDA) exchange-correlation kernel, as well as from a many-body perspective using "scissors operators" matched to an ab initio G W calculation to account for self-energy corrections. These results demonstrate some cancellation of errors between self-energy and excitonic effects, even for excitations from the Hf 4 f shell. We also simulate the dispersion with increasing momentum transfer for plasmon and collective excitation peaks.

Mild cognitive impairment is associated with poor physical function but not bone structure or density in late adulthood: findings from the Hertfordshire cohort study.

PubMed

Patel, A; Jameson, K A; Edwards, M H; Ward, K; Gale, C R; Cooper, C; Dennison, Elaine M

2018-04-24

This study investigated the association between mild cognitive impairment (MCI) and physical function and bone health in older adults. MCI was associated with poor physical performance but not bone mineral density or bone microarchitecture. Cross-sectional study to investigate the association between mild cognitive impairment (MCI) and physical performance, and bone health, in a community-dwelling cohort of older adults. Cognitive function of 222 men and 221 women (mean age 75.5 and 75.8 years in men and women, respectively) was assessed by the Strawbridge questionnaire and Mini Mental State Exam (MMSE). Participants underwent dual-energy X-ray absorptiometry (DXA), peripheral-quantitative computed tomography (pQCT) and high-resolution peripheral-quantitative computed tomography (HR-pQCT) scans to assess their bone density, strength and microarchitecture. Their physical function was assessed and a physical performance (PP) score was recorded. In the study, 11.8% of women and 8.1% of men were cognitively impaired on the MMSE (score < 24). On the Strawbridge questionnaire, 24% of women were deemed cognitively impaired compared to 22.3% of men. Cognitive impairment on the Strawbridge questionnaire was associated with poorer physical performance score in men but not in women in the unadjusted analysis. MMSE < 24 was strongly associated with the risk of low physical performance in men (OR 12.9, 95% CI 1.67, 99.8, p = 0.01). Higher MMSE score was associated with better physical performance in both sexes. Poorer cognitive function, whether assessed by the Strawbridge questionnaire, or by MMSE score, was not associated with bone density, shape or microarchitecture, in either sex. MCI in older adults was associated with poor physical performance, but not bone density, shape or microarchitecture.

Performance assessment of density functional methods with Gaussian and Slater basis sets using 7σ orbital momentum distributions of N2O

NASA Astrophysics Data System (ADS)

Wang, Feng; Pang, Wenning; Duffy, Patrick

2012-12-01

Performance of a number of commonly used density functional methods in chemistry (B3LYP, Bhandh, BP86, PW91, VWN, LB94, PBe0, SAOP and X3LYP and the Hartree-Fock (HF) method) has been assessed using orbital momentum distributions of the 7σ orbital of nitrous oxide (NNO), which models electron behaviour in a chemically significant region. The density functional methods are combined with a number of Gaussian basis sets (Pople's 6-31G*, 6-311G**, DGauss TZVP and Dunning's aug-cc-pVTZ as well as even-tempered Slater basis sets, namely, et-DZPp, et-QZ3P, et-QZ+5P and et-pVQZ). Orbital momentum distributions of the 7σ orbital in the ground electronic state of NNO, which are obtained from a Fourier transform into momentum space from single point electronic calculations employing the above models, are compared with experimental measurement of the same orbital from electron momentum spectroscopy (EMS). The present study reveals information on performance of (a) the density functional methods, (b) Gaussian and Slater basis sets, (c) combinations of the density functional methods and basis sets, that is, the models, (d) orbital momentum distributions, rather than a group of specific molecular properties and (e) the entire region of chemical significance of the orbital. It is found that discrepancies of this orbital between the measured and the calculated occur in the small momentum region (i.e. large r region). In general, Slater basis sets achieve better overall performance than the Gaussian basis sets. Performance of the Gaussian basis sets varies noticeably when combining with different Vxc functionals, but Dunning's augcc-pVTZ basis set achieves the best performance for the momentum distributions of this orbital. The overall performance of the B3LYP and BP86 models is similar to newer models such as X3LYP and SAOP. The present study also demonstrates that the combinations of the density functional methods and the basis sets indeed make a difference in the quality of the calculated orbitals.

High-fat diet induces cardiac remodelling and dysfunction: assessment of the role played by SIRT3 loss.

PubMed

Zeng, Heng; Vaka, Venkata Ramana; He, Xiaochen; Booz, George W; Chen, Jian-Xiong

2015-08-01

Mitochondrial dysfunction plays an important role in obesity-induced cardiac impairment. SIRT3 is a mitochondrial protein associated with increased human life span and metabolism. This study investigated the functional role of SIRT3 in obesity-induced cardiac dysfunction. Wild-type (WT) and SIRT3 knockout (KO) mice were fed a normal diet (ND) or high-fat diet (HFD) for 16 weeks. Body weight, fasting glucose levels, reactive oxygen species (ROS) levels, myocardial capillary density, cardiac function and expression of hypoxia-inducible factor (HIF)-1α/-2α were assessed. HFD resulted in a significant reduction in SIRT3 expression in the heart. Both HFD and SIRT3 KO mice showed increased ROS formation, impaired HIF signalling and reduced capillary density in the heart. HFD induced cardiac hypertrophy and impaired cardiac function. SIRT3 KO mice fed HFD showed greater ROS production and a further reduction in cardiac function compared to SIRT3 KO mice on ND. Thus, the adverse effects of HFD on cardiac function were not attributable to SIRT3 loss alone. However, HFD did not further reduce capillary density in SIRT3 KO hearts, implicating SIRT3 loss in HFD-induced capillary rarefaction. Our study demonstrates the importance of SIRT3 in preserving heart function and capillary density in the setting of obesity. Thus, SIRT3 may be a potential therapeutic target for obesity-induced heart failure. © 2015 The Authors. Journal of Cellular and Molecular Medicine published by John Wiley & Sons Ltd and Foundation for Cellular and Molecular Medicine.

Effects of Wavelength and Defect Density on the Efficiency of (In,Ga)N-Based Light-Emitting Diodes

NASA Astrophysics Data System (ADS)

Pristovsek, Markus; Bao, An; Oliver, Rachel A.; Badcock, Tom; Ali, Muhammad; Shields, Andrew

2017-06-01

We measure the electroluminescence of light-emitting diodes (LEDs) on substrates with low dislocation densities (LDD) at 106 cm-2 and low 108 cm-2 , and compare them to LEDs on substrates with high dislocation densities (HDD) closer to 1010 cm-2 . The external quantum efficiencies (EQEs) are fitted using the A B C model with and without localization. The nonradiative-recombination (NR) coefficient A is constant for HDD LEDs, indicating that the NR is dominated by dislocations at all wavelengths. However, A strongly increases for LDD LEDs by a factor of 20 when increasing the emission wavelength from 440 to 540 nm. We attribute this to an increased density of point defects due to the lower growth temperatures used for longer wavelengths. The radiative recombination coefficient B follows the squared wave-function overlap for all samples. Using the observed coefficients, we calculate the peak efficiency as a function of the wavelength. For HDD LEDs the change of wave-function overlap (i.e., B ) is sufficient to reduce the EQE as observed, while for LDD LEDs also the NR coefficient A must increase to explain the observed EQEs. Thus, reducing NR is important to improving the EQEs of green LEDs, but this cannot be achieved solely by reducing the dislocation density: point defects must also be addressed.

Statistical analysis of dislocations and dislocation boundaries from EBSD data.

PubMed

Moussa, C; Bernacki, M; Besnard, R; Bozzolo, N

2017-08-01

Electron BackScatter Diffraction (EBSD) is often used for semi-quantitative analysis of dislocations in metals. In general, disorientation is used to assess Geometrically Necessary Dislocations (GNDs) densities. In the present paper, we demonstrate that the use of disorientation can lead to inaccurate results. For example, using the disorientation leads to different GND density in recrystallized grains which cannot be physically justified. The use of disorientation gradients allows accounting for measurement noise and leads to more accurate results. Misorientation gradient is then used to analyze dislocations boundaries following the same principle applied on TEM data before. In previous papers, dislocations boundaries were defined as Geometrically Necessary Boundaries (GNBs) and Incidental Dislocation Boundaries (IDBs). It has been demonstrated in the past, through transmission electron microscopy data, that the probability density distribution of the disorientation of IDBs and GNBs can be described with a linear combination of two Rayleigh functions. Such function can also describe the probability density of disorientation gradient obtained through EBSD data as reported in this paper. This opens the route for determining IDBs and GNBs probability density distribution functions separately from EBSD data, with an increased statistical relevance as compared to TEM data. The method is applied on deformed Tantalum where grains exhibit dislocation boundaries, as observed using electron channeling contrast imaging. Copyright © 2017 Elsevier B.V. All rights reserved.

Simulation of Mach Probes in Non-Uniform Magnetized Plasmas: the Influence of a Background Density Gradient

NASA Astrophysics Data System (ADS)

Haakonsen, Christian Bernt; Hutchinson, Ian H.

2013-10-01

Mach probes can be used to measure transverse flow in magnetized plasmas, but what they actually measure in strongly non-uniform plasmas has not been definitively established. A fluid treatment in previous work has suggested that the diamagnetic drifts associated with background density and temperature gradients affect transverse flow measurements, but detailed computational study is required to validate and elaborate on those results; it is really a kinetic problem, since the probe deforms and introduces voids in the ion and electron distribution functions. A new code, the Plasma-Object Simulator with Iterated Trajectories (POSIT) has been developed to self-consistently compute the steady-state six-dimensional ion and electron distribution functions in the perturbed plasma. Particle trajectories are integrated backwards in time to the domain boundary, where arbitrary background distribution functions can be specified. This allows POSIT to compute the ion and electron density at each node of its unstructured mesh, update the potential based on those densities, and then iterate until convergence. POSIT is used to study the impact of a background density gradient on transverse Mach probe measurements, and the results compared to the previous fluid theory. C.B. Haakonsen was supported in part by NSF/DOE Grant No. DE-FG02-06ER54512, and in part by an SCGF award administered by ORISE under DOE Contract No. DE-AC05-06OR23100.

Accuracy of lung nodule density on HRCT: analysis by PSF-based image simulation.

PubMed

Ohno, Ken; Ohkubo, Masaki; Marasinghe, Janaka C; Murao, Kohei; Matsumoto, Toru; Wada, Shinichi

2012-11-08

A computed tomography (CT) image simulation technique based on the point spread function (PSF) was applied to analyze the accuracy of CT-based clinical evaluations of lung nodule density. The PSF of the CT system was measured and used to perform the lung nodule image simulation. Then, the simulated image was resampled at intervals equal to the pixel size and the slice interval found in clinical high-resolution CT (HRCT) images. On those images, the nodule density was measured by placing a region of interest (ROI) commonly used for routine clinical practice, and comparing the measured value with the true value (a known density of object function used in the image simulation). It was quantitatively determined that the measured nodule density depended on the nodule diameter and the image reconstruction parameters (kernel and slice thickness). In addition, the measured density fluctuated, depending on the offset between the nodule center and the image voxel center. This fluctuation was reduced by decreasing the slice interval (i.e., with the use of overlapping reconstruction), leading to a stable density evaluation. Our proposed method of PSF-based image simulation accompanied with resampling enables a quantitative analysis of the accuracy of CT-based evaluations of lung nodule density. These results could potentially reveal clinical misreadings in diagnosis, and lead to more accurate and precise density evaluations. They would also be of value for determining the optimum scan and reconstruction parameters, such as image reconstruction kernels and slice thicknesses/intervals.

Using the Opposition Effect in Remotely Sensed Data to Assist in the Retrieval of Bulk Density

NASA Astrophysics Data System (ADS)

Ambeau, Brittany L.

Bulk density is an important geophysical property that impacts the mobility of military vehicles and personnel. Accurate retrieval of bulk density from remotely sensed data is, therefore, needed to estimate the mobility on "off-road" terrain. For a particulate surface, the functional form of the opposition effect can provide valuable information about composition and structure. In this research, we examine the relationship between bulk density and angular width of the opposition effect for a controlled set of laboratory experiments. Given a sample with a known bulk density, we collect reflectance measurements on a spherical grid for various illumination and view geometries -- increasing the amount of reflectance measurements collected at small phase angles near the opposition direction. Bulk densities are varied using a custom-made pluviation device, samples are measured using the Goniometer of the Rochester Institute of Technology-Two (GRIT-T), and observations are fit to the Hapke model using a grid-search method. The method that is selected allows for the direct estimation of five parameters: the single-scattering albedo, the amplitude of the opposition effect, the angular width of the opposition effect, and the two parameters that describe the single-particle phase function. As a test of the Hapke model, the retrieved bulk densities are compared to the known bulk densities. Results show that with an increase in the availability of multi-angular reflectance measurements, the prospects for retrieving the spatial distribution of bulk density from satellite and airborne sensors are imminent.

A density spike on astrophysical scales from an N-field waterfall transition

NASA Astrophysics Data System (ADS)

Halpern, Illan F.; Hertzberg, Mark P.; Joss, Matthew A.; Sfakianakis, Evangelos I.

2015-09-01

Hybrid inflation models are especially interesting as they lead to a spike in the density power spectrum on small scales, compared to the CMB, while also satisfying current bounds on tensor modes. Here we study hybrid inflation with N waterfall fields sharing a global SO (N) symmetry. The inclusion of many waterfall fields has the obvious advantage of avoiding topologically stable defects for N > 3. We find that it also has another advantage: it is easier to engineer models that can simultaneously (i) be compatible with constraints on the primordial spectral index, which tends to otherwise disfavor hybrid models, and (ii) produce a spike on astrophysically large length scales. The latter may have significant consequences, possibly seeding the formation of astrophysically large black holes. We calculate correlation functions of the time-delay, a measure of density perturbations, produced by the waterfall fields, as a convergent power series in both 1 / N and the field's correlation function Δ (x). We show that for large N, the two-point function is < δt (x) δt (0) > ∝Δ2 (| x |) / N and the three-point function is < δt (x) δt (y) δt (0) > ∝ Δ (| x - y |) Δ (| x |) Δ (| y |) /N2. In accordance with the central limit theorem, the density perturbations on the scale of the spike are Gaussian for large N and non-Gaussian for small N.

Benchmarking density functional tight binding models for barrier heights and reaction energetics of organic molecules.

PubMed

Gruden, Maja; Andjeklović, Ljubica; Jissy, Akkarapattiakal Kuriappan; Stepanović, Stepan; Zlatar, Matija; Cui, Qiang; Elstner, Marcus

2017-09-30

Density Functional Tight Binding (DFTB) models are two to three orders of magnitude faster than ab initio and Density Functional Theory (DFT) methods and therefore are particularly attractive in applications to large molecules and condensed phase systems. To establish the applicability of DFTB models to general chemical reactions, we conduct benchmark calculations for barrier heights and reaction energetics of organic molecules using existing databases and several new ones compiled in this study. Structures for the transition states and stable species have been fully optimized at the DFTB level, making it possible to characterize the reliability of DFTB models in a more thorough fashion compared to conducting single point energy calculations as done in previous benchmark studies. The encouraging results for the diverse sets of reactions studied here suggest that DFTB models, especially the most recent third-order version (DFTB3/3OB augmented with dispersion correction), in most cases provide satisfactory description of organic chemical reactions with accuracy almost comparable to popular DFT methods with large basis sets, although larger errors are also seen for certain cases. Therefore, DFTB models can be effective for mechanistic analysis (e.g., transition state search) of large (bio)molecules, especially when coupled with single point energy calculations at higher levels of theory. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

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.

A comparative density functional study on electrical properties of layered penta-graphene

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

Yu, Zhi Gen, E-mail: yuzg@ihpc.a-star.edu.sg; Zhang, Yong-Wei, E-mail: zhangyw@ihpc.a-star.edu.sg

We present a comparative study of the influence of the number of layers, the biaxial strain in the range of −3% to 3%, and the stacking misalignments on the electronic properties of a new 2D carbon allotrope, penta-graphene (PG), based on hybrid-functional method within the density functional theory (DFT). In comparison with local exchange-correlation approximation in the DFT, the hybrid-functional provides an accurate description on the degree of p{sub z} orbitals localization and bandgap. Importantly, the predicted bandgap of few-layer PG has a weak layer dependence. The bandgap of monolayer PG is 3.27 eV, approximately equal to those of GaN andmore » ZnO; and the bandgap of few-layer PG decreases slowly with the number of layers (N) and converge to 2.57 eV when N ≥ 4. Our calculations using HSE06 functional on few-layer PG reveal that bandgap engineering by stacking misalignment can further tune the bandgap down to 1.37 eV. Importantly, there is no direct-to-indirect bandgap transition in PG by varying strain, layer number, and stacking misalignment. Owing to its tunable, robustly direct, and wide bandgap characteristics, few-layer PG is promising for optoelectronic and photovoltaic applications.« less

Scanning tunneling microscopy image simulation of the rutile (110) TiO2 surface with hybrid functionals and the localized basis set approach

NASA Astrophysics Data System (ADS)

Di Valentin, Cristiana

2007-10-01

In this work we present a simplified procedure to use hybrid functionals and localized atomic basis sets to simulate scanning tunneling microscopy (STM) images of stoichiometric, reduced and hydroxylated rutile (110) TiO2 surface. For the two defective systems it is necessary to introduce some exact Hartree-Fock exchange in the exchange functional in order to correctly describe the details of the electronic structure. Results are compared to the standard density functional theory and planewave basis set approach. Both methods have advantages and drawbacks that are analyzed in detail. In particular, for the localized basis set approach, it is necessary to introduce a number of Gaussian function in the vacuum region above the surface in order to correctly describe the exponential decay of the integrated local density of states from the surface. In the planewave periodic approach, a thick vacuum region is required to achieve correct results. Simulated STM images are obtained for both the reduced and hydroxylated surface which nicely compare with experimental findings. A direct comparison of the two defects as displayed in the simulated STM images indicates that the OH groups should appear brighter than oxygen vacancies in perfect agreement with the experimental STM data.

Prediction of electronic and optical properties of ZnAl2Te4 defect chalcopyrite semiconductor: an ab-initio study

NASA Astrophysics Data System (ADS)

Mayengbam, Rishikanta; Tripathy, S. K.; Pandey, B. P.

2018-03-01

In this paper, we have investigated the structural, electronic and optical properties of ZnAl2Te4 defect chalcopyrite semiconductor using generalized gradient approximation (GGA) within density functional theory (DFT). We have calculated the optimized lattice constants (a and c) and compared with the available experimental values. The optimized lattice constants have been used to calculate the energy band gap and found to be 1.57 eV. The partial density of states and total density of states have been discussed in detail. The frequency dependent dielectric constant and refractive index have been calculated and plotted in the energy range 0-13 eV. All the above parameters have been compared with the available experimental and theoretical values and found good agreement between them.

An efficient method for quantum transport simulations in the time domain

NASA Astrophysics Data System (ADS)

Wang, Y.; Yam, C.-Y.; Frauenheim, Th.; Chen, G. H.; Niehaus, T. A.

2011-11-01

An approximate method based on adiabatic time dependent density functional theory (TDDFT) is presented, that allows for the description of the electron dynamics in nanoscale junctions under arbitrary time dependent external potentials. The density matrix of the device region is propagated according to the Liouville-von Neumann equation. The semi-infinite leads give rise to dissipative terms in the equation of motion which are calculated from first principles in the wide band limit. In contrast to earlier ab initio implementations of this formalism, the Hamiltonian is here approximated in the spirit of the density functional based tight-binding (DFTB) method. Results are presented for two prototypical molecular devices and compared to full TDDFT calculations. The temporal profile of the current traces is qualitatively well captured by the DFTB scheme. Steady state currents show considerable variations, both in comparison of approximate and full TDDFT, but also among TDDFT calculations with different basis sets.

Self-consistent electronic structure of disordered Fe/sub 0. 65/Ni/sub 0. 35/

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

Johnson, D.D.; Pinski, F.J.; Stocks, G.M.

1985-04-15

We present the results of the first ab initio calculation of the electronic structure of the disordered alloy Fe/sub 0.65/Ni/sub 0.35/. The calculation is based on the multiple-scattering coherent-potential approach (KKR-CPA) and is fully self-consistent and spin polarized. Magnetic effects are included within local-spin-density functional theory using the exchange-correlation function of Vosko--Wilk--Nusair. The most striking feature of the calculation is that electrons of different spins experience different degrees of disorder. The minority spin electrons see a very large disorder, whereas the majority spin electrons see little disorder. Consequently, the minority spin density of states is smooth compared to the verymore » structured majority spin density of states. This difference is due to a subtle balance between exchange splitting and charge neutrality.« less

Self-consistent electronic structure of disordered Fe/sub 0/ /sub 65/Ni/sub 0/ /sub 35/

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

Johnson, D.D.; Pinski, F.J.; Stocks, G.M.

1984-01-01

We present the results of the first ab-initio calculation of the electronic structure of a disordered Fe/sub 0/ /sub 65/Ni/sub 0/ /sub 35/ alloy. The calculation is based on the multiple-scattering coherent-potential approach (KKR-CPA) and is fully self-consistent and spin-polarized. Magnetic effects are included within local-spin-density functional theory using the exchange-correlation function of Vosko-Wilk-Nusair. The most striking feature of the calculation is that electrons of different spins experience different degrees of disorder. The minority spin electrons see a very large disorder; whereas, the majority spin electrons see little disorder. Consequently, the minority spin density of states is smooth compared tomore » the very structured majority spin density of states. This difference is due to a subtle balance between exchange-splitting and charge neutrality. 15 references, 2 figures.« less

Density Functional Study of the Structure, Stability and Oxygen Reduction Activity of Ultrathin Platinum Nanowires

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

Matanovic, Ivana; Kent, Paul; Garzon, Fernando

2013-03-14

We used density functional theory to study the difference in the structure, stability and catalytic reactivity between ultrathin, 0.5–1.0 nm diameter, platinum nanotubes and nanowires. Model nanowires were formed by inserting an inner chain of platinum atoms in small diameter nanotubes. In this way more stable, non-hollow structures were formed. The difference in the electronic structure of platinum nanotubes and nanowires was examined by inspecting the density of surface states and band structure. Furthermore, reactivity toward the oxygen reduction reaction of platinum nanowires was assessed by studying the change in the chemisorption energies of oxygen, hydroxyl, and hydroperoxyl groups, inducedmore » by converting the nanotube models to nanowires. Both ultrathin platinum nanotubes and nanowires show distinct properties compared to bulk platinum. Single-wall nanotubes and platinum nanowires with diameters larger than 1 nm show promise for use as oxygen reduction catalysts.« less

Density functional theory (DFT) study of a new novel bionanosensor hybrid; tryptophan/Pd doped single walled carbon nanotube

NASA Astrophysics Data System (ADS)

Yoosefian, Mehdi; Etminan, Nazanin

2016-07-01

In order to explore a new novel L-amino acid/transition metal doped single walled carbon nanotube based biosensor, density functional theory calculations were studied. These hybrid structures of organic-inorganic nanobiosensors are able to detect the smallest amino acid building block of proteins. The configurations of amine and carbonyl group coordination of tryptophan aromatic amino acid adsorbed on Pd/doped single walled carbon nanotube were compared. The frontier molecular orbital theory, quantum theory atom in molecule and natural bond orbital analysis were performed. The molecular electrostatic potential and the electron density surfaces were constructed. The calculations indicated that the Pd/SWCNT was sensitive to tryptophan suggesting the importance of interaction with biological molecule and potential detecting application. The proposed nanobiosensor represents a highly sensitive detection of protein at ultra-low concentration in diagnosis applications.

Simulations of Turbulent Momentum and Scalar Transport in Non-Reacting Confined Swirling Coaxial Jets

NASA Technical Reports Server (NTRS)

Shih, Tsan-Hsing; Liu, Nan-Suey; Moder, Jeffrey P.

2015-01-01

This paper presents the numerical simulations of confined three-dimensional coaxial water jets. The objectives are to validate the newly proposed nonlinear turbulence models of momentum and scalar transport, and to evaluate the newly introduced scalar APDF and DWFDF equation along with its Eulerian implementation in the National Combustion Code (NCC). Simulations conducted include the steady RANS, the unsteady RANS (URANS), and the time-filtered Navier-Stokes (TFNS); both without and with invoking the APDF or DWFDF equation. When the APDF (ensemble averaged probability density function) or DWFDF (density weighted filtered density function) equation is invoked, the simulations are of a hybrid nature, i.e., the transport equations of energy and species are replaced by the APDF or DWFDF equation. Results of simulations are compared with the available experimental data. Some positive impacts of the nonlinear turbulence models and the Eulerian scalar APDF and DWFDF approach are observed.

Mass-number and excitation-energy dependence of the spin cutoff parameter

DOE PAGES

Grimes, S. M.; Voinov, A. V.; Massey, T. N.

2016-07-12

Here, the spin cutoff parameter determining the nuclear level density spin distribution ρ(J) is defined through the spin projection as < J 2 z > 1/2 or equivalently for spherical nuclei, (< J(J+1) >/3) 1/2. It is needed to divide the total level density into levels as a function of J. To obtain the total level density at the neutron binding energy from the s-wave resonance count, the spin cutoff parameter is also needed. The spin cutoff parameter has been calculated as a function of excitation energy and mass with a super-conducting Hamiltonian. Calculations have been compared with two commonlymore » used semiempirical formulas. A need for further measurements is also observed. Some complications for deformed nuclei are discussed. The quality of spin cut off parameter data derived from isomeric ratio measurement is examined.« less

Solid-state modeling of the terahertz spectrum of the high explosive HMX.

PubMed

Allis, Damian G; Prokhorova, Darya A; Korter, Timothy M

2006-02-09

The experimental solid-state terahertz (THz) spectrum (3-120 cm(-1)) of the beta-crystal form of the high explosive octahydro-1,3,5,7-tetranitro-1,3,5,7-tetrazocine (HMX) has been analyzed using solid-state density functional theory calculations. Various density functionals (both generalized gradient approximation and local density approximation) are compared in terms of their abilities to reproduce the experimentally observed solid-state structure and low-frequency vibrational motions. Good-to-excellent agreement between solid-state theory and experiment can be achieved in the THz region where isolated-molecule calculations fail to reproduce the observed spectral features, demonstrating a clear limitation of using isolated-molecule calculations for the assignment of THz frequency motions in molecular solids. The deficiency of isolated-molecule calculations is traced to modification of the molecular structure in the solid state through crystal packing effects and the formation of weak C-H...O hydrogen bonds.

Density functional theory for the description of spherical non-associating monomers in confined media using the SAFT-VR equation of state and weighted density approximations.

PubMed

Malheiro, Carine; Mendiboure, Bruno; Plantier, Frédéric; Blas, Felipe J; Miqueu, Christelle

2014-04-07

As a first step of an ongoing study of thermodynamic properties and adsorption of complex fluids in confined media, we present a new theoretical description for spherical monomers using the Statistical Associating Fluid Theory for potential of Variable Range (SAFT-VR) and a Non-Local Density Functional Theory (NLDFT) with Weighted Density Approximations (WDA). The well-known Modified Fundamental Measure Theory is used to describe the inhomogeneous hard-sphere contribution as a reference for the monomer and two WDA approaches are developed for the dispersive terms from the high-temperature Barker and Henderson perturbation expansion. The first approach extends the dispersive contributions using the scalar and vector weighted densities introduced in the Fundamental Measure Theory (FMT) and the second one uses a coarse-grained (CG) approach with a unique weighted density. To test the accuracy of this new NLDFT/SAFT-VR coupling, the two versions of the theoretical model are compared with Grand Canonical Monte Carlo (GCMC) molecular simulations using the same molecular model. Only the version with the "CG" approach for the dispersive terms provides results in excellent agreement with GCMC calculations in a wide range of conditions while the "FMT" extension version gives a good representation solely at low pressures. Hence, the "CG" version of the theoretical model is used to reproduce methane adsorption isotherms in a Carbon Molecular Sieve and compared with experimental data after a characterization of the material. The whole results show an excellent agreement between modeling and experiments. Thus, through a complete and consistent comparison both with molecular simulations and with experimental data, the NLDFT/SAFT-VR theory has been validated for the description of monomers.

Evaluating a linearized Euler equations model for strong turbulence effects on sound propagation.

PubMed

Ehrhardt, Loïc; Cheinet, Sylvain; Juvé, Daniel; Blanc-Benon, Philippe

2013-04-01

Sound propagation outdoors is strongly affected by atmospheric turbulence. Under strongly perturbed conditions or long propagation paths, the sound fluctuations reach their asymptotic behavior, e.g., the intensity variance progressively saturates. The present study evaluates the ability of a numerical propagation model based on the finite-difference time-domain solving of the linearized Euler equations in quantitatively reproducing the wave statistics under strong and saturated intensity fluctuations. It is the continuation of a previous study where weak intensity fluctuations were considered. The numerical propagation model is presented and tested with two-dimensional harmonic sound propagation over long paths and strong atmospheric perturbations. The results are compared to quantitative theoretical or numerical predictions available on the wave statistics, including the log-amplitude variance and the probability density functions of the complex acoustic pressure. The match is excellent for the evaluated source frequencies and all sound fluctuations strengths. Hence, this model captures these many aspects of strong atmospheric turbulence effects on sound propagation. Finally, the model results for the intensity probability density function are compared with a standard fit by a generalized gamma function.

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

Effects of transcranial direct current stimulation on hemichannel pannexin-1 and neural plasticity in rat model of cerebral infarction.

PubMed

Jiang, T; Xu, R X; Zhang, A W; Di, W; Xiao, Z J; Miao, J Y; Luo, N; Fang, Y N

2012-12-13

The aim of this study was to investigate the effects of transcranial direct current stimulation (TDCS) on hemichannel pannexin-1 (PX1) in cortical neurons and neural plasticity, and explore the optimal time window of TDCS therapy after stroke. Adult male Sprague-Dawley rats (n=90) were randomly assigned to sham operation, middle cerebral artery occlusion (MCAO), and TDCS groups, and underwent sham operation, unilateral middle cerebral artery (MCA) electrocoagulation, and unilateral MCA electrocoagulation plus TDCS (daily anodal and cathodal 10 Hz, 0.1 mA TDCS for 30 min beginning day 1 after stroke), respectively. Motor function was assessed using the beam walking test (BWT), and density of dendritic spines (DS) and PX1 mRNA expression were compared among groups on days 3, 7, and 14 after stroke. Effects of PX1 blockage on DS in hippocampal neurons after hypoxia-ischemia were observed. TDCS significantly improved motor function on days 7 and 14 after stroke as indicated by reduced BWT scores compared with the MCAO group. The density of DS was decreased after stroke; the TDCS group had increased DS density compared with the MCAO group on days 3, 7, and 14 (all P<0.0001). Cerebral infarction induced increased PX1 mRNA expression on days 3, 7, and 14 (P<0.0001), and the peak PX1 mRNA expression was observed on day 7. TDCS did not decrease the up-regulated PX1 mRNA expression after stroke on day 3, but did reduce the increased post-stroke PX1 mRNA expression on days 7 and 14 (P<0.0001). TDCS increased the DS density after stroke, indicating that it may promote neural plasticity after stroke. TDCS intervention from day 7 to day 14 after stroke demonstrated motor function improvement and can down-regulate the elevated PX1 mRNA expression after stroke. Copyright © 2012 IBRO. Published by Elsevier Ltd. All rights reserved.

The Correlated Jacobi and the Correlated Cauchy-Lorentz Ensembles

NASA Astrophysics Data System (ADS)

Wirtz, Tim; Waltner, Daniel; Kieburg, Mario; Kumar, Santosh

2016-01-01

We calculate the k-point generating function of the correlated Jacobi ensemble using supersymmetric methods. We use the result for complex matrices for k=1 to derive a closed-form expression for the eigenvalue density. For real matrices we obtain the density in terms of a twofold integral that we evaluate numerically. For both expressions we find agreement when comparing with Monte Carlo simulations. Relations between these quantities for the Jacobi and the Cauchy-Lorentz ensemble are derived.

Ultrasonic fluid densitometer for process control

DOEpatents

Greenwood, Margaret S.

2000-01-01

The present invention is an ultrasonic fluid densitometer that uses at least one pair of transducers for transmitting and receiving ultrasonic signals internally reflected within a material wedge. A temperature sensor is provided to monitor the temperature of the wedge material. Density of a fluid is determined by immersing the wedge into the fluid and measuring reflection of ultrasound at the wedge-fluid interface and comparing a transducer voltage and wedge material temperature to a tabulation as a function of density.

The relationship between epicuticular long-chained hydrocarbons and surface area - volume ratios in insects (Diptera, Hymenoptera, Lepidoptera)

PubMed Central

Brückner, Adrian; Heethoff, Michael; Blüthgen, Nico

2017-01-01

Long-chain cuticular hydrocarbons (CHCs) are common components of the epicuticle of terrestrial arthropods. CHC serve as a protective barrier against environmental influences but also act as semiochemicals in animal communication. Regarding the latter aspect, species- or intra-functional group specific CHCs composition and variation are relatively well studied. However, comparative knowledge about the relationship of CHC quantity and their relation to surface area—volume ratios in the context of water loss and protection is fragmentary. Hence, we aim to study the taxon-specific relationship of the CHC amount and surface-area to volume ratio related to their functional role (e.g. in water loss). We focused on flower visiting insects and analyzed the CHC amounts of three insect orders (Hymenoptera, Lepidoptera and Diptera) using gas chromatography—mass spectrometry (GC-MS). We included 113 species from two grassland plots, quantified their CHCs, and measured their body mass and surface area. We found differences in the surface area, CHCs per body mass and the CHC density (= amount of CHCs per surface area) across the three insect taxa. Especially the Hymenoptera had a higher CHC density compared to Diptera and Lepidoptera. CHC density could be explained by surface area-volume ratios in Hymenoptera but not in Diptera and Lepidoptera. Unexpectedly, CHC density decreased with increasing surface area—volume ratios. PMID:28384308

ELSI: A unified software interface for Kohn–Sham electronic structure solvers

DOE PAGES

Yu, Victor Wen-zhe; Corsetti, Fabiano; Garcia, Alberto; ...

2017-09-15

Solving the electronic structure from a generalized or standard eigenproblem is often the bottleneck in large scale calculations based on Kohn-Sham density-functional theory. This problem must be addressed by essentially all current electronic structure codes, based on similar matrix expressions, and by high-performance computation. We here present a unified software interface, ELSI, to access different strategies that address the Kohn-Sham eigenvalue problem. Currently supported algorithms include the dense generalized eigensolver library ELPA, the orbital minimization method implemented in libOMM, and the pole expansion and selected inversion (PEXSI) approach with lower computational complexity for semilocal density functionals. The ELSI interface aimsmore » to simplify the implementation and optimal use of the different strategies, by offering (a) a unified software framework designed for the electronic structure solvers in Kohn-Sham density-functional theory; (b) reasonable default parameters for a chosen solver; (c) automatic conversion between input and internal working matrix formats, and in the future (d) recommendation of the optimal solver depending on the specific problem. As a result, comparative benchmarks are shown for system sizes up to 11,520 atoms (172,800 basis functions) on distributed memory supercomputing architectures.« less

Equation of state for detonation product gases

NASA Astrophysics Data System (ADS)

Nagayama, Kunihito; Kubota, Shiro

2003-03-01

A thermodynamic analysis procedure of the detonation product equation of state (EOS) together with the experimental data set of the detonation velocity as a function of initial density has been formulated. The Chapman-Jouguet (CJ) state [W. Ficket and W. C. Davis, Detonation: Theory and Experiment (University of California Press, Berkeley 1979)] on the p-ν plane is found to be well approximated by the envelope function formed by the collection of Rayleigh lines with many different initial density states. The Jones-Stanyukovich-Manson relation [W. Ficket and W. C. Davis, Detonation: Theory and Experiment (University of California Press, Berkeley, 1979)] is used to estimate the error included in this approximation. Based on this analysis, a simplified integration method to calculate the Grüneisen parameter along the CJ state curve with different initial densities utilizing the cylinder expansion data has been presented. The procedure gives a simple way of obtaining the EOS function, compatible with the detonation velocity data. Theoretical analysis has been performed for the precision of the estimated EOS function. EOS of the pentaerithrytoltetranitrate explosive is calculated and compared with some of the experimental data such as CJ pressure data and cylinder expansion data.

ELSI: A unified software interface for Kohn-Sham electronic structure solvers

NASA Astrophysics Data System (ADS)

Yu, Victor Wen-zhe; Corsetti, Fabiano; García, Alberto; Huhn, William P.; Jacquelin, Mathias; Jia, Weile; Lange, Björn; Lin, Lin; Lu, Jianfeng; Mi, Wenhui; Seifitokaldani, Ali; Vázquez-Mayagoitia, Álvaro; Yang, Chao; Yang, Haizhao; Blum, Volker

2018-01-01

Solving the electronic structure from a generalized or standard eigenproblem is often the bottleneck in large scale calculations based on Kohn-Sham density-functional theory. This problem must be addressed by essentially all current electronic structure codes, based on similar matrix expressions, and by high-performance computation. We here present a unified software interface, ELSI, to access different strategies that address the Kohn-Sham eigenvalue problem. Currently supported algorithms include the dense generalized eigensolver library ELPA, the orbital minimization method implemented in libOMM, and the pole expansion and selected inversion (PEXSI) approach with lower computational complexity for semilocal density functionals. The ELSI interface aims to simplify the implementation and optimal use of the different strategies, by offering (a) a unified software framework designed for the electronic structure solvers in Kohn-Sham density-functional theory; (b) reasonable default parameters for a chosen solver; (c) automatic conversion between input and internal working matrix formats, and in the future (d) recommendation of the optimal solver depending on the specific problem. Comparative benchmarks are shown for system sizes up to 11,520 atoms (172,800 basis functions) on distributed memory supercomputing architectures.

Hybrid functional studies of stability and diffusion of hydrogen in Mg-doped GaN

NASA Astrophysics Data System (ADS)

Park, Ji-Sang; Chang, K. J.

2012-02-01

Nitride semiconductors are known to suffer from low p-type doping efficiency due to the high activation energy of Mg acceptors and the compensation of hole carriers. To enhance hole carrier concentration, the hydrogen co-doping method is widely used, in which hydrogen is intentionally doped with Mg dopants and removed by subsequent thermal annealing. In this work, we perform first-principles density functional calculations to study the stability and diffusion of hydrogen in Mg-doped GaN. For the exchange-correlation potential, we employ both the generalized gradient approximation (GGA) proposed by Perdew, Burke, and Ernzerhof and the hybrid density functional of Heyd, Scuseria, and Ernzerhof. We examine the diffusion pathways and dissociation barriers of H from the Mg-H complex using the nudged elastic band and dimer methods. We compare the results of the GGA and hybrid density functional calculations for the stability of various H interstitial configurations and the migration barriers for H diffusion. Finally, using the calculated migration barriers as inputs, we perform kinetic Monte Carlo simulations for the dissociation of the Mg-H complex and find that the Mg acceptors are activated by thermal annealing up to 700-800 ^oC, in good agreement with experiments.

ELSI: A unified software interface for Kohn–Sham electronic structure solvers

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

Yu, Victor Wen-zhe; Corsetti, Fabiano; Garcia, Alberto

Solving the electronic structure from a generalized or standard eigenproblem is often the bottleneck in large scale calculations based on Kohn-Sham density-functional theory. This problem must be addressed by essentially all current electronic structure codes, based on similar matrix expressions, and by high-performance computation. We here present a unified software interface, ELSI, to access different strategies that address the Kohn-Sham eigenvalue problem. Currently supported algorithms include the dense generalized eigensolver library ELPA, the orbital minimization method implemented in libOMM, and the pole expansion and selected inversion (PEXSI) approach with lower computational complexity for semilocal density functionals. The ELSI interface aimsmore » to simplify the implementation and optimal use of the different strategies, by offering (a) a unified software framework designed for the electronic structure solvers in Kohn-Sham density-functional theory; (b) reasonable default parameters for a chosen solver; (c) automatic conversion between input and internal working matrix formats, and in the future (d) recommendation of the optimal solver depending on the specific problem. As a result, comparative benchmarks are shown for system sizes up to 11,520 atoms (172,800 basis functions) on distributed memory supercomputing architectures.« less

Data for the synthesis of resorcinol-formaldehyde aerogels in acidic and basic media.

PubMed

Molina-Campos, Daniel F; Fonseca-Correa, Rafael A; Vargas-Delgadillo, Diana P; Giraldo, Liliana; Moreno-Piraján, Juan Carlos

2017-06-01

The aim of this research is to synthesise carbon aerogels and to compare the differences in their textural, morphological and chemical properties when synthesised in basic and acidic media, and with two different types of pretreatment carbonization and activation with CO 2 . Four samples are prepared and characterised using TGA-DTA, SEM, DRX, isotherm determination of N 2 adsorption-desorption at -196 °C and immersion calorimetry. The data for pore distribution are reported using non-local density functional theory and quenched solid density functional theory. Finally, with the immersion calorimetry data, the consistency between the results using this technique and those obtained using the nitrogen isotherms is analysed.

Application of Density Functional Theory to Systems Containing Metal Atoms

NASA Technical Reports Server (NTRS)

Bauschlicher, Charles W., Jr.; Arnold, James O. (Technical Monitor)

1997-01-01

The accuracy of density functional theory (DFT) for problems involving metal atoms is considered. The DFT results are compared with experiment as well as results obtained using the coupled cluster approach. The comparisons include geometries, frequencies, and bond energies. The systems considered include MO2, M(OH)+(sub n), MNO+, and MCO+(sub 2). The DFT works well for frequencies and geometries, even in cases with symmetry breaking; however, some examples have been found where the symmetry breaking is quite severe and the DFT methods do not work well. The calculation of bond energies is more difficult and examples of the successes as well as failures of DFT will be given.

AB INITIO Molecular Dynamics Simulations of Water Under Static and Shock Compressed Conditions

NASA Astrophysics Data System (ADS)

Goldman, Nir; Fried, Laurence E.; Mundy, Christopher J.; Kuo, I.-F. William; Curioni, Alessandro; Reed, Evan J.

2007-12-01

We report herein a series of ab initio simulations of water under both static and shocked conditions. We have calculated the coherent x-ray scattering intensity of several phases of water under high pressure, using ab initio Density Functional Theory (DFT). We provide new atomic scattering form factors for water at extreme conditions, which take into account frequently neglected changes in ionic charge and electron delocalization. We have also simulated liquid water undergoing shock loading of velocities from 5-11 km/s using the Multi-Scale Shock Technique (MSST). We show that Density Functional Theory (DFT) molecular dynamics results compare extremely well to experiments on the water shock Hugoniot.

Generalized-active-space pair-density functional theory: an efficient method to study large, strongly correlated, conjugated systems.

PubMed

Ghosh, Soumen; Cramer, Christopher J; Truhlar, Donald G; Gagliardi, Laura

2017-04-01

Predicting ground- and excited-state properties of open-shell organic molecules by electronic structure theory can be challenging because an accurate treatment has to correctly describe both static and dynamic electron correlation. Strongly correlated systems, i.e. , systems with near-degeneracy correlation effects, are particularly troublesome. Multiconfigurational wave function methods based on an active space are adequate in principle, but it is impractical to capture most of the dynamic correlation in these methods for systems characterized by many active electrons. We recently developed a new method called multiconfiguration pair-density functional theory (MC-PDFT), that combines the advantages of wave function theory and density functional theory to provide a more practical treatment of strongly correlated systems. Here we present calculations of the singlet-triplet gaps in oligoacenes ranging from naphthalene to dodecacene. Calculations were performed for unprecedently large orbitally optimized active spaces of 50 electrons in 50 orbitals, and we test a range of active spaces and active space partitions, including four kinds of frontier orbital partitions. We show that MC-PDFT can predict the singlet-triplet splittings for oligoacenes consistent with the best available and much more expensive methods, and indeed MC-PDFT may constitute the benchmark against which those other models should be compared, given the absence of experimental data.

Density-functional theory for internal magnetic fields

NASA Astrophysics Data System (ADS)

Tellgren, Erik I.

2018-01-01

A density-functional theory is developed based on the Maxwell-Schrödinger equation with an internal magnetic field in addition to the external electromagnetic potentials. The basic variables of this theory are the electron density and the total magnetic field, which can equivalently be represented as a physical current density. Hence, the theory can be regarded as a physical current density-functional theory and an alternative to the paramagnetic current density-functional theory due to Vignale and Rasolt. The energy functional has strong enough convexity properties to allow a formulation that generalizes Lieb's convex analysis formulation of standard density-functional theory. Several variational principles as well as a Hohenberg-Kohn-like mapping between potentials and ground-state densities follow from the underlying convex structure. Moreover, the energy functional can be regarded as the result of a standard approximation technique (Moreau-Yosida regularization) applied to the conventional Schrödinger ground-state energy, which imposes limits on the maximum curvature of the energy (with respect to the magnetic field) and enables construction of a (Fréchet) differentiable universal density functional.

Mapping out the QCD phase transition in multiparticle production

NASA Astrophysics Data System (ADS)

Kabana, Sonja; Minkowski, Peter

2001-04-01

We analyse multiparticle production in a thermal framework for seven central nucleus + nucleus collisions, e+ + e- annihilation into hadrons on the Z resonance and four hadronic reactions p + p and p + pbar with partial centrality selection), with centre of mass energies ranging from √(s) = 2.6 GeV (per nucleon pair) to 1.8 TeV. Thermodynamic parameters at chemical freeze-out (temperature and baryon and strangeness fugacities) are obtained from appropriate fits, generally improving in quality for reactions subjected to centrality cuts. All systems with non-vanishing fugacities are extrapolated along trajectories of equal energy density, density and entropy density to zero fugacities. The so-obtained temperatures extrapolated to zero fugacities as a function of initial energy density ɛin universally show a strong rise followed by a saturating limit of Tlim = 155 +/- 6 +/- 20 MeV. We interpret this behaviour as mapping out the boundary between quark gluon plasma and hadronic phases. The ratio of strange antiquarks to light ones as a function of the initial energy density ɛin shows the same behaviour as the temperature, saturating at a value of 0.365 +/- 0.033 +/- 0.07. No distinctive feature of `strangeness enhancement' is seen for heavy ion collisions relative to hadronic and leptonic reactions, when compared at the same initial energy density.

Reentrant equilibrium disordering in nanoparticle–polymer mixtures

DOE PAGES

Meng, Dong; Kumar, Sanat K.; Grest, Gary S.; ...

2017-01-31

A large body of experimental work has established that athermal colloid/polymer mixtures undergo a sequence of transitions from a disordered fluid state to a colloidal crystal to a second disordered phase with increasing polymer concentration. These transitions are driven by polymer-mediated interparticle attraction, which is a function of both the polymer density and size. It has been posited that the disordered state at high polymer density is a consequence of strong interparticle attractions that kinetically inhibit the formation of the colloidal crystal, i.e., the formation of a non-equilibrium gel phase interferes with crystallization. Here we use molecular dynamics simulations andmore » density functional theory on polymers and nanoparticles (NPs) of comparable size and show that the crystal-disordered phase coexistence at high polymer density for sufficiently long chains corresponds to an equilibrium thermodynamic phase transition. While the crystal is, indeed, stabilized at intermediate polymer density by polymer-induced intercolloid attractions, it is destabilized at higher densities because long chains lose significant configurational entropy when they are forced to occupy all of the crystal voids. Finally, our results are in quantitative agreement with existing experimental data and show that, at least in the nanoparticle limit of sufficiently small colloidal particles, the crystal phase only has a modest range of thermodynamic stability.« less

Hybrid functional study of α-uranium

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

Kaur, Gurpreet, E-mail: gurpreet@igcar.gov.in; Chinnappan, Ravi; Panigrahi, B. K.

2016-05-23

We have used the hybrid density functionals to study the structural and electronic properties of alpha-U. The fraction of exact Hartree Folk exchange used is varied from 0.0 to 0.6. The equilibrium volume is found to be underestimated and bulk modulus overestimated with HSE as compared to both calculated by PBE and the experimental values. Electronic bands below the Fermi level are found to shift to lower energy with respect to PBE electronic bands which itself gives the bands shifted to lower energies as compared to UPS experiments.

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

Lee, Hyewon; Cheong, S.W.; Kim, Bog G., E-mail: boggikim@pusan.ac.kr

We have studied the properties of SnO{sub 6} octahedra-containing perovskites and their derived structures using ab initio calculations with different density functionals. In order to predict the correct band gap of the materials, we have used B3LYP hybrid density functional, and the results of B3LYP were compared with those obtained using the local density approximation and generalized gradient approximation data. The calculations have been conducted for the orthorhombic ground state of the SnO{sub 6} containing perovskites. We also have expended the hybrid density functional calculation to the ASnO{sub 3}/A'SnO{sub 3} system with different cation orderings. We propose an empirical relationshipmore » between the tolerance factor and the band gap of SnO{sub 6} containing oxide materials based on first principles calculation. - Graphical abstract: (a) Structure of ASnO{sub 3} for orthorhombic ground state. The green ball is A (Ba, Sr, Ca) cation and the small (red) ball on edge is oxygen. SnO{sub 6} octahedrons are plotted as polyhedron. (b) Band gap of ASnO{sub 3} as a function of the tolerance factor for different density functionals. The experimental values of the band gap are marked as green pentagons. (c) ASnO{sub 3}/A'SnO{sub 3} superlattices with two types cation arrangement: [001] layered structure and [111] rocksalt structure, respectively. (d) B3LYP hybrid functional band gaps of ASnO{sub 3}, [001] ordered superlattices, and [111] ordered superlattices of ASnO{sub 3}/A'SnO{sub 3} as a function of the effective tolerance factor. Note the empirical linear relationship between the band gap and effective tolerance factor. - Highlights: • We report the hybrid functional band gap calculation of ASnO{sub 3} and ASnO{sub 3}/A'SnO{sub 3}. • The band gap of ASnO{sub 3} using B3LYP functional reproduces the experimental value. • We propose the linear relationship between the tolerance factor and the band gap.« less

A spatially explicit capture-recapture estimator for single-catch traps.

PubMed

Distiller, Greg; Borchers, David L

2015-11-01

Single-catch traps are frequently used in live-trapping studies of small mammals. Thus far, a likelihood for single-catch traps has proven elusive and usually the likelihood for multicatch traps is used for spatially explicit capture-recapture (SECR) analyses of such data. Previous work found the multicatch likelihood to provide a robust estimator of average density. We build on a recently developed continuous-time model for SECR to derive a likelihood for single-catch traps. We use this to develop an estimator based on observed capture times and compare its performance by simulation to that of the multicatch estimator for various scenarios with nonconstant density surfaces. While the multicatch estimator is found to be a surprisingly robust estimator of average density, its performance deteriorates with high trap saturation and increasing density gradients. Moreover, it is found to be a poor estimator of the height of the detection function. By contrast, the single-catch estimators of density, distribution, and detection function parameters are found to be unbiased or nearly unbiased in all scenarios considered. This gain comes at the cost of higher variance. If there is no interest in interpreting the detection function parameters themselves, and if density is expected to be fairly constant over the survey region, then the multicatch estimator performs well with single-catch traps. However if accurate estimation of the detection function is of interest, or if density is expected to vary substantially in space, then there is merit in using the single-catch estimator when trap saturation is above about 60%. The estimator's performance is improved if care is taken to place traps so as to span the range of variables that affect animal distribution. As a single-catch likelihood with unknown capture times remains intractable for now, researchers using single-catch traps should aim to incorporate timing devices with their traps.

Random density matrices versus random evolution of open system

NASA Astrophysics Data System (ADS)

Pineda, Carlos; Seligman, Thomas H.

2015-10-01

We present and compare two families of ensembles of random density matrices. The first, static ensemble, is obtained foliating an unbiased ensemble of density matrices. As criterion we use fixed purity as the simplest example of a useful convex function. The second, dynamic ensemble, is inspired in random matrix models for decoherence where one evolves a separable pure state with a random Hamiltonian until a given value of purity in the central system is achieved. Several families of Hamiltonians, adequate for different physical situations, are studied. We focus on a two qubit central system, and obtain exact expressions for the static case. The ensemble displays a peak around Werner-like states, modulated by nodes on the degeneracies of the density matrices. For moderate and strong interactions good agreement between the static and the dynamic ensembles is found. Even in a model where one qubit does not interact with the environment excellent agreement is found, but only if there is maximal entanglement with the interacting one. The discussion is started recalling similar considerations for scattering theory. At the end, we comment on the reach of the results for other convex functions of the density matrix, and exemplify the situation with the von Neumann entropy.

Communication: Density functional theory embedding with the orthogonality constrained basis set expansion procedure

NASA Astrophysics Data System (ADS)

Culpitt, Tanner; Brorsen, Kurt R.; Hammes-Schiffer, Sharon

2017-06-01

Density functional theory (DFT) embedding approaches have generated considerable interest in the field of computational chemistry because they enable calculations on larger systems by treating subsystems at different levels of theory. To circumvent the calculation of the non-additive kinetic potential, various projector methods have been developed to ensure the orthogonality of molecular orbitals between subsystems. Herein the orthogonality constrained basis set expansion (OCBSE) procedure is implemented to enforce this subsystem orbital orthogonality without requiring a level shifting parameter. This scheme is a simple alternative to existing parameter-free projector-based schemes, such as the Huzinaga equation. The main advantage of the OCBSE procedure is that excellent convergence behavior is attained for DFT-in-DFT embedding without freezing any of the subsystem densities. For the three chemical systems studied, the level of accuracy is comparable to or higher than that obtained with the Huzinaga scheme with frozen subsystem densities. Allowing both the high-level and low-level DFT densities to respond to each other during DFT-in-DFT embedding calculations provides more flexibility and renders this approach more generally applicable to chemical systems. It could also be useful for future extensions to embedding approaches combining wavefunction theories and DFT.

Multiconfiguration Pair-Density Functional Theory Outperforms Kohn-Sham Density Functional Theory and Multireference Perturbation Theory for Ground-State and Excited-State Charge Transfer.

PubMed

Ghosh, Soumen; Sonnenberger, Andrew L; Hoyer, Chad E; Truhlar, Donald G; Gagliardi, Laura

2015-08-11

The correct description of charge transfer in ground and excited states is very important for molecular interactions, photochemistry, electrochemistry, and charge transport, but it is very challenging for Kohn-Sham (KS) density functional theory (DFT). KS-DFT exchange-correlation functionals without nonlocal exchange fail to describe both ground- and excited-state charge transfer properly. We have recently proposed a theory called multiconfiguration pair-density functional theory (MC-PDFT), which is based on a combination of multiconfiguration wave function theory with a new type of density functional called an on-top density functional. Here we have used MC-PDFT to study challenging ground- and excited-state charge-transfer processes by using on-top density functionals obtained by translating KS exchange-correlation functionals. For ground-state charge transfer, MC-PDFT performs better than either the PBE exchange-correlation functional or CASPT2 wave function theory. For excited-state charge transfer, MC-PDFT (unlike KS-DFT) shows qualitatively correct behavior at long-range with great improvement in predicted excitation energies.

CAPILLARY CONDENSATION IN MMS AND PORE STRUCTURE CHARACTERIZATION. (R825959)

EPA Science Inventory

Phenomena of capillary condensation and desorption in siliceous mesoporous molecular sieves (MMS) with cylindrical channels are studied by means of the non-local density functional theory (NLDFT). The results are compared with macroscopic thermodynamic approaches based on Kelv...

Alterations in hippocampal and cortical densities of functionally different interneurons in rat models of absence epilepsy.

PubMed

Papp, Péter; Kovács, Zsolt; Szocsics, Péter; Juhász, Gábor; Maglóczky, Zsófia

2018-05-31

Recent data from absence epileptic patients and animal models provide evidence for significant impairments of attention, memory, and psychosocial functioning. Here, we outline aspects of the electrophysiological and structural background of these dysfunctions by investigating changes in hippocampal and cortical GABAergic inhibitory interneurons in two genetically absence epileptic rat strains: the Genetic Absence Epilepsy Rats from Strasbourg (GAERS) and the Wistar Albino Glaxo/Rijswijk (WAG/Rij) rats. Using simultaneously recorded field potentials from the primary somatosensory cortex (S1 cortex, seizure focus) and the hippocampal hilus, we demonstrated that typical frequencies of spike-wave discharges (SWDs; 7-8 Hz, GAERS; 7-9 Hz, WAG/Rij) and their harmonics appeared and their EEG spectral power markedly increased on recordings not only from the S1 cortex, but also from the hilus in both GAERS and WAG/Rij rats during SWDs. Moreover, we observed an increased synchronization between S1 cortex and hilus at 7-8 Hz (GAERS) and 7-9 Hz (WAG/Rij) and at their harmonics when SWDs occurred in the S1 cortex in both rat strains. In addition, using immunohistochemistry we demonstrated changes in the densities of perisomatic (parvalbumin-immunopositive, PV+) and interneuron-selective (calretinin-immunopositive, CR+) GABAergic inhibitory interneuron somata. Specifically, GAERS and WAG/Rij rats displayed lower densities of PV-immunopositivity in the hippocampal hilus compared to non-epileptic control (NEC) and normal Wistar rats. GAERS and WAG/Rij rats also show a marked reduction in the density of CR + interneurons in the same region in comparison with NEC rats. Data from the S1 cortex reveals bidirectional differences in PV + density, with GAERS displaying a significant increase, whereas WAG/Rij a reduction compared to control rat strains. Our results suggest an enhanced synchronization and functional connections between the hippocampus and S1 cortex as well as thalamocortical activities during SWDs and a functional alteration of inhibitory mechanisms in the hippocampus and S1 cortex of two genetic models of absence epilepsy, presumably in relation with increased neuronal activity and seizure-induced neuronal injury. Copyright © 2018 Elsevier B.V. All rights reserved.

Efficacy and safety of lipid lowering by alirocumab in chronic kidney disease.

PubMed

Toth, Peter P; Dwyer, Jamie P; Cannon, Christopher P; Colhoun, Helen M; Rader, Daniel J; Upadhyay, Ashish; Louie, Michael J; Koren, Andrew; Letierce, Alexia; Mandel, Jonas; Banach, Maciej

2018-06-01

Individuals with chronic kidney disease are at increased risk of premature cardiovascular disease. Among them, many with elevated low-density lipoprotein cholesterol (LDL-C) are unable to achieve optimal LDL-C on statins and require additional lipid-lowering therapy. To study this, we compared the LDL-C-lowering efficacy and safety of alirocumab in individuals with hypercholesterolemia with impaired renal function, defined as eGFR 30-59 ml/min/1.73 m 2 , to those without impaired renal function eGFR ≥60 ml/min/1.73 m 2 . A total of 4629 hypercholesterolemic individuals without or with impaired renal function, pooled from eight phase 3 ODYSSEY trials (double-blind treatments of 24-104 weeks), were on alirocumab 150 mg or 75/150 mg every two weeks vs. placebo or ezetimibe. Overall, 10.1% had impaired renal function and over 99% were receiving statin treatment. Baseline LDL-C in alirocumab and control groups was comparable in subgroups analyzed. LDL-C reductions at week 24 ranged from 46.1 to 62.2% or 48.3 to 60.1% with alirocumab among individuals with or without impaired renal function, respectively. Similar reductions were observed for lipoprotein (a), non-high-density lipoprotein cholesterol, apolipoprotein B, and triglycerides. Safety data were similar in both treatment subgroups, regardless of the degree of CKD. Renal function did not change over time in response to alirocumab. This post hoc efficacy analysis is limited by evaluation of alirocumab treatment effects on renal and lipid parameters by serum biochemistry. Thus, alirocumab consistently lowered LDL-C regardless of impaired renal function, with safety comparable to control, among individuals with hypercholesterolemia who nearly all were on statin treatment. Copyright © 2018 International Society of Nephrology. Published by Elsevier Inc. All rights reserved.

Covalent functionalization of graphene by azobenzene with molecular hydrogen bonds for long-term solar thermal storage

NASA Astrophysics Data System (ADS)

Feng, Yiyu; Liu, Hongpo; Luo, Wen; Liu, Enzuo; Zhao, Naiqin; Yoshino, Katsumi; Feng, Wei

2013-11-01

Reduced graphene oxide-azobenzene (RGO-AZO) hybrids were prepared via covalent functionalization for long-term solar thermal storage. Thermal barrier (ΔEa) of cis to tran reversion and thermal storage (ΔH) were improved by molecular hydrogen bonds (H-bonds) through ortho- or para-substitution of AZO. Intramolecular H-bonds thermally stabilized cis-ortho-AZO on RGO with a long-term half-life of 5400 h (ΔEa = 1.2 eV), which was much longer than that of RGO-para-AZO (116 h). RGO-para-AZO with one intermolecular H-bond showed a high density of thermal storage up to 269.8 kJ kg-1 compared with RGO-ortho-AZO (149.6 kJ kg-1) with multiple intra- and intermolecular H-bonds of AZO according to relaxed stable structures. Thermal storage in experiment was the same order magnitude to theoretical data based on ΔH calculated by density functional theory and packing density. Photoactive RGO-AZO hybrid can be developed for high-performance solar thermal storage by optimizing molecular H-bonds.

CuPc/Au(1 1 0): Determination of the azimuthal alignment by a combination of angle-resolved photoemission and density functional theory

PubMed Central

Lüftner, Daniel; Milko, Matus; Huppmann, Sophia; Scholz, Markus; Ngyuen, Nam; Wießner, Michael; Schöll, Achim; Reinert, Friedrich; Puschnig, Peter

2014-01-01

Here we report on a combined experimental and theoretical study on the structural and electronic properties of a monolayer of Copper-Phthalocyanine (CuPc) on the Au(1 1 0) surface. Low-energy electron diffraction reveals a commensurate overlayer unit cell containing one adsorbate species. The azimuthal alignment of the CuPc molecule is revealed by comparing experimental constant binding energy (kxky)-maps using angle-resolved photoelectron spectroscopy with theoretical momentum maps of the free molecule's highest occupied molecular orbital (HOMO). This structural information is confirmed by total energy calculations within the framework of van-der-Waals corrected density functional theory. The electronic structure is further analyzed by computing the molecule-projected density of states, using both a semi-local and a hybrid exchange-correlation functional. In agreement with experiment, the HOMO is located about 1.2 eV below the Fermi-level, while there is no significant charge transfer into the molecule and the CuPc LUMO remains unoccupied on the Au(1 1 0) surface. PMID:25284953

Covalent functionalization of graphene by azobenzene with molecular hydrogen bonds for long-term solar thermal storage

PubMed Central

Feng, Yiyu; Liu, Hongpo; Luo, Wen; Liu, Enzuo; Zhao, Naiqin; Yoshino, Katsumi; Feng, Wei

2013-01-01

Reduced graphene oxide-azobenzene (RGO-AZO) hybrids were prepared via covalent functionalization for long-term solar thermal storage. Thermal barrier (ΔEa) of cis to tran reversion and thermal storage (ΔH) were improved by molecular hydrogen bonds (H-bonds) through ortho- or para-substitution of AZO. Intramolecular H-bonds thermally stabilized cis-ortho-AZO on RGO with a long-term half-life of 5400 h (ΔEa = 1.2 eV), which was much longer than that of RGO-para-AZO (116 h). RGO-para-AZO with one intermolecular H-bond showed a high density of thermal storage up to 269.8 kJ kg−1 compared with RGO-ortho-AZO (149.6 kJ kg−1) with multiple intra- and intermolecular H-bonds of AZO according to relaxed stable structures. Thermal storage in experiment was the same order magnitude to theoretical data based on ΔH calculated by density functional theory and packing density. Photoactive RGO-AZO hybrid can be developed for high-performance solar thermal storage by optimizing molecular H-bonds. PMID:24247355

Covalent functionalization of graphene by azobenzene with molecular hydrogen bonds for long-term solar thermal storage.

PubMed

Feng, Yiyu; Liu, Hongpo; Luo, Wen; Liu, Enzuo; Zhao, Naiqin; Yoshino, Katsumi; Feng, Wei

2013-11-19

Reduced graphene oxide-azobenzene (RGO-AZO) hybrids were prepared via covalent functionalization for long-term solar thermal storage. Thermal barrier (ΔEa) of cis to tran reversion and thermal storage (ΔH) were improved by molecular hydrogen bonds (H-bonds) through ortho- or para-substitution of AZO. Intramolecular H-bonds thermally stabilized cis-ortho-AZO on RGO with a long-term half-life of 5400 h (ΔEa = 1.2 eV), which was much longer than that of RGO-para-AZO (116 h). RGO-para-AZO with one intermolecular H-bond showed a high density of thermal storage up to 269.8 kJ kg(-1) compared with RGO-ortho-AZO (149.6 kJ kg(-1)) with multiple intra- and intermolecular H-bonds of AZO according to relaxed stable structures. Thermal storage in experiment was the same order magnitude to theoretical data based on ΔH calculated by density functional theory and packing density. Photoactive RGO-AZO hybrid can be developed for high-performance solar thermal storage by optimizing molecular H-bonds.

Assessment of energy density usage during 180W lithium triborate laser photoselective vaporization of the prostate for benign prostatic hyperplasia. Is there an optimum amount of kilo-Joules per gram of prostate?

PubMed

Valdivieso, Roger; Meyer, Christian P; Hueber, Pierre-Alain; Meskawi, Malek; Alenizi, Abdullah M; Azizi, Mounsif; Trinh, Quoc-Dien; Misrai, Vincent; Rutman, Matthew; Te, Alexis E; Chughtai, Bilal; Barber, Neil J; Emara, Amr M; Munver, Ravi; Zorn, Kevin C

2016-10-01

To assess the effect of energy density (kJ/mL) applied on adenoma during photoselective vaporization of the prostate (PVP) treatment for benign prostate hyperplasia (BPH) on functional outcomes, prostate-specific antigen (PSA) reduction and complications. After exclusions, a total of 440 patients who underwent GreenLight (tm) laser XPS-180W lithium triborate PVP for the treatment of BPH were retrospectively reviewed. Data were collected from seven different international centres (Canada, USA, UK and France). Patients were stratified into four energy density groups (kJ/mL) according to intra-operative energy delivered and prostate volume as determined by preoperative transrectal ultrasonography (TRUS): group 1: <3 kJ/mL; group 2: 3-5 kJ/mL; group 3: 5-7 kJ/mL; and group 4: ≥7 kJ/mL. Energy density groups were chosen arbitrarily. PSA reduction and functional outcomes (International Prostate Symptom Score, quality of life, post-void residual urine volume, maximum urinary flow rate) were compared at 6, 12 and 24 months. Peri-operative complications and retreatment rates were also compared among the groups. The PSA reduction rates at 24 months after the procedure were 51, 61, 79 and 83% for the energy density groups <3, 3-5, 5-7 and ≥7 kJ/mL, respectively (P ≤ 0.01). This held true after accounting for baseline confounders. Energy density was not associated with higher complication rates, including haematuria, stricture formation, incontinence, refractory urinary retention, urinary tract infection and conversion to transurethral resection of the prostate. Functional outcomes at 2 years of follow-up were equivalent among the groups (P > 0.05 for all) and similar retreatment rates were observed (P = 0.36). Higher energy usage per cc of prostate was associated with a more significant reduction in PSA level (>50%) at 6, 12 and 24 months, suggesting increased vaporization of adenoma tissue; however, this did not translate into differences in functional outcomes at 2-year follow-up. © 2016 The Authors BJU International © 2016 BJU International Published by John Wiley & Sons Ltd.

Bisphosphonate therapy for osteogenesis imperfecta.

PubMed

Dwan, Kerry; Phillipi, Carrie A; Steiner, Robert D; Basel, Donald

2016-10-19

Osteogenesis imperfecta is caused by a genetic defect resulting in an abnormal type I collagen bone matrix which typically results in multiple fractures with little or no trauma. Bisphosphonates are used in an attempt to increase bone mineral density and reduce these fractures in people with osteogenesis imperfecta. This is an update of a previously published Cochrane Review. To assess the effectiveness and safety of bisphosphonates in increasing bone mineral density, reducing fractures and improving clinical function in people with osteogenesis imperfecta. We searched the Cochrane Cystic Fibrosis and Genetic Disorders Group Inborn Errors of Metabolism Trials Register which comprises references identified from comprehensive electronic database searches, handsearches of journals and conference proceedings. We additionally searched PubMed and major conference proceedings.Date of the most recent search of the Cochrane Cystic Fibrosis and Genetic Disorders Group's Inborn Errors of Metabolism Register: 28 April 2016. Randomised and quasi-randomised controlled trials comparing bisphosphonates to placebo, no treatment, or comparator interventions in all types of osteogenesis imperfecta. Two authors independently extracted data and assessed the risk of bias of the included trials. Fourteen trials (819 participants) were included. Overall, the trials were mainly at a low risk of bias, although selective reporting was an issue in several of the trials. Data for oral bisphosphonates versus placebo could not be aggregated; a statistically significant difference favouring oral bisphosphonates in fracture risk reduction and number of fractures was noted in two trials. No differences were reported in the remaining three trials which commented on fracture incidence. Five trials reported data for spine bone mineral density; all found statistically significant increased lumbar spine density z scores for at least one time point studied. For intravenous bisphosphonates versus placebo, aggregated data from two trials showed no statistically significant difference for the number of participants with at least one fracture, risk ratio 0.56 (95% confidence interval 0.30 to 1.06). In the remaining trial no statistically significant difference was noted in fracture incidence. For spine bone mineral density, no statistically significant difference was noted in the aggregated data from two trials, mean difference 9.96 (95% confidence interval -2.51 to 22.43). In the remaining trial a statistically significant difference in mean per cent change in spine bone mineral density z score favoured intravenous bisphosphonates at six and 12 months. Data describing growth, bone pain, and functional outcomes after oral or intravenous bisphosphonate therapy, or both, as compared to placebo were incomplete among all studies, but do not show consistent improvements in these outcomes. Two studies compared different doses of bisphosphonates. No differences were found between doses when bone mineral density, fractures, and height or length z score were assessed. One trial compared oral versus intravenous bisphosphonates and found no differences in primary outcomes. Two studies compared the intravenous bisphosphonates zoledronic acid and pamidronate. There were no significant differences in primary outcome. However, the studies were at odds as to the relative benefit of zoledronic acid over pamidronate for lumbosacral bone mineral density at 12 months. Bisphophonates are commonly prescribed to individuals with osteogenesis imperfecta. Current evidence, albeit limited, demonstrates oral or intravenous bisphosphonates increase bone mineral density in children and adults with this condition. These were not shown to be different in their ability to increase bone mineral density. It is unclear whether oral or intravenous bisphosphonate treatment consistently decreases fractures, though multiple studies report this independently and no studies report an increased fracture rate with treatment. The studies included here do not show bisphosphonates conclusively improve clinical status (reduce pain; improve growth and functional mobility) in people with osteogenesis imperfecta. Given their current widespread and expected continued use, the optimal method, duration of therapy and long-term safety of bisphosphonate therapy require further investigation. In addition, attention should be given to long-term fracture reduction and improvement in quality of life indicators.

Bisphosphonate therapy for osteogenesis imperfecta.

PubMed

Dwan, Kerry; Phillipi, Carrie A; Steiner, Robert D; Basel, Donald

2014-07-23

Osteogenesis imperfecta is caused by a genetic defect resulting in an abnormal type I collagen bone matrix which typically results in multiple fractures with little or no trauma. Bisphosphonates are used in an attempt to increase bone mineral density and reduce these fractures in people with osteogenesis imperfecta. To assess the effectiveness and safety of bisphosphonates in increasing bone mineral density, reducing fractures and improving clinical function in people with osteogenesis imperfecta. We searched the Cochrane Cystic Fibrosis and Genetic Disorders Group Inborn Errors of Metabolism Trials Register which comprises references identified from comprehensive electronic database searches, handsearches of journals and conference proceedings. We additionally searched PubMed and major conference proceedings.Date of the most recent search: 07 April 2014. Randomised and quasi-randomised controlled trials comparing bisphosphonates to placebo, no treatment, or comparator interventions in all types of osteogenesis imperfecta. Two authors independently extracted data and assessed the risk of bias of the included trials. Fourteen trials (819 participants) were included. Overall, the trials were mainly at a low risk of bias, although selective reporting was an issue in several of the trials. Data for oral bisphosphonates versus placebo could not be aggregated; a statistically significant difference favouring oral bisphosphonates in fracture risk reduction and number of fractures was noted in two trials. No differences were reported in the remaining three trials which commented on fracture incidence. Five trials reported data for spine bone mineral density; all found statistically significant increased lumbar spine density z scores for at least one time point studied. For intravenous bisphosphonates versus placebo, aggregated data from two trials showed no statistically significant difference for the number of participants with at least one fracture, risk ratio 0.56 (95% confidence interval 0.30 to 1.06). In the remaining trial no statistically significant difference was noted in fracture incidence. For spine bone mineral density, no statistically significant difference was noted in the aggregated data from two trials, mean difference 9.96 (95% confidence interval -2.51 to 22.43). In the remaining trial a statistically significant difference in mean per cent change in spine bone mineral density z score favoured intravenous bisphosphonates at six and 12 months. Data describing growth, bone pain, and functional outcomes after oral or intravenous bisphosphonate therapy, or both, as compared to placebo were incomplete among all studies, but do not show consistent improvements in these outcomes. Two studies compared different doses of bisphosphonates. No differences were found between doses when bone mineral density, fractures, and height or length z score were assessed. One study compared oral versus intravenous bisphosphonates and found no differences in primary outcomes. Two studies compared the intravenous bisphosphonates zoledronic acid and pamidronate. There were no significant differences in primary outcome. However, the studies were at odds as to the relative benefit of zoledronic acid over pamidronate for lumbosacral bone mineral density at 12 months. Bisphophonates are commonly prescribed to individuals with osteogenesis imperfecta. Current evidence, albeit limited, demonstrates oral or intravenous bisphosphonates increase bone mineral density in children and adults with this condition. These were not shown to be different in their ability to increase bone mineral density. It is unclear whether oral or intravenous bisphosphonate treatment consistently decreases fractures, though multiple studies report this independently and no studies report an increased fracture rate with treatment. The studies included here do not show bisphosphonates conclusively improve clinical status (reduce pain; improve growth and functional mobility) in people with osteogenesis imperfecta. Given their current widespread and expected continued use, the optimal method, duration of therapy and long-term safety of bisphosphonate therapy require further investigation. In addition, attention should be given to long-term fracture reduction and improvement in quality of life indicators.

Intermittent fasting protects against the deterioration of cognitive function, energy metabolism and dyslipidemia in Alzheimer's disease-induced estrogen deficient rats.

PubMed

Shin, Bae Kun; Kang, Suna; Kim, Da Sol; Park, Sunmin

2018-02-01

Intermittent fasting may be an effective intervention to protect against age-related metabolic disturbances, although it is still controversial. Here, we investigated the effect of intermittent fasting on the deterioration of the metabolism and cognitive functions in rats with estrogen deficiency and its mechanism was also explored. Ovariectomized rats were infused with β-amyloid (25-35; Alzheimer's disease) or β-amyloid (35-25, Non-Alzheimer's disease; normal cognitive function) into the hippocampus. Each group was randomly divided into two sub-groups: one with intermittent fasting and the other fed ad libitum: Alzheimer's disease-ad libitum, Alzheimer's disease-intermittent fasting, Non-Alzheimer's disease-ad libitum, and Non-Alzheimer's disease-intermittent fasting. Rats in the intermittent fasting groups had a restriction of food consumption to a 3-h period every day. Each group included 10 rats and all rats fed a high-fat diet for four weeks. Interestingly, Alzheimer's disease increased tail skin temperature more than Non-Alzheimer's disease and intermittent fasting prevented the increase. Alzheimer's disease reduced bone mineral density in the spine and femur compared to the Non-Alzheimer's disease, whereas bone mineral density in the hip and leg was reduced by intermittent fasting. Fat mass only in the abdomen was decreased by intermittent fasting. Intermittent fasting decreased food intake without changing energy expenditure. Alzheimer's disease increased glucose oxidation, whereas intermittent fasting elevated fat oxidation as a fuel source. Alzheimer's disease and intermittent fasting deteriorated insulin resistance in the fasting state but intermittent fasting decreased serum glucose levels after oral glucose challenge by increasing insulin secretion. Alzheimer's disease deteriorated short and spatial memory function compared to the Non-Alzheimer's disease, whereas intermittent fasting prevented memory loss in comparison to ad libitum. Unexpectedly, cortisol levels were increased by Alzheimer's disease but decreased by intermittent fasting. Intermittent fasting improved dyslipidemia and liver damage index compared to ad libitum. Alzheimer's disease lowered low-density lipoprotein cholesterol and serum triglyceride levels compared to Non-Alzheimer's disease. In conclusion, Alzheimer's disease impaired not only cognitive function but also disturbed energy, glucose, lipid, and bone metabolism in ovariectomized rats. Intermittent fasting protected against the deterioration of these metabolic parameters, but it exacerbated bone mineral density loss and insulin resistance at fasting in Alzheimer's disease-induced estrogen-deficient rats. Impact statement Intermittent fasting was evaluated for its effects on cognitive function and metabolic disturbances in a rat model of menopause and Alzheimer's disease. Intermittent fasting decreased skin temperature and fat mass, and improved glucose tolerance with decreasing food intake. Intermittent fasting also prevented memory loss: short-term and special memory loss. Therefore, intermittent fasting may prevent some of the metabolic pathologies associated with menopause and protect against age-related memory decline.

Exact density functional and wave function embedding schemes based on orbital localization

NASA Astrophysics Data System (ADS)

Hégely, Bence; Nagy, Péter R.; Ferenczy, György G.; Kállay, Mihály

2016-08-01

Exact schemes for the embedding of density functional theory (DFT) and wave function theory (WFT) methods into lower-level DFT or WFT approaches are introduced utilizing orbital localization. First, a simple modification of the projector-based embedding scheme of Manby and co-workers [J. Chem. Phys. 140, 18A507 (2014)] is proposed. We also use localized orbitals to partition the system, but instead of augmenting the Fock operator with a somewhat arbitrary level-shift projector we solve the Huzinaga-equation, which strictly enforces the Pauli exclusion principle. Second, the embedding of WFT methods in local correlation approaches is studied. Since the latter methods split up the system into local domains, very simple embedding theories can be defined if the domains of the active subsystem and the environment are treated at a different level. The considered embedding schemes are benchmarked for reaction energies and compared to quantum mechanics (QM)/molecular mechanics (MM) and vacuum embedding. We conclude that for DFT-in-DFT embedding, the Huzinaga-equation-based scheme is more efficient than the other approaches, but QM/MM or even simple vacuum embedding is still competitive in particular cases. Concerning the embedding of wave function methods, the clear winner is the embedding of WFT into low-level local correlation approaches, and WFT-in-DFT embedding can only be more advantageous if a non-hybrid density functional is employed.

Electron and ion distribution functions in magnetopause reconnection

NASA Astrophysics Data System (ADS)

Wang, S.; Chen, L. J.; Bessho, N.; Hesse, M.; Kistler, L. M.; Torbert, R. B.; Mouikis, C.; Pollock, C. J.

2015-12-01

We investigate electron and ion velocity distribution functions in dayside magnetopause reconnection events observed by the Cluster and MMS spacecraft. The goal is to build a spatial map of electron and ion distribution features to enable the indication of the spacecraft location in the reconnection structure, and to understand plasma energization processes. Distribution functions, together with electromagnetic field structures, plasma densities, and bulk velocities, are organized and compared with particle-in-cell simulation results to indicate the proximities to the reconnection X-line. Anisotropic features in the distributions of magnetospheric- and magnetosheath- origin electrons at different locations in the reconnection inflow and exhaust are identified. In particular, parallel electron heating is observed in both the magnetosheath and magnetosphere inflow regions. Possible effects of the guide field strength, waves, and upstream density and temperature asymmetries on the distribution features will be discussed.

Time dependent density functional theory study of the near-edge x-ray absorption fine structure of benzene in gas phase and on metal surfaces.

PubMed

Asmuruf, Frans A; Besley, Nicholas A

2008-08-14

The near-edge x-ray absorption fine structure of benzene in the gas phase and adsorbed on the Au(111) and Pt(111) surfaces is studied with time dependent density functional theory. Excitation energies computed with hybrid exchange-correlation functionals are too low compared to experiment. However, after applying a constant shift the spectra are in good agreement with experiment. For benzene on the Au(111) surface, two bands arising from excitation to the e(2u)(pi(*)) and b(2g)(pi(*)) orbitals of benzene are observed for photon incidence parallel to the surface. On Pt(111) surface, a broader band arises from excitation to benzene orbitals that are mixed with the surface and have both sigma(*)(Pt-C) and pi(*) characters.

The Structure and Stability of Bn(+) Clusters

NASA Technical Reports Server (NTRS)

Ricca, Alessandra; Bauschlicher, Charles W., Jr.; Langhoff, Stephen R. (Technical Monitor)

1995-01-01

The geometries of B+n clusters for n less than 14 have been optimized using density functional theory with the B3LYP functional. The most stable structure for each cluster is planar or quasi-planar. The B3LYP fragmentation energies are calibrated using coupled cluster theory. Overall, our corrected fragmentation energies are in reasonable agreement with experiment. Our results are compared with previous theoretical results.

IGM CONSTRAINTS FROM THE SDSS-III/BOSS DR9 Lyα FOREST TRANSMISSION PROBABILITY DISTRIBUTION FUNCTION

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

Lee, Khee-Gan; Hennawi, Joseph F.; Spergel, David N.

2015-02-01

The Lyα forest transmission probability distribution function (PDF) is an established probe of the intergalactic medium (IGM) astrophysics, especially the temperature-density relationship of the IGM. We measure the transmission PDF from 3393 Baryon Oscillations Spectroscopic Survey (BOSS) quasars from Sloan Digital Sky Survey Data Release 9, and compare with mock spectra that include careful modeling of the noise, continuum, and astrophysical uncertainties. The BOSS transmission PDFs, measured at (z) = [2.3, 2.6, 3.0], are compared with PDFs created from mock spectra drawn from a suite of hydrodynamical simulations that sample the IGM temperature-density relationship, γ, and temperature at mean density,more » T {sub 0}, where T(Δ) = T {sub 0}Δ{sup γ} {sup –} {sup 1}. We find that a significant population of partial Lyman-limit systems (LLSs) with a column-density distribution slope of β{sub pLLS} ∼ – 2 are required to explain the data at the low-transmission end of transmission PDF, while uncertainties in the mean Lyα forest transmission affect the high-transmission end. After modeling the LLSs and marginalizing over mean transmission uncertainties, we find that γ = 1.6 best describes the data over our entire redshift range, although constraints on T {sub 0} are affected by systematic uncertainties. Within our model framework, isothermal or inverted temperature-density relationships (γ ≤ 1) are disfavored at a significance of over 4σ, although this could be somewhat weakened by cosmological and astrophysical uncertainties that we did not model.« less

Minkowski Tensors in Two Dimensions: Probing the Morphology and Isotropy of the Matter and Galaxy Density Fields

NASA Astrophysics Data System (ADS)

Appleby, Stephen; Chingangbam, Pravabati; Park, Changbom; Hong, Sungwook E.; Kim, Juhan; Ganesan, Vidhya

2018-05-01

We apply the Minkowski tensor statistics to two-dimensional slices of the three-dimensional matter density field. The Minkowski tensors are a set of functions that are sensitive to directionally dependent signals in the data and, furthermore, can be used to quantify the mean shape of density fields. We begin by reviewing the definition of Minkowski tensors and introducing a method of calculating them from a discretely sampled field. Focusing on the statistic {W}21,1—a 2 × 2 matrix—we calculate its value for both the entire excursion set and individual connected regions and holes within the set. To study the morphology of structures within the excursion set, we calculate the eigenvalues λ 1, λ 2 for the matrix {W}21,1 of each distinct connected region and hole and measure their mean shape using the ratio β \\equiv < {λ }2/{λ }1> . We compare both {W}21,1 and β for a Gaussian field and a smoothed density field generated from the latest Horizon Run 4 cosmological simulation to study the effect of gravitational collapse on these functions. The global statistic {W}21,1 is essentially independent of gravitational collapse, as the process maintains statistical isotropy. However, β is modified significantly, with overdensities becoming relatively more circular compared to underdensities at low redshifts. When applying the statistics to a redshift-space distorted density field, the matrix {W}21,1 is no longer proportional to the identity matrix, and measurements of its diagonal elements can be used to probe the large-scale velocity field.

A new wavelet transform to sparsely represent cortical current densities for EEG/MEG inverse problems.

PubMed

Liao, Ke; Zhu, Min; Ding, Lei

2013-08-01

The present study investigated the use of transform sparseness of cortical current density on human brain surface to improve electroencephalography/magnetoencephalography (EEG/MEG) inverse solutions. Transform sparseness was assessed by evaluating compressibility of cortical current densities in transform domains. To do that, a structure compression method from computer graphics was first adopted to compress cortical surface structure, either regular or irregular, into hierarchical multi-resolution meshes. Then, a new face-based wavelet method based on generated multi-resolution meshes was proposed to compress current density functions defined on cortical surfaces. Twelve cortical surface models were built by three EEG/MEG softwares and their structural compressibility was evaluated and compared by the proposed method. Monte Carlo simulations were implemented to evaluate the performance of the proposed wavelet method in compressing various cortical current density distributions as compared to other two available vertex-based wavelet methods. The present results indicate that the face-based wavelet method can achieve higher transform sparseness than vertex-based wavelet methods. Furthermore, basis functions from the face-based wavelet method have lower coherence against typical EEG and MEG measurement systems than vertex-based wavelet methods. Both high transform sparseness and low coherent measurements suggest that the proposed face-based wavelet method can improve the performance of L1-norm regularized EEG/MEG inverse solutions, which was further demonstrated in simulations and experimental setups using MEG data. Thus, this new transform on complicated cortical structure is promising to significantly advance EEG/MEG inverse source imaging technologies. Copyright © 2013 Elsevier Ireland Ltd. All rights reserved.

Effect of exponential density transition on self-focusing of q-Gaussian laser beam in collisionless plasma

NASA Astrophysics Data System (ADS)

Valkunde, Amol T.; Vhanmore, Bandopant D.; Urunkar, Trupti U.; Gavade, Kusum M.; Patil, Sandip D.; Takale, Mansing V.

2018-05-01

In this work, nonlinear aspects of a high intensity q-Gaussian laser beam propagating in collisionless plasma having upward density ramp of exponential profiles is studied. We have employed the nonlinearity in dielectric function of plasma by considering ponderomotive nonlinearity. The differential equation governing the dimensionless beam width parameter is achieved by using Wentzel-Kramers-Brillouin (WKB) and paraxial approximations and solved it numerically by using Runge-Kutta fourth order method. Effect of exponential density ramp profile on self-focusing of q-Gaussian laser beam for various values of q is systematically carried out and compared with results Gaussian laser beam propagating in collisionless plasma having uniform density. It is found that exponential plasma density ramp causes the laser beam to become more focused and gives reasonably interesting results.

Anti-inflammatory treatment improves high-density lipoprotein function in rheumatoid arthritis

PubMed Central

O'Neill, Francis; Charakida, Marietta; Topham, Eric; McLoughlin, Eve; Patel, Neha; Sutill, Emma; Kay, Christopher W M; D'Aiuto, Francesco; Landmesser, Ulf; Taylor, Peter C; Deanfield, John

2017-01-01

Objective Patients with rheumatoid arthritis (RA) are at increased cardiovascular risk. Recent studies suggest that high-density lipoprotein (HDL) may lose its protective vascular phenotype in inflammatory conditions. However, the effects of common anti-inflammatory treatments on HDL function are not yet known. Methods We compared the function of HDL in 18 patients with RA and 18 matched healthy controls. Subsequently, patients were randomised to (methotrexate+infliximab (M+I) (5 mg/kg)) or methotrexate+placebo (M+P) infusions for 54 weeks. At week 54 and thereafter, all patients received infliximab therapy until completion of the trial (110 weeks), enabling assessment of the impact of 1 year of infliximab therapy in all patients. HDL functional properties were assessed at baseline, 54 weeks and 110 weeks by measuring the impact on endothelial nitric oxide (NO) bioavailability and superoxide production (SO), paraoxonase activity (PON-1) and cholesterol efflux. Results All HDL vascular assays were impaired in patients compared with controls. After 54 weeks, NO in response to HDL was significantly greater in patients who received M+I compared with those who received M+P. Endothelial SO in response to HDL was reduced in both groups, but PON-1 and cholesterol efflux remained unchanged. All vascular measures improved compared with baseline after ≥1 infliximab therapy in the analysis at 110 weeks. No significant trend was noted for cholesterol efflux. Conclusions HDL function can be improved with anti-inflammatory treatment in patients with RA. The M+I combination was superior to the M+P alone, suggesting that the tumour necrosis factor-α pathway may have a role in HDL vascular properties. PMID:27852695

A note on the accuracy of KS-DFT densities

NASA Astrophysics Data System (ADS)

Ranasinghe, Duminda S.; Perera, Ajith; Bartlett, Rodney J.

2017-11-01

The accuracy of the density of wave function methods and Kohn-Sham (KS) density functionals is studied using moments of the density, ⟨rn ⟩ =∫ ρ (r )rnd τ =∫0∞4 π r2ρ (r ) rnd r ,where n =-1 ,-2,0,1,2 ,and 3 provides information about the short- and long-range behavior of the density. Coupled cluster (CC) singles, doubles, and perturbative triples (CCSD(T)) is considered as the reference density. Three test sets are considered: boron through neon neutral atoms, two and four electron cations, and 3d transition metals. The total density and valence only density are distinguished by dropping appropriate core orbitals. Among density functionals tested, CAMQTP00 and ωB97x show the least deviation for boron through neon neutral atoms. They also show accurate eigenvalues for the HOMO indicating that they should have a more correct long-range behavior for the density. For transition metals, some density functional approximations outperform some wave function methods, suggesting that the KS determinant could be a better starting point for some kinds of correlated calculations. By using generalized many-body perturbation theory (MBPT), the convergence of second-, third-, and fourth-order KS-MBPT for the density is addressed as it converges to the infinite-order coupled cluster result. For the transition metal test set, the deviations in the KS density functional theory methods depend on the amount of exact exchange the functional uses. Functionals with exact exchange close to 25% show smaller deviations from the CCSD(T) density.

17β Estradiol increases resilience and improves hippocampal synaptic function in helpless ovariectomized rats

PubMed Central

Bredemann, Teruko M.; McMahon, Lori L.

2014-01-01

Summary Memory impairment is the most commonly reported cognitive symptom associated with major depressive disorder. Decreased hippocampal volume and neurogenesis in depression link hippocampal dysfunction with deficits in memory. Stress decreases hippocampal dendritic spine density and long-term potentiation (LTP) at glutamate synapses, a cellular correlate of learning and memory. However, elevated plasma levels of 17β estradiol (E2) during proestrus increase hippocampal structure and function, directly opposing the negative consequences of stress. In women, significant fluctuations in ovarian hormones likely increase vulnerability of hippocampal circuits to stress, potentially contributing to the greater incidence of depression compared to men. Using the learned helplessness model of depression and ovariectomized female rats, we investigated whether acquisition of helplessness and hippocampal synaptic dysfunction is differentially impacted by the presence or absence of plasma E2. We find that inescapable shock induces a greater incidence of helplessness in vehicle- versus E2-treated OVX rats. In the vehicle-treated group, LTP was absent at CA3-CA1 synapses in slices only from helpless rats, and CA1 spine density was decreased compared to resilient rats. In contrast, significant LTP was observed in slices from E2-treated helpless rats; importantly, spine density was not different between E2-treated helpless and resilient rats, dissociating spine density from the LTP magnitude. We also find that E2 replacement can reverse previously established helpless behavior. Thus, our results show that E2 replacement in OVX rats increases resilience and improves hippocampal plasticity, suggesting that E2 therapy may increase resilience to stress and preserve hippocampal function in women experiencing large fluctuations in plasma estrogen levels. PMID:24636504

Segmentation Algorithms for Detection of Targets in IR Imagery (Algorithmes de Segmentation pour la Detection de Cibles sur Images IR),

DTIC Science & Technology

1981-01-01

This fact being established, leptokurtic and platykurtic density functions are defined in terms of deviations from the normal density function. Thus...the usual definitions (Ref. 6) are: Leptokurtic - A density function that is peaked, K > 0, [18] and Platykurtic - A density function that is flat, K...has long Deen accepted that a symmetrical platykurtic density function, with K<O, is characterized by a flatter top and more abrupt terminals than the

Synthesis, spectroscopic and structural characterization of 5-benzoyl-4-phenyl-2-methylthio-1H-pyrimidine with theoretical calculations using density functional theory.

PubMed

Inkaya, Ersin; Dinçer, Muharrem; Sahan, Emine; Yıldırım, Ismail

2013-10-01

In this paper, we will report a combined experimental and theoretical investigation of the molecular structure and spectroscopic parameters (FT-IR, (1)H NMR, (13)C NMR) of 5-benzoyl-4-phenyl-2-methylthio-1H-pyrimidine. The compound crystallizes in the triclinic space group P-1 with Z=2. The molecular geometry was also optimized using density functional theory (DFT/B3LYP) method with the 6-311G(d,p) and 6-311++G(d,p) basis sets in ground state and compared with the experimental data. All the assignments of the theoretical frequencies were performed by potential energy distributions using VEDA 4 program. Information about the size, shape, charge density distribution and site of chemical reactivity of the molecules has been obtained by mapping electron density isosurface with electrostatic potential (ESP). Also, non-linear optical properties of the title compound were performed at B3LYP/6-311++G(d,p) level. The theoretical results showed an excellent agreement with the experimental values. Copyright © 2013 Elsevier B.V. All rights reserved.

Synthesis, spectroscopic and structural characterization of 5-benzoyl-4-phenyl-2-methylthio-1H-pyrimidine with theoretical calculations using density functional theory

NASA Astrophysics Data System (ADS)

İnkaya, Ersin; Dinçer, Muharrem; Şahan, Emine; Yıldırım, İsmail

2013-10-01

In this paper, we will report a combined experimental and theoretical investigation of the molecular structure and spectroscopic parameters (FT-IR, 1H NMR, 13C NMR) of 5-benzoyl-4-phenyl-2-methylthio-1H-pyrimidine. The compound crystallizes in the triclinic space group P-1 with Z = 2. The molecular geometry was also optimized using density functional theory (DFT/B3LYP) method with the 6-311G(d,p) and 6-311++G(d,p) basis sets in ground state and compared with the experimental data. All the assignments of the theoretical frequencies were performed by potential energy distributions using VEDA 4 program. Information about the size, shape, charge density distribution and site of chemical reactivity of the molecules has been obtained by mapping electron density isosurface with electrostatic potential (ESP). Also, non-linear optical properties of the title compound were performed at B3LYP/6-311++G(d,p) level. The theoretical results showed an excellent agreement with the experimental values.

A density-functional study on the electronic and vibrational properties of layered antimony telluride.

PubMed

Stoffel, Ralf P; Deringer, Volker L; Simon, Ronnie E; Hermann, Raphaël P; Dronskowski, Richard

2015-03-04

We present a comprehensive survey of electronic and lattice-dynamical properties of crystalline antimony telluride (Sb2Te3). In a first step, the electronic structure and chemical bonding have been investigated, followed by calculations of the atomic force constants, phonon dispersion relationships and densities of states. Then, (macroscopic) physical properties of Sb2Te3 have been computed, namely, the atomic thermal displacement parameters, the Grüneisen parameter γ, the volume expansion of the lattice, and finally the bulk modulus B. We compare theoretical results from three popular and economic density-functional theory (DFT) approaches: the local density approximation (LDA), the generalized gradient approximation (GGA), and a posteriori dispersion corrections to the latter. Despite its simplicity, the LDA shows excellent performance for all properties investigated-including the Grüneisen parameter, which only the LDA is able to recover with confidence. In the absence of computationally more demanding hybrid DFT methods, the LDA seems to be a good choice for further lattice dynamical studies of Sb2Te3 and related layered telluride materials.

Measurement of Electron Density Using the Multipole Resonance Probe, Langmuir Probe and Optical Emission Spectroscopy in Low Pressure Plasmas with Different Electron Energy Distribution Functions

NASA Astrophysics Data System (ADS)

Oberberg, Moritz; Bibinov, Nikita; Ries, Stefan; Awakowicz, Peter; Institute of Electrical Engineering; Plasma Technology Team

2016-09-01

In recently publication, the young diagnostic tool Multipole Resonance Probe (MRP) for electron density measurements was introduced. It is based on active plasma resonance spectroscopy (APRS). The probe was simulated und evaluated for different devices. The geometrical and electrical symmetry simplifies the APRS model, so that the electron density can be easily calculated from the measured resonance. In this work, low pressure nitrogen mixture plasmas with different electron energy distribution functions (EEDF) are investigated. The results of the MRP measurement are compared with measurements of a Langmuir Probe (LP) and Optical Emission Spectroscopy (OES). Probes and OES measure in different regimes of kinetic electron energy. Both probes measure electrons with low kinetic energy (<10 eV), whereas the OES is influenced by electrons with high kinetic energy which are needed for transitions of molecule bands. By the determination of the absolute intensity of N2(C-B) and N2+(B-X)electron temperature and density can be calculated. In a non-maxwellian plasma, all plasma diagnostics need to be combined.

The Equation of State of Triamino-Trinitrobenzene from Density Functional Theory Molecular Dynamics

NASA Astrophysics Data System (ADS)

Wixom, Ryan R.

2017-06-01

The US-uP shock Hugoniot has long been the fundamental relationship used to experimentally define the unreacted equations of state of explosives. These experiments are typically performed on porous or composite samples, providing data that is specific to the density of the samples being tested. However, If the crystalline Hugoniot is known, analytical or numerical methods can be used to transform the US-uP relationship to describe the shock response of the porous material. To obtain an accurate crystalline equation of state for TATB, density functional theory based molecular dynamics were used to map out points on the Hugoniot. Since this method provides the pressure, temperature, density, and internal energy at each point on the Hugoniot, a complete equation of state can be constructed. Isotropic, uniaxial, hydrostatic, and isothermal compression of the simulation cell were used to examine TATB under different thermodynamic conditions. A cusp is observed in the Hugoniot that correlates to loss of aromaticity of the molecule. Results of the calculations will be presented and compared to the available experimental data. Center for Integrated Nanotechnologies, Sandia National Laboratories, Albuquerque NM.

Thermodynamic Properties of HCFC142b

NASA Astrophysics Data System (ADS)

Fukushima, Masato; Watanabe, Naohiro

Thermodynamic properties of HCFC142b,namely saturated densities,vapor pressures and PVT properties,were measured and the critical parameters were determined through those experimental results. The correlations for vpor pressure, saturated liquid density and PVT properties deduced from those experimental results were compared with the measured data and also with the estimates of the other correlations published in literatures. The thermodynamic functions,such as enthalpy,entropy,heat capacity and etc.,could be considered to be reasonab1y estimatedby the expression reported in this paper.

Heterochromatic Flicker Photometry for Objective Lens Density Quantification.

PubMed

Najjar, Raymond P; Teikari, Petteri; Cornut, Pierre-Loïc; Knoblauch, Kenneth; Cooper, Howard M; Gronfier, Claude

2016-03-01

Although several methods have been proposed to evaluate lens transmittance, to date there is no consensual in vivo approach in clinical practice. The aim of this study was to compare ocular lens density and transmittance measurements obtained by an improved psychophysical scotopic heterochromatic flicker photometry (sHFP) technique to the results obtained by three other measures: a psychophysical threshold technique, a Scheimpflug imaging technique, and a clinical assessment using a validated subjective scale. Forty-three subjects (18 young, 9 middle aged, and 16 older) were included in the study. Individual lens densities were measured and transmittance curves were derived from sHFP indexes. Ocular lens densities were compared across methods by using linear regression analysis. The four approaches showed a quadratic increase in lens opacification with age. The sHFP technique revealed that transmittance decreased with age over the entire visual spectrum. This decrease was particularly pronounced between young and older participants in the short (53.03% decrease in the 400-500 nm range) wavelength regions of the light spectrum. Lens density derived from sHFP highly correlated with the values obtained with the other approaches. Compared to other objective measures, sHFP also showed the lowest variability and the best fit with a quadratic trend (r2 = 0.71) of lens density increase as a function of age. The sHFP technique offers a practical, reliable, and accurate method to measure lens density in vivo and predict lens transmittance over the visible spectrum. An accurate quantification of lens transmittance should be obtained in clinical practice, but also in research in visual and nonvisual photoreception.

Direct comparison of Viking 2.3-GHz signal phase fluctuation and columnar electron density between 2 and 160 solar radii

NASA Technical Reports Server (NTRS)

Berman, A. L.; Wackley, J. A.; Hietzke, W. H.

1982-01-01

The relationship between solar wind induced signal phase fluctuation and solar wind columnar electron density has been the subject of intensive analysis during the last two decades. In this article, a sizeable volume of 2.3-GHz signal phase fluctuation and columnar electron density measurements separately and concurrently inferred from Viking spacecraft signals are compared as a function of solar geometry. These data demonstrate that signal phase fluctuation and columnar electron density are proportional over a very wide span of solar elongation angle. A radially dependent electron density model which provides a good fit to the columnar electron density measurements and, when appropriately scaled, to the signal phase fluctuation measurements, is given. This model is also in good agreement with K-coronameter observations at 2 solar radii (2r0), with pulsar time delay measurements at 10r0, and with spacecraft in situ electron density measurements at 1 AU.

Dynamic Structure Factor: An Introduction

NASA Astrophysics Data System (ADS)

Sturm, K.

1993-02-01

The doubly differential cross-section for weak inelastic scattering of waves or particles by manybody systems is derived in Born approximation and expressed in terms of the dynamic structure factor according to van Hove. The application of this very general scheme to scattering of neutrons, x-rays and high-energy electrons is discussed briefly. The dynamic structure factor, which is the space and time Fourier transform of the density-density correlation function, is a property of the many-body system independent of the external probe and carries information on the excitation spectrum of the system. The relation of the electronic structure factor to the density-density response function defined in linear-response theory is shown using the fluctuation-dissipation theorem. This is important for calculations, since the response function can be calculated approximately from the independent-particle response function in self-consistent field approximations, such as the random-phase approximation or the local-density approximation of the density functional theory. Since the density-density response function also determines the dielectric function, the dynamic structure can be expressed by the dielectric function.

Phase space explorations in time dependent density functional theory

NASA Astrophysics Data System (ADS)

Rajam, Aruna K.

Time dependent density functional theory (TDDFT) is one of the useful tools for the study of the dynamic behavior of correlated electronic systems under the influence of external potentials. The success of this formally exact theory practically relies on approximations for the exchange-correlation potential which is a complicated functional of the co-ordinate density, non-local in space and time. Adiabatic approximations (such as ALDA), which are local in time, are most commonly used in the increasing applications of the field. Going beyond ALDA, has been proved difficult leading to mathematical inconsistencies. We explore the regions where the theory faces challenges, and try to answer some of them via the insights from two electron model systems. In this thesis work we propose a phase-space extension of the TDDFT. We want to answer the challenges the theory is facing currently by exploring the one-body phase-space. We give a general introduction to this theory and its mathematical background in the first chapter. In second chapter, we carryout a detailed study of instantaneous phase-space densities and argue that the functionals of distributions can be a better alternative to the nonlocality issue of the exchange-correlation potentials. For this we study in detail the interacting and the non-interacting phase-space distributions for Hookes atom model. The applicability of ALDA-based TDDFT for the dynamics in strongfields can become severely problematic due to the failure of single-Slater determinant picture.. In the third chapter, we analyze how the phase-space distributions can shine some light into this problem. We do a comparative study of Kohn-Sham and interacting phase-space and momentum distributions for single ionization and double ionization systems. Using a simple model of two-electron systems, we have showed that the momentum distribution computed directly from the exact KS system contains spurious oscillations: a non-classical description of the essentially classical two-electron dynamics. In Time dependent density matrix functional theory (TDDMFT), the evolution scheme of the 1RDM (first order reduced density matrix) contains second-order reduced density matrix (2RDM), which has to be expressed in terms of 1RDMs. Any non-correlated approximations (Hartree-Fock) for 2RDM would fail to capture the natural occupations of the system. In our fourth chapter, we show that by applying the quasi-classical and semi-classical approximations one can capture the natural occupations of the excited systems. We study a time-dependent Moshinsky atom model for this. The fifth chapter contains a comparative work on the existing non-local exchange-correlation kernels that are based on current density response frame work and the co-moving frame work. We show that the two approaches though coinciding with each other in linear response regime, actually turn out to be different in non-linear regime.

Local and linear chemical reactivity response functions at finite temperature in density functional theory

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

Franco-Pérez, Marco, E-mail: francopj@mcmaster.ca, E-mail: ayers@mcmaster.ca, E-mail: jlgm@xanum.uam.mx, E-mail: avela@cinvestav.mx; Departamento de Química, Universidad Autónoma Metropolitana-Iztapalapa, Av. San Rafael Atlixco 186, México, D.F. 09340; Ayers, Paul W., E-mail: francopj@mcmaster.ca, E-mail: ayers@mcmaster.ca, E-mail: jlgm@xanum.uam.mx, E-mail: avela@cinvestav.mx

2015-12-28

We explore the local and nonlocal response functions of the grand canonical potential density functional at nonzero temperature. In analogy to the zero-temperature treatment, local (e.g., the average electron density and the local softness) and nonlocal (e.g., the softness kernel) intrinsic response functions are defined as partial derivatives of the grand canonical potential with respect to its thermodynamic variables (i.e., the chemical potential of the electron reservoir and the external potential generated by the atomic nuclei). To define the local and nonlocal response functions of the electron density (e.g., the Fukui function, the linear density response function, and the dualmore » descriptor), we differentiate with respect to the average electron number and the external potential. The well-known mathematical relationships between the intrinsic response functions and the electron-density responses are generalized to nonzero temperature, and we prove that in the zero-temperature limit, our results recover well-known identities from the density functional theory of chemical reactivity. Specific working equations and numerical results are provided for the 3-state ensemble model.« less

Local and linear chemical reactivity response functions at finite temperature in density functional theory.

PubMed

Franco-Pérez, Marco; Ayers, Paul W; Gázquez, José L; Vela, Alberto

2015-12-28

We explore the local and nonlocal response functions of the grand canonical potential density functional at nonzero temperature. In analogy to the zero-temperature treatment, local (e.g., the average electron density and the local softness) and nonlocal (e.g., the softness kernel) intrinsic response functions are defined as partial derivatives of the grand canonical potential with respect to its thermodynamic variables (i.e., the chemical potential of the electron reservoir and the external potential generated by the atomic nuclei). To define the local and nonlocal response functions of the electron density (e.g., the Fukui function, the linear density response function, and the dual descriptor), we differentiate with respect to the average electron number and the external potential. The well-known mathematical relationships between the intrinsic response functions and the electron-density responses are generalized to nonzero temperature, and we prove that in the zero-temperature limit, our results recover well-known identities from the density functional theory of chemical reactivity. Specific working equations and numerical results are provided for the 3-state ensemble model.

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.

Constraints on rapidity-dependent initial conditions from charged-particle pseudorapidity densities and two-particle correlations

NASA Astrophysics Data System (ADS)

Ke, Weiyao; Moreland, J. Scott; Bernhard, Jonah E.; Bass, Steffen A.

2017-10-01

We study the initial three-dimensional spatial configuration of the quark-gluon plasma (QGP) produced in relativistic heavy-ion collisions using centrality and pseudorapidity-dependent measurements of the medium's charged particle density and two-particle correlations. A cumulant-generating function is first used to parametrize the rapidity dependence of local entropy deposition and extend arbitrary boost-invariant initial conditions to nonzero beam rapidities. The model is then compared to p +Pb and Pb + Pb charged-particle pseudorapidity densities and two-particle pseudorapidity correlations and systematically optimized using Bayesian parameter estimation to extract high-probability initial condition parameters. The optimized initial conditions are then compared to a number of experimental observables including the pseudorapidity-dependent anisotropic flows, event-plane decorrelations, and flow correlations. We find that the form of the initial local longitudinal entropy profile is well constrained by these experimental measurements.

Local population density and group composition influence the signal-preference relationship in Enchenopa treehoppers (Hemiptera: Membracidae).

PubMed

Fowler-Finn, K D; Cruz, D C; Rodríguez, R L

2017-01-01

Many animals exhibit social plasticity - changes in phenotype or behaviour in response to experience with conspecifics that change how evolutionary processes like sexual selection play out. Here, we asked whether social plasticity arising from variation in local population density in male advertisement signals and female mate preferences influences the form of sexual selection. We manipulated local density and determined whether this changed how the distribution of male signals overlapped with female preferences - the signal preference relationship. We specifically look at the shape of female mate preference functions, which, when compared to signal distributions, provide hypotheses about the form of sexual selection. We used Enchenopa binotata treehoppers, a group of plant-feeding insects that exhibit natural variation in local densities across individual host plants, populations, species and years. We measured male signal frequency and female preference functions across the density treatments. We found that male signals varied across local social groups, but not according to local density. By contrast, female preferences varied with local density - favouring higher signal frequencies in denser environments. Thus, local density changes the signal-preference relationship and, consequently, the expected form of sexual selection. We found no influence of sex ratio on the signal-preference relationship. Our findings suggest that plasticity arising from variation in local group density and composition can alter the form of sexual selection with potentially important consequences both for the maintenance of variation and for speciation. © 2016 European Society For Evolutionary Biology. Journal of Evolutionary Biology © 2016 European Society For Evolutionary Biology.

Estimation and Modeling of Enceladus Plume Jet Density Using Reaction Wheel Control Data

NASA Technical Reports Server (NTRS)

Lee, Allan Y.; Wang, Eric K.; Pilinski, Emily B.; Macala, Glenn A.; Feldman, Antonette

2010-01-01

The Cassini spacecraft was launched on October 15, 1997 by a Titan 4B launch vehicle. After an interplanetary cruise of almost seven years, it arrived at Saturn on June 30, 2004. In 2005, Cassini completed three flybys of Enceladus, a small, icy satellite of Saturn. Observations made during these flybys confirmed the existence of a water vapor plume in the south polar region of Enceladus. Five additional low-altitude flybys of Enceladus were successfully executed in 2008-9 to better characterize these watery plumes. The first of these flybys was the 50-km Enceladus-3 (E3) flyby executed on March 12, 2008. During the E3 flyby, the spacecraft attitude was controlled by a set of three reaction wheels. During the flyby, multiple plume jets imparted disturbance torque on the spacecraft resulting in small but visible attitude control errors. Using the known and unique transfer function between the disturbance torque and the attitude control error, the collected attitude control error telemetry could be used to estimate the disturbance torque. The effectiveness of this methodology is confirmed using the E3 telemetry data. Given good estimates of spacecraft's projected area, center of pressure location, and spacecraft velocity, the time history of the Enceladus plume density is reconstructed accordingly. The 1-sigma uncertainty of the estimated density is 7.7%. Next, we modeled the density due to each plume jet as a function of both the radial and angular distances of the spacecraft from the plume source. We also conjecture that the total plume density experienced by the spacecraft is the sum of the component plume densities. By comparing the time history of the reconstructed E3 plume density with that predicted by the plume model, values of the plume model parameters are determined. Results obtained are compared with those determined by other Cassini science instruments.

Estimation and Modeling of Enceladus Plume Jet Density Using Reaction Wheel Control Data

NASA Technical Reports Server (NTRS)

Lee, Allan Y.; Wang, Eric K.; Pilinski, Emily B.; Macala, Glenn A.; Feldman, Antonette

2010-01-01

The Cassini spacecraft was launched on October 15, 1997 by a Titan 4B launch vehicle. After an interplanetary cruise of almost seven years, it arrived at Saturn on June 30, 2004. In 2005, Cassini completed three flybys of Enceladus, a small, icy satellite of Saturn. Observations made during these flybys confirmed the existence of a water vapor plume in the south polar region of Enceladus. Five additional low-altitude flybys of Enceladus were successfully executed in 2008-9 to better characterize these watery plumes. The first of these flybys was the 50-km Enceladus-3 (E3) flyby executed on March 12, 2008. During the E3 flyby, the spacecraft attitude was controlled by a set of three reaction wheels. During the flyby, multiple plume jets imparted disturbance torque on the spacecraft resulting in small but visible attitude control errors. Using the known and unique transfer function between the disturbance torque and the attitude control error, the collected attitude control error telemetry could be used to estimate the disturbance torque. The effectiveness of this methodology is confirmed using the E3 telemetry data. Given good estimates of spacecraft's projected area, center of pressure location, and spacecraft velocity, the time history of the Enceladus plume density is reconstructed accordingly. The 1 sigma uncertainty of the estimated density is 7.7%. Next, we modeled the density due to each plume jet as a function of both the radial and angular distances of the spacecraft from the plume source. We also conjecture that the total plume density experienced by the spacecraft is the sum of the component plume densities. By comparing the time history of the reconstructed E3 plume density with that predicted by the plume model, values of the plume model parameters are determined. Results obtained are compared with those determined by other Cassini science instruments.

Alterations of brain grey matter density and olfactory bulb volume in patients with olfactory loss after traumatic brain injury.

PubMed

Han, Pengfei; Winkler, Nicole; Hummel, Cornelia; Hähner, Antje; Gerber, Johannes; Hummel, Thomas

2018-04-27

Olfactory loss and traumatic brain injury (TBI) both lead to anatomical brain alterations in humans. Little research has been done on the structural brain changes for TBI patients with olfactory loss. Using voxel-based morphometry, the grey matter (GM) density was examined for twenty-two TBI patients with hyposmia, twenty-four TBI patients with anosmia, and twenty-two age-matched controls. Olfactory bulb (OB) volumes were measured by manual segmentation of acquired T2 weighted coronal slices using a standardized protocol. Brain lesions in the olfactory relevant areas were also examined for TBI patients. Results showed that patients with anosmia have more frequent lesions in the OB, orbitofrontal cortex (OFC) and the temporal lobe pole, as compared to patients with hyposmia. GM density in the primary olfactory area was decreased in both groups of patients. In addition, compared to controls, patients with anosmia showed GM density reduction in several secondary olfactory eloquent regions, including the gyrus rectus, medial OFC, anterior cingulate cortex, insula, and cerebellum. However, patients with hyposmia showed a lesser degree of GM reduction compared to healthy controls. Smaller OB volumes were found for patients with olfactory loss as compared to controls. TBI patients with anosmia had the smallest OB volumes which were caused by the lesions for OB. In addition, post-TBI duration was negatively correlated with GM density in the secondary olfactory areas in patients with hyposmia, but was positively correlated with GM density in the frontal and temporal gyrus in patients with anosmia. The GM density and OB volume reduction among TBI patients with olfactory loss was largely depend on the location and severity of brain lesions in olfactory relevant regions. Longer post-TBI duration had an impact on brain GM density changes, which indicate a decreased olfactory function in patients with hyposmia and possible compensatory mechanisms in patients with anosmia.

Free Energy Calculations of Crystalline Hard Sphere Complexes Using Density Functional Theory

DOE PAGES

Gunawardana, K. G.S.H.; Song, Xueyu

2014-12-22

Recently developed fundamental measure density functional theory (FMT) is used to study binary hard sphere (HS) complexes in crystalline phases. By comparing the excess free energy, pressure and phase diagram, we show that the fundamental measure functional yields good agreements to the available simulation results of AB, AB 2 and AB 13 crystals. Additionally, we use this functional to study the HS models of five binary crystals, Cu 5Zr(C15 b), Cu 51Zr 14(β), Cu 10Zr 7(φ), CuZr(B2) and CuZr 2 (C11 b), which are observed in the Cu-Zr system. The FMT functional gives well behaved minimum for most of themore » hard sphere crystal complexes in the two dimensional Gaussian space, namely a crystalline phase. However, the current version of FMT functional (white Bear) fails to give a stable minimum for the structure Cu 10Zr 7(φ). We argue that the observed solid phases for the HS models of the Cu-Zr system are true thermodynamic stable phases and can be used as a reference system in perturbation calculations.« less

On the subsystem formulation of linear-response time-dependent DFT.

PubMed

Pavanello, Michele

2013-05-28

A new and thorough derivation of linear-response subsystem time-dependent density functional theory (TD-DFT) is presented and analyzed in detail. Two equivalent derivations are presented and naturally yield self-consistent subsystem TD-DFT equations. One reduces to the subsystem TD-DFT formalism of Neugebauer [J. Chem. Phys. 126, 134116 (2007)]. The other yields Dyson type equations involving three types of subsystem response functions: coupled, uncoupled, and Kohn-Sham. The Dyson type equations for subsystem TD-DFT are derived here for the first time. The response function formalism reveals previously hidden qualities and complications of subsystem TD-DFT compared with the regular TD-DFT of the supersystem. For example, analysis of the pole structure of the subsystem response functions shows that each function contains information about the electronic spectrum of the entire supersystem. In addition, comparison of the subsystem and supersystem response functions shows that, while the correlated response is subsystem additive, the Kohn-Sham response is not. Comparison with the non-subjective partition DFT theory shows that this non-additivity is largely an artifact introduced by the subjective nature of the density partitioning in subsystem DFT.

Correlation functional in screened-exchange density functional theory procedures.

PubMed

Chan, Bun; Kawashima, Yukio; Hirao, Kimihiko

2017-10-15

In the present study, we have explored several prospects for the further development of screened-exchange density functional theory (SX-DFT) procedures. Using the performance of HSE06 as our measure, we find that the use of alternative correlation functionals (as oppose to PBEc in HSE06) also yields adequate results for a diverse set of thermochemical properties. We have further examined the performance of new SX-DFT procedures (termed HSEB-type methods) that comprise the HSEx exchange and a (near-optimal) reparametrized B97c (c OS,0  = c SS,0  = 1, c OS,1  = -1.5, c OS,2  = -0.644, c SS,1  = -0.5, and c SS,2  = 1.10) correlation functionals. The different variants of HSEB all perform comparably to or slightly better than the original HSE-type procedures. These results, together with our fundamental analysis of correlation functionals, point toward various directions for advancing SX-DFT methods. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

Getting More Power from Your Flowers: Multi-Functional Flower Strips Enhance Pollinators and Pest Control Agents in Apple Orchards.

PubMed

Campbell, Alistair John; Wilby, Andrew; Sutton, Peter; Wäckers, Felix

2017-09-20

Flower strips are commonly recommended to boost biodiversity and multiple ecosystem services (e.g., pollination and pest control) on farmland. However, significant knowledge gaps remain regards the extent to which they deliver on these aims. Here, we tested the efficacy of flower strips that targeted different subsets of beneficial arthropods (pollinators and natural enemies) and their ecosystem services in cider apple orchards. Treatments included mixes that specifically targeted: (1) pollinators ('concealed-nectar plants'); (2) natural enemies ('open-nectar plants'); or (3) both groups concurrently (i.e., 'multi-functional' mix). Flower strips were established in alleyways of four orchards and compared to control alleyways (no flowers). Pollinator (e.g., bees) and natural enemy (e.g., parasitoid wasps, predatory flies and beetles) visitation to flower strips, alongside measures of pest control (aphid colony densities, sentinel prey predation), and fruit production, were monitored in orchards over two consecutive growing seasons. Targeted flower strips attracted either pollinators or natural enemies, whereas mixed flower strips attracted both groups in similar abundance to targeted mixes. Natural enemy densities on apple trees were higher in plots containing open-nectar plants compared to other treatments, but effects were stronger for non-aphidophagous taxa. Predation of sentinel prey was enhanced in all flowering plots compared to controls but pest aphid densities and fruit yield were unaffected by flower strips. We conclude that 'multi-functional' flower strips that contain flowering plant species with opposing floral traits can provide nectar and pollen for both pollinators and natural enemies, but further work is required to understand their potential for improving pest control services and yield in cider apple orchards.

PAREMD: A parallel program for the evaluation of momentum space properties of atoms and molecules

NASA Astrophysics Data System (ADS)

Meena, Deep Raj; Gadre, Shridhar R.; Balanarayan, P.

2018-03-01

The present work describes a code for evaluating the electron momentum density (EMD), its moments and the associated Shannon information entropy for a multi-electron molecular system. The code works specifically for electronic wave functions obtained from traditional electronic structure packages such as GAMESS and GAUSSIAN. For the momentum space orbitals, the general expression for Gaussian basis sets in position space is analytically Fourier transformed to momentum space Gaussian basis functions. The molecular orbital coefficients of the wave function are taken as an input from the output file of the electronic structure calculation. The analytic expressions of EMD are evaluated over a fine grid and the accuracy of the code is verified by a normalization check and a numerical kinetic energy evaluation which is compared with the analytic kinetic energy given by the electronic structure package. Apart from electron momentum density, electron density in position space has also been integrated into this package. The program is written in C++ and is executed through a Shell script. It is also tuned for multicore machines with shared memory through OpenMP. The program has been tested for a variety of molecules and correlated methods such as CISD, Møller-Plesset second order (MP2) theory and density functional methods. For correlated methods, the PAREMD program uses natural spin orbitals as an input. The program has been benchmarked for a variety of Gaussian basis sets for different molecules showing a linear speedup on a parallel architecture.

NeutrAvidin Functionalization of CdSe/CdS Quantum Nanorods and Quantification of Biotin Binding Sites using Biotin-4-Fluorescein Fluorescence Quenching.

PubMed

Lippert, Lisa G; Hallock, Jeffrey T; Dadosh, Tali; Diroll, Benjamin T; Murray, Christopher B; Goldman, Yale E

2016-03-16

We developed methods to solubilize, coat, and functionalize with NeutrAvidin elongated semiconductor nanocrystals (quantum nanorods, QRs) for use in single molecule polarized fluorescence microscopy. Three different ligands were compared with regard to efficacy for attaching NeutrAvidin using the "zero-length cross-linker" 1-ethyl-3-[3-(dimethylamino)propyl]carbodiimide (EDC). Biotin-4-fluorescene (B4F), a fluorophore that is quenched when bound to avidin proteins, was used to quantify biotin binding activity of the NeutrAvidin coated QRs and biotin binding activity of commercially available streptavidin coated quantum dots (QDs). All three coating methods produced QRs with NeutrAvidin coating density comparable to the streptavidin coating density of the commercially available quantum dots (QDs) in the B4F assay. One type of QD available from the supplier (ITK QDs) exhibited ∼5-fold higher streptavidin surface density compared to our QRs, whereas the other type of QD (PEG QDs) had 5-fold lower density. The number of streptavidins per QD increased from ∼7 streptavidin tetramers for the smallest QDs emitting fluorescence at 525 nm (QD525) to ∼20 tetramers for larger, longer wavelength QDs (QD655, QD705, and QD800). QRs coated with NeutrAvidin using mercaptoundecanoicacid (MUA) and QDs coated with streptavidin bound to biotinylated cytoplasmic dynein in single molecule TIRF microscopy assays, whereas Poly(maleic anhydride-alt-1-ocatdecene) (PMAOD) or glutathione (GSH) QRs did not bind cytoplasmic dynein. The coating methods require optimization of conditions and concentrations to balance between substantial NeutrAvidin binding vs tendency of QRs to aggregate and degrade over time.

Theoretical characterization and design of small molecule donor material containing naphthodithiophene central unit for efficient organic solar cells.

PubMed

Duan, Yu-Ai; Geng, Yun; Li, Hai-Bin; Jin, Jun-Ling; Wu, Yong; Su, Zhong-Min

2013-07-15

To seek for high-performance small molecule donor materials used in heterojunction solar cell, six acceptor-donor-acceptor small molecules based on naphtho[2,3-b:6,7-b']dithiophene (NDT) units with different acceptor units were designed and characterized using density functional theory and time-dependent density functional theory. Their geometries, electronic structures, photophysical, and charge transport properties have been scrutinized comparing with the reported donor material NDT(TDPP)2 (TDPP  =  thiophene-capped diketopyrrolopyrrole). The open circuit voltage (V(oc)), energetic driving force(ΔE(L-L)), and exciton binding energy (E(b)) were also provided to give an elementary understanding on their cell performance. The results reveal that the frontier molecular orbitals of 3-7 match well with the acceptor material PC61 BM, and compounds 3-5 were found to exhibit the comparable performances to 1 and show promising potential in organic solar cells. In particular, comparing with 1, system 7 with naphthobisthiadiazole acceptor unit displays broader absorption spectrum, higher V(oc), lower E(b), and similar carrier mobility. An in-depth insight into the nature of the involved excited states based on transition density matrix and charge density difference indicates that all S1 states are mainly intramolecular charge transfer states with the charge transfer from central NDT unit to bilateral acceptor units, and also imply that the exciton of 7 can be dissociated easily due to its large extent of the charge transfer. In a word, 7 maybe superior to 1 and may act as a promising donor candidate for organic solar cell. Copyright © 2013 Wiley Periodicals, Inc.

Light drives vertical gradients of leaf morphology in a sugar maple (Acer saccharum) forest.

PubMed

Coble, Adam P; Cavaleri, Molly A

2014-02-01

Leaf mass per area (LMA, g m(-2)) is an essential trait for modeling canopy function due to its strong association with photosynthesis, respiration and leaf nitrogen. Leaf mass per area, which is influenced by both leaf thickness and density (LMA = thickness × density), generally increases from the bottom to the top of tree canopies, yet the mechanisms behind this universal pattern are not yet resolved. For decades, the light environment was assumed to be the most influential driver of within-canopy variation in LMA, yet recent evidence has shown hydrostatic gradients to be more important in upper canopy positions, especially in tall evergreen trees in temperate and tropical forests. The aim of this study was to disentangle the importance of various environmental drivers on vertical LMA gradients in a mature sugar maple (Acer saccharum Marshall) forest. We compared LMA, leaf density and leaf thickness relationships with height, light and predawn leaf water potential (ΨPre) within a closed and an exposed canopy to assess leaf morphological traits at similar heights but different light conditions. Contrary to our expectations and recent findings in the literature, we found strong evidence that light was the primary driver of vertical gradients in leaf morphology. At similar heights (13-23 m), LMA was greater within the exposed canopy than the closed canopy, and light had a stronger influence over LMA compared with ΨPre. Light also had a stronger influence over both leaf thickness and density compared with ΨPre; however, the increase in LMA within both canopy types was primarily due to increasing leaf thickness with increasing light availability. This study provides strong evidence that canopy structure and crown exposure, in addition to height, should be considered as a parameter for determining vertical patterns in LMA and modeling canopy function.

Energy transmission transformer for a wireless capsule endoscope: analysis of specific absorption rate and current density in biological tissue.

PubMed

Shiba, Kenji; Nagato, Tomohiro; Tsuji, Toshio; Koshiji, Kohji

2008-07-01

This paper reports on the electromagnetic influences on the analysis of biological tissue surrounding a prototype energy transmission system for a wireless capsule endoscope. Specific absorption rate (SAR) and current density were analyzed by electromagnetic simulator in a model consisting of primary coil and a human trunk including the skin, fat, muscle, small intestine, backbone, and blood. First, electric and magnetic strength in the same conditions as the analytical model were measured and compared to the analytical values to confirm the validity of the analysis. Then, SAR and current density as a function of frequency and output power were analyzed. The validity of the analysis was confirmed by comparing the analytical values with the measured ones. The SAR was below the basic restrictions of the International Commission on Nonionizing Radiation Protection (ICNIRP). At the same time, the results for current density show that the influence on biological tissue was lowest in the 300-400 kHz range, indicating that it was possible to transmit energy safely up to 160 mW. In addition, we confirmed that the current density has decreased by reducing the primary coil's current.

[Phytoestrogens role in bone functional structure protection in the ovariectomized rat].

PubMed

Mihalache, Gr; Mihalache, Gr D; Indrei, L L; Indrei, Anca; Hegsted, Maren

2002-01-01

Effects of soy protein diet on bone formation and density were evaluated in ovariectomized rats as a model for postmenopausal women. Twenty-seven 9-month-old rats were assigned to 3 treatment groups for the 9-week study: sham-surgery (Sh, n = 9); ovariectomy (Ovx, n = 9); ovariectomy + soy diet (OvxS, n = 9). Rats had free access to an AIN-93 M diet or AIN-93 M diet with 7% soy protein concentration and water. At sacrifice, rear legs were removed, and the right femur and tibia were cleaned manually. Serum alkaline phosphatase, a marker of bone formation, was measured colorimetrically. Bone density was measured using Archimedes' Principle. Alkaline phosphatase activity was greater in OvxS (114 +/- 19 U/L) and Ovx (128 +/- 26 U/L) compared to Sh (110 +/- 22 U/L). Femur bone density was greater for OvxS (1.520 +/- 0.02 g/cc) compared to Ovx (1.510 +/- 0.017 g/cc), but not to Sh (1532 +/- 0.025 g/cc). Tibia bone density was greater for OvxS (1.560 +/- 0.019 g/cc) compared to Ovx (1.553 +/- 0.015 g/cc), but not to Sh (1566 +/- 0.03 g/cc). In conclusion soy protein diet increased the rate of bone formation and bone density in some bones, suggesting that may help prevent bone loss in postmenopausal women.

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.

Hybrid-PIC Modeling of the Transport of Atomic Boron in a Hall Thruster

NASA Technical Reports Server (NTRS)

Smith, Brandon D.; Boyd, Iaian D.; Kamhawi, Hani

2015-01-01

Computational analysis of the transport of boron eroded from the walls of a Hall thruster is performed by implementing sputter yields of hexagonal boron nitride and velocity distribution functions of boron within the hybrid-PIC model HPHall. The model is applied to simulate NASA's HiVHAc Hall thruster at a discharge voltage of 500V and discharge powers of 1-3 kW. The number densities of ground- and 4P-state boron are computed. The density of ground-state boron is shown to be a factor of about 30 less than the plasma density. The density of the excited state is shown to be about three orders of magnitude less than that of the ground state, indicating that electron impact excitation does not significantly affect the density of ground-state boron in the discharge channel or near-field plume of a Hall thruster. Comparing the rates of excitation and ionization suggests that ionization has a greater influence on the density of ground-state boron, but is still negligible. The ground-state boron density is then integrated and compared to cavity ring-down spectroscopy (CRDS) measurements for each operating point. The simulation results show good agreement with the measurements for all operating points and provide evidence in support of CRDS as a tool for measuring Hall thruster erosion in situ.

Sum-over-states density functional perturbation theory: Prediction of reliable 13C, 15N, and 17O nuclear magnetic resonance chemical shifts

NASA Astrophysics Data System (ADS)

Olsson, Lars; Cremer, Dieter

1996-11-01

Sum-over-states density functional perturbation theory (SOS-DFPT) has been used to calculate 13C, 15N, and 17O NMR chemical shifts of 20 molecules, for which accurate experimental gas-phase values are available. Compared to Hartree-Fock (HF), SOS-DFPT leads to improved chemical shift values and approaches the degree of accuracy obtained with second order Møller-Plesset perturbation theory (MP2). This is particularly true in the case of 15N chemical shifts where SOS-DFPT performs even better than MP2. Additional improvements of SOS-DFPT chemical shifts can be obtained by empirically correcting diamagnetic and paramagnetic contributions to compensate for deficiencies which are typical of DFT.

Relativistic Brueckner-Hartree-Fock theory for neutron drops

NASA Astrophysics Data System (ADS)

Shen, Shihang; Liang, Haozhao; Meng, Jie; Ring, Peter; Zhang, Shuangquan

2018-05-01

Neutron drops confined in an external field are studied in the framework of relativistic Brueckner-Hartree-Fock theory using the bare nucleon-nucleon interaction. The ground-state energies and radii of neutron drops with even numbers from N =4 to N =50 are calculated and compared with results obtained from other nonrelativistic ab initio calculations and from relativistic density functional theory. Special attention has been paid to the magic numbers and to the subshell closures. The single-particle energies are investigated and the monopole effect of the tensor force on the evolutions of the spin-orbit and the pseudospin-orbit splittings is discussed. The results provide interesting insights into neutron-rich systems and can form an important guide for future density functionals.

Boundary Conditions for Infinite Conservation Laws

NASA Astrophysics Data System (ADS)

Rosenhaus, V.; Bruzón, M. S.; Gandarias, M. L.

2016-12-01

Regular soliton equations (KdV, sine-Gordon, NLS) are known to possess infinite sets of local conservation laws. Some other classes of nonlinear PDE possess infinite-dimensional symmetries parametrized by arbitrary functions of independent or dependent variables; among them are Zabolotskaya-Khokhlov, Kadomtsev-Petviashvili, Davey-Stewartson equations and Born-Infeld equation. Boundary conditions were shown to play an important role for the existence of local conservation laws associated with infinite-dimensional symmetries. In this paper, we analyze boundary conditions for the infinite conserved densities of regular soliton equations: KdV, potential KdV, Sine-Gordon equation, and nonlinear Schrödinger equation, and compare them with boundary conditions for the conserved densities obtained from infinite-dimensional symmetries with arbitrary functions of independent and dependent variables.

Ab initio density functional theory investigation of electronic properties of semiconducting single-walled carbon nanotube bundles

NASA Astrophysics Data System (ADS)

Moradian, Rostam; Behzad, Somayeh; Azadi, Sam

2008-09-01

By using ab initio density functional theory we investigated the structural and electronic properties of semiconducting (7, 0), (8, 0) and (10, 0) carbon nanotube bundles. The energetic and electronic evolutions of nanotubes in the bundling process are also studied. The effects of inter-tube coupling on the electronic dispersions of semiconducting carbon nanotube bundles are demonstrated. Our results show that the inter-tube coupling decreases the energy gap in semiconducting nanotubes. We found that bundles of (7, 0) and (8, 0) carbon nanotubes have metallic feature, while (10, 0) bundle is a semiconductor with an energy gap of 0.22 eV. To clarify our results the band structures of isolated and bundled nanotubes are compared.

A comparative density functional theory study of electronic structure and optical properties of γ-aminobutyric acid and its cocrystals with oxalic and benzoic acid

NASA Astrophysics Data System (ADS)

da Silva Filho, J. G.; Freire, V. N.; Caetano, E. W. S.; Ladeira, L. O.; Fulco, U. L.; Albuquerque, E. L.

2013-11-01

In this letter, we study the electronic structure and optical properties of the active medicinal component γ-aminobutyric acid (GABA) and its cocrystals with oxalic (OXA) and benzoic (BZA) acid by means of the density functional theory formalism. It is shown that the cocrystallization strongly weakens the zwitterionic character of the GABA molecule leading to striking differences among the electronic band structures and optical absorption spectra of the GABA crystal and GABA:OXA, GABA:BZA cocrystals, originating from distinct sets of hydrogen bonds. Calculated band widths and Δ-sol band gap estimates indicate that both GABA and GABA:OXA, GABA:BZA cocrystals are indirect gap insulators.

Actinide chemistry using singlet-paired coupled cluster and its combinations with density functionals

NASA Astrophysics Data System (ADS)

Garza, Alejandro J.; Sousa Alencar, Ana G.; Scuseria, Gustavo E.

2015-12-01

Singlet-paired coupled cluster doubles (CCD0) is a simplification of CCD that relinquishes a fraction of dynamic correlation in order to be able to describe static correlation. Combinations of CCD0 with density functionals that recover specifically the dynamic correlation missing in the former have also been developed recently. Here, we assess the accuracy of CCD0 and CCD0+DFT (and variants of these using Brueckner orbitals) as compared to well-established quantum chemical methods for describing ground-state properties of singlet actinide molecules. The f0 actinyl series (UO22+, NpO23+, PuO24+), the isoelectronic NUN, and thorium (ThO, ThO2+) and nobelium (NoO, NoO2) oxides are studied.

Towards the stabilization of the low density elements in topology optimization with large deformation

NASA Astrophysics Data System (ADS)

Lahuerta, Ricardo Doll; Simões, Eduardo T.; Campello, Eduardo M. B.; Pimenta, Paulo M.; Silva, Emilio C. N.

2013-10-01

This work addresses the treatment of lower density regions of structures undergoing large deformations during the design process by the topology optimization method (TOM) based on the finite element method. During the design process the nonlinear elastic behavior of the structure is based on exact kinematics. The material model applied in the TOM is based on the solid isotropic microstructure with penalization approach. No void elements are deleted and all internal forces of the nodes surrounding the void elements are considered during the nonlinear equilibrium solution. The distribution of design variables is solved through the method of moving asymptotes, in which the sensitivity of the objective function is obtained directly. In addition, a continuation function and a nonlinear projection function are invoked to obtain a checkerboard free and mesh independent design. 2D examples with both plane strain and plane stress conditions hypothesis are presented and compared. The problem of instability is overcome by adopting a polyconvex constitutive model in conjunction with a suggested relaxation function to stabilize the excessive distorted elements. The exact tangent stiffness matrix is used. The optimal topology results are compared to the results obtained by using the classical Saint Venant-Kirchhoff constitutive law, and strong differences are found.

Comparisons of thermospheric density data sets and models

NASA Astrophysics Data System (ADS)

Doornbos, Eelco; van Helleputte, Tom; Emmert, John; Drob, Douglas; Bowman, Bruce R.; Pilinski, Marcin

During the past decade, continuous long-term data sets of thermospheric density have become available to researchers. These data sets have been derived from accelerometer measurements made by the CHAMP and GRACE satellites and from Space Surveillance Network (SSN) tracking data and related Two-Line Element (TLE) sets. These data have already resulted in a large number of publications on physical interpretation and improvement of empirical density modelling. This study compares four different density data sets and two empirical density models, for the period 2002-2009. These data sources are the CHAMP (1) and GRACE (2) accelerometer measurements, the long-term database of densities derived from TLE data (3), the High Accuracy Satellite Drag Model (4) run by Air Force Space Command, calibrated using SSN data, and the NRLMSISE-00 (5) and Jacchia-Bowman 2008 (6) empirical models. In describing these data sets and models, specific attention is given to differences in the geo-metrical and aerodynamic satellite modelling, applied in the conversion from drag to density measurements, which are main sources of density biases. The differences in temporal and spa-tial resolution of the density data sources are also described and taken into account. With these aspects in mind, statistics of density comparisons have been computed, both as a function of solar and geomagnetic activity levels, and as a function of latitude and local solar time. These statistics give a detailed view of the relative accuracy of the different data sets and of the biases between them. The differences are analysed with the aim at providing rough error bars on the data and models and pinpointing issues which could receive attention in future iterations of data processing algorithms and in future model development.

Association between ethnicity and obesity with high-density lipoprotein (HDL) function and subclass distribution.

PubMed

Woudberg, Nicholas J; Goedecke, Julia H; Blackhurst, Dee; Frias, Miguel; James, Richard; Opie, Lionel H; Lecour, Sandrine

2016-05-11

Obesity and low high-density lipoprotein-cholesterol (HDL-C) levels are associated with cardiovascular risk. Surprisingly, despite a greater prevalence of obesity and lower HDL concentrations than white women, black South African women are relatively protected against ischaemic heart disease. We investigated whether this apparent discrepancy may be related to different HDL function and subclass distribution in black and white, normal-weight and obese South African women (n = 40). HDL functionality was assessed by measuring paraoxonase (PON) activity, platelet activating factor acetylhydrolase (PAF-AH) activity, Oxygen Radical Absorbance Capacity (ORAC) and quantification of the expression of vascular cell adhesion molecule in endothelial cells. PON-1 and PAF-AH expression was determined in isolated HDL and serum using Western blotting. Levels of large, intermediate and small HDL subclasses were measured using the Lipoprint® system. PON activity was lower in white compared to black women (0.49 ± 0.09 U/L vs 0.78 ± 0.10 U/L, p < 0.05), regardless of PON-1 protein levels. Obese black women had lower PAF-AH activity (9.34 ± 1.15 U/L vs 13.89 ± 1.21 U/L, p <0.05) and HDL-associated PAF-AH expression compared to obese white women. Compared to normal-weight women, obese women had lower large HDL, greater intermediate and small HDL; an effect that was more pronounced in white women than black women. There were no differences in antioxidant capacity or anti-inflammatory function across groups. Our data show that both obesity and ethnicity are associated with differences in HDL functionality, while obesity was associated with decreases in large HDL subclass distribution. Measuring HDL functionality and subclass may, therefore, be important factors to consider when assessing cardiovascular risk.

Magnetic-Field Density-Functional Theory (BDFT): Lessons from the Adiabatic Connection.

PubMed

Reimann, Sarah; Borgoo, Alex; Tellgren, Erik I; Teale, Andrew M; Helgaker, Trygve

2017-09-12

We study the effects of magnetic fields in the context of magnetic field density-functional theory (BDFT), where the energy is a functional of the electron density ρ and the magnetic field B. We show that this approach is a worthwhile alternative to current-density functional theory (CDFT) and may provide a viable route to the study of many magnetic phenomena using density-functional theory (DFT). The relationship between BDFT and CDFT is developed and clarified within the framework of the four-way correspondence of saddle functions and their convex and concave parents in convex analysis. By decomposing the energy into its Kohn-Sham components, we demonstrate that the magnetizability is mainly determined by those energy components that are related to the density. For existing density functional approximations, this implies that, for the magnetizability, improvements of the density will be more beneficial than introducing a magnetic-field dependence in the correlation functional. However, once a good charge density is achieved, we show that high accuracy is likely only obtainable by including magnetic-field dependence. We demonstrate that adiabatic-connection (AC) curves at different field strengths resemble one another closely provided each curve is calculated at the equilibrium geometry of that field strength. In contrast, if all AC curves are calculated at the equilibrium geometry of the field-free system, then the curves change strongly with increasing field strength due to the increasing importance of static correlation. This holds also for density functional approximations, for which we demonstrate that the main error encountered in the presence of a field is already present at zero field strength, indicating that density-functional approximations may be applied to systems in strong fields, without the need to treat additional static correlation.

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

Ren, X. G.; Ning, C. G.; Zhang, S. F.

The measurements of electron density distributions and binding-energy spectrum of the complete valence shell of cyclopentene (C{sub 5}H{sub 8}) using a binary (e,2e) electron momentum spectrometer are reported. The experimental momentum profiles of the valence orbitals are compared with the theoretical distributions calculated using Hartree-Fock and density-functional-theory (DFT) methods with various basis sets. The agreement between theory and experiment for the shape and intensity of the orbital electron momentum distributions is generally good. The DFT calculations employing B3LYP hybrid functional with a saturated and diffuse AUG-CC-PVTZ basis set provide the better descriptions of the experimental data. Some ''turn up'' effectsmore » in the low momentum region of the measured (e,2e) cross section compared with the calculations of 3a{sup ''}, 2a{sup ''}, and 3a{sup '} orbitals could be mainly attributed to distorted-wave effects. The pole strengths of the main ionization peaks from the orbitals in the inner valence are estimated.« less

Equation of state of mixtures: density functional theory (DFT) simulations and experiments on Sandia's Z machine

NASA Astrophysics Data System (ADS)

Magyar, R. J.; Root, S.; Haill, T. A.; Schroen, D. G.; Mattsson, T. R.; Flicker, D. G.; Sandia National Laboratories Collaboration

2011-06-01

Mixtures of materials are expected to behave quite differently from their isolated constituents, particularly when the constituents atomic numbers differ significantly. To investigate the mixture behavior, we performed density functional theory (DFT) calculations on xenon/hydrogen, xenon/ethane, and platinum/hydrocarbon mixtures. In addition, we performed shock compression experiments on platinum-doped hydrocarbon foams up to 480 GPa using the Sandia Z-accelerator. Since the DFT simulations treat electrons and nuclei generically, simulations of pure and mix systems are expected to be of comparable accuracy. The DFT and experimental results are compared to hydrodynamic simulations using different mixing models in the equation of state. The role of de-mixing and the relative contributions of the enthalpy of mixing are explored. Sandia National Laboratories is a multi-program laboratory operated by Sandia Corporation, a wholly owned subsidiary of the Lockheed Martin company, for the U.S. Department of Energy's National Nuclear Security Administration under contract DE-AC04-94AL85000.

Computational phase diagrams of noble gas hydrates under pressure

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

Teeratchanan, Pattanasak, E-mail: s1270872@sms.ed.ac.uk; Hermann, Andreas, E-mail: a.hermann@ed.ac.uk

2015-10-21

We present results from a first-principles study on the stability of noble gas-water compounds in the pressure range 0-100 kbar. Filled-ice structures based on the host water networks ice-I{sub h}, ice-I{sub c}, ice-II, and C{sub 0} interacting with guest species He, Ne, and Ar are investigated, using density functional theory (DFT) with four different exchange-correlation functionals that include dispersion effects to various degrees: the non-local density-based optPBE-van der Waals (vdW) and rPW86-vdW2 functionals, the semi-empirical D2 atom pair correction, and the semi-local PBE functional. In the He-water system, the sequence of stable phases closely matches that seen in the hydrogenmore » hydrates, a guest species of comparable size. In the Ne-water system, we predict a novel hydrate structure based on the C{sub 0} water network to be stable or at least competitive at relatively low pressure. In the Ar-water system, as expected, no filled-ice phases are stable; however, a partially occupied Ar-C{sub 0} hydrate structure is metastable with respect to the constituents. The ability of the different DFT functionals to describe the weak host-guest interactions is analysed and compared to coupled cluster results on gas phase systems.« less

What can volumes reveal about human brain evolution? A framework for bridging behavioral, histometric, and volumetric perspectives

PubMed Central

de Sousa, Alexandra A.; Proulx, Michael J.

2014-01-01

An overall relationship between brain size and cognitive ability exists across primates. Can more specific information about neural function be gleaned from cortical area volumes? Numerous studies have found significant relationships between brain structures and behaviors. However, few studies have speculated about brain structure-function relationships from the microanatomical to the macroanatomical level. Here we address this problem in comparative neuroanatomy, where the functional relevance of overall brain size and the sizes of cortical regions have been poorly understood, by considering comparative psychology, with measures of visual acuity and the perception of visual illusions. We outline a model where the macroscopic size (volume or surface area) of a cortical region (such as the primary visual cortex, V1) is related to the microstructure of discrete brain regions. The hypothesis developed here is that an absolutely larger V1 can process more information with greater fidelity due to having more neurons to represent a field of space. This is the first time that the necessary comparative neuroanatomical research at the microstructural level has been brought to bear on the issue. The evidence suggests that as the size of V1 increases: the number of neurons increases, the neuron density decreases, and the density of neuronal connections increases. Thus, we describe how information about gross neuromorphology, using V1 as a model for the study of other cortical areas, may permit interpretations of cortical function. PMID:25009469

Multiconfiguration Pair-Density Functional Theory Is as Accurate as CASPT2 for Electronic Excitation.

PubMed

Hoyer, Chad E; Ghosh, Soumen; Truhlar, Donald G; Gagliardi, Laura

2016-02-04

A correct description of electronically excited states is critical to the interpretation of visible-ultraviolet spectra, photochemical reactions, and excited-state charge-transfer processes in chemical systems. We have recently proposed a theory called multiconfiguration pair-density functional theory (MC-PDFT), which is based on a combination of multiconfiguration wave function theory and a new kind of density functional called an on-top density functional. Here, we show that MC-PDFT with a first-generation on-top density functional performs as well as CASPT2 for an organic chemistry database including valence, Rydberg, and charge-transfer excitations. The results are very encouraging for practical applications.

Wireless sensor node for surface seawater density measurements.

PubMed

Baronti, Federico; Fantechi, Gabriele; Roncella, Roberto; Saletti, Roberto

2012-01-01

An electronic meter to measure surface seawater density is presented. It is based on the measurement of the difference in displacements of a surface level probe and a weighted float, which according to Archimedes' law depends on the density of the water. The displacements are simultaneously measured using a high-accuracy magnetostrictive sensor, to which a custom electronic board provides a wireless connection and power supply so that it can become part of a wireless sensor network. The electronics are designed so that different kinds of wireless networks can be used, by simply changing the wireless module and the relevant firmware of the microcontroller. Lastly, laboratory and at-sea tests are presented and discussed in order to highlight the functionality and the performance of a prototype of the wireless density meter node in a Bluetooth radio network. The experimental results show a good agreement of the values of the calculated density compared to reference hydrometer readings.

Wireless Sensor Node for Surface Seawater Density Measurements

PubMed Central

Baronti, Federico; Fantechi, Gabriele; Roncella, Roberto; Saletti, Roberto

2012-01-01

An electronic meter to measure surface seawater density is presented. It is based on the measurement of the difference in displacements of a surface level probe and a weighted float, which according to Archimedes’ law depends on the density of the water. The displacements are simultaneously measured using a high-accuracy magnetostrictive sensor, to which a custom electronic board provides a wireless connection and power supply so that it can become part of a wireless sensor network. The electronics are designed so that different kinds of wireless networks can be used, by simply changing the wireless module and the relevant firmware of the microcontroller. Lastly, laboratory and at-sea tests are presented and discussed in order to highlight the functionality and the performance of a prototype of the wireless density meter node in a Bluetooth radio network. The experimental results show a good agreement of the values of the calculated density compared to reference hydrometer readings. PMID:22736986

Analysis of laser shock experiments on precompressed samples using a quartz reference and application to warm dense hydrogen and helium

DOE PAGES

Brygoo, Stephanie; Millot, Marius; Loubeyre, Paul; ...

2015-11-16

Megabar (1 Mbar = 100 GPa) laser shocks on precompressed samples allow reaching unprecedented high densities and moderately high ~10 3–10 4 K temperatures. We describe in this paper a complete analysis framework for the velocimetry (VISAR) and pyrometry (SOP) data produced in these experiments. Since the precompression increases the initial density of both the sample of interest and the quartz reference for pressure-density, reflectivity, and temperature measurements, we describe analytical corrections based on available experimental data on warm dense silica and density-functional-theory based molecular dynamics computer simulations. Finally, using our improved analysis framework, we report a re-analysis of previouslymore » published data on warm dense hydrogen and helium, compare the newly inferred pressure, density, and temperature data with most advanced equation of state models and provide updated reflectivity values.« less

Brief communication: Hair density and body mass in mammals and the evolution of human hairlessness.

PubMed

Sandel, Aaron A

2013-09-01

Humans are unusual among mammals in appearing hairless. Several hypotheses propose explanations for this phenotype, but few data are available to test these hypotheses. To elucidate the evolutionary history of human "hairlessness," a comparative approach is needed. One previous study on primate hair density concluded that great apes have systematically less dense hair than smaller primates. While there is a negative correlation between body size and hair density, it remains unclear whether great apes have less dense hair than is expected for their body size. To revisit the scaling relationship between hair density and body size in mammals, I compiled data from the literature on 23 primates and 29 nonprimate mammals and conducted Phylogenetic Generalized Least Squares regressions. Among anthropoids, there is a significant negative correlation between hair density and body mass. Chimpanzees display the largest residuals, exhibiting less dense hair than is expected for their body size. There is a negative correlation between hair density and body mass among the broader mammalian sample, although the functional significance of this scaling relationship remains to be tested. Results indicate that all primates, and chimpanzees in particular, are relatively hairless compared to other mammals. This suggests that there may have been selective pressures acting on the ancestor of humans and chimpanzees that led to an initial reduction in hair density. To further understand the evolution of human hairlessness, a systematic study of hair density and physiology in a wide range of species is necessary. Copyright © 2013 Wiley Periodicals, Inc.

Graphene-induced band gap renormalization in polythiophene: a many-body perturbation study

NASA Astrophysics Data System (ADS)

Marsusi, F.; Fedorov, I. A.; Gerivani, S.

2018-01-01

Density functional theory and many-body perturbation theory at the G0W0 level are employed to study the electronic properties of polythiophene (PT) adsorbed on the graphene surface. Analysis of the charge density difference shows that substrate-adsorbate interaction leads to a strong physisorption and interfacial electric dipole moment formation. The electrostatic potential displays a  -0.19 eV shift in the graphene work function from its initial value of 4.53 eV, as the result of the interaction. The LDA band gap of the polymer does not show any change. However, the band structure exhibits weak orbital hybridizations resulting from slight overlapping between the polymer and graphene states wave functions. The interfacial polarization effects on the band gap and levels alignment are investigated at the G0W0 level and show a notable reduction of PT band gap compared to that of the isolated chain.

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

Van Vleet, Mary J.; Misquitta, Alston J.; Stone, Anthony J.

Short-range repulsion within inter-molecular force fields is conventionally described by either Lennard-Jones or Born-Mayer forms. Despite their widespread use, these simple functional forms are often unable to describe the interaction energy accurately over a broad range of inter-molecular distances, thus creating challenges in the development of ab initio force fields and potentially leading to decreased accuracy and transferability. Herein, we derive a novel short-range functional form based on a simple Slater-like model of overlapping atomic densities and an iterated stockholder atom (ISA) partitioning of the molecular electron density. We demonstrate that this Slater-ISA methodology yields a more accurate, transferable, andmore » robust description of the short-range interactions at minimal additional computational cost compared to standard Lennard-Jones or Born-Mayer approaches. Lastly, we show how this methodology can be adapted to yield the standard Born-Mayer functional form while still retaining many of the advantages of the Slater-ISA approach.« less

Using time-dependent density functional theory in real time for calculating electronic transport

NASA Astrophysics Data System (ADS)

Schaffhauser, Philipp; Kümmel, Stephan

2016-01-01

We present a scheme for calculating electronic transport within the propagation approach to time-dependent density functional theory. Our scheme is based on solving the time-dependent Kohn-Sham equations on grids in real space and real time for a finite system. We use absorbing and antiabsorbing boundaries for simulating the coupling to a source and a drain. The boundaries are designed to minimize the effects of quantum-mechanical reflections and electrical polarization build-up, which are the major obstacles when calculating transport by applying an external bias to a finite system. We show that the scheme can readily be applied to real molecules by calculating the current through a conjugated molecule as a function of time. By comparing to literature results for the conjugated molecule and to analytic results for a one-dimensional model system we demonstrate the reliability of the concept.

Continuous description of fluctuating eccentricities

NASA Astrophysics Data System (ADS)

Blaizot, Jean-Paul; Broniowski, Wojciech; Ollitrault, Jean-Yves

2014-11-01

We consider the initial energy density in the transverse plane of a high energy nucleus-nucleus collision as a random field ρ (x), whose probability distribution P [ ρ ], the only ingredient of the present description, encodes all possible sources of fluctuations. We argue that it is a local Gaussian, with a short-range 2-point function, and that the fluctuations relevant for the calculation of the eccentricities that drive the anisotropic flow have small relative amplitudes. In fact, this 2-point function, together with the average density, contains all the information needed to calculate the eccentricities and their variances, and we derive general model independent expressions for these quantities. The short wavelength fluctuations are shown to play no role in these calculations, except for a renormalization of the short range part of the 2-point function. As an illustration, we compare to a commonly used model of independent sources, and recover the known results of this model.

Bond breaking and bond formation: how electron correlation is captured in many-body perturbation theory and density-functional theory.

PubMed

Caruso, Fabio; Rohr, Daniel R; Hellgren, Maria; Ren, Xinguo; Rinke, Patrick; Rubio, Angel; Scheffler, Matthias

2013-04-05

For the paradigmatic case of H(2) dissociation, we compare state-of-the-art many-body perturbation theory in the GW approximation and density-functional theory in the exact-exchange plus random-phase approximation (RPA) for the correlation energy. For an unbiased comparison and to prevent spurious starting point effects, both approaches are iterated to full self-consistency (i.e., sc-RPA and sc-GW). The exchange-correlation diagrams in both approaches are topologically identical, but in sc-RPA they are evaluated with noninteracting and in sc-GW with interacting Green functions. This has a profound consequence for the dissociation region, where sc-RPA is superior to sc-GW. We argue that for a given diagrammatic expansion, sc-RPA outperforms sc-GW when it comes to bond breaking. We attribute this to the difference in the correlation energy rather than the treatment of the kinetic energy.

Ab initio studies of hydrogen adatoms on bilayer graphene

NASA Astrophysics Data System (ADS)

Mapasha, R. E.; Ukpong, A. M.; Chetty, N.

2012-05-01

We present a comparative density functional study of the adsorption of hydrogen on bilayer graphene. Six different exchange-correlation functionals are employed to explore the possible configurations of hydrogen adsorption at 50% coverage. Using the four variants of the nonlocal van der Waals density functional, we identify three distinct competing configurations that retain the coupled bilayer structure at 0 K. One of the configurations undergoes a spontaneous transformation from hexagonal to tetrahedral structure, under hydrogenation, with heat of formation ranging between -0.03 eV (vdW-DF) and -0.37 eV (vdW-DFC09x). This configuration has a finite band gap of around 3 eV, whereas all other competing configurations are either semimetallic or metallic. We also find two unique low-energy competing configurations of decoupled bilayer graphene, and therefore suggest the possibility of graphene exfoliation by hydrogen intercalation.

The ordering of symmetric diblock copolymers: A comparison of self-consistent-field and density functional approaches

NASA Astrophysics Data System (ADS)

Nath, Shyamal K.; McCoy, John D.; Curro, John G.; Saunders, Randall S.

1997-02-01

Polymer reference interaction site model (PRISM) based density functional (DF) theory is used to evaluate the structure and thermodynamics of structurally symmetric, freely jointed, diblock chains with 0.50 volume fraction. These results are compared to the results of self-consistent-field (SCF) theory. Agreement between the predictions of the SCF and DF theories is found for the lamella spacing well above the order-disorder transition (ODT) and for the qualitative behavior of the interfacial thickness as a function of both chain length and Flory-Huggins χ parameter. Disagreement is found for the magnitude of the interfacial thickness where DF theory indicates that the thickness is 1.7±0.2 times larger than that predicted by SCF theory. It appears that behavior on the monomer length scale is sensitive to system specific details which are neglected by SCF theory.

The influences of delay time on the stability of a market model with stochastic volatility

NASA Astrophysics Data System (ADS)

Li, Jiang-Cheng; Mei, Dong-Cheng

2013-02-01

The effects of the delay time on the stability of a market model are investigated, by using a modified Heston model with a cubic nonlinearity and cross-correlated noise sources. These results indicate that: (i) There is an optimal delay time τo which maximally enhances the stability of the stock price under strong demand elasticity of stock price, and maximally reduces the stability of the stock price under weak demand elasticity of stock price; (ii) The cross correlation coefficient of noises and the delay time play an opposite role on the stability for the case of the delay time <τo and the same role for the case of the delay time >τo. Moreover, the probability density function of the escape time of stock price returns, the probability density function of the returns and the correlation function of the returns are compared with other literatures.

Energy decomposition analysis of single bonds within Kohn-Sham density functional theory.

PubMed

Levine, Daniel S; Head-Gordon, Martin

2017-11-28

An energy decomposition analysis (EDA) for single chemical bonds is presented within the framework of Kohn-Sham density functional theory based on spin projection equations that are exact within wave function theory. Chemical bond energies can then be understood in terms of stabilization caused by spin-coupling augmented by dispersion, polarization, and charge transfer in competition with destabilizing Pauli repulsions. The EDA reveals distinguishing features of chemical bonds ranging across nonpolar, polar, ionic, and charge-shift bonds. The effect of electron correlation is assessed by comparison with Hartree-Fock results. Substituent effects are illustrated by comparing the C-C bond in ethane against that in bis(diamantane), and dispersion stabilization in the latter is quantified. Finally, three metal-metal bonds in experimentally characterized compounds are examined: a [Formula: see text]-[Formula: see text] dimer, the [Formula: see text]-[Formula: see text] bond in dizincocene, and the Mn-Mn bond in dimanganese decacarbonyl.

Analysis of density effects in plasmas and their influence on electron-impact cross sections

NASA Astrophysics Data System (ADS)

Belkhiri, M.; Poirier, M.

2014-12-01

Density effects in plasmas are analyzed using a Thomas-Fermi approach for free electrons. First, scaling properties are determined for the free-electron potential and density. For hydrogen-like ions, the first two terms of an analytical expansion of this potential as a function of the plasma coupling parameter are obtained. In such ions, from these properties and numerical calculations, a simple analytical fit is proposed for the plasma potential, which holds for any electron density, temperature, and atomic number, at least assuming that Maxwell-Boltzmann statistics is applicable. This allows one to analyze perturbatively the influence of the plasma potential on energies, wave functions, transition rates, and electron-impact collision rates for single-electron ions. Second, plasmas with an arbitrary charge state are considered, using a modified version of the Flexible Atomic Code (FAC) package with a plasma potential based on a Thomas-Fermi approach. Various methods for the collision cross-section calculations are reviewed. The influence of plasma density on these cross sections is analyzed in detail. Moreover, it is demonstrated that, in a given transition, the radiative and collisional-excitation rates are differently affected by the plasma density. Some analytical expressions are proposed for hydrogen-like ions in the limit where the Born or Lotz approximation applies and are compared to the numerical results from the FAC.

Enhancing Post-Expansion Chondrogenic Potential of Costochondral Cells in Self-Assembled Neocartilage

PubMed Central

Murphy, Meghan K.; Huey, Daniel J.; Reimer, Andrew J.; Hu, Jerry C.; Athanasiou, Kyriacos A.

2013-01-01

The insufficient healing capacity of articular cartilage necessitates mechanically functional biologic tissue replacements. Using cells to form biomimetic cartilage implants is met with the challenges of cell scarcity and donor site morbidity, requiring expanded cells that possess the ability to generate robust neocartilage. To address this, this study assesses the effects of expansion medium supplementation (bFGF, TFP, FBS) and self-assembled construct seeding density (2, 3, 4 million cells/5 mm dia. construct) on the ability of costochondral cells to generate biochemically and biomechanically robust neocartilage. Results show TFP (1 ng/mL TGF-β1, 5 ng/mL bFGF, 10 ng/mL PDGF) supplementation of serum-free chondrogenic expansion medium enhances the post-expansion chondrogenic potential of costochondral cells, evidenced by increased glycosaminoglycan content, decreased type I/II collagen ratio, and enhanced compressive properties. Low density (2 million cells/construct) enhances matrix synthesis and tensile and compressive mechanical properties. Combined, TFP and Low density interact to further enhance construct properties. That is, with TFP, Low density increases type II collagen content by over 100%, tensile stiffness by over 300%, and compressive moduli by over 140%, compared with High density. In conclusion, the interaction of TFP and Low density seeding enhances construct material properties, allowing for a mechanically functional, biomimetic cartilage to be formed using clinically relevant costochondral cells. PMID:23437288

Accurate first-principles structures and energies of diversely bonded systems from an efficient density functional

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

Sun, Jianwei; Remsing, Richard C.; Zhang, Yubo

2016-06-13

One atom or molecule binds to another through various types of bond, the strengths of which range from several meV to several eV. Although some computational methods can provide accurate descriptions of all bond types, those methods are not efficient enough for many studies (for example, large systems, ab initio molecular dynamics and high-throughput searches for functional materials). Here, we show that the recently developed non-empirical strongly constrained and appropriately normed (SCAN) meta-generalized gradient approximation (meta-GGA) within the density functional theory framework predicts accurate geometries and energies of diversely bonded molecules and materials (including covalent, metallic, ionic, hydrogen and vanmore » der Waals bonds). This represents a significant improvement at comparable efficiency over its predecessors, the GGAs that currently dominate materials computation. Often, SCAN matches or improves on the accuracy of a computationally expensive hybrid functional, at almost-GGA cost. SCAN is therefore expected to have a broad impact on chemistry and materials science.« less

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

Gledhill, Jonathan D.; Tozer, David J., E-mail: d.j.tozer@durham.ac.uk

Density scaling considerations are used to derive an exchange–correlation explicit density functional that is appropriate for the electron deficient side of the integer and which recovers the exact r → ∞ asymptotic behaviour of the exchange–correlation potential. The functional has an unconventional mathematical form with parameters that are system-dependent; the parameters for an N-electron system are determined in advance from generalised gradient approximation (GGA) calculations on the N- and (N − 1)-electron systems. Compared to GGA results, the functional yields similar exchange–correlation energies, but HOMO energies that are an order of magnitude closer to the negative of the vertical ionisationmore » potential; for anions, the HOMO energies are negative, as required. Rydberg excitation energies are also notably improved and the exchange–correlation potential is visibly lowered towards the near-exact potential. Further development is required to improve valence excitations, static isotropic polarisabilities, and the shape of the potential in non-asymptotic regions. The functional is fundamentally different to conventional approximations.« less

Noncovalent Interactions of DNA Bases with Naphthalene and Graphene.

PubMed

Cho, Yeonchoo; Min, Seung Kyu; Yun, Jeonghun; Kim, Woo Youn; Tkatchenko, Alexandre; Kim, Kwang S

2013-04-09

The complexes of a DNA base bound to graphitic systems are studied. Considering naphthalene as the simplest graphitic system, DNA base-naphthalene complexes are scrutinized at high levels of ab initio theory including coupled cluster theory with singles, doubles, and perturbative triples excitations [CCSD(T)] at the complete basis set (CBS) limit. The stacked configurations are the most stable, where the CCSD(T)/CBS binding energies of guanine, adenine, thymine, and cytosine are 9.31, 8.48, 8.53, 7.30 kcal/mol, respectively. The energy components are investigated using symmetry-adapted perturbation theory based on density functional theory including the dispersion energy. We compared the CCSD(T)/CBS results with several density functional methods applicable to periodic systems. Considering accuracy and availability, the optB86b nonlocal functional and the Tkatchenko-Scheffler functional are used to study the binding energies of nucleobases on graphene. The predicted values are 18-24 kcal/mol, though many-body effects on screening and energy need to be further considered.

First-principles calculations on the four phases of BaTiO3.

PubMed

Evarestov, Robert A; Bandura, Andrei V

2012-04-30

The calculations based on linear combination of atomic orbitals basis functions as implemented in CRYSTAL09 computer code have been performed for cubic, tetragonal, orthorhombic, and rhombohedral modifications of BaTiO(3) crystal. Structural and electronic properties as well as phonon frequencies were obtained using local density approximation, generalized gradient approximation, and hybrid exchange-correlation density functional theory (DFT) functionals for four stable phases of BaTiO(3). A comparison was made between the results of different DFT techniques. It is concluded that the hybrid PBE0 [J. P. Perdew, K. Burke, M. Ernzerhof, J. Chem. Phys. 1996, 105, 9982.] functional is able to predict correctly the structural stability and phonon properties both for cubic and ferroelectric phases of BaTiO(3). The comparative phonon symmetry analysis in BaTiO(3) four phases has been made basing on the site symmetry and irreducible representation indexes for the first time. Copyright © 2012 Wiley Periodicals, Inc.

Accurate first-principles structures and energies of diversely bonded systems from an efficient density functional.

PubMed

Sun, Jianwei; Remsing, Richard C; Zhang, Yubo; Sun, Zhaoru; Ruzsinszky, Adrienn; Peng, Haowei; Yang, Zenghui; Paul, Arpita; Waghmare, Umesh; Wu, Xifan; Klein, Michael L; Perdew, John P

2016-09-01

One atom or molecule binds to another through various types of bond, the strengths of which range from several meV to several eV. Although some computational methods can provide accurate descriptions of all bond types, those methods are not efficient enough for many studies (for example, large systems, ab initio molecular dynamics and high-throughput searches for functional materials). Here, we show that the recently developed non-empirical strongly constrained and appropriately normed (SCAN) meta-generalized gradient approximation (meta-GGA) within the density functional theory framework predicts accurate geometries and energies of diversely bonded molecules and materials (including covalent, metallic, ionic, hydrogen and van der Waals bonds). This represents a significant improvement at comparable efficiency over its predecessors, the GGAs that currently dominate materials computation. Often, SCAN matches or improves on the accuracy of a computationally expensive hybrid functional, at almost-GGA cost. SCAN is therefore expected to have a broad impact on chemistry and materials science.

New Evidence for a Large Local Void From the UKIDSS LAS + SDSS

NASA Astrophysics Data System (ADS)

Keenan, Ryan; Barger, A. J.

2013-01-01

Recent cosmological modeling efforts have shown that a local under-density on scales of a few hundred Mpc (out to z ~ 0.1) could produce the apparent acceleration of the expansion of the universe observed via type Ia supernovae. Several studies of galaxy counts in the near-infrared (NIR) have found that the local universe appears underdense by ~25 - 50% compared with regions a few hundred Mpc distant (e.g. Keenan et al., 2010). An accurate characterization of any such under-density will be important for studies seeking to understand the nature of dark energy. If the space density of galaxies is rising as a function of redshift, then the luminosity density, as measured via the NIR galaxy luminosity function (LF), should be rising as well. In Keenan et al. (2012), we presented a study of the NIR LF at z ~ 0.2 and found that the product φ*L* (the peak of the luminosity density distribution) at z ~ 0.2 is roughly ~ 30% higher than that measured at z ~ 0.05. Here we present the results from a study of the NIR LF derived from galaxies selected from the UKIRT Infrared Deep Sky Large Area Survey (UKIDSS LAS) combined with spectroscopy from the Sloan Digital Sky Survey (SDSS). We confirm the apparent rise in luminosity density found in Keenan et al. (2012) from z = 0.05 to z = 0.1 and provide the first self-consistent measurements of the NIR luminosity density out to z ~ 0.15.

A computational study on the electronic and field emission properties of Mg and Si doped AlN nanocones

NASA Astrophysics Data System (ADS)

Saedi, Leila; Soleymanabadi, Hamed; Panahyab, Ataollah

2018-05-01

Following an experimental work, we explored the effect of replacing an Al atom of an AlN nanocone by Si or Mg atom on its electronic and field emission properties using density functional theory calculations. We found that both Si-doping and Mg-doping increase the electrical conductivity of AlN nanocone, but their influences on the filed emission properties are significantly different. The Si-doping increases the electron concentration of AlN nanocone and results in a large electron mobility and a low work function, whereas Mg-doping leads to a high hole concentration below the conduction level and increases the work function in agreement with the experimental results. It is predicted that Si-doped AlN nanocones show excellent filed emission performance with higher emitted electron current density compared to the pristine AlN nanocone. But the Mg-doping meaningfully decreases the emitted electron current density from the surface of AlN nanocone. The Mg-doping can increase the work function about 41.9% and the Si-doping can decrease it about 6.3%. The Mg-doping and Si-doping convert the AlN nanocone to a p-type and n-type semiconductors, respectively. Our results explain in a molecular level what observed in the experiment.

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

Castaño-González, E.-E.; Seña, N.; Mendoza-Estrada, V.

In this paper, we carried out first-principles calculations in order to investigate the structural and electronic properties of the binary compound gallium antimonide (GaSb). This theoretical study was carried out using the Density Functional Theory within the plane-wave pseudopotential method. The effects of exchange and correlation (XC) were treated using the functional Local Density Approximation (LDA), generalized gradient approximation (GGA): Perdew–Burke–Ernzerhof (PBE), Perdew-Burke-Ernzerhof revised for solids (PBEsol), Perdew-Wang91 (PW91), revised Perdew–Burke–Ernzerhof (rPBE), Armiento–Mattson 2005 (AM05) and meta-generalized gradient approximation (meta-GGA): Tao–Perdew–Staroverov–Scuseria (TPSS) and revised Tao–Perdew–Staroverov–Scuseria (RTPSS) and modified Becke-Johnson (MBJ). We calculated the densities of state (DOS) and band structuremore » with different XC potentials identified and compared them with the theoretical and experimental results reported in the literature. It was discovered that functional: LDA, PBEsol, AM05 and RTPSS provide the best results to calculate the lattice parameters (a) and bulk modulus (B{sub 0}); while for the cohesive energy (E{sub coh}), functional: AM05, RTPSS and PW91 are closer to the values obtained experimentally. The MBJ, Rtpss and AM05 values found for the band gap energy is slightly underestimated with those values reported experimentally.« less

Accurate critical pressures for structural phase transitions of group IV, III-V, and II-VI compounds from the SCAN density functional

NASA Astrophysics Data System (ADS)

Shahi, Chandra; Sun, Jianwei; Perdew, John P.

2018-03-01

Most of the group IV, III-V, and II-VI compounds crystallize in semiconductor structures under ambient conditions. Upon application of pressure, they undergo structural phase transitions to more closely packed structures, sometimes metallic phases. We have performed density functional calculations using projector augmented wave (PAW) pseudopotentials to determine the transition pressures for these transitions within the local density approximation (LDA), the Perdew-Burke-Ernzerhof (PBE) generalized gradient approximation (GGA), and the strongly constrained and appropriately normed (SCAN) meta-GGA. LDA underestimates the transition pressure for most of the studied materials. PBE under- or overestimates in many cases. SCAN typically corrects the errors of LDA and PBE for the transition pressure. The accuracy of SCAN is comparable to that of computationally expensive methods like the hybrid functional HSE06, the random phase approximation (RPA), and quantum Monte Carlo (QMC), in cases where calculations with these methods have been reported, but at a more modest computational cost. The improvement from LDA to PBE to SCAN is especially clearcut and dramatic for covalent semiconductor-metal transitions, as for Si and Ge, where it reflects the increasing relative stabilization of the covalent semiconducting phases under increasing functional sophistication.

On Galactic Density Modeling in the Presence of Dust Extinction

NASA Astrophysics Data System (ADS)

Bovy, Jo; Rix, Hans-Walter; Green, Gregory M.; Schlafly, Edward F.; Finkbeiner, Douglas P.

2016-02-01

Inferences about the spatial density or phase-space structure of stellar populations in the Milky Way require a precise determination of the effective survey volume. The volume observed by surveys such as Gaia or near-infrared spectroscopic surveys, which have good coverage of the Galactic midplane region, is highly complex because of the abundant small-scale structure in the three-dimensional interstellar dust extinction. We introduce a novel framework for analyzing the importance of small-scale structure in the extinction. This formalism demonstrates that the spatially complex effect of extinction on the selection function of a pencil-beam or contiguous sky survey is equivalent to a low-pass filtering of the extinction-affected selection function with the smooth density field. We find that the angular resolution of current 3D extinction maps is sufficient for analyzing Gaia sub-samples of millions of stars. However, the current distance resolution is inadequate and needs to be improved by an order of magnitude, especially in the inner Galaxy. We also present a practical and efficient method for properly taking the effect of extinction into account in analyses of Galactic structure through an effective selection function. We illustrate its use with the selection function of red-clump stars in APOGEE using and comparing a variety of current 3D extinction maps.

Effect of Hartree-Fock exact exchange on intramolecular magnetic coupling constants of organic diradicals

NASA Astrophysics Data System (ADS)

Cho, Daeheum; Ko, Kyoung Chul; Ikabata, Yasuhiro; Wakayama, Kazufumi; Yoshikawa, Takeshi; Nakai, Hiromi; Lee, Jin Yong

2015-01-01

The intramolecular magnetic coupling constant (J) of diradical systems linked with five- or six-membered aromatic rings was calculated to obtain the scaling factor (experimental J/calculated J ratio) for various density functional theory (DFT) functionals. Scaling factors of group A (PBE, TPSSh, B3LYP, B97-1, X3LYP, PBE0, and BH&HLYP) and B (M06-L, M06, M06-2X, and M06-HF) were shown to decrease as the amount of Hartree-Fock exact exchange (HFx) increases, in other words, overestimation of calculated J becomes more severe as the HFx increases. We further investigated the effect of HFx fraction of DFT functional on J value, spin contamination, and spin density distributions by comparing the B3LYP analogues containing different amount of HFx. It was revealed that spin contamination and spin densities at each atom increases as the HFx increases. Above all, newly developed BLYP-5 functional, which has 5% of HFx, was found to have the scaling factor of 1.029, indicating that calculated J values are very close to that of experimental values without scaling. BLYP-5 has potential to be utilized for accurate evaluation of intramolecular magnetic coupling constant (J) of diradicals linked by five- or six-membered aromatic ring couplers.

Effect of Hartree-Fock exact exchange on intramolecular magnetic coupling constants of organic diradicals.

PubMed

Cho, Daeheum; Ko, Kyoung Chul; Ikabata, Yasuhiro; Wakayama, Kazufumi; Yoshikawa, Takeshi; Nakai, Hiromi; Lee, Jin Yong

2015-01-14

The intramolecular magnetic coupling constant (J) of diradical systems linked with five- or six-membered aromatic rings was calculated to obtain the scaling factor (experimental J/calculated J ratio) for various density functional theory (DFT) functionals. Scaling factors of group A (PBE, TPSSh, B3LYP, B97-1, X3LYP, PBE0, and BH&HLYP) and B (M06-L, M06, M06-2X, and M06-HF) were shown to decrease as the amount of Hartree-Fock exact exchange (HFx) increases, in other words, overestimation of calculated J becomes more severe as the HFx increases. We further investigated the effect of HFx fraction of DFT functional on J value, spin contamination, and spin density distributions by comparing the B3LYP analogues containing different amount of HFx. It was revealed that spin contamination and spin densities at each atom increases as the HFx increases. Above all, newly developed BLYP-5 functional, which has 5% of HFx, was found to have the scaling factor of 1.029, indicating that calculated J values are very close to that of experimental values without scaling. BLYP-5 has potential to be utilized for accurate evaluation of intramolecular magnetic coupling constant (J) of diradicals linked by five- or six-membered aromatic ring couplers.

New Kohn-Sham density functional based on microscopic nuclear and neutron matter equations of state

NASA Astrophysics Data System (ADS)

Baldo, M.; Robledo, L. M.; Schuck, P.; Viñas, X.

2013-06-01

A new version of the Barcelona-Catania-Paris energy functional is applied to a study of nuclear masses and other properties. The functional is largely based on calculated ab initio nuclear and neutron matter equations of state. Compared to typical Skyrme functionals having 10-12 parameters apart from spin-orbit and pairing terms, the new functional has only 2 or 3 adjusted parameters, fine tuning the nuclear matter binding energy and fixing the surface energy of finite nuclei. An energy rms value of 1.58 MeV is obtained from a fit of these three parameters to the 579 measured masses reported in the Audi and Wapstra [Nucl. Phys. ANUPABL0375-947410.1016/j.nuclphysa.2003.11.003 729, 337 (2003)] compilation. This rms value compares favorably with the one obtained using other successful mean field theories, which range from 1.5 to 3.0 MeV for optimized Skyrme functionals and 0.7 to 3.0 for the Gogny functionals. The other properties that have been calculated and compared to experiment are nuclear radii, the giant monopole resonance, and spontaneous fission lifetimes.

Evaluation of microvascular endothelial function and capillary density in patients with infective endocarditis using laser speckle contrast imaging and video-capillaroscopy.

PubMed

Barcelos, Amanda; Tibirica, Eduardo; Lamas, Cristiane

2018-07-01

To evaluate the systemic microcirculation of patients with infective endocarditis (IE). This is a comparative study of patients with definite IE by the modified Duke criteria admitted to our center for treatment. A reference group of sex- and age-matched healthy volunteers was included. Microvascular flow was evaluated in the forearm using a laser speckle contrast imaging system, for noninvasive measurement of cutaneous microvascular perfusion, in combination with skin iontophoresis of acetylcholine (ACh) and sodium nitroprusside (SNP) to test microvascular reactivity. Microvascular density was evaluated using skin video-capillaroscopy. We studied 22 patients with IE; 15 were male and seven female. The mean age and standard deviation (SD) were 45.5 ± 17.3 years. Basal skin microvascular conductance was significantly increased in patients with IE, compared with healthy individuals (0.36 ± 0.13 versus 0.21 ± 0.08 APU/mmHg; P < 0.0001). The increase in microvascular conductance induced by ACh in patients was 0.21 ± 0.17 and in the reference group, it was 0.37 ± 0.14 APU/mmHg (P = 0.0012). The increase in microvascular conductance induced by SNP in patients was 0.18 ± 0.14 and it was 0.29 ± 0.15 APU/mmHg (P = 0.0140) in the reference group. The basal mean skin capillary density of patients (135 ± 24 capillaries/mm 2 ) was significantly higher, compared with controls (97 ± 21 capillaries/mm 2 ; P < 0.0001). The main findings in the microcirculation of patients with IE were greater basal vasodilation and a reduction of the endothelium-dependent and -independent microvascular reactivity, as well as greater functional skin capillary density compared to healthy individuals. Copyright © 2018 Elsevier Inc. All rights reserved.

Inoculum size-dependent interactive regulation of metabolism and stress response of Saccharomyces cerevisiae revealed by comparative metabolomics.

PubMed

Ding, Ming-Zhu; Tian, Hong-Chi; Cheng, Jing-Sheng; Yuan, Ying-Jin

2009-12-01

To investigate the metabolic regulation against inoculum density and stress response to high cell density, comparative metabolomic analysis was employed on Saccharomyces cerevisiae under fermentations with five different inoculum sizes by gas chromatography time-of-flight mass spectrometry. Samples from these fermentations were clearly distinguished by principal components analysis, indicating that inoculum size had a profound effect on the metabolism of S. cerevisiae. Potential biomarkers responsible for the discrimination were identified as glycerol, phosphoric acid, succinate, glycine, isoleucine, proline, palmitoleic acid, myo-inositol and ethanolamine. It indicated that enhanced stress protectants in glycerol biosynthesis and amino acid metabolism, depressed citric acid cycle intermediates, as well as decreased metabolites relating to membrane structure and function were involved as the inoculum size of yeast increased. Furthermore, significantly higher levels of glycerol and proline in yeast cells of higher inoculum size fermentation (40 g l(-1)) revealed that they played important roles in protecting yeast from stresses in high cell density fermentation. These findings provided new insights into characterizing the metabolic regulation and stress response depending on inoculum density during ethanol fermentation.

Active Space Dependence in Multiconfiguration Pair-Density Functional Theory.

PubMed

Sharma, Prachi; Truhlar, Donald G; Gagliardi, Laura

2018-02-13

In multiconfiguration pair-density functional theory (MC-PDFT), multiconfiguration self-consistent-field calculations and on-top density functionals are combined to describe both static and dynamic correlation. Here, we investigate how the MC-PDFT total energy and its components depend on the active space choice in the case of the H 2 and N 2 molecules. The active space dependence of the on-top pair density, the total density, the ratio of on-top pair density to half the square of the electron density, and the satisfaction of the virial theorem are also explored. We find that the density and on-top pair density do not change significantly with changes in the active space. However, the on-top ratio does change significantly with respect to active space change, and this affects the on-top energy. This study provides a foundation for designing on-top density functionals and automatizing the active space choice in MC-PDFT.