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.

Spacecraft observations of a Maxwell Demon coating the separatrix of asymmetric magnetic reconnection with crescent-shaped electron distributions

NASA Astrophysics Data System (ADS)

Egedal, J.; Le, A.; Daughton, W.; Wetherton, B.; Cassak, Pa; Chen, Lj; Lavraud, B.; Dorell, J.; Avanov, L.; Gershman, D.

2016-10-01

During asymmetric magnetic reconnection in the dayside magnetopause in situ spacecraft mea- surements show that electrons from the high density inflow penetrate some distance into the low density inflow. Supported by a kinetic simulation, we present a general derivation of an exclusion energy parameter, which provides a lower kinetic energy bound for an electron to jump across the reconnection region from one inflow region to the other. As by a Maxwell Demon, only high energy electrons are permitted to cross the inner reconnection region, strongly impacting the form of the electron distribution function observed along the low density side separatrix. The dynamics produce two distinct flavors of crescent-shaped electron distributions in a thin boundary layer along the separatrix between the magnetospheric inflow and the reconnection exhaust. The analytical model presented relates these salient details of the distribution function to the electron dynamics in the inner reconnection region.

Time-dependent density functional theory for open systems with a positivity-preserving decomposition scheme for environment spectral functions

NASA Astrophysics Data System (ADS)

Wang, RuLin; Zheng, Xiao; Kwok, YanHo; Xie, Hang; Chen, GuanHua; Yam, ChiYung

2015-04-01

Understanding electronic dynamics on material surfaces is fundamentally important for applications including nanoelectronics, inhomogeneous catalysis, and photovoltaics. Practical approaches based on time-dependent density functional theory for open systems have been developed to characterize the dissipative dynamics of electrons in bulk materials. The accuracy and reliability of such approaches depend critically on how the electronic structure and memory effects of surrounding material environment are accounted for. In this work, we develop a novel squared-Lorentzian decomposition scheme, which preserves the positive semi-definiteness of the environment spectral matrix. The resulting electronic dynamics is guaranteed to be both accurate and convergent even in the long-time limit. The long-time stability of electronic dynamics simulation is thus greatly improved within the current decomposition scheme. The validity and usefulness of our new approach are exemplified via two prototypical model systems: quasi-one-dimensional atomic chains and two-dimensional bilayer graphene.

How electronic dynamics with Pauli exclusion produces Fermi-Dirac statistics.

PubMed

Nguyen, Triet S; Nanguneri, Ravindra; Parkhill, John

2015-04-07

It is important that any dynamics method approaches the correct population distribution at long times. In this paper, we derive a one-body reduced density matrix dynamics for electrons in energetic contact with a bath. We obtain a remarkable equation of motion which shows that in order to reach equilibrium properly, rates of electron transitions depend on the density matrix. Even though the bath drives the electrons towards a Boltzmann distribution, hole blocking factors in our equation of motion cause the electronic populations to relax to a Fermi-Dirac distribution. These factors are an old concept, but we show how they can be derived with a combination of time-dependent perturbation theory and the extended normal ordering of Mukherjee and Kutzelnigg for a general electronic state. The resulting non-equilibrium kinetic equations generalize the usual Redfield theory to many-electron systems, while ensuring that the orbital occupations remain between zero and one. In numerical applications of our equations, we show that relaxation rates of molecules are not constant because of the blocking effect. Other applications to model atomic chains are also presented which highlight the importance of treating both dephasing and relaxation. Finally, we show how the bath localizes the electron density matrix.

Theory of time-resolved photoelectron imaging. Comparison of a density functional with a time-dependent density functional approach

NASA Astrophysics Data System (ADS)

Suzuki, Yoshi-ichi; Seideman, Tamar; Stener, Mauro

2004-01-01

Time-resolved photoelectron differential cross sections are computed within a quantum dynamical theory that combines a formally exact solution of the nuclear dynamics with density functional theory (DFT)-based approximations of the electronic dynamics. Various observables of time-resolved photoelectron imaging techniques are computed at the Kohn-Sham and at the time-dependent DFT levels. Comparison of the results serves to assess the reliability of the former method and hence its usefulness as an economic approach for time-domain photoelectron cross section calculations, that is applicable to complex polyatomic systems. Analysis of the matrix elements that contain the electronic dynamics provides insight into a previously unexplored aspect of femtosecond-resolved photoelectron imaging.

Dynamic correlations in the highly dilute 2D electron liquid: Loss function, critical wave vector and analytic plasmon dispersion

NASA Astrophysics Data System (ADS)

Drachta, Jürgen T.; Kreil, Dominik; Hobbiger, Raphael; Böhm, Helga M.

2018-03-01

Correlations, highly important in low-dimensional systems, are known to decrease the plasmon dispersion of two-dimensional electron liquids. Here we calculate the plasmon properties, applying the 'Dynamic Many-Body Theory', accounting for correlated two-particle-two-hole fluctuations. These dynamic correlations are found to significantly lower the plasmon's energy. For the data obtained numerically, we provide an analytic expression that is valid across a wide range both of densities and of wave vectors. Finally, we demonstrate how this can be invoked in determining the actual electron densities from measurements on an AlGaAs quantum well.

Dynamical simulation of electron transfer processes in self-assembled monolayers at metal surfaces using a density matrix approach.

PubMed

Prucker, V; Bockstedte, M; Thoss, M; Coto, P B

2018-03-28

A single-particle density matrix approach is introduced to simulate the dynamics of heterogeneous electron transfer (ET) processes at interfaces. The characterization of the systems is based on a model Hamiltonian parametrized by electronic structure calculations and a partitioning method. The method is applied to investigate ET in a series of nitrile-substituted (poly)(p-phenylene)thiolate self-assembled monolayers adsorbed at the Au(111) surface. The results show a significant dependence of the ET on the orbital symmetry of the donor state and on the molecular and electronic structure of the spacer.

Towards a formal definition of static and dynamic electronic correlations.

PubMed

Benavides-Riveros, Carlos L; Lathiotakis, Nektarios N; Marques, Miguel A L

2017-05-24

Some of the most spectacular failures of density-functional and Hartree-Fock theories are related to an incorrect description of the so-called static electron correlation. Motivated by recent progress in the N-representability problem of the one-body density matrix for pure states, we propose a method to quantify the static contribution to the electronic correlation. By studying several molecular systems we show that our proposal correlates well with our intuition of static and dynamic electron correlation. Our results bring out the paramount importance of the occupancy of the highest occupied natural spin-orbital in such quantification.

Dynamical and electronic properties of rare-earth aluminides

NASA Astrophysics Data System (ADS)

Sharma, Ramesh; Sharma, Yamini

2018-04-01

Rare-earth dialuminides belong to a large family of compounds that stabilize in cubic MgCu2 structure. A large number of these compounds are superconducting, amongst these YAl2, LaAl2 and LuAl2 have been chosen as reference materials for studying 4f-electron systems. In order to understand the role of the RE atoms, we have applied the FPLAPW and PAW methods within the density functional theory (DFT). Our results show that the contribution of RE atoms is dominant in both electronic structure and phonon dispersion. The anomalous behavior of superconducting LaAl2 is well explained from an analysis of the electron localization function (ELF), Bader charge analysis, density of electronic states as well as the dynamical phonon vibrational modes. The interaction of phonon modes contributed by low frequency vibrations of La atoms with the high density La 5d-states at EF in LaAl2 lead to strong electron-phonon coupling.

Stereocontrol of attosecond time-scale electron dynamics in ABCU using ultrafast laser pulses: a computational study.

PubMed

Mignolet, B; Gijsbertsen, A; Vrakking, M J J; Levine, R D; Remacle, F

2011-05-14

The attosecond time-scale electronic dynamics induced by an ultrashort laser pulse is computed using a multi configuration time dependent approach in ABCU (C(10)H(19)N), a medium size polyatomic molecule with a rigid cage geometry. The coupling between the electronic states induced by the strong pulse is included in the many electron Hamiltonian used to compute the electron dynamics. We show that it is possible to implement control of the electron density stereodynamics in this medium size molecule by varying the characteristics of the laser pulse, for example by polarizing the electric field either along the N-C axis of the cage, or in the plane perpendicular to it. The excitation produces an oscillatory, non-stationary, electronic state that exhibits localization of the electron density in different parts of the molecule both during and after the pulse. The coherent oscillations of the non-stationary electronic state are also demonstrated through the alternation of the dipole moment of the molecule.

Dynamics of electron injection and acceleration driven by laser wakefield in tailored density profiles

DOE PAGES

Lee, Patrick; Maynard, G.; Audet, T. L.; ...

2016-11-16

The dynamics of electron acceleration driven by laser wakefield is studied in detail using the particle-in-cell code WARP with the objective to generate high-quality electron bunches with narrow energy spread and small emittance, relevant for the electron injector of a multistage accelerator. Simulation results, using experimentally achievable parameters, show that electron bunches with an energy spread of ~11% can be obtained by using an ionization-induced injection mechanism in a mm-scale length plasma. By controlling the focusing of a moderate laser power and tailoring the longitudinal plasma density profile, the electron injection beginning and end positions can be adjusted, while themore » electron energy can be finely tuned in the last acceleration section.« less

Tuning of electronic properties and dynamical stability of graphene oxide with different functional groups

NASA Astrophysics Data System (ADS)

Dabhi, Shweta D.; Jha, Prafulla K.

2017-09-01

The structural, electronic and vibrational properties of graphene oxide (GO) with varying proportion of epoxy and hydroxyl functional groups have been studied using density functional theory. The functional groups and oxygen density have an obvious influence on the electronic and vibrational properties. The dependence of band gap on associated functional groups and oxygen density shows a possibility of tuning the band gap of graphene by varying the functional groups as well as oxidation level. The absorption of high oxygen content in graphene leads to the gap opening and resulting in a transition from semimetal to semiconductor. Phonon dispersion curves show no imaginary frequency or no softening of any phonon mode throughout the Brillouin zone which confirms the dynamical stability of all considered GO models. Different groups and different oxygen density result into the varying characteristics of phonon modes. The computed results show good agreement with the experimental observations. Our results present interesting possibilities for engineering the electronic properties of graphene and GO and impact the fabrication of new electronics.

Temporal-spatial measurement of electron relaxation time in femtosecond laser induced plasma using two-color pump-probe imaging technique

NASA Astrophysics Data System (ADS)

Pan, Changji; Jiang, Lan; Wang, Qingsong; Sun, Jingya; Wang, Guoyan; Lu, Yongfeng

2018-05-01

The femtosecond (fs) laser is a powerful tool to study ultrafast plasma dynamics, especially electron relaxation in strong ionization of dielectrics. Herein, temporal-spatial evolution of femtosecond laser induced plasma in fused silica was investigated using a two-color pump-probe technique (i.e., 400 nm and 800 nm, respectively). We demonstrated that when ionized electron density is lower than the critical density, free electron relaxation time is inversely proportional to electron density, which can be explained by the electron-ion scattering regime. In addition, electron density evolution within plasma was analyzed in an early stage (first 800 fs) of the laser-material interaction.

Carrier-density-dependent recombination dynamics of excitons and electron-hole plasma in m -plane InGaN/GaN quantum wells

NASA Astrophysics Data System (ADS)

Liu, W.; Butté, R.; Dussaigne, A.; Grandjean, N.; Deveaud, B.; Jacopin, G.

2016-11-01

We study the carrier-density-dependent recombination dynamics in m -plane InGaN/GaN multiple quantum wells in the presence of n -type background doping by time-resolved photoluminescence. Based on Fermi's golden rule and Saha's equation, we decompose the radiative recombination channel into an excitonic and an electron-hole pair contribution, and extract the injected carrier-density-dependent bimolecular recombination coefficients. Contrary to the standard electron-hole picture, our results confirm the strong influence of excitons even at room temperature. Indeed, at 300 K, excitons represent up to 63 ± 6% of the photoexcited carriers. In addition, following the Shockley-Read-Hall model, we extract the electron and hole capture rates by deep levels and demonstrate that the increase in the effective lifetime with injected carrier density is due to asymmetric capture rates in presence of an n -type background doping. Thanks to the proper determination of the density-dependent recombination coefficients up to high injection densities, our method provides a way to evaluate the importance of Auger recombination.

Structural, elastic, electronic and dynamical properties of OsB and ReB: Density functional calculations

NASA Astrophysics Data System (ADS)

Li, Yanling; Zeng, Zhi; Lin, Haiqing

2010-06-01

The structural, elastic, electronic and dynamical properties of ReB and OsB are investigated by first-principles calculations based on density functional theory. It turns out that ReB and OsB are metallic ultra-incompressible solids with small elastic anisotropy and high hardness. The change of c/ a ratio in OsB indicates that there is a structural phase transition at about 31 GPa. Phonon spectra calculations show that both OsB and ReB are stable dynamically and there are abnormal phonon dispersions along special directions in Brillouin zone. OsB and ReB do not show superconductivity due to very weak electron-phonon interactions in them.

On-top density functionals for the short-range dynamic correlation between electrons of opposite and parallel spin

NASA Astrophysics Data System (ADS)

Hollett, Joshua W.; Pegoretti, Nicholas

2018-04-01

Separate, one-parameter, on-top density functionals are derived for the short-range dynamic correlation between opposite and parallel-spin electrons, in which the electron-electron cusp is represented by an exponential function. The combination of both functionals is referred to as the Opposite-spin exponential-cusp and Fermi-hole correction (OF) functional. The two parameters of the OF functional are set by fitting the ionization energies and electron affinities, of the atoms He to Ar, predicted by ROHF in combination with the OF functional to the experimental values. For ionization energies, the overall performance of ROHF-OF is better than completely renormalized coupled-cluster [CR-CC(2,3)] and better than, or as good as, conventional density functional methods. For electron affinities, the overall performance of ROHF-OF is less impressive. However, for both ionization energies and electron affinities of third row atoms, the mean absolute error of ROHF-OF is only 3 kJ mol-1.

Theoretical investigation of the electron capture and loss processes in the collisions of He2+ + Ne.

PubMed

Hong, Xuhai; Wang, Feng; Jiao, Yalong; Su, Wenyong; Wang, Jianguo; Gou, Bingcong

2013-08-28

Based on the time-dependent density functional theory, a method is developed to study ion-atom collision dynamics, which self-consistently couples the quantum mechanical description of electron dynamics with the classical treatment of the ion motion. Employing real-time and real-space method, the coordinate space translation technique is introduced to allow one to focus on the region of target or projectile depending on the actual concerned process. The benchmark calculations are performed for the collisions of He(2+) + Ne, and the time evolution of electron density distribution is monitored, which provides interesting details of the interaction dynamics between the electrons and ion cores. The cross sections of single and many electron capture and loss have been calculated in the energy range of 1-1000 keV/amu, and the results show a good agreement with the available experiments over a wide range of impact energies.

Dynamics of photoionization from molecular electronic wavepacket states in intense pulse laser fields: A nonadiabatic electron wavepacket study.

PubMed

Matsuoka, Takahide; Takatsuka, Kazuo

2017-04-07

A theory for dynamics of molecular photoionization from nonadiabatic electron wavepackets driven by intense pulse lasers is proposed. Time evolution of photoelectron distribution is evaluated in terms of out-going electron flux (current of the probability density of electrons) that has kinetic energy high enough to recede from the molecular system. The relevant electron flux is in turn evaluated with the complex-valued electronic wavefunctions that are time evolved in nonadiabatic electron wavepacket dynamics in laser fields. To uniquely rebuild such wavefunctions with its electronic population being lost by ionization, we adopt the complex-valued natural orbitals emerging from the electron density as building blocks of the total wavefunction. The method has been implemented into a quantum chemistry code, which is based on configuration state mixing for polyatomic molecules. Some of the practical aspects needed for its application will be presented. As a first illustrative example, we show the results of hydrogen molecule and its isotope substitutes (HD and DD), which are photoionized by a two-cycle pulse laser. Photon emission spectrum associated with above threshold ionization is also shown. Another example is taken from photoionization dynamics from an excited state of a water molecule. Qualitatively significant effects of nonadiabatic interaction on the photoelectron spectrum are demonstrated.

Electron density and plasma dynamics of a colliding plasma experiment

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

Wiechula, J., E-mail: wiechula@physik.uni-frankfurt.de; Schönlein, A.; Iberler, M.

2016-07-15

We present experimental results of two head-on colliding plasma sheaths accelerated by pulsed-power-driven coaxial plasma accelerators. The measurements have been performed in a small vacuum chamber with a neutral-gas prefill of ArH{sub 2} at gas pressures between 17 Pa and 400 Pa and load voltages between 4 kV and 9 kV. As the plasma sheaths collide, the electron density is significantly increased. The electron density reaches maximum values of ≈8 ⋅ 10{sup 15} cm{sup −3} for a single accelerated plasma and a maximum value of ≈2.6 ⋅ 10{sup 16} cm{sup −3} for the plasma collision. Overall a raise of the plasma density by a factor ofmore » 1.3 to 3.8 has been achieved. A scaling behavior has been derived from the values of the electron density which shows a disproportionately high increase of the electron density of the collisional case for higher applied voltages in comparison to a single accelerated plasma. Sequences of the plasma collision have been taken, using a fast framing camera to study the plasma dynamics. These sequences indicate a maximum collision velocity of 34 km/s.« less

Structural, Electronic and Dynamical Properties of Curium Monopnictides: Density Functional Calculations

NASA Astrophysics Data System (ADS)

Roondhe, Basant; Upadhyay, Deepak; Som, Narayan; Pillai, Sharad B.; Shinde, Satyam; Jha, Prafulla K.

2017-03-01

The structural, electronic, dynamical and thermodynamical properties of CmX (X = N, P, As, Sb, and Bi) compounds are studied using first principles calculations within density functional theory. The Perdew-Burke-Ernzerhof spin polarized generalized gradient approximation and Perdew-Wang (PW) spin polarized local density approximation as the exchange correlational functionals are used in these calculations. There is a good agreement between the present and previously reported data. The calculated electronic density of states suggests that the curium monopnictides are metallic in nature, which is consistent with earlier studies. The significant values of magnetic moment suggest their magnetic nature. The phonon dispersion curves and phonon density of states are also calculated, which depict the dynamical stability of these compounds. There is a significant separation between the optical and acoustical phonon branches. The temperature dependence of the thermodynamical functions are also calculated and discussed. Internal energy and vibrational contribution to the Helmholtz free energy increases and decreases, respectively, with temperature. The entropy increases with temperature. The specific heat at constant volume and Debye temperature obey Debye theory. The temperature variation of the considered thermodynamical functions is in line with those of other crystalline solids.

The structural, electronic and dynamic properties of the L1{sub 2}- type Co{sub 3}Ti alloy

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

Arikan, Nihat; Özduran, Mustafa

2014-10-06

The structural, electronic and dynamic properties of the cubic Co{sub 3}Ti alloy in L1{sub 2} structure have been investigated using a pseudopotential plane wave (PP-PW) method within the generalized gradient approximation proposed by Perdew–Burke–Ernzerhof (GGA-PBE). The structural properties, including the lattice constant, the bulk modulus and its pressure derivative agree reasonably with the previous results. The density of state (DOS), projected density of state (PDOS) and electronic band structure are also reported. The DOS shows that Co{sub 3}Ti alloy has a metallic character since the energy bands cross the Fermi level. The density of states at Fermi level mainly comesmore » from the Co-3d states. Phonon dispersion curves and their corresponding total densities of states were obtained using a linear response in the framework of the density functional perturbation theory. All computed phonon frequencies are no imaginer and thus, Co{sub 3}Ti alloy is dynamically stable. The zone center phonon modes have been founded to be 9.307, 9.626 and 13.891 THz for Co{sub 3}Ti.« less

Combining Density Functional Theory and Green's Function Theory: Range-Separated, Nonlocal, Dynamic, and Orbital-Dependent Hybrid Functional.

PubMed

Kananenka, Alexei A; Zgid, Dominika

2017-11-14

We present a rigorous framework which combines single-particle Green's function theory with density functional theory based on a separation of electron-electron interactions into short- and long-range components. Short-range contribution to the total energy and exchange-correlation potential is provided by a density functional approximation, while the long-range contribution is calculated using an explicit many-body Green's function method. Such a hybrid results in a nonlocal, dynamic, and orbital-dependent exchange-correlation functional of a single-particle Green's function. In particular, we present a range-separated hybrid functional called srSVWN5-lrGF2 which combines the local-density approximation and the second-order Green's function theory. We illustrate that similarly to density functional approximations, the new functional is weakly basis-set dependent. Furthermore, it offers an improved description of the short-range dynamic correlation. The many-body contribution to the functional mitigates the many-electron self-interaction error present in many density functional approximations and provides a better description of molecular properties. Additionally, we illustrate that the new functional can be used to scale down the self-energy and, therefore, introduce an additional sparsity to the self-energy matrix that in the future can be exploited in calculations for large molecules or periodic systems.

Extreme ultraviolet probing of nonequilibrium dynamics in high energy density germanium

NASA Astrophysics Data System (ADS)

Principi, E.; Giangrisostomi, E.; Mincigrucci, R.; Beye, M.; Kurdi, G.; Cucini, R.; Gessini, A.; Bencivenga, F.; Masciovecchio, C.

2018-05-01

Intense femtosecond infrared laser pulses induce a nonequilibrium between thousands of Kelvin hot valence electrons and room-temperature ions in a germanium sample foil. The evolution of this exotic state of matter is monitored with time-resolved extreme ultraviolet absorption spectroscopy across the Ge M2 ,3 edge (≃30 eV ) using the FERMI free-electron laser. We analyze two distinct regimes in the ultrafast dynamics in laser-excited Ge: First, on a subpicosecond time scale, the electron energy distribution thermalizes to an extreme temperature unreachable in equilibrium solid germanium; then, during the following picoseconds, the lattice reacts strongly altering the electronic structure and resulting in melting to a metallic state alongside a breakdown of the local atomic order. Data analysis, based on a hybrid approach including both numerical and analytical calculations, provides an estimation of the electron and ion temperatures, the electron density of states, the carrier-phonon relaxation time, as well as the carrier density and lattice heat capacity under those extreme nonequilibrium conditions. Related structural anomalies, such as the occurrence of a transient low-density liquid phase and the possible drop in lattice heat capacity are discussed.

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

Strong influence of coadsorbate interaction on CO desorption dynamics on Ru(0001) probed by ultrafast x-ray spectroscopy and ab initio simulations

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

Xin, H.; LaRue, J.; Oberg, H.

2015-04-16

We show that coadsorbed oxygen atoms have a dramatic influence on the CO desorption dynamics from Ru(0001). In contrast to the precursor-mediated desorption mechanism on Ru(0001), the presence of surface oxygen modifies the electronic structure of Ru atoms such that CO desorption occurs predominantly via the direct pathway. This phenomenon is directly observed in an ultrafast pump-probe experiment using a soft x-ray free-electron laser to monitor the dynamic evolution of the valence electronic structure of the surface species. This is supported with the potential of mean force along the CO desorption path obtained from density-functional theory calculations. Charge density distributionmore » and frozen-orbital analysis suggest that the oxygen-induced reduction of the Pauli repulsion, and consequent increase of the dative interaction between the CO 5σ and the charged Ru atom, is the electronic origin of the distinct desorption dynamics. Ab initio molecular dynamics simulations of CO desorption from Ru(0001) and oxygen-coadsorbed Ru(0001) provide further insights into the surface bond-breaking process.« less

Exciton recombination dynamics in CdSe nanowires: bimolecular to three-carrier Auger kinetics.

PubMed

Robel, István; Bunker, Bruce A; Kamat, Prashant V; Kuno, Masaru

2006-07-01

Ultrafast relaxation dynamics of charge carriers in CdSe quantum wires with diameters between 6 and 8 nm are studied as a function of carrier density. At high electron-hole pair densities above 10(19) cm(-3) the dominant process for carrier cooling is the "bimolecular" Auger recombination of one-dimensional (1D) excitons. However, below this excitation level an unexpected transition from a bimolecular (exciton-exciton) to a three-carrier Auger relaxation mechanism occurs. Thus, depending on excitation intensity, electron-hole pair relaxation dynamics in the nanowires exhibit either 1D or 0D (quantum dot) character. This dual nature of the recovery kinetics defines an optimal intensity for achieving optical gain in solution-grown nanowires given the different carrier-density-dependent scaling of relaxation rates in either regime.

Unexpected storm-time nightside plasmaspheric density enhancement at low L shell

NASA Astrophysics Data System (ADS)

Chu, X.; Bortnik, J.; Denton, R. E.; Yue, C.

2017-12-01

We have developed a three-dimensional dynamic electron density (DEN3D) model in the inner magnetosphere using a neural network approach. The DEN3D model can provide spatiotemporal distribution of the electron density at any location and time that spacecraft observations are not available. Given DEN3D's good performance in predicting the structure and dynamic evolution of the plasma density, the salient features of the DEN3D model can be used to gain further insight into the physics. For instance, the DEN3D models can be used to find unusual phenomena that are difficult to detect in observations or simulations. We report, for the first time, an unexpected plasmaspheric density increase at low L shell regions on the nightside during the main phase of a moderate storm during 12-16 October 2004, as opposed to the expected density decrease due to storm-time plasmaspheric erosion. The unexpected density increase is first discovered in the modeled electron density distribution using the DEN3D model, and then validated using in-situ density measurements obtained from the IMAGE satellite. The density increase was likely caused by increased earthward transverse field plasma transport due to enhanced nightside ExB drift, which coincided with enhanced solar wind electric field and substorm activity. This is consistent with the results of physics-based simulation SAMI3 model which show earthward enhanced plasma transport and electron density increase at low L shells during storm main phase.

Density-functional theory simulation of large quantum dots

NASA Astrophysics Data System (ADS)

Jiang, Hong; Baranger, Harold U.; Yang, Weitao

2003-10-01

Kohn-Sham spin-density functional theory provides an efficient and accurate model to study electron-electron interaction effects in quantum dots, but its application to large systems is a challenge. Here an efficient method for the simulation of quantum dots using density-function theory is developed; it includes the particle-in-the-box representation of the Kohn-Sham orbitals, an efficient conjugate-gradient method to directly minimize the total energy, a Fourier convolution approach for the calculation of the Hartree potential, and a simplified multigrid technique to accelerate the convergence. We test the methodology in a two-dimensional model system and show that numerical studies of large quantum dots with several hundred electrons become computationally affordable. In the noninteracting limit, the classical dynamics of the system we study can be continuously varied from integrable to fully chaotic. The qualitative difference in the noninteracting classical dynamics has an effect on the quantum properties of the interacting system: integrable classical dynamics leads to higher-spin states and a broader distribution of spacing between Coulomb blockade peaks.

Theoretical investigation of the structural, electronic, dynamical and thermal properties of YSn3 and YPb3

NASA Astrophysics Data System (ADS)

Kılıçarslan, Aynur; Salmankurt, Bahadır; Duman, Sıtkı

2017-02-01

We have performed an ab initio study of the structural, electronic, dynamical and thermal properties of the cubic AuCu3-type YSn3 and YPb3 by using the density functional theory, plane-wave pseudopotential method and a linear response scheme, within the generalized gradient approximation. An analysis of the electronic density of states at the Fermi level is found to be governed by the p states of Sn and Pb atoms with some contributions from the d states of Y atoms. The obtained phonon figures indicate that these material are dynamically stable in the cubic structure. Due to the metallic behavior of the compounds, the calculated zone-center phonon modes are triply degenerate. Also the thermal properties have been examined.

Ab initio studies of ultrafast x-ray scattering of the photodissociation of iodine

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

Debnarova, Andrea; Techert, Simone; Schmatz, Stefan

2010-09-28

We computationally examine various aspects of the reaction dynamics of the photodissociation and recombination of molecular iodine. We use our recently proposed formalism to calculate time-dependent x-ray scattering signal changes from first principles. Different aspects of the dynamics of this prototypical reaction are studied, such as coherent and noncoherent processes, features of structural relaxation that are periodic in time versus nonperiodic dissociative processes, as well as small electron density changes caused by electronic excitation, all with respect to x-ray scattering. We can demonstrate that wide-angle x-ray scattering offers a possibility to study the changes in electron densities in nonperiodic systems,more » which render it a suitable technique for the investigation of chemical reactions from a structural dynamics point of view.« less

Time-Dependent Density Functional Theory for Open Systems and Its Applications.

PubMed

Chen, Shuguang; Kwok, YanHo; Chen, GuanHua

2018-02-20

Photovoltaic devices, electrochemical cells, catalysis processes, light emitting diodes, scanning tunneling microscopes, molecular electronics, and related devices have one thing in common: open quantum systems where energy and matter are not conserved. Traditionally quantum chemistry is confined to isolated and closed systems, while quantum dissipation theory studies open quantum systems. The key quantity in quantum dissipation theory is the reduced system density matrix. As the reduced system density matrix is an O(M! × M!) matrix, where M is the number of the particles of the system of interest, quantum dissipation theory can only be employed to simulate systems of a few particles or degrees of freedom. It is thus important to combine quantum chemistry and quantum dissipation theory so that realistic open quantum systems can be simulated from first-principles. We have developed a first-principles method to simulate the dynamics of open electronic systems, the time-dependent density functional theory for open systems (TDDFT-OS). Instead of the reduced system density matrix, the key quantity is the reduced single-electron density matrix, which is an N × N matrix where N is the number of the atomic bases of the system of interest. As the dimension of the key quantity is drastically reduced, the TDDFT-OS can thus be used to simulate the dynamics of realistic open electronic systems and efficient numerical algorithms have been developed. As an application, we apply the method to study how quantum interference develops in a molecular transistor in time domain. We include electron-phonon interaction in our simulation and show that quantum interference in the given system is robust against nuclear vibration not only in the steady state but also in the transient dynamics. As another application, by combining TDDFT-OS with Ehrenfest dynamics, we study current-induced dissociation of water molecules under scanning tunneling microscopy and follow its time dependent dynamics. Given the rapid development in ultrafast experiments with atomic resolution in recent years, time dependent simulation of open electronic systems will be useful to gain insight and understanding of such experiments. This Account will mainly focus on the practical aspects of the TDDFT-OS method, describing the numerical implementation and demonstrating the method with applications.

Real-time electron dynamics for massively parallel excited-state simulations

NASA Astrophysics Data System (ADS)

Andrade, Xavier

The simulation of the real-time dynamics of electrons, based on time dependent density functional theory (TDDFT), is a powerful approach to study electronic excited states in molecular and crystalline systems. What makes the method attractive is its flexibility to simulate different kinds of phenomena beyond the linear-response regime, including strongly-perturbed electronic systems and non-adiabatic electron-ion dynamics. Electron-dynamics simulations are also attractive from a computational point of view. They can run efficiently on massively parallel architectures due to the low communication requirements. Our implementations of electron dynamics, based on the codes Octopus (real-space) and Qball (plane-waves), allow us to simulate systems composed of thousands of atoms and to obtain good parallel scaling up to 1.6 million processor cores. Due to the versatility of real-time electron dynamics and its parallel performance, we expect it to become the method of choice to apply the capabilities of exascale supercomputers for the simulation of electronic excited states.

Analysis of microscopic parameters of surface charging in polymer caused by defocused electron beam irradiation.

PubMed

Liu, Jing; Zhang, Hai-Bo

2014-12-01

The relationship between microscopic parameters and polymer charging caused by defocused electron beam irradiation is investigated using a dynamic scattering-transport model. The dynamic charging process of an irradiated polymer using a defocused 30 keV electron beam is conducted. In this study, the space charge distribution with a 30 keV non-penetrating e-beam is negative and supported by some existing experimental data. The internal potential is negative, but relatively high near the surface, and it decreases to a maximum negative value at z=6 μm and finally tend to 0 at the bottom of film. The leakage current and the surface potential behave similarly, and the secondary electron and leakage currents follow the charging equilibrium condition. The surface potential decreases with increasing beam current density, trap concentration, capture cross section, film thickness and electron-hole recombination rate, but with decreasing electron mobility and electron energy. The total charge density increases with increasing beam current density, trap concentration, capture cross section, film thickness and electron-hole recombination rate, but with decreasing electron mobility and electron energy. This study shows a comprehensive analysis of microscopic factors of surface charging characteristics in an electron-based surface microscopy and analysis. Copyright © 2014 Elsevier Ltd. All rights reserved.

Structure and dynamics of the umagnetized plasma around comet 67P/CG

NASA Astrophysics Data System (ADS)

Henri, P.; Vallières, X.; Gilet, N.; Hajra, R.; Moré, J.; Goetz, C.; Richter, I.; Glassmeier, K. H.; Galand, M. F.; Heritier, K. L.; Eriksson, A. I.; Nemeth, Z.; Tsurutani, B.; Rubin, M.; Altwegg, K.

2016-12-01

At distances close enough to the Sun, when comets are characterised by a significant outgassing, the cometary neutral density may become large enough for both the cometary plasma and the cometary gas to be coupled, through ion-neutral and electron-neutral collisions. This coupling enables the formation of an unmagnetised expanding cometary ionosphere around the comet nucleus, also called diamagnetic cavity, within which the solar wind magnetic field cannot penetrate. The instruments of the Rosetta Plasma Consortium (RPC), onboard the Rosetta Orbiter, enable us to better constrain the structure, dynamics and stability of the plasma around comet 67P/CG. Recently, magnetic field measurements (RPC-MAG) have shown the existence of such a diamagnetic region around comet 67P/CG [Götz et al., 2016]. Contrary to a single, large scale, diamagnetic cavity such as what was observed around comet Halley, Rosetta have crossed several diamagnetic structures along its trajectory around comet 67P/CG. Using electron density measurements from the Mutual Impedance Probe (RPC-MIP) during the different diamagnetic cavity crossings, identified by the flux gate magnetometer (RPC-MAG), we map the unmagnetised plasma density around comet 67P/CG. Our aims is to better constrain the structure, dynamics and stability of this inner cometary plasma layer characterised by cold electrons (as witnessed by the Langmuir Probes RPC-LAP). The ionisation ratio in these unmagnetised region(s) is computed from the measured electron (RPC-MIP) and neutral gas (ROSINA/COPS) densities. In order to assess the importance of solar EUV radiation as a source of ionisation, the observed electron density will be compared to a the density expected from an ionospheric model taking into account solar radiation absorption. The crossings of diamagnetic region(s) by Rosetta show that the unmagnetised cometary plasma is particularly homogeneous, compared to the highly dynamical magnetised plasma observed in adjacent magnetised regions. Moreover, during the crossings of multiple, successive diamagnetic region(s) over time scales of tens of minutes or hours, the plasma density is almost identical in the different unmagnetised regions, suggesting that these unmagnetised regions may be a single diamagnetic structure crossed several times by Rosetta.

Extended Lagrangian Density Functional Tight-Binding Molecular Dynamics for Molecules and Solids.

PubMed

Aradi, Bálint; Niklasson, Anders M N; Frauenheim, Thomas

2015-07-14

A computationally fast quantum mechanical molecular dynamics scheme using an extended Lagrangian density functional tight-binding formulation has been developed and implemented in the DFTB+ electronic structure program package for simulations of solids and molecular systems. The scheme combines the computational speed of self-consistent density functional tight-binding theory with the efficiency and long-term accuracy of extended Lagrangian Born-Oppenheimer molecular dynamics. For systems without self-consistent charge instabilities, only a single diagonalization or construction of the single-particle density matrix is required in each time step. The molecular dynamics simulation scheme can be applied to a broad range of problems in materials science, chemistry, and biology.

Cross Comparison of Electron Density and Electron Temperature Observations from the DICE CubeSat Langmuir Probes and the Millstone Hill Incoherent Scatter Radar.

NASA Astrophysics Data System (ADS)

Swenson, C.; Erickson, P. J.; Crowley, G.; Pilinski, M.; Barjatya, A.; Fish, C. S.

2014-12-01

The Dynamic Ionosphere CubeSat Experiment (DICE) consists of two identical 1.5U CubeSats deployed simultaneously from a single P-POD (Poly Picosatellite Orbital Deployer) into the same orbit. Several observational campaigns were planned between the DICE CubeSats and the mid-latitude Millstone Hill Incoherent Scatter Radar (ISR) in order to calibrate the DICE measurements of electron density and electron temperature. In this presentation, we compare in-situ observations from the Dynamic Ionosphere CubeSat Experiment (DICE) and from the Millstone Hill ISR. Both measurements are cross-calibrated against an assimilative model of the global ionospheric electron density. The electron density and electron temperature were obtained for three Millstone Hill DICE overflights (2013-03-12, 2013-03-15, 2013-03-17). We compare the data during quiet and geomagnetically disturbed conditions and find evidence of an storm enhanced density (SED) plume in the topside ionosphere on 2013-03-17 at 19? UTC. During this disturbed interval, American longitude sector high density plasma was convected near 15 SLT towards the noontime cusp. DICE was selected for flight under the NSF "CubeSat-based Science Mission for Space Weather and Atmospheric Research" program. The DICE twin satellites were launched on a Delta II rocket on October 28, 2011. The satellites are flying in a "leader-follower" formation in an elliptical orbit which ranges from 820 to 400 km in altitude. Each satellite carries a fixed-bias DC Langmuir Probe (DCP) to measure in-situ ionospheric plasma densities and a science grade magnetometer to measure DC and AC geomagnetic fields. The purpose of these measurements was to permit accurate identification of storm-time features such as the SED bulge and plume. The mission team combines expertise from ASTRA, Utah State University/Space Dynamics Laboratory (USU/SDL), and Embry-Riddle Aeronautical University. In this paper we present a comparison of data from DICE and Millstone Hill ISR during quiet and magnetically disturbed conditions.

Electron correlation by polarization of interacting densities

NASA Astrophysics Data System (ADS)

Whitten, Jerry L.

2017-02-01

Coulomb interactions that occur in electronic structure calculations are correlated by allowing basis function components of the interacting densities to polarize dynamically, thereby reducing the magnitude of the interaction. Exchange integrals of molecular orbitals are not correlated. The modified Coulomb interactions are used in single-determinant or configuration interaction calculations. The objective is to account for dynamical correlation effects without explicitly introducing higher spherical harmonic functions into the molecular orbital basis. Molecular orbital densities are decomposed into a distribution of spherical components that conserve the charge and each of the interacting components is considered as a two-electron wavefunction embedded in the system acted on by an average field Hamiltonian plus r12-1. A method of avoiding redundancy is described. Applications to atoms, negative ions, and molecules representing different types of bonding and spin states are discussed.

Identification of parameters through which surface chemistry determines the lifetimes of hot electrons in small Au nanoparticles

PubMed Central

Aruda, Kenneth O.; Tagliazucchi, Mario; Sweeney, Christina M.; Hannah, Daniel C.; Schatz, George C.; Weiss, Emily A.

2013-01-01

This paper describes measurements of the dynamics of hot electron cooling in photoexcited gold nanoparticles (Au NPs) with diameters of ∼3.5 nm, and passivated with either a hexadecylamine or hexadecanethiolate adlayer, using ultrafast transient absorption spectroscopy. Fits of these dynamics with temperature-dependent Mie theory reveal that both the electronic heat capacity and the electron–phonon coupling constant are larger for the thiolated NPs than for the aminated NPs, by 40% and 30%, respectively. Density functional theory calculations on ligand-functionalized Au slabs show that the increase in these quantities is due to an increased electronic density of states near the Fermi level upon ligand exchange from amines to thiolates. The lifetime of hot electrons, which have thermalized from the initial plasmon excitation, increases with increasing electronic heat capacity, but decreases with increasing electron–phonon coupling, so the effects of changing surface chemistry on these two quantities partially cancel to yield a hot electron lifetime of thiolated NPs that is only 20% longer than that of aminated NPs. This analysis also reveals that incorporation of a temperature-dependent electron–phonon coupling constant is necessary to adequately fit the dynamics of electron cooling. PMID:23440215

Modeling of dynamic bipolar plasma sheaths

NASA Astrophysics Data System (ADS)

Grossmann, J. M.; Swanekamp, S. B.; Ottinger, P. F.

1991-08-01

The behavior of a one dimensional plasma sheath is described in regimes where the sheath is not in equilibrium because it carries current densities that are either time dependent, or larger than the bipolar Child-Langmuir level determined from the injected ion flux. Earlier models of dynamic bipolar sheaths assumed that ions and electrons evolve in a series of quasi-equilibria. In addition, sheath growth was described by the equation Zenoxs = (ji)-Zenouo, where xs is the velocity of the sheath edge, ji is the ion current density, nouo is the injected ion flux density, and Ze is the ion charge. In this paper, a generalization of the bipolar electron-to-ion current density ratio formula is derived to study regimes where ions are not in equilibrium. A generalization of the above sheath growth equation is also developed which is consistent with the ion continuity equation and which reveals new physics of sheath behavior associated with the emitted electrons and their evolution. Based on these findings, two new models of dynamic bipolar sheaths are developed. Larger sheath sizes and potentials than those of earlier models are found. In certain regimes, explosive sheath growth is predicted.

Monitoring nonadiabatic avoided crossing dynamics in molecules by ultrafast X-ray diffraction

DOE PAGES

Kowalewski, Markus; Bennett, Kochise; Mukamel, Shaul

2017-05-26

We examine time-resolved X-ray diffraction from molecules in the gas phase which undergo nonadiabatic avoided-crossing dynamics involving strongly coupled electrons and nuclei. Several contributions to the signal are identified, representing (in decreasing strength) elastic scattering, contributions of the electronic coherences created by nonadiabatic couplings in the avoided crossing regime, and inelastic scattering. The former probes the charge density and delivers direct information on the evolving molecular geometry. The latter two contributions are weaker and carry spatial information through the transition charge densities (off-diagonal elements of the charge-density operator). Furthermore, simulations are presented for the nonadiabatic harpooning process in the excitedmore » state of sodium fluoride.« less

Probing the Milky Way electron density using multi-messenger astronomy

NASA Astrophysics Data System (ADS)

Breivik, Katelyn; Larson, Shane

2015-04-01

Multi-messenger observations of ultra-compact binaries in both gravitational waves and electromagnetic radiation supply highly complementary information, providing new ways of characterizing the internal dynamics of these systems, as well as new probes of the galaxy itself. Electron density models, used in pulsar distance measurements via the electron dispersion measure, are currently not well constrained. Simultaneous radio and gravitational wave observations of pulsars in binaries provide a method of measuring the average electron density along the line of sight to the pulsar, thus giving a new method for constraining current electron density models. We present this method and assess its viability with simulations of the compact binary component of the Milky Way using the public domain binary evolution code, BSE. This work is supported by NASA Award NNX13AM10G.

Static, dynamic and electronic properties of expanded fluid mercury in the metal-nonmetal transition range. An ab initio study.

PubMed

Calderín, L; González, L E; González, D J

2011-09-21

Fluid Hg undergoes a metal-nonmetal (M-NM) transition when expanded toward a density of around 9 g cm(-3). We have performed ab initio molecular dynamics simulations for several thermodynamic states around the M-NM transition range and the associated static, dynamic and electronic properties have been analyzed. The calculated static structure shows a good agreement with the available experimental data. It is found that the volume expansion decreases the number of nearest neighbors from 10 (near the triple point) to around 8 at the M-NM transition region. Moreover, these neighbors are arranged into two subshells and the decrease in the number of neighbors occurs in the inner subshell. The calculated dynamic structure factors agree fairly well with their experimental counterparts obtained by inelastic x-ray scattering experiments, which display inelastic side peaks. The derived dispersion relation exhibits some positive dispersion for all the states, although its value around the M-NM transition region is not as marked as suggested by the experiment. We have also calculated the electronic density of states, which shows the appearance of a gap at a density of around 8.3 g cm(-3).

Effect of electron-phonon coupling on energy and density of states renormalizations of dynamically screened graphene

NASA Astrophysics Data System (ADS)

Leblanc, J. P. F.; Carbotte, J. P.; Nicol, E. J.

2012-02-01

Motivated by recent tunneling and angle-resolved photoemission (ARPES) work [1,2], we explore the combined effect of electron-electron and electron-phonon couplings on the renormalized energy dispersion, the spectral function, and the density of states of doped graphene. We find that the plasmarons seen in ARPES are also observable in the density of states and appear as structures with quadratic dependence on energy about the minima. Further, we illustrate how knowledge of the slopes of both the density of states and the renormalized dispersion near the Fermi level can allow for the separation of momentum and frequency dependent renormalizations to the Fermi velocity. This analysis should allow for the isolation of the renormalization due to the electron-phonon interaction from that of the electron-electron interaction. [4pt] [1] Brar et al. Phys. Rev. Lett. 104, 036805 (2010) [2] Bostwick et al. Science 328, p.999 (2010)

Atomic quantum corrals for Bose-Einstein condensates

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

Xiong Hongwei; Kavli Institute for Theoretical Physics China, Chinese Academy of Sciences, Beijing 100190; Wu Biao

2010-11-15

We consider the dynamics of Bose-Einstein condensates in a corral-like potential. Compared to the electronic quantum corrals, the atomic quantum corrals have the advantages of allowing direct and convenient observation of the wave dynamics, together with adjustable interaction strength. Our numerical study shows that these advantages not only allow exploration of the rich dynamical structures in the density distribution but also make the corrals useful in many other aspects. In particular, the corrals for atoms can be arranged into a stadium shape for the experimental visualization of quantum chaos, which has been elusive with electronic quantum corrals. The density correlationmore » is used to describe quantitatively the dynamical quantum chaos. Furthermore, we find that the interatomic interaction can greatly enhance the dynamical quantum chaos, for example, inducing a chaotic behavior even in circle-shaped corrals.« less

Unbiased reduced density matrices and electronic properties from full configuration interaction quantum Monte Carlo.

PubMed

Overy, Catherine; Booth, George H; Blunt, N S; Shepherd, James J; Cleland, Deidre; Alavi, Ali

2014-12-28

Properties that are necessarily formulated within pure (symmetric) expectation values are difficult to calculate for projector quantum Monte Carlo approaches, but are critical in order to compute many of the important observable properties of electronic systems. Here, we investigate an approach for the sampling of unbiased reduced density matrices within the full configuration interaction quantum Monte Carlo dynamic, which requires only small computational overheads. This is achieved via an independent replica population of walkers in the dynamic, sampled alongside the original population. The resulting reduced density matrices are free from systematic error (beyond those present via constraints on the dynamic itself) and can be used to compute a variety of expectation values and properties, with rapid convergence to an exact limit. A quasi-variational energy estimate derived from these density matrices is proposed as an accurate alternative to the projected estimator for multiconfigurational wavefunctions, while its variational property could potentially lend itself to accurate extrapolation approaches in larger systems.

Influence of carrier density on the electronic cooling channels of bilayer graphene

NASA Astrophysics Data System (ADS)

Limmer, T.; Houtepen, A. J.; Niggebaum, A.; Tautz, R.; Da Como, E.

2011-09-01

We study the electronic cooling dynamics in a single flake of bilayer graphene by femtosecond transient absorption probing the photon-energy range 0.25-1.3 eV. From the transients, we extract the carrier cooling curves for different initial temperatures and densities of the photoexcited electrons and holes. Two regimes of carrier cooling, dominated by optical and acoustic phonons emission, are clearly identified. For increasing carrier density, the crossover between the two regimes occurs at larger carrier temperatures, since cooling via optical phonons experiences a bottleneck. Acoustic phonons, which are less sensitive to saturation, show an increasing contribution at high density.

Electronic Correlation and Magnetism in the Ferromagnetic Metal Fe 3GeTe 2

DOE PAGES

Zhu, Jian-Xin; Janoschek, Marc; Chaves, D. S.; ...

2016-04-05

Motivated by the search for design principles of rare-earth-free strong magnets, we present a study of electronic structure and magnetic properties of the ferromagnetic metal Fe3GeTe2 within local density approximation (LDA) of the density functional theory, and its combination with dynamical mean-field theory (DMFT). For comparison to these calculations, we have measured magnetic and thermodynamic properties as well as X-ray magnetic circular dichroism and the photoemission spectrum of single crystal Fe3GeTe2. We find that the experimentally determined Sommerfeld coefficient is enhanced by an order of magnitude with respect to the LDA value. This enhancement can be partially explained by LDA+DMFT.more » Additionally, the inclusion of dynamical electronic correlation effects provides the experimentally observed magnetic moments, and the spectral density is in better agreement with photoemission data. Lastly, these results establish the importance of electronic correlations in this ferromagnet.« less

Extended Lagrangian Density Functional Tight-Binding Molecular Dynamics for Molecules and Solids

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

Aradi, Bálint; Niklasson, Anders M. N.; Frauenheim, Thomas

A computationally fast quantum mechanical molecular dynamics scheme using an extended Lagrangian density functional tight-binding formulation has been developed and implemented in the DFTB+ electronic structure program package for simulations of solids and molecular systems. The scheme combines the computational speed of self-consistent density functional tight-binding theory with the efficiency and long-term accuracy of extended Lagrangian Born–Oppenheimer molecular dynamics. Furthermore, for systems without self-consistent charge instabilities, only a single diagonalization or construction of the single-particle density matrix is required in each time step. The molecular dynamics simulation scheme can also be applied to a broad range of problems in materialsmore » science, chemistry, and biology.« less

Extended Lagrangian Density Functional Tight-Binding Molecular Dynamics for Molecules and Solids

DOE PAGES

Aradi, Bálint; Niklasson, Anders M. N.; Frauenheim, Thomas

2015-06-26

A computationally fast quantum mechanical molecular dynamics scheme using an extended Lagrangian density functional tight-binding formulation has been developed and implemented in the DFTB+ electronic structure program package for simulations of solids and molecular systems. The scheme combines the computational speed of self-consistent density functional tight-binding theory with the efficiency and long-term accuracy of extended Lagrangian Born–Oppenheimer molecular dynamics. Furthermore, for systems without self-consistent charge instabilities, only a single diagonalization or construction of the single-particle density matrix is required in each time step. The molecular dynamics simulation scheme can also be applied to a broad range of problems in materialsmore » science, chemistry, and biology.« less

Dust characteristics of dusty plasma ring of Saturn

NASA Astrophysics Data System (ADS)

Morooka, M.; Wahlund, J.-E.; Ye, S.-Y.; Persoon, A. M.; Kurth, W. S.

2017-09-01

During the Ring Grazing orbit, starting from December 2016, Cassini carried out twenty of the faint Saturn ring crossing observations at the distance of 2.45-2.51 RS (1RS 60,268 km) from Saturn center. We will show the electron and the ion density measurements of the RPWS/Langmuir Probe (LP) during these orbits. In most of the orbits significant ion/electron density differences have been observed, which indicates the presence of the charged nm and µm sized grains. The relationship between the observed charge densities and the electrical potential of the grains shows that the grains and the ambient electrons and ions are electro dynamical ensemble, a dusty plasma. The results show that characteristic dust size changes depending on the distance from the ring center. The result suggests that a dusty plasma state is related to the dynamics of the grain sizes.

Density functional theory based molecular dynamics study of hydration and electronic properties of aqueous La(3+).

PubMed

Terrier, Cyril; Vitorge, Pierre; Gaigeot, Marie-Pierre; Spezia, Riccardo; Vuilleumier, Rodolphe

2010-07-28

Structural and electronic properties of La(3+) immersed in bulk water have been assessed by means of density functional theory (DFT)-based Car-Parrinello molecular dynamics (CPMD) simulations. Correct structural properties, i.e., La(III)-water distances and La(III) coordination number, can be obtained within the framework of Car-Parrinello simulations providing that both the La pseudopotential and conditions of the dynamics (fictitious mass and time step) are carefully set up. DFT-MD explicitly treats electronic densities and is shown here to provide a theoretical justification to the necessity of including polarization when studying highly charged cations such as lanthanoids(III) with classical MD. La(3+) was found to strongly polarize the water molecules located in the first shell, giving rise to dipole moments about 0.5 D larger than those of bulk water molecules. Finally, analyzing Kohn-Sham orbitals, we found La(3+) empty 4f orbitals extremely compact and to a great extent uncoupled from the water conduction band, while the 5d empty orbitals exhibit mixing with unoccupied states of water.

Electronic-structure and quantum dynamical study of the photochromism of the aromatic Schiff base salicylideneaniline

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

Ortiz-Sanchez, Juan Manuel; Gelabert, Ricard; Moreno, Miquel

2008-12-07

The ultrafast proton transfer dynamics of salicylideneaniline has been theoretically analyzed in the ground and first singlet excited electronic states using density functional theory (DFT) and time-dependent DFT calculations, which predict a ({pi},{pi}*) barrierless excited state intramolecular proton transfer (ESIPT). In addition to this, the photochemistry of salicylideneaniline is experimentally known to present fast depopulation processes of the photoexcited species before and after the proton transfer reaction. Such processes are explained by means of conical intersections between the ground and first singlet ({pi},{pi}*) excited electronic states. The electronic energies obtained by the time-dependent density functional theory formalism have been fittedmore » to a monodimensional potential energy surface in order to perform quantum dynamics study of the processes. Our results show that the proton transfer and deactivation of the photoexcited species before the ESIPT processes are completed within 49.6 and 37.7 fs, respectively, which is in remarkable good agreement with experiments.« less

Full Quantum Dynamics Simulation of a Realistic Molecular System Using the Adaptive Time-Dependent Density Matrix Renormalization Group Method.

PubMed

Yao, Yao; Sun, Ke-Wei; Luo, Zhen; Ma, Haibo

2018-01-18

The accurate theoretical interpretation of ultrafast time-resolved spectroscopy experiments relies on full quantum dynamics simulations for the investigated system, which is nevertheless computationally prohibitive for realistic molecular systems with a large number of electronic and/or vibrational degrees of freedom. In this work, we propose a unitary transformation approach for realistic vibronic Hamiltonians, which can be coped with using the adaptive time-dependent density matrix renormalization group (t-DMRG) method to efficiently evolve the nonadiabatic dynamics of a large molecular system. We demonstrate the accuracy and efficiency of this approach with an example of simulating the exciton dissociation process within an oligothiophene/fullerene heterojunction, indicating that t-DMRG can be a promising method for full quantum dynamics simulation in large chemical systems. Moreover, it is also shown that the proper vibronic features in the ultrafast electronic process can be obtained by simulating the two-dimensional (2D) electronic spectrum by virtue of the high computational efficiency of the t-DMRG method.

Accurate van der Waals coefficients from density functional theory

PubMed Central

Tao, Jianmin; Perdew, John P.; Ruzsinszky, Adrienn

2012-01-01

The van der Waals interaction is a weak, long-range correlation, arising from quantum electronic charge fluctuations. This interaction affects many properties of materials. A simple and yet accurate estimate of this effect will facilitate computer simulation of complex molecular materials and drug design. Here we develop a fast approach for accurate evaluation of dynamic multipole polarizabilities and van der Waals (vdW) coefficients of all orders from the electron density and static multipole polarizabilities of each atom or other spherical object, without empirical fitting. Our dynamic polarizabilities (dipole, quadrupole, octupole, etc.) are exact in the zero- and high-frequency limits, and exact at all frequencies for a metallic sphere of uniform density. Our theory predicts dynamic multipole polarizabilities in excellent agreement with more expensive many-body methods, and yields therefrom vdW coefficients C6, C8, C10 for atom pairs with a mean absolute relative error of only 3%. PMID:22205765

Collision dynamics of H+ + N2 at low energies based on time-dependent density-functional theory

NASA Astrophysics Data System (ADS)

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

2018-02-01

Using time-dependent density-functional theory at the level of local density approximation augmented by a self-interaction correction and coupled non-adiabatically to molecular dynamics, we study, from a theoretical perspective, scattering dynamics of the proton in collisions with the N2 molecule at 30 eV. Nine different collision configurations are employed to analyze the proton energy loss spectra, electron depletion, scattering angles and self-interaction effects. Our results agree qualitatively with the experimental data and previous theoretical calculations. The discrepancies are ascribed to the limitation of the theoretical models in use. We find that self-interaction effects can significantly influence the electron capture and the excited diatomic vibrational motion, which is in consistent with other calculations. In addition, it is found that the molecular structure can be readily retrieved from the proton energy loss spectra due to a significant momentum transfer in head-on collisions.

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium

DOE PAGES

Zurch, Michael; Chang, Hung -Tzu; Borja, Lauren J.; ...

2017-06-01

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M 4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 10 20 cm –3. Separate electron and hole relaxation times are observedmore » as a function of hot carrier energies. A first-order electron and hole decay of ~1 ps suggests a Shockley–Read–Hall recombination mechanism. Furthermore, the simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.« less

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium

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

Zurch, Michael; Chang, Hung -Tzu; Borja, Lauren J.

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M 4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 10 20 cm –3. Separate electron and hole relaxation times are observedmore » as a function of hot carrier energies. A first-order electron and hole decay of ~1 ps suggests a Shockley–Read–Hall recombination mechanism. Furthermore, the simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.« less

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium.

PubMed

Zürch, Michael; Chang, Hung-Tzu; Borja, Lauren J; Kraus, Peter M; Cushing, Scott K; Gandman, Andrey; Kaplan, Christopher J; Oh, Myoung Hwan; Prell, James S; Prendergast, David; Pemmaraju, Chaitanya D; Neumark, Daniel M; Leone, Stephen R

2017-06-01

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M 4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 10 20  cm -3 . Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first-order electron and hole decay of ∼1 ps suggests a Shockley-Read-Hall recombination mechanism. The simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.

Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium

PubMed Central

Zürch, Michael; Chang, Hung-Tzu; Borja, Lauren J.; Kraus, Peter M.; Cushing, Scott K.; Gandman, Andrey; Kaplan, Christopher J.; Oh, Myoung Hwan; Prell, James S.; Prendergast, David; Pemmaraju, Chaitanya D.; Neumark, Daniel M.; Leone, Stephen R.

2017-01-01

Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 1020 cm−3. Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first-order electron and hole decay of ∼1 ps suggests a Shockley–Read–Hall recombination mechanism. The simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions. PMID:28569752

Time-Domain Ab Initio Analysis of Excitation Dynamics in a Quantum Dot/Polymer Hybrid: Atomistic Description Rationalizes Experiment.

PubMed

Long, Run; Prezhdo, Oleg V

2015-07-08

Hybrid organic/inorganic polymer/quantum dot (QD) solar cells are an attractive alternative to the traditional cells. The original, simple models postulate that one-dimensional polymers have continuous energy levels, while zero-dimensional QDs exhibit atom-like electronic structure. A realistic, atomistic viewpoint provides an alternative description. Electronic states in polymers are molecule-like: finite in size and discrete in energy. QDs are composed of many atoms and have high, bulk-like densities of states. We employ ab initio time-domain simulation to model the experimentally observed ultrafast photoinduced dynamics in a QD/polymer hybrid and show that an atomistic description is essential for understanding the time-resolved experimental data. Both electron and hole transfers across the interface exhibit subpicosecond time scales. The interfacial processes are fast due to strong electronic donor-acceptor, as evidenced by the densities of the photoexcited states which are delocalized between the donor and the acceptor. The nonadiabatic charge-phonon coupling is also strong, especially in the polymer, resulting in rapid energy losses. The electron transfer from the polymer is notably faster than the hole transfer from the QD, due to a significantly higher density of acceptor states. The stronger molecule-like electronic and charge-phonon coupling in the polymer rationalizes why the electron-hole recombination inside the polymer is several orders of magnitude faster than in the QD. As a result, experiments exhibit multiple transfer times for the long-lived hole inside the QD, ranging from subpicoseconds to nanoseconds. In contrast, transfer of the short-lived electron inside the polymer does not occur beyond the first picosecond. The energy lost by the hole on its transit into the polymer is accommodated by polymer's high-frequency vibrations. The energy lost by the electron injected into the QD is accommodated primarily by much lower-frequency collective and QD modes. The electron dynamics is exponential, whereas evolution of the injected hole through the low density manifold of states of the polymer is highly nonexponential. The time scale of the electron-hole recombination at the interface is intermediate between those in pristine polymer and QD and is closer to that in the polymer. The detailed atomistic insights into the photoinduced charge and energy dynamics at the polymer/QD interface provide valuable guidelines for optimization of solar light harvesting and photovoltaic efficiency in modern nanoscale materials.

Short-range density functional correlation within the restricted active space CI method

NASA Astrophysics Data System (ADS)

Casanova, David

2018-03-01

In the present work, I introduce a hybrid wave function-density functional theory electronic structure method based on the range separation of the electron-electron Coulomb operator in order to recover dynamic electron correlations missed in the restricted active space configuration interaction (RASCI) methodology. The working equations and the computational algorithm for the implementation of the new approach, i.e., RAS-srDFT, are presented, and the method is tested in the calculation of excitation energies of organic molecules. The good performance of the RASCI wave function in combination with different short-range exchange-correlation functionals in the computation of relative energies represents a quantitative improvement with respect to the RASCI results and paves the path for the development of RAS-srDFT as a promising scheme in the computation of the ground and excited states where nondynamic and dynamic electron correlations are important.

Structural, electronic, and vibrational properties of high-density amorphous silicon: a first-principles molecular-dynamics study.

PubMed

Morishita, Tetsuya

2009-05-21

We report a first-principles study of the structural, electronic, and dynamical properties of high-density amorphous (HDA) silicon, which was found to be formed by pressurizing low-density amorphous (LDA) silicon (a normal amorphous Si) [T. Morishita, Phys. Rev. Lett. 93, 055503 (2004); P. F. McMillan, M. Wilson, D. Daisenberger, and D. Machon, Nature Mater. 4, 680 (2005)]. Striking structural differences between HDA and LDA are revealed. The LDA structure holds a tetrahedral network, while the HDA structure contains a highly distorted tetrahedral network. The fifth neighboring atom in HDA tends to be located at an interstitial position of a distorted tetrahedron composed of the first four neighboring atoms. Consequently, the coordination number of HDA is calculated to be approximately 5 unlike that of LDA. The electronic density of state (EDOS) shows that HDA is metallic, which is consistent with a recent experimental measurement of the electronic resistance of HDA Si. We find from local EDOS that highly distorted tetrahedral configurations enhance the metallic nature of HDA. The vibrational density of state (VDOS) also reflects the structural differences between HDA and LDA. Some of the characteristic vibrational modes of LDA are dematerialized in HDA, indicating the degradation of covalent bonds. The overall profile of the VDOS for HDA is found to be an intermediate between that for LDA and liquid Si under pressure (high-density liquid Si).

Direct evaluation of boson dynamics via finite-temperature time-dependent variation with multiple Davydov states.

PubMed

Fujihashi, Yuta; Wang, Lu; Zhao, Yang

2017-12-21

Recent advances in quantum optics allow for exploration of boson dynamics in dissipative many-body systems. However, the traditional descriptions of quantum dissipation using reduced density matrices are unable to capture explicit information of bath dynamics. In this work, efficient evaluation of boson dynamics is demonstrated by combining the multiple Davydov Ansatz with finite-temperature time-dependent variation, going beyond what state-of-the-art density matrix approaches are capable to offer for coupled electron-boson systems. To this end, applications are made to excitation energy transfer in photosynthetic systems, singlet fission in organic thin films, and circuit quantum electrodynamics in superconducting devices. Thanks to the multiple Davydov Ansatz, our analysis of boson dynamics leads to clear revelation of boson modes strongly coupled to electronic states, as well as in-depth description of polaron creation and destruction in the presence of thermal fluctuations.

Electron-Ion Dynamics with Time-Dependent Density Functional Theory: Towards Predictive Solar Cell Modeling: Final Technical Report

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

Maitra, Neepa

2016-07-14

This project investigates the accuracy of currently-used functionals in time-dependent density functional theory, which is today routinely used to predict and design materials and computationally model processes in solar energy conversion. The rigorously-based electron-ion dynamics method developed here sheds light on traditional methods and overcomes challenges those methods have. The fundamental research undertaken here is important for building reliable and practical methods for materials discovery. The ultimate goal is to use these tools for the computational design of new materials for solar cell devices of high efficiency.

Fast and precise processing of material by means of an intensive electron beam

NASA Astrophysics Data System (ADS)

Beisswenger, S.

1984-07-01

For engraving a picture carrying screen of cells into the copper-surface of gravure cylinders, an electron beam system was developed. Numerical computations of the power density in the image planes of the electron beam determined the design of the electron optical assembly. A highly stable electron beam of high power density is generated by a ribbon-like cathode. A system of magnetic lenses is used for fast control of the engraving processes and for dynamic changing of the electron optical demagnification. The electron beam engraving system is capable of engraving up to 150,000 gravure cells per sec.

Directly calculated electrical conductivity of hot dense hydrogen from molecular dynamics simulation beyond Kubo-Greenwood formula

NASA Astrophysics Data System (ADS)

Ma, Qian; Kang, Dongdong; Zhao, Zengxiu; Dai, Jiayu

2018-01-01

Electrical conductivity of hot dense hydrogen is directly calculated by molecular dynamics simulation with a reduced electron force field method, in which the electrons are represented as Gaussian wave packets with fixed sizes. Here, the temperature is higher than electron Fermi temperature ( T > 300 eV , ρ = 40 g / cc ). The present method can avoid the Coulomb catastrophe and give the limit of electrical conductivity based on the Coulomb interaction. We investigate the effect of ion-electron coupled movements, which is lost in the static method such as density functional theory based Kubo-Greenwood framework. It is found that the ionic dynamics, which contributes to the dynamical electrical microfield and electron-ion collisions, will reduce the conductivity significantly compared with the fixed ion configuration calculations.

Atomic-scale diffractive imaging of sub-cycle electron dynamics in condensed matter

PubMed Central

Yakovlev, Vladislav S.; Stockman, Mark I.; Krausz, Ferenc; Baum, Peter

2015-01-01

For interaction of light with condensed-matter systems, we show with simulations that ultrafast electron and X-ray diffraction can provide a time-dependent record of charge-density maps with sub-cycle and atomic-scale resolutions. Using graphene as an example material, we predict that diffraction can reveal localised atomic-scale origins of optical and electronic phenomena. In particular, we point out nontrivial relations between microscopic electric current and density in undoped graphene. PMID:26412407

Atomic-scale diffractive imaging of sub-cycle electron dynamics in condensed matter

DOE PAGES

Yakovlev, Vladislav S.; Stockman, Mark I.; Krausz, Ferenc; ...

2015-09-28

For interaction of light with condensed-matter systems, we show with simulations that ultrafast electron and X-ray diffraction can provide a time-dependent record of charge-density maps with sub-cycle and atomic-scale resolutions. Using graphene as an example material, we predict that diffraction can reveal localised atomic-scale origins of optical and electronic phenomena. Here, we point out nontrivial relations between microscopic electric current and density in undoped graphene.

Beta electron fluxes inside a magnetic plasma cavern: Calculation and comparison with experiment

NASA Astrophysics Data System (ADS)

Stupitskii, E. L.; Smirnov, E. V.; Kulikova, N. A.

2010-12-01

We study the possibility of electrostatic blanking of beta electrons in the expanding spherical blob of a radioactive plasma in a rarefied ionosphere. From numerical studies on the dynamics of beta electrons departing a cavern, we obtain the form of a function that determines the portion of departing electrons and calculate the flux density of beta electrons inside the cavern in relation to the Starfish Prime nuclear blast. We show that the flux density of electrons in geomagnetic flux tubes and inside the cavern depend on a correct allowance for the quantity of beta electrons returning to the cavern. On the basis of a physical analysis, we determine the approximate criterion for the return of electrons from a geomagnetic flux tube to the cavern. We compare calculation results in terms of the flux density of beta electrons inside the cavern with the recently published experimental results from operation Starfish Prime.

Target surface area effects on hot electron dynamics from high intensity laser–plasma interactions

DOE PAGES

Zulick, C.; Raymond, A.; McKelvey, A.; ...

2016-06-15

Reduced surface area targets were studied using an ultra-high intensity femtosecond laser in order to determine the effect of electron sheath field confinement on electron dynamics. X-ray emission due to energetic electrons was imaged using a K α imaging crystal. Electrons were observed to travel along the surface of wire targets, and were slowed mainly by the induced fields. Targets with reduced surface areas were correlated with increased hot electron densities and proton energies. Furthermore, Hybrid Vlasov–Fokker–Planck simulations demonstrated increased electric sheath field strength in reduced surface area targets.

Avoiding fractional electrons in subsystem DFT based ab-initio molecular dynamics yields accurate models for liquid water and solvated OH radical

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

Genova, Alessandro, E-mail: alessandro.genova@rutgers.edu; Pavanello, Michele, E-mail: m.pavanello@rutgers.edu; Ceresoli, Davide, E-mail: davide.ceresoli@cnr.it

2016-06-21

In this work we achieve three milestones: (1) we present a subsystem DFT method capable of running ab-initio molecular dynamics simulations accurately and efficiently. (2) In order to rid the simulations of inter-molecular self-interaction error, we exploit the ability of semilocal frozen density embedding formulation of subsystem DFT to represent the total electron density as a sum of localized subsystem electron densities that are constrained to integrate to a preset, constant number of electrons; the success of the method relies on the fact that employed semilocal nonadditive kinetic energy functionals effectively cancel out errors in semilocal exchange–correlation potentials that aremore » linked to static correlation effects and self-interaction. (3) We demonstrate this concept by simulating liquid water and solvated OH{sup •} radical. While the bulk of our simulations have been performed on a periodic box containing 64 independent water molecules for 52 ps, we also simulated a box containing 256 water molecules for 22 ps. The results show that, provided one employs an accurate nonadditive kinetic energy functional, the dynamics of liquid water and OH{sup •} radical are in semiquantitative agreement with experimental results or higher-level electronic structure calculations. Our assessments are based upon comparisons of radial and angular distribution functions as well as the diffusion coefficient of the liquid.« less

Avoiding fractional electrons in subsystem DFT based ab-initio molecular dynamics yields accurate models for liquid water and solvated OH radical.

PubMed

Genova, Alessandro; Ceresoli, Davide; Pavanello, Michele

2016-06-21

In this work we achieve three milestones: (1) we present a subsystem DFT method capable of running ab-initio molecular dynamics simulations accurately and efficiently. (2) In order to rid the simulations of inter-molecular self-interaction error, we exploit the ability of semilocal frozen density embedding formulation of subsystem DFT to represent the total electron density as a sum of localized subsystem electron densities that are constrained to integrate to a preset, constant number of electrons; the success of the method relies on the fact that employed semilocal nonadditive kinetic energy functionals effectively cancel out errors in semilocal exchange-correlation potentials that are linked to static correlation effects and self-interaction. (3) We demonstrate this concept by simulating liquid water and solvated OH(•) radical. While the bulk of our simulations have been performed on a periodic box containing 64 independent water molecules for 52 ps, we also simulated a box containing 256 water molecules for 22 ps. The results show that, provided one employs an accurate nonadditive kinetic energy functional, the dynamics of liquid water and OH(•) radical are in semiquantitative agreement with experimental results or higher-level electronic structure calculations. Our assessments are based upon comparisons of radial and angular distribution functions as well as the diffusion coefficient of the liquid.

Transverse Space-Charge Field-Induced Plasma Dynamics for Ultraintense Electron-Beam Characterization

NASA Astrophysics Data System (ADS)

Tarkeshian, R.; Vay, J. L.; Lehe, R.; Schroeder, C. B.; Esarey, E. H.; Feurer, T.; Leemans, W. P.

2018-04-01

Similarly to laser or x-ray beams, the interaction of sufficiently intense particle beams with neutral gases will result in the creation of plasma. In contrast to photon-based ionization, the strong unipolar field of a particle beam can generate a plasma where the electron population receives a large initial momentum kick and escapes, leaving behind unshielded ions. Measuring the properties of the ensuing Coulomb exploding ions—such as their kinetic energy distribution, yield, and spatial distribution—can provide information about the peak electric fields that are achieved in the electron beams. Particle-in-cell simulations and analytical models are presented for high-brightness electron beams of a few femtoseconds or even hundreds of attoseconds, and transverse beam sizes on the micron scale, as generated by today's free electron lasers. Different density regimes for the utilization as a potential diagnostics are explored, and the fundamental differences in plasma dynamical behavior for e-beam or photon-based ionization are highlighted. By measuring the dynamics of field-induced ions for different gas and beam densities, a lower bound on the beam charge density can be obtained in a single shot and in a noninvasive way. The exponential dependency of the ionization yield on the beam properties can provide unprecedented spatial and temporal resolution, at the submicrometer and subfemtosecond scales, respectively, offering a practical and powerful approach to characterizing beams from accelerators at the frontiers of performance.

A neural network model of three-dimensional dynamic electron density in the inner magnetosphere

NASA Astrophysics Data System (ADS)

Chu, X.; Bortnik, J.; Li, W.; Ma, Q.; Denton, R.; Yue, C.; Angelopoulos, V.; Thorne, R. M.; Darrouzet, F.; Ozhogin, P.; Kletzing, C. A.; Wang, Y.; Menietti, J.

2017-09-01

A plasma density model of the inner magnetosphere is important for a variety of applications including the study of wave-particle interactions, and wave excitation and propagation. Previous empirical models have been developed under many limiting assumptions and do not resolve short-term variations, which are especially important during storms. We present a three-dimensional dynamic electron density (DEN3D) model developed using a feedforward neural network with electron densities obtained from four satellite missions. The DEN3D model takes spacecraft location and time series of solar and geomagnetic indices (F10.7, SYM-H, and AL) as inputs. It can reproduce the observed density with a correlation coefficient of 0.95 and predict test data set with error less than a factor of 2. Its predictive ability on out-of-sample data is tested on field-aligned density profiles from the IMAGE satellite. DEN3D's predictive ability provides unprecedented opportunities to gain insight into the 3-D behavior of the inner magnetospheric plasma density at any time and location. As an example, we apply DEN3D to a storm that occurred on 1 June 2013. It successfully reproduces various well-known dynamic features in three dimensions, such as plasmaspheric erosion and recovery, as well as plume formation. Storm time long-term density variations are consistent with expectations; short-term variations appear to be modulated by substorm activity or enhanced convection, an effect that requires further study together with multispacecraft in situ or imaging measurements. Investigating plasmaspheric refilling with the model, we find that it is not monotonic in time and is more complex than expected from previous studies, deserving further attention.

Adequacy of damped dynamics to represent the electron-phonon interaction in solids

DOE PAGES

Caro, A.; Correa, A. A.; Tamm, A.; ...

2015-10-16

Time-dependent density functional theory and Ehrenfest dynamics are used to calculate the electronic excitations produced by a moving Ni ion in a Ni crystal in the case of energetic MeV range (electronic stopping power regime), as well as thermal energy meV range (electron-phonon interaction regime). Results at high energy compare well to experimental databases of stopping power, and at low energy the electron-phonon interaction strength determined in this way is very similar to the linear response calculation and experimental measurements. This approach to electron-phonon interaction as an electronic stopping process provides the basis for a unified framework to perform classicalmore » molecular dynamics of ion-solid interaction with ab initio type nonadiabatic terms in a wide range of energies.« less

Proton cooling in ultracold low-density electron gas

NASA Astrophysics Data System (ADS)

Bobrov, A. A.; Bronin, S. Y.; Manykin, E. A.; Zelener, B. B.; Zelener, B. V.; Khikhlukha, D. R.

2015-11-01

A sole proton energy loss processes in an electron gas and the dependence of these processes on temperature and magnetic field are studied using molecular dynamics techniques in present work. It appears that for electron temperatures less than 100 K many body collisions affect the proton energy loss and these collisions must be taken into account. The influence of a strong magnetic field on the relaxation processes is also considered in this work. Calculations were performed for electron densities 10 cm-3, magnetic field 1-3 Tesla, electron temperatures 10-50 K, initial proton energies 100-10000 K.

Vibrational Properties of Hydrogen-Bonded Systems Using the Multireference Generalization to the "On-the-Fly" Electronic Structure within Quantum Wavepacket ab Initio Molecular Dynamics (QWAIMD).

PubMed

Li, Junjie; Li, Xiaohu; Iyengar, Srinivasan S

2014-06-10

We discuss a multiconfigurational treatment of the "on-the-fly" electronic structure within the quantum wavepacket ab initio molecular dynamics (QWAIMD) method for coupled treatment of quantum nuclear effects with electronic structural effects. Here, multiple single-particle electronic density matrices are simultaneously propagated with a quantum nuclear wavepacket and other classical nuclear degrees of freedom. The multiple density matrices are coupled through a nonorthogonal configuration interaction (NOCI) procedure to construct the instantaneous potential surface. An adaptive-mesh-guided set of basis functions composed of Gaussian primitives are used to simplify the electronic structure calculations. Specifically, with the replacement of the atom-centered basis functions positioned on the centers of the quantum-mechanically treated nuclei by a mesh-guided band of basis functions, the two-electron integrals used to compute the electronic structure potential surface become independent of the quantum nuclear variable and hence reusable along the entire Cartesian grid representing the quantum nuclear coordinates. This reduces the computational complexity involved in obtaining a potential surface and facilitates the interpretation of the individual density matrices as representative diabatic states. The parametric nuclear position dependence of the diabatic states is evaluated at the initial time-step using a Shannon-entropy-based sampling function that depends on an approximation to the quantum nuclear wavepacket and the potential surface. This development is meant as a precursor to an on-the-fly fully multireference electronic structure procedure embedded, on-the-fly, within a quantum nuclear dynamics formalism. We benchmark the current development by computing structural, dynamic, and spectroscopic features for a series of bihalide hydrogen-bonded systems: FHF(-), ClHCl(-), BrHBr(-), and BrHCl(-). We find that the donor-acceptor structural features are in good agreement with experiments. Spectroscopic features are computed using a unified velocity/flux autocorrelation function and include vibrational fundamentals and combination bands. These agree well with experiments and other theories.

Bypassing the Kohn-Sham equations with machine learning.

PubMed

Brockherde, Felix; Vogt, Leslie; Li, Li; Tuckerman, Mark E; Burke, Kieron; Müller, Klaus-Robert

2017-10-11

Last year, at least 30,000 scientific papers used the Kohn-Sham scheme of density functional theory to solve electronic structure problems in a wide variety of scientific fields. Machine learning holds the promise of learning the energy functional via examples, bypassing the need to solve the Kohn-Sham equations. This should yield substantial savings in computer time, allowing larger systems and/or longer time-scales to be tackled, but attempts to machine-learn this functional have been limited by the need to find its derivative. The present work overcomes this difficulty by directly learning the density-potential and energy-density maps for test systems and various molecules. We perform the first molecular dynamics simulation with a machine-learned density functional on malonaldehyde and are able to capture the intramolecular proton transfer process. Learning density models now allows the construction of accurate density functionals for realistic molecular systems.Machine learning allows electronic structure calculations to access larger system sizes and, in dynamical simulations, longer time scales. Here, the authors perform such a simulation using a machine-learned density functional that avoids direct solution of the Kohn-Sham equations.

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.

Multigrid based First-Principles Molecular Dynamics

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

Fattebert, Jean-Luc; Osei-Kuffuor, Daniel; Dunn, Ian

2017-06-01

MGmol ls a First-Principles Molecular Dynamics code. It relies on the Born-Oppenheimer approximation and models the electronic structure using Density Functional Theory, either LDA or PBE. Norm-conserving pseudopotentials are used to model atomic cores.

Kinetic theory for strongly coupled Coulomb systems

NASA Astrophysics Data System (ADS)

Dufty, James; Wrighton, Jeffrey

2018-01-01

The calculation of dynamical properties for matter under extreme conditions is a challenging task. The popular Kubo-Greenwood model exploits elements from equilibrium density-functional theory (DFT) that allow a detailed treatment of electron correlations, but its origin is largely phenomenological; traditional kinetic theories have a more secure foundation but are limited to weak ion-electron interactions. The objective here is to show how a combination of the two evolves naturally from the short-time limit for the generator of the effective single-electron dynamics governing time correlation functions without such limitations. This provides a theoretical context for the current DFT-related approach, the Kubo-Greenwood model, while showing the nature of its corrections. The method is to calculate the short-time dynamics in the single-electron subspace for a given configuration of the ions. This differs from the usual kinetic theory approach in which an average over the ions is performed as well. In this way the effective ion-electron interaction includes strong Coulomb coupling and is shown to be determined from DFT. The correlation functions have the form of the random-phase approximation for an inhomogeneous system but with renormalized ion-electron and electron-electron potentials. The dynamic structure function, density response function, and electrical conductivity are calculated as examples. The static local field corrections in the dielectric function are identified in this way. The current analysis is limited to semiclassical electrons (quantum statistical potentials), so important quantum conditions are excluded. However, a quantization of the kinetic theory is identified for broader application while awaiting its detailed derivation.

Femtosecond-laser induced dynamics of CO on Ru(0001): Deep insights from a hot-electron friction model including surface motion

NASA Astrophysics Data System (ADS)

Scholz, Robert; Floß, Gereon; Saalfrank, Peter; Füchsel, Gernot; Lončarić, Ivor; Juaristi, J. I.

2016-10-01

A Langevin model accounting for all six molecular degrees of freedom is applied to femtosecond-laser induced, hot-electron driven dynamics of Ru(0001)(2 ×2 ):CO. In our molecular dynamics with electronic friction approach, a recently developed potential energy surface based on gradient-corrected density functional theory accounting for van der Waals interactions is adopted. Electronic friction due to the coupling of molecular degrees of freedom to electron-hole pairs in the metal are included via a local density friction approximation, and surface phonons by a generalized Langevin oscillator model. The action of ultrashort laser pulses enters through a substrate-mediated, hot-electron mechanism via a time-dependent electronic temperature (derived from a two-temperature model), causing random forces acting on the molecule. The model is applied to laser induced lateral diffusion of CO on the surface, "hot adsorbate" formation, and laser induced desorption. Reaction probabilities are strongly enhanced compared to purely thermal processes, both for diffusion and desorption. Reaction yields depend in a characteristic (nonlinear) fashion on the applied laser fluence, as well as branching ratios for various reaction channels. Computed two-pulse correlation traces for desorption and other indicators suggest that aside from electron-hole pairs, phonons play a non-negligible role for laser induced dynamics in this system, acting on a surprisingly short time scale. Our simulations on precomputed potentials allow for good statistics and the treatment of long-time dynamics (300 ps), giving insight into this system which hitherto has not been reached. We find generally good agreement with experimental data where available and make predictions in addition. A recently proposed laser induced population of physisorbed precursor states could not be observed with the present low-coverage model.

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.

Preliminary analysis of coronal electron content measurements from spacecraft Helios A around first solar occultation

NASA Technical Reports Server (NTRS)

Edenhofer, P.; Esposito, P. B.; Martin, W. L.; Zygielbaum, A. I.; Hansen, R. T.; Hansen, S. F.; Lueneburg, E.

1977-01-01

Steady-state and dynamical features of the electron density distribution in the solar corona emerge from a preliminary analysis of Helios A electron content measurements. There are strong indications that correlations can be established with earth-bound K-coronagraph measurements.

Longitudinal density modulation and energy conversion in intense beams.

PubMed

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

2007-08-01

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

Accounting for intra-molecular vibrational modes in open quantum system description of molecular systems.

PubMed

Roden, Jan; Strunz, Walter T; Whaley, K Birgitta; Eisfeld, Alexander

2012-11-28

Electronic-vibrational dynamics in molecular systems that interact with an environment involve a large number of degrees of freedom and are therefore often described by means of open quantum system approaches. A popular approach is to include only the electronic degrees of freedom into the system part and to couple these to a non-Markovian bath of harmonic vibrational modes that is characterized by a spectral density. Since this bath represents both intra-molecular and external vibrations, it is important to understand how to construct a spectral density that accounts for intra-molecular vibrational modes that couple further to other modes. Here, we address this problem by explicitly incorporating an intra-molecular vibrational mode together with the electronic degrees of freedom into the system part and using the Fano theory for a resonance coupled to a continuum to derive an "effective" bath spectral density, which describes the contribution of intra-molecular modes. We compare this effective model for the intra-molecular mode with the method of pseudomodes, a widely used approach in simulation of non-Markovian dynamics. We clarify the difference between these two approaches and demonstrate that the respective resulting dynamics and optical spectra can be very different.

An observational study of the nightside ionospheres of Mars and Venus with radio occultation methods

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

Zhang, M.H.G.; Luhmann, J.G.; Kliore, A.J.

1990-10-01

An analysis of Mars and Venus nightside electron density profiles obtained with radio occultation methods shows how the nightside ionospheres of both planets vary with solar zenith angle. From previous studies it is known that the dayside peak electron densities at Mars and Venus show a basic similarity in that they both exhibit Chapman layer-like behavior. In contrast, the peak altitudes at mars behave like an ideal Chapman layer on the dayside, whereas the altitude of the peak at Venus is fairly constant up to the terminator. The effect of major dust storms can also be seen in the peakmore » altitudes at Mars. All Venus nightside electron density profiles show a distinct main peak for both solar minimum and maximum, whereas many profiles from the nightside of Mars do not show any peak at all. This suggests that the electron density in the Mars nightside ionosphere is frequently too low to be detected by radio occultation. On the Pioneer Venus orbiter, disappearing ionospheres were observed near solar maximum in the in-situ data when the solar wind dynamic pressure was exceptionally high. This condition occurs because the high solar wind dynamic pressure decreases the altitude of the ionopause near the terminator below {approximately}250 km, thus reducing the normal nightward transport of dayside ionospheric plasma. On the basis of the Venus observations, one might predict that if a positive correlation of nightside peak density with dynamic pressure was found, it could mean that transport from the dayside is the only significant source for the nightside ionosphere of Mars. The lack of a correlation would imply that the precipitation source at Mars is quite variable.« less

Time delay occultation data of the Helios spacecraft for probing the electron density distribution in the solar corona

NASA Technical Reports Server (NTRS)

Edenhofer, P.; Lueneburg, E.; Esposito, P. B.; Martin, W. L.; Zygielbaum, A. I.; Hansen, R. T.; Hansen, S. F.

1978-01-01

S-band time delay measurements were collected from the spacecraft Helios A and B during three solar occultations in 1975/76 within heliocentric distances of about 3 and 215 earth radius in terms of range, Doppler frequency shift, and electron content. Characteristic features of measurement and data processing are described. Typical data sets are discussed to probe the electron density distribution near the sun (west and east limb as well) including the outer and extended corona. Steady-state and dynamical aspects of the solar corona are presented and compared with earth-bound-K-coronagraph measurements. Using a weighted least squares estimation, parameters of an average coronal electron density profile are derived in a preliminary analysis to yield electron densities at r = 3, 65, 215 earth radius. Transient phenomena are discussed and a velocity of propagation v is nearly equal to 900 km/s is determined for plasma ejecta from a solar flare observed during an extraordinary set of Helios B electron content measurements.

Flavin Charge Transfer Transitions Assist DNA Photolyase Electron Transfer

NASA Astrophysics Data System (ADS)

Skourtis, Spiros S.; Prytkova, Tatiana; Beratan, David N.

2007-12-01

This contribution describes molecular dynamics, semi-empirical and ab-initio studies of the primary photo-induced electron transfer reaction in DNA photolyase. DNA photolyases are FADH--containing proteins that repair UV-damaged DNA by photo-induced electron transfer. A DNA photolyase recognizes and binds to cyclobutatne pyrimidine dimer lesions of DNA. The protein repairs a bound lesion by transferring an electron to the lesion from FADH-, upon photo-excitation of FADH- with 350-450 nm light. We compute the lowest singlet excited states of FADH- in DNA photolyase using INDO/S configuration interaction, time-dependent density-functional, and time-dependent Hartree-Fock methods. The calculations identify the lowest singlet excited state of FADH- that is populated after photo-excitation and that acts as the electron donor. For this donor state we compute conformationally-averaged tunneling matrix elements to empty electron-acceptor states of a thymine dimer bound to photolyase. The conformational averaging involves different FADH--thymine dimer confromations obtained from molecular dynamics simulations of the solvated protein with a thymine dimer docked in its active site. The tunneling matrix element computations use INDO/S-level Green's function, energy splitting, and Generalized Mulliken-Hush methods. These calculations indicate that photo-excitation of FADH- causes a π→π* charge-transfer transition that shifts electron density to the side of the flavin isoalloxazine ring that is adjacent to the docked thymine dimer. This shift in electron density enhances the FADH--to-dimer electronic coupling, thus inducing rapid electron transfer.

Dynamics of electron injection in a laser-wakefield accelerator

NASA Astrophysics Data System (ADS)

Xu, J.; Buck, A.; Chou, S.-W.; Schmid, K.; Shen, B.; Tajima, T.; Kaluza, M. C.; Veisz, L.

2017-08-01

The detailed temporal evolution of the laser-wakefield acceleration process with controlled injection, producing reproducible high-quality electron bunches, has been investigated. The localized injection of electrons into the wakefield has been realized in a simple way—called shock-front injection—utilizing a sharp drop in plasma density. Both experimental and numerical results reveal the electron injection and acceleration process as well as the electron bunch's temporal properties. The possibility to visualize the plasma wave gives invaluable spatially resolved information about the local background electron density, which in turn allows for an efficient suppression of electron self-injection before the controlled process of injection at the sharp density jump. Upper limits for the electron bunch duration of 6.6 fs FWHM, or 2.8 fs (r.m.s.) were found. These results indicate that shock-front injection not only provides stable and tunable, but also few-femtosecond short electron pulses for applications such as ultrashort radiation sources, time-resolved electron diffraction or for the seeding of further acceleration stages.

Quantum electron-vibrational dynamics at finite temperature: Thermo field dynamics approach

NASA Astrophysics Data System (ADS)

Borrelli, Raffaele; Gelin, Maxim F.

2016-12-01

Quantum electron-vibrational dynamics in molecular systems at finite temperature is described using an approach based on the thermo field dynamics theory. This formulation treats temperature effects in the Hilbert space without introducing the Liouville space. A comparison with the theoretically equivalent density matrix formulation shows the key numerical advantages of the present approach. The solution of thermo field dynamics equations with a novel technique for the propagation of tensor trains (matrix product states) is discussed. Numerical applications to model spin-boson systems show that the present approach is a promising tool for the description of quantum dynamics of complex molecular systems at finite temperature.

Unified first principles description from warm dense matter to ideal ionized gas plasma: electron-ion collisions induced friction.

PubMed

Dai, Jiayu; Hou, Yong; Yuan, Jianmin

2010-06-18

Electron-ion interactions are central to numerous phenomena in the warm dense matter (WDM) regime and at higher temperature. The electron-ion collisions induced friction at high temperature is introduced in the procedure of ab initio molecular dynamics using the Langevin equation based on density functional theory. In this framework, as a test for Fe and H up to 1000 eV, the equation of state and the transition of electronic structures of the materials with very wide density and temperature can be described, which covers a full range of WDM up to high energy density physics. A unified first principles description from condensed matter to ideal ionized gas plasma is constructed.

Dynamics and reactivity of trapped electrons on supported ice crystallites.

PubMed

Stähler, Julia; Gahl, Cornelius; Wolf, Martin

2012-01-17

The solvation dynamics and reactivity of localized excess electrons in aqueous environments have attracted great attention in many areas of physics, chemistry, and biology. This manifold attraction results from the importance of water as a solvent in nature as well as from the key role of low-energy electrons in many chemical reactions. One prominent example is the electron-induced dissociation of chlorofluorocarbons (CFCs). Low-energy electrons are also critical in the radiation chemistry that occurs in nuclear reactors. Excess electrons in an aqueous environment are localized and stabilized by the local rearrangement of the surrounding water dipoles. Such solvated or hydrated electrons are known to play an important role in systems such as biochemical reactions and atmospheric chemistry. Despite numerous studies over many years, little is known about the microscopic details of these electron-induced chemical processes, and interest in the fundamental processes involved in the reactivity of trapped electrons continues. In this Account, we present a surface science study of the dynamics and reactivity of such localized low-energy electrons at D(2)O crystallites that are supported by a Ru(001) single crystal metal surface. This approach enables us to investigate the generation and relaxation dynamics as well as dissociative electron attachment (DEA) reaction of excess electrons under well-defined conditions. They are generated by photoexcitation in the metal template and transferred to trapping sites at the vacuum interface of crystalline D(2)O islands. In these traps, the electrons are effectively decoupled from the electronic states of the metal template, leading to extraordinarily long excited state lifetimes on the order of minutes. Using these long-lived, low-energy electrons, we study the DEA to CFCl(3) that is coadsorbed at very low concentrations (∼10(12) cm(-2)). Using rate equations and direct measurement of the change of surface dipole moment, we estimated the electron surface density for DEA, yielding cross sections that are orders of magnitude higher than the electron density measured in the gas phase.

From Geometry Optimization to Time Dependent Molecular Structure Modeling: Method Developments, ab initio Theories and Applications

NASA Astrophysics Data System (ADS)

Liang, Wenkel

This dissertation consists of two general parts: (I) developments of optimization algorithms (both nuclear and electronic degrees of freedom) for time-independent molecules and (II) novel methods, first-principle theories and applications in time dependent molecular structure modeling. In the first part, we discuss in specific two new algorithms for static geometry optimization, the eigenspace update (ESU) method in nonredundant internal coordinate that exhibits an enhanced performace with up to a factor of 3 savings in computational cost for large-sized molecular systems; the Car-Parrinello density matrix search (CP-DMS) method that enables direct minimization of the SCF energy as an effective alternative to conventional diagonalization approach. For the second part, we consider the time dependence and first presents two nonadiabatic dynamic studies that model laser controlled molecular photo-dissociation for qualitative understandings of intense laser-molecule interaction, using ab initio direct Ehrenfest dynamics scheme implemented with real-time time-dependent density functional theory (RT-TDDFT) approach developed in our group. Furthermore, we place our special interest on the nonadiabatic electronic dynamics in the ultrafast time scale, and presents (1) a novel technique that can not only obtain energies but also the electron densities of doubly excited states within a single determinant framework, by combining methods of CP-DMS with RT-TDDFT; (2) a solvated first-principles electronic dynamics method by incorporating the polarizable continuum solvation model (PCM) to RT-TDDFT, which is found to be very effective in describing the dynamical solvation effect in the charge transfer process and yields a consistent absorption spectrum in comparison to the conventional linear response results in solution. (3) applications of the PCM-RT-TDDFT method to study the intramolecular charge-transfer (CT) dynamics in a C60 derivative. Such work provides insights into the characteristics of ultrafast dynamics in photoexcited fullerene derivatives, and aids in the rational design for pre-dissociative exciton in the intramolecular CT process in organic solar cells.

Counterion effects on the ultrafast dynamics of charge-transfer-to-solvent electrons.

PubMed

Rivas, N; Moriena, G; Domenianni, L; Hodak, J H; Marceca, E

2017-12-06

We performed femtosecond transient absorption (TA) experiments to monitor the solvation dynamics of charge-transfer-to-solvent (CTTS) electrons originating from UV photoexcitation of ammoniated iodide in close proximity to the counterions. Solutions of KI were prepared in liquid ammonia and TA experiments were carried out at different temperatures and densities, along the liquid-gas coexistence curve of the fluid. The results complement previous femtosecond TA work by P. Vöhringer's group in neat ammonia via multiphoton ionization. The dynamics of CTTS-detached electrons in ammonia was found to be strongly affected by ion pairing. Geminate recombination time constants as well as escape probabilities were determined from the measured temporal profiles and analysed as a function of the medium density. A fast unresolved (τ < 250 fs) increase of absorption related to the creation/thermalization of solvated electron species was followed by two decay components: one with a characteristic time around 10 ps, and a slower one that remains active for hundreds of picoseconds. While the first process is attributed to an early recombination of (I, e - ) pairs, the second decay and its asymptote reflects the effect of the K + counterion on the geminate recombination dynamics, rate and yield. The cation basically acts as an electron anchor that restricts the ejection distance, leading to solvent-separated counterion-electron species. The formation of (K + , NH 3 , e - ) pairs close to the parent iodine atom brings the electron escape probability to very low values. Transient spectra of the electron species have also been estimated as a function of time by probing the temporal profiles at different wavelengths.

Probing the structural and dynamical properties of liquid water with models including non-local electron correlation

NASA Astrophysics Data System (ADS)

Del Ben, Mauro; Hutter, Jürg; VandeVondele, Joost

2015-08-01

Water is a ubiquitous liquid that displays a wide range of anomalous properties and has a delicate structure that challenges experiment and simulation alike. The various intermolecular interactions that play an important role, such as repulsion, polarization, hydrogen bonding, and van der Waals interactions, are often difficult to reproduce faithfully in atomistic models. Here, electronic structure theories including all these interactions at equal footing, which requires the inclusion of non-local electron correlation, are used to describe structure and dynamics of bulk liquid water. Isobaric-isothermal (NpT) ensemble simulations based on the Random Phase Approximation (RPA) yield excellent density (0.994 g/ml) and fair radial distribution functions, while various other density functional approximations produce scattered results (0.8-1.2 g/ml). Molecular dynamics simulation in the microcanonical (NVE) ensemble based on Møller-Plesset perturbation theory (MP2) yields dynamical properties in the condensed phase, namely, the infrared spectrum and diffusion constant. At the MP2 and RPA levels of theory, ice is correctly predicted to float on water, resolving one of the anomalies as resulting from a delicate balance between van der Waals and hydrogen bonding interactions. For several properties, obtaining quantitative agreement with experiment requires correction for nuclear quantum effects (NQEs), highlighting their importance, for structure, dynamics, and electronic properties. A computed NQE shift of 0.6 eV for the band gap and absorption spectrum illustrates the latter. Giving access to both structure and dynamics of condensed phase systems, non-local electron correlation will increasingly be used to study systems where weak interactions are of paramount importance.

Ring current electron dynamics during geomagnetic storms based on the Van Allen Probes measurements: Ring Current Electrons

DOE PAGES

Zhao, H.; Li, X.; Baker, D. N.; ...

2016-04-16

Based on comprehensive measurements from Helium, Oxygen, Proton, and Electron Mass Spectrometer Ion Spectrometer, Relativistic Electron-Proton Telescope, and Radiation Belt Storm Probes Ion Composition Experiment instruments on the Van Allen Probes, comparative studies of ring current electrons and ions are performed and the role of energetic electrons in the ring current dynamics is investigated. The deep injections of tens to hundreds of keV electrons and tens of keV protons into the inner magnetosphere occur frequently; after the injections the electrons decay slowly in the inner belt but protons in the low L region decay very fast. Intriguing similarities between lowermore » energy protons and higher-energy electrons are also found. The evolution of ring current electron and ion energy densities and energy content are examined in detail during two geomagnetic storms, one moderate and one intense. Here, the results show that the contribution of ring current electrons to the ring current energy content is much smaller than that of ring current ions (up to ~12% for the moderate storm and ~7% for the intense storm), and <35 keV electrons dominate the ring current electron energy content at the storm main phases. Though the electron energy content is usually much smaller than that of ions, the enhancement of ring current electron energy content during the moderate storm can get to ~30% of that of ring current ions, indicating a more dynamic feature of ring current electrons and important role of electrons in the ring current buildup. Lastly, the ring current electron energy density is also shown to be higher at midnight and dawn while lower at noon and dusk.« less

Compression of a mixed antiproton and electron non-neutral plasma to high densities

NASA Astrophysics Data System (ADS)

Aghion, Stefano; Amsler, Claude; Bonomi, Germano; Brusa, Roberto S.; Caccia, Massimo; Caravita, Ruggero; Castelli, Fabrizio; Cerchiari, Giovanni; Comparat, Daniel; Consolati, Giovanni; Demetrio, Andrea; Di Noto, Lea; Doser, Michael; Evans, Craig; Fanì, Mattia; Ferragut, Rafael; Fesel, Julian; Fontana, Andrea; Gerber, Sebastian; Giammarchi, Marco; Gligorova, Angela; Guatieri, Francesco; Haider, Stefan; Hinterberger, Alexander; Holmestad, Helga; Kellerbauer, Alban; Khalidova, Olga; Krasnický, Daniel; Lagomarsino, Vittorio; Lansonneur, Pierre; Lebrun, Patrice; Malbrunot, Chloé; Mariazzi, Sebastiano; Marton, Johann; Matveev, Victor; Mazzotta, Zeudi; Müller, Simon R.; Nebbia, Giancarlo; Nedelec, Patrick; Oberthaler, Markus; Pacifico, Nicola; Pagano, Davide; Penasa, Luca; Petracek, Vojtech; Prelz, Francesco; Prevedelli, Marco; Rienaecker, Benjamin; Robert, Jacques; Røhne, Ole M.; Rotondi, Alberto; Sandaker, Heidi; Santoro, Romualdo; Smestad, Lillian; Sorrentino, Fiodor; Testera, Gemma; Tietje, Ingmari C.; Widmann, Eberhard; Yzombard, Pauline; Zimmer, Christian; Zmeskal, Johann; Zurlo, Nicola; Antonello, Massimiliano

2018-04-01

We describe a multi-step "rotating wall" compression of a mixed cold antiproton-electron non-neutral plasma in a 4.46 T Penning-Malmberg trap developed in the context of the AEḡIS experiment at CERN. Such traps are routinely used for the preparation of cold antiprotons suitable for antihydrogen production. A tenfold antiproton radius compression has been achieved, with a minimum antiproton radius of only 0.17 mm. We describe the experimental conditions necessary to perform such a compression: minimizing the tails of the electron density distribution is paramount to ensure that the antiproton density distribution follows that of the electrons. Such electron density tails are remnants of rotating wall compression and in many cases can remain unnoticed. We observe that the compression dynamics for a pure electron plasma behaves the same way as that of a mixed antiproton and electron plasma. Thanks to this optimized compression method and the high single shot antiproton catching efficiency, we observe for the first time cold and dense non-neutral antiproton plasmas with particle densities n ≥ 1013 m-3, which pave the way for an efficient pulsed antihydrogen production in AEḡIS.

Dynamic Characteristics of Positive Pulsed Dielectric Barrier Discharge for Ozone Generation in Air

NASA Astrophysics Data System (ADS)

Wei, Linsheng; Peng, Bangfa; Li, Ming; Zhang, Yafang; Hu, Zhaoji

2016-02-01

A comprehensive dynamic model consisting of 66 reactions and 24 species is developed to investigate the dynamic characteristics of ozone generation by positive pulsed dielectric barrier discharge (DBD) using parallel-plate reactor in air. The electron energy conservation equation is coupled to the electron continuity equation, the heavy species continuity equation, and Poisson's equation for a better description. The reliability of the model is experimentally confirmed. The model can be used to predict the temporal and spatial evolution of species, as well as streamer propagation. The simulation results show that electron density increases nearly exponentially in the direction to the anode at the electron avalanche. Streamer propagation velocity is about 5.26 × 104 m/s from anode to cathode in the simulated condition. The primary positive ion, negative ion, and excited species are O2+, O3- and O2(1Δg) in pulsed DBD in air, respectively. N2O has the largest density among nitrogen oxides. e and N2+ densities in the streamer head increase gradually to maximum values with the development of the streamer. Meanwhile, the O2+, O, O3, N2(A3Σ) and N2O densities reach maximum values in the vicinity of the anode. supported by National Natural Science Foundation of China (Nos. 51366012 and 11105067), Jiangxi Province Young Scientists (Jinggang Star) Cultivation Plan of China (No. 20133BCB23008), Natural Science Foundation of Jiangxi, China (No. 20151BAB206047) and Jiangxi Province Higher School Science and Technology Landing Plan of China (No. KJLD-14015)

Kinetic theory molecular dynamics and hot dense matter: theoretical foundations.

PubMed

Graziani, F R; Bauer, J D; Murillo, M S

2014-09-01

Electrons are weakly coupled in hot, dense matter that is created in high-energy-density experiments. They are also mildly quantum mechanical and the ions associated with them are classical and may be strongly coupled. In addition, the dynamical evolution of plasmas under these hot, dense matter conditions involve a variety of transport and energy exchange processes. Quantum kinetic theory is an ideal tool for treating the electrons but it is not adequate for treating the ions. Molecular dynamics is perfectly suited to describe the classical, strongly coupled ions but not the electrons. We develop a method that combines a Wigner kinetic treatment of the electrons with classical molecular dynamics for the ions. We refer to this hybrid method as "kinetic theory molecular dynamics," or KTMD. The purpose of this paper is to derive KTMD from first principles and place it on a firm theoretical foundation. The framework that KTMD provides for simulating plasmas in the hot, dense regime is particularly useful since current computational methods are generally limited by their inability to treat the dynamical quantum evolution of the electronic component. Using the N-body von Neumann equation for the electron-proton plasma, three variations of KTMD are obtained. Each variant is determined by the physical state of the plasma (e.g., collisional versus collisionless). The first variant of KTMD yields a closed set of equations consisting of a mean-field quantum kinetic equation for the electron one-particle distribution function coupled to a classical Liouville equation for the protons. The latter equation includes both proton-proton Coulombic interactions and an effective electron-proton interaction that involves the convolution of the electron density with the electron-proton Coulomb potential. The mean-field approach is then extended to incorporate equilibrium electron-proton correlations through the Singwi-Tosi-Land-Sjolander (STLS) ansatz. This is the second variant of KTMD. The STLS contribution produces an effective electron-proton interaction that involves the electron-proton structure factor, thereby extending the usual mean-field theory to correlated but near equilibrium systems. Finally, a third variant of KTMD is derived. It includes dynamical electrons and their correlations coupled to a MD description for the ions. A set of coupled equations for the one-particle electron Wigner function and the electron-electron and electron-proton correlation functions are coupled to a classical Liouville equation for the protons. This latter variation has both time and momentum dependent correlations.

An improved model to estimate trapping parameters in polymeric materials and its application on normal and aged low-density polyethylenes

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

Liu, Ning, E-mail: nl4g12@soton.ac.uk; He, Miao; Alghamdi, Hisham

2015-08-14

Trapping parameters can be considered as one of the important attributes to describe polymeric materials. In the present paper, a more accurate charge dynamics model has been developed, which takes account of charge dynamics in both volts-on and off stage into simulation. By fitting with measured charge data with the highest R-square value, trapping parameters together with injection barrier of both normal and aged low-density polyethylene samples were estimated using the improved model. The results show that, after long-term ageing process, the injection barriers of both electrons and holes is lowered, overall trap depth is shallower, and trap density becomesmore » much greater. Additionally, the changes in parameters for electrons are more sensitive than those of holes after ageing.« less

An Experiment to Study Sporadic Sodium Layers in the Earth's Mesosphere and Lower Thermosphere

NASA Technical Reports Server (NTRS)

Swenson, Charles M.

2002-01-01

The Utah State University / Space Dynamics Lab was funded under a NASA Grant. This investigation has been part of Rockwell Universities Sudden Atom Layer Investigation (SAL). USU/SDL provided an electron density measurement instrument, the plasma frequency probe, which was launched on the vehicle 21.117 from Puerto-Rico in February of 1998. The instrument successfully measured electron density as designed and measurement techniques included in this version of the Plasma Frequency probe provided valuable insight into the electron density structures associated with sudden sodium layers in a collisional plasma. Electron density data was furnished to Rockwell University but no science meetings were held by Rockwell Data from the instrument was presented to the scientific community at the URSI General Session in 1999. A paper is in preparation for publication in Geophysical Research Letters. The following document provides a summary of the experiment and data obtained as a final report on this grant.

Time-resolved photoelectron spectroscopy of IR-driven electron dynamics in a charge transfer model system.

PubMed

Falge, Mirjam; Fröbel, Friedrich Georg; Engel, Volker; Gräfe, Stefanie

2017-08-02

If the adiabatic approximation is valid, electrons smoothly adapt to molecular geometry changes. In contrast, as a characteristic of diabatic dynamics, the electron density does not follow the nuclear motion. Recently, we have shown that the asymmetry in time-resolved photoelectron spectra serves as a tool to distinguish between these dynamics [Falge et al., J. Phys. Chem. Lett., 2012, 3, 2617]. Here, we investigate the influence of an additional, moderately intense infrared (IR) laser field, as often applied in attosecond time-resolved experiments, on such asymmetries. This is done using a simple model for coupled electronic-nuclear motion. We calculate time-resolved photoelectron spectra and their asymmetries and demonstrate that the spectra directly map the bound electron-nuclear dynamics. From the asymmetries, we can trace the IR field-induced population transfer and both the field-driven and intrinsic (non-)adiabatic dynamics. This holds true when considering superposition states accompanied by electronic coherences. The latter are observable in the asymmetries for sufficiently short XUV pulses to coherently probe the coupled states. It is thus documented that the asymmetry is a measure for phases in bound electron wave packets and non-adiabatic dynamics.

Dynamics of the Trapped Electron Phase Space Density in Relation to the Wave Activity in the Inner Magnetosphere

NASA Astrophysics Data System (ADS)

Vassiliadis, D.; Green, J.

2008-05-01

The phase space density fe of the radiation belt electron population is reconstructed based on measurements made by POLAR/HIST. The density peaks in invariant space (mu, K, L*) are shown to be responding to changes in the solar wind velocity and density, and the interplanetary magnetic field. We have associated specific types of storms with the appearance of peaks thereby producing a climatology of fe. We will report on comparing the phase space density changes during these storms to the ULF wave power in the inner magnetosphere remote- sensed by the IMAGE magnetometer array and related properties of the wave environment.

Nonequilibrium response of an electron-mediated charge density wave ordered material to a large dc electric field

NASA Astrophysics Data System (ADS)

Matveev, O. P.; Shvaika, A. M.; Devereaux, T. P.; Freericks, J. K.

2016-01-01

Using the Kadanoff-Baym-Keldysh formalism, we employ nonequilibrium dynamical mean-field theory to exactly solve for the nonlinear response of an electron-mediated charge-density-wave-ordered material. We examine both the dc current and the order parameter of the conduction electrons as the ordered system is driven by the electric field. Although the formalism we develop applies to all models, for concreteness, we examine the charge-density-wave phase of the Falicov-Kimball model, which displays a number of anomalous behaviors including the appearance of subgap density of states as the temperature increases. These subgap states should have a significant impact on transport properties, particularly the nonlinear response of the system to a large dc electric field.

Ab initio molecular dynamics simulation study of successive hydrogenation reactions of carbon monoxide producing methanol

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

Pham, Thi Nu; Ono, Shota; Ohno, Kaoru, E-mail: ohno@ynu.ac.jp

Doing ab initio molecular dynamics simulations, we demonstrate a possibility of hydrogenation of carbon monoxide producing methanol step by step. At first, the hydrogen atom reacts with the carbon monoxide molecule at the excited state forming the formyl radical. Formaldehyde was formed after adding one more hydrogen atom to the system. Finally, absorption of two hydrogen atoms to formaldehyde produces methanol molecule. This study is performed by using the all-electron mixed basis approach based on the time dependent density functional theory within the adiabatic local density approximation for an electronic ground-state configuration and the one-shot GW approximation for an electronicmore » excited state configuration.« less

Nonlinear interactions between electromagnetic waves and electron plasma oscillations in quantum plasmas.

PubMed

Shukla, P K; Eliasson, B

2007-08-31

We consider nonlinear interactions between intense circularly polarized electromagnetic (CPEM) waves and electron plasma oscillations (EPOs) in a dense quantum plasma, taking into account the electron density response in the presence of the relativistic ponderomotive force and mass increase in the CPEM wave fields. The dynamics of the CPEM waves and EPOs is governed by the two coupled nonlinear Schrödinger equations and Poisson's equation. The nonlinear equations admit the modulational instability of an intense CPEM pump wave against EPOs, leading to the formation and trapping of localized CPEM wave pipes in the electron density hole that is associated with a positive potential distribution in our dense plasma. The relevance of our investigation to the next generation intense laser-solid density plasma interaction experiments is discussed.

Ultrafast Solvation Dynamics and Vibrational Coherences of Halogenated Boron-Dipyrromethene Derivatives Revealed through Two-Dimensional Electronic Spectroscopy.

PubMed

Lee, Yumin; Das, Saptaparna; Malamakal, Roy M; Meloni, Stephen; Chenoweth, David M; Anna, Jessica M

2017-10-18

Boron-dipyrromethene (BODIPY) chromophores have a wide range of applications, spanning areas from biological imaging to solar energy conversion. Understanding the ultrafast dynamics of electronically excited BODIPY chromophores could lead to further advances in these areas. In this work, we characterize and compare the ultrafast dynamics of halogenated BODIPY chromophores through applying two-dimensional electronic spectroscopy (2DES). Through our studies, we demonstrate a new data analysis procedure for extracting the dynamic Stokes shift from 2DES spectra revealing an ultrafast solvent relaxation. In addition, we extract the frequency of the vibrational modes that are strongly coupled to the electronic excitation, and compare the results of structurally different BODIPY chromophores. We interpret our results with the aid of DFT calculations, finding that structural modifications lead to changes in the frequency, identity, and magnitude of Franck-Condon active vibrational modes. We attribute these changes to differences in the electron density of the electronic states of the structurally different BODIPY chromophores.

Floquet theory of microwave absorption by an impurity in the two-dimensional electron gas

NASA Astrophysics Data System (ADS)

Chepelianskii, Alexei D.; Shepelyansky, Dima L.

2018-03-01

We investigate the dynamics of a two-dimensional electron gas (2DEG) under circular polarized microwave radiation in the presence of dilute localized impurities. Inspired by recent developments on Floquet topological insulators we obtain the Floquet wave functions of this system which allow us to predict the microwave absorption and charge density responses of the electron gas; we demonstrate how these properties can be understood from the underlying semiclassical dynamics even for impurities with a size of around a magnetic length. The charge density response takes the form of a rotating charge density vortex around the impurity that can lead to a significant renormalization of the external microwave field which becomes strongly inhomogeneous on the scale of a cyclotron radius around the impurity. We show that this inhomogeneity can suppress the circular polarization dependence which is theoretically expected for microwave induced resistance oscillations but which was not observed in experiments on semiconducting 2DEGs. Our explanation for this so far unexplained polarization independence has close similarities with the Azbel'-Kaner effect in metals where the interaction length between the microwave field and conduction electrons is much smaller than the cyclotron radius due to skin effect generating harmonics of the cyclotron resonance.

Unbiased reduced density matrices and electronic properties from full configuration interaction quantum Monte Carlo

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

Overy, Catherine; Blunt, N. S.; Shepherd, James J.

2014-12-28

Properties that are necessarily formulated within pure (symmetric) expectation values are difficult to calculate for projector quantum Monte Carlo approaches, but are critical in order to compute many of the important observable properties of electronic systems. Here, we investigate an approach for the sampling of unbiased reduced density matrices within the full configuration interaction quantum Monte Carlo dynamic, which requires only small computational overheads. This is achieved via an independent replica population of walkers in the dynamic, sampled alongside the original population. The resulting reduced density matrices are free from systematic error (beyond those present via constraints on the dynamicmore » itself) and can be used to compute a variety of expectation values and properties, with rapid convergence to an exact limit. A quasi-variational energy estimate derived from these density matrices is proposed as an accurate alternative to the projected estimator for multiconfigurational wavefunctions, while its variational property could potentially lend itself to accurate extrapolation approaches in larger systems.« less

Dynamics of the spatial electron density distribution of EUV-induced plasmas

NASA Astrophysics Data System (ADS)

van der Horst, R. M.; Beckers, J.; Osorio, E. A.; Banine, V. Y.

2015-11-01

We studied the temporal evolution of the electron density distribution in a low pressure pulsed plasma induced by high energy extreme ultraviolet (EUV) photons using microwave cavity resonance spectroscopy (MCRS). In principle, MCRS only provides space averaged information about the electron density. However, we demonstrate here the possibility to obtain spatial information by combining multiple resonant modes. It is shown that EUV-induced plasmas, albeit being a rather exotic plasma, can be explained by known plasma physical laws and processes. Two stages of plasma behaviour are observed: first the electron density distribution contracts, after which it expands. It is shown that the contraction is due to cooling of the electrons. The moment when the density distribution starts to expand is related to the inertia of the ions. After tens of microseconds, the electrons reached the wall of the cavity. The speed of this expansion is dependent on the gas pressure and can be divided into two regimes. It is shown that the acoustic dominated regime the expansion speed is independent of the gas pressure and that in the diffusion dominated regime the expansion depends reciprocal on the gas pressure.

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.

Dynamics and density distributions in a capillary-discharge waveguide with an embedded supersonic jet

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

Matlis, N. H., E-mail: nmatlis@gmail.com; Gonsalves, A. J.; Steinke, S.

We present an analysis of the gas dynamics and density distributions within a capillary-discharge waveguide with an embedded supersonic jet. This device provides a target for a laser plasma accelerator which uses longitudinal structuring of the gas-density profile to enable control of electron trapping and acceleration. The functionality of the device depends sensitively on the details of the density profile, which are determined by the interaction between the pulsed gas in the jet and the continuously-flowing gas in the capillary. These dynamics are captured by spatially resolving recombination light from several emission lines of the plasma as a function ofmore » the delay between the jet and the discharge. We provide a phenomenological description of the gas dynamics as well as a quantitative evaluation of the density evolution. In particular, we show that the pressure difference between the jet and the capillary defines three regimes of operation with qualitatively different longitudinal density profiles and show that jet timing provides a sensitive method for tuning between these regimes.« less

DE 1 observations of type 1 counterstreaming electrons and field-aligned currents

NASA Technical Reports Server (NTRS)

Lin, C. S.; Burch, J. L.; Barfield, J. N.; Sugiura, M.; Nielsen, E.

1984-01-01

Dynamics Explorer 1 satellite observations of plasma and magnetic fields during type one counterstreaming electron events are presented. Counterstreaming electrons are observed at high altitudes in the region of field-aligned current. The total current density computed from the plasma data in the 18-10,000 eV energy range is generally about 1-2 micro-A/sq m. For the downward current, low-energy electrons contribute more than 40 percent of the total plasma current density integrated above 18 eV. For the upward current, such electrons contribute less than 50 percent of that current density. Electron beams in the field-aligned direction are occasionally detected. The pitch angle distributions of counterstreaming electrons are generally enhanced at both small and large pitch angles. STARE simultaneous observations for one DE 1 pass indicated that the field-aligned current was closed through Pedersen currents in the ionosphere. The directions of the ionospheric current systems are consistent with the DE 1 observations at high altitudes.

Nuclear spatial delocalization silences electron density oscillations in 2-phenyl-ethyl-amine (PEA) and 2-phenylethyl-N,N-dimethylamine (PENNA) cations

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

Jenkins, Andrew J.; Vacher, Morgane; Bearpark, Michael J.

2016-03-14

We simulate electron dynamics following ionization in 2-phenyl-ethyl-amine and 2-phenylethyl-N,N-dimethylamine as examples of systems where 3 coupled cationic states are involved. We study two nuclear effects on electron dynamics: (i) coupled electron-nuclear motion and (ii) nuclear spatial delocalization as a result of the zero-point energy in the neutral molecule. Within the Ehrenfest approximation, our calculations show that the coherent electron dynamics in these molecules is not lost as a result of coupled electron-nuclear motion. In contrast, as a result of nuclear spatial delocalization, dephasing of the oscillations occurs on a time scale of only a few fs, long before anymore » significant nuclear motion can occur. The results have been rationalized using a semi-quantitative model based upon the gradients of the potential energy surfaces.« less

Electronic entanglement in late transition metal oxides.

PubMed

Thunström, Patrik; Di Marco, Igor; Eriksson, Olle

2012-11-02

We present a study of the entanglement in the electronic structure of the late transition metal monoxides--MnO, FeO, CoO, and NiO--obtained by means of density-functional theory in the local density approximation combined with dynamical mean-field theory. The impurity problem is solved through exact diagonalization, which grants full access to the thermally mixed many-body ground state density operator. The quality of the electronic structure is affirmed through a direct comparison between the calculated electronic excitation spectrum and photoemission experiments. Our treatment allows for a quantitative investigation of the entanglement in the electronic structure. Two main sources of entanglement are explicitly resolved through the use of a fidelity based geometrical entanglement measure, and additional information is gained from a complementary entropic entanglement measure. We show that the interplay of crystal field effects and Coulomb interaction causes the entanglement in CoO to take a particularly intricate form.

Trajectory-based nonadiabatic dynamics with time-dependent density functional theory.

PubMed

Curchod, Basile F E; Rothlisberger, Ursula; Tavernelli, Ivano

2013-05-10

Understanding the fate of an electronically excited molecule constitutes an important task for theoretical chemistry, and practical implications range from the interpretation of atto- and femtosecond spectroscopy to the development of light-driven molecular machines, the control of photochemical reactions, and the possibility of capturing sunlight energy. However, many challenging conceptual and technical problems are involved in the description of these phenomena such as 1) the failure of the well-known Born-Oppenheimer approximation; 2) the need for accurate electronic properties such as potential energy surfaces, excited nuclear forces, or nonadiabatic coupling terms; and 3) the necessity of describing the dynamics of the photoexcited nuclear wavepacket. This review provides an overview of the current methods to address points 1) and 3) and shows how time-dependent density functional theory (TDDFT) and its linear-response extension can be used for point 2). First, the derivation of Ehrenfest dynamics and nonadiabatic Bohmian dynamics is discussed and linked to Tully's trajectory surface hopping. Second, the coupling of these trajectory-based nonadiabatic schemes with TDDFT is described in detail with special emphasis on the derivation of the required electronic structure properties. Copyright © 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

Quantum wavepacket ab initio molecular dynamics: an approach for computing dynamically averaged vibrational spectra including critical nuclear quantum effects.

PubMed

Sumner, Isaiah; Iyengar, Srinivasan S

2007-10-18

We have introduced a computational methodology to study vibrational spectroscopy in clusters inclusive of critical nuclear quantum effects. This approach is based on the recently developed quantum wavepacket ab initio molecular dynamics method that combines quantum wavepacket dynamics with ab initio molecular dynamics. The computational efficiency of the dynamical procedure is drastically improved (by several orders of magnitude) through the utilization of wavelet-based techniques combined with the previously introduced time-dependent deterministic sampling procedure measure to achieve stable, picosecond length, quantum-classical dynamics of electrons and nuclei in clusters. The dynamical information is employed to construct a novel cumulative flux/velocity correlation function, where the wavepacket flux from the quantized particle is combined with classical nuclear velocities to obtain the vibrational density of states. The approach is demonstrated by computing the vibrational density of states of [Cl-H-Cl]-, inclusive of critical quantum nuclear effects, and our results are in good agreement with experiment. A general hierarchical procedure is also provided, based on electronic structure harmonic frequencies, classical ab initio molecular dynamics, computation of nuclear quantum-mechanical eigenstates, and employing quantum wavepacket ab initio dynamics to understand vibrational spectroscopy in hydrogen-bonded clusters that display large degrees of anharmonicities.

Beyond Point Charges: Dynamic Polarization from Neural Net Predicted Multipole Moments.

PubMed

Darley, Michael G; Handley, Chris M; Popelier, Paul L A

2008-09-09

Intramolecular polarization is the change to the electron density of a given atom upon variation in the positions of the neighboring atoms. We express the electron density in terms of multipole moments. Using glycine and N-methylacetamide (NMA) as pilot systems, we show that neural networks can capture the change in electron density due to polarization. After training, modestly sized neural networks successfully predict the atomic multipole moments from the nuclear positions of all atoms in the molecule. Accurate electrostatic energies between two atoms can be then obtained via a multipole expansion, inclusive of polarization effects. As a result polarization is successfully modeled at short-range and without an explicit polarizability tensor. This approach puts charge transfer and multipolar polarization on a common footing. The polarization procedure is formulated within the context of quantum chemical topology (QCT). Nonbonded atom-atom interactions in glycine cover an energy range of 948 kJ mol(-1), with an average energy difference between true and predicted energy of 0.2 kJ mol(-1), the largest difference being just under 1 kJ mol(-1). Very similar energy differences are found for NMA, which spans a range of 281 kJ mol(-1). The current proof-of-concept enables the construction of a new protein force field that incorporates electron density fragments that dynamically respond to their fluctuating environment.

Modeling light-induced charge transfer dynamics across a metal-molecule-metal junction: Bridging classical electrodynamics and quantum dynamics

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

Hu, Zixuan; Ratner, Mark A.; Seideman, Tamar, E-mail: t-seideman@northwestern.edu

2014-12-14

We develop a numerical approach for simulating light-induced charge transport dynamics across a metal-molecule-metal conductance junction. The finite-difference time-domain method is used to simulate the plasmonic response of the metal structures. The Huygens subgridding technique, as adapted to Lorentz media, is used to bridge the vastly disparate length scales of the plasmonic metal electrodes and the molecular system, maintaining accuracy. The charge and current densities calculated with classical electrodynamics are transformed to an electronic wavefunction, which is then propagated through the molecular linker via the Heisenberg equations of motion. We focus mainly on development of the theory and exemplify ourmore » approach by a numerical illustration of a simple system consisting of two silver cylinders bridged by a three-site molecular linker. The electronic subsystem exhibits fascinating light driven dynamics, wherein the charge density oscillates at the driving optical frequency, exhibiting also the natural system timescales, and a resonance phenomenon leads to strong conductance enhancement.« less

Structural and mechanical properties of cardiolipin lipid bilayers determined using neutron spin echo, small angle neutron and X-ray scattering, and molecular dynamics simulations

DOE PAGES

Pan, Jianjun; Cheng, Xiaolin; Sharp, Melissa; ...

2014-10-29

We report that the detailed structural and mechanical properties of a tetraoleoyl cardiolipin (TOCL) bilayer were determined using neutron spin echo (NSE) spectroscopy, small angle neutron and X-ray scattering (SANS and SAXS, respectively), and molecular dynamics (MD) simulations. We used MD simulations to develop a scattering density profile (SDP) model, which was then utilized to jointly refine SANS and SAXS data. In addition to commonly reported lipid bilayer structural parameters, component distributions were obtained, including the volume probability, electron density and neutron scattering length density.

A dynamic model of the radiation-belt electron phase-space density based on POLAR/HIST measurements

NASA Astrophysics Data System (ADS)

Vassiliadis, D.; Green, J. C.

2007-12-01

The response of the energetic-electron phase-space density (PSD) in the radiation belts is subject to a delicate combination of acceleration and loss processes which are strongly determined by the magnetospheric configuration and field disturbance level. We quantify the response of the density to stormtime fields as observed by the HIST detector on board POLAR. Several distinct modes are identified, characterized by peak second- and third- adiabatic invariants and peak delay time. The modes represent quasiadiabatic transport due to ring current activity; high L* (~6), day-long acceleration linked to ULF wave-particle interaction; and low-L* (~3), minute- to hour-long acceleration interpreted to be due to transient inductive fields or VLF wave-particle interaction. The net transport due to these responses is not always or everywhere diffusive, therefore we quantify the degree of departure from diffusive transport for specific storm intervals and radial ranges. Taken together the response modes comprise a dynamic, nonlinear model which allows us to better understand the historic variability of the high-energy tail of the electron distribution in the inner magnetosphere.

Metalloid Aluminum Clusters with Fluorine

DTIC Science & Technology

2016-12-01

molecular dynamics, binding energy , siesta code, density of states, projected density of states 15. NUMBER OF PAGES 69 16. PRICE CODE 17. SECURITY...high energy density compared to explosives, but typically release this energy slowly via diffusion-limited combustion. There is recent interest in using...examine the cluster binding energy and electronic structure. Partial fluorine substitution in a prototypical aluminum-cyclopentadienyl cluster results

Nodeless vibrational amplitudes and quantum nonadiabatic dynamics in the nested funnel for a pseudo Jahn-Teller molecule or homodimer

NASA Astrophysics Data System (ADS)

Peters, William K.; Tiwari, Vivek; Jonas, David M.

2017-11-01

The nonadiabatic states and dynamics are investigated for a linear vibronic coupling Hamiltonian with a static electronic splitting and weak off-diagonal Jahn-Teller coupling through a single vibration with a vibrational-electronic resonance. With a transformation of the electronic basis, this Hamiltonian is also applicable to the anti-correlated vibration in a symmetric homodimer with marginally strong constant off-diagonal coupling, where the non-adiabatic states and dynamics model electronic excitation energy transfer or self-exchange electron transfer. For parameters modeling a free-base naphthalocyanine, the nonadiabatic couplings are deeply quantum mechanical and depend on wavepacket width; scalar couplings are as important as the derivative couplings that are usually interpreted to depend on vibrational velocity in semiclassical curve crossing or surface hopping theories. A colored visualization scheme that fully characterizes the non-adiabatic states using the exact factorization is developed. The nonadiabatic states in this nested funnel have nodeless vibrational factors with strongly avoided zeroes in their vibrational probability densities. Vibronic dynamics are visualized through the vibrational coordinate dependent density of the time-dependent dipole moment in free induction decay. Vibrational motion is amplified by the nonadiabatic couplings, with asymmetric and anisotropic motions that depend upon the excitation polarization in the molecular frame and can be reversed by a change in polarization. This generates a vibrational quantum beat anisotropy in excess of 2/5. The amplitude of vibrational motion can be larger than that on the uncoupled potentials, and the electronic population transfer is maximized within one vibrational period. Most of these dynamics are missed by the adiabatic approximation, and some electronic and vibrational motions are completely suppressed by the Condon approximation of a coordinate-independent transition dipole between adiabatic states. For all initial conditions investigated, the initial nonadiabatic electronic motion is driven towards the lower adiabatic state, and criteria for this directed motion are discussed.

Nodeless vibrational amplitudes and quantum nonadiabatic dynamics in the nested funnel for a pseudo Jahn-Teller molecule or homodimer.

PubMed

Peters, William K; Tiwari, Vivek; Jonas, David M

2017-11-21

The nonadiabatic states and dynamics are investigated for a linear vibronic coupling Hamiltonian with a static electronic splitting and weak off-diagonal Jahn-Teller coupling through a single vibration with a vibrational-electronic resonance. With a transformation of the electronic basis, this Hamiltonian is also applicable to the anti-correlated vibration in a symmetric homodimer with marginally strong constant off-diagonal coupling, where the non-adiabatic states and dynamics model electronic excitation energy transfer or self-exchange electron transfer. For parameters modeling a free-base naphthalocyanine, the nonadiabatic couplings are deeply quantum mechanical and depend on wavepacket width; scalar couplings are as important as the derivative couplings that are usually interpreted to depend on vibrational velocity in semiclassical curve crossing or surface hopping theories. A colored visualization scheme that fully characterizes the non-adiabatic states using the exact factorization is developed. The nonadiabatic states in this nested funnel have nodeless vibrational factors with strongly avoided zeroes in their vibrational probability densities. Vibronic dynamics are visualized through the vibrational coordinate dependent density of the time-dependent dipole moment in free induction decay. Vibrational motion is amplified by the nonadiabatic couplings, with asymmetric and anisotropic motions that depend upon the excitation polarization in the molecular frame and can be reversed by a change in polarization. This generates a vibrational quantum beat anisotropy in excess of 2/5. The amplitude of vibrational motion can be larger than that on the uncoupled potentials, and the electronic population transfer is maximized within one vibrational period. Most of these dynamics are missed by the adiabatic approximation, and some electronic and vibrational motions are completely suppressed by the Condon approximation of a coordinate-independent transition dipole between adiabatic states. For all initial conditions investigated, the initial nonadiabatic electronic motion is driven towards the lower adiabatic state, and criteria for this directed motion are discussed.

A divide-conquer-recombine algorithmic paradigm for large spatiotemporal quantum molecular dynamics simulations

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

Shimojo, Fuyuki; Hattori, Shinnosuke; Department of Physics, Kumamoto University, Kumamoto 860-8555

We introduce an extension of the divide-and-conquer (DC) algorithmic paradigm called divide-conquer-recombine (DCR) to perform large quantum molecular dynamics (QMD) simulations on massively parallel supercomputers, in which interatomic forces are computed quantum mechanically in the framework of density functional theory (DFT). In DCR, the DC phase constructs globally informed, overlapping local-domain solutions, which in the recombine phase are synthesized into a global solution encompassing large spatiotemporal scales. For the DC phase, we design a lean divide-and-conquer (LDC) DFT algorithm, which significantly reduces the prefactor of the O(N) computational cost for N electrons by applying a density-adaptive boundary condition at themore » peripheries of the DC domains. Our globally scalable and locally efficient solver is based on a hybrid real-reciprocal space approach that combines: (1) a highly scalable real-space multigrid to represent the global charge density; and (2) a numerically efficient plane-wave basis for local electronic wave functions and charge density within each domain. Hybrid space-band decomposition is used to implement the LDC-DFT algorithm on parallel computers. A benchmark test on an IBM Blue Gene/Q computer exhibits an isogranular parallel efficiency of 0.984 on 786 432 cores for a 50.3 × 10{sup 6}-atom SiC system. As a test of production runs, LDC-DFT-based QMD simulation involving 16 661 atoms is performed on the Blue Gene/Q to study on-demand production of hydrogen gas from water using LiAl alloy particles. As an example of the recombine phase, LDC-DFT electronic structures are used as a basis set to describe global photoexcitation dynamics with nonadiabatic QMD (NAQMD) and kinetic Monte Carlo (KMC) methods. The NAQMD simulations are based on the linear response time-dependent density functional theory to describe electronic excited states and a surface-hopping approach to describe transitions between the excited states. A series of techniques are employed for efficiently calculating the long-range exact exchange correction and excited-state forces. The NAQMD trajectories are analyzed to extract the rates of various excitonic processes, which are then used in KMC simulation to study the dynamics of the global exciton flow network. This has allowed the study of large-scale photoexcitation dynamics in 6400-atom amorphous molecular solid, reaching the experimental time scales.« less

Semiclassical dynamics of spin density waves

NASA Astrophysics Data System (ADS)

Chern, Gia-Wei; Barros, Kipton; Wang, Zhentao; Suwa, Hidemaro; Batista, Cristian D.

2018-01-01

We present a theoretical framework for equilibrium and nonequilibrium dynamical simulation of quantum states with spin-density-wave (SDW) order. Within a semiclassical adiabatic approximation that retains electron degrees of freedom, we demonstrate that the SDW order parameter obeys a generalized Landau-Lifshitz equation. With the aid of an enhanced kernel polynomial method, our linear-scaling quantum Landau-Lifshitz dynamics (QLLD) method enables dynamical SDW simulations with N ≃105 lattice sites. Our real-space formulation can be used to compute dynamical responses, such as the dynamical structure factor, of complex and even inhomogeneous SDW configurations at zero or finite temperatures. Applying the QLLD to study the relaxation of a noncoplanar topological SDW under the excitation of a short pulse, we further demonstrate the crucial role of spatial correlations and fluctuations in the SDW dynamics.

Ball lightning dynamics and stability at moderate ion densities

NASA Astrophysics Data System (ADS)

Morrow, R.

2017-10-01

A general mechanism is presented for the dynamics and structure of ball lightning and for the maintenance of the ball lightning structure for several seconds. Results are obtained using a spherical geometry for air at atmospheric pressure, by solving the continuity equations for electrons, positive ions and negative ions coupled with Poisson’s equation. A lightning strike can generate conditions in the lightning channel with a majority of positive nitrogen ions, and a minority of negative oxygen ions and electrons. The calculations are initiated with electrons included; however, at the moderate ion densities chosen the electrons are rapidly lost to form negative ions, and after 1 µs their influence on the ion dynamics is negligible. Further development after 1 µs is followed using a simpler set of equations involving only positive ions and negative ions, but including ion diffusion. The space-charge electric field generated by the majority positive ions drives them from the centre of the distribution and drives the minority negative ions and electrons towards the centre of the distribution. In the central region the positive and negative ion distributions eventually overlap exactly and their space-charge fields cancel resulting in zero electric field, and the plasma ball formed is quite stable for a number of seconds. The formation of such plasma balls is not critically dependent on the initial diameter of the ion distributions, or the initial density of minority negative ions. The ion densities decrease relatively slowly due to mutual neutralization of positive and negative ions. The radiation from this neutralization process involving positive nitrogen ions and negative oxygen ions is not sufficient to account for the reported luminosity of ball lightning and some other source of luminosity is shown to be required; the plasma ball model used could readily incorporate other ions in order to account for the luminosity and range of colours reported for ball lightning. Additionally, ‘phantom plasma balls’ may well be generated and go unnoticed due to very low luminosity; luminous ball lightning may be the exception. Finally, the mechanism described here may also be active in the dynamics of bead lightning.

Unequal density effect on static structure factor of coupled electron layers

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

Saini, L. K., E-mail: lks@ashd.svnit.ac.in; Nayak, Mukesh G., E-mail: lks@ashd.svnit.ac.in

In order to understand the ordered phase, if any, in a real coupled electron layers (CEL), there is a need to take into account the effect of unequal layer density. Such phase is confirmed by a strong peak in a static structure factor. With the aid of quantum/dynamical version of Singwi, Tosi, Land and Sjölander (so-called qSTLS) approximation, we have calculated the intra- and interlayer static structure factors, S{sub ll}(q) and S{sub 12}(q), over a wide range of density parameter r{sub sl} and interlayer spacing d. In our present study, the sharp peak in S{sub 22}(q) has been found atmore » critical density with sufficiently lower interlayer spacing. Further, to find the resultant effect of unequal density on intra- and interlayer static structure factors, we have compared our results with that of the recent CEL system with equal layer density and isolated single electron layer.« less

Electronic coupling through natural amino acids.

PubMed

Berstis, Laura; Beckham, Gregg T; Crowley, Michael F

2015-12-14

Myriad scientific domains concern themselves with biological electron transfer (ET) events that span across vast scales of rate and efficiency through a remarkably fine-tuned integration of amino acid (AA) sequences, electronic structure, dynamics, and environment interactions. Within this intricate scheme, many questions persist as to how proteins modulate electron-tunneling properties. To help elucidate these principles, we develop a model set of peptides representing the common α-helix and β-strand motifs including all natural AAs within implicit protein-environment solvation. Using an effective Hamiltonian strategy with density functional theory, we characterize the electronic coupling through these peptides, furthermore considering side-chain dynamics. For both motifs, predictions consistently show that backbone-mediated electronic coupling is distinctly sensitive to AA type (aliphatic, polar, aromatic, negatively charged and positively charged), and to side-chain orientation. The unique properties of these residues may be employed to design activated, deactivated, or switch-like superexchange pathways. Electronic structure calculations and Green's function analyses indicate that localized shifts in the electron density along the peptide play a role in modulating these pathways, and further substantiate the experimentally observed behavior of proline residues as superbridges. The distinct sensitivities of tunneling pathways to sequence and conformation revealed in this electronic coupling database help improve our fundamental understanding of the broad diversity of ET reactivity and provide guiding principles for peptide design.

Nonlocal and Nonadiabatic Effects in the Charge-Density Response of Solids: A Time-Dependent Density-Functional Approach

NASA Astrophysics Data System (ADS)

Panholzer, Martin; Gatti, Matteo; Reining, Lucia

2018-04-01

The charge-density response of extended materials is usually dominated by the collective oscillation of electrons, the plasmons. Beyond this feature, however, intriguing many-body effects are observed. They cannot be described by one of the most widely used approaches for the calculation of dielectric functions, which is time-dependent density functional theory (TDDFT) in the adiabatic local density approximation (ALDA). Here, we propose an approximation to the TDDFT exchange-correlation kernel which is nonadiabatic and nonlocal. It is extracted from correlated calculations in the homogeneous electron gas, where we have tabulated it for a wide range of wave vectors and frequencies. A simple mean density approximation allows one to use it in inhomogeneous materials where the density varies on a scale of 1.6 rs or faster. This kernel contains effects that are completely absent in the ALDA; in particular, it correctly describes the double plasmon in the dynamic structure factor of sodium, and it shows the characteristic low-energy peak that appears in systems with low electronic density. It also leads to an overall quantitative improvement of spectra.

Nonlocal and Nonadiabatic Effects in the Charge-Density Response of Solids: A Time-Dependent Density-Functional Approach.

PubMed

Panholzer, Martin; Gatti, Matteo; Reining, Lucia

2018-04-20

The charge-density response of extended materials is usually dominated by the collective oscillation of electrons, the plasmons. Beyond this feature, however, intriguing many-body effects are observed. They cannot be described by one of the most widely used approaches for the calculation of dielectric functions, which is time-dependent density functional theory (TDDFT) in the adiabatic local density approximation (ALDA). Here, we propose an approximation to the TDDFT exchange-correlation kernel which is nonadiabatic and nonlocal. It is extracted from correlated calculations in the homogeneous electron gas, where we have tabulated it for a wide range of wave vectors and frequencies. A simple mean density approximation allows one to use it in inhomogeneous materials where the density varies on a scale of 1.6 r_{s} or faster. This kernel contains effects that are completely absent in the ALDA; in particular, it correctly describes the double plasmon in the dynamic structure factor of sodium, and it shows the characteristic low-energy peak that appears in systems with low electronic density. It also leads to an overall quantitative improvement of spectra.

Effect of EMIC Wave Normal Angle Distribution on Relativistic Electron Scattering Based on the Newly Developed Self-consistent RC/EMIC Waves Model by Khazanov et al. [2006

NASA Technical Reports Server (NTRS)

Khazanov, G. V.; Gallagher, D. L.; Gamayunov, K.

2007-01-01

It is well known that the effects of EMIC waves on RC ion and RB electron dynamics strongly depend on such particle/wave characteristics as the phase-space distribution function, frequency, wave-normal angle, wave energy, and the form of wave spectral energy density. Therefore, realistic characteristics of EMIC waves should be properly determined by modeling the RC-EMIC waves evolution self-consistently. Such a selfconsistent model progressively has been developing by Khaznnov et al. [2002-2006]. It solves a system of two coupled kinetic equations: one equation describes the RC ion dynamics and another equation describes the energy density evolution of EMIC waves. Using this model, we present the effectiveness of relativistic electron scattering and compare our results with previous work in this area of research.

Formation Process of Non-Neutral Plasmas by Multiple Electron Beams on BX-U

NASA Astrophysics Data System (ADS)

Sanpei, Akio; Himura, Haruhiko; Masamune, Sadao

An imaging diagnostic system, which is composed of a handmade phosphor screen and a high-speed camera, has been applied to identify the dynamics of multiple electron beams on BX-U. The relaxation process of those toward a non-neutral plasma is experimentally identified. Also, the radial density profile of the plasma is measured as a function of time. Assuming that the plasma is a spheroidal shape, the value of electron density ne is in the range between 2.2 × 106 and 4.4 × 108 cm-3 on BX-U.

Characterizing water-metal interfaces and machine learning potential energy surfaces

NASA Astrophysics Data System (ADS)

Ryczko, Kevin

In this thesis, we first discuss the fundamentals of ab initio electronic structure theory and density functional theory (DFT). We also discuss statistics related to computing thermodynamic averages of molecular dynamics (MD). We then use this theory to analyze and compare the structural, dynamical, and electronic properties of liquid water next to prototypical metals including platinum, graphite, and graphene. Our results are built on Born-Oppenheimer molecular dynamics (BOMD) generated using density functional theory (DFT) which explicitly include van der Waals (vdW) interactions within a first principles approach. All calculations reported use large simulation cells, allowing for an accurate treatment of the water-electrode interfaces. We have included vdW interactions through the use of the optB86b-vdW exchange correlation functional. Comparisons with the Perdew-Burke-Ernzerhof (PBE) exchange correlation functional are also shown. We find an initial peak, due to chemisorption, in the density profile of the liquid water-Pt interface not seen in the liquid water-graphite interface, liquid watergraphene interface, nor interfaces studied previously. To further investigate this chemisorption peak, we also report differences in the electronic structure of single water molecules on both Pt and graphite surfaces. We find that a covalent bond forms between the single water molecule and the platinum surface, but not between the single water molecule and the graphite surface. We also discuss the effects that defects and dopants in the graphite and graphene surfaces have on the structure and dynamics of liquid water. Lastly, we introduce artificial neural networks (ANNs), and demonstrate how they can be used to machine learn electronic structure calculations. As a proof of principle, we show the success of an ANN potential energy surfaces for a dimer molecule with a Lennard-Jones potential.

Low-Dimensional Materials for Optoelectronic and Bioelectronic Applications

NASA Astrophysics Data System (ADS)

Hong, Tu

In this thesis, we first discuss the fundamentals of ab initio electronic structure theory and density functional theory (DFT). We also discuss statistics related to computing thermodynamic averages of molecular dynamics (MD). We then use this theory to analyze and compare the structural, dynamical, and electronic properties of liquid water next to prototypical metals including platinum, graphite, and graphene. Our results are built on Born-Oppenheimer molecular dynamics (BOMD) generated using density functional theory (DFT) which explicitly include van der Waals (vdW) interactions within a first principles approach. All calculations reported use large simulation cells, allowing for an accurate treatment of the water-electrode interfaces. We have included vdW interactions through the use of the optB86b-vdW exchange correlation functional. Comparisons with the Perdew-Burke-Ernzerhof (PBE) exchange correlation functional are also shown. We find an initial peak, due to chemisorption, in the density profile of the liquid water-Pt interface not seen in the liquid water-graphite interface, liquid watergraphene interface, nor interfaces studied previously. To further investigate this chemisorption peak, we also report differences in the electronic structure of single water molecules on both Pt and graphite surfaces. We find that a covalent bond forms between the single water molecule and the platinum surface, but not between the single water molecule and the graphite surface. We also discuss the effects that defects and dopants in the graphite and graphene surfaces have on the structure and dynamics of liquid water. Lastly, we introduce artificial neural networks (ANNs), and demonstrate how they can be used to machine learn electronic structure calculations. As a proof of principle, we show the success of an ANN potential energy surfaces for a dimer molecule with a Lennard-Jones potential.

Ultrafast direct electron transfer at organic semiconductor and metal interfaces.

PubMed

Xiang, Bo; Li, Yingmin; Pham, C Huy; Paesani, Francesco; Xiong, Wei

2017-11-01

The ability to control direct electron transfer can facilitate the development of new molecular electronics, light-harvesting materials, and photocatalysis. However, control of direct electron transfer has been rarely reported, and the molecular conformation-electron dynamics relationships remain unclear. We describe direct electron transfer at buried interfaces between an organic polymer semiconductor film and a gold substrate by observing the first dynamical electric field-induced vibrational sum frequency generation (VSFG). In transient electric field-induced VSFG measurements on this system, we observe dynamical responses (<150 fs) that depend on photon energy and polarization, demonstrating that electrons are directly transferred from the Fermi level of gold to the lowest unoccupied molecular orbital of organic semiconductor. Transient spectra further reveal that, although the interfaces are prepared without deliberate alignment control, a subensemble of surface molecules can adopt conformations for direct electron transfer. Density functional theory calculations support the experimental results and ascribe the observed electron transfer to a flat-lying polymer configuration in which electronic orbitals are found to be delocalized across the interface. The present observation of direct electron transfer at complex interfaces and the insights gained into the relationship between molecular conformations and electron dynamics will have implications for implementing novel direct electron transfer in energy materials.

Electron density and gas density measurements in a millimeter-wave discharge

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

Schaub, S. C., E-mail: sschaub@mit.edu; Hummelt, J. S.; Guss, W. C.

2016-08-15

Electron density and neutral gas density have been measured in a non-equilibrium air breakdown plasma using optical emission spectroscopy and two-dimensional laser interferometry, respectively. A plasma was created with a focused high frequency microwave beam in air. Experiments were run with 110 GHz and 124.5 GHz microwaves at powers up to 1.2 MW. Microwave pulses were 3 μs long at 110 GHz and 2.2 μs long at 124.5 GHz. Electron density was measured over a pressure range of 25 to 700 Torr as the input microwave power was varied. Electron density was found to be close to the critical density, where the collisional plasma frequency is equal tomore » the microwave frequency, over the pressure range studied and to vary weakly with input power. Neutral gas density was measured over a pressure range from 150 to 750 Torr at power levels high above the threshold for initiating breakdown. The two-dimensional structure of the neutral gas density was resolved. Intense, localized heating was found to occur hundreds of nanoseconds after visible plasma formed. This heating led to neutral gas density reductions of greater than 80% where peak plasma densities occurred. Spatial structure and temporal dynamics of gas heating at atmospheric pressure were found to agree well with published numerical simulations.« less

Observations of ionospheric electron beams in the plasma sheet.

PubMed

Zheng, H; Fu, S Y; Zong, Q G; Pu, Z Y; Wang, Y F; Parks, G K

2012-11-16

Electrons streaming along the magnetic field direction are frequently observed in the plasma sheet of Earth's geomagnetic tail. The impact of these field-aligned electrons on the dynamics of the geomagnetic tail is however not well understood. Here we report the first detection of field-aligned electrons with fluxes increasing at ~1 keV forming a "cool" beam just prior to the dissipation of energy in the current sheet. These field-aligned beams at ~15 R(E) in the plasma sheet are nearly identical to those commonly observed at auroral altitudes, suggesting the beams are auroral electrons accelerated upward by electric fields parallel (E([parallel])) to the geomagnetic field. The density of the beams relative to the ambient electron density is δn(b)/n(e)~5-13% and the current carried by the beams is ~10(-8)-10(-7) A m(-2). These beams in high β plasmas with large density and temperature gradients appear to satisfy the Bohm criteria to initiate current driven instabilities.

Plasma dynamics near critical density inferred from direct measurements of laser hole boring

NASA Astrophysics Data System (ADS)

Gong, Chao; Tochitsky, Sergei Ya.; Fiuza, Frederico; Pigeon, Jeremy J.; Joshi, Chan

2016-06-01

We have used multiframe picosecond optical interferometry to make direct measurements of the hole boring velocity, vHB, of the density cavity pushed forward by a train of C O2 laser pulses in a near critical density helium plasma. As the pulse train intensity rises, the increasing radiation pressure of each pulse pushes the density cavity forward and the plasma electrons are strongly heated. After the peak laser intensity, the plasma pressure exerted by the heated electrons strongly impedes the hole boring process and the vHB falls rapidly as the laser pulse intensity falls at the back of the laser pulse train. A heuristic theory is presented that allows the estimation of the plasma electron temperature from the measurements of the hole boring velocity. The measured values of vHB, and the estimated values of the heated electron temperature as a function of laser intensity are in reasonable agreement with those obtained from two-dimensional numerical simulations.

Plasma dynamics near critical density inferred from direct measurements of laser hole boring

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

Gong, Chao; Tochitsky, Sergei Ya.; Fiuza, Frederico

Here, we use multiframe picosecond optical interferometry to make direct measurements of the hole boring velocity, vHB, of the density cavity pushed forward by a train of CO 2 laser pulses in a near critical density helium plasma. As the pulse train intensity rises, the increasing radiation pressure of each pulse pushes the density cavity forward and the plasma electrons are strongly heated. After the peak laser intensity, the plasma pressure exerted by the heated electrons strongly impedes the hole boring process and the vHB falls rapidly as the laser pulse intensity falls at the back of the laser pulsemore » train. We present a heuristic theory that allows the estimation of the plasma electron temperature from the measurements of the hole boring velocity. Furthermore, the measured values of v HB, and the estimated values of the heated electron temperature as a function of laser intensity are in reasonable agreement with those obtained from two-dimensional numerical simulations.« less

The First Results About Earthquake Study with FORMOSAT-3/COSMIC

NASA Astrophysics Data System (ADS)

Liu, J. Y.; Oyama, K.; Jhuang, H. K.; Istep, M.; Hsiao, C. C.; Wang, Y. H.

2007-12-01

To improve the global weather prediction and space weather monitoring, six microsatellites termed the Formosa Satellite 3 - Constellation Observing System for Meteorology, Ionosphere, and Climate (FORMOSAT-3/COSMIC) were launched into a circular low-Earth orbit (LEO) from Vandenberg Air Force Base, California, at 0140 UTC on 15 April 2006. Each microsatellite of the joint Taiwan-US satellite constellation mission has a GPS occultation experiment (GOX) payload to operate the atmospheric and ionospheric radio occultation, a tiny ionospheric photometer (TIP) to observe the nighttime ionospheric airglow OI 135.6 nm emission, and a tri-band beacon (TBB) to tomographically estimate fine structures of ionospheric electron density on the satellite-to-receiver plane. While the GOX daily observes about 2500 vertical electron density profiles up to the satellite altitude, the TIP provides accurate horizontal gradients of nighttime electron density. In this study, anomalies in the ionospheric electron density structure and dynamics concurrently observed by FORMOSAT-3/COSMIC and co-located ground- based GPS receivers before recent large earthquakes are presented and discussed.

Plasma dynamics near critical density inferred from direct measurements of laser hole boring.

PubMed

Gong, Chao; Tochitsky, Sergei Ya; Fiuza, Frederico; Pigeon, Jeremy J; Joshi, Chan

2016-06-01

We have used multiframe picosecond optical interferometry to make direct measurements of the hole boring velocity, v_{HB}, of the density cavity pushed forward by a train of CO_{2} laser pulses in a near critical density helium plasma. As the pulse train intensity rises, the increasing radiation pressure of each pulse pushes the density cavity forward and the plasma electrons are strongly heated. After the peak laser intensity, the plasma pressure exerted by the heated electrons strongly impedes the hole boring process and the v_{HB} falls rapidly as the laser pulse intensity falls at the back of the laser pulse train. A heuristic theory is presented that allows the estimation of the plasma electron temperature from the measurements of the hole boring velocity. The measured values of v_{HB}, and the estimated values of the heated electron temperature as a function of laser intensity are in reasonable agreement with those obtained from two-dimensional numerical simulations.

Plasma dynamics near critical density inferred from direct measurements of laser hole boring

DOE PAGES

Gong, Chao; Tochitsky, Sergei Ya.; Fiuza, Frederico; ...

2017-06-24

Here, we use multiframe picosecond optical interferometry to make direct measurements of the hole boring velocity, vHB, of the density cavity pushed forward by a train of CO 2 laser pulses in a near critical density helium plasma. As the pulse train intensity rises, the increasing radiation pressure of each pulse pushes the density cavity forward and the plasma electrons are strongly heated. After the peak laser intensity, the plasma pressure exerted by the heated electrons strongly impedes the hole boring process and the vHB falls rapidly as the laser pulse intensity falls at the back of the laser pulsemore » train. We present a heuristic theory that allows the estimation of the plasma electron temperature from the measurements of the hole boring velocity. Furthermore, the measured values of v HB, and the estimated values of the heated electron temperature as a function of laser intensity are in reasonable agreement with those obtained from two-dimensional numerical simulations.« less

Fast and stable redox reactions of MnO2/CNT hybrid electrodes for dynamically stretchable pseudocapacitors

NASA Astrophysics Data System (ADS)

Gu, Taoli; Wei, Bingqing

2015-07-01

Pseudocapacitors, which are energy storage devices that take advantage of redox reactions to store electricity, have a different charge storage mechanism compared to lithium-ion batteries (LIBs) and electric double-layer capacitors (EDLCs), and they could realize further gains if they were used as stretchable power sources. The realization of dynamically stretchable pseudocapacitors and understanding of the underlying fundamentals of their mechanical-electrochemical relationship have become indispensable. We report herein the electrochemical performance of dynamically stretchable pseudocapacitors using buckled MnO2/CNT hybrid electrodes. The extremely small relaxation time constant of less than 0.15 s indicates a fast redox reaction at the MnO2/CNT hybrid electrodes, securing a stable electrochemical performance for the dynamically stretchable pseudocapacitors. This finding and the fundamental understanding gained from the pseudo-capacitive behavior coupled with mechanical deformation under a dynamic stretching mode would provide guidance to further improve their overall performance including a higher power density than LIBs, a higher energy density than EDLCs, and a long-life cycling stability. Most importantly, these results will potentially accelerate the applications of stretchable pseudocapacitors for flexible and biomedical electronics.Pseudocapacitors, which are energy storage devices that take advantage of redox reactions to store electricity, have a different charge storage mechanism compared to lithium-ion batteries (LIBs) and electric double-layer capacitors (EDLCs), and they could realize further gains if they were used as stretchable power sources. The realization of dynamically stretchable pseudocapacitors and understanding of the underlying fundamentals of their mechanical-electrochemical relationship have become indispensable. We report herein the electrochemical performance of dynamically stretchable pseudocapacitors using buckled MnO2/CNT hybrid electrodes. The extremely small relaxation time constant of less than 0.15 s indicates a fast redox reaction at the MnO2/CNT hybrid electrodes, securing a stable electrochemical performance for the dynamically stretchable pseudocapacitors. This finding and the fundamental understanding gained from the pseudo-capacitive behavior coupled with mechanical deformation under a dynamic stretching mode would provide guidance to further improve their overall performance including a higher power density than LIBs, a higher energy density than EDLCs, and a long-life cycling stability. Most importantly, these results will potentially accelerate the applications of stretchable pseudocapacitors for flexible and biomedical electronics. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr02310f

Evolution of Field-Aligned Electron and Ion Densities From Whistler Mode Radio Soundings During Quiet to Moderately Active Period and Comparisons With SAMI2 Simulations

NASA Astrophysics Data System (ADS)

Reddy, A.; Sonwalkar, V. S.; Huba, J. D.

2018-02-01

Knowledge of field-aligned electron and ion distributions is necessary for understanding the physical processes causing variations in field-aligned electron and ion densities. Using whistler mode sounding by Radio Plasma Imager/Imager for Magnetopause-to-Aurora Global Exploration (RPI/IMAGE), we determined the evolution of dayside electron and ion densities along L ˜ 2 and L ˜ 3 (90-4,000 km) during a 7 day (21-27 November 2005) geomagnetically quiet to moderately active period. Over this period the O+/H+ transition height was ˜880 ± 60 km and ˜1000 ± 100 km, respectively, at L ˜ 2 and L ˜ 3. The electron density varied in a complex manner; it was different at L ˜ 2 and L ˜ 3 and below and above the O+/H+ transition height. The measured electron and ion densities are consistent with those from Challenging Minisatellite Payload (CHAMP) and Defense Meteorological Satellite Program (DMSP) and other past measurements, but they deviated from bottomside sounding and International Reference Ionosphere (IRI) 2012 empirical model results. Using SAMI2 (Naval Research Laboratory (NRL) ionosphere model) with reasonably adjusted values of inputs (neutral densities, winds, electric fields, and photoelectron heating), we simulated the evolution of O+/H+ transition height and field-aligned electron and ion densities so that a fair agreement was obtained between the simulation results and observations. Simulation studies indicated that reduced neutral densities (H and/or O) with time limited O+-H charge exchange process. This reduction in neutral densities combined with changes in neutral winds and plasma temperature led to the observed variations in the electron and ion densities. The observation/simulation method presented here can be extended to investigate the role of neutral densities and composition, disturbed winds, and prompt penetration electric fields in the storm time ionosphere/plasmasphere dynamics.

Influence of Plasma Unsteadiness on the Spectrum and Shape of Microwave Pulses in a Plasma Relativistic Microwave Amplifier

NASA Astrophysics Data System (ADS)

Kartashov, I. N.; Kuzelev, M. V.; Strelkov, P. S.; Tarakanov, V. P.

2018-02-01

Dependence of the shape of a microwave pulse in a plasma relativistic microwave amplifier (PRMA) on the initial plasma electron density in the system is detected experimentally. Depending on the plasma density, fast disruption of amplification, stable operation of the amplifier during the relativistic electron beam (REB) pulse, and its delayed actuation can take place. A reduction in the output signal frequency relative to the input frequency is observed experimentally. The change in the shape of the microwave signal and the reduction in its frequency are explained by a decrease in the plasma density in the system. The dynamics of the plasma density during the REB pulse is determined qualitatively from the experimental data by using the linear theory of a PRMA with a thin-wall hollow electron beam. The processes in a PRMA are analyzed by means of the KARAT particle-in-cell code. It is shown that REB injection is accompanied by an increase in the mean energy of plasma electrons and a significant decrease in their density.

Semiconductors Under Ion Radiation: Ultrafast Electron-Ion Dynamics in Perfect Crystals and the Effect of Defects

NASA Astrophysics Data System (ADS)

Lee, Cheng-Wei; Schleife, André

Stability and safety issues have been challenging difficulties for materials and devices under radiation such as solar panels in outer space. On the other hand, radiation can be utilized to modify materials and increase their performance via focused-ion beam patterning at nano-scale. In order to grasp the underlying processes, further understanding of the radiation-material and radiation-defect interactions is required and inevitably involves the electron-ion dynamics that was traditionally hard to capture. By applying Ehrenfest dynamics based on time-dependent density functional theory, we have been able to perform real-time simulation of electron-ion dynamics in MgO and InP/GaP. By simulating a high-energy proton penetrating the material, the energy gain of electronic system can be interpreted as electronic stopping power and the result is compared to existing data. We also study electronic stopping in the vicinity of defects: for both oxygen vacancy in MgO and interface of InP/GaP superlattice, electronic stopping shows strong dependence on the velocity of the proton. To study the energy transfer from electronic system to lattice, simulations of about 100 femto-seconds are performed and we analyze the difference between Ehrenfest and Born-Oppenheimer molecular dynamics.

Self-amplified photo-induced gap quenching in a correlated electron material

PubMed Central

Mathias, S.; Eich, S.; Urbancic, J.; Michael, S.; Carr, A. V.; Emmerich, S.; Stange, A.; Popmintchev, T.; Rohwer, T.; Wiesenmayer, M.; Ruffing, A.; Jakobs, S.; Hellmann, S.; Matyba, P.; Chen, C.; Kipp, L.; Bauer, M.; Kapteyn, H. C.; Schneider, H. C.; Rossnagel, K.; Murnane, M. M.; Aeschlimann, M.

2016-01-01

Capturing the dynamic electronic band structure of a correlated material presents a powerful capability for uncovering the complex couplings between the electronic and structural degrees of freedom. When combined with ultrafast laser excitation, new phases of matter can result, since far-from-equilibrium excited states are instantaneously populated. Here, we elucidate a general relation between ultrafast non-equilibrium electron dynamics and the size of the characteristic energy gap in a correlated electron material. We show that carrier multiplication via impact ionization can be one of the most important processes in a gapped material, and that the speed of carrier multiplication critically depends on the size of the energy gap. In the case of the charge-density wave material 1T-TiSe2, our data indicate that carrier multiplication and gap dynamics mutually amplify each other, which explains—on a microscopic level—the extremely fast response of this material to ultrafast optical excitation. PMID:27698341

Lewis Base Passivation of Hybrid Halide Perovskites Slows Electron-Hole Recombination: Time-Domain Ab Initio Analysis.

PubMed

Liu, Lihong; Fang, Wei-Hai; Long, Run; Prezhdo, Oleg V

2018-03-01

Nonradiative electron-hole recombination plays a key role in determining photon conversion efficiencies in solar cells. Experiments demonstrate significant reduction in the recombination rate upon passivation of methylammonium lead iodide perovskite with Lewis base molecules. Using nonadiabatic molecular dynamics combined with time-domain density functional theory, we find that the nonradiative charge recombination is decelerated by an order of magnitude upon adsorption of the molecules. Thiophene acts by the traditional passivation mechanism, forcing electron density away from the surface. In contrast, pyridine localizes the electron at the surface while leaving it energetically near the conduction band edge. This is because pyridine creates a stronger coordinative bond with a lead atom of the perovskite and has a lower energy unoccupied orbital compared with thiophene due to the more electronegative nitrogen atom relative to thiophene's sulfur. Both molecules reduce two-fold the nonadiabatic coupling and electronic coherence time. A broad range of vibrational modes couple to the electronic subsystem, arising from inorganic and organic components. The simulations reveal the atomistic mechanisms underlying the enhancement of the excited-state lifetime achieved by the perovskite passivation, rationalize the experimental results, and advance our understanding of charge-phonon dynamics in perovskite solar cells.

Linking the micro and macro: L-H transition dynamics and threshold physics

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

Malkov, M. A., E-mail: mmalkov@ucsd.edu; Diamond, P. H.; Miki, K.

2015-03-15

The links between the microscopic dynamics and macroscopic threshold physics of the L → H transition are elucidated. Emphasis is placed on understanding the physics of power threshold scalings, and especially on understanding the minimum in the power threshold as a function of density P{sub thr} (n). By extending a numerical 1D model to evolve both electron and ion temperatures, including collisional coupling, we find that the decrease in P{sub thr} (n) along the low-density branch is due to the combination of an increase in collisional electron-to-ion energy transfer and an increase in the heating fraction coupled to the ions.more » Both processes strengthen the edge diamagnetic electric field needed to lock in the mean electric field shear for the L→H transition. The increase in P{sub thr} (n) along the high-density branch is due to the increase with ion collisionality of damping of turbulence-driven shear flows. Turbulence driven shear flows are needed to trigger the transition by extracting energy from the turbulence. Thus, we identify the critical transition physics components of the separatrix ion heat flux and the zonal flow excitation. The model reveals a power threshold minimum in density scans as a crossover between the threshold decrease supported by an increase in heat fraction received by ions (directly or indirectly, from electrons) and a threshold increase, supported by the rise in shear flow damping. The electron/ion heating mix emerges as important to the transition, in that it, together with electron-ion coupling, regulates the edge diamagnetic electric field shear. The importance of possible collisionless electron-ion heat transfer processes is explained.« less

Ab initio molecular dynamics with nuclear quantum effects at classical cost: Ring polymer contraction for density functional theory.

PubMed

Marsalek, Ondrej; Markland, Thomas E

2016-02-07

Path integral molecular dynamics simulations, combined with an ab initio evaluation of interactions using electronic structure theory, incorporate the quantum mechanical nature of both the electrons and nuclei, which are essential to accurately describe systems containing light nuclei. However, path integral simulations have traditionally required a computational cost around two orders of magnitude greater than treating the nuclei classically, making them prohibitively costly for most applications. Here we show that the cost of path integral simulations can be dramatically reduced by extending our ring polymer contraction approach to ab initio molecular dynamics simulations. By using density functional tight binding as a reference system, we show that our ring polymer contraction scheme gives rapid and systematic convergence to the full path integral density functional theory result. We demonstrate the efficiency of this approach in ab initio simulations of liquid water and the reactive protonated and deprotonated water dimer systems. We find that the vast majority of the nuclear quantum effects are accurately captured using contraction to just the ring polymer centroid, which requires the same number of density functional theory calculations as a classical simulation. Combined with a multiple time step scheme using the same reference system, which allows the time step to be increased, this approach is as fast as a typical classical ab initio molecular dynamics simulation and 35× faster than a full path integral calculation, while still exactly including the quantum sampling of nuclei. This development thus offers a route to routinely include nuclear quantum effects in ab initio molecular dynamics simulations at negligible computational cost.

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.

Dynamics of Different Bacterial Communities Are Capable of Generating Sustainable Electricity from Microbial Fuel Cells with Organic Waste

PubMed Central

Yamamoto, Shuji; Suzuki, Kei; Araki, Yoko; Mochihara, Hiroki; Hosokawa, Tetsuya; Kubota, Hiroko; Chiba, Yusuke; Rubaba, Owen; Tashiro, Yosuke; Futamata, Hiroyuki

2014-01-01

The relationship between the bacterial communities in anolyte and anode biofilms and the electrochemical properties of microbial fuel cells (MFCs) was investigated when a complex organic waste-decomposing solution was continuously supplied to MFCs as an electron donor. The current density increased gradually and was maintained at approximately 100 to 150 mA m−2. Polarization curve analyses revealed that the maximum power density was 7.4 W m−3 with an internal resistance of 110 Ω. Bacterial community structures in the organic waste-decomposing solution and MFCs differed from each other. Clonal analyses targeting 16S rRNA genes indicated that bacterial communities in the biofilms on MFCs developed to specific communities dominated by novel Geobacter. Multidimensional scaling analyses based on DGGE profiles revealed that bacterial communities in the organic waste-decomposing solution fluctuated and had no dynamic equilibrium. Bacterial communities on the anolyte in MFCs had a dynamic equilibrium with fluctuations, while those of the biofilm converged to the Geobacter-dominated structure. These bacterial community dynamics of MFCs differed from those of control-MFCs under open circuit conditions. These results suggested that bacterial communities in the anolyte and biofilm have a gentle symbiotic system through electron flow, which resulted in the advance of current density from complex organic waste. PMID:24789988

Dynamics of different bacterial communities are capable of generating sustainable electricity from microbial fuel cells with organic waste.

PubMed

Yamamoto, Shuji; Suzuki, Kei; Araki, Yoko; Mochihara, Hiroki; Hosokawa, Tetsuya; Kubota, Hiroko; Chiba, Yusuke; Rubaba, Owen; Tashiro, Yosuke; Futamata, Hiroyuki

2014-01-01

The relationship between the bacterial communities in anolyte and anode biofilms and the electrochemical properties of microbial fuel cells (MFCs) was investigated when a complex organic waste-decomposing solution was continuously supplied to MFCs as an electron donor. The current density increased gradually and was maintained at approximately 100 to 150 mA m(-2). Polarization curve analyses revealed that the maximum power density was 7.4 W m(-3) with an internal resistance of 110 Ω. Bacterial community structures in the organic waste-decomposing solution and MFCs differed from each other. Clonal analyses targeting 16S rRNA genes indicated that bacterial communities in the biofilms on MFCs developed to specific communities dominated by novel Geobacter. Multidimensional scaling analyses based on DGGE profiles revealed that bacterial communities in the organic waste-decomposing solution fluctuated and had no dynamic equilibrium. Bacterial communities on the anolyte in MFCs had a dynamic equilibrium with fluctuations, while those of the biofilm converged to the Geobacter-dominated structure. These bacterial community dynamics of MFCs differed from those of control-MFCs under open circuit conditions. These results suggested that bacterial communities in the anolyte and biofilm have a gentle symbiotic system through electron flow, which resulted in the advance of current density from complex organic waste.

TIME-DEPENDENT DENSITY DIAGNOSTICS OF SOLAR FLARE PLASMAS USING SDO/EVE

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

Milligan, Ryan O.; Kennedy, Michael B.; Mathioudakis, Mihalis

2012-08-10

Temporally resolved electron density measurements of solar flare plasmas are presented using data from the EUV Variability Experiment (EVE) on board the Solar Dynamics Observatory. The EVE spectral range contains emission lines formed between 10{sup 4} and 10{sup 7} K, including transitions from highly ionized iron ({approx}>10 MK). Using three density-sensitive Fe XXI ratios, peak electron densities of 10{sup 11.2}-10{sup 12.1} cm{sup -3} were found during four X-class flares. While previous measurements of densities at such high temperatures were made at only one point during a flaring event, EVE now allows the temporal evolution of these high-temperature densities to bemore » determined at 10 s cadence. A comparison with GOES data revealed that the peak of the density time profiles for each line ratio correlated well with that of the emission measure time profile for each of the events studied.« less

Recombination dynamics of optically excited charge carriers in bulk MoS2

NASA Astrophysics Data System (ADS)

Völzer, Tim; Lütgens, Matthias; Fennel, Franziska; Lochbrunner, Stefan

2017-10-01

Transition metal dichalcogenides (TMDCs), such as MoS2, are promising candidates for optoelectronic or catalytic applications. On that account, a detailed characterization of the electronic dynamics in these materials is of pivotal importance. Here, we investigate the temporal evolution of an excited carrier population by all-optical pump-probe spectroscopy. On the sub-picosecond time scale we observe thermal relaxation of the excited carriers by electron-phonon coupling. The dynamics on the nanosecond time scale can be understood in terms of defect-assisted Auger recombination over a broad carrier density regime spanning more than one order of magnitude. Hence, our results emphasize the importance of defect states for electronic processes in TMDCs at room temperature.

Electron and ion dynamics study of iron in warm dense matter regime by time-resolved XAS measurements and from first-principles

NASA Astrophysics Data System (ADS)

Ogitsu, T.; Fernandez-Paãella, A.; Correa, A.; Engelhorn, K.; Barbrel, B.; Prendergast, D. G.; Pemmaraju, D.; Beckwith, M.; Kraus, D.; Hamel, S.; Cho, B. I.; Jin, L.; Wong, J.; Heinman, P.; Collins, G. W.; Falcone, R.; Ping, Y.

2016-10-01

We present a study of the electron-phonon coupling of warm dense iron upon femtosecond laser excitation by time-resolved x-ray absorption near edge spectroscopy (XANES). The dynamics of iron in electron-ion non-equilibrium conditions was studied using ab-initio density-functional-theory (DFT) simulations combined with the Two Temperature Model (TTM) where spatial inhomogeneity of electron (and ion) temperature(s) due to short ballistic electron transport length in iron was explicitly taken into consideration. Detailed comparison between our simulation results and experiments indicates that the ion temperature dependence on specific heat and on electron-phonon coupling also plays a relevant role in modeling the relaxation dynamics of electrons and ions. These results are the first experimental evidence of the suppression of the electron-phonon coupling factor of a transition metal at electron temperatures ranging 5000- 10000 K. This work was performed under DOE contract DE-AC52-07NA27344 with support from OFES Early Career program and LLNL LDRD program.

Investigation of the Electron Acceleration by a High-Power Laser and a Density-Tapered Mixed-Gas Cell

NASA Astrophysics Data System (ADS)

Kim, Jinju; Phung, Vanessa L. J.; Kim, Minseok; Hur, Min-Sup; Suk, Hyyong

2017-10-01

Plasma-based accelerators can generate about 1000 times stronger acceleration field compared with RF-based conventional accelerators, which can be done by high power laser and plasma. There are many issues in this research and one of them is development of a good plasma source for higher electron beam energy. For this purpose, we are investigating a special type of plasma source, which is a density-tapered gas cell with a mixed-gas for easy injection. By this type of special gas cell, we expect higher electron beam energies with easy injection in the wakefield. In this poster, some experimental results for electron beam generation with the density-tapered mixed-gas cell are presented. In addition to the experimental results, CFD (Computational-Fluid-Dynamics) and PIC (Particle-In-Cell) simulation results are also presented for comparison studies.

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

PubMed

Lee, Mi Kyung; Coker, David F

2016-08-18

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

High-latitude electron density observations from the IMAGE radio plasma imager

NASA Astrophysics Data System (ADS)

Henize, Vance Karl

2003-11-01

Before the IMAGE mission, electron densities in the high latitude, high altitude region of the magnetosphere were measured exclusively by in situ means. The Radio Plasma Imager instrument onboard IMAGE is capable of remotely observing electron densities between 0.01 and 100,000 e-/cm-3 from distances of several Earth radii or more. This allows a global view of the high latitude region that has a far greater accuracy than was previously possible. Soundings of the terrestrial magnetic cusp provide the first remote observations of the dynamics and poleward density profile of this feature continuously over a 60- minute interval. During steady quiet-time solar wind and interplanetary magnetic field conditions, the cusp is shown to be stable in both position and density structure with only slight variations in both. Peak electron densities within the cusp during this time are found to be somewhat higher than predicted. New procedures for deriving electron densities from radio sounding measurements are developed. The addition of curve fitting algorithms significantly increases the amount of useable data. Incorporating forward modeling techniques greatly reduces the computational time over traditional inversion methods. These methods are described in detail. A large number high latitude observations of ducted right-hand extraordinary mode waves made over the course of one year of the IMAGE mission are used to create a three dimensional model of the electron density profile of the terrestrial polar cap region. The dependence of electron density in the polar cap on average geocentric distance (d) is found to vary as d-6.6. This is a significantly steeper gradient than cited in earlier works such as Persoon et al., although the introduction of an asymptotic term provides for basic agreement in the limited region of their joint validity. Latitudinal and longitudinal variations are found to be insignificant. Both the mean profile power law index of the electron density profile and, to a stronger degree, its variance show dependence with the DST index.

Electron quantum dynamics in atom-ion interaction

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

Sabzyan, H., E-mail: sabzyan@sci.ui.ac.ir; Jenabi, M. J.

2016-04-07

Electron transfer (ET) process and its dependence on the system parameters are investigated by solving two-dimensional time-dependent Schrödinger equation numerically using split operator technique. Evolution of the electron wavepacket occurs from the one-electron species hydrogen atom to another bare nucleus of charge Z > 1. This evolution is quantified by partitioning the simulation box and defining regional densities belonging to the two nuclei of the system. It is found that the functional form of the time-variations of these regional densities and the extent of ET process depend strongly on the inter-nuclear distance and relative values of the nuclear charges, whichmore » define the potential energy surface governing the electron wavepacket evolution. Also, the initial electronic state of the single-electron atom has critical effect on this evolution and its consequent (partial) electron transfer depending on its spreading extent and orientation with respect to the inter-nuclear axis.« less

Watching excitons move: the time-dependent transition density matrix

NASA Astrophysics Data System (ADS)

Ullrich, Carsten

2012-02-01

Time-dependent density-functional theory allows one to calculate excitation energies and the associated transition densities in principle exactly. The transition density matrix (TDM) provides additional information on electron-hole localization and coherence of specific excitations of the many-body system. We have extended the TDM concept into the real-time domain in order to visualize the excited-state dynamics in conjugated molecules. The time-dependent TDM is defined as an implicit density functional, and can be approximately obtained from the time-dependent Kohn-Sham orbitals. The quality of this approximation is assessed in simple model systems. A computational scheme for real molecular systems is presented: the time-dependent Kohn-Sham equations are solved with the OCTOPUS code and the time-dependent Kohn-Sham TDM is calculated using a spatial partitioning scheme. The method is applied to show in real time how locally created electron-hole pairs spread out over neighboring conjugated molecular chains. The coupling mechanism, electron-hole coherence, and the possibility of charge separation are discussed.

Nonlinear dynamics of electromagnetic turbulence in a nonuniform magnetized plasma

NASA Astrophysics Data System (ADS)

Shukla, P. K.; Mirza, Arshad M.; Faria, R. T.

1998-03-01

By using the hydrodynamic electron response with fixed (kinetic) ions along with Poisson's equation as well as Ampère's law, a system of nonlinear equations for low-frequency (in comparison with the electron gyrofrequency) long-(short-) wavelength electromagnetic waves in a nonuniform resistive magnetoplasma has been derived. The plasma contains equilibrium density gradient and sheared equilibrium plasma flows. In the linear limit, local dispersion relations are obtained and analyzed. It is found that sheared equilibrium flows can cause instability of Alfvén-like electromagnetic waves even in the absence of a density gradient. Furthermore, it is shown that possible stationary solutions of the nonlinear equations without dissipation can be represented in the form of various types of vortices. On the other hand, the temporal behavior of our nonlinear dissipative systems without the equilibrium density inhomogeneity can be described by the generalized Lorenz equations which admit chaotic trajectories. The density inhomogeneity may lead to even qualitative changes in the chaotic dynamics. The results of our investigation should be useful in understanding the linear and nonlinear properties of nonthermal electromagnetic waves in space and laboratory plasmas.

Laser-driven relativistic electron dynamics in a cylindrical plasma channel

NASA Astrophysics Data System (ADS)

Geng, Pan-Fei; Lv, Wen-Juan; Li, Xiao-Liang; Tang, Rong-An; Xue, Ju-Kui

2018-03-01

The energy and trajectory of the electron, which is irradiated by a high-power laser pulse in a cylindrical plasma channel with a uniform positive charge and a uniform negative current, have been analyzed in terms of a single-electron model of direct laser acceleration. We find that the energy and trajectory of the electron strongly depend on the positive charge density, the negative current density, and the intensity of the laser pulse. The electron can be accelerated significantly only when the positive charge density, the negative current density, and the intensity of the laser pulse are in suitable ranges due to the dephasing rate between the wave and electron motion. Particularly, when their values satisfy a critical condition, the electron can stay in phase with the laser and gain the largest energy from the laser. With the enhancement of the electron energy, strong modulations of the relativistic factor cause a considerable enhancement of the electron transverse oscillations across the channel, which makes the electron trajectory become essentially three-dimensional, even if it is flat at the early stage of the acceleration. Project supported by the National Natural Science Foundation of China (Grant Nos. 11475027, 11765017, 11764039, 11305132, and 11274255), the Natural Science Foundation of Gansu Province, China (Grant No. 17JR5RA076), and the Scientific Research Project of Gansu Higher Education, China (Grant No. 2016A-005).

Exchange and correlation effects on plasmon dispersions and Coulomb drag in low-density electron bilayers

NASA Astrophysics Data System (ADS)

Badalyan, S. M.; Kim, C. S.; Vignale, G.; Senatore, G.

2007-03-01

We investigate the effect of exchange and correlation (XC) on the plasmon spectrum and the Coulomb drag between spatially separated low-density two-dimensional electron layers. We adopt a different approach, which employs dynamic XC kernels in the calculation of the bilayer plasmon spectra and of the plasmon-mediated drag, and static many-body local field factors in the calculation of the particle-hole contribution to the drag. The spectrum of bilayer plasmons and the drag resistivity are calculated in a broad range of temperatures taking into account both intra- and interlayer correlation effects. We observe that both plasmon modes are strongly affected by XC corrections. After the inclusion of the complex dynamic XC kernels, a decrease of the electron density induces shifts of the plasmon branches in opposite directions. This is in stark contrast with the tendency observed within random phase approximation that both optical and acoustical plasmons move away from the boundary of the particle-hole continuum with a decrease in the electron density. We find that the introduction of XC corrections results in a significant enhancement of the transresistivity and qualitative changes in its temperature dependence. In particular, the large high-temperature plasmon peak that is present in the random phase approximation is found to disappear when the XC corrections are included. Our numerical results at low temperatures are in good agreement with the results of recent experiments by Kellogg [Solid State Commun. 123, 515 (2002)].

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

A Density Functional Approach to Polarizable Models: A Kim-Gordon-Response Density Interaction Potential for Molecular Simulations

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

Tabacchi, G; Hutter, J; Mundy, C

2005-04-07

A combined linear response--frozen electron density model has been implemented in a molecular dynamics scheme derived from an extended Lagrangian formalism. This approach is based on a partition of the electronic charge distribution into a frozen region described by Kim-Gordon theory, and a response contribution determined by the instaneous ionic configuration of the system. The method is free from empirical pair-potentials and the parameterization protocol involves only calculations on properly chosen subsystems. They apply this method to a series of alkali halides in different physical phases and are able to reproduce experimental structural and thermodynamic properties with an accuracy comparablemore » to Kohn-Sham density functional calculations.« less

The electrons and ion characteristics of Saturn's plasma disk inside the Enceladus orbit

NASA Astrophysics Data System (ADS)

Morooka, Michiko; Wahlund, Jan-Erik; Ye, Sheng-Yi; Kurth, William; Persoon, Ann; Holmberg, Mika

2017-04-01

Cassini observations revealed that Saturn's icy moon Enceladus and surrounding E ring are the significant plasma source of the magnetosphere. However, the observations sometimes show the electron density enhancement even inside the Enceladus orbiting distance, 4RS. Further plasma contribution from the inner rings, the G and the F rings and main A ring are the natural candidate as an additional plasma source. The Cassini/RPWS Langmuir Probe (LP) measurement provides the characteristics of the electrons and ions independently in a cold dense plasma. The observations near the center of the E ring showed that the ion density being larger than the electron density, indicating that there is additional particle as a negative charge carrier. Those are the small nm and μm sized dust grains that are negatively charged by the electron attachments. The faint F and G rings, located at R=2RS and 3RS, consist of small grains and similar electron/ion density discrepancies can be expected. We will show different types of the LP observations when Cassini traveled the equator region of the plasma disk down to 3RS. One with the electron density increasing inside 4RS, and another with the electron density decreasing inside 4RS. During the orbit 016 (2005 doy-284/285), the electron density continued to increase toward the planet. On the other hand, the ion currents, the LP measured currents from the negative bias voltage, turn to decreasing inside 4RS, implying the density decrease of the ions. By comparing the observed LP ion current characteristics and the modeled values using the obtained electron density, we found that the characteristic ion mass can be several times larger than the water ions (AMU=18) that we expected in this region. During the orbit 015 (2005 doy-266/267), on the other hand, the LP observed sharp electron density drop near 3RS. The dust signals from the RPWS antenna showed the density enhancement of the μm sized grains coincide the electron density drop and we have estimated that the characteristic ion mass can exceed AMU=100. Throughout the whole Cassini observation near the equator inside 4RS, we didn't find the case with the ion densities larger than the electron densities as were found near the E ring and the Enceladus plume. We suggest that Saturn's plasmadisk inside the Enceladus orbit is dynamic in ion characteristics where the water molecules coagulate and grow into a small icy dust grains. In the presentation we discuss the relationship between the electron/ion density and the density of the nm and μm sized grains.

The Relationship between Ionospheric Slab Thickness and the Peak Density Height, hmF2

NASA Astrophysics Data System (ADS)

Meehan, J.; Sojka, J. J.

2017-12-01

The electron density profile is one of the most critical elements in the ionospheric modeling-related applications today. Ionosphere parameters, hmF2, the height of the peak density layer, and slab thickness, the ratio of the total electron content, TEC, to the peak density value, NmF2, are generally obtained from any global sounding observation network and are easily incorporated into models, theoretical or empirical, as numerical representations. Slab thickness is a convenient one-parameter summary of the electron density profile and can relate a variety of elements of interest that effect the overall electron profile shape, such as the neutral and ionospheric temperatures and gradients, the ionospheric composition, and dynamics. Using ISR data from the 2002 Millstone Hill ISR data campaign, we found, for the first time, slab thickness to be correlated to hmF2. For this, we introduce a new ionospheric index, k, which ultimately relates electron density parameters and can be a very useful tool for describing the topside ionosphere shape. Our study is an initial one location, one season, 30-day study, and future work is needed to verify the robustness of our claim. Generally, the ionospheric profile shape, requires knowledge of several ionospheric parameters: electron, ion and neutral temperatures, ion composition, electric fields, and neutral winds, and is dependent upon seasons, local time, location, and the level of solar and geomagnetic activity; however, with this new index, only readily-available, ionospheric density information is needed. Such information, as used in this study, is obtained from a bottomside electron density profile provided by an ionosonde, and TEC data provided by a local, collocated GPS receiver.

Modeling dynamic plasmas driven by ultraintense nano-focused x-ray laser pulses in solid iron targets

NASA Astrophysics Data System (ADS)

Royle, Ryan; Sentoku, Yasuhiko; Mancini, Roberto

2017-10-01

The hard x-ray free electron laser has proven to be a valuable tool for high energy density (HED) physics as it is able to produce well-characterized samples of HED matter at exactly solid density and homogeneous temperatures. However, if the x-ray pulses are focused to sub-micron spot sizes, where peak intensities can exceed 1020 W/cm2, the plasmas driven by sources of non-thermal photoelectrons and Auger electrons can be highly dynamic and so cannot be modeled by atomic kinetics or fluid codes. We apply the 2D/3D particle-in-cell code, PICLS-which has been extended with numerous physics models to enable the simulation of XFEL-driven plasmas-to the modeling of such dynamic plasmas driven by nano-focused XFEL pulses in solid iron targets. In the case of the smallest focal spot investigated of just 100 nm in diameter, keV plasmas induce strong radial E-fields that accelerate keV ions radially as well as sheath fields that accelerate surface ions to hundreds of keV. The heated spot, which is initially larger than the laser spot due to the kinetic nature of the fast Auger electrons, expands as ion and electron waves propagate radially, leaving a low density region along the laser axis. This research was supported by the US DOE-OFES under Grant No. DE-SC0008827, the DOE-NNSA under Grant No. DE-NA0002075, and the JSPS KAKENHI under Grant No. JP15K21767.

Electronic properties of liquid Hg-In alloys : Ab-initio molecular dynamics study

NASA Astrophysics Data System (ADS)

Sharma, Nalini; Thakur, Anil; Ahluwalia, P. K.

2016-05-01

Ab-initio molecular dynamics simulations are performed to study the structural properties of liquid Hg-In alloys. The interatomic interactions are described by ab-initio pseudopotentials given by Troullier and Martins. Three liquid Hg-In alloys (Hg10In90, Hg30In70,. Hg50In50, Hg70In30, and Hg90Pb10) at 299 K are considered. The calculated results for liquid Hg (l-Hg) and lead (l-In) are also drawn. Along with the calculated results of considered five liquid alloys of Hg-In alloy. The results obtained from electronic properties namely total density of state and partial density of states help to find the local arrangement of Hg and In atoms and the presence of liquid state in the considered five alloys.

Nanosecond time resolved x-ray diagnostics of relativistic electron beam initiated events

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

Kuswa, Glenn W.; Chang, James

The dynamic behavior of a test sample during aid shortly after it has teen irradiated by an intense relativistic electron beam (REB) is of great interest to the study of team energy deposition. Since the sample densities are far beyond the cutoff in the optical region, flash x-radiography techniques have been developed to diagnose the evolution of the samples. The conventional approach of analyzing the dynamic behavior of solid densities utilizes one or more short x-ray bursts to record images on photographic emulsion. This technique is not useful in the presence of the intense x-rays from the REB interacting withmore » the sample. We report two techniques for isolating the film package from the REB x-ray pulse.« less

Communication: Improved ab initio molecular dynamics by minimally biasing with experimental data

NASA Astrophysics Data System (ADS)

White, Andrew D.; Knight, Chris; Hocky, Glen M.; Voth, Gregory A.

2017-01-01

Accounting for electrons and nuclei simultaneously is a powerful capability of ab initio molecular dynamics (AIMD). However, AIMD is often unable to accurately reproduce properties of systems such as water due to inaccuracies in the underlying electronic density functionals. This shortcoming is often addressed by added empirical corrections and/or increasing the simulation temperature. We present here a maximum-entropy approach to directly incorporate limited experimental data via a minimal bias. Biased AIMD simulations of water and an excess proton in water are shown to give significantly improved properties both for observables which were biased to match experimental data and for unbiased observables. This approach also yields new physical insight into inaccuracies in the underlying density functional theory as utilized in the unbiased AIMD.

Communication: Improved ab initio molecular dynamics by minimally biasing with experimental data.

PubMed

White, Andrew D; Knight, Chris; Hocky, Glen M; Voth, Gregory A

2017-01-28

Accounting for electrons and nuclei simultaneously is a powerful capability of ab initio molecular dynamics (AIMD). However, AIMD is often unable to accurately reproduce properties of systems such as water due to inaccuracies in the underlying electronic density functionals. This shortcoming is often addressed by added empirical corrections and/or increasing the simulation temperature. We present here a maximum-entropy approach to directly incorporate limited experimental data via a minimal bias. Biased AIMD simulations of water and an excess proton in water are shown to give significantly improved properties both for observables which were biased to match experimental data and for unbiased observables. This approach also yields new physical insight into inaccuracies in the underlying density functional theory as utilized in the unbiased AIMD.

Electronic and elastic mode locking in charge density wave conductors

NASA Astrophysics Data System (ADS)

Zettl, A.

1986-12-01

Mode locking phenomena are investigated in the charge density wave (CDW) materials NbSe 3 and TaS 3. The joint application of ac and dc electric fields results in free running and mode locked solutions for the CDW drift velocity, with associated ac-induced dynamic coherence lengths ξ D(ac) on the order of several hundred microns. The electronic response couples directly to the elastic properties of the crystal, with corresponding free running and mode locked solutions for the velocity of sound. Phase slip center-induced discontinuities in the CDW phase velocity lead to mode locked solutions with period doubling routes to chaos, and noisy precursor effects at bifurcation points. These results are discussed in terms of simple models of CDW domain synchronization, and internal CDW dynamics.

Nonlinear model for thermal effects in free-electron lasers

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

Peter, E., E-mail: peterpeter@uol.com.br; Endler, A., E-mail: aendler@if.ufrgs.br; Rizzato, F. B., E-mail: rizzato@if.ufrgs.br

2014-11-15

In the present work, we extend results of a previous paper [Peter et al., Phys. Plasmas 20, 12 3104 (2013)] and develop a semi-analytical model to account for thermal effects on the nonlinear dynamics of the electron beam in free-electron lasers. We relax the condition of a cold electron beam but still use the concept of compressibility, now associated with a warm beam model, to evaluate the time scale for saturation and the peak laser intensity in high-gain regimes. Although vanishing compressibilites and the associated divergent densities are absent in warm models, a series of discontinuities in the electron density precedemore » the saturation process. We show that full wave-particle simulations agree well with the predictions of the model.« less

Electronic coupling through natural amino acids

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

Berstis, Laura; Beckham, Gregg T., E-mail: michael.crowley@nrel.gov, E-mail: gregg.beckham@nrel.gov; Crowley, Michael F., E-mail: michael.crowley@nrel.gov, E-mail: gregg.beckham@nrel.gov

2015-12-14

Myriad scientific domains concern themselves with biological electron transfer (ET) events that span across vast scales of rate and efficiency through a remarkably fine-tuned integration of amino acid (AA) sequences, electronic structure, dynamics, and environment interactions. Within this intricate scheme, many questions persist as to how proteins modulate electron-tunneling properties. To help elucidate these principles, we develop a model set of peptides representing the common α-helix and β-strand motifs including all natural AAs within implicit protein-environment solvation. Using an effective Hamiltonian strategy with density functional theory, we characterize the electronic coupling through these peptides, furthermore considering side-chain dynamics. For bothmore » motifs, predictions consistently show that backbone-mediated electronic coupling is distinctly sensitive to AA type (aliphatic, polar, aromatic, negatively charged and positively charged), and to side-chain orientation. The unique properties of these residues may be employed to design activated, deactivated, or switch-like superexchange pathways. Electronic structure calculations and Green’s function analyses indicate that localized shifts in the electron density along the peptide play a role in modulating these pathways, and further substantiate the experimentally observed behavior of proline residues as superbridges. The distinct sensitivities of tunneling pathways to sequence and conformation revealed in this electronic coupling database help improve our fundamental understanding of the broad diversity of ET reactivity and provide guiding principles for peptide design.« less

Density-Gradient Theory: A Macroscopic Approach to Quantum Confinement and Tunneling in Semiconductor Devices

DTIC Science & Technology

2011-01-01

that are attractive as luminescent biolabels, and possibly also for optoelectronic devices and solar cells . The equilibrium nature of such situations...The boundary layers as- sociated with the diffusion and Debye lengths are familiar, while that of LQ defines the layer in which the quantum in...circuits, transmission lines Diffusion -drift, density-gradient Semi-classical electron dynamics, Boltzmann transport Schrödinger, density- matrix, Wigner

Importance of strong-correlation on the lattice dynamics of light-actinides Th-Pa alloy

NASA Astrophysics Data System (ADS)

de La Peã+/-A Seaman, Omar; Heid, Rolf; Bohnen, Klaus-Peter

We have studied the structural, electronic, and lattice dynamics of the Th1-xPax actinide alloy. This system have been analyzed within the framework of density functional perturbation theory, using a mixed-basis pseudopotential method and the virtual crystal approximation (VCA) for modeling the alloy. In particular, the energetics is analyzed as the ground-state crystal structure is changed form fcc to bct, as well as the electronic density of states (DOS), and the phonon frequencies. Such properties have been calculated with and without strong correlations effects through the LDA+U formalism. Although the strong-correlation does not influence on a great manner the Th properties, such effects are more important as the content increases towards Pa, affecting even the definition of the ground-state crystal structure for Pa (experimentally determined as bct). The evolution of the density of states at the Fermi level (N (EF)) and the phonon frequencies as a function of Pa-content are presented and discussed in detail, aiming to understand their influence on the electron-phonon coupling for the Th-Pa alloy. This research was supported by Conacyt-México under project No. CB2013-221807-F.

Simultaneous use of camera and probe diagnostics to unambiguously identify and study the dynamics of multiple underlying instabilities during the route to plasma turbulence.

PubMed

Thakur, S C; Brandt, C; Light, A; Cui, L; Gosselin, J J; Tynan, G R

2014-11-01

We use multiple-tip Langmuir probes and fast imaging to unambiguously identify and study the dynamics of underlying instabilities during the controlled route to fully-developed plasma turbulence in a linear magnetized helicon plasma device. Langmuir probes measure radial profiles of electron temperature, plasma density and potential; from which we compute linear growth rates of instabilities, cross-phase between density and potential fluctuations, Reynold's stress, particle flux, vorticity, time-delay estimated velocity, etc. Fast imaging complements the 1D probe measurements by providing temporally and spatially resolved 2D details of plasma structures associated with the instabilities. We find that three radially separated plasma instabilities exist simultaneously. Density gradient driven resistive drift waves propagating in the electron diamagnetic drift direction separate the plasma into an edge region dominated by strong, velocity shear driven Kelvin-Helmholtz instabilities and a central core region which shows coherent Rayleigh-Taylor modes propagating in the ion diamagnetic drift direction. The simultaneous, complementary use of both probes and camera was crucial to identify the instabilities and understand the details of the very rich plasma dynamics.

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

Zhao, H.; Li, X.; Baker, D. N.

Based on comprehensive measurements from Helium, Oxygen, Proton, and Electron Mass Spectrometer Ion Spectrometer, Relativistic Electron-Proton Telescope, and Radiation Belt Storm Probes Ion Composition Experiment instruments on the Van Allen Probes, comparative studies of ring current electrons and ions are performed and the role of energetic electrons in the ring current dynamics is investigated. The deep injections of tens to hundreds of keV electrons and tens of keV protons into the inner magnetosphere occur frequently; after the injections the electrons decay slowly in the inner belt but protons in the low L region decay very fast. Intriguing similarities between lowermore » energy protons and higher-energy electrons are also found. The evolution of ring current electron and ion energy densities and energy content are examined in detail during two geomagnetic storms, one moderate and one intense. Here, the results show that the contribution of ring current electrons to the ring current energy content is much smaller than that of ring current ions (up to ~12% for the moderate storm and ~7% for the intense storm), and <35 keV electrons dominate the ring current electron energy content at the storm main phases. Though the electron energy content is usually much smaller than that of ions, the enhancement of ring current electron energy content during the moderate storm can get to ~30% of that of ring current ions, indicating a more dynamic feature of ring current electrons and important role of electrons in the ring current buildup. Lastly, the ring current electron energy density is also shown to be higher at midnight and dawn while lower at noon and dusk.« less

Martian Dust Devil Electron Avalanche Process and Associated Electrochemistry

NASA Technical Reports Server (NTRS)

Jackson, Telana L.; Farrell, William M.; Delory, Gregory T.; Nithianandam, Jeyasingh

2010-01-01

Mars' dynamic atmosphere displays localized dust devils and larger, global dust storms. Based on terrestrial analog studies, electrostatic modeling, and laboratory work these features will contain large electrostatic fields formed via triboelectric processes. In the low-pressure Martian atmosphere, these fields may create an electron avalanche and collisional plasma due to an increase in electron density driven by the internal electrical forces. To test the hypothesis that an electron avalanche is sustained under these conditions, a self-consistent atmospheric process model is created including electron impact ionization sources and electron losses via dust absorption, electron dissociation attachment, and electron/ion recombination. This new model is called the Dust Devil Electron Avalanche Model (DDEAM). This model solves simultaneously nine continuity equations describing the evolution of the primary gaseous chemical species involved in the electrochemistry. DDEAM monitors the evolution of the electrons and primary gas constituents, including electron/water interactions. We especially focus on electron dynamics and follow the electrons as they evolve in the E field driven collisional gas. When sources and losses are self-consistently included in the electron continuity equation, the electron density grows exponentially with increasing electric field, reaching an equilibrium that forms a sustained time-stable collisional plasma. However, the character of this plasma differs depending upon the assumed growth rate saturation process (chemical saturation versus space charge). DDEAM also shows the possibility of the loss of atmospheric methane as a function of electric field due to electron dissociative attachment of the hydrocarbon. The methane destruction rates are presented and can be included in other larger atmospheric models.

Heterogeneous to homogeneous melting transition visualized with ultrafast electron diffraction

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

None

The ultrafast laser excitation of matters leads to non-equilibrium states with complex solid-liquid phase transition dynamics. We used electron diffraction at mega-electronvolt energies to visualize the ultrafast melting of gold on the atomic scale length. For energy densities approaching the irreversible melting regime, we first observed heterogeneous melting on time scales of 100 ps to 1000 ps, transitioning to homogeneous melting that occurs catastrophically within 10-20 ps at higher energy densities. We showed evidence for the heterogeneous coexistence of solid and liquid. We determined the ion and electron temperature evolution and found superheated conditions. Our results constrain the electron-ion couplingmore » rate, determine the Debye temperature and reveal the melting sensitivity to nucleation seeds.« less

Ab initio molecular dynamics simulation of LiBr association in water

NASA Astrophysics Data System (ADS)

Izvekov, Sergei; Philpott, Michael R.

2000-12-01

A computationally economical scheme which unifies the density functional description of an ionic solute and the classical description of a solvent was developed. The density functional part of the scheme comprises Car-Parrinello and related formalisms. The substantial saving in the computer time is achieved by performing the ab initio molecular dynamics of the solute electronic structure in a relatively small basis set constructed from lowest energy Kohn-Sham orbitals calculated for a single anion in vacuum, instead of using plane wave basis. The methodology permits simulation of an ionic solution for longer time scales while keeping accuracy in the prediction of the solute electronic structure. As an example the association of the Li+-Br- ion-pair system in water is studied. The results of the combined molecular dynamics simulation are compared with that obtained from the classical simulation with ion-ion interaction described by the pair potential of Born-Huggins-Mayer type. The comparison reveals an important role played by the polarization of the Br- ion in the dynamics of ion pair association.

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

Robust, Rework-able Thermal Electronic Packaging: Applications in High Power TR Modules for Space

NASA Technical Reports Server (NTRS)

Hoffman, James Patrick; Del Castillo, Linda; Hunter, Don; Miller, Jennifer

2012-01-01

The higher output power densities required of modern radar architectures, such as the proposed DESDynI [Deformation, Ecosystem Structure, and Dynamics of Ice] SAR [Synthetic Aperture Radar] Instrument (or DSI) require increasingly dense high power electronics. To enable these higher power densities, while maintaining or even improving hardware reliability, requires improvements in integrating advanced thermal packaging technologies into radar transmit/receive (TR) modules. New materials and techniques have been studied and are now being implemented side-by-side with more standard technology typically used in flight hardware.

Role of the dielectric for the charging dynamics of the dielectric/barrier interface in AlGaN/GaN based metal-insulator-semiconductor structures under forward gate bias stress

NASA Astrophysics Data System (ADS)

Lagger, P.; Steinschifter, P.; Reiner, M.; Stadtmüller, M.; Denifl, G.; Naumann, A.; Müller, J.; Wilde, L.; Sundqvist, J.; Pogany, D.; Ostermaier, C.

2014-07-01

The high density of defect states at the dielectric/III-N interface in GaN based metal-insulator-semiconductor structures causes tremendous threshold voltage drifts, ΔVth, under forward gate bias conditions. A comprehensive study on different dielectric materials, as well as varying dielectric thickness tD and barrier thickness tB, is performed using capacitance-voltage analysis. It is revealed that the density of trapped electrons, ΔNit, scales with the dielectric capacitance under spill-over conditions, i.e., the accumulation of a second electron channel at the dielectric/AlGaN barrier interface. Hence, the density of trapped electrons is defined by the charging of the dielectric capacitance. The scaling behavior of ΔNit is explained universally by the density of accumulated electrons at the dielectric/III-N interface under spill-over conditions. We conclude that the overall density of interface defects is higher than what can be electrically measured, due to limits set by dielectric breakdown. These findings have a significant impact on the correct interpretation of threshold voltage drift data and are of relevance for the development of normally off and normally on III-N/GaN high electron mobility transistors with gate insulation.

Density matrix-based time-dependent configuration interaction approach to ultrafast spin-flip dynamics

NASA Astrophysics Data System (ADS)

Wang, Huihui; Bokarev, Sergey I.; Aziz, Saadullah G.; Kühn, Oliver

2017-08-01

Recent developments in attosecond spectroscopy yield access to the correlated motion of electrons on their intrinsic timescales. Spin-flip dynamics is usually considered in the context of valence electronic states, where spin-orbit coupling is weak and processes related to the electron spin are usually driven by nuclear motion. However, for core-excited states, where the core-hole has a nonzero angular momentum, spin-orbit coupling is strong enough to drive spin-flips on a much shorter timescale. Using density matrix-based time-dependent restricted active space configuration interaction including spin-orbit coupling, we address an unprecedentedly short spin-crossover for the example of L-edge (2p→3d) excited states of a prototypical Fe(II) complex. This process occurs on a timescale, which is faster than that of Auger decay (∼4 fs) treated here explicitly. Modest variations of carrier frequency and pulse duration can lead to substantial changes in the spin-state yield, suggesting its control by soft X-ray light.

Storm-time radiation belt electron dynamics: Repeatability in the outer radiation belt

NASA Astrophysics Data System (ADS)

Murphy, K. R.; Mann, I. R.; Rae, J.; Watt, C.; Boyd, A. J.; Turner, D. L.; Claudepierre, S. G.; Baker, D. N.; Spence, H. E.; Reeves, G. D.; Blake, J. B.; Fennell, J. F.

2017-12-01

During intervals of enhanced solar wind driving the outer radiation belt becomes extremely dynamic leading to geomagnetic storms. During these storms the flux of energetic electrons can vary by over 4 orders of magnitude. Despite recent advances in understanding the nature of competing storm-time electron loss and acceleration processes the dynamic behavior of the outer radiation belt remains poorly understood; the outer radiation belt can exhibit either no change, an enhancement, or depletion in radiation belt electrons. Using a new analysis of the total radiation belt electron content, calculated from the Van Allen probes phase space density (PSD), we statistically analyze the time-dependent and global response of the outer radiation belt during storms. We demonstrate that by removing adiabatic effects there is a clear and repeatable sequence of events in storm-time radiation belt electron dynamics. Namely, the relativistic (μ=1000 MeV/G) and ultra-relativistic (μ=4000 MeV/G) electron populations can be separated into two phases; an initial phase dominated by loss followed by a second phase dominated by acceleration. At lower energies, the radiation belt seed population of electrons (μ=150 MeV/G) shows no evidence of loss but rather a net enhancement during storms. Further, we investigate the dependence of electron dynamics as a function of the second adiabatic invariant, K. These results demonstrate a global coherency in the dynamics of the source, relativistic and ultra-relativistic electron populations as function of the second adiabatic invariant K. This analysis demonstrates two key aspects of storm-time radiation belt electron dynamics. First, the radiation belt responds repeatably to solar wind driving during geomagnetic storms. Second, the response of the radiation belt is energy dependent, relativistic electrons behaving differently than lower energy seed electrons. These results have important implications in radiation belt research. In particular, the repeatability in electron dynamics coupled with observations of processes leading to electron loss (EMIC waves) and acceleration (VLF or ULF waves) can be used to diagnose the relative importance of physical processes in radiation belt dynamics during storms.

Ab initio molecular dynamics with nuclear quantum effects at classical cost: Ring polymer contraction for density functional theory

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

Marsalek, Ondrej; Markland, Thomas E., E-mail: tmarkland@stanford.edu

Path integral molecular dynamics simulations, combined with an ab initio evaluation of interactions using electronic structure theory, incorporate the quantum mechanical nature of both the electrons and nuclei, which are essential to accurately describe systems containing light nuclei. However, path integral simulations have traditionally required a computational cost around two orders of magnitude greater than treating the nuclei classically, making them prohibitively costly for most applications. Here we show that the cost of path integral simulations can be dramatically reduced by extending our ring polymer contraction approach to ab initio molecular dynamics simulations. By using density functional tight binding asmore » a reference system, we show that our ring polymer contraction scheme gives rapid and systematic convergence to the full path integral density functional theory result. We demonstrate the efficiency of this approach in ab initio simulations of liquid water and the reactive protonated and deprotonated water dimer systems. We find that the vast majority of the nuclear quantum effects are accurately captured using contraction to just the ring polymer centroid, which requires the same number of density functional theory calculations as a classical simulation. Combined with a multiple time step scheme using the same reference system, which allows the time step to be increased, this approach is as fast as a typical classical ab initio molecular dynamics simulation and 35× faster than a full path integral calculation, while still exactly including the quantum sampling of nuclei. This development thus offers a route to routinely include nuclear quantum effects in ab initio molecular dynamics simulations at negligible computational cost.« less

Unified theory of quantized electrons, phonons, and photons out of equilibrium: A simplified ab initio approach based on the generalized Baym-Kadanoff ansatz

NASA Astrophysics Data System (ADS)

de Melo, Pedro Miguel M. C.; Marini, Andrea

2016-04-01

We present a full ab initio description of the coupled out-of-equilibrium dynamics of photons, phonons, and electrons. In the present approach, the quantized nature of the electromagnetic field as well as of the nuclear oscillations is fully taken into account. The result is a set of integrodifferential equations, written on the Keldysh contour, for the Green's functions of electrons, phonons, and photons where the different kinds of interactions are merged together. We then concentrate on the electronic dynamics in order to reduce the problem to a computationally feasible approach. By using the generalized Baym-Kadanoff ansatz and the completed collision approximation, we introduce a series of efficient but controllable approximations. In this way, we reduce all equations to a set of decoupled equations for the density matrix that describe all kinds of static and dynamical correlations. The final result is a coherent, general, and inclusive scheme to calculate several physical quantities: carrier dynamics, transient photoabsorption, and light emission, all of which include, at the same time, electron-electron, electron-phonon, and electron-photon interactions. We further discuss how all these observables can be easily calculated within the present scheme using a fully atomistic ab initio approach.

Correlated electron-nuclear dissociation dynamics: classical versus quantum motion

NASA Astrophysics Data System (ADS)

Schaupp, Thomas; Albert, Julian; Engel, Volker

2017-01-01

We investigate the coupled electron-nuclear dynamics in a model system which undergoes dissociation. In choosing different initial conditions, the cases of adiabatic and non-adiabatic dissociation are realized. We treat the coupled electronic and nuclear motion in the complete configuration space so that classically, no surface hopping procedures have to be incorporated in the case that more than a single adiabatic electronic state is populated during the fragmentation. Due to the anharmonic interaction potential, it is expected that classical mechanics substantially deviate from quantum mechanics. However, we provide examples where the densities and fragmentation yields obtained from the two treatments are in astonishingly strong agreement in the case that one starts in the electronic ground state initially. As expected, larger deviations are found if one starts in electronically excited states where trajectories are sampled from the more spatially extended electronic wave function. In that case, higher initial energies are accessed, and the motion proceeds in regions with increasing degree of anharmonicity. Contribution to the Topical Issue "Dynamics of Molecular Systems (MOLEC 2016)", edited by Alberto Garcia-Vela, Luis Banares and Maria Luisa Senent.

DE/ISIS conjunction comparisons of high-latitude electron density features

NASA Technical Reports Server (NTRS)

Hoegy, Walter R.; Benson, Robert F.

1988-01-01

This paper presents a comparison between the ISIS-1 and -2 topside sounder measurements of electron number density, N(e), with the in situ ion and N(e) measurements by the Langmuir probe aboard the Dynamics Explorer 2 (DE 2) during four high-latitude ISIS/DE magnetic field-aligned conjunctions. The ISIS-derived N(e) values, even at the greatest distance from the sounder, were found to agree with the Langmuir probe measurements to within about 30 percent over a density range of more than two decades on three of the four comparisons; the fourth comparison which included data with strong N(e) irregularities, showed a difference of 60 percent.

MAVEN Observations of the Effects of Crustal Magnetic Fields on the Mars Ionosphere

NASA Astrophysics Data System (ADS)

Vogt, M. F.; Flynn, C. L.; Withers, P.; Andersson, L.; Girazian, Z.; Mitchell, D. L.; Xu, S.; Connerney, J. E. P.; Espley, J. R.

2017-12-01

Mars lacks a global intrinsic magnetic field but possesses regions of strong crustal magnetic field that influence the planetary interaction with the solar wind and affect the structure and dynamics of the ionosphere. Since entering Mars orbit in 2014, the MAVEN spacecraft has collected comprehensive measurements of the local plasma and magnetic field properties in the Martian dayside ionosphere. Here we discuss how crustal magnetic fields affect the structure, composition, and electrodynamics of the Martian ionosphere as seen by MAVEN. We present a survey of 17 months of MAVEN LPW measurements of the electron density and temperature in the dayside ionosphere and show that, above 200 km altitude, regions of strong crustal magnetic fields feature cooler electron temperatures and enhanced electron densities compared to regions with little or no crustal magnetic field. We also report on the influence of the magnetic field direction and topology on MAVEN electron density measurements in the southern crustal field areas, particularly in magnetic cusp regions. Finally, we discuss the effects of crustal magnetic fields on plasma boundaries like the ionopause, located at the top of the ionosphere and marked by a sharp and substantial gradient in the electron density.

Large-scale atomistic calculations of clusters in intense x-ray pulses

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

Ho, Phay J.; Knight, Chris

Here, we present the methodology of our recently developed Monte-Carlo/ Molecular-Dynamics method for studying the fundamental ultrafast dynamics induced by high-fluence, high-intensity x-ray free electron laser (XFEL) pulses in clusters. The quantum nature of the initiating ionization process is accounted for by a Monte Carlo method to calculate probabilities of electronic transitions, including photo absorption, inner-shell relaxation, photon scattering, electron collision and recombination dynamics, and thus track the transient electronic configurations explicitly. The freed electrons and ions are followed by classical particle trajectories using a molecular dynamics algorithm. These calculations reveal the surprising role of electron-ion recombination processes that leadmore » to the development of nonuniform spatial charge density profiles in x-ray excited clusters over femtosecond timescales. In the high-intensity limit, it is important to include the recombination dynamics in the calculated scattering response even for a 2- fs pulse. We also demonstrate that our numerical codes and algorithms can make e!cient use of the computational power of massively parallel supercomputers to investigate the intense-field dynamics in systems with increasing complexity and size at the ultrafast timescale and in non-linear x-ray interaction regimes. In particular, picosecond trajectories of XFEL clusters with attosecond time resolution containing millions of particles can be e!ciently computed on upwards of 262,144 processes.« less

Large-scale atomistic calculations of clusters in intense x-ray pulses

DOE PAGES

Ho, Phay J.; Knight, Chris

2017-04-28

Here, we present the methodology of our recently developed Monte-Carlo/ Molecular-Dynamics method for studying the fundamental ultrafast dynamics induced by high-fluence, high-intensity x-ray free electron laser (XFEL) pulses in clusters. The quantum nature of the initiating ionization process is accounted for by a Monte Carlo method to calculate probabilities of electronic transitions, including photo absorption, inner-shell relaxation, photon scattering, electron collision and recombination dynamics, and thus track the transient electronic configurations explicitly. The freed electrons and ions are followed by classical particle trajectories using a molecular dynamics algorithm. These calculations reveal the surprising role of electron-ion recombination processes that leadmore » to the development of nonuniform spatial charge density profiles in x-ray excited clusters over femtosecond timescales. In the high-intensity limit, it is important to include the recombination dynamics in the calculated scattering response even for a 2- fs pulse. We also demonstrate that our numerical codes and algorithms can make e!cient use of the computational power of massively parallel supercomputers to investigate the intense-field dynamics in systems with increasing complexity and size at the ultrafast timescale and in non-linear x-ray interaction regimes. In particular, picosecond trajectories of XFEL clusters with attosecond time resolution containing millions of particles can be e!ciently computed on upwards of 262,144 processes.« less

Electron Correlation from the Adiabatic Connection for Multireference Wave Functions

NASA Astrophysics Data System (ADS)

Pernal, Katarzyna

2018-01-01

An adiabatic connection (AC) formula for the electron correlation energy is derived for a broad class of multireference wave functions. The AC expression recovers dynamic correlation energy and assures a balanced treatment of the correlation energy. Coupling the AC formalism with the extended random phase approximation allows one to find the correlation energy only from reference one- and two-electron reduced density matrices. If the generalized valence bond perfect pairing model is employed a simple closed-form expression for the approximate AC formula is obtained. This results in the overall M5 scaling of the computation cost making the method one of the most efficient multireference approaches accounting for dynamic electron correlation also for the strongly correlated systems.

Elucidating the electron transport in semiconductors via Monte Carlo simulations: an inquiry-driven learning path for engineering undergraduates

NASA Astrophysics Data System (ADS)

Persano Adorno, Dominique; Pizzolato, Nicola; Fazio, Claudio

2015-09-01

Within the context of higher education for science or engineering undergraduates, we present an inquiry-driven learning path aimed at developing a more meaningful conceptual understanding of the electron dynamics in semiconductors in the presence of applied electric fields. The electron transport in a nondegenerate n-type indium phosphide bulk semiconductor is modelled using a multivalley Monte Carlo approach. The main characteristics of the electron dynamics are explored under different values of the driving electric field, lattice temperature and impurity density. Simulation results are presented by following a question-driven path of exploration, starting from the validation of the model and moving up to reasoned inquiries about the observed characteristics of electron dynamics. Our inquiry-driven learning path, based on numerical simulations, represents a viable example of how to integrate a traditional lecture-based teaching approach with effective learning strategies, providing science or engineering undergraduates with practical opportunities to enhance their comprehension of the physics governing the electron dynamics in semiconductors. Finally, we present a general discussion about the advantages and disadvantages of using an inquiry-based teaching approach within a learning environment based on semiconductor simulations.

Generalized-active-space pair-density functional theory: an efficient method to study large, strongly correlated, conjugated systems

DOE PAGES

Ghosh, Soumen; Cramer, Christopher J.; Truhlar, Donald G.; ...

2017-01-19

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. Here, we recently developed a new method called multiconfiguration pair-density functional theory (MC-PDFT), that combines the advantages of wave function theory and density functionalmore » 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.« less

Generalized-active-space pair-density functional theory: an efficient method to study large, strongly correlated, conjugated systems

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

Ghosh, Soumen; Cramer, Christopher J.; Truhlar, Donald G.

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. Here, we recently developed a new method called multiconfiguration pair-density functional theory (MC-PDFT), that combines the advantages of wave function theory and density functionalmore » 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.« less

Self-amplified photo-induced gap quenching in a correlated electron material

DOE PAGES

Mathias, S.; Eich, S.; Urbancic, J.; ...

2016-10-04

Capturing the dynamic electronic band structure of a correlated material presents a powerful capability for uncovering the complex couplings between the electronic and structural degrees of freedom. When combined with ultrafast laser excitation, new phases of matter can result, since far-from-equilibrium excited states are instantaneously populated. Here, we elucidate a general relation between ultrafast non-equilibrium electron dynamics and the size of the characteristic energy gap in a correlated electron material. Here, we show that carrier multiplication via impact ionization can be one of the most important processes in a gapped material, and that the speed of carrier multiplication critically dependsmore » on the size of the energy gap. In the case of the charge-density wave material 1T-TiSe 2, our data indicate that carrier multiplication and gap dynamics mutually amplify each other, which explains—on a microscopic level—the extremely fast response of this material to ultrafast optical excitation.« less

Three-dimensional structural dynamics and fluctuations of DNA-nanogold conjugates by individual-particle electron tomography

NASA Astrophysics Data System (ADS)

Zhang, Lei; Lei, Dongsheng; Smith, Jessica M.; Zhang, Meng; Tong, Huimin; Zhang, Xing; Lu, Zhuoyang; Liu, Jiankang; Alivisatos, A. Paul; Ren, Gang

2016-03-01

DNA base pairing has been used for many years to direct the arrangement of inorganic nanocrystals into small groupings and arrays with tailored optical and electrical properties. The control of DNA-mediated assembly depends crucially on a better understanding of three-dimensional structure of DNA-nanocrystal-hybridized building blocks. Existing techniques do not allow for structural determination of these flexible and heterogeneous samples. Here we report cryo-electron microscopy and negative-staining electron tomography approaches to image, and three-dimensionally reconstruct a single DNA-nanogold conjugate, an 84-bp double-stranded DNA with two 5-nm nanogold particles for potential substrates in plasmon-coupling experiments. By individual-particle electron tomography reconstruction, we obtain 14 density maps at ~2-nm resolution. Using these maps as constraints, we derive 14 conformations of dsDNA by molecular dynamics simulations. The conformational variation is consistent with that from liquid solution, suggesting that individual-particle electron tomography could be an expected approach to study DNA-assembling and flexible protein structure and dynamics.

Scaling relationships for nonadiabatic energy relaxation times in warm dense matter: toward understanding the equation of state.

PubMed

Pradhan, Ekadashi; Magyar, Rudolph J; Akimov, Alexey V

2016-11-30

Understanding the dynamics of electron-ion energy transfer in warm dense (WD) matter is important to the measurement of equation of state (EOS) properties and for understanding the energy balance in dynamic simulations. In this work, we present a comprehensive investigation of nonadiabatic electron relaxation and thermal excitation dynamics in aluminum under high pressure and temperature. Using quantum-classical trajectory surface hopping approaches, we examine the role of nonadiabatic couplings and electronic decoherence in electron-nuclear energy transfer in WD aluminum. The computed timescales range from 400 fs to 4.0 ps and are consistent with existing experimental studies. We have derived general scaling relationships between macroscopic parameters of WD systems such as temperature or mass density and the timescales of energy redistribution between quantum and classical degrees of freedom. The scaling laws are supported by computational results. We show that electronic decoherence plays essential role and can change the functional dependencies qualitatively. The established scaling relationships can be of use in modelling of WD matter.

Chemical dynamics of the first proton-coupled electron transfer of water oxidation on TiO2 anatase.

PubMed

Chen, Jia; Li, Ye-Fei; Sit, Patrick; Selloni, Annabella

2013-12-18

Titanium dioxide (TiO2) is a prototype, water-splitting (photo)catalyst, but its performance is limited by the large overpotential for the oxygen evolution reaction (OER). We report here a first-principles density functional theory study of the chemical dynamics of the first proton-coupled electron transfer (PCET), which is considered responsible for the large OER overpotential on TiO2. We use a periodic model of the TiO2/water interface that includes a slab of anatase TiO2 and explicit water molecules, sample the solvent configurations by first principles molecular dynamics, and determine the energy profiles of the two electronic states involved in the electron transfer (ET) by hybrid functional calculations. Our results suggest that the first PCET is sequential, with the ET following the proton transfer. The ET occurs via an inner sphere process, which is facilitated by a state in which one electronic hole is shared by the two oxygen ions involved in the transfer.

Average-atom model for two-temperature states and ionic transport properties of aluminum in the warm dense matter regime

NASA Astrophysics Data System (ADS)

Hou, Yong; Fu, Yongsheng; Bredow, Richard; Kang, Dongdong; Redmer, Ronald; Yuan, Jianmin

2017-03-01

The average-atom model combined with the hyper-netted chain approximation is an efficient tool for electronic and ionic structure calculations for warm dense matter. Here we generalize this method in order to describe non-equilibrium states with different electron and ion temperature as produced in laser-matter interactions on ultra-short time scales. In particular, the electron-ion and ion-ion correlation effects are considered when calculating the electron structure. We derive an effective ion-ion pair-potential using the electron densities in the framework of temperature-depended density functional theory. Using this ion-ion potential we perform molecular dynamics simulations in order to determine the ionic transport properties such as the ionic diffusion coefficient and the shear viscosity through the ionic velocity autocorrelation functions.

Electron mobility in monoclinic β-Ga2O3—Effect of plasmon-phonon coupling, anisotropy, and confinement

NASA Astrophysics Data System (ADS)

Ghosh, Krishnendu; Singisetti, Uttam

2017-11-01

This work reports an investigation of electron transport in monoclinic \\beta-Ga2O3 based on a combination of density functional perturbation theory based lattice dynamical computations, coupling calculation of lattice modes with collective plasmon oscillations and Boltzmann theory based transport calculations. The strong entanglement of the plasmon with the different longitudinal optical (LO) modes make the role LO-plasmon coupling crucial for transport. The electron density dependence of the electron mobility in \\beta-Ga2O3 is studied in bulk material form and also in the form of two-dimensional electron gas. Under high electron density a bulk mobility of 182 cm2/ V.s is predicted while in 2DEG form the corresponding mobility is about 418 cm2/V.s when remote impurities are present at the interface and improves further as the remote impurity center moves away from the interface. The trend of the electron mobility shows promise for realizing high electron mobility in dopant isolated electron channels. The experimentally observed small anisotropy in mobility is traced through a transient Monte Carlo simulation. It is found that the anisotropy of the IR active phonon modes is responsible for giving rise to the anisotropy in low-field electron mobility.

Detection of Ionospheric Alfven Resonator Signatures Onboard C/NOFS: Implications for IRI Modeling

NASA Technical Reports Server (NTRS)

Simoes, F.; Klenzing, J.; Ivanov, S.; Pfaff, R.; Rowland, D.; Bilitza, D.

2011-01-01

The 2008-2009 long-lasting solar minimum activity has been the one of its kind since the dawn of space age, offering exceptional conditions for investigating space weather in the near-Earth environment. First ever detection of Ionospheric Alfven Resonator (IAR) signatures in orbit offers new means for investigating ionospheric electrodynamics, namely MHD (MagnetoHydroDynamics) wave propagation, aeronomy processes, ionospheric dynamics, and Sun-Earth connection mechanisms at a local scale. Local and global plasma density heterogeneities in the ionosphere and magnetosphere allow for formation of waveguides and resonators where magnetosonic and shear Alfven waves propagate. The ionospheric magnetosonic waveguide results from complete magnetosonic wave reflection about the ionospheric F-region peak, where the Alfven index of refraction presents a maximum. MHD waves can also be partially trapped in the vertical direction between the lower boundary of the ionosphere and the magnetosphere, a resonance mechanism known as IAR. In this work we present C/NOFS (Communications/Navigation Outage Forecasting System) Extremely Low Frequency (ELF) electric field measurements related to IAR signatures, discuss the resonance and wave propagation mechanisms in the ionosphere, and address the electromagnetic inverse problem from which electron/ion distributions can be derived. These peculiar IAR electric field measurements provide new, complementary methodologies for inferring ionospheric electron and ion density profiles, and also contribute for the investigation of ionosphere dynamics and space weather monitoring. Specifically, IAR spectral signatures measured by C/NOFS contribute for improving the International Reference Ionosphere (IRI) model, namely electron density and ion composition.

Dynamic instabilities in strongly correlated VSe2 monolayers and bilayers

NASA Astrophysics Data System (ADS)

Esters, Marco; Hennig, Richard G.; Johnson, David C.

2017-12-01

With the emergence of graphene and other two-dimensional (2D) materials, transition-metal dichalcogenides have been investigated intensely as potential 2D materials using experimental and theoretical methods. VSe2 is an especially interesting material since its bulk modification exhibits a charge-density wave (CDW), the CDW is retained even for few-layer nanosheets, and monolayers of VSe2 are predicted to be ferromagnetic. In this work, we show that electron correlation has a profound effect on the magnetic properties and dynamic stability of VSe2 monolayers and bilayers. Including a Hubbard-U term in the density-functional-theory calculations strongly affects the magnetocrystalline anisotropy in the 1 T -VSe2 structure while leaving the 2 H -polytype virtually unchanged. This demonstrates the importance of electronic correlations for the electrical and magnetic properties of 1 T -VSe2 . The Hubbard-U term changes the dynamic stability and the presence of imaginary modes of ferromagnetic 1 T -VSe2 while affecting only the amplitudes in the nonmagnetic phase. The Fermi surface of nonmagnetic 1 T -VSe2 allows for nesting along the CDW vector, but it plays no role in ferromagnetic 1 T -VSe2 . Following the eigenvectors of the soft modes in nonmagnetic 1 T -VSe2 monolayers yields a CDW structure with a 4 ×4 supercell and Peierls-type distortion in the atomic positions and electronic structure. The magnetic order indicates the potential for spin-density-wave structures.

Neutral particle dynamics in a high-power RF source

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

Todorov, D., E-mail: dimitar-tdrv@phys.uni-sofia.bg; Paunska, Ts.; Shivarova, A.

2015-04-08

Previous studies on the spatial discharge structure in the SPIDER source of negative hydrogen/deuterium ions carried out at low applied power are extended towards description of the discharge maintenance under the conditions of the actual rf power deposition of 100 kW planned for a single driver of the source. In addition to the expected higher electron density, the results show strong increase of the electron temperature and of the temperatures of the neutral species (hydrogen atoms and molecules). In the discussions, not only the spatial distribution of the plasma parameters but also that of the fluxes in the discharge (particlemore » and energy fluxes) is involved. The obtained results come in confirmation of basic concepts for low-pressure discharge maintenance: (i) mutually related electron density and temperature as a display of the generalized Schottky condition, (ii) discharge behavior governed by the fluxes, i.e. strong nonlocality in the discharge, and (iii) a non-ambipolarity in the discharge regime, which originates from shifted maxima of the electron density and temperature and shows evidence in a vortex electron flux and in a dc current in a rf discharge, the latter resulting from a shift in the positions of the maxima of the electron density and plasma potential.« less

Dynamic kinetic energy potential for orbital-free density functional theory.

PubMed

Neuhauser, Daniel; Pistinner, Shlomo; Coomar, Arunima; Zhang, Xu; Lu, Gang

2011-04-14

A dynamic kinetic energy potential (DKEP) is developed for time-dependent orbital-free (TDOF) density function theory applications. This potential is constructed to affect only the dynamical (ω ≠ 0) response of an orbital-free electronic system. It aims at making the orbital-free simulation respond in the same way as that of a noninteracting homogenous electron gas (HEG), as required by a correct kinetic energy, therefore enabling extension of the success of orbital-free density functional theory in the static case (e.g., for embedding and description of processes in bulk materials) to dynamic processes. The potential is constructed by expansions of terms, each of which necessitates only simple time evolution (concurrent with the TDOF evolution) and a spatial convolution at each time-step. With 14 such terms a good fit is obtained to the response of the HEG at a large range of frequencies, wavevectors, and densities. The method is demonstrated for simple jellium spheres, approximating Na(9)(+) and Na(65)(+) clusters. It is applicable both to small and large (even ultralarge) excitations and the results converge (i.e., do not blow up) as a function of time. An extension to iterative frequency-resolved extraction is briefly outlined, as well as possibly numerically simpler expansions. The approach could also be extended to fit, instead of the HEG susceptibility, either an experimental susceptibility or a theoretically derived one for a non-HEG system. The DKEP potential should be a powerful tool for embedding a dynamical system described by a more accurate method (such as time-dependent density functional theory, TDDFT) in a large background described by TDOF with a DKEP potential. The type of expansions used and envisioned should be useful for other approaches, such as memory functionals in TDDFT. Finally, an appendix details the formal connection between TDOF and TDDFT.

Observations of non-linear plasmon damping in dense plasmas

NASA Astrophysics Data System (ADS)

Witte, B. B. L.; Sperling, P.; French, M.; Recoules, V.; Glenzer, S. H.; Redmer, R.

2018-05-01

We present simulations using finite-temperature density-functional-theory molecular-dynamics to calculate dynamic dielectric properties in warm dense aluminum. The comparison between exchange-correlation functionals in the Perdew, Burke, Ernzerhof approximation, Strongly Constrained and Appropriately Normed Semilocal Density Functional, and Heyd, Scuseria, Ernzerhof (HSE) approximation indicates evident differences in the electron transition energies, dc conductivity, and Lorenz number. The HSE calculations show excellent agreement with x-ray scattering data [Witte et al., Phys. Rev. Lett. 118, 225001 (2017)] as well as dc conductivity and absorption measurements. These findings demonstrate non-Drude behavior of the dynamic conductivity above the Cooper minimum that needs to be taken into account to determine optical properties in the warm dense matter regime.

Electron dynamics in complex environments with real-time time dependent density functional theory in a QM-MM framework.

PubMed

Morzan, Uriel N; Ramírez, Francisco F; Oviedo, M Belén; Sánchez, Cristián G; Scherlis, Damián A; Lebrero, Mariano C González

2014-04-28

This article presents a time dependent density functional theory (TDDFT) implementation to propagate the Kohn-Sham equations in real time, including the effects of a molecular environment through a Quantum-Mechanics Molecular-Mechanics (QM-MM) hamiltonian. The code delivers an all-electron description employing Gaussian basis functions, and incorporates the Amber force-field in the QM-MM treatment. The most expensive parts of the computation, comprising the commutators between the hamiltonian and the density matrix-required to propagate the electron dynamics-, and the evaluation of the exchange-correlation energy, were migrated to the CUDA platform to run on graphics processing units, which remarkably accelerates the performance of the code. The method was validated by reproducing linear-response TDDFT results for the absorption spectra of several molecular species. Two different schemes were tested to propagate the quantum dynamics: (i) a leap-frog Verlet algorithm, and (ii) the Magnus expansion to first-order. These two approaches were confronted, to find that the Magnus scheme is more efficient by a factor of six in small molecules. Interestingly, the presence of iron was found to seriously limitate the length of the integration time step, due to the high frequencies associated with the core-electrons. This highlights the importance of pseudopotentials to alleviate the cost of the propagation of the inner states when heavy nuclei are present. Finally, the methodology was applied to investigate the shifts induced by the chemical environment on the most intense UV absorption bands of two model systems of general relevance: the formamide molecule in water solution, and the carboxy-heme group in Flavohemoglobin. In both cases, shifts of several nanometers are observed, consistently with the available experimental data.

Nonadiabatic Molecular Dynamics and Orthogonality Constrained Density Functional Theory

NASA Astrophysics Data System (ADS)

Shushkov, Philip Georgiev

The exact quantum dynamics of realistic, multidimensional systems remains a formidable computational challenge. In many chemical processes, however, quantum effects such as tunneling, zero-point energy quantization, and nonadiabatic transitions play an important role. Therefore, approximate approaches that improve on the classical mechanical framework are of special practical interest. We propose a novel ring polymer surface hopping method for the calculation of chemical rate constants. The method blends two approaches, namely ring polymer molecular dynamics that accounts for tunneling and zero-point energy quantization, and surface hopping that incorporates nonadiabatic transitions. We test the method against exact quantum mechanical calculations for a one-dimensional, two-state model system. The method reproduces quite accurately the tunneling contribution to the rate and the distribution of reactants between the electronic states for this model system. Semiclassical instanton theory, an approach related to ring polymer molecular dynamics, accounts for tunneling by the use of periodic classical trajectories on the inverted potential energy surface. We study a model of electron transfer in solution, a chemical process where nonadiabatic events are prominent. By representing the tunneling electron with a ring polymer, we derive Marcus theory of electron transfer from semiclassical instanton theory after a careful analysis of the tunneling mode. We demonstrate that semiclassical instanton theory can recover the limit of Fermi's Golden Rule rate in a low-temperature, deep-tunneling regime. Mixed quantum-classical dynamics treats a few important degrees of freedom quantum mechanically, while classical mechanics describes affordably the rest of the system. But the interface of quantum and classical description is a challenging theoretical problem, especially for low-energy chemical processes. We therefore focus on the semiclassical limit of the coupled nuclear-electronic dynamics. We show that the time-dependent Schrodinger equation for the electrons employed in the widely used fewest switches surface hopping method is applicable only in the limit of nearly identical classical trajectories on the different potential energy surfaces. We propose a short-time decoupling algorithm that restricts the use of the Schrodinger equation only to the interaction regions. We test the short-time approximation on three model systems against exact quantum-mechanical calculations. The approximation improves the performance of the surface hopping approach. Nonadiabatic molecular dynamics simulations require the efficient and accurate computation of ground and excited state potential energy surfaces. Unlike the ground state calculations where standard methods exist, the computation of excited state properties is a challenging task. We employ time-independent density functional theory, in which the excited state energy is represented as a functional of the total density. We suggest an adiabatic-like approximation that simplifies the excited state exchange-correlation functional. We also derive a set of minimal conditions to impose exactly the orthogonality of the excited state Kohn-Sham determinant to the ground state determinant. This leads to an efficient, variational algorithm for the self-consistent optimization of the excited state energy. Finally, we assess the quality of the excitation energies obtained by the new method on a set of 28 organic molecules. The new approach provides results of similar accuracy to time-dependent density functional theory.

Nonadiabatic Dynamics for Electrons at Second-Order: Real-Time TDDFT and OSCF2.

PubMed

Nguyen, Triet S; Parkhill, John

2015-07-14

We develop a new model to simulate nonradiative relaxation and dephasing by combining real-time Hartree-Fock and density functional theory (DFT) with our recent open-systems theory of electronic dynamics. The approach has some key advantages: it has been systematically derived and properly relaxes noninteracting electrons to a Fermi-Dirac distribution. This paper combines the new dissipation theory with an atomistic, all-electron quantum chemistry code and an atom-centered model of the thermal environment. The environment is represented nonempirically and is dependent on molecular structure in a nonlocal way. A production quality, O(N(3)) closed-shell implementation of our theory applicable to realistic molecular systems is presented, including timing information. This scaling implies that the added cost of our nonadiabatic relaxation model, time-dependent open self-consistent field at second order (OSCF2), is computationally inexpensive, relative to adiabatic propagation of real-time time-dependent Hartree-Fock (TDHF) or time-dependent density functional theory (TDDFT). Details of the implementation and numerical algorithm, including factorization and efficiency, are discussed. We demonstrate that OSCF2 approaches the stationary self-consistent field (SCF) ground state when the gap is large relative to k(b)T. The code is used to calculate linear-response spectra including the effects of bath dynamics. Finally, we show how our theory of finite-temperature relaxation can be used to correct ground-state DFT calculations.

Partially coherent electron transport in terahertz quantum cascade lasers based on a Markovian master equation for the density matrix

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

Jonasson, O.; Karimi, F.; Knezevic, I.

2016-08-01

We derive a Markovian master equation for the single-electron density matrix, applicable to quantum cascade lasers (QCLs). The equation conserves the positivity of the density matrix, includes off-diagonal elements (coherences) as well as in-plane dynamics, and accounts for electron scattering with phonons and impurities. We use the model to simulate a terahertz-frequency QCL, and compare the results with both experiment and simulation via nonequilibrium Green's functions (NEGF). We obtain very good agreement with both experiment and NEGF when the QCL is biased for optimal lasing. For the considered device, we show that the magnitude of coherences can be a significantmore » fraction of the diagonal matrix elements, which demonstrates their importance when describing THz QCLs. We show that the in-plane energy distribution can deviate far from a heated Maxwellian distribution, which suggests that the assumption of thermalized subbands in simplified density-matrix models is inadequate. As a result, we also show that the current density and subband occupations relax towards their steady-state values on very different time scales.« 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.

Excess electrons in ice: a density functional theory study.

PubMed

Bhattacharya, Somesh Kr; Inam, Fakharul; Scandolo, Sandro

2014-02-21

We present a density functional theory study of the localization of excess electrons in the bulk and on the surface of crystalline and amorphous water ice. We analyze the initial stages of electron solvation in crystalline and amorphous ice. In the case of crystalline ice we find that excess electrons favor surface states over bulk states, even when the latter are localized at defect sites. In contrast, in amorphous ice excess electrons find it equally favorable to localize in bulk and in surface states which we attribute to the preexisting precursor states in the disordered structure. In all cases excess electrons are found to occupy the vacuum regions of the molecular network. The electron localization in the bulk of amorphous ice is assisted by its distorted hydrogen bonding network as opposed to the crystalline phase. Although qualitative, our results provide a simple interpretation of the large differences observed in the dynamics and localization of excess electrons in crystalline and amorphous ice films on metals.

Covariant Formulation of Fluid Dynamics and Estakhr's Material Geodesic Equation, far down the Rabbit hole

NASA Astrophysics Data System (ADS)

Estakhr, Ahmad Reza

2013-11-01

``When i meet God, I am going to ask him two questions, why relativity and why turbulence. A. Einstein'' You probably will not need to ask these questions of God, I've already answered both of them. Uμ = γ (c , u (r --> , t)) denotes four-velocity field. Jμ = ρUμ denotes four-current mass density. Estakhr's Material-Geodesic equation is developed analogy of Navier Stokes equation and Einstein Geodesic equation. DJμ/Dτ =dJμ/Dτ +ΓαβμJαUβ =JνΩμν +∂νTμν +ΓαβμJαUβ Covariant formulation of fluid dynamics, describe the motion of fluid substances. The local existence and uniqueness theorem for geodesics states that geodesics on a smooth manifold with an affine connection exist, and are unique. EMG equation is also applicable in different branches of physics, it all depend on what you mean by 4-current density, if you mean 4-current electron number density then it is plasma physics, if you mean 4-current electron charge density then it is DJμ/Dτ =JνFμν +∂νTμν +ΓαβμJαUβ electromagnetism.

Influence of local-field corrections on Thomson scattering in collision-dominated two-component plasmas.

PubMed

Fortmann, Carsten; Wierling, August; Röpke, Gerd

2010-02-01

The dynamic structure factor, which determines the Thomson scattering spectrum, is calculated via an extended Mermin approach. It incorporates the dynamical collision frequency as well as the local-field correction factor. This allows to study systematically the impact of electron-ion collisions as well as electron-electron correlations due to degeneracy and short-range interaction on the characteristics of the Thomson scattering signal. As such, the plasmon dispersion and damping width is calculated for a two-component plasma, where the electron subsystem is completely degenerate. Strong deviations of the plasmon resonance position due to the electron-electron correlations are observed at increasing Brueckner parameters r(s). These results are of paramount importance for the interpretation of collective Thomson scattering spectra, as the determination of the free electron density from the plasmon resonance position requires a precise theory of the plasmon dispersion. Implications due to different approximations for the electron-electron correlation, i.e., different forms of the one-component local-field correction, are discussed.

Four-electron model for singlet and triplet excitation energy transfers with inclusion of coherence memory, inelastic tunneling and nuclear quantum effects

NASA Astrophysics Data System (ADS)

Suzuki, Yosuke; Ebina, Kuniyoshi; Tanaka, Shigenori

2016-08-01

A computational scheme to describe the coherent dynamics of excitation energy transfer (EET) in molecular systems is proposed on the basis of generalized master equations with memory kernels. This formalism takes into account those physical effects in electron-bath coupling system such as the spin symmetry of excitons, the inelastic electron tunneling and the quantum features of nuclear motions, thus providing a theoretical framework to perform an ab initio description of EET through molecular simulations for evaluating the spectral density and the temporal correlation function of electronic coupling. Some test calculations have then been carried out to investigate the dependence of exciton population dynamics on coherence memory, inelastic tunneling correlation time, magnitude of electronic coupling, quantum correction to temporal correlation function, reorganization energy and energy gap.

Tuning ultrafast electron injection dynamics at organic-graphene/metal interfaces.

PubMed

Ravikumar, Abhilash; Kladnik, Gregor; Müller, Moritz; Cossaro, Albano; Bavdek, Gregor; Patera, Laerte L; Sánchez-Portal, Daniel; Venkataraman, Latha; Morgante, Alberto; Brivio, Gian Paolo; Cvetko, Dean; Fratesi, Guido

2018-05-03

We compare the ultrafast charge transfer dynamics of molecules on epitaxial graphene and bilayer graphene grown on Ni(111) interfaces through first principles calculations and X-ray resonant photoemission spectroscopy. We use 4,4'-bipyridine as a prototypical molecule for these explorations as the energy level alignment of core-excited molecular orbitals allows ultrafast injection of electrons from a substrate to a molecule on a femtosecond timescale. We show that the ultrafast injection of electrons from the substrate to the molecule is ∼4 times slower on weakly coupled bilayer graphene than on epitaxial graphene. Through our experiments and calculations, we can attribute this to a difference in the density of states close to the Fermi level between graphene and bilayer graphene. We therefore show how graphene coupling with the substrate influences charge transfer dynamics between organic molecules and graphene interfaces.

Temporal Behavior of the Ionospheric Electron Density at Low Latitudes: First Glimpse

NASA Astrophysics Data System (ADS)

Gjerloev, J. W.; Humberset, B. K.; Gonzalez, S. A.; Garnett Marques Brum, C.

2013-12-01

In this paper we address the spatiotemporal characteristics of the electron density at 150 km altitude in the low latitude ionosphere above the Arecibo Observatory. We utilize a new pointing mode that allows us to probe the same volume in the ionosphere for a continuous period of approximately 25 min. or more. The ISR profiles have 150 m range resolution and samples have a 10-second time resolution; we probed 60 individual regions uniformly spaced in local times and covering the full 24 hours. For each time series we determine the total derivative of the electron density using a narrow Hanning bandpass filter that allow us to determine the variability at different frequencies. This is done for each of the 60 local time regions. We further compare to widely used static statistical models and test their underlying assumption: Dynamics can be ignored.

A real-time extension of density matrix embedding theory for non-equilibrium electron dynamics

NASA Astrophysics Data System (ADS)

Kretchmer, Joshua S.; Chan, Garnet Kin-Lic

2018-02-01

We introduce real-time density matrix embedding theory (DMET), a dynamical quantum embedding theory for computing non-equilibrium electron dynamics in strongly correlated systems. As in the previously developed static DMET, real-time DMET partitions the system into an impurity corresponding to the region of interest coupled to the surrounding environment, which is efficiently represented by a quantum bath of the same size as the impurity. In this work, we focus on a simplified single-impurity time-dependent formulation as a first step toward a multi-impurity theory. The equations of motion of the coupled impurity and bath embedding problem are derived using the time-dependent variational principle. The accuracy of real-time DMET is compared to that of time-dependent complete active space self-consistent field (TD-CASSCF) theory and time-dependent Hartree-Fock (TDHF) theory for a variety of quantum quenches in the single impurity Anderson model (SIAM), in which the Hamiltonian is suddenly changed (quenched) to induce a non-equilibrium state. Real-time DMET shows a marked improvement over the mean-field TDHF, converging to the exact answer even in the non-trivial Kondo regime of the SIAM. However, as expected from analogous behavior in static DMET, the constrained structure of the real-time DMET wavefunction leads to a slower convergence with respect to active space size, in the single-impurity formulation, relative to TD-CASSCF. Our initial results suggest that real-time DMET provides a promising framework to simulate non-equilibrium electron dynamics in which strong electron correlation plays an important role, and lays the groundwork for future multi-impurity formulations.

A real-time extension of density matrix embedding theory for non-equilibrium electron dynamics.

PubMed

Kretchmer, Joshua S; Chan, Garnet Kin-Lic

2018-02-07

We introduce real-time density matrix embedding theory (DMET), a dynamical quantum embedding theory for computing non-equilibrium electron dynamics in strongly correlated systems. As in the previously developed static DMET, real-time DMET partitions the system into an impurity corresponding to the region of interest coupled to the surrounding environment, which is efficiently represented by a quantum bath of the same size as the impurity. In this work, we focus on a simplified single-impurity time-dependent formulation as a first step toward a multi-impurity theory. The equations of motion of the coupled impurity and bath embedding problem are derived using the time-dependent variational principle. The accuracy of real-time DMET is compared to that of time-dependent complete active space self-consistent field (TD-CASSCF) theory and time-dependent Hartree-Fock (TDHF) theory for a variety of quantum quenches in the single impurity Anderson model (SIAM), in which the Hamiltonian is suddenly changed (quenched) to induce a non-equilibrium state. Real-time DMET shows a marked improvement over the mean-field TDHF, converging to the exact answer even in the non-trivial Kondo regime of the SIAM. However, as expected from analogous behavior in static DMET, the constrained structure of the real-time DMET wavefunction leads to a slower convergence with respect to active space size, in the single-impurity formulation, relative to TD-CASSCF. Our initial results suggest that real-time DMET provides a promising framework to simulate non-equilibrium electron dynamics in which strong electron correlation plays an important role, and lays the groundwork for future multi-impurity formulations.

Thermal conductivity of graphene with defects induced by electron beam irradiation

NASA Astrophysics Data System (ADS)

Malekpour, Hoda; Ramnani, Pankaj; Srinivasan, Srilok; Balasubramanian, Ganesh; Nika, Denis L.; Mulchandani, Ashok; Lake, Roger K.; Balandin, Alexander A.

2016-07-01

We investigate the thermal conductivity of suspended graphene as a function of the density of defects, ND, introduced in a controllable way. High-quality graphene layers are synthesized using chemical vapor deposition, transferred onto a transmission electron microscopy grid, and suspended over ~7.5 μm size square holes. Defects are induced by irradiation of graphene with the low-energy electron beam (20 keV) and quantified by the Raman D-to-G peak intensity ratio. As the defect density changes from 2.0 × 1010 cm-2 to 1.8 × 1011 cm-2 the thermal conductivity decreases from ~(1.8 +/- 0.2) × 103 W mK-1 to ~(4.0 +/- 0.2) × 102 W mK-1 near room temperature. At higher defect densities, the thermal conductivity reveals an intriguing saturation-type behavior at a relatively high value of ~400 W mK-1. The thermal conductivity dependence on the defect density is analyzed using the Boltzmann transport equation and molecular dynamics simulations. The results are important for understanding phonon - point defect scattering in two-dimensional systems and for practical applications of graphene in thermal management.We investigate the thermal conductivity of suspended graphene as a function of the density of defects, ND, introduced in a controllable way. High-quality graphene layers are synthesized using chemical vapor deposition, transferred onto a transmission electron microscopy grid, and suspended over ~7.5 μm size square holes. Defects are induced by irradiation of graphene with the low-energy electron beam (20 keV) and quantified by the Raman D-to-G peak intensity ratio. As the defect density changes from 2.0 × 1010 cm-2 to 1.8 × 1011 cm-2 the thermal conductivity decreases from ~(1.8 +/- 0.2) × 103 W mK-1 to ~(4.0 +/- 0.2) × 102 W mK-1 near room temperature. At higher defect densities, the thermal conductivity reveals an intriguing saturation-type behavior at a relatively high value of ~400 W mK-1. The thermal conductivity dependence on the defect density is analyzed using the Boltzmann transport equation and molecular dynamics simulations. The results are important for understanding phonon - point defect scattering in two-dimensional systems and for practical applications of graphene in thermal management. Electronic supplementary information (ESI) available: Additional thermal conductivity measurements data. See DOI: 10.1039/c6nr03470e

Ab initio simulations of the dynamic ion structure factor of warm dense lithium

DOE PAGES

Witte, B. B. L.; Shihab, M.; Glenzer, S. H.; ...

2017-04-06

Here, we present molecular dynamics simulations based on finite-temperature density functional theory that determine self-consistently the dynamic ion structure factor and the electronic form factor in lithium. Our comprehensive data set allows for the calculation of the dispersion relation for collective excitations, the calculation of the sound velocity, and the determination of the ion feature from the total electronic form factor and the ion structure factor. The results are compared with available experimental x-ray and neutron scattering data. Good agreement is found for both the liquid metal and warm dense matter domain. Finally, we study the impact of possible targetmore » inhomogeneities on x-ray scattering spectra.« less

Ab initio simulations of the dynamic ion structure factor of warm dense lithium

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

Witte, B. B. L.; Shihab, M.; Glenzer, S. H.

Here, we present molecular dynamics simulations based on finite-temperature density functional theory that determine self-consistently the dynamic ion structure factor and the electronic form factor in lithium. Our comprehensive data set allows for the calculation of the dispersion relation for collective excitations, the calculation of the sound velocity, and the determination of the ion feature from the total electronic form factor and the ion structure factor. The results are compared with available experimental x-ray and neutron scattering data. Good agreement is found for both the liquid metal and warm dense matter domain. Finally, we study the impact of possible targetmore » inhomogeneities on x-ray scattering spectra.« less

Investigation of an electronic image enhancer for radiographs

NASA Technical Reports Server (NTRS)

Vary, A.

1972-01-01

Radiographs of nuclear and aerospace components were studied with a closed-circuit television system to determine the advantages of electronic enhancement in radiographic nondestructive evaluation. The radiographic images were examined on a television monitor under various degrees of magnification and enhancement. The enhancement was accomplished by generating a video signal whose amplitude is proportional to the rate of change of density. Points, lines, edges, and other density variations that are faintly registered in the original image are rendered in sharp relief. Examples of the applications of this mode of enhancement are discussed together with the system's dynamic response and resolution.

Investigation of an electronic image enhancer for radiographs.

NASA Technical Reports Server (NTRS)

Vary, A.

1972-01-01

Radiographs of nuclear and aerospace components were studied with a closed-circuit television system to determine the advantages of electronic enhancement in radiographic nondestructive evaluation. The radiographic images were examined on a television monitor under various degrees of magnification and enhancement. The enhancement was accomplished by generating a video signal whose amplitude is proportional to the rate of change of density. Points, lines, edges, and other density variations that are faintly registered in the original image are rendered in sharp relief. Examples of the applications of this mode of enhancement are discussed together with the system's dynamic response and resolution.

Electron correlation and the self-interaction error of density functional theory

NASA Astrophysics Data System (ADS)

Polo, Victor; Kraka, Elfi; Cremer, Dieter

The self-interaction error (SIE) of commonly used DFT functionals has been systematically investigated by comparing the electron density distribution ρ( r ) generated by self-interaction corrected DFT (SIC-DFT) with a series of reference densities obtained by DFT or wavefunction theory (WFT) methods that cover typical electron correlation effects. Although the SIE of GGA functionals is considerably smaller than that of LDA functionals, it has significant consequences for the coverage of electron correlation effects at the DFT level of theory. The exchange SIE mimics long range (non-dynamic) pair correlation effects, and is responsible for the fact that the electron density of DFT exchange-only calculations resembles often that of MP4, MP2 or even CCSD(T) calculations. Changes in the electron density caused by SICDFT exchange are comparable with those that are associated with HF exchange. Correlation functionals contract the density towards the bond and the valence region, thus taking negative charge out of the van der Waals region where these effects are exaggerated by the influence of the SIE of the correlation functional. Hence, SIC-DFT leads in total to a relatively strong redistribution of negative charge from van der Waals, non-bonding, and valence regions of heavy atoms to the bond regions. These changes, although much stronger, resemble those obtained when comparing the densities of hybrid functionals such as B3LYP with the corresponding GGA functional BLYP. Hence, the balanced mixing of local and non-local exchange and correlation effects as it is achieved by hybrid functionals mimics SIC-DFT and can be considered as an economic way to include some SIC into standard DFT. However, the investigation shows also that the SIC-DFT description of molecules is unreliable because the standard functionals used were optimized for DFT including the SIE.

Photo-induced reactions from efficient molecular dynamics with electronic transitions using the FIREBALL local-orbital density functional theory formalism.

PubMed

Zobač, Vladimír; Lewis, James P; Abad, Enrique; Mendieta-Moreno, Jesús I; Hapala, Prokop; Jelínek, Pavel; Ortega, José

2015-05-08

The computational simulation of photo-induced processes in large molecular systems is a very challenging problem. Firstly, to properly simulate photo-induced reactions the potential energy surfaces corresponding to excited states must be appropriately accessed; secondly, understanding the mechanisms of these processes requires the exploration of complex configurational spaces and the localization of conical intersections; finally, photo-induced reactions are probability events, that require the simulation of hundreds of trajectories to obtain the statistical information for the analysis of the reaction profiles. Here, we present a detailed description of our implementation of a molecular dynamics with electronic transitions algorithm within the local-orbital density functional theory code FIREBALL, suitable for the computational study of these problems. As an example of the application of this approach, we also report results on the [2 + 2] cycloaddition of ethylene with maleic anhydride and on the [2 + 2] photo-induced polymerization reaction of two C60 molecules. We identify different deactivation channels of the initial electron excitation, depending on the time of the electronic transition from LUMO to HOMO, and the character of the HOMO after the transition.

Time-Dependent Density Functional Theory for Extreme Environments

NASA Astrophysics Data System (ADS)

Baczewski, Andrew; Magyar, Rudolph; Shulenburger, Luke

2013-10-01

In recent years, DFT-MD has been shown to be a powerful tool for calculating the equation of state and constitutive properties of warm dense matter (WDM). These studies are validated through a number of experiments, including recently developed X-Ray Thomson Scattering (XRTS) techniques. Here, electronic temperatures and densities of WDM are accessible through x-ray scattering data, which is related to the system's dynamic structure factor (DSF)-a quantity that is accessible through DFT-MD calculations. Previous studies predict the DSF within the Born-Oppenheimer approximation, with the electronic state computed using Mermin DFT. A capability for including more general coupled electron-ion dynamics is desirable, to study both the effect on XRTS observables and the broader problem of electron-ion energy transfer in extreme WDM conditions. Progress towards such a capability will be presented, in the form of an Ehrenfest MD framework using TDDFT. Computational challenges and open theoretical questions will be discussed. Sandia National Laboratories is a multi-program laboratory managed and operated by Sandia Corporation, a wholly owned subsidiary of Lockheed Martin Corporation, for the U.S. Department of Energy's National Security Administration under contract DE-AC04-94AL85000.

Self-consistent implementation of ensemble density functional theory method for multiple strongly correlated electron pairs

DOE PAGES

Filatov, Michael; Liu, Fang; Kim, Kwang S.; ...

2016-12-22

Here, the spin-restricted ensemble-referenced Kohn-Sham (REKS) method is based on an ensemble representation of the density and is capable of correctly describing the non-dynamic electron correlation stemming from (near-)degeneracy of several electronic configurations. The existing REKS methodology describes systems with two electrons in two fractionally occupied orbitals. In this work, the REKS methodology is extended to treat systems with four fractionally occupied orbitals accommodating four electrons and self-consistent implementation of the REKS(4,4) method with simultaneous optimization of the orbitals and their fractional occupation numbers is reported. The new method is applied to a number of molecular systems where simultaneous dissociationmore » of several chemical bonds takes place, as well as to the singlet ground states of organic tetraradicals 2,4-didehydrometaxylylene and 1,4,6,9-spiro[4.4]nonatetrayl.« less

Cylindrical ion-acoustic solitary waves in electronegative plasmas with superthermal electrons

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

Eslami, Parvin; Mottaghizadeh, Marzieh

2012-06-15

By using the standard reductive perturbation technique, a three-dimensional cylindrical Kadomtsev-Petviashvili equation (CKPE), which governs the dynamics of ion acoustic solitary waves (IASWs), is derived for small but finite amplitude ion-acoustic waves in cylindrical geometry in a collisionless unmagnetized plasma with kappa distributed electrons, thermal positrons, and cold ions. The generalized expansion method is used to solve analytically the CKPE. The existence regions of localized pulses are investigated. It is found that the solution of the CKPE supports only compressive solitary waves. Furthermore, the effects of superthermal electrons, the ratio of the electron temperature to positron temperature, the ratio ofmore » the positron density to electron density and direction cosine of the wave propagation on the profiles of the amplitudes, and widths of the solitary structures are examined numerically. It is shown these parameters play a vital role in the formation of ion acoustic solitary waves.« less

Ion-ion dynamic structure factor, acoustic modes, and equation of state of two-temperature warm dense aluminum

NASA Astrophysics Data System (ADS)

Harbour, L.; Förster, G. D.; Dharma-wardana, M. W. C.; Lewis, Laurent J.

2018-04-01

The ion-ion dynamical structure factor and the equation of state of warm dense aluminum in a two-temperature quasiequilibrium state, with the electron temperature higher than the ion temperature, are investigated using molecular-dynamics simulations based on ion-ion pair potentials constructed from a neutral pseudoatom model. Such pair potentials based on density functional theory are parameter-free and depend directly on the electron temperature and indirectly on the ion temperature, enabling efficient computation of two-temperature properties. Comparison with ab initio simulations and with other average-atom calculations for equilibrium aluminum shows good agreement, justifying a study of quasiequilibrium situations. Analyzing the van Hove function, we find that ion-ion correlations vanish in a time significantly smaller than the electron-ion relaxation time so that dynamical properties have a physical meaning for the quasiequilibrium state. A significant increase in the speed of sound is predicted from the modification of the dispersion relation of the ion acoustic mode as the electron temperature is increased. The two-temperature equation of state including the free energy, internal energy, and pressure is also presented.

Nonequilibrium Green's functions and atom-surface dynamics: Simple views from a simple model system

NASA Astrophysics Data System (ADS)

Boström, E.; Hopjan, M.; Kartsev, A.; Verdozzi, C.; Almbladh, C.-O.

2016-03-01

We employ Non-equilibrium Green's functions (NEGF) to describe the real-time dynamics of an adsorbate-surface model system exposed to ultrafast laser pulses. For a finite number of electronic orbitals, the system is solved exactly and within different levels of approximation. Specifically i) the full exact quantum mechanical solution for electron and nuclear degrees of freedom is used to benchmark ii) the Ehrenfest approximation (EA) for the nuclei, with the electron dynamics still treated exactly. Then, using the EA, electronic correlations are treated with NEGF within iii) 2nd Born and with iv) a recently introduced hybrid scheme, which mixes 2nd Born self-energies with non-perturbative, local exchange- correlation potentials of Density Functional Theory (DFT). Finally, the effect of a semi-infinite substrate is considered: we observe that a macroscopic number of de-excitation channels can hinder desorption. While very preliminary in character and based on a simple and rather specific model system, our results clearly illustrate the large potential of NEGF to investigate atomic desorption, and more generally, the non equilibrium dynamics of material surfaces subject to ultrafast laser fields.

Orbital disproportionation of electronic density is a universal feature of alkali-doped fullerides

PubMed Central

Iwahara, Naoya; Chibotaru, Liviu F.

2016-01-01

Alkali-doped fullerides show a wide range of electronic phases in function of alkali atoms and the degree of doping. Although the presence of strong electron correlations is well established, recent investigations also give evidence for dynamical Jahn–Teller instability in the insulating and the metallic trivalent fullerides. In this work, to reveal the interplay of these interactions in fullerides with even electrons, we address the electronic phase of tetravalent fulleride with accurate many-body calculations within a realistic electronic model including all basic interactions extracted from first principles. We find that the Jahn–Teller instability is always realized in these materials too. In sharp contrast to the correlated metals, tetravalent system displays uncorrelated band-insulating state despite similar interactions present in both fullerides. Our results show that the Jahn–Teller instability and the accompanying orbital disproportionation of electronic density in the degenerate lowest unoccupied molecular orbital band is a universal feature of fullerides. PMID:27713426

Examinations of tRNA Range of Motion Using Simulations of Cryo-EM Microscopy and X-Ray Data.

PubMed

Caulfield, Thomas R; Devkota, Batsal; Rollins, Geoffrey C

2011-01-01

We examined tRNA flexibility using a combination of steered and unbiased molecular dynamics simulations. Using Maxwell's demon algorithm, molecular dynamics was used to steer X-ray structure data toward that from an alternative state obtained from cryogenic-electron microscopy density maps. Thus, we were able to fit X-ray structures of tRNA onto cryogenic-electron microscopy density maps for hybrid states of tRNA. Additionally, we employed both Maxwell's demon molecular dynamics simulations and unbiased simulation methods to identify possible ribosome-tRNA contact areas where the ribosome may discriminate tRNAs during translation. Herein, we collected >500 ns of simulation data to assess the global range of motion for tRNAs. Biased simulations can be used to steer between known conformational stop points, while unbiased simulations allow for a general testing of conformational space previously unexplored. The unbiased molecular dynamics data describes the global conformational changes of tRNA on a sub-microsecond time scale for comparison with steered data. Additionally, the unbiased molecular dynamics data was used to identify putative contacts between tRNA and the ribosome during the accommodation step of translation. We found that the primary contact regions were H71 and H92 of the 50S subunit and ribosomal proteins L14 and L16.

Possible link of sudden onset and short-time periodic pulsation of polar mesosphere summer echoes to ULF Pc5 geomagnetic pulsations and solar wind dynamic pressure enhancement

NASA Astrophysics Data System (ADS)

Lee, Y.; Kirkwood, S.; Kwak, Y. S.

2016-12-01

The EISCAT VHF incoherent scatter radar in Tromsö, Norway, makes occasional observations of electron densities and Polar Mesosphere Summer Echoes, in the summer polar D-region ionosphere. In one of those datasets, pulsating polar mesospheric summer echoes (PMSE) are observed, with periodicities in the ultra-low frequency (ULF) Pc5 band (1.6-6.7 mHz), following an abrupt increase of the radar reflectivity when a geomagnetic field excursion is started, in turn linked to dynamic pressure (Pdyn) enhancement in the solar wind. At the excursion of the magnetic field, at auroral altitudes of 90 km and above, electron density is abruptly enhanced, followed by a series of short-lived peaks, superimposed on an enhanced level. The short-lived peaks are likely a signature of transient Pc5 geomagnetic pulsations and associated energetic electron precipitation from pitch-angle scattering into the loss cone in the magnetosphere. At the same time, at altitudes around 80-90 km, a sharp increase of PMSE reflectivity occurs, 100 times greater than the increase of electron density, and is followed by pulsating PMSE reflectivity with periodicities in the Pc5 band, increasing and decreasing in magnitude during the course of the next hour. The increase of the pulsation magnitude may be attributed to an increase of high-energy electron precipitation flux ( >30 keV) penetrating to at least the height of maximum PMSE reflectivity. This study suggests that Pc5 pulsation bursts in both magnetic field and high energy electron precipitation could play a crucial role in producing PMSE fluctuations on minute-to-minute time scales.

Dynamic electronic correlation effects in NbO 2 as compared to VO 2

DOE PAGES

Brito, W. H.; Aguiar, M. C. O.; Haule, K.; ...

2017-11-01

In this study we present a comparative investigation of the electronic structures of NbO 2 and VO 2 obtained within a combination of density functional theory and cluster-dynamical mean-field theory calculations. We investigate the role of dynamic electronic correlations on the electronic structure of the metallic and insulating phases of NbO 2 and VO 2, with a focus on the mechanism responsible for the gap opening in the insulating phases. For the rutile metallic phases of both oxides, we obtain that electronic correlations lead to a strong renormalization of the t 2g subbands, as well as the emergence of incoherentmore » Hubbard subbands, signaling that electronic correlations are also important in the metallic phase of NbO 2. Interestingly, we find that nonlocal dynamic correlations do play a role in the gap formation of the [body-centered-tetragonal (bct)] insulating phase of NbO 2, by a similar physical mechanism as that recently proposed by us in the case of the monoclinic (M 1) dimerized phase of VO 2. Finally, although the effect of nonlocal dynamic correlations in the gap opening of bct phase is less important than in the (M 1 and M 2) monoclinic phases of VO 2, their presence indicates that the former is not a purely Peierls-type insulator, as it was recently proposed.« less

Electronic properties of liquid Hg-In alloys : Ab-initio molecular dynamics study

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

Sharma, Nalini, E-mail: nalini-2808@yahoo.co.in; Ahluwalia, P. K.; Thakur, Anil

2016-05-23

Ab-initio molecular dynamics simulations are performed to study the structural properties of liquid Hg-In alloys. The interatomic interactions are described by ab-initio pseudopotentials given by Troullier and Martins. Three liquid Hg-In alloys (Hg{sub 10}In{sub 90}, Hg{sub 30}In{sub 70,.} Hg{sub 50}In{sub 50}, Hg{sub 70}In{sub 30}, and Hg{sub 90}Pb{sub 10}) at 299 K are considered. The calculated results for liquid Hg (l-Hg) and lead (l-In) are also drawn. Along with the calculated results of considered five liquid alloys of Hg-In alloy. The results obtained from electronic properties namely total density of state and partial density of states help to find the localmore » arrangement of Hg and In atoms and the presence of liquid state in the considered five alloys.« less

HDL surface lipids mediate CETP binding as revealed by electron microscopy and molecular dynamics simulation

PubMed Central

Zhang, Meng; Charles, River; Tong, Huimin; Zhang, Lei; Patel, Mili; Wang, Francis; Rames, Matthew J.; Ren, Amy; Rye, Kerry-Anne; Qiu, Xiayang; Johns, Douglas G.; Charles, M. Arthur; Ren, Gang

2015-01-01

Cholesteryl ester transfer protein (CETP) mediates the transfer of cholesterol esters (CE) from atheroprotective high-density lipoproteins (HDL) to atherogenic low-density lipoproteins (LDL). CETP inhibition has been regarded as a promising strategy for increasing HDL levels and subsequently reducing the risk of cardiovascular diseases (CVD). Although the crystal structure of CETP is known, little is known regarding how CETP binds to HDL. Here, we investigated how various HDL-like particles interact with CETP by electron microscopy and molecular dynamics simulations. Results showed that CETP binds to HDL via hydrophobic interactions rather than protein-protein interactions. The HDL surface lipid curvature generates a hydrophobic environment, leading to CETP hydrophobic distal end interaction. This interaction is independent of other HDL components, such as apolipoproteins, cholesteryl esters and triglycerides. Thus, disrupting these hydrophobic interactions could be a new therapeutic strategy for attenuating the interaction of CETP with HDL. PMID:25737239

Proton deflectometry of laser-driven relativistic electron jet from thin foil target

NASA Astrophysics Data System (ADS)

Huang, Chengkun; Palaniyappan, S.; Gautier, D. C.; Johnson, R. P.; Shimada, T.; Fernandez, J. C.; Tsung, F. S.; Mori, W. B.

2017-10-01

Near critical density relativistic electron jets from laser solid interaction carry currents approaching the Alfvén-limit and tens of kilo-Tesla magnetic fields. Such jets are often found in kinetic simulations with low areal density targets, but have not been confirmed experimentally. They may be used for X/gamma-ray generation and is also important for the understanding of post-transparency plasma dynamics. With a short-pulse probe beam at the Trident laser facility, we employed proton deflectometry to infer the jet's properties, structure and the long-time dynamics. We develop corresponding GEANT4 simulation model of the proton deflectometry, with input from the kinetic PIC simulations in 2D and quasi-3D geometry, to compare with the experimental radiography images. Detail comparison of the experimental and simulation features in the deflectometry will be discussed. Work supported by the LDRD program at LANL.

From Two‐ to Three‐Dimensional Structures of a Supertetrahedral Boran Using Density Functional Calculations

PubMed Central

Getmanskii, Iliya V.; Steglenko, Dmitrii V.; Koval, Vitaliy V.; Zaitsev, Stanislav A.

2017-01-01

Abstract With help of the DFT calculations and imposing of periodic boundary conditions the geometrical and electronic structures were investigated of two‐ and three‐dimensional boron systems designed on the basis of graphane and diamond lattices in which carbons were replaced with boron tetrahedrons. The consequent studies of two‐ and three‐layer systems resulted in the construction of a three‐dimensional supertetrahedral borane crystal structure. The two‐dimensional supertetrahedral borane structures with less than seven layers are dynamically unstable. At the same time the three‐dimensional superborane systems were found to be dynamically stable. Lack of the forbidden electronic zone for the studied boron systems testifies that these structures can behave as good conductors. The low density of the supertetrahedral borane crystal structures (0.9 g cm−3) is close to that of water, which offers the perspective for their application as aerospace and cosmic materials. PMID:28402596

HDL surface lipids mediate CETP binding as revealed by electron microscopy and molecular dynamics simulation

DOE PAGES

Zhang, Meng; Charles, River; Tong, Huimin; ...

2015-03-04

Cholesteryl ester transfer protein (CETP) mediates the transfer of cholesterol esters (CE) from atheroprotective high-density lipoproteins (HDL) to atherogenic low-density lipoproteins (LDL). CETP inhibition has been regarded as a promising strategy for increasing HDL levels and subsequently reducing the risk of cardiovascular diseases (CVD). Although the crystal structure of CETP is known, little is known regarding how CETP binds to HDL. Here, we investigated how various HDL-like particles interact with CETP by electron microscopy and molecular dynamics simulations. Results showed that CETP binds to HDL via hydrophobic interactions rather than protein-protein interactions. The HDL surface lipid curvature generates a hydrophobicmore » environment, leading to CETP hydrophobic distal end interaction. This interaction is independent of other HDL components, such as apolipoproteins, cholesteryl esters and triglycerides. Thus, disrupting these hydrophobic interactions could be a new therapeutic strategy for attenuating the interaction of CETP with HDL.« less

HDL surface lipids mediate CETP binding as revealed by electron microscopy and molecular dynamics simulation

NASA Astrophysics Data System (ADS)

Zhang, Meng; Charles, River; Tong, Huimin; Zhang, Lei; Patel, Mili; Wang, Francis; Rames, Matthew J.; Ren, Amy; Rye, Kerry-Anne; Qiu, Xiayang; Johns, Douglas G.; Charles, M. Arthur; Ren, Gang

2015-03-01

Cholesteryl ester transfer protein (CETP) mediates the transfer of cholesterol esters (CE) from atheroprotective high-density lipoproteins (HDL) to atherogenic low-density lipoproteins (LDL). CETP inhibition has been regarded as a promising strategy for increasing HDL levels and subsequently reducing the risk of cardiovascular diseases (CVD). Although the crystal structure of CETP is known, little is known regarding how CETP binds to HDL. Here, we investigated how various HDL-like particles interact with CETP by electron microscopy and molecular dynamics simulations. Results showed that CETP binds to HDL via hydrophobic interactions rather than protein-protein interactions. The HDL surface lipid curvature generates a hydrophobic environment, leading to CETP hydrophobic distal end interaction. This interaction is independent of other HDL components, such as apolipoproteins, cholesteryl esters and triglycerides. Thus, disrupting these hydrophobic interactions could be a new therapeutic strategy for attenuating the interaction of CETP with HDL.

Structural, electronic, mechanical, and dynamical properties of graphene oxides: A first principles study

NASA Astrophysics Data System (ADS)

Dabhi, Shweta D.; Gupta, Sanjay D.; Jha, Prafulla K.

2014-05-01

We report the results of a theoretical study on the structural, electronic, mechanical, and vibrational properties of some graphene oxide models (GDO, a-GMO, z-GMO, ep-GMO and mix-GMO) at ambient pressure. The calculations are based on the ab-initio plane-wave pseudo potential density functional theory, within the generalized gradient approximations for the exchange and correlation functional. The calculated values of lattice parameters, bulk modulus, and its first order pressure derivative are in good agreement with other reports. A linear response approach to the density functional theory is used to derive the phonon frequencies. We discuss the contribution of the phonons in the dynamical stability of graphene oxides and detailed analysis of zone centre phonon modes in all the above mentioned models. Our study demonstrates a wide range of energy gap available in the considered models of graphene oxide and hence the possibility of their use in nanodevices.

A Statitstical Study of Energetic Electron Phase Space Density with RBSP and BD-IES Data

NASA Astrophysics Data System (ADS)

Chen, X.; Zong, Q.; Zhou, X.; Zou, H.; Wang, Y.

2017-12-01

We present a statistical study of energetic electron phase space density (PSD) with combined observations from the Magnetic Electron Ion Spectrometer (MagEIS) instruments onboard the Van Allen Probes and the Image Electron Spectrometer (BD-IES) onboard an inclined geosynchronous orbit satellite. The electron PSD as a function of the adiabatic invariants is derived using one year data (Nov. 2015 to Oct. 2016) of these instruments. The orbits of the satellites cover a wide range of L-shells, allowing for the distribution of electron PSD throughout the radiation belt (L* 1 to 10). A persistent peak of energetic electron ( 30 to 1000 MeV/G) PSD is unambiguously identified at L* 5.5, which may help to understand the role of local acceleration and radial diffusion in the dynamics of energetic electrons. In addition, the electron PSD shows a power-law distribution with the exponent varying from about -2 to -4 depending on L*. The variance of electron PSD during storm and substorm activities indicating by SYMH and AE indices are also discussed.

Lattice dynamic properties of Rh2XAl (X=Fe and Y) alloys

NASA Astrophysics Data System (ADS)

Al, Selgin; Arikan, Nihat; Demir, Süleyman; Iyigör, Ahmet

2018-02-01

The electronic band structure, elastic and vibrational spectra of Rh2FeAl and Rh2YAl alloys were computed in detail by employing an ab-initio pseudopotential method and a linear-response technique based on the density-functional theory (DFT) scheme within a generalized gradient approximation (GGA). Computed lattice constants, bulk modulus and elastic constants were compared. Rh2YAl exhibited higher ability to resist volume change than Rh2FeAl. The elastic constants, shear modulus, Young modulus, Poisson's ratio, B/G ratio electronic band structure, total and partial density of states, and total magnetic moment of alloys were also presented. Rh2FeAl showed spin up and spin down states whereas Rh2YAl showed none due to being non-magnetic. The calculated total densities of states for both materials suggest that both alloys are metallic in nature. Full phonon spectra of Rh2FeAl and Rh2YA1 alloys in the L21 phase were collected using the ab-initio linear response method. The obtained phonon frequencies were in the positive region indicating that both alloys are dynamically stable.

Nanosecond repetitively pulsed discharges in air at atmospheric pressure—the spark regime

NASA Astrophysics Data System (ADS)

Pai, David Z.; Lacoste, Deanna A.; Laux, Christophe O.

2010-12-01

Nanosecond repetitively pulsed (NRP) spark discharges have been studied in atmospheric pressure air preheated to 1000 K. Measurements of spark initiation and stability, plasma dynamics, gas temperature and current-voltage characteristics of the spark regime are presented. Using 10 ns pulses applied repetitively at 30 kHz, we find that 2-400 pulses are required to initiate the spark, depending on the applied voltage. Furthermore, about 30-50 pulses are required for the spark discharge to reach steady state, following initiation. Based on space- and time-resolved optical emission spectroscopy, the spark discharge in steady state is found to ignite homogeneously in the discharge gap, without evidence of an initial streamer. Using measured emission from the N2 (C-B) 0-0 band, it is found that the gas temperature rises by several thousand Kelvin in the span of about 30 ns following the application of the high-voltage pulse. Current-voltage measurements show that up to 20-40 A of conduction current is generated, which corresponds to an electron number density of up to 1015 cm-3 towards the end of the high-voltage pulse. The discharge dynamics, gas temperature and electron number density are consistent with a streamer-less spark that develops homogeneously through avalanche ionization in volume. This occurs because the pre-ionization electron number density of about 1011 cm-3 produced by the high frequency train of pulses is above the critical density for streamer-less discharge development, which is shown to be about 108 cm-3.

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

PubMed

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

2016-12-15

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

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

PubMed Central

2018-01-01

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

Erosion and refilling of the plasmasphere during a geomagnetic storm modeled by a neural network

NASA Astrophysics Data System (ADS)

Chu, X. N.; Bortnik, J.; Li, W.; Ma, Q.; Angelopoulos, V.; Thorne, R. M.

2017-07-01

We present a history-dependent model of the equatorial plasma density of the inner magnetosphere using a feedforward neural network with two hidden layers. As the model inputs, we take locations and time series of SYM-H, AL, and F10.7 indices. By considering not only the instantaneous values but also the past values of geomagnetic and solar indices, the model is history dependent on levels of geomagnetic and solar activity. The modeled electron density is continuous both spatially and temporally so that the evolution of the density can be studied (such as plasmaspheric refilling). The model is trained using the electron density inferred from the spacecraft potential from three THEMIS probes. The equatorial electron density is shown to be accurately reconstructed with a correlation coefficient of r 0.953 between data and model target. Since the model is history dependent, it succeeds in reconstructing various density features and dynamic behaviors, such as the quiet time plasmasphere, erosion and recovery of the plasmasphere, as well as the plume formation during a storm on 4 February 2011. Our model may provide unprecedented insight into the behavior of the equatorial density at any time and location; as an example we show the inferred refilling rate from our model and compare it to previous estimates.

Electron dynamics and prompt ablation of aluminum surface excited by intense femtosecond laser pulse

NASA Astrophysics Data System (ADS)

Ionin, A. A.; Kudryashov, S. I.; Makarov, S. V.; Seleznev, L. V.; Sinitsyn, D. V.

2014-12-01

Thin aluminum film homogeneously heated by intense IR femtosecond laser pulses exhibits on the excitation timescale consequent fluence-dependent rise and drop of the IR-pump self-reflectivity, followed by its final saturation at higher fluences F > 0.3 J/cm2. This prompt optical dynamics correlates with the initial monotonic increase in the accompanying laser-induced electron emission, which is succeeded by its non-linear (three-photon) increase for F > 0.3 J/cm2. The underlying electronic dynamics is related to the initial saturation of IR resonant interband transitions in this material, followed by its strong instantaneous electronic heating via intraband transitions during the pump pulse resulting in thermionic emission. Above the threshold fluence of 0.3 J/cm2, the surface electronic heating is balanced during the pump pulse by simultaneous cooling via intense plasma removal (prompt ablation). The relationship between the deposited volume energy density in the film and its prompt electronic temperature derived from the self-reflection measurements using a Drude model, demonstrates a kind of electron "liquid-vapor" phase transition, driven by strong cubic optical non-linearity of the photo-excited aluminum.

Generation of neutral and high-density electron-positron pair plasmas in the laboratory.

PubMed

Sarri, G; Poder, K; Cole, J M; Schumaker, W; Di Piazza, A; Reville, B; Dzelzainis, T; Doria, D; Gizzi, L A; Grittani, G; Kar, S; Keitel, C H; Krushelnick, K; Kuschel, S; Mangles, S P D; Najmudin, Z; Shukla, N; Silva, L O; Symes, D; Thomas, A G R; Vargas, M; Vieira, J; Zepf, M

2015-04-23

Electron-positron pair plasmas represent a unique state of matter, whereby there exists an intrinsic and complete symmetry between negatively charged (matter) and positively charged (antimatter) particles. These plasmas play a fundamental role in the dynamics of ultra-massive astrophysical objects and are believed to be associated with the emission of ultra-bright gamma-ray bursts. Despite extensive theoretical modelling, our knowledge of this state of matter is still speculative, owing to the extreme difficulty in recreating neutral matter-antimatter plasmas in the laboratory. Here we show that, by using a compact laser-driven setup, ion-free electron-positron plasmas with unique characteristics can be produced. Their charge neutrality (same amount of matter and antimatter), high-density and small divergence finally open up the possibility of studying electron-positron plasmas in controlled laboratory experiments.

Empirical STORM-E Model. [I. Theoretical and Observational Basis

NASA Technical Reports Server (NTRS)

Mertens, Christopher J.; Xu, Xiaojing; Bilitza, Dieter; Mlynczak, Martin G.; Russell, James M., III

2013-01-01

Auroral nighttime infrared emission observed by the Sounding of the Atmosphere using Broadband Emission Radiometry (SABER) instrument onboard the Thermosphere-Ionosphere-Mesosphere Energetics and Dynamics (TIMED) satellite is used to develop an empirical model of geomagnetic storm enhancements to E-region peak electron densities. The empirical model is called STORM-E and will be incorporated into the 2012 release of the International Reference Ionosphere (IRI). The proxy for characterizing the E-region response to geomagnetic forcing is NO+(v) volume emission rates (VER) derived from the TIMED/SABER 4.3 lm channel limb radiance measurements. The storm-time response of the NO+(v) 4.3 lm VER is sensitive to auroral particle precipitation. A statistical database of storm-time to climatological quiet-time ratios of SABER-observed NO+(v) 4.3 lm VER are fit to widely available geomagnetic indices using the theoretical framework of linear impulse-response theory. The STORM-E model provides a dynamic storm-time correction factor to adjust a known quiescent E-region electron density peak concentration for geomagnetic enhancements due to auroral particle precipitation. Part II of this series describes the explicit development of the empirical storm-time correction factor for E-region peak electron densities, and shows comparisons of E-region electron densities between STORM-E predictions and incoherent scatter radar measurements. In this paper, Part I of the series, the efficacy of using SABER-derived NO+(v) VER as a proxy for the E-region response to solar-geomagnetic disturbances is presented. Furthermore, a detailed description of the algorithms and methodologies used to derive NO+(v) VER from SABER 4.3 lm limb emission measurements is given. Finally, an assessment of key uncertainties in retrieving NO+(v) VER is presented

Real-Space Imaging of Carrier Dynamics of Materials Surfaces by Second-Generation Four-Dimensional Scanning Ultrafast Electron Microscopy.

PubMed

Sun, Jingya; Melnikov, Vasily A; Khan, Jafar I; Mohammed, Omar F

2015-10-01

In the fields of photocatalysis and photovoltaics, ultrafast dynamical processes, including carrier trapping and recombination on material surfaces, are among the key factors that determine the overall energy conversion efficiency. A precise knowledge of these dynamical events on the nanometer (nm) and femtosecond (fs) scales was not accessible until recently. The only way to access such fundamental processes fully is to map the surface dynamics selectively in real space and time. In this study, we establish a second generation of four-dimensional scanning ultrafast electron microscopy (4D S-UEM) and demonstrate the ability to record time-resolved images (snapshots) of material surfaces with 650 fs and ∼5 nm temporal and spatial resolutions, respectively. In this method, the surface of a specimen is excited by a clocking optical pulse and imaged using a pulsed primary electron beam as a probe pulse, generating secondary electrons (SEs), which are emitted from the surface of the specimen in a manner that is sensitive to the local electron/hole density. This method provides direct and controllable information regarding surface dynamics. We clearly demonstrate how the surface morphology, grains, defects, and nanostructured features can significantly impact the overall dynamical processes on the surface of photoactive-materials. In addition, the ability to access two regimes of dynamical probing in a single experiment and the energy loss of SEs in semiconductor-nanoscale materials will also be discussed.

Electron beam-plasma interaction and electron-acoustic solitary waves in a plasma with suprathermal electrons

NASA Astrophysics Data System (ADS)

Danehkar, A.

2018-06-01

Suprathermal electrons and inertial drifting electrons, so called electron beam, are crucial to the nonlinear dynamics of electrostatic solitary waves observed in several astrophysical plasmas. In this paper, the propagation of electron-acoustic solitary waves (EAWs) is investigated in a collisionless, unmagnetized plasma consisting of cool inertial background electrons, hot suprathermal electrons (modeled by a κ-type distribution), and stationary ions. The plasma is penetrated by a cool electron beam component. A linear dispersion relation is derived to describe small-amplitude wave structures that shows a weak dependence of the phase speed on the electron beam velocity and density. A (Sagdeev-type) pseudopotential approach is employed to obtain the existence domain of large-amplitude solitary waves, and investigate how their nonlinear structures depend on the kinematic and physical properties of the electron beam and the suprathermality (described by κ) of the hot electrons. The results indicate that the electron beam can largely alter the EAWs, but can only produce negative polarity solitary waves in this model. While the electron beam co-propagates with the solitary waves, the soliton existence domain (Mach number range) becomes narrower (nearly down to nil) with increasing the beam speed and the beam-to-hot electron temperature ratio, and decreasing the beam-to-cool electron density ratio in high suprathermality (low κ). It is found that the electric potential amplitude largely declines with increasing the beam speed and the beam-to-cool electron density ratio for co-propagating solitary waves, but is slightly decreased by raising the beam-to-hot electron temperature ratio.

Pairing from dynamically screened Coulomb repulsion in bismuth

NASA Astrophysics Data System (ADS)

Ruhman, Jonathan; Lee, Patrick A.

2017-12-01

Recently, Prakash et al. have discovered bulk superconductivity in single crystals of bismuth, which is a semimetal with extremely low carrier density. At such low density, we argue that conventional electron-phonon coupling is too weak to be responsible for the binding of electrons into Cooper pairs. We study a dynamically screened Coulomb interaction with effective attraction generated on the scale of the collective plasma modes. We model the electronic states in bismuth to include three Dirac pockets with high velocity and one hole pocket with a significantly smaller velocity. We find a weak-coupling instability, which is greatly enhanced by the presence of the hole pocket. Therefore we argue that bismuth is the first material to exhibit superconductivity driven by retardation effects of Coulomb repulsion alone. By using realistic parameters for bismuth we find that the acoustic plasma mode does not play the central role in pairing. We also discuss a matrix element effect, resulting from the Dirac nature of the conduction band, which may affect Tc in the s -wave channel without breaking time-reversal symmetry.

Tempo-spatially resolved dynamics of elec- trons and holes in bilayer MoS2 -WS2

NASA Astrophysics Data System (ADS)

Galicia-Hernandez, J. M.; Turkowski, V.; Hernandez-Cocoletzi, G.; Rahman, T. S.

We have performed a Density-Matrix Time-Dependent Density-Functional Theory analysis of the response of bilayer MoS2-WS2 to external laser-pulse perturbations. Time-resolved study of the dynamics of electrons and holes, including formation and dissociation of strongly-bound intra- and inter-layer excitonic states, shows that the experimentally observed ultrafast inter-layer MoS2 to WS2 migration of holes may be attributed to unusually large delocalization of the hole state which extends far into the inter-layer region. We also argue that the velocity of the hole transfer may be further enhanced by its interaction with transfer phonon modes. We analyze other possible consequences of the hole delocalization in the system, including reduction of the effects of the electron-electron and hole-hole repulsion in the trions and biexcitons as compared to that in the monolayers Work supported in part by DOE Grant No. DOE-DE-FG02-07ER46354 and by CONACYT Scholarship No. 23210 (J.M.G.H.).

X-ray Thomson Scattering in Warm Dense Matter without the Chihara Decomposition.

PubMed

Baczewski, A D; Shulenburger, L; Desjarlais, M P; Hansen, S B; Magyar, R J

2016-03-18

X-ray Thomson scattering is an important experimental technique used to measure the temperature, ionization state, structure, and density of warm dense matter (WDM). The fundamental property probed in these experiments is the electronic dynamic structure factor. In most models, this is decomposed into three terms [J. Chihara, J. Phys. F 17, 295 (1987)] representing the response of tightly bound, loosely bound, and free electrons. Accompanying this decomposition is the classification of electrons as either bound or free, which is useful for gapped and cold systems but becomes increasingly questionable as temperatures and pressures increase into the WDM regime. In this work we provide unambiguous first principles calculations of the dynamic structure factor of warm dense beryllium, independent of the Chihara form, by treating bound and free states under a single formalism. The computational approach is real-time finite-temperature time-dependent density functional theory (TDDFT) being applied here for the first time to WDM. We compare results from TDDFT to Chihara-based calculations for experimentally relevant conditions in shock-compressed beryllium.

Clocking Femtosecond Collisional Dynamics via Resonant X-Ray Spectroscopy

NASA Astrophysics Data System (ADS)

van den Berg, Q. Y.; Fernandez-Tello, E. V.; Burian, T.; Chalupský, J.; Chung, H.-K.; Ciricosta, O.; Dakovski, G. L.; Hájková, V.; Hollebon, P.; Juha, L.; Krzywinski, J.; Lee, R. W.; Minitti, M. P.; Preston, T. R.; de la Varga, A. G.; Vozda, V.; Zastrau, U.; Wark, J. S.; Velarde, P.; Vinko, S. M.

2018-02-01

Electron-ion collisional dynamics is of fundamental importance in determining plasma transport properties, nonequilibrium plasma evolution, and electron damage in diffraction imaging applications using bright x-ray free-electron lasers (FELs). Here we describe the first experimental measurements of ultrafast electron impact collisional ionization dynamics using resonant core-hole spectroscopy in a solid-density magnesium plasma, created and diagnosed with the Linac Coherent Light Source x-ray FEL. By resonantly pumping the 1 s →2 p transition in highly charged ions within an optically thin plasma, we have measured how off-resonance charge states are populated via collisional processes on femtosecond time scales. We present a collisional cross section model that matches our results and demonstrates how the cross sections are enhanced by dense-plasma effects including continuum lowering. Nonlocal thermodynamic equilibrium collisional radiative simulations show excellent agreement with the experimental results and provide new insight on collisional ionization and three-body-recombination processes in the dense-plasma regime.

Clocking Femtosecond Collisional Dynamics via Resonant X-Ray Spectroscopy

DOE PAGES

van den Berg, Q. Y.; Fernandez-Tello, E. V.; Burian, T.; ...

2018-02-01

Electron-ion collisional dynamics is of fundamental importance in determining plasma transport properties, nonequilibrium plasma evolution, and electron damage in diffraction imaging applications using bright x-ray free-electron lasers (FELs). Here in this paper, we describe the first experimental measurements of ultrafast electron impact collisional ionization dynamics using resonant core-hole spectroscopy in a solid-density magnesium plasma, created and diagnosed with the Linac Coherent Light Source x-ray FEL. By resonantly pumping the 1s → 2p transition in highly charged ions within an optically thin plasma, we have measured how off-resonance charge states are populated via collisional processes on femtosecond time scales. We presentmore » a collisional cross section model that matches our results and demonstrates how the cross sections are enhanced by dense-plasma effects including continuum lowering. Nonlocal thermodynamic equilibrium collisional radiative simulations show excellent agreement with the experimental results and provide new insight on collisional ionization and three-body-recombination processes in the dense-plasma regime.« less

Exploration of dynamical regimes of irradiated small protonated water clusters

NASA Astrophysics Data System (ADS)

Ndongmouo Taffoti, U. F.; Dinh, P. M.; Reinhard, P.-G.; Suraud, E.; Wang, Z. P.

2010-05-01

We explore from a theoretical perspective the dynamical response of small water clusters, (H2O)nH3O+ with n=1,2,3, to a short laser pulse for various frequencies, from infrared (IR) to ultra-violet (UV) and intensities (from 6×10^{13} W/cm^2 to 5×10^{14} W/cm^2). To that end, we use time-dependent local-density approximation for the electrons, coupled to molecular dynamics for the atomic cores (TDLDA-MD). The local-density approximation is augmented by a self-interaction correction (SIC) to allow for a correct description of electron emission. For IR frequencies, we see a direct coupling of the laser field to the very light H+ ions in the clusters. Resonant coupling (in the UV) and/or higher intensities lead to fast ionization with subsequent Coulomb explosion. The stability against Coulomb pressure increases with system size. Excitation to lower ionization stages induced strong ionic vibrations. The latter maintain a rather harmonic pattern in spite of the sizeable amplitudes (often 10% of the bond length).

Self-consistent Green's function embedding for advanced electronic structure methods based on a dynamical mean-field concept

NASA Astrophysics Data System (ADS)

Chibani, Wael; Ren, Xinguo; Scheffler, Matthias; Rinke, Patrick

2016-04-01

We present an embedding scheme for periodic systems that facilitates the treatment of the physically important part (here a unit cell or a supercell) with advanced electronic structure methods, that are computationally too expensive for periodic systems. The rest of the periodic system is treated with computationally less demanding approaches, e.g., Kohn-Sham density-functional theory, in a self-consistent manner. Our scheme is based on the concept of dynamical mean-field theory formulated in terms of Green's functions. Our real-space dynamical mean-field embedding scheme features two nested Dyson equations, one for the embedded cluster and another for the periodic surrounding. The total energy is computed from the resulting Green's functions. The performance of our scheme is demonstrated by treating the embedded region with hybrid functionals and many-body perturbation theory in the GW approach for simple bulk systems. The total energy and the density of states converge rapidly with respect to the computational parameters and approach their bulk limit with increasing cluster (i.e., computational supercell) size.

Electron density and plasma dynamics of a spherical theta pinch

NASA Astrophysics Data System (ADS)

Teske, C.; Liu, Y.; Blaes, S.; Jacoby, J.

2012-03-01

A spherical theta pinch for plasma stripper applications has been developed and investigated regarding the electron density and the plasma confinement during the pinching sequence. The setup consists of a 6 μH induction coil surrounding a 4000 ml spherical discharge vessel and a capacitor bank with interchangeable capacitors leading to an overall capacitance of 34 μF and 50 μF, respectively. A thyristor switch is used for driving the resonant circuit. Pulsed coil currents reached values of up to 26 kA with maximum induction of 500 mT. Typical gas pressures were 0.7 Pa up to 120 Pa with ArH2 (2.8% H2)-gas as a discharge medium. Stark broadening measurements of the Hβ emission line were carried out in order to evaluate the electron density of the discharge. In accordance with the density measurements, the transfer efficiency was estimated and a scaling law between electron density and discharge energy was established for the current setup. The densities reached values of up to 8 × 1022 m-3 for an energy of 1.6 kJ transferred into the plasma. Further, the pinching of the discharge plasma was documented and the different stages of the pinching process were analyzed. The experimental evidence suggests that concerning the recent setup of the spherical theta pinch, a linear scaling law between the transferred energy and the achievable plasma density can be applied for various applications like plasma strippers and pulsed ion sources.

Electron-acoustic solitary waves in dense quantum electron-ion plasmas

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

Misra, A. P.; Shukla, P. K.; Bhowmik, C.

2007-08-15

A quantum hydrodynamic (QHD) model is used to investigate the propagation characteristics of nonlinear electron-acoustic solitary waves (EASWs) in a dense quantum plasma whose constituents are two groups of electrons: one inertial cold electrons and other inertialess hot electrons, and the stationary ions which form the neutralizing background. By using the standard reductive perturbation technique, a Kadomtsev-Petviashvili (KP) equation, which governs the dynamics of EASWs, is derived in both spherical and cylindrical geometry. The effects of cold electrons and the density correlations due to quantum fluctuations on the profiles of the amplitudes and widths of the solitary structures are examinedmore » numerically. The nondimensional parameter {delta}=n{sub c0}/n{sub h0}, which is the equilibrium density ratio of the cold to hot electron component, is shown to play a vital role in the formation of both bright and dark solitons. It is also found that the angular dependence of the physical quantities and the presence of cold electrons in a quantum plasma lead to the coexistence of some new interesting novel solitary structures quite distinctive from the classical ones.« less

Decoupled electron and phonon transports in hexagonal boron nitride-silicene bilayer heterostructure

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

Cai, Yongqing; Pei, Qing-Xiang, E-mail: peiqx@ihpc.a-star.edu.sg, E-mail: zhangg@ihpc.a-star.edu.sg; Zhang, Gang, E-mail: peiqx@ihpc.a-star.edu.sg, E-mail: zhangg@ihpc.a-star.edu.sg

2016-02-14

Calculations based on the density functional theory and empirical molecular dynamics are performed to investigate interlayer interaction, electronic structure and thermal transport of a bilayer heterostructure consisting of silicene and hexagonal boron nitride (h-BN). In this heterostructure, the two layers are found to interact weakly via a non-covalent binding. As a result, the Dirac cone of silicene is preserved with the Dirac cone point being located exactly at the Fermi level, and only a small amount of electrons are transferred from h-BN to silicene, suggesting that silicene dominates the electronic transport. Molecular dynamics calculation results demonstrate that the heat currentmore » along h-BN is six times of that along silicene, suggesting that h-BN dominates the thermal transport. This decoupled role of h-BN and silicene in thermal and electronic transport suggests that the BN-silicene bilayer heterostructure is promising for thermoelectric applications.« less

Spin noise spectroscopy of donor-bound electrons in ZnO

NASA Astrophysics Data System (ADS)

Horn, H.; Balocchi, A.; Marie, X.; Bakin, A.; Waag, A.; Oestreich, M.; Hübner, J.

2013-01-01

We investigate the intrinsic spin dynamics of electrons bound to Al impurities in bulk ZnO by optical spin noise spectroscopy. Spin noise spectroscopy enables us to investigate the longitudinal and transverse spin relaxation time with respect to nuclear and external magnetic fields in a single spectrum. On one hand, the spin dynamic is dominated by the intrinsic hyperfine interaction with the nuclear spins of the naturally occurring 67Zn isotope. We measure a typical spin dephasing time of 23 ns, in agreement with the expected theoretical values. On the other hand, we measure a third, very high spin dephasing rate which is attributed to a high defect density of the investigated ZnO material. Measurements of the spin dynamics under the influence of transverse as well as longitudinal external magnetic fields unambiguously reveal the intriguing connections of the electron spin with its nuclear and structural environment.

Mode Specific Electronic Friction in Dissociative Chemisorption on Metal Surfaces: H2 on Ag(111)

NASA Astrophysics Data System (ADS)

Maurer, Reinhard J.; Jiang, Bin; Guo, Hua; Tully, John C.

2017-06-01

Electronic friction and the ensuing nonadiabatic energy loss play an important role in chemical reaction dynamics at metal surfaces. Using molecular dynamics with electronic friction evaluated on the fly from density functional theory, we find strong mode dependence and a dominance of nonadiabatic energy loss along the bond stretch coordinate for scattering and dissociative chemisorption of H2 on the Ag(111) surface. Exemplary trajectories with varying initial conditions indicate that this mode specificity translates into modulated energy loss during a dissociative chemisorption event. Despite minor nonadiabatic energy loss of about 5%, the directionality of friction forces induces dynamical steering that affects individual reaction outcomes, specifically for low-incidence energies and vibrationally excited molecules. Mode-specific friction induces enhanced loss of rovibrational rather than translational energy and will be most visible in its effect on final energy distributions in molecular scattering experiments.

Dynamic diffraction effects and coherent breathing oscillations in ultrafast electron diffraction in layered 1T-TaSeTe

PubMed Central

Wei, Linlin; Sun, Shuaishuai; Guo, Cong; Li, Zhongwen; Sun, Kai; Liu, Yu; Lu, Wenjian; Sun, Yuping; Tian, Huanfang; Yang, Huaixin; Li, Jianqi

2017-01-01

Anisotropic lattice movements due to the difference between intralayer and interlayer bonding are observed in the layered transition-metal dichalcogenide 1T-TaSeTe following femtosecond laser pulse excitation. Our ultrafast electron diffraction investigations using 4D-transmission electron microscopy (4D-TEM) clearly reveal that the intensity of Bragg reflection spots often changes remarkably due to the dynamic diffraction effects and anisotropic lattice movement. Importantly, the temporal diffracted intensity from a specific crystallographic plane depends on the deviation parameter s, which is commonly used in the theoretical study of diffraction intensity. Herein, we report on lattice thermalization and structural oscillations in layered 1T-TaSeTe, analyzed by dynamic diffraction theory. Ultrafast alterations of satellite spots arising from the charge density wave in the present system are also briefly discussed. PMID:28470025

Three-dimensional structural dynamics and fluctuations of DNA-nanogold conjugates by individual-particle electron tomography

DOE PAGES

Zhang, Lei; Lei, Dongsheng; Smith, Jessica M.; ...

2016-03-30

DNA base pairing has been used for many years to direct the arrangement of inorganic nanocrystals into small groupings and arrays with tailored optical and electrical properties. The control of DNA-mediated assembly depends crucially on a better understanding of three-dimensional structure of DNA-nanocrystal-hybridized building blocks. Existing techniques do not allow for structural determination of these flexible and heterogeneous samples. Here we report cryo-electron microscopy and negative-staining electron tomography approaches to image, and three-dimensionally reconstruct a single DNA-nanogold conjugate, an 84-bp double-stranded DNA with two 5-nm nanogold particles for potential substrates in plasmon-coupling experiments. By individual-particle electron tomography reconstruction, we obtainmore » 14 density maps at ~ 2-nm resolution . Using these maps as constraints, we derive 14 conformations of dsDNA by molecular dynamics simulations. The conformational variation is consistent with that from liquid solution, suggesting that individual-particle electron tomography could be an expected approach to study DNA-assembling and flexible protein structure and dynamics.« less

Uncovering Highly-Excited State Mixing in Acetone Using Ultrafast VUV Pulses and Coincidence Imaging Techniques

DOE PAGES

Couch, David E.; Kapteyn, Henry C.; Murnane, Margaret M.; ...

2017-03-17

Here, understanding the ultrafast dynamics of highly-excited electronic states of small molecules is critical for a better understanding of atmospheric and astrophysical processes, as well as for designing coherent control strategies for manipulating chemical dynamics. In highly excited states, nonadiabatic coupling, electron-electron interactions, and the high density of states govern dynamics. However, these states are computationally and experimentally challenging to access. Fortunately, new sources of ultrafast vacuum ultraviolet pulses, in combination with electron-ion coincidence spectroscopies, provide new tools to unravel the complex electronic landscape. Here we report time-resolved photoelectron-photoion coincidence experiments using 8 eV pump photons to study the highlymore » excited states of acetone. We uncover for the first time direct evidence that the resulting excited state consists of a mixture of both n y → 3p and π → π* character, which decays with a time constant of 330 fs. In the future, this approach can inform models of VUV photochemistry and aid in designing coherent control strategies for manipulating chemical reactions.« less

Uncovering Highly-Excited State Mixing in Acetone Using Ultrafast VUV Pulses and Coincidence Imaging Techniques

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

Couch, David E.; Kapteyn, Henry C.; Murnane, Margaret M.

Here, understanding the ultrafast dynamics of highly-excited electronic states of small molecules is critical for a better understanding of atmospheric and astrophysical processes, as well as for designing coherent control strategies for manipulating chemical dynamics. In highly excited states, nonadiabatic coupling, electron-electron interactions, and the high density of states govern dynamics. However, these states are computationally and experimentally challenging to access. Fortunately, new sources of ultrafast vacuum ultraviolet pulses, in combination with electron-ion coincidence spectroscopies, provide new tools to unravel the complex electronic landscape. Here we report time-resolved photoelectron-photoion coincidence experiments using 8 eV pump photons to study the highlymore » excited states of acetone. We uncover for the first time direct evidence that the resulting excited state consists of a mixture of both n y → 3p and π → π* character, which decays with a time constant of 330 fs. In the future, this approach can inform models of VUV photochemistry and aid in designing coherent control strategies for manipulating chemical reactions.« less

Classical molecular dynamics simulation of electronically non-adiabatic processes.

PubMed

Miller, William H; Cotton, Stephen J

2016-12-22

Both classical and quantum mechanics (as well as hybrids thereof, i.e., semiclassical approaches) find widespread use in simulating dynamical processes in molecular systems. For large chemical systems, however, which involve potential energy surfaces (PES) of general/arbitrary form, it is usually the case that only classical molecular dynamics (MD) approaches are feasible, and their use is thus ubiquitous nowadays, at least for chemical processes involving dynamics on a single PES (i.e., within a single Born-Oppenheimer electronic state). This paper reviews recent developments in an approach which extends standard classical MD methods to the treatment of electronically non-adiabatic processes, i.e., those that involve transitions between different electronic states. The approach treats nuclear and electronic degrees of freedom (DOF) equivalently (i.e., by classical mechanics, thereby retaining the simplicity of standard MD), and provides "quantization" of the electronic states through a symmetrical quasi-classical (SQC) windowing model. The approach is seen to be capable of treating extreme regimes of strong and weak coupling between the electronic states, as well as accurately describing coherence effects in the electronic DOF (including the de-coherence of such effects caused by coupling to the nuclear DOF). A survey of recent applications is presented to illustrate the performance of the approach. Also described is a newly developed variation on the original SQC model (found universally superior to the original) and a general extension of the SQC model to obtain the full electronic density matrix (at no additional cost/complexity).

Reaction Dynamics at Liquid Interfaces

NASA Astrophysics Data System (ADS)

Benjamin, Ilan

2015-04-01

The liquid interface is a narrow, highly anisotropic region, characterized by rapidly varying density, polarity, and molecular structure. I review several aspects of interfacial solvation and show how these affect reactivity at liquid/liquid interfaces. I specifically consider ion transfer, electron transfer, and SN2 reactions, showing that solvent effects on these reactions can be understood by examining the unique structure and dynamics of the liquid interface region.

Morphologic and proteomic characterization of exosomes released by cultured extravillous trophoblast cells

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

Atay, Safinur; Gercel-Taylor, Cicek; Kesimer, Mehmet

Exosomes represent an important intercellular communication vehicle, mediating events essential for the decidual microenvironment. While we have demonstrated exosome induction of pro-inflammatory cytokines, to date, no extensive characterization of trophoblast-derived exosomes has been provided. Our objective was to provide a morphologic and proteomic characterization of these exosomes. Exosomes were isolated from the conditioned media of Swan71 human trophoblast cells by ultrafiltration and ultracentrifugation. These were analyzed for density (sucrose density gradient centrifugation), morphology (electron microscopy), size (dynamic light scattering) and protein composition (Ion Trap mass spectrometry and western immunoblotting). Based on density gradient centrifugation, microvesicles from Sw71 cells exhibit amore » density between 1.134 and 1.173 g/ml. Electron microscopy demonstrated that microvesicles from Sw71 cells exhibit the characteristic cup-shaped morphology of exosomes. Dynamic light scattering showed a bell-shaped curve, indicating a homogeneous population with a mean size of 165 nm {+-} 0.5 nm. Ion Trap mass spectrometry demonstrated the presence of exosome marker proteins (including CD81, Alix, cytoskeleton related proteins, and Rab family). The MS results were confirmed by western immunoblotting. Based on morphology, density, size and protein composition, we defined the release of exosomes from extravillous trophoblast cells and provide their first extensive characterization. This characterization is essential in furthering our understanding of 'normal' early pregnancy.« less

Magnetic behavior study of samarium nitride using density functional theory

NASA Astrophysics Data System (ADS)

Som, Narayan N.; Mankad, Venu H.; Dabhi, Shweta D.; Patel, Anjali; Jha, Prafulla K.

2018-02-01

In this work, the state-of-art density functional theory is employed to study the structural, electronic and magnetic properties of samarium nitride (SmN). We have performed calculation for both ferromagnetic and antiferromagnetic states in rock-salt phase. The calculated results of optimized lattice parameter and magnetic moment agree well with the available experimental and theoretical values. From energy band diagram and electronic density of states, we observe a half-metallic behaviour in FM phase of rock salt SmN in while metallicity in AFM I and AFM III phases. We present and discuss our current understanding of the possible half-metallicity together with the magnetic ordering in SmN. The calculated phonon dispersion curves shows dynamical stability of the considered structures. The phonon density of states and Eliashberg functional have also been analysed to understand the superconductivity in SmN.

On the Relation Between Soft Electron Precipitations in the Cusp Region and Solar Wind Coupling Functions

NASA Astrophysics Data System (ADS)

Dang, Tong; Zhang, Binzheng; Wiltberge, Michael; Wang, Wenbin; Varney, Roger; Dou, Xiankang; Wan, Weixing; Lei, Jiuhou

2018-01-01

In this study, the correlations between the fluxes of precipitating soft electrons in the cusp region and solar wind coupling functions are investigated utilizing the Lyon-Fedder-Mobarry global magnetosphere model simulations. We conduct two simulation runs during periods from 20 March 2008 to 16 April 2008 and from 15 to 24 December 2014, which are referred as "Equinox Case" and "Solstice Case," respectively. The simulation results of Equinox Case show that the plasma number density in the high-latitude cusp region scales well with the solar wind number density (ncusp/nsw=0.78), which agrees well with the statistical results from the Polar spacecraft measurements. For the Solstice Case, the plasma number density of high-latitude cusp in both hemispheres increases approximately linearly with upstream solar wind number density with prominent hemispheric asymmetry. Due to the dipole tilt effect, the average number density ratio ncusp/nsw in the Southern (summer) Hemisphere is nearly 3 times that in the Northern (winter) Hemisphere. In addition to the solar wind number density, 20 solar wind coupling functions are tested for the linear correlation with the fluxes of precipitating cusp soft electrons. The statistical results indicate that the solar wind dynamic pressure p exhibits the highest linear correlation with the cusp electron fluxes for both equinox and solstice conditions, with correlation coefficients greater than 0.75. The linear regression relations for equinox and solstice cases may provide an empirical calculation for the fluxes of cusp soft electron precipitation based on the upstream solar wind driving conditions.

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

PubMed

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

2018-05-11

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

One-Dimensional Hybrid Satellite Track Model for the Dynamics Explorer 2 (DE 2) Satellite

NASA Technical Reports Server (NTRS)

Deng, Wei; Killeen, T. L.; Burns, A. G.; Johnson, R. M.; Emery, B. A.; Roble, R. G.; Winningham, J. D.; Gary, J. B.

1995-01-01

A one-dimensional hybrid satellite track model has been developed to calculate the high-latitude thermospheric/ionospheric structure below the satellite altitude using Dynamics Explorer 2 (DE 2) satellite measurements and theory. This model is based on Emery et al. satellite track code but also includes elements of Roble et al. global mean thermosphere/ionosphere model. A number of parameterizations and data handling techniques are used to input satellite data from several DE 2 instruments into this model. Profiles of neutral atmospheric densities are determined from the MSIS-90 model and measured neutral temperatures. Measured electron precipitation spectra are used in an auroral model to calculate particle impact ionization rates below the satellite. These rates are combined with a solar ionization rate profile and used to solve the O(+) diffusion equation, with the measured electron density as an upper boundary condition. The calculated O(+) density distribution, as well as the ionization profiles, are then used in a photochemical equilibrium model to calculate the electron and molecular ion densities. The electron temperature is also calculated by solving the electron energy equation with an upper boundary condition determined by the DE 2 measurement. The model enables calculations of altitude profiles of conductivity and Joule beating rate along and below the satellite track. In a first application of the new model, a study is made of thermospheric and ionospheric structure below the DE 2 satellite for a single orbit which occurred on October 25, 1981. The field-aligned Poynting flux, which is independently obtained for this orbit, is compared with the model predictions of the height-integrated energy conversion rate. Good quantitative agreement between these two estimates has been reached. In addition, measurements taken at the incoherent scatter radar site at Chatanika (65.1 deg N, 147.4 deg W) during a DE 2 overflight are compared with the model calculations. A good agreement was found in lower thermospheric conductivities and Joule heating rate.

Communication: a density functional with accurate fractional-charge and fractional-spin behaviour for s-electrons.

PubMed

Johnson, Erin R; Contreras-García, Julia

2011-08-28

We develop a new density-functional approach combining physical insight from chemical structure with treatment of multi-reference character by real-space modeling of the exchange-correlation hole. We are able to recover, for the first time, correct fractional-charge and fractional-spin behaviour for atoms of groups 1 and 2. Based on Becke's non-dynamical correlation functional [A. D. Becke, J. Chem. Phys. 119, 2972 (2003)] and explicitly accounting for core-valence separation and pairing effects, this method is able to accurately describe dissociation and strong correlation in s-shell many-electron systems. © 2011 American Institute of Physics

Collective charge excitations and the metal-insulator transition in the square lattice Hubbard-Coulomb model

DOE PAGES

Ulybyshev, Maksim; Winterowd, Christopher; Zafeiropoulos, Savvas

2017-11-09

Here in this article, we discuss the nontrivial collective charge excitations (plasmons) of the extended square lattice Hubbard model. Using a fully nonperturbative approach, we employ the hybrid Monte Carlo algorithm to simulate the system at half-filling. A modified Backus-Gilbert method is introduced to obtain the spectral functions via numerical analytic continuation. We directly compute the single-particle density of states which demonstrates the formation of Hubbard bands in the strongly correlated phase. The momentum-resolved charge susceptibility also is computed on the basis of the Euclidean charge-density-density correlator. In agreement with previous extended dynamical mean-field theory studies, we find that, atmore » high strength of the electron-electron interaction, the plasmon dispersion develops two branches.« less

Collective charge excitations and the metal-insulator transition in the square lattice Hubbard-Coulomb model

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

Ulybyshev, Maksim; Winterowd, Christopher; Zafeiropoulos, Savvas

Here in this article, we discuss the nontrivial collective charge excitations (plasmons) of the extended square lattice Hubbard model. Using a fully nonperturbative approach, we employ the hybrid Monte Carlo algorithm to simulate the system at half-filling. A modified Backus-Gilbert method is introduced to obtain the spectral functions via numerical analytic continuation. We directly compute the single-particle density of states which demonstrates the formation of Hubbard bands in the strongly correlated phase. The momentum-resolved charge susceptibility also is computed on the basis of the Euclidean charge-density-density correlator. In agreement with previous extended dynamical mean-field theory studies, we find that, atmore » high strength of the electron-electron interaction, the plasmon dispersion develops two branches.« less

Ultra-stiff metallic glasses through bond energy density design.

PubMed

Schnabel, Volker; Köhler, Mathias; Music, Denis; Bednarcik, Jozef; Clegg, William J; Raabe, Dierk; Schneider, Jochen M

2017-07-05

The elastic properties of crystalline metals scale with their valence electron density. Similar observations have been made for metallic glasses. However, for metallic glasses where covalent bonding predominates, such as metalloid metallic glasses, this relationship appears to break down. At present, the reasons for this are not understood. Using high energy x-ray diffraction analysis of melt spun and thin film metallic glasses combined with density functional theory based molecular dynamics simulations, we show that the physical origin of the ultrahigh stiffness in both metalloid and non-metalloid metallic glasses is best understood in terms of the bond energy density. Using the bond energy density as novel materials design criterion for ultra-stiff metallic glasses, we are able to predict a Co 33.0 Ta 3.5 B 63.5 short range ordered material by density functional theory based molecular dynamics simulations with a high bond energy density of 0.94 eV Å -3 and a bulk modulus of 263 GPa, which is 17% greater than the stiffest Co-B based metallic glasses reported in literature.

Covariant Formulation of Fluid Dynamics and Estakhr's Material Geodesic Equation, far down the Rabbit hole

NASA Astrophysics Data System (ADS)

Estakhr, Ahmad Reza

2012-07-01

``When i meet God, I am going to ask him two questions, why relativity and why turbulence. A. Einstein'' You probably will not need to ask these questions of God, I've already answered both of them. U^{μ}=γ (c,u({r}, t)) denotes four-velocity field. J^ {μ}=ρ U^{μ} denotes four-current mass density. Estakhr's Material-Geodesic equation is developed analogy of Navier Stokes equation and Einstein Geodesic equation. {DJ^ {μ}}/{Dτ}={dJ^{μ}}/{D τ}+Γ^{μ}_{α β}J^{α}U^{β}=J_ {ν}Ω^{μν}+npartial_ {ν}T^{μν}+Γ^{μ} _{αβ}J^{α}U^{β} Covariant formulation of fluid dynamics, describe the motion of fluid substances. The local existence and uniqueness theorem for geodesics states that geodesics on a smooth manifold with an affine connection exist, and are unique. EMG equation is also applicable in different branches of physics, it all depend on what you mean by 4-current density, if you mean 4-current electron number density then it is plasma physics, if you mean 4-current electron charge density then it is {DJ^ {μ}}/{Dτ}=J_{ν}F^{μν} +partial_{ν}T^{μν}+ Γ^{μ}_{αβ}J^ {α}U^{β} electromagnetism.

III-Nitride, SiC and Diamond Materials for Electronic Devices. Symposium Held April 8-12 1996, San Francisco, California, U.S.A. Volume 423.

DTIC Science & Technology

1996-12-01

gallium, nitrogen and gallium nitride structures. Thus it can be shown to be transferable and efficient for predictive molecular -dynamic simulations on...potentials and forces for the molecular dynamics simulations are derived by means of a density-functional based nonorthogonal tight-binding (DF-TB) scheme...LDA). Molecular -dynamics simulations for determining the different reconstructions of the SiC surface use the slab method (two-dimensional periodic

Reconstruction of the ionospheric electron density by geostatistical inversion

NASA Astrophysics Data System (ADS)

Minkwitz, David; van den Boogaart, Karl Gerald; Hoque, Mainul; Gerzen, Tatjana

2015-04-01

The ionosphere is the upper part of the atmosphere where sufficient free electrons exist to affect the propagation of radio waves. Typically, the ionosphere extends from about 50 - 1000 km and its morphology is mainly driven by solar radiation, particle precipitation and charge exchange. Due to the strong ionospheric impact on many applications dealing with trans-ionospheric signals such as Global Navigation Satellite Systems (GNSS) positioning, navigation and remote sensing, the demand for a highly accurate reconstruction of the electron density is ever increasing. Within the Helmholtz Alliance project "Remote Sensing and Earth System Dynamics" (EDA) the utilization of the upcoming radar mission TanDEM-L and its related products are prepared. The TanDEM-L mission will operate in L-band with a wavelength of approximately 24 cm and aims at an improved understanding of environmental processes and ecosystem change, e.g. earthquakes, volcanos, glaciers, soil moisture and carbon cycle. Since its lower frequency compared to the X-band (3 cm) and C-band (5 cm) radar missions, the influence of the ionosphere will increase and might lead to a significant degradation of the radar image quality if no correction is applied. Consequently, our interest is the reconstruction of the ionospheric electron density in order to mitigate the ionospheric delay. Following the ionosphere's behaviour we establish a non-stationary and anisotropic spatial covariance model of the electron density separated into a vertical and horizontal component. In order to estimate the model's parameters we chose a maximum likelihood approach. This approach incorporates GNSS total electron content measurements, representing integral measurements of the electron density between satellite to receiver ray paths, and the NeQuick model as a non-stationary trend. Based on a multivariate normal distribution the spatial covariance model parameters are optimized and afterwards the 3D electron density can be calculated by kriging for arbitrary points or grids of interest.

Comparison of electron transport calculations in warm dense matter using the Ziman formula

DOE PAGES

Burrill, D. J.; Feinblum, D. V.; Charest, M. R. J.; ...

2016-02-10

The Ziman formulation of electrical conductivity is tested in warm and hot dense matter using the pseudo-atom molecular dynamics method. Several implementation options that have been widely used in the literature are systematically tested through a comparison to the accurate, but expensive Kohn–Sham density functional theory molecular dynamics (KS-DFT-MD) calculations. As a result, the comparison is made for several elements and mixtures and for a wide range of temperatures and densities, and reveals a preferred method that generally gives very good agreement with the KS-DFT-MD results, but at a fraction of the computational cost.

Fast and accurate quantum molecular dynamics of dense plasmas across temperature regimes

DOE PAGES

Sjostrom, Travis; Daligault, Jerome

2014-10-10

Here, we develop and implement a new quantum molecular dynamics approximation that allows fast and accurate simulations of dense plasmas from cold to hot conditions. The method is based on a carefully designed orbital-free implementation of density functional theory. The results for hydrogen and aluminum are in very good agreement with Kohn-Sham (orbital-based) density functional theory and path integral Monte Carlo calculations for microscopic features such as the electron density as well as the equation of state. The present approach does not scale with temperature and hence extends to higher temperatures than is accessible in the Kohn-Sham method and lowermore » temperatures than is accessible by path integral Monte Carlo calculations, while being significantly less computationally expensive than either of those two methods.« less

Ionising sources in the coma of 67P probed by Rosetta

NASA Astrophysics Data System (ADS)

Heritier, Kevin; Galand, Marina; Henri, Pierre; Eriksson, Anders; Odelstad, Elias; Altwegg, Kathrin; Beth, Arnaud; Broiles, Thomas; Burch, Jim; Carr, Christopher; Cupido, Emanuele; Glassmeier, Karl-Heinz; Nilsson, Hans; Richter, Ingo; Rubin, Martin; Vallieres, Xavier; Vigren, Erik

2017-04-01

An ionospheric model has been developed in order to quantify the ion number density in the coma of 67P/Churyumov-Gerasimenko. The model is driven by Rosetta Orbiter Spectrometer for Ion and Neutral Analysis (ROSINA)/Cometary Pressure Sensor (COPS) neutral density and assumes isentropic expansion for the neutral density profile. The two ionisation sources considered are photo-ionisation by solar extreme ultraviolet (EUV) radiation and electron-impact ionisation. The EUV radiation is estimated from fluxes measured by the Thermosphere Ionosphere Mesosphere Energetics and Dynamics (TIMED)/ Solar EUV Experiment (SEE), taking into account the phase shift and the heliocentric distance ratio; between Earth and comet 67P. The electron-impact ionisation production rates are derived from Rosetta Plasma Consortium (RPC)-Ion and Electron Sensor (IES) integrated electron fluxes and corrected for the S/C potential from RPC/LAngmuir Probe (LAP) measurements. Our results are compared with in situ measurements of the plasma density from RPC-Mutual Impedance Probe (MIP) and RPC-LAP. There is a good agreement between the modelled and RPC observed electron densities. The ionospheric model enables to distinguish the relative contributions of the different sources to the total cometary plasma. At high heliocentric distances, electron-impact ionisation becomes the dominant ionisation source and is enhanced over the winter hemisphere. As the solar activity has decreased since the beginning of the mission in 2014, the relative importance of photo-ionisation has decreased as well. However, at low heliocentric distances, photo-ionisation seems to be the most dominant ionising source, in particular through the perihelion period in summer 2015.

Physics based model of D-region variability related to VLF propagation effects

NASA Astrophysics Data System (ADS)

Chakravarty, S. C.

2012-07-01

D-region (~60-85 km) electron density profiles measured using large number of sounding rocket experiments carried out from two Indian low latitude stations show large variations with solar zenith angle, season and solar activity. Similarly the ground based multi frequency radio wave absorption technique has provided continuous data on the morphology of the hourly electron density variations. However suitable models of the D-region electron density profile variations both during quiet and disturbed solar conditions over the Indian region are lacking. The renewed interest in the study of the VLF/LF propagation anomalies taking place through perturbations in the D-region electron densities due to various geophysical phenomena requires the availability of a baseline D-region model over low latitudes. The purpose of this paper is to critically review the physical processes of D-region production and loss of free electrons, dynamical coupling due to variety of vertically propagating atmospheric waves, sudden changes brought about by the solar energetic events like CMEs and different categories of X-ray flares. Low latitude region is not likely to be affected by the PMSE or PCA type of events but the changes due to lightning induced mesospheric red sprites and LEPs need to be considered. Based on this analysis, a preliminary low latitude D-region electron density profile model development is proposed. Sample results would illustrate key requirements from such a model in terms of its effectiveness to simulate the low latitude observations of VLF/LF amplitude and phase variations using waveguide propagation models like LWPC.

Resolving the role of femtosecond heated electrons in ultrafast spin dynamics.

PubMed

Mendil, J; Nieves, P; Chubykalo-Fesenko, O; Walowski, J; Santos, T; Pisana, S; Münzenberg, M

2014-02-05

Magnetization manipulation is essential for basic research and applications. A fundamental question is, how fast can the magnetization be reversed in nanoscale magnetic storage media. When subject to an ultrafast laser pulse, the speed of the magnetization dynamics depends on the nature of the energy transfer pathway. The order of the spin system can be effectively influenced through spin-flip processes mediated by hot electrons. It has been predicted that as electrons drive spins into the regime close to almost total demagnetization, characterized by a loss of ferromagnetic correlations near criticality, a second slower demagnetization process takes place after the initial fast drop of magnetization. By studying FePt, we unravel the fundamental role of the electronic structure. As the ferromagnet Fe becomes more noble in the FePt compound, the electronic structure is changed and the density of states around the Fermi level is reduced, thereby driving the spin correlations into the limit of critical fluctuations. We demonstrate the impact of the electrons and the ferromagnetic interactions, which allows a general insight into the mechanisms of spin dynamics when the ferromagnetic state is highly excited, and identifies possible recording speed limits in heat-assisted magnetization reversal.

Global Characteristics of the Correlation and Time Lag Between Solar and Ionospheric Parameters in the 27-day Period

NASA Technical Reports Server (NTRS)

Lee, Choon-Ki; Han, Shin-Chan; Dieter,Bilitza; Ki-Weon,Seo

2012-01-01

The 27-day variations of topside ionosphere are investigated using the in-situ electron density measurements from the CHAMP planar Langmuir probe and GRACE K-band ranging system. As the two satellite systems orbit at the altitudes of approx. 370 km and approx. 480 km, respectively, the satellite data sets are greatly valuable for examining the electron density variations in the vicinity of F2-peak. In a 27-day period, the electron density measurements from the satellites are in good agreements with the solar flux, except during the solar minimum period. The time delays are mostly 1-2 day and represent the hemispherical asymmetry. The globally-estimated spatial patterns of the correlation between solar flux and in-situ satellite measurements show poor correlations in the (magnetic) equatorial region, which are not found from the ground measurements of vertically-integrated electron content. We suggest that the most plausible cause for the poor correlation is the vertical movement of ionization due to atmospheric dynamic processes that is not controlled by the solar extreme ultraviolet radiation.

Using the Flipchem Photochemistry Model When Fitting Incoherent Scatter Radar Data

NASA Astrophysics Data System (ADS)

Reimer, A. S.; Varney, R. H.

2017-12-01

The North face Resolute Bay Incoherent Scatter Radar (RISR-N) routinely images the dynamics of the polar ionosphere, providing measurements of the plasma density, electron temperature, ion temperature, and line of sight velocity with seconds to minutes time resolution. RISR-N does not directly measure ionospheric parameters, but backscattered signals, recording them as voltage samples. Using signal processing techniques, radar autocorrelation functions (ACF) are estimated from the voltage samples. A model of the signal ACF is then fitted to the ACF using non-linear least-squares techniques to obtain the best-fit ionospheric parameters. The signal model, and therefore the fitted parameters, depend on the ionospheric ion composition that is used [e.g. Zettergren et. al. (2010), Zou et. al. (2017)].The software used to process RISR-N ACF data includes the "flipchem" model, which is an ion photochemistry model developed by Richards [2011] that was adapted from the Field LineInterhemispheric Plasma (FLIP) model. Flipchem requires neutral densities, neutral temperatures, electron density, ion temperature, electron temperature, solar zenith angle, and F10.7 as inputs to compute ion densities, which are input to the signal model. A description of how the flipchem model is used in RISR-N fitting software will be presented. Additionally, a statistical comparison of the fitted electron density, ion temperature, electron temperature, and velocity obtained using a flipchem ionosphere, a pure O+ ionosphere, and a Chapman O+ ionosphere will be presented. The comparison covers nearly two years of RISR-N data (April 2015 - December 2016). Richards, P. G. (2011), Reexamination of ionospheric photochemistry, J. Geophys. Res., 116, A08307, doi:10.1029/2011JA016613.Zettergren, M., Semeter, J., Burnett, B., Oliver, W., Heinselman, C., Blelly, P.-L., and Diaz, M.: Dynamic variability in F-region ionospheric composition at auroral arc boundaries, Ann. Geophys., 28, 651-664, https://doi.org/10.5194/angeo-28-651-2010, 2010.Zou, S., D. Ozturk, R. Varney, and A. Reimer (2017), Effects of sudden commencement on the ionosphere: PFISR observations and global MHD simulation, Geophys. Res. Lett., 44, 3047-3058, doi:10.1002/2017GL072678.

Spatial and Time Dynamics of Non-Linear Vortices in Plasma Lens for High-Current Ion Beam Focusing

NASA Astrophysics Data System (ADS)

Goncharov, Alexei A.; Maslov, Vasyl I.; Onishchenko, Ivan N.; Tretyakov, Vitalij N.

2002-11-01

It is known from numerical simulation (see, for example, [1]) and from experiments (see, for example, [2]), that an electron density bunches as discrete vortices are long - living structures in vacuum. However, in laboratory experiments [2] it has been shown that the vortices are changed faster, when they are submersed in electrons, distributed around them. The charged plasma lens intended for a focussing of high-current ion beams, has the same crossed configuration of a radial electrical and longitudinal magnetic field [3], as only electron plasma. In this lens the vortical turbulence is excited [3]. The vortex - bunch and vortex - hole are rotated in the inverse directions in system of their rest. The instability development in initially homogeneous plasma causes that the vortices are excited by pairs. Namely, if the vortex - bunch of electrons is generated, near the vortex - hole of electrons is also generated. It is shown, that in nonuniform plasma the vortices behave is various in time. Namely, the vortex - bunch goes to area of larger electron density, and the vortex - hole goes to area of smaller electron density. The speed of the vortex - hole is less than speed of the vortex - bunch. It is shown, that the electron vortices, generated in the plasma lens, can result in to formation of spiral distribution of electron density. The physical mechanism of coalescence of electron vortices - bunches is proposed. 1.Driscoll C.F. et al. Plasma Phys. Contr. Fus. Res. 3 (1989) 507. 2.Kiwamoto Y. et al. Non-neutral plasma physics. Princeton. 1999. P. 99-105. 3.Goncharov A. et al. Plasma Phys. Rep. 20 (1994) 499.

Time-resolved electronic and optical properties of a thiolate-protected Au38 nanocluster

NASA Astrophysics Data System (ADS)

Meng, Qingguo; May, Stanley P.; Berry, Mary T.; Kilin, Dmitri S.

2015-02-01

Density functional theory and density matrix theory are employed to investigate the time-dependent optical and electronic properties of an Au14 nanocluster protected by six cyclic thiolate ligands, Au4(SCH3)4. The Au14[Au4(SCH3)4]6 nanocluster, i.e. Au38(SCH3)24, is equivalent to a truncated-octahedral face-centred cubic Au38 core coated by a monolayer of 24 methylthiol molecules. The electronic and optical properties, such as density of states, linear absorption spectra, nonradiative nonadiabatic dissipative electronic dynamics and radiative emission spectra were calculated and compared for the core Au14 and thiolate-protected Au38(SCH3)24 nanocluster. The main observation from computed photoluminescence for both models is a mechanism of radiative emission. Specifically, a strong contribution to light emission intensity originates from intraband transitions inside the conduction band (CB) in addition to interband LUMO → HOMO transition (HOMO: highest occupied molecular orbital and LUMO: lowest unoccupied molecular orbital). Such comparison clarifies the contributions from Au core and methylthiol ligands to the electronic and optical properties of the Au38(SCH3)24 nanocluster.

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

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

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

2014-12-08

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

Dephasing of LO-phonon-plasmon hybrid modes in n-type GaAs

NASA Astrophysics Data System (ADS)

Vallée, F.; Ganikhanov, F.; Bogani, F.

1997-11-01

The relaxation dynamics of coherent phononlike LO-phonon-plasmon hybrid modes is investigated in n-doped GaAs using an infrared time-resolved coherent anti-Stokes Raman scattering technique. Measurements performed for different crystal temperatures in the range 10-300 K as a function of the electron density injected by doping show a large reduction of the hybrid mode dephasing time compared to the bare LO-phonon one for densities larger than 1016 cm-3. The results are interpreted in terms of coherent decay of the LO-phonon-plasmon mixed mode in the weak-coupling regime and yield information on the plasmon and electron relaxation. The estimated average electron momentum relaxation times are smaller than those deduced from Hall mobility measurements, as expected from our theoretical model.

Electron and hole dynamics in the electronic and structural phase transitions of VO2

NASA Astrophysics Data System (ADS)

Haglund, Richard

2015-03-01

The ultrafast, optically induced insulator-to-metal transition (IMT) and the associated structural phase transition (SPT) in vanadium dioxide (VO2) have been studied for over a decade. However, only recently have effects due to the combined presence of electron-hole pairs and injected electrons been observed. Here we compare and contrast IMT dynamics when both hot electrons and optically excited electron-hole pairs are involved, in (1) thin films of VO2 overlaid by a thin gold foil, in which hot electrons are generated by 1.5 eV photons absorbed in the foil and accelerated through the VO2 by an applied electric field; (2) VO2 nanoparticles covered with a sparse mesh of gold nanoparticles averaging 20-30 nm in diameter in which hot electrons are generated by resonant excitation and decay of the localized surface plasmon; and (3) bare VO2 thin films excited by intense near-single-cycle THz pulses. In the first case, the IMT is driven by excitation of the bulk gold plasmon, and the SPT appears on a few-picosecond time scale. In the second case, density-functional calculations indicate that above a critical carrier density, the addition of a single electron to a 27-unit supercell drives the catastrophic collapse of the coherent phonon associated with, and leading to, the SPT. In the third case, sub-bandgap-energy photons (approximately 0.1 eV) initiate the IMT, but exhibit the same sub-100 femtosecond switching time and coherent phonon dynamics as observed when the IMT is initiated by 1.5 eV photons. This suggests that the underlying mechanism must be quite different, possibly THz-field induced interband tunneling of spatially separated electron-hole pairs. The implications of these findings for ultrafast switching in opto-electronic devices - such as hybrid VO2 silicon ring resonators - are briefly considered. Support from the National Science Foundation (DMR-1207407), the Office of Science, U.S. Department of Energy (DE-FG02-01ER45916) and the Defense Threat-Reduction Agency (HDTRA1-10-1-0047) for these studies is gratefully acknowledged.

Simulation of Space Charge Dynamic in Polyethylene Under DC Continuous Electrical Stress

NASA Astrophysics Data System (ADS)

Boukhari, Hamed; Rogti, Fatiha

2016-10-01

The space charge dynamic plays a very important role in the aging and breakdown of polymeric insulation materials under high voltage. This is due to the intensification of the local electric field and the attendant chemical-mechanical effects in the vicinity around the trapped charge. In this paper, we have investigated the space charge dynamic in low-density polyethylene under high direct-current voltage, which is evaluated by experimental conditions. The evaluation is on the basis of simulation using a bipolar charge transport model consisting of charge injection, transports, trapping, detrapping, and recombination phenomena. The theoretical formulation of the physical problem is based on the Poisson, the continuity, and the transport equations. Numerical results provide temporal and local distributions of the electric field, the space charge density for the different kinds of charges (net charge density, mobile and trapped of electron density, mobile hole density), conduction and displacement current densities, and the external current. The result shows the appearance of the negative packet-like space charge with a large amount of the bulk under the dc electric field of 100 kV/mm, and the induced distortion of the electric field is largely near to the anode, about 39% higher than the initial electric field applied.

Formation of orbital-selective electron states in LaTiO3/SrTiO3 superlattices

NASA Astrophysics Data System (ADS)

Lechermann, Frank; Boehnke, Lewin; Grieger, Daniel

2013-06-01

The interface electronic structure of correlated LaTiO3/SrTiO3 superlattices is investigated by means of the charge self-consistent combination of the local density approximation (LDA) to density functional theory with dynamical mean-field theory. Utilizing a pseudopotential technique together with a continuous-time quantum Monte Carlo approach, the resulting complex multiorbital electronic states are addressed in a coherent fashion beyond static mean field. General structural relaxations are taken into account on the LDA level and cooperate with the driving forces from strong electronic correlations. This alliance leads to a Ti(3dxy) dominated low-energy quasiparticle peak and a lower Hubbard band in line with photoemission studies. Furthermore correlation effects close to the band-insulating bulk SrTiO3 limit as well as the Mott-insulating bulk LaTiO3 limit are studied via realistic single-layer embeddings.

Experimental and theoretical study of topology and electronic correlations in PuB4

NASA Astrophysics Data System (ADS)

Choi, Hongchul; Zhu, Wei; Cary, S. K.; Winter, L. E.; Huang, Zhoushen; McDonald, R. D.; Mocko, V.; Scott, B. L.; Tobash, P. H.; Thompson, J. D.; Kozimor, S. A.; Bauer, E. D.; Zhu, Jian-Xin; Ronning, F.

2018-05-01

We synthesize single crystals of PuB4 using an Al-flux technique. Single-crystal diffraction data provide structural parameters for first-principles density functional theory (DFT) calculations. By computing the density of states, the Z2 topological invariant using the Wilson loop method, and the surface electronic structure from slab calculations, we find that PuB4 is a nonmagnetic strong topological insulator with a band gap of 254 meV. Our magnetic susceptibility, heat capacity, and resistivity measurements are consistent with this analysis, albeit with a smaller gap of 35 meV. DFT plus dynamical mean-field theory calculations show that electronic correlations reduce the size of the band gap, and provide better agreement with the value determined by resistivity. These results demonstrate that PuB4 is a promising actinide material to investigate the interplay of electronic correlations and nontrivial topology.

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

Knyazev, D. V.; Moscow Institute of Physics and Technology; State Scientific Center of the Russian Federation – Institute for Theoretical and Experimental Physics of National Research Centre “Kurchatov Institute,” Bolshaya Cheremushkinskaya 25, 117218 Moscow

This work covers an ab initio calculation of thermodynamic, transport, and optical properties of plastics of the effective composition CH{sub 2} at density 0.954 g/cm{sup 3} in the temperature range from 5 kK up to 100 kK. The calculation is based on the quantum molecular dynamics, density functional theory, and the Kubo-Greenwood formula. The temperature dependence of the static electrical conductivity σ{sub 1{sub D{sub C}}}(T) has a step-like shape: σ{sub 1{sub D{sub C}}}(T) grows rapidly for 5 kK ≤ T ≤ 10 kK and is almost constant for 20 kK ≤ T ≤ 60 kK. The additional analysis based on the investigation of the electron density of states (DOS) is performed.more » The rapid growth of σ{sub 1{sub D{sub C}}}(T) at 5 kK ≤ T ≤ 10 kK is connected with the increase of DOS at the electron energy equal to the chemical potential ϵ = μ. The frequency dependence of the dynamic electrical conductivity σ{sub 1}(ω) at 5 kK has the distinct non-Drude shape with the peak at ω ≈ 10 eV. This behavior of σ{sub 1}(ω) was explained by the dip at the electron DOS.« less

Ultrafast non-radiative dynamics of atomically thin MoSe 2

DOE PAGES

Lin, Ming -Fu; Kochat, Vidya; Krishnamoorthy, Aravind; ...

2017-10-17

Non-radiative energy dissipation in photoexcited materials and resulting atomic dynamics provide a promising pathway to induce structural phase transitions in two-dimensional materials. However, these dynamics have not been explored in detail thus far because of incomplete understanding of interaction between the electronic and atomic degrees of freedom, and a lack of direct experimental methods to quantify real-time atomic motion and lattice temperature. Here, we explore the ultrafast conversion of photoenergy to lattice vibrations in a model bi-layered semiconductor, molybdenum diselenide, MoSe 2. Specifically, we characterize sub-picosecond lattice dynamics initiated by the optical excitation of electronic charge carriers in the highmore » electron-hole plasma density regime. Our results focuses on the first ten picosecond dynamics subsequent to photoexcitation before the onset of heat transfer to the substrate, which occurs on a ~100 picosecond time scale. Photoinduced atomic motion is probed by measuring the time dependent Bragg diffraction of a delayed mega-electronvolt femtosecond electron beam. Transient lattice temperatures are characterized through measurement of Bragg peak intensities and calculation of the Debye-Waller factor (DWF). These measurements show a sub-picosecond decay of Bragg diffraction and a correspondingly rapid rise in lattice temperatures. We estimate a high quantum yield for the conversion of excited charge carrier energy to lattice motion under our experimental conditions, indicative of a strong electron-phonon interaction. First principles nonadiabatic quantum molecular dynamics simulations (NAQMD) on electronically excited MoSe 2 bilayers reproduce the observed picosecond-scale increase in lattice temperature and ultrafast conversion of photoenergy to lattice vibrations. Calculation of excited-state phonon dispersion curves suggests that softened vibrational modes in the excited state are involved in efficient and rapid energy transfer between the electronic system and the lattice.« less

Ultrafast non-radiative dynamics of atomically thin MoSe 2

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

Lin, Ming -Fu; Kochat, Vidya; Krishnamoorthy, Aravind

Non-radiative energy dissipation in photoexcited materials and resulting atomic dynamics provide a promising pathway to induce structural phase transitions in two-dimensional materials. However, these dynamics have not been explored in detail thus far because of incomplete understanding of interaction between the electronic and atomic degrees of freedom, and a lack of direct experimental methods to quantify real-time atomic motion and lattice temperature. Here, we explore the ultrafast conversion of photoenergy to lattice vibrations in a model bi-layered semiconductor, molybdenum diselenide, MoSe 2. Specifically, we characterize sub-picosecond lattice dynamics initiated by the optical excitation of electronic charge carriers in the highmore » electron-hole plasma density regime. Our results focuses on the first ten picosecond dynamics subsequent to photoexcitation before the onset of heat transfer to the substrate, which occurs on a ~100 picosecond time scale. Photoinduced atomic motion is probed by measuring the time dependent Bragg diffraction of a delayed mega-electronvolt femtosecond electron beam. Transient lattice temperatures are characterized through measurement of Bragg peak intensities and calculation of the Debye-Waller factor (DWF). These measurements show a sub-picosecond decay of Bragg diffraction and a correspondingly rapid rise in lattice temperatures. We estimate a high quantum yield for the conversion of excited charge carrier energy to lattice motion under our experimental conditions, indicative of a strong electron-phonon interaction. First principles nonadiabatic quantum molecular dynamics simulations (NAQMD) on electronically excited MoSe 2 bilayers reproduce the observed picosecond-scale increase in lattice temperature and ultrafast conversion of photoenergy to lattice vibrations. Calculation of excited-state phonon dispersion curves suggests that softened vibrational modes in the excited state are involved in efficient and rapid energy transfer between the electronic system and the lattice.« less

QTAIM and Stress Tensor Characterization of Intramolecular Interactions Along Dynamics Trajectories of a Light-Driven Rotary Molecular Motor.

PubMed

Wang, Lingling; Huan, Guo; Momen, Roya; Azizi, Alireza; Xu, Tianlv; Kirk, Steven R; Filatov, Michael; Jenkins, Samantha

2017-06-29

A quantum theory of atoms in molecules (QTAIM) and stress tensor analysis was applied to analyze intramolecular interactions influencing the photoisomerization dynamics of a light-driven rotary molecular motor. For selected nonadiabatic molecular dynamics trajectories characterized by markedly different S 1 state lifetimes, the electron densities were obtained using the ensemble density functional theory method. The analysis revealed that torsional motion of the molecular motor blades from the Franck-Condon point to the S 1 energy minimum and the S 1 /S 0 conical intersection is controlled by two factors: greater numbers of intramolecular bonds before the hop-time and unusually strongly coupled bonds between the atoms of the rotor and the stator blades. This results in the effective stalling of the progress along the torsional path for an extended period of time. This finding suggests a possibility of chemical tuning of the speed of photoisomerization of molecular motors and related molecular switches by reshaping their molecular backbones to decrease or increase the degree of coupling and numbers of intramolecular bond critical points as revealed by the QTAIM/stress tensor analysis of the electron density. Additionally, the stress tensor scalar and vector analysis was found to provide new methods to follow the trajectories, and from this, new insight was gained into the behavior of the S 1 state in the vicinity of the conical intersection.

Longitudinal and transverse spin dynamics of donor-bound electrons in fluorine-doped ZnSe: Spin inertia versus Hanle effect

NASA Astrophysics Data System (ADS)

Heisterkamp, F.; Zhukov, E. A.; Greilich, A.; Yakovlev, D. R.; Korenev, V. L.; Pawlis, A.; Bayer, M.

2015-06-01

The spin dynamics of strongly localized donor-bound electrons in fluorine-doped ZnSe epilayers is studied using pump-probe Kerr rotation techniques. A method exploiting the spin inertia is developed and used to measure the longitudinal spin relaxation time T1 in a wide range of magnetic fields, temperatures, and pump densities. The T1 time of the donor-bound electron spin of about 1.6 μ s remains nearly constant for external magnetic fields varied from zero up to 2.5 T (Faraday geometry) and in a temperature range 1.8-45 K. These findings impose severe restrictions on possible spin relaxation mechanisms. In our opinion they allow us to rule out scattering between free and donor-bound electrons, jumping of electrons between different donor centers, scattering between phonons and donor-bound electrons, and with less certainty charge fluctuations in the environment of the donors caused by the 1.5 ps pulsed laser excitation.

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

Brito, W. H.; Aguiar, M. C. O.; Haule, K.

In this study we present a comparative investigation of the electronic structures of NbO 2 and VO 2 obtained within a combination of density functional theory and cluster-dynamical mean-field theory calculations. We investigate the role of dynamic electronic correlations on the electronic structure of the metallic and insulating phases of NbO 2 and VO 2, with a focus on the mechanism responsible for the gap opening in the insulating phases. For the rutile metallic phases of both oxides, we obtain that electronic correlations lead to a strong renormalization of the t 2g subbands, as well as the emergence of incoherentmore » Hubbard subbands, signaling that electronic correlations are also important in the metallic phase of NbO 2. Interestingly, we find that nonlocal dynamic correlations do play a role in the gap formation of the [body-centered-tetragonal (bct)] insulating phase of NbO 2, by a similar physical mechanism as that recently proposed by us in the case of the monoclinic (M 1) dimerized phase of VO 2. Finally, although the effect of nonlocal dynamic correlations in the gap opening of bct phase is less important than in the (M 1 and M 2) monoclinic phases of VO 2, their presence indicates that the former is not a purely Peierls-type insulator, as it was recently proposed.« less

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

Size effects on the structural, electronic, and optical properties of (5,0) finite-length carbon nanotube: An ab-initio electronic structure study

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

Tarighi Ahmadpour, Mahdi; Rostamnejadi, Ali; Hashemifar, S. Javad

2016-07-07

We use density functional computations to study the zero temperature structural, electronic, magnetic, and optical properties of (5,0) finite carbon nanotubes (FCNT), with length in the range of 4–44 Å. It is found that the structural and electronic properties of (5,0) FCNTs, in the ground state, converge at a length of about 30 Å, while the excited state properties exhibit long-range edge effects. We discuss that curvature effects enhance energy gap of FCNTs, in contrast to the known trend in the periodic limit. It is seen that compensation of curvature effects in two special small sizes may give rise to spontaneous magnetization.more » The obtained cohesive energies provide some insights into the effects of environment on the growth of FCNTs. The second-order difference of the total energies reveals an important magic size of about 15 Å. The optical and dynamical magnetic responses of the FCNTs to polarized electromagnetic pulses are studied by time dependent density functional theory. The results show that the static and dynamic magnetic properties mainly come from the edge carbon atoms. The optical absorption properties are described in terms of local field effects and characterized by Casida linear response method.« less

Nanoscale femtosecond imaging of transient hot solid density plasmas with elemental and charge state sensitivity using resonant coherent diffraction

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

Kluge, T., E-mail: t.kluge@hzdr.de; Bussmann, M.; Huang, L. G., E-mail: lingen.huang@hzdr.de

Here, we propose to exploit the low energy bandwidth, small wavelength, and penetration power of ultrashort pulses from XFELs for resonant Small Angle Scattering (SAXS) on plasma structures in laser excited plasmas. Small angle scattering allows to detect nanoscale density fluctuations in forward scattering direction. Typically, the SAXS signal from laser excited plasmas is expected to be dominated by the free electron distribution. We propose that the ionic scattering signal becomes visible when the X-ray energy is in resonance with an electron transition between two bound states (resonant coherent X-ray diffraction). In this case, the scattering cross-section dramatically increases somore » that the signal of X-ray scattering from ions silhouettes against the free electron scattering background which allows to measure the opacity and derived quantities with high spatial and temporal resolution, being fundamentally limited only by the X-ray wavelength and timing. Deriving quantities such as ion spatial distribution, charge state distribution, and plasma temperature with such high spatial and temporal resolution will make a vast number of processes in shortpulse laser-solid interaction accessible for direct experimental observation, e.g., hole-boring and shock propagation, filamentation and instability dynamics, electron transport, heating, and ultrafast ionization dynamics.« less

On the importance of excited state dynamic response electron correlation in polarizable embedding methods.

PubMed

Eriksen, Janus J; Sauer, Stephan P A; Mikkelsen, Kurt V; Jensen, Hans J Aa; Kongsted, Jacob

2012-09-30

We investigate the effect of including a dynamic reaction field at the lowest possible ab inito wave function level of theory, namely the Hartree-Fock (HF) self-consistent field level within the polarizable embedding (PE) formalism. We formulate HF based PE within the linear response theory picture leading to the PE-random-phase approximation (PE-RPA) and bridge the expressions to a second-order polarization propagator approximation (SOPPA) frame such that dynamic reaction field contributions are included at the RPA level in addition to the static response described at the SOPPA level but with HF induced dipole moments. We conduct calculations on para-nitro-aniline and para-nitro-phenolate using said model in addition to dynamic PE-RPA and PE-CAM-B3LYP. We compare the results to recently published PE-CCSD data and demonstrate how the cost effective SOPPA-based model successfully recovers a great portion of the inherent PE-RPA error when the observable is the solvatochromic shift. We furthermore demonstrate that whenever the change in density resulting from the ground state-excited state electronic transition in the solute is not associated with a significant change in the electric field, dynamic response contributions formulated at the HF level of theory manage to capture the majority of the system response originating from derivative densities. Copyright © 2012 Wiley Periodicals, Inc.

Examinations of tRNA Range of Motion Using Simulations of Cryo-EM Microscopy and X-Ray Data

PubMed Central

Caulfield, Thomas R.; Devkota, Batsal; Rollins, Geoffrey C.

2011-01-01

We examined tRNA flexibility using a combination of steered and unbiased molecular dynamics simulations. Using Maxwell's demon algorithm, molecular dynamics was used to steer X-ray structure data toward that from an alternative state obtained from cryogenic-electron microscopy density maps. Thus, we were able to fit X-ray structures of tRNA onto cryogenic-electron microscopy density maps for hybrid states of tRNA. Additionally, we employed both Maxwell's demon molecular dynamics simulations and unbiased simulation methods to identify possible ribosome-tRNA contact areas where the ribosome may discriminate tRNAs during translation. Herein, we collected >500 ns of simulation data to assess the global range of motion for tRNAs. Biased simulations can be used to steer between known conformational stop points, while unbiased simulations allow for a general testing of conformational space previously unexplored. The unbiased molecular dynamics data describes the global conformational changes of tRNA on a sub-microsecond time scale for comparison with steered data. Additionally, the unbiased molecular dynamics data was used to identify putative contacts between tRNA and the ribosome during the accommodation step of translation. We found that the primary contact regions were H71 and H92 of the 50S subunit and ribosomal proteins L14 and L16. PMID:21716650

Simulations of nanocrystals under pressure: combining electronic enthalpy and linear-scaling density-functional theory.

PubMed

Corsini, Niccolò R C; Greco, Andrea; Hine, Nicholas D M; Molteni, Carla; Haynes, Peter D

2013-08-28

We present an implementation in a linear-scaling density-functional theory code of an electronic enthalpy method, which has been found to be natural and efficient for the ab initio calculation of finite systems under hydrostatic pressure. Based on a definition of the system volume as that enclosed within an electronic density isosurface [M. Cococcioni, F. Mauri, G. Ceder, and N. Marzari, Phys. Rev. Lett. 94, 145501 (2005)], it supports both geometry optimizations and molecular dynamics simulations. We introduce an approach for calibrating the parameters defining the volume in the context of geometry optimizations and discuss their significance. Results in good agreement with simulations using explicit solvents are obtained, validating our approach. Size-dependent pressure-induced structural transformations and variations in the energy gap of hydrogenated silicon nanocrystals are investigated, including one comparable in size to recent experiments. A detailed analysis of the polyamorphic transformations reveals three types of amorphous structures and their persistence on depressurization is assessed.

Simulations of nanocrystals under pressure: Combining electronic enthalpy and linear-scaling density-functional theory

NASA Astrophysics Data System (ADS)

Corsini, Niccolò R. C.; Greco, Andrea; Hine, Nicholas D. M.; Molteni, Carla; Haynes, Peter D.

2013-08-01

We present an implementation in a linear-scaling density-functional theory code of an electronic enthalpy method, which has been found to be natural and efficient for the ab initio calculation of finite systems under hydrostatic pressure. Based on a definition of the system volume as that enclosed within an electronic density isosurface [M. Cococcioni, F. Mauri, G. Ceder, and N. Marzari, Phys. Rev. Lett. 94, 145501 (2005)], 10.1103/PhysRevLett.94.145501, it supports both geometry optimizations and molecular dynamics simulations. We introduce an approach for calibrating the parameters defining the volume in the context of geometry optimizations and discuss their significance. Results in good agreement with simulations using explicit solvents are obtained, validating our approach. Size-dependent pressure-induced structural transformations and variations in the energy gap of hydrogenated silicon nanocrystals are investigated, including one comparable in size to recent experiments. A detailed analysis of the polyamorphic transformations reveals three types of amorphous structures and their persistence on depressurization is assessed.

JDFTx: Software for joint density-functional theory

DOE PAGES

Sundararaman, Ravishankar; Letchworth-Weaver, Kendra; Schwarz, Kathleen A.; ...

2017-11-14

Density-functional theory (DFT) has revolutionized computational prediction of atomic-scale properties from first principles in physics, chemistry and materials science. Continuing development of new methods is necessary for accurate predictions of new classes of materials and properties, and for connecting to nano- and mesoscale properties using coarse-grained theories. JDFTx is a fully-featured open-source electronic DFT software designed specifically to facilitate rapid development of new theories, models and algorithms. Using an algebraic formulation as an abstraction layer, compact C++11 code automatically performs well on diverse hardware including GPUs (Graphics Processing Units). This code hosts the development of joint density-functional theory (JDFT) thatmore » combines electronic DFT with classical DFT and continuum models of liquids for first-principles calculations of solvated and electrochemical systems. In addition, the modular nature of the code makes it easy to extend and interface with, facilitating the development of multi-scale toolkits that connect to ab initio calculations, e.g. photo-excited carrier dynamics combining electron and phonon calculations with electromagnetic simulations.« less

JDFTx: Software for joint density-functional theory

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

Sundararaman, Ravishankar; Letchworth-Weaver, Kendra; Schwarz, Kathleen A.

Density-functional theory (DFT) has revolutionized computational prediction of atomic-scale properties from first principles in physics, chemistry and materials science. Continuing development of new methods is necessary for accurate predictions of new classes of materials and properties, and for connecting to nano- and mesoscale properties using coarse-grained theories. JDFTx is a fully-featured open-source electronic DFT software designed specifically to facilitate rapid development of new theories, models and algorithms. Using an algebraic formulation as an abstraction layer, compact C++11 code automatically performs well on diverse hardware including GPUs (Graphics Processing Units). This code hosts the development of joint density-functional theory (JDFT) thatmore » combines electronic DFT with classical DFT and continuum models of liquids for first-principles calculations of solvated and electrochemical systems. In addition, the modular nature of the code makes it easy to extend and interface with, facilitating the development of multi-scale toolkits that connect to ab initio calculations, e.g. photo-excited carrier dynamics combining electron and phonon calculations with electromagnetic simulations.« less

Optical and electronic properties of sub-surface conducting layers in diamond created by MeV B-implantation at elevated temperatures

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

Willems van Beveren, L. H., E-mail: laurensw@unimelb.edu.au; Bowers, H.; Ganesan, K.

2016-06-14

Boron implantation with in-situ dynamic annealing is used to produce highly conductive sub-surface layers in type IIa (100) diamond plates for the search of a superconducting phase transition. Here, we demonstrate that high-fluence MeV ion-implantation, at elevated temperatures avoids graphitization and can be used to achieve doping densities of 6 at. %. In order to quantify the diamond crystal damage associated with implantation Raman spectroscopy was performed, demonstrating high temperature annealing recovers the lattice. Additionally, low-temperature electronic transport measurements show evidence of charge carrier densities close to the metal-insulator-transition. After electronic characterization, secondary ion mass spectrometry was performed to mapmore » out the ion profile of the implanted plates. The analysis shows close agreement with the simulated ion-profile assuming scaling factors that take into account an average change in diamond density due to device fabrication. Finally, the data show that boron diffusion is negligible during the high temperature annealing process.« less

A molecular dynamics and ab initio analysis of the electronic structure of single-walled carbon nanotubes adhered to a substrate

NASA Astrophysics Data System (ADS)

Van Der Geest, A. G.; Lu, Z.; Lusk, M. T.; Dunn, M. L.

2011-04-01

Single-wall nanotubes can adhere to planar surfaces via van der Waals forces, and this causes the tubes to deform. We use classical molecular dynamics to estimate this deformation and density functional theory to quantify its impact on electronic band structure. For (n,0) tubes, adhesion causes the maximum bandgap to rise more rapidly with diameter, but the value of the maximum is not affected. The influence of adhesion forces on bandgap was found to correlate with that associated with lateral, uniaxial compression for moderate values of adhesion energy and compressive distortion.

Unusual instability mode of transparent all oxide thin film transistor under dynamic bias condition

NASA Astrophysics Data System (ADS)

Oh, Himchan; Hwang, Chi-Sun; Pi, Jae-Eun; Ki Ryu, Min; Ko Park, Sang-Hee; Yong Chu, Hye

2013-09-01

We report a degradation behavior of fully transparent oxide thin film transistor under dynamic bias stress which is the condition similar to actual pixel switching operation in active matrix display. After the stress test, drain current increased while the threshold voltage was almost unchanged. We found that shortening of effective channel length is leading cause of increase in drain current. Electrons activate the neutral donor defects by colliding with them during short gate-on period. These ionized donors are stabilized during the subsequent gate-off period due to electron depletion. This local increase in doping density reduces the channel length.

Many-Body Theory of Proton-Generated Point Defects for Losses of Electron Energy and Photons in Quantum Wells

NASA Astrophysics Data System (ADS)

Huang, Danhong; Iurov, Andrii; Gao, Fei; Gumbs, Godfrey; Cardimona, D. A.

2018-02-01

The effects of point defects on the loss of either energies of ballistic electron beams or incident photons are studied by using a many-body theory in a multi-quantum-well system. This theory includes the defect-induced vertex correction to a bare polarization function of electrons within the ladder approximation, and the intralayer and interlayer screening of defect-electron interactions is also taken into account in the random-phase approximation. The numerical results of defect effects on both energy-loss and optical-absorption spectra are presented and analyzed for various defect densities, numbers of quantum wells, and wave vectors. The diffusion-reaction equation is employed for calculating distributions of point defects in a layered structure. For completeness, the production rate for Frenkel-pair defects and their initial concentration are obtained based on atomic-level molecular-dynamics simulations. By combining the defect-effect, diffusion-reaction, and molecular-dynamics models with an available space-weather-forecast model, it will be possible in the future to enable specific designing for electronic and optoelectronic quantum devices that will be operated in space with radiation-hardening protection and, therefore, effectively extend the lifetime of these satellite onboard electronic and optoelectronic devices. Specifically, this theory can lead to a better characterization of quantum-well photodetectors not only for high quantum efficiency and low dark current density but also for radiation tolerance or mitigating the effects of the radiation.

Ionic structures and transport properties of hot dense W and U plasmas

NASA Astrophysics Data System (ADS)

Hou, Yong; Yuan, Jianmin

2016-10-01

We have combined the average-atom model with the hyper-netted chain approximation (AAHNC) to describe the electronic and ionic structure of uranium and tungsten in the hot dense matter regime. When the electronic structure is described within the average-atom model, the effects of others ions on the electronic structure are considered by the correlation functions. And the ionic structure is calculated though using the hyper-netted chain (HNC) approximation. The ion-ion pair potential is calculated using the modified Gordon-Kim model based on the electronic density distribution in the temperature-depended density functional theory. And electronic and ionic structures are determined self-consistently. On the basis of the ion-ion pair potential, we perform the classical (CMD) and Langevin (LMD) molecular dynamics to simulate the ionic transport properties, such as ionic self-diffusion and shear viscosity coefficients, through the ionic velocity correlation functions. Due that the free electrons become more and more with increasing the plasma temperature, the influence of the electron-ion collisions on the transport properties become more and more important.

Dynamic electron-ion collisions and nuclear quantum effects in quantum simulation of warm dense matter.

PubMed

Kang, Dongdong; Dai, Jiayu

2018-02-21

The structural, thermodynamic and transport properties of warm dense matter (WDM) are crucial to the fields of astrophysics and planet science, as well as inertial confinement fusion. WDM refers to the states of matter in a regime of temperature and density between cold condensed matter and hot ideal plasmas, where the density is from near-solid up to ten times solid density, and the temperature between 0.1 and 100 eV. In the WDM regime, matter exhibits moderately or strongly coupled, partially degenerate properties. Therefore, the methods used to deal with condensed matter and isolated atoms need to be properly validated for WDM. It is therefore a big challenge to understand WDM within a unified theoretical description with reliable accuracy. Here, we review the progress in the theoretical study of WDM with state-of-the-art simulations, i.e. quantum Langevin molecular dynamics and first principles path integral molecular dynamics. The related applications for WDM are also included.

Dynamic electron-ion collisions and nuclear quantum effects in quantum simulation of warm dense matter

NASA Astrophysics Data System (ADS)

Kang, Dongdong; Dai, Jiayu

2018-02-01

The structural, thermodynamic and transport properties of warm dense matter (WDM) are crucial to the fields of astrophysics and planet science, as well as inertial confinement fusion. WDM refers to the states of matter in a regime of temperature and density between cold condensed matter and hot ideal plasmas, where the density is from near-solid up to ten times solid density, and the temperature between 0.1 and 100 eV. In the WDM regime, matter exhibits moderately or strongly coupled, partially degenerate properties. Therefore, the methods used to deal with condensed matter and isolated atoms need to be properly validated for WDM. It is therefore a big challenge to understand WDM within a unified theoretical description with reliable accuracy. Here, we review the progress in the theoretical study of WDM with state-of-the-art simulations, i.e. quantum Langevin molecular dynamics and first principles path integral molecular dynamics. The related applications for WDM are also included.

Remote sensing of electron density and ion composition using nonducted whistler observations on OGO 1 and Van Allen Probes

NASA Astrophysics Data System (ADS)

Sonwalkar, V. S.; Butler, J.; Reddy, A.

2017-12-01

We present a new method to remotely measure magnetospheric electron density and ion composition using lightning generated nonducted whistlers observed on a satellite. Electron and ion densities play important roles in magnetospheric processes such as wave-particle interactions in the equatorial region and ion-neutral dynamics in the ionosphere, and are important for calculating space weather effects such as particle precipitation, GPS scintillations, and satellite drag. The nonducted whistler resulting from a single lightning appears on a spectrogram as a series of magnetospherically reflected traces with characteristic dispersion (time delay versus frequency) and upper and lower cut off frequencies. Ray tracing simulations show that these observed characteristics depend on the magnetospheric electron density and ion composition. The cut off frequencies depend on both electron density and ion composition. The dispersion depends strongly on electron density, but weakly on ion composition. Using an iterative process to fit the measured dispersion and cutoff frequencies to those obtained from ray tracing simulations, it is possible to construct the electron and ion density profiles of the magnetosphere. We demonstrate our method by applying it to nonducted whistlers observed on OGO 1 and Van Allen probe satellites. In one instance (08 Nov 1965), whistler traces observed on OGO 1 (L = 2.4, λm = -6°) displayed a few seconds of dispersion and cutoff frequencies in the 1-10 kHz range. Ray tracing analysis showed that a diffusive equilibrium density model with the following parameters can reproduce the observed characteristics of the whistler traces: 1900 el/cc at L=2.4 and the equator, 358,000 el/cc at F2 peak (hmF2 = 220 km), the relative ion concentrations αH+ = 0.2, αHe+ = 0.2, and αO+ = 0.6 at 1000 km, and temperature 1600 K. The method developed here can be applied to whistlers observed on the past, current, and future magnetospheric satellite missions carrying wave instrument (e.g. OGO, ISEE 1, DE 1, POLAR, CLUSTER, Van Allen Probes). The method can be easily extended to make tomographic measurements of magnetospheric electron and ion density by analyzing a series of whistlers observed along the satellite orbit.

β -B i2O3 under compression: Optical and elastic properties and electron density topology analysis

NASA Astrophysics Data System (ADS)

Pereira, A. L. J.; Gomis, O.; Sans, J. A.; Contreras-García, J.; Manjón, F. J.; Rodríguez-Hernández, P.; Muñoz, A.; Beltrán, A.

2016-06-01

We report a joint experimental and theoretical study of the optical properties of tetragonal bismuth oxide (β -B i2O3 ) at high pressure by means of optical absorption measurements combined with ab initio electronic band structure calculations. Our results are consistent with previous results that show the presence of a second-order isostructural phase transition in B i2O3 (from β to β') around 2 GPa and a phase transition above 15 GPa combined with a pressure-induced amorphization above 17-20 GPa. In order to further understand the pressure-induced phase transitions and amorphization occurring in β -B i2O3 , we theoretically studied the mechanical and dynamical stability of the tetragonal structures of β - and β'-B i2O3 at high pressure through calculations of their elastic constants, elastic stiffness coefficients, and phonon dispersion curves. The pressure dependence of the elastic stiffness coefficients and phonon dispersion curves confirms that the isostructural phase transition near 2 GPa is of ferroelastic nature. Furthermore, a topological study of the electron density shows that the ferroelastic transition is not caused by a change in number of critical points (cusp catastrophe), but by the equalization of the electron densities of both independent O atoms in the unit cell due to a local rise in symmetry. Finally, from theoretical simulations, β'-B i2O3 is found to be mechanically and dynamically stable at least up to 26.7 GPa under hydrostatic conditions; thus, the pressure-induced amorphization reported above 17-20 GPa in powder β'-B i2O3 using methanol-ethanol-water as pressure-transmitting medium could be related to the frustration of a reconstructive phase transition at room temperature and the presence of mechanical or dynamical instabilities under nonhydrostatic conditions.

Warm Dense Matter Demonstrating Non-Drude Conductivity from Observations of Nonlinear Plasmon Damping

NASA Astrophysics Data System (ADS)

Witte, Bastian B. L.

2017-10-01

The thermal and electrical conductivity, equation of state and the spectral opacity in warm dense matter (WDM) are essential properties for modeling, e.g., fusion experiments or the magnetic field generation in planets. In the last decade it has been shown that x-ray Thomson scattering (XRTS) is an effective tool to determine plasma parameters like temperature and density in the WDM regime. Recently, the electrical conductivity was extracted from XRTS experiments for the first time. The spectrally resolved scattering data of aluminum, isochorically heated by the Linac Coherent Light Source (LCLS), show strong dependence on electron correlations. Therefore, the damping of plasmons, the collective electron oscillations, has to be treated beyond perturbation theory. We present results for the dynamic transport properties in warm dense aluminum using density-functional-theory molecular dynamics (DFT-MD) simulations. The choice of the exchange-correlation (XC) functional, describing the interactions in the electronic subsystem, has significant impact on the ionization energy of bound electrons and the dynamic dielectric function. Our newly developed method for the calculation of XRTS signals including plasmon and bound-free transitions is based on transition matrix elements together with ionic contributions using uniquely DFT-MD simulations. The results show excellent agreement with the LCLS data if hybrid functionals are applied. The experimental finding of nonlinear plasmon damping is caused by the non-Drude conductivity in warm dense aluminum. Here, we show further validation by comparing with x-ray absorption data. These findings enable new insights into the impact of XC functionals on calculated properties of WDM and allow detailed predictions for future experiments at the unprecedented densities on the NIF. This work was performed in collaboration with P. Sperling, S.H. Glenzer, R. Redmer and was supported by the DFG via the Collaborative Research Center SFB 652 and the DOE Office of Science, Fusion Energy Science under Grant No. FWP 100182.

First-principles investigation of the dissociation and coupling of methane on small copper clusters: Interplay of collision dynamics and geometric and electronic effects

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

Varghese, Jithin J.; Mushrif, Samir H., E-mail: shmushrif@ntu.edu.sg

Small metal clusters exhibit unique size and morphology dependent catalytic activity. The search for alternate minimum energy pathways and catalysts to transform methane to more useful chemicals and carbon nanomaterials led us to investigate collision induced dissociation of methane on small Cu clusters. We report here for the first time, the free energy barriers for the collision induced activation, dissociation, and coupling of methane on small Cu clusters (Cu{sub n} where n = 2–12) using ab initio molecular dynamics and metadynamics simulations. The collision induced activation of the stretching and bending vibrations of methane significantly reduces the free energy barriermore » for its dissociation. Increase in the cluster size reduces the barrier for dissociation of methane due to the corresponding increase in delocalisation of electron density within the cluster, as demonstrated using the electron localisation function topology analysis. This enables higher probability of favourable alignment of the C–H stretching vibration of methane towards regions of high electron density within the cluster and makes higher number of sites available for the chemisorption of CH{sub 3} and H upon dissociation. These characteristics contribute in lowering the barrier for dissociation of methane. Distortion and reorganisation of cluster geometry due to high temperature collision dynamics disturb electron delocalisation within them and increase the barrier for dissociation. Coupling reactions of CH{sub x} (x = 1–3) species and recombination of H with CH{sub x} have free energy barriers significantly lower than complete dehydrogenation of methane to carbon. Thus, competition favours the former reactions at high hydrogen saturation on the clusters.« less

Ionization asymmetry effects on the properties modulation of atmospheric pressure dielectric barrier discharge sustained by tailored voltage waveforms

NASA Astrophysics Data System (ADS)

Zhang, Z. L.; Nie, Q. Y.; Zhang, X. N.; Wang, Z. B.; Kong, F. R.; Jiang, B. H.; Lim, J. W. M.

2018-04-01

The dielectric barrier discharge (DBD) is a promising technology to generate high density and uniform cold plasmas in atmospheric pressure gases. The effective independent tuning of key plasma parameters is quite important for both application-focused and fundamental studies. In this paper, based on a one-dimensional fluid model with semi-kinetics treatment, numerical studies of ionization asymmetry effects on the properties modulation of atmospheric DBD sustained by tailored voltage waveforms are reported. The driving voltage waveform is characterized by an asymmetric-slope fundamental sinusoidal radio frequency signal superimposing one or more harmonics, and the effects of the number of harmonics, phase shift, as well as the fluctuation of harmonics on the sheath dynamics, impact ionization of electrons and key plasma parameters are investigated. The results have shown that the electron density can exhibit a substantial increase due to the effective electron heating by a spatially asymmetric sheath structure. The strategic modulation of harmonics number and phase shift is capable of raising the electron density significantly (e.g., nearly three times in this case), but without a significant increase in the gas temperature. Moreover, by tailoring the fluctuation of harmonics with a steeper slope, a more profound efficiency in electron impact ionization can be achieved, and thus enhancing the electron density effectively. This method then enables a novel alternative approach to realize the independent control of the key plasma parameters under atmospheric pressure.

Persistent order due to transiently enhanced nesting in an electronically excited charge density wave

DOE PAGES

Rettig, L.; Cortés, R.; Chu, J. -H.; ...

2016-01-25

Non-equilibrium conditions may lead to novel properties of materials with broken symmetry ground states not accessible in equilibrium as vividly demonstrated by non-linearly driven mid-infrared active phonon excitation. Potential energy surfaces of electronically excited states also allow to direct nuclear motion, but relaxation of the excess energy typically excites fluctuations leading to a reduced or even vanishing order parameter as characterized by an electronic energy gap. Here, using femtosecond time-and angle-resolved photoemission spectroscopy, we demonstrate a tendency towards transient stabilization of a charge density wave after near-infrared excitation, counteracting the suppression of order in the non-equilibrium state. Analysis of themore » dynamic electronic structure reveals a remaining energy gap in a highly excited transient state. In conclusion, our observation can be explained by a competition between fluctuations in the electronically excited state, which tend to reduce order, and transiently enhanced Fermi surface nesting stabilizing the order.« less

Gradual Diffusion and Punctuated Phase Space Density Enhancements of Highly Relativistic Electrons: Van Allen Probes Observations

NASA Technical Reports Server (NTRS)

Baker, D. N.; Jaynes, A. N.; Li, X.; Henderson, M. G.; Kanekal, S. G.; Reeves, G. D.; Spence, H. E.; Claudepierre, S. G.; Fennell, J. F.; Hudson, M. K.

2014-01-01

The dual-spacecraft Van Allen Probes mission has provided a new window into mega electron volt (MeV) particle dynamics in the Earth's radiation belts. Observations (up to E (is) approximately 10MeV) show clearly the behavior of the outer electron radiation belt at different timescales: months-long periods of gradual inward radial diffusive transport and weak loss being punctuated by dramatic flux changes driven by strong solar wind transient events. We present analysis of multi-MeV electron flux and phase space density (PSD) changes during March 2013 in the context of the first year of Van Allen Probes operation. This March period demonstrates the classic signatures both of inward radial diffusive energization and abrupt localized acceleration deep within the outer Van Allen zone (L (is) approximately 4.0 +/- 0.5). This reveals graphically that both 'competing' mechanisms of multi-MeV electron energization are at play in the radiation belts, often acting almost concurrently or at least in rapid succession.

Dynamic unmagnetized plasma in the diamagnetic cavity around comet 67P/Churyumov-Gerasimenko

NASA Astrophysics Data System (ADS)

Hajra, Rajkumar; Henri, Pierre; Vallières, Xavier; Moré, Jerome; Gilet, Nicolas; Wattieaux, Gaetan; Goetz, Charlotte; Richter, Ingo; Tsurutani, Bruce T.; Gunell, Herbert; Nilsson, Hans; Eriksson, Anders I.; Nemeth, Zoltan; Burch, James L.; Rubin, Martin

2018-04-01

The Rosetta orbiter witnessed several hundred diamagnetic cavity crossings (unmagnetized regions) around comet 67P/Churyumov-Gerasimenko during its two year survey of the comet. The characteristics of the plasma environment inside these diamagnetic regions are studied using in situ measurements by the Rosetta Plasma Consortium instruments. Although the unmagnetized plasma density has been observed to exhibit little dynamics compared to the very dynamical magnetized cometary plasma, we detected several localized dynamic plasma structures inside those diamagnetic regions. These plasma structures are not related to the direct ionization of local cometary neutrals. The structures are found to be steepened, asymmetric plasma enhancements with typical rising-to-descending slope ratio of ˜2.8 (±1.9), skewness ˜0.43 (±0.36), mean duration of ˜2.7 (±0.9) min and relative density variation ΔN/N of ˜0.5 (±0.2), observed close to the electron exobase. Similar steepened plasma density enhancements were detected at the magnetized boundaries of the diamagnetic cavity as well as outside the diamagnetic region. The plausible scalelength and propagation direction of the structures are estimated from simple plasma dynamics considerations. It is suggested that they are large-scale unmagnetized plasma enhancements, transmitted from the very dynamical outer magnetized region to the inner magnetic field-free cavity region.

ON THE ELECTRON-TO-NEUTRAL NUMBER DENSITY RATIO IN THE COMA OF COMET 67P/CHURYUMOV–GERASIMENKO: GUIDING EXPRESSION AND SOURCES FOR DEVIATIONS

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

Vigren, E.; Eriksson, A. I.; Edberg, N. J. T.

2015-10-10

We compute partial photoionization frequencies of H{sub 2}O, CO{sub 2}, and CO, the major molecules in the coma of comet 67P/Churyumov–Gerasimenko, the target comet of the ongoing ESA Rosetta mission. Values are computed from Thermosphere Ionosphere Mesosphere Energy and Dynamics/Solar EUV Experiment solar EUV spectra for 2014 August 1, 2015 March 1, and for perihelion (2015 August, as based on prediction). From the varying total photoionization frequency of H{sub 2}O, as computed from 2014 August 1 to 2015 May 20, we derive a simple analytical expression for the electron-to-neutral number density ratio as a function of cometocentric and heliocentric distance. Themore » underlying model assumes radial movement of the coma constituents and does not account for chemical loss or the presence of electric fields. We discuss various effects/processes that can cause deviations between values from the analytical expression and actual electron-to-neutral number density ratios. The analytical expression is thus not strictly meant as predicting the actual electron-to-neutral number density ratio, but is useful in comparisons with observations as an indicator of processes at play in the cometary coma.« less

REVIEW ARTICLE: On correlation effects in electron spectroscopies and the GW approximation

NASA Astrophysics Data System (ADS)

Hedin, Lars

1999-10-01

The GW approximation (GWA) extends the well-known Hartree-Fock approximation (HFA) for the self-energy (exchange potential), by replacing the bare Coulomb potential v by the dynamically screened potential W, e.g. Vex = iGv is replaced by icons/Journals/Common/Sigma" ALT="Sigma" ALIGN="TOP"/>GW = iGW. Here G is the one-electron Green's function. The GWA like the HFA is self-consistent, which allows for solutions beyond perturbation theory, like say spin-density waves. In a first approximation, iGW is a sum of a statically screened exchange potential plus a Coulomb hole (equal to the electrostatic energy associated with the charge pushed away around a given electron). The Coulomb hole part is larger in magnitude, but the two parts give comparable contributions to the dispersion of the quasi-particle energy. The GWA can be said to describe an electronic polaron (an electron surrounded by an electronic polarization cloud), which has great similarities to the ordinary polaron (an electron surrounded by a cloud of phonons). The dynamical screening adds new crucial features beyond the HFA. With the GWA not only bandstructures but also spectral functions can be calculated, as well as charge densities, momentum distributions, and total energies. We will discuss the ideas behind the GWA, and generalizations which are necessary to improve on the rather poor GWA satellite structures in the spectral functions. We will further extend the GWA approach to fully describe spectroscopies like photoemission, x-ray absorption, and electron scattering. Finally we will comment on the relation between the GWA and theories for strongly correlated electronic systems. In collecting the material for this review, a number of new results and perspectives became apparent, which have not been published elsewhere.

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

Vaezi, P.; Holland, C.; Thakur, S. C.

The Controlled Shear Decorrelation Experiment (CSDX) linear plasma device provides a unique platform for investigating the underlying physics of self-regulating drift-wave turbulence/zonal flow dynamics. A minimal model of 3D drift-reduced nonlocal cold ion fluid equations which evolves density, vorticity, and electron temperature fluctuations, with proper sheath boundary conditions, is used to simulate dynamics of the turbulence in CSDX and its response to changes in parallel boundary conditions. These simulations are then carried out using the BOUndary Turbulence (BOUT++) framework and use equilibrium electron density and temperature profiles taken from experimental measurements. The results show that density gradient-driven drift-waves are themore » dominant instability in CSDX. However, the choice of insulating or conducting endplate boundary conditions affects the linear growth rates and energy balance of the system due to the absence or addition of Kelvin-Helmholtz modes generated by the sheath-driven equilibrium E × B shear and sheath-driven temperature gradient instability. Moreover, nonlinear simulation results show that the boundary conditions impact the turbulence structure and zonal flow formation, resulting in less broadband (more quasi-coherent) turbulence and weaker zonal flow in conducting boundary condition case. These results are qualitatively consistent with earlier experimental observations.« less

Photoinduced discommensuration of the commensurate charge-density wave phase in 1 T -Ta S2

NASA Astrophysics Data System (ADS)

Tanimura, Katsumi

2018-06-01

The dynamics induced by femtosecond-laser excitation of the commensurate phase of the charge-density wave (CDW) in 1 T -Ta S2 have been studied using both time-resolved electron diffraction and the time-resolved spectroscopy of coherent-phonon dynamics. Electron diffraction results show that the commensurate CDW phase is transformed into a new phase with CDW order that is similar to the nearly commensurate phase with threshold-type transition rates; the threshold excitation density of 0.2 per 13 Ta atoms is evaluated. Coherent-phonon spectroscopy results show that, together with the amplitude mode of CDW with a frequency of 2.41 THz, two other modes with frequencies of 2.34 and 2.07 THz are excited in the photoexcited commensurate CDW phase over a timescale of several tens of picoseconds after excitation. Spectroscopic, temporal, and excitation-intensity dependent characteristics of the three coherent phonons reveal that a photoinduced decomposition of the commensurate CDW order into an ensemble of domains with different CDW orders is induced before the CDW-phase transition occurs. The physics underlying the photoinduced decomposition and evolution into discommensurations responsible for the CDW-order transformation are discussed.

Ultrafast equilibration of excited electrons in dynamical simulations.

PubMed

Lin, Zhibin; Allen, Roland E

2009-12-02

In our density-functional-based simulations of materials responding to femtosecond-scale laser pulses, we have observed a potentially useful phenomenon: the excited electrons automatically equilibrate to a Fermi-Dirac distribution within ∼100 fs, solely because of their coupling to the nuclear motion, even though the resulting electronic temperature is one to two orders of magnitude higher than the kinetic temperature defined by the nuclear motion. Microscopic simulations like these can then provide the separate electronic and kinetic temperatures, chemical potentials, pressures, and nonhydrostatic stresses as input for studies on larger lengths and timescales.

Self-consistent modelling of electrochemical strain microscopy in mixed ionic-electronic conductors: Nonlinear and dynamic regimes

DOE PAGES

Varenyk, O. V.; Silibin, M. V.; Kiselev, Dmitri A.; ...

2015-08-19

The frequency dependent Electrochemical Strain Microscopy (ESM) response of mixed ionic-electronic conductors is analyzed within the framework of Fermi-Dirac statistics and the Vegard law, accounting for steric effects from mobile donors. The emergence of dynamic charge waves and nonlinear deformation of the surface in response to bias applied to the tip-surface junction is numerically explored. The 2D maps of the strain and concentration distributions across the mixed ionic-electronic conductor and bias-induced surface displacements are calculated. Furthermore, the obtained numerical results can be applied to quantify the ESM response of Li-based solid electrolytes, materials with resistive switching, and electroactive ferroelectric polymers,more » which are of potential interest for flexible and high-density non-volatile memory devices.« less

Self-consistent modelling of electrochemical strain microscopy in mixed ionic-electronic conductors: Nonlinear and dynamic regimes

NASA Astrophysics Data System (ADS)

Varenyk, O. V.; Silibin, M. V.; Kiselev, D. A.; Eliseev, E. A.; Kalinin, S. V.; Morozovska, A. N.

2015-08-01

The frequency dependent Electrochemical Strain Microscopy (ESM) response of mixed ionic-electronic conductors is analyzed within the framework of Fermi-Dirac statistics and the Vegard law, accounting for steric effects from mobile donors. The emergence of dynamic charge waves and nonlinear deformation of the surface in response to bias applied to the tip-surface junction is numerically explored. The 2D maps of the strain and concentration distributions across the mixed ionic-electronic conductor and bias-induced surface displacements are calculated. The obtained numerical results can be applied to quantify the ESM response of Li-based solid electrolytes, materials with resistive switching, and electroactive ferroelectric polymers, which are of potential interest for flexible and high-density non-volatile memory devices.

Manipulation of electron transport in graphene by nanopatterned electrostatic potential on an electret

NASA Astrophysics Data System (ADS)

Wang, Xiaowei; Wang, Rui; Wang, Shengnan; Zhang, Dongdong; Jiang, Xingbin; Cheng, Zhihai; Qiu, Xiaohui

2018-01-01

The electron transport characteristics of graphene can be finely tuned using local electrostatic fields. Here, we use a scanning probe technique to construct a statically charged electret gate that enables in-situ fabrication of graphene devices with precisely designed potential landscapes, including p-type and n-type unipolar graphene transistors and p-n junctions. Electron dynamic simulation suggests that electron beam collimation and focusing in graphene can be achieved via periodic charge lines and concentric charge circles. This approach to spatially manipulating carrier density distribution may offer an efficient way to investigate the novel electronic properties of graphene and other low-dimensional materials.

Communication: On the calculation of time-dependent electron flux within the Born-Oppenheimer approximation: A flux-flux reflection principle

NASA Astrophysics Data System (ADS)

Albert, Julian; Hader, Kilian; Engel, Volker

2017-12-01

It is commonly assumed that the time-dependent electron flux calculated within the Born-Oppenheimer (BO) approximation vanishes. This is not necessarily true if the flux is directly determined from the continuity equation obeyed by the electron density. This finding is illustrated for a one-dimensional model of coupled electronic-nuclear dynamics. There, the BO flux is in perfect agreement with the one calculated from a solution of the time-dependent Schrödinger equation for the coupled motion. A reflection principle is derived where the nuclear BO flux is mapped onto the electronic flux.

Correlated phonons and the Tc-dependent dynamical phonon anomalies

NASA Astrophysics Data System (ADS)

Hakioğlu, T.; Türeci, H.

1997-11-01

Anomalously large low-temperature phonon anharmonicities can lead to static as well as dynamical changes in the low-temperature properties of the electron-phonon system. In this work, we focus our attention on the dynamically generated low-temperature correlations in an interacting electron-phonon system using a self-consistent dynamical approach in the intermediate coupling range. In the context of the model, the polaron correlations are produced by the charge-density fluctuations which are generated dynamically by the electron-phonon coupling. Conversely, the latter is influenced in the presence of the former. The purpose of this work is to examine the dynamics of this dual mechanism between the two using the illustrative Fröhlich model. In particular, the influence of the low-temperature phonon dynamics on the superconducting properties in the intermediate coupling range is investigated. The influence on the Holstein reduction factor as well as the enhancement in the zero-point fluctuations and in the electron-phonon coupling are calculated numerically. We also examine these effects in the presence of superconductivity. Within this model, the contribution of the electron-phonon interaction as one of the important elements in the mechanisms of superconductivity can reach values as high as 15-20% of the characteristic scale of the lattice vibrational energy. The second motivation of this work is to understand the nature of the Tc-dependent temperature anomalies observed in the Debye-Waller factor, dynamical pair correlations, and average atomic vibrational energies for a number of high-temperature superconductors. In our approach we do not claim nor believe that the electron-phonon interaction is the primary mechanism leading to high-temperature superconductivity. Nevertheless, our calculations suggest that the dynamically induced low-temperature phonon correlation model can account for these anomalies and illustrates their possible common origin. Finally, the relevance of incorporating these low-temperature effects into more realistic models of high-temperature superconductivity including both the charge and spin degrees and other similar ideas existing in the literature are discussed.

Stopping power beyond the adiabatic approximation

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

Caro, M.; Correa, A. A.; Artacho, E.

2017-06-01

Energetic ions traveling in solids deposit energy in a variety of ways, being nuclear and electronic stopping the two avenues in which dissipation is usually treated. This separation between electrons and ions relies on the adiabatic approximation in which ions interact via forces derived from the instantaneous electronic ground state. In a more detailed view, in which non-adiabatic effects are explicitly considered, electronic excitations alter the atomic bonding, which translates into changes in the interatomic forces. In this work, we use time dependent density functional theory and forces derived from the equations of Ehrenfest dynamics that depend instantaneously on themore » time-dependent electronic density. With them we analyze how the inter-ionic forces are affected by electronic excitations in a model of a Ni projectile interacting with a Ni target, a metallic system with strong electronic stopping and shallow core level states. We find that the electronic excitations induce substantial modifications to the inter-ionic forces, which translate into nuclear stopping power well above the adiabatic prediction. Particularly, we observe that most of the alteration of the adiabatic potential in early times comes from the ionization of the core levels of the target ions, not readily screened by the valence electrons.« less

Theory of hydrodynamic transport in fluctuating electronic charge density wave states

NASA Astrophysics Data System (ADS)

Delacrétaz, Luca V.; Goutéraux, Blaise; Hartnoll, Sean A.; Karlsson, Anna

2017-11-01

We describe the collective hydrodynamic motion of an incommensurate charge density wave state in a clean electronic system. Our description simultaneously incorporates the effects of both pinning due to weak disorder and also phase relaxation due to proliferating dislocations. We show that the interplay between these two phenomena has important consequences for charge and momentum transport. For instance, it can lead to metal-insulator transitions. We furthermore identify signatures of fluctuating density waves in frequency and spatially resolved conductivities. Phase disordering is well known to lead to a large viscosity. We derive a precise formula for the phase relaxation rate in terms of the viscosity in the dislocation cores. We thereby determine the viscosity of the superconducting state of BSCCO from the observed melting dynamics of Abrikosov lattices and show that the result is consistent with dissipation into Bogoliubov quasiparticles.

Comment on: Polar Plumes and Fine-scale Coronal Structures - On the Interpretation of Coronal Radio Sounding Data by Patzold and Bird

NASA Technical Reports Server (NTRS)

Woo, R.; Habbal, S. R.

1998-01-01

Radio occultation measurements, which probe electron density over a wide dynamic range with high sensitivity and high spatial and temporal resolution reveal a solar corona permeated by a hierarchy of filamentary structures.

Multi-charge-state molecular dynamics and self-diffusion coefficient in the warm dense matter regime

NASA Astrophysics Data System (ADS)

Fu, Yongsheng; Hou, Yong; Kang, Dongdong; Gao, Cheng; Jin, Fengtao; Yuan, Jianmin

2018-01-01

We present a multi-ion molecular dynamics (MIMD) simulation and apply it to calculating the self-diffusion coefficients of ions with different charge-states in the warm dense matter (WDM) regime. First, the method is used for the self-consistent calculation of electron structures of different charge-state ions in the ion sphere, with the ion-sphere radii being determined by the plasma density and the ion charges. The ionic fraction is then obtained by solving the Saha equation, taking account of interactions among different charge-state ions in the system, and ion-ion pair potentials are computed using the modified Gordon-Kim method in the framework of temperature-dependent density functional theory on the basis of the electron structures. Finally, MIMD is used to calculate ionic self-diffusion coefficients from the velocity correlation function according to the Green-Kubo relation. A comparison with the results of the average-atom model shows that different statistical processes will influence the ionic diffusion coefficient in the WDM regime.

Molecular dynamics simulation of Coulomb explosion, melting and shock wave creation in silicon after an ionization pulse

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

Li, Zhongyu; Shao, Lin, E-mail: lshao@tamu.edu; Chen, Di

Strong electronic stopping power of swift ions in a semiconducting or insulating substrate can lead to localized electron stripping. The subsequent repulsive interactions among charged target atoms can cause Coulomb explosion. Using molecular dynamics simulation, we simulate Coulomb explosion in silicon by introducing an ionization pulse lasting for different periods, and at different substrate temperatures. We find that the longer the pulse period, the larger the melting radius. The observation can be explained by a critical energy density model assuming that melting required thermal energy density is a constant value and the total thermal energy gained from Coulomb explosion ismore » linearly proportional to the ionization period. Our studies also show that melting radius is larger at higher substrate temperatures. The temperature effect is explained due to a longer structural relaxation above the melting temperature at original ionization boundary due to lower heat dissipation rates. Furthermore, simulations show the formation of shock waves, created due to the compression from the melting core.« less

Structural, electronic, mechanical, and dynamical properties of graphene oxides: A first principles study

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

Dabhi, Shweta D.; Gupta, Sanjay D.; Jha, Prafulla K., E-mail: prafullaj@yahoo.com

We report the results of a theoretical study on the structural, electronic, mechanical, and vibrational properties of some graphene oxide models (GDO, a-GMO, z-GMO, ep-GMO and mix-GMO) at ambient pressure. The calculations are based on the ab-initio plane-wave pseudo potential density functional theory, within the generalized gradient approximations for the exchange and correlation functional. The calculated values of lattice parameters, bulk modulus, and its first order pressure derivative are in good agreement with other reports. A linear response approach to the density functional theory is used to derive the phonon frequencies. We discuss the contribution of the phonons in themore » dynamical stability of graphene oxides and detailed analysis of zone centre phonon modes in all the above mentioned models. Our study demonstrates a wide range of energy gap available in the considered models of graphene oxide and hence the possibility of their use in nanodevices.« less

Simulating Excitons in MoS2 with Time-Dependent Density Functional Theory

NASA Astrophysics Data System (ADS)

Flamant, Cedric; Kolesov, Grigory; Kaxiras, Efthimios

Monolayer molybdenum disulfide, owing to its graphene-like two-dimensional geometry whilst still having a finite bandgap, is a material of great interest in condensed matter physics and for potential application in electronic devices. In particular, MoS2 exhibits significant excitonic effects, a desirable quality for fundamental many-body research. Time-dependent density functional theory (TD-DFT) allows us to simulate dynamical effects as well as temperature-based effects in a natural way given the direct treatment of the time evolution of the system. We present a TD-DFT study of monolayer MoS2 exciton dynamics, examining various qualitative and quantitative predictions in pure samples and in the presence of defects. In particular, we generate an absorption spectrum through simulated pulse excitation for comparison to experiment and also analyze the response of the exciton in an external electric field.In this work we also discuss the electronic structure of the exciton in MoS2 with and without vacancies.

From Two- to Three-Dimensional Structures of a Supertetrahedral Boran Using Density Functional Calculations.

PubMed

Getmanskii, Iliya V; Minyaev, Ruslan M; Steglenko, Dmitrii V; Koval, Vitaliy V; Zaitsev, Stanislav A; Minkin, Vladimir I

2017-08-14

With help of the DFT calculations and imposing of periodic boundary conditions the geometrical and electronic structures were investigated of two- and three-dimensional boron systems designed on the basis of graphane and diamond lattices in which carbons were replaced with boron tetrahedrons. The consequent studies of two- and three-layer systems resulted in the construction of a three-dimensional supertetrahedral borane crystal structure. The two-dimensional supertetrahedral borane structures with less than seven layers are dynamically unstable. At the same time the three-dimensional superborane systems were found to be dynamically stable. Lack of the forbidden electronic zone for the studied boron systems testifies that these structures can behave as good conductors. The low density of the supertetrahedral borane crystal structures (0.9 g cm -3 ) is close to that of water, which offers the perspective for their application as aerospace and cosmic materials. © 2017 The Authors. Published by Wiley-VCH Verlag GmbH & Co. KGaA.

Enhanced doping effect on tuning structural phases of monolayer antimony

NASA Astrophysics Data System (ADS)

Wang, Jizhang; Yang, Teng; Zhang, Zhidong; Yang, Li

2018-05-01

Doping is capable to control the atomistic structure, electronic structure, and even to dynamically realize a semiconductor-metal transition in two-dimensional (2D) transition metal dichalcogenides (TMDs). However, the high critical doping density (˜1014 electron/cm2), compound nature, and relatively low carrier mobility of TMDs limits broader applications. Using first-principles calculations, we predict that, via a small transition potential, a substantially lower hole doping density (˜6 × 1012 hole/cm2) can switch the ground-state structure of monolayer antimony from the hexagonal β-phase, a 2D semiconductor with excellent transport performance and air stability but an indirect bandgap, to the orthorhombic α phase with a direct bandgap and potentially better carrier mobility. We further show that this structural engineering can be achieved by the established electrostatic doping, surface functional adsorption, or directly using graphene substrate. This gives hope to dynamically tuning and large-scale production of 2D single-element semiconductors that simultaneously exhibit remarkable transport and optical performance.

Generation of lower and upper bands of electrostatic electron cyclotron harmonic waves in the Van Allen radiation belts

DOE PAGES

Zhou, Qinghua; Xiao, Fuliang; Yang, Chang; ...

2017-05-22

Electrostatic electron cyclotron harmonic (ECH) waves generated by the electron loss cone distribution can produce efficient scattering loss of plasma sheet electrons, which has a significant effect on the dynamics in the outer magnetosphere. Here we report two ECH emission events around the same location L≈ 5.7–5.8, MLT ≈ 12 from Van Allen Probes on 11 February (event A) and 9 January 2014 (event B), respectively. The spectrum of ECH waves was centered at the lower half of the harmonic bands during event A, but the upper half during event B. The observed electron phase space density in both eventsmore » is fitted by the subtracted bi-Maxwellian distribution, and the fitting functions are used to evaluate the local growth rates of ECH waves based on a linear theory for homogeneous plasmas. ECH waves are excited by the loss cone instability of 50 eV–1 keV electrons in the lower half of harmonic bands in the low-density plasmasphere in event A, and 1–10 keV electrons in the upper half of harmonic bands in a relatively high-density region in event B. Here, the current results successfully explain observations and provide a first direct evidence on how ECH waves are generated in the lower and upper half of harmonic frequency bands.« less

Generation of lower and upper bands of electrostatic electron cyclotron harmonic waves in the Van Allen radiation belts

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

Zhou, Qinghua; Xiao, Fuliang; Yang, Chang

Electrostatic electron cyclotron harmonic (ECH) waves generated by the electron loss cone distribution can produce efficient scattering loss of plasma sheet electrons, which has a significant effect on the dynamics in the outer magnetosphere. Here we report two ECH emission events around the same location L≈ 5.7–5.8, MLT ≈ 12 from Van Allen Probes on 11 February (event A) and 9 January 2014 (event B), respectively. The spectrum of ECH waves was centered at the lower half of the harmonic bands during event A, but the upper half during event B. The observed electron phase space density in both eventsmore » is fitted by the subtracted bi-Maxwellian distribution, and the fitting functions are used to evaluate the local growth rates of ECH waves based on a linear theory for homogeneous plasmas. ECH waves are excited by the loss cone instability of 50 eV–1 keV electrons in the lower half of harmonic bands in the low-density plasmasphere in event A, and 1–10 keV electrons in the upper half of harmonic bands in a relatively high-density region in event B. Here, the current results successfully explain observations and provide a first direct evidence on how ECH waves are generated in the lower and upper half of harmonic frequency bands.« less

Dynamic spin injection into a quantum well coupled to a spin-split bound state

NASA Astrophysics Data System (ADS)

Maslova, N. S.; Rozhansky, I. V.; Mantsevich, V. N.; Arseyev, P. I.; Averkiev, N. S.; Lähderanta, E.

2018-05-01

We present a theoretical analysis of dynamic spin injection due to spin-dependent tunneling between a quantum well (QW) and a bound state split in spin projection due to an exchange interaction or external magnetic field. We focus on the impact of Coulomb correlations at the bound state on spin polarization and sheet density kinetics of the charge carriers in the QW. The theoretical approach is based on kinetic equations for the electron occupation numbers taking into account high order correlation functions for the bound state electrons. It is shown that the on-site Coulomb repulsion leads to an enhanced dynamic spin polarization of the electrons in the QW and a delay in the carriers tunneling into the bound state. The interplay of these two effects leads to nontrivial dependence of the spin polarization degree, which can be probed experimentally using time-resolved photoluminescence experiments. It is demonstrated that the influence of the Coulomb interactions can be controlled by adjusting the relaxation rates. These findings open a new way of studying the Hubbard-like electron interactions experimentally.

Atomic and electronic structure transformations of silver nanoparticles under rapid cooling conditions.

PubMed

Lobato, I; Rojas, J; Landauro, C V; Torres, J

2009-02-04

The structural evolution and dynamics of silver nanodrops Ag(2869) (4.4 nm in diameter) under rapid cooling conditions have been studied by means of molecular dynamics simulations and electronic density of state calculations. The interaction of silver atoms is modelled by a tight-binding semiempirical interatomic potential proposed by Cleri and Rosato. The pair correlation functions and the pair analysis technique are used to reveal the structural transition in the process of solidification. It is shown that Ag nanoparticles evolve into different nanostructures under different cooling processes. At a cooling rate of 1.5625 × 10(13) K s(-1) the nanoparticles preserve an amorphous-like structure containing a large amount of 1551 and 1541 pairs which correspond to icosahedral symmetry. For a lower cooling rate (1.5625 × 10(12) K s(-1)), the nanoparticles transform into a crystal-like structure consisting mainly of 1421 and 1422 pairs which correspond to the face centred cubic and hexagonal close packed structures, respectively. The variations of the electronic density of states for the differently cooled nanoparticles are small, but in correspondence with the structural changes.

Under-the-barrier dynamics in laser-induced relativistic tunneling.

PubMed

Klaiber, Michael; Yakaboylu, Enderalp; Bauke, Heiko; Hatsagortsyan, Karen Z; Keitel, Christoph H

2013-04-12

The tunneling dynamics in relativistic strong-field ionization is investigated with the aim to develop an intuitive picture for the relativistic tunneling regime. We demonstrate that the tunneling picture applies also in the relativistic regime by introducing position dependent energy levels. The quantum dynamics in the classically forbidden region features two time scales, the typical time that characterizes the probability density's decay of the ionizing electron under the barrier (Keldysh time) and the time interval which the electron spends inside the barrier (Eisenbud-Wigner-Smith tunneling time). In the relativistic regime, an electron momentum shift as well as a spatial shift along the laser propagation direction arise during the under-the-barrier motion which are caused by the laser magnetic field induced Lorentz force. The momentum shift is proportional to the Keldysh time, while the wave-packet's spatial drift is proportional to the Eisenbud-Wigner-Smith time. The signature of the momentum shift is shown to be present in the ionization spectrum at the detector and, therefore, observable experimentally. In contrast, the signature of the Eisenbud-Wigner-Smith time delay disappears at far distances for pure quasistatic tunneling dynamics.

Time-domain ab initio modeling of photoinduced dynamics at nanoscale interfaces.

PubMed

Wang, Linjun; Long, Run; Prezhdo, Oleg V

2015-04-01

Nonequilibrium processes involving electronic and vibrational degrees of freedom in nanoscale materials are under active experimental investigation. Corresponding theoretical studies are much scarcer. The review starts with the basics of time-dependent density functional theory, recent developments in nonadiabatic molecular dynamics, and the fusion of the two techniques. Ab initio simulations of this kind allow us to directly mimic a great variety of time-resolved experiments performed with pump-probe laser spectroscopies. The focus is on the ultrafast photoinduced charge and exciton dynamics at interfaces formed by two complementary materials. We consider purely inorganic materials, inorganic-organic hybrids, and all organic interfaces, involving bulk semiconductors, metallic and semiconducting nanoclusters, graphene, carbon nanotubes, fullerenes, polymers, molecular crystals, molecules, and solvent. The detailed atomistic insights available from time-domain ab initio studies provide a unique description and a comprehensive understanding of the competition between electron transfer, thermal relaxation, energy transfer, and charge recombination processes. These advances now make it possible to directly guide the development of organic and hybrid solar cells, as well as photocatalytic, electronic, spintronic, and other devices relying on complex interfacial dynamics.

Ultrafast 25-fs relaxation in highly excited states of methyl azide mediated by strong nonadiabatic coupling.

PubMed

Peters, William K; Couch, David E; Mignolet, Benoit; Shi, Xuetao; Nguyen, Quynh L; Fortenberry, Ryan C; Schlegel, H Bernhard; Remacle, Françoise; Kapteyn, Henry C; Murnane, Margaret M; Li, Wen

2017-12-26

Highly excited electronic states are challenging to explore experimentally and theoretically-due to the large density of states and the fact that small structural changes lead to large changes in electronic character with associated strong nonadiabatic dynamics. They can play a key role in astrophysical and ionospheric chemistry, as well as the detonation chemistry of high-energy density materials. Here, we implement ultrafast vacuum-UV (VUV)-driven electron-ion coincidence imaging spectroscopy to directly probe the reaction pathways of highly excited states of energetic molecules-in this case, methyl azide. Our data, combined with advanced theoretical simulations, show that photoexcitation of methyl azide by a 10-fs UV pulse at 8 eV drives fast structural changes and strong nonadiabatic coupling that leads to relaxation to other excited states on a surprisingly fast timescale of 25 fs. This ultrafast relaxation differs from dynamics occurring on lower excited states, where the timescale required for the wavepacket to reach a region of strong nonadiabatic coupling is typically much longer. Moreover, our theoretical calculations show that ultrafast relaxation of the wavepacket to a lower excited state occurs along one of the conical intersection seams before reaching the minimum energy conical intersection. These findings are important for understanding the unique strongly coupled non-Born-Oppenheimer molecular dynamics of VUV-excited energetic molecules. Although such observations have been predicted for many years, this study represents one of the few where such strongly coupled non-Born-Oppenheimer molecular dynamics of VUV-excited energetic molecules have been conclusively observed directly, making it possible to identify the ultrafast reaction pathways.

Ab initio determination of effective electron-phonon coupling factor in copper

NASA Astrophysics Data System (ADS)

Ji, Pengfei; Zhang, Yuwen

2016-04-01

The electron temperature Te dependent electron density of states g (ε), Fermi-Dirac distribution f (ε), and electron-phonon spectral function α2 F (Ω) are computed as prerequisites before achieving effective electron-phonon coupling factor Ge-ph. The obtained Ge-ph is implemented into a molecular dynamics (MD) and two-temperature model (TTM) coupled simulation of femtosecond laser heating. By monitoring temperature evolutions of electron and lattice subsystems, the result utilizing Ge-ph from ab initio calculation shows a faster decrease of Te and increase of Tl than those using Ge-ph from phenomenological treatment. The approach of calculating Ge-ph and its implementation into MD-TTM simulation is applicable to other metals.

Spatial and temporal dynamics of a pulsed spark microplasma used for aerosol analysis

NASA Astrophysics Data System (ADS)

Zheng, Lina; Kulkarni, Pramod; Diwakar, Prasoon

2018-06-01

The spatial and temporal dynamics of a pulsed, electrical spark microplasma used for spectrochemical analysis of aerosols was investigated. The spark discharge was generated by applying a high voltage pulse between a coaxial anode and cathode. Aerosol particles of black carbon were collected on the cathode for 2 min, following which the pulsed microplasma was introduced, leading to ablation and atomization of the collected particles. The space- and time-resolved emission spectra showed that the atomic emission signal from the carbon species originated from the region close to the cathode surface during the early evolution of the microplasma. The C I and C II atomic emission reached peak intensities at 11 and 6 μs delay time, respectively. Peak emission intensities occurred between 0.5-1.3 mm above the cathode surface. The average excitation temperature and the electron number density of the spark microplasma were estimated to be 23,000 K, and 1.6 × 1017 cm-3, respectively. The effects of pulse energy on the excitation temperature and electron density were also investigated. The results provide insights into the dynamics of the pulsed spark microplasma and are helpful in optimizing elemental analysis of aerosols using this technique.

Bunch Length Measurements Using CTR at the AWA with Comparison to Simulation

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

Neveu, N.; Spentzouris, L.; Halavanau, A.

In this paper we present electron bunch length measurements at the Argonne Wakefield Accelerator (AWA) photoinjector facility. The AWA accelerator has a large dynamic charge density range, with electron beam charge varying between 0.1 nC - 100 nC, and laser spot size diameter at the cathode between 0.1 mm - 18 mm. The bunch length measurements were taken at different charge densities using a metallic screen and a Michelson interferometer to perform autocorrelation scans of the corresponding coherent transition radiation (CTR). A liquid helium-cooled 4K bolometer was used to register the interferometer signal. The experimental results are compared with OPAL-Tmore » numerical simulations.« less

Conductance signatures of electron confinement induced by strained nanobubbles in graphene

NASA Astrophysics Data System (ADS)

Bahamon, Dario A.; Qi, Zenan; Park, Harold S.; Pereira, Vitor M.; Campbell, David K.

2015-09-01

We investigate the impact of strained nanobubbles on the conductance characteristics of graphene nanoribbons using a combined molecular dynamics - tight-binding simulation scheme. We describe in detail how the conductance, density of states, and current density of zigzag or armchair graphene nanoribbons are modified by the presence of a nanobubble. In particular, we establish that low-energy electrons can be confined in the vicinity of or within the nanobubbles by the delicate interplay among the pseudomagnetic field pattern created by the shape of the bubble, mode mixing, and substrate interaction. The coupling between confined evanescent states and propagating modes can be enhanced under different clamping conditions, which translates into Fano resonances in the conductance traces.

Stopping dynamics of ions passing through correlated honeycomb clusters

NASA Astrophysics Data System (ADS)

Balzer, Karsten; Schlünzen, Niclas; Bonitz, Michael

2016-12-01

A combined nonequilibrium Green functions-Ehrenfest dynamics approach is developed that allows for a time-dependent study of the energy loss of a charged particle penetrating a strongly correlated system at zero and finite temperatures. Numerical results are presented for finite inhomogeneous two-dimensional Fermi-Hubbard models, where the many-electron dynamics in the target are treated fully quantum mechanically and the motion of the projectile is treated classically. The simulations are based on the solution of the two-time Dyson (Keldysh-Kadanoff-Baym) equations using the second-order Born, third-order, and T -matrix approximations of the self-energy. As application, we consider protons and helium nuclei with a kinetic energy between 1 and 500 keV/u passing through planar fragments of the two-dimensional honeycomb lattice and, in particular, examine the influence of electron-electron correlations on the energy exchange between projectile and electron system. We investigate the time dependence of the projectile's kinetic energy (stopping power), the electron density, the double occupancy, and the photoemission spectrum. Finally, we show that, for a suitable choice of the Hubbard model parameters, the results for the stopping power are in fair agreement with ab initio simulations for particle irradiation of single-layer graphene.

Ab Initio Study of Electronic Excitation Effects on SrTiO 3

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

Zhao, Shijun; Zhang, Yanwen; Weber, William J.

Interaction of energetic ions or lasers with solids often induces electronic excitations that may modify material properties significantly. In this study, effects of electronic excitations on strontium titanate SrTiO 3 (STO) are investigated based on first-principles calculations. The lattice structure, electronic properties, lattice vibrational frequencies, and dynamical stabilities are studied in detail. The results suggest that electronic excitation induces charge redistribution that is mainly observed in Ti–O bonds. The electronic band gap increases with increasing electronic excitation, as excitation mainly induces depopulation of Ti 3d states. Phonon analysis indicates that there is a large phonon band gap induced by electronicmore » excitation because of the changes in the vibrational properties of Ti and O atoms. In addition, a new peak appears in the phonon density of states with imaginary frequencies, an indication of lattice instability. Further dynamics simulations confirm that STO undergoes transition to an amorphous structure under strong electronic excitations. In conclusion, the optical properties of STO under electronic excitation are consistent with the evolution of atomic and electronic structures, which suggests a possibility to probe the properties of STO in nonequilibrium state using optical measurement.« less

Ab Initio Study of Electronic Excitation Effects on SrTiO 3

DOE PAGES

Zhao, Shijun; Zhang, Yanwen; Weber, William J.

2017-11-14

Interaction of energetic ions or lasers with solids often induces electronic excitations that may modify material properties significantly. In this study, effects of electronic excitations on strontium titanate SrTiO 3 (STO) are investigated based on first-principles calculations. The lattice structure, electronic properties, lattice vibrational frequencies, and dynamical stabilities are studied in detail. The results suggest that electronic excitation induces charge redistribution that is mainly observed in Ti–O bonds. The electronic band gap increases with increasing electronic excitation, as excitation mainly induces depopulation of Ti 3d states. Phonon analysis indicates that there is a large phonon band gap induced by electronicmore » excitation because of the changes in the vibrational properties of Ti and O atoms. In addition, a new peak appears in the phonon density of states with imaginary frequencies, an indication of lattice instability. Further dynamics simulations confirm that STO undergoes transition to an amorphous structure under strong electronic excitations. In conclusion, the optical properties of STO under electronic excitation are consistent with the evolution of atomic and electronic structures, which suggests a possibility to probe the properties of STO in nonequilibrium state using optical measurement.« less

Arbitrarily shaped high-coherence electron bunches from cold atoms

NASA Astrophysics Data System (ADS)

McCulloch, A. J.; Sheludko, D. V.; Saliba, S. D.; Bell, S. C.; Junker, M.; Nugent, K. A.; Scholten, R. E.

2011-10-01

Ultrafast electron diffractive imaging of nanoscale objects such as biological molecules and defects in solid-state devices provides crucial information on structure and dynamic processes: for example, determination of the form and function of membrane proteins, vital for many key goals in modern biological science, including rational drug design. High brightness and high coherence are required to achieve the necessary spatial and temporal resolution, but have been limited by the thermal nature of conventional electron sources and by divergence due to repulsive interactions between the electrons, known as the Coulomb explosion. It has been shown that, if the electrons are shaped into ellipsoidal bunches with uniform density, the Coulomb explosion can be reversed using conventional optics, to deliver the maximum possible brightness at the target. Here we demonstrate arbitrary and real-time control of the shape of cold electron bunches extracted from laser-cooled atoms. The ability to dynamically shape the electron source itself and to observe this shape in the propagated electron bunch provides a remarkable experimental demonstration of the intrinsically high spatial coherence of a cold-atom electron source, and the potential for alleviation of electron-source brightness limitations due to Coulomb explosion.

Computational Analysis of Hybrid Two-Photon Absorbers with Excited State Absorption

DTIC Science & Technology

2007-03-01

level. This hybrid arrangement creates a complex dynamical system in which the electron carrier concentration of every photo-activated energy level...spatiotemporal details of the electron population densities of each photo-activated energy level as well as the pulse shape in space and time. The main...experiments at low input energy . However, further additions must be done to the calculation of the optical path for high input energy . 1 15. SUBJECT TERM

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

Zhu, Yuanyuan; Sushko, Peter V.; Melzer, Daniel

A novel pathway of increasing the surface density of catalytically active oxygen radical sites on a MoVTeNb oxide (M1 phase) catalyst during alkane oxidative dehydrogenation is reported. The novel sites form when a fraction of Te4+ is reduced and emitted from the M1 crystals under catalytic operating conditions, without compromising structural integrity of the catalyst framework. Density functional theory calculations show this Te reduction induces multiple inter-related electron transfers, and the associated cooperative effects lead to the formation of O- radicals. The in situ observations identify complex dynamic changes in the catalyst on an atomistic level, highlighting a new waymore » to tailor structure and dynamics for highly active catalysts.« less

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.

Anomalous X-Ray yields under surface wave resonance during reflection high energy electron diffraction and adatom site determination

PubMed

Yamanaka; Ino

2000-05-08

In L x-ray emissions from a Si(111)-sqrt[3]xsqrt[3]-In surface induced by electron beam irradiation were measured as functions of the incident glancing angle. Under surface wave resonance conditions, anomalous x-ray intensities were clearly observed. Using dynamical calculations, these intensities are well explained as changes in density of the electron wave field at adatom positions. From these intensities, the adatom site was analyzed, and it was found that the T4 model is better than the H3 model.

Cassini measurements of cold plasma in the ionosphere of Titan.

PubMed

Wahlund, J E; Boström, R; Gustafsson, G; Gurnett, D A; Kurth, W S; Pedersen, A; Averkamp, T F; Hospodarsky, G B; Persoon, A M; Canu, P; Neubauer, F M; Dougherty, M K; Eriksson, A I; Morooka, M W; Gill, R; André, M; Eliasson, L; Müller-Wodarg, I

2005-05-13

The Cassini Radio and Plasma Wave Science (RPWS) Langmuir probe (LP) sensor observed the cold plasma environment around Titan during the first two flybys. The data show that conditions in Saturn's magnetosphere affect the structure and dynamics deep in the ionosphere of Titan. The maximum measured ionospheric electron number density reached 3800 per cubic centimeter near closest approach, and a complex chemistry was indicated. The electron temperature profiles are consistent with electron heat conduction from the hotter Titan wake. The ionospheric escape flux was estimated to be 10(25) ions per second.

RF plasma modeling of the Linac4 H- ion source

NASA Astrophysics Data System (ADS)

Mattei, S.; Ohta, M.; Hatayama, A.; Lettry, J.; Kawamura, Y.; Yasumoto, M.; Schmitzer, C.

2013-02-01

This study focuses on the modelling of the ICP RF-plasma in the Linac4 H- ion source currently being constructed at CERN. A self-consistent model of the plasma dynamics with the RF electromagnetic field has been developed by a PIC-MCC method. In this paper, the model is applied to the analysis of a low density plasma discharge initiation, with particular interest on the effect of the external magnetic field on the plasma properties, such as wall loss, electron density and electron energy. The employment of a multi-cusp magnetic field effectively limits the wall losses, particularly in the radial direction. Preliminary results however indicate that a reduced heating efficiency results in such a configuration. The effect is possibly due to trapping of electrons in the multi-cusp magnetic field, preventing their continuous acceleration in the azimuthal direction.

Separated spin-up and spin-down quantum hydrodynamics of degenerated electrons: Spin-electron acoustic wave appearance.

PubMed

Andreev, Pavel A

2015-03-01

The quantum hydrodynamic (QHD) model of charged spin-1/2 particles contains physical quantities defined for all particles of a species including particles with spin-up and with spin-down. Different populations of states with different spin directions are included in the spin density (the magnetization). In this paper I derive a QHD model, which separately describes spin-up electrons and spin-down electrons. Hence electrons with different projections of spins on the preferable direction are considered as two different species of particles. It is shown that the numbers of particles with different spin directions do not conserve. Hence the continuity equations contain sources of particles. These sources are caused by the interactions of the spins with the magnetic field. Terms of similar nature arise in the Euler equation. The z projection of the spin density is no longer an independent variable. It is proportional to the difference between the concentrations of the electrons with spin-up and the electrons with spin-down. The propagation of waves in the magnetized plasmas of degenerate electrons is considered. Two regimes for the ion dynamics, the motionless ions and the motion of the degenerate ions as the single species with no account of the spin dynamics, are considered. It is shown that this form of the QHD equations gives all solutions obtained from the traditional form of QHD equations with no distinction of spin-up and spin-down states. But it also reveals a soundlike solution called the spin-electron acoustic wave. Coincidence of most solutions is expected since this derivation was started with the same basic equation: the Pauli equation. Solutions arise due to the different Fermi pressures for the spin-up electrons and the spin-down electrons in the magnetic field. The results are applied to degenerate electron gas of paramagnetic and ferromagnetic metals in the external magnetic field. The dispersion of the spin-electron acoustic waves in the partially spin-polarized degenerate neutron matter are also considered.

Transportation of high-current ion and electron beams in the accelerator drift gap in the presence of an additional electron background

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

Karas’, V. I., E-mail: karas@kipt.kharkov.ua; Kornilov, E. A.; Manuilenko, O. V.

2015-12-15

The dynamics of a high-current ion beam propagating in the drift gap of a linear induction accelerator with collective focusing is studied using 3D numerical simulations in the framework of the full system of the Vlasov–Maxwell equations (code KARAT). The ion beam is neutralized by a comoving electron beam in the current density and, partially, in space charge, since the velocities of electrons and ions differ substantially. The dynamics of the high-current ion beam is investigated for different versions of additional neutralization of its space charge. It is established that, for a given configuration of the magnetic field and inmore » the presence of a specially programmed injection of additional electrons from the boundary opposite to the ion injection boundary, the angular divergence of the ion beam almost vanishes, whereas the current of the ion beam at the exit from the accelerator drift gap changes insignificantly and the beam remains almost monoenergetic.« less

Transportation of high-current ion and electron beams in the accelerator drift gap in the presence of an additional electron background

NASA Astrophysics Data System (ADS)

Karas', V. I.; Kornilov, E. A.; Manuilenko, O. V.; Tarakanov, V. P.; Fedorovskaya, O. V.

2015-12-01

The dynamics of a high-current ion beam propagating in the drift gap of a linear induction accelerator with collective focusing is studied using 3D numerical simulations in the framework of the full system of the Vlasov-Maxwell equations (code KARAT). The ion beam is neutralized by a comoving electron beam in the current density and, partially, in space charge, since the velocities of electrons and ions differ substantially. The dynamics of the high-current ion beam is investigated for different versions of additional neutralization of its space charge. It is established that, for a given configuration of the magnetic field and in the presence of a specially programmed injection of additional electrons from the boundary opposite to the ion injection boundary, the angular divergence of the ion beam almost vanishes, whereas the current of the ion beam at the exit from the accelerator drift gap changes insignificantly and the beam remains almost monoenergetic.

Inelastic X-ray Scattering Measurements of Ionization in Warm, Dense Matter

NASA Astrophysics Data System (ADS)

Davis, Paul F.

In this work we demonstrate spectrally resolved x-ray scattering from electron-plasma waves in shock-compressed deuterium and proton-heated matter. Because the spectral signature of inelastic x-ray scattering is strongly dependent on the free electron density of the system, it is used to infer ionization in dynamically heated samples. Using 2-6 ns, 500 J laser pulses from LLNL's Janus laser, we shocked liquid deuterium to pressures approaching 50 GPa, reaching compressions of 4 times liquid density. A second laser produced intense 2 keV x-rays. By collecting and spectrally dispersing forward scattered photons at 45°, the onset of ionization was detected at compressions of about 3 times in the form of plasmon oscillations. Backscattered x-rays bolstered this observation by measuring the free electron distribution through Compton scattering. Comparison with simulations shows very close agreement between the pressure dependence of ionization and molecular dissociation in dynamically compressed deuterium. In a second set of experiments, a 10 ps, 200 J Titan laser pulse was split into two beams. One created a stream of MeV protons to heat samples of boron and boron-nitride and the other pumped 4.5 keV K-alpha radiation in a titanium foil to probe the hot target. We observed scattered x-rays 300 ps after heating, noting a strong difference in average ionization between the two target materials at temperatures of 16 eV and very similar mass densities. Comparison with electron structure calculations suggests that this difference is due to a persistence of long-range ion structure in BN resulting in high-temperature band structure. These results underscore the importance of understanding the complex electron structure of materials even at electron-volt temperatures and gigapascal pressures. Our results provide new data to guide the theoretical modeling of warm, dense matter important to understanding giant planets and inertial fusion targets.

Effect of spin-orbit and on-site Coulomb interactions on the electronic structure and lattice dynamics of uranium monocarbide

NASA Astrophysics Data System (ADS)

Wdowik, U. D.; Piekarz, P.; Legut, D.; Jagło, G.

2016-08-01

Uranium monocarbide, a potential fuel material for the generation IV reactors, is investigated within density functional theory. Its electronic, magnetic, elastic, and phonon properties are analyzed and discussed in terms of spin-orbit interaction and localized versus itinerant behavior of the 5 f electrons. The localization of the 5 f states is tuned by varying the local Coulomb repulsion interaction parameter. We demonstrate that the theoretical electronic structure, elastic constants, phonon dispersions, and their densities of states can reproduce accurately the results of x-ray photoemission and bremsstrahlung isochromat measurements as well as inelastic neutron scattering experiments only when the 5 f states experience the spin-orbit interaction and simultaneously remain partially localized. The partial localization of the 5 f electrons could be represented by a moderate value of the on-site Coulomb interaction parameter of about 2 eV. The results of the present studies indicate that both strong electron correlations and spin-orbit effects are crucial for realistic theoretical description of the ground-state properties of uranium carbide.

Augmented Ehrenfest dynamics yields a rate for surface hopping

NASA Astrophysics Data System (ADS)

Subotnik, Joseph E.

2010-04-01

We present a new algorithm for mixed quantum-classical dynamics that helps bridge the gap between mean-field (Ehrenfest) and surface-hopping dynamics by defining a natural rate of decoherence. In order to derive this decoherence result, we have expanded the number of independent variables in the usual Ehrenfest routine so that mixed quantum-classical derivatives are now propagated in time alongside the usual Ehrenfest variables. Having done so, we compute a unique rate of decoherence using two independent approaches: (i) by comparing the equations of motion for the joint nuclear-electronic probability density in phase space according to Ehrenfest dynamics versus partial Wigner transform dynamics and (ii) by introducing a frozen Gaussian interpretation of Ehrenfest dynamics which allows nuclear wave packets to separate. The first consequence of this work is a means to rigorously check the accuracy of standard Ehrenfest dynamics. Second, this paper suggests a nonadiabatic dynamics algorithm, whereby the nuclei are propagated on the mean-field (Ehrenfest) potential energy surface and undergo stochastic decoherence events. Our work resembles the surface-hopping algorithm of Schwartz and co-workers [J. Chem. Phys. 123, 234106 (2005)]—only now without any adjustable parameters. For the case of two electronic states, we present numerical results on the so-called "Tully problems" and emphasize that future numerical benchmarking is still needed. Future work will also treat the problem of three or more electronic states.

Ultrafast Intramolecular Electron and Proton Transfer in Bis(imino)isoindole Derivatives.

PubMed

Driscoll, Eric; Sorenson, Shayne; Dawlaty, Jahan M

2015-06-04

Concerted motion of electrons and protons in the excited state is pertinent to a wide range of chemical phenomena, including those relevant for solar-to-fuel light harvesting. The excited state dynamics of small proton-bearing molecules are expected to serve as models for better understanding such phenomena. In particular, for designing the next generation of multielectron and multiproton redox catalysts, understanding the dynamics of more than one proton in the excited state is important. Toward this goal, we have measured the ultrafast dynamics of intramolecular excited state proton transfer in a recently synthesized dye with two equivalent transferable protons. We have used a visible ultrafast pump to initiate the proton transfer in the excited state, and have probed the transient absorption of the molecule over a wide bandwidth in the visible range. The measurement shows that the signal which is characteristic of proton transfer emerges within ∼710 fs. To identify whether both protons were transferred in the excited state, we have measured the ultrafast dynamics of a related derivative, where only a single proton was available for transfer. The measured proton transfer time in that molecule was ∼427 fs. The observed dynamics in both cases were reasonably fit with single exponentials. Supported by the ultrafast observations, steady-state fluorescence, and preliminary computations of the relaxed excited states, we argue that the doubly protonated derivative most likely transfers only one of its two protons in the excited state. We have performed calculations of the frontier molecular orbitals in the Franck-Condon region. The calculations show that in both derivatives, the excitation is primarily from the HOMO to LUMO causing a large rearrangement of the electronic charge density immediately after photoexcitation. In particular, charge density is shifted away from the phenolic protons and toward the proton acceptor nitrogens. The proton transfer is hypothesized to occur both due to enhanced acidity of the phenolic proton and enhanced basicity of the nitrogen in the excited state. We hope this study can provide insight for better understanding of the general class of excited state concerted electron-proton dynamics.

On the role of electronic friction for dissociative adsorption and scattering of hydrogen molecules at a Ru(0001) surface.

PubMed

Füchsel, Gernot; Schimka, Selina; Saalfrank, Peter

2013-09-12

The role of electronic friction and, more generally, of nonadiabatic effects during dynamical processes at the gas/metal surface interface is still a matter of discussion. In particular, it is not clear if electronic nonadiabaticity has an effect under "mild" conditions, when molecules in low rovibrational states interact with a metal surface. In this paper, we investigate the role of electronic friction on the dissociative sticking and (inelastic) scattering of vibrationally and rotationally cold H2 molecules at a Ru(0001) surface theoretically. For this purpose, classical molecular dynamics with electronic friction (MDEF) calculations are performed and compared to MD simulations without friction. The two H atoms move on a six-dimensional potential energy surface generated from gradient-corrected density functional theory (DFT), that is, all molecular degrees of freedom are accounted for. Electronic friction is included via atomic friction coefficients obtained from an embedded atom, free electron gas (FEG) model, with embedding densities taken from gradient-corrected DFT. We find that within this model, dissociative sticking probabilities as a function of impact kinetic energies and impact angles are hardly affected by nonadiabatic effects. If one accounts for a possibly enhanced electronic friction near the dissociation barrier, on the other hand, reduced sticking probabilities are observed, in particular, at high impact energies. Further, there is always an influence on inelastic scattering, in particular, as far as the translational and internal energy distribution of the reflected molecules is concerned. Additionally, our results shed light on the role played by the velocity distribution of the incident molecular beam for adsorption probabilities, where, in particular, at higher impact energies, large effects are found.

A Static and Dynamic Investigation of Quantum Nonlinear Transport in Highly Dense and Mobile 2D Electron Systems

NASA Astrophysics Data System (ADS)

Dietrich, Scott

Heterostructures made of semiconductor materials may be one of most versatile environments for the study of the physics of electron transport in two dimensions. These systems are highly customizable and demonstrate a wide range of interesting physical phenomena. In response to both microwave radiation and DC excitations, strongly nonlinear transport that gives rise to non-equilibrium electron states has been reported and investigated. We have studied GaAs quantum wells with a high density of high mobility two-dimensional electrons placed in a quantizing magnetic field. This study presents the observation of several nonlinear transport mechanisms produced by the quantum nature of these materials. The quantum scattering rate, 1tau/q, is an important parameter in these systems, defining the width of the quantized energy levels. Traditional methods of extracting 1tau/q involve studying the amplitude of Shubnikov-de Haas oscillations. We analyze the quantum positive magnetoresistance due to the cyclotron motion of electrons in a magnetic field. This method gives 1tau/q and has the additional benefit of providing access to the strength of electron-electron interactions, which is not possible by conventional techniques. The temperature dependence of the quantum scattering rate is found to be proportional to the square of the temperature and is in very good agreement with theory that considers electron-electron interactions in 2D systems. In quantum wells with a small scattering rate - which corresponds to well-defined Landau levels - quantum oscillations of nonlinear resistance that are independent of magnetic field strength have been observed. These oscillations are periodic in applied bias current and are connected to quantum oscillations of resistance at zero bias: either Shubnikov-de Haas oscillations for single subband systems or magnetointersubband oscillations for two subband systems. The bias-induced oscillations can be explained by a spatial variation of electron density across the sample. The theoretical model predicts the period of these oscillations to depend on the total electron density, which has been confirmed by controlling the density through a voltage top-gate on the sample. The peculiar nonlinear mechanism of quantal heating has garned much attention recently. This bulk phenomenon is a quantum manifestation of Joule heating where an applied bias current causes selective flattening in the electron distribution function but conserves overall broadening. This produces a highly non-equilibrium distribution of electrons that drastically effects the transport properties of the system. Recent studies have proposed contributions from edge states and/or skipping orbitals. We have shown that these contributions are minimal by studying the transition to the zero differential conductance state and comparing results between Hall and Corbino geometries. This demonstrated quantal heating as the dominant nonlinear mechanism in these systems. To study the dynamics of quantal heating, we applied microwave radiation simultaneously from two sources at frequencies ƒ1 and ƒ2 and measured the response of the system at the difference frequency, ƒ=|ƒ 1-ƒ2|. This provides direct access to the rate of inelastic scattering processes, 1tau/in, that tend to bring the electron distribution back to thermal equilibrium. While conventional measurements of the temperature dependence indicate that 1tau/in is proportional to temperature, recent DC investigations and our new dynamic measurements show either T2 or T3 dependence in different magnetic fields. Our microwave experiment is the first direct access to the inelastic relaxation rate and confirms the non-linear temperature dependence.

Multiconfiguration Pair-Density Functional Theory.

PubMed

Li Manni, Giovanni; Carlson, Rebecca K; Luo, Sijie; Ma, Dongxia; Olsen, Jeppe; Truhlar, Donald G; Gagliardi, Laura

2014-09-09

We present a new theoretical framework, called Multiconfiguration Pair-Density Functional Theory (MC-PDFT), which combines multiconfigurational wave functions with a generalization of density functional theory (DFT). A multiconfigurational self-consistent-field (MCSCF) wave function with correct spin and space symmetry is used to compute the total electronic density, its gradient, the on-top pair density, and the kinetic and Coulomb contributions to the total electronic energy. We then use a functional of the total density, its gradient, and the on-top pair density to calculate the remaining part of the energy, which we call the on-top-density-functional energy in contrast to the exchange-correlation energy of Kohn-Sham DFT. Because the on-top pair density is an element of the two-particle density matrix, this goes beyond the Hohenberg-Kohn theorem that refers only to the one-particle density. To illustrate the theory, we obtain first approximations to the required new type of density functionals by translating conventional density functionals of the spin densities using a simple prescription, and we perform post-SCF density functional calculations using the total density, density gradient, and on-top pair density from the MCSCF calculations. Double counting of dynamic correlation or exchange does not occur because the MCSCF energy is not used. The theory is illustrated by applications to the bond energies and potential energy curves of H2, N2, F2, CaO, Cr2, and NiCl and the electronic excitation energies of Be, C, N, N(+), O, O(+), Sc(+), Mn, Co, Mo, Ru, N2, HCHO, C4H6, c-C5H6, and pyrazine. The method presented has a computational cost and scaling similar to MCSCF, but a quantitative accuracy, even with the present first approximations to the new types of density functionals, that is comparable to much more expensive multireference perturbation theory methods.

Three-dimensional structural dynamics of DNA origami Bennett linkages using individual-particle electron tomography

DOE PAGES

Lei, Dongsheng; Marras, Alexander E.; Liu, Jianfang; ...

2018-02-09

Scaffolded DNA origami has proven to be a powerful and efficient technique to fabricate functional nanomachines by programming the folding of a single-stranded DNA template strand into three-dimensional (3D) nanostructures, designed to be precisely motion-controlled. Although two-dimensional (2D) imaging of DNA nanomachines using transmission electron microscopy and atomic force microscopy suggested these nanomachines are dynamic in 3D, geometric analysis based on 2D imaging was insufficient to uncover the exact motion in 3D. In this paper, we use the individual-particle electron tomography method and reconstruct 129 density maps from 129 individual DNA origami Bennett linkage mechanisms at ~6-14 nm resolution. The statisticalmore » analyses of these conformations lead to understanding the 3D structural dynamics of Bennett linkage mechanisms. Moreover, our effort provides experimental verification of a theoretical kinematics model of DNA origami, which can be used as feedback to improve the design and control of motion via optimized DNA sequences and routing.« less

Three-dimensional structural dynamics of DNA origami Bennett linkages using individual-particle electron tomography

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

Lei, Dongsheng; Marras, Alexander E.; Liu, Jianfang

Scaffolded DNA origami has proven to be a powerful and efficient technique to fabricate functional nanomachines by programming the folding of a single-stranded DNA template strand into three-dimensional (3D) nanostructures, designed to be precisely motion-controlled. Although two-dimensional (2D) imaging of DNA nanomachines using transmission electron microscopy and atomic force microscopy suggested these nanomachines are dynamic in 3D, geometric analysis based on 2D imaging was insufficient to uncover the exact motion in 3D. In this paper, we use the individual-particle electron tomography method and reconstruct 129 density maps from 129 individual DNA origami Bennett linkage mechanisms at ~6-14 nm resolution. The statisticalmore » analyses of these conformations lead to understanding the 3D structural dynamics of Bennett linkage mechanisms. Moreover, our effort provides experimental verification of a theoretical kinematics model of DNA origami, which can be used as feedback to improve the design and control of motion via optimized DNA sequences and routing.« less

Active control of bright electron beams with RF optics for femtosecond microscopy

DOE PAGES

Williams, J.; Zhou, F.; Sun, T.; ...

2017-08-01

A frontier challenge in implementing femtosecond electron microscopy is to gain precise optical control of intense beams to mitigate collective space charge effects for significantly improving the throughput. In this paper, we explore the flexible uses of an RF cavity as a longitudinal lens in a high-intensity beam column for condensing the electron beams both temporally and spectrally, relevant to the design of ultrafast electron microscopy. Through the introduction of a novel atomic grating approach for characterization of electron bunch phase space and control optics, we elucidate the principles for predicting and controlling the phase space dynamics to reach optimalmore » compressions at various electron densities and generating conditions. We provide strategies to identify high-brightness modes, achieving ~100 fs and ~1 eV resolutions with 10 6 electrons per bunch, and establish the scaling of performance for different bunch charges. These results benchmark the sensitivity and resolution from the fundamental beam brightness perspective and also validate the adaptive optics concept to enable delicate control of the density-dependent phase space structures to optimize the performance, including delivering ultrashort, monochromatic, high-dose, or coherent electron bunches.« less

Active control of bright electron beams with RF optics for femtosecond microscopy

PubMed Central

Williams, J.; Zhou, F.; Sun, T.; Tao, Z.; Chang, K.; Makino, K.; Berz, M.; Duxbury, P. M.; Ruan, C.-Y.

2017-01-01

A frontier challenge in implementing femtosecond electron microscopy is to gain precise optical control of intense beams to mitigate collective space charge effects for significantly improving the throughput. Here, we explore the flexible uses of an RF cavity as a longitudinal lens in a high-intensity beam column for condensing the electron beams both temporally and spectrally, relevant to the design of ultrafast electron microscopy. Through the introduction of a novel atomic grating approach for characterization of electron bunch phase space and control optics, we elucidate the principles for predicting and controlling the phase space dynamics to reach optimal compressions at various electron densities and generating conditions. We provide strategies to identify high-brightness modes, achieving ∼100 fs and ∼1 eV resolutions with 106 electrons per bunch, and establish the scaling of performance for different bunch charges. These results benchmark the sensitivity and resolution from the fundamental beam brightness perspective and also validate the adaptive optics concept to enable delicate control of the density-dependent phase space structures to optimize the performance, including delivering ultrashort, monochromatic, high-dose, or coherent electron bunches. PMID:28868325

Thermal conductivity of graphene with defects induced by electron beam irradiation.

PubMed

Malekpour, Hoda; Ramnani, Pankaj; Srinivasan, Srilok; Balasubramanian, Ganesh; Nika, Denis L; Mulchandani, Ashok; Lake, Roger K; Balandin, Alexander A

2016-08-14

We investigate the thermal conductivity of suspended graphene as a function of the density of defects, ND, introduced in a controllable way. High-quality graphene layers are synthesized using chemical vapor deposition, transferred onto a transmission electron microscopy grid, and suspended over ∼7.5 μm size square holes. Defects are induced by irradiation of graphene with the low-energy electron beam (20 keV) and quantified by the Raman D-to-G peak intensity ratio. As the defect density changes from 2.0 × 10(10) cm(-2) to 1.8 × 10(11) cm(-2) the thermal conductivity decreases from ∼(1.8 ± 0.2) × 10(3) W mK(-1) to ∼(4.0 ± 0.2) × 10(2) W mK(-1) near room temperature. At higher defect densities, the thermal conductivity reveals an intriguing saturation-type behavior at a relatively high value of ∼400 W mK(-1). The thermal conductivity dependence on the defect density is analyzed using the Boltzmann transport equation and molecular dynamics simulations. The results are important for understanding phonon - point defect scattering in two-dimensional systems and for practical applications of graphene in thermal management.

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.

Computational Modeling of Low-Density Ultracold Plasmas

NASA Astrophysics Data System (ADS)

Witte, Craig

In this dissertation I describe a number of different computational investigations which I have undertaken during my time at Colorado State University. Perhaps the most significant of my accomplishments was the development of a general molecular dynamic model that simulates a wide variety of physical phenomena in ultracold plasmas (UCPs). This model formed the basis of most of the numerical investigations discussed in this thesis. The model utilized the massively parallel architecture of GPUs to achieve significant computing speed increases (up to 2 orders of magnitude) above traditional single core computing. This increased computing power allowed for each particle in an actual UCP experimental system to be explicitly modeled in simulations. By using this model, I was able to undertake a number of theoretical investigations into ultracold plasma systems. Chief among these was our lab's investigation of electron center-of-mass damping, in which the molecular dynamics model was an essential tool in interpreting the results of the experiment. Originally, it was assumed that this damping would solely be a function of electron-ion collisions. However, the model was able to identify an additional collisionless damping mechanism that was determined to be significant in the first iteration of our experiment. To mitigate this collisionless damping, the model was used to find a new parameter range where this mechanism was negligible. In this new parameter range, the model was an integral part in verifying the achievement of a record low measured UCP electron temperature of 1.57 +/- 0.28K and a record high electron strong coupling parameter, Gamma, of 0.35 +/-0.08$. Additionally, the model, along with experimental measurements, was used to verify the breakdown of the standard weak coupling approximation for Coulomb collisions. The general molecular dynamics model was also used in other contexts. These included the modeling of both the formation process of ultracold plasmas and the thermalization of the electron component of an ultracold plasma. Our modeling of UCP formation is still in its infancy, and there is still much outstanding work. However, we have already discovered a previously unreported electron heating mechanism that arises from an external electric field being applied during UCP formation. Thermalization modeling showed that the ion density distribution plays a role in the thermalization of electrons in ultracold plasma, a consideration not typically included in plasma modeling. A Gaussian ion density distribution was shown to lead to a slightly faster electron thermalization rate than an equivalent uniform ion density distribution as a result of collisionless effects. Three distinct phases of UCP electron thermalization during formation were identified. Finally, the dissertation will describe additional computational investigations that preceded the general molecular dynamics model. These include simulations of ultracold plasma ion expansion driven by non-neutrality, as well as an investigation into electron evaporation. To test the effects of non-neutrality on ion expansion, a numerical model was developed that used the King model of the electron to describe the electron distribution for an arbitrary charge imbalance. The model found that increased non-neutrality of the plasma led to the rapid expansion of ions on the plasma exterior, which in turn led to a sharp ion cliff-like spatial structure. Additionally, this rapid expansion led to additional cooling of the electron component of the plasma. The evaporation modeling was used to test the underlying assumptions of previously developed analytical expression for charged particle evaporation. The model used Monte Carlo techniques to simulate the collisions and the evaporation process. The model found that neither of the underlying assumption of the charged particle evaporation expressions held true for typical ultracold plasma parameters and provides a route for computations in spite of the breakdown of these two typical assumptions.

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.

Role of 6-Mercaptopurine in the potential therapeutic targets DNA base pairs and G-quadruplex DNA: insights from quantum chemical and molecular dynamics simulations.

PubMed

Radhika, R; Shankar, R; Vijayakumar, S; Kolandaivel, P

2018-05-01

The theoretical studies on DNA with the anticancer drug 6-Mercaptopurine (6-MP) are investigated using theoretical methods to shed light on drug designing. Among the DNA base pairs considered, 6-MP is stacked with GC with the highest interaction energy of -46.19 kcal/mol. Structural parameters revealed that structure of the DNA base pairs is deviated from the planarity of the equilibrium position due to the formation of hydrogen bonds and stacking interactions with 6-MP. These deviations are verified through the systematic comparison between X-H bond contraction and elongation and the associated blue shift and red shift values by both NBO analysis and vibrational analysis. Bent's rule is verified for the C-H bond contraction in the 6-MP interacted base pairs. The AIM results disclose that the higher values of electron density (ρ) and Laplacian of electron density (∇ 2 ρ) indicate the increased overlap between the orbitals that represent the strong interaction and positive values of the total electron density show the closed-shell interaction. The relative sensitivity of the chemical shift values for the DNA base pairs with 6-MP is investigated to confirm the hydrogen bond strength. Molecular dynamics simulation studies of G-quadruplex DNA d(TGGGGT) 4 with 6-MP revealed that the incorporation of 6-MP appears to cause local distortions and destabilize the G-quadruplex DNA.

Stochastic three-wave interaction in flaring solar loops

NASA Technical Reports Server (NTRS)

Vlahos, L.; Sharma, R. R.; Papadopoulos, K.

1983-01-01

A model is proposed for the dynamic structure of high-frequency microwave bursts. The dynamic component is attributed to beams of precipitating electrons which generate electrostatic waves in the upper hybrid branch. Coherent upconversion of the electrostatic waves to electromagnetic waves produces an intrinsically stochastic emission component which is superposed on the gyrosynchrotron continuum generated by stably trapped electron fluxes. The role of the density and temperature of the ambient plasma in the wave growth and the transition of the three wave upconversion to stochastic, despite the stationarity of the energy source, are discussed in detail. The model appears to reproduce the observational features for reasonable parameters of the solar flare plasma.

A coarse-grained polarizable force field for the ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate

NASA Astrophysics Data System (ADS)

Zeman, Johannes; Uhlig, Frank; Smiatek, Jens; Holm, Christian

2017-12-01

We present a coarse-grained polarizable molecular dynamics force field for the ionic liquid 1-butyl-3-methylimidazolium hexafluorophosphate ([BMIm][PF6]). For the treatment of electronic polarizability, we employ the Drude model. Our results show that the new explicitly polarizable force field reproduces important static and dynamic properties such as mass density, enthalpy of vaporization, diffusion coefficients, or electrical conductivity in the relevant temperature range. In situations where an explicit treatment of electronic polarizability might be crucial, we expect the force field to be an improvement over non-polarizable models, while still profiting from the reduction of computational cost due to the coarse-grained representation.

The effect of cross linking density on the mechanical properties and structure of the epoxy polymers: molecular dynamics simulation.

PubMed

Shokuhfar, Ali; Arab, Behrouz

2013-09-01

Recently, great attention has been focused on using epoxy polymers in different fields such as aerospace, automotive, biotechnology, and electronics, owing to their superior properties. In this study, the classical molecular dynamics (MD) was used to simulate the cross linking of diglycidyl ether of bisphenol-A (DGEBA) with diethylenetriamine (DETA) curing agent, and to study the behavior of resulted epoxy polymer with different conversion rates. The constant-strain (static) approach was then applied to calculate the mechanical properties (Bulk, shear and Young's moduli, elastic stiffness constants, and Poisson's ratio) of the uncured and cross-linked systems. Estimated material properties were found to be in good agreement with experimental observations. Moreover, the dependency of mechanical properties on the cross linking density was investigated and revealed improvements in the mechanical properties with increasing the cross linking density. The radial distribution function (RDF) was also used to study the evolution of local structures of the simulated systems as a function of cross linking density.

Ion sheath dynamics in a plasma for plasma-based ion implantation

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

Yatsuzuka, M.; Miki, S.; Azuma, K.

1999-07-01

Spatial and temporal growth and collapse of ion sheath around an electrode of a negative high-voltage pulse (voltage: {minus}10 kV, pulse duration: 10 {micro}s) have been studied in a plasma for plasma-based ion implantation. A spherical electrode of 1.9 cm in a diameter is immersed in a nitrogen plasma with the plasma density range of 10{sup 9} to 10{sup 10} cm{sup {minus}3}, the electron temperature of 1.4 eV and the gas pressure of 8x10{sup {minus}4} Torr. The transient sheath dynamics was observed by the measurement of electron saturation current to a Langmuir probe, where a depletion of electron saturation currentmore » indicates the arrival time of sheath edge at the probe position. The expanding speed of sheath edge is higher than the ion acoustic speed until the sheath length reaches the steady-state extent determined by Child-Langmuir law. In the region beyond the steady-state extent, the rarefying disturbance produced by sheath expansion continues to propagate into the plasma at the ion acoustic peed. After the pulse voltage is returned to zero (more exactly, the floating potential), the electron current begins to recover. When the pulse fall time is shorter than the plasma transit time, the electron saturation current overshoots the steady-state saturation current at once, resulting in an excess of plasma density which propagates like a tidal wave into the plasma at the ion acoustic speed.« less

The interface of SrTiO3 and H2O from density functional theory molecular dynamics

PubMed Central

Spijker, P.; Foster, A. S.

2016-01-01

We use dispersion-corrected density functional theory molecular dynamics simulations to predict the ionic, electronic and vibrational properties of the SrTiO3/H2O solid–liquid interface. Approximately 50% of surface oxygens on the planar SrO termination are hydroxylated at all studied levels of water coverage, the corresponding number being 15% for the planar TiO2 termination and 5% on the stepped TiO2-terminated surface. The lateral ordering of the hydration structure is largely controlled by covalent-like surface cation to H2O bonding and surface corrugation. We find a featureless electronic density of states in and around the band gap energy region at the solid–liquid interface. The vibrational spectrum indicates redshifting of the O–H stretching band due to surface-to-liquid hydrogen bonding and blueshifting due to high-frequency stretching vibrations of OH fragments within the liquid, as well as strong suppression of the OH stretching band on the stepped surface. We find highly varying rates of proton transfer above different SrTiO3 surfaces, owing to differences in hydrogen bond strength and the degree of dissociation of incident water. Trends in proton dynamics and the mode of H2O adsorption among studied surfaces can be explained by the differential ionicity of the Ti–O and Sr–O bonds in the SrTiO3 crystal. PMID:27713660

Comparing ab initio density-functional and wave function theories: the impact of correlation on the electronic density and the role of the correlation potential.

PubMed

Grabowski, Ireneusz; Teale, Andrew M; Śmiga, Szymon; Bartlett, Rodney J

2011-09-21

The framework of ab initio density-functional theory (DFT) has been introduced as a way to provide a seamless connection between the Kohn-Sham (KS) formulation of DFT and wave-function based ab initio approaches [R. J. Bartlett, I. Grabowski, S. Hirata, and S. Ivanov, J. Chem. Phys. 122, 034104 (2005)]. Recently, an analysis of the impact of dynamical correlation effects on the density of the neon atom was presented [K. Jankowski, K. Nowakowski, I. Grabowski, and J. Wasilewski, J. Chem. Phys. 130, 164102 (2009)], contrasting the behaviour for a variety of standard density functionals with that of ab initio approaches based on second-order Møller-Plesset (MP2) and coupled cluster theories at the singles-doubles (CCSD) and singles-doubles perturbative triples [CCSD(T)] levels. In the present work, we consider ab initio density functionals based on second-order many-body perturbation theory and coupled cluster perturbation theory in a similar manner, for a range of small atomic and molecular systems. For comparison, we also consider results obtained from MP2, CCSD, and CCSD(T) calculations. In addition to this density based analysis, we determine the KS correlation potentials corresponding to these densities and compare them with those obtained for a range of ab initio density functionals via the optimized effective potential method. The correlation energies, densities, and potentials calculated using ab initio DFT display a similar systematic behaviour to those derived from electronic densities calculated using ab initio wave function theories. In contrast, typical explicit density functionals for the correlation energy, such as VWN5 and LYP, do not show behaviour consistent with this picture of dynamical correlation, although they may provide some degree of correction for already erroneous explicitly density-dependent exchange-only functionals. The results presented here using orbital dependent ab initio density functionals show that they provide a treatment of exchange and correlation contributions within the KS framework that is more consistent with traditional ab initio wave function based methods.

Toward calculations of the 129Xe chemical shift in Xe@C60 at experimental conditions: relativity, correlation, and dynamics.

PubMed

Straka, Michal; Lantto, Perttu; Vaara, Juha

2008-03-27

We calculate the 129Xe chemical shift in endohedral Xe@C60 with systematic inclusion of the contributing physical effects to model the real experimental conditions. These are relativistic effects, electron correlation, the temperature-dependent dynamics, and solvent effects. The ultimate task is to obtain the right result for the right reason and to develop a physically justified methodological model for calculations and simulations of endohedral Xe fullerenes and other confined Xe systems. We use the smaller Xe...C6H6 model to calibrate density functional theory approaches against accurate correlated wave function methods. Relativistic effects as well as the coupling of relativity and electron correlation are evaluated using the leading-order Breit-Pauli perturbation theory. The dynamic effects are treated in two ways. In the first approximation, quantum dynamics of the Xe atom in a rigid cage takes advantage of the centrosymmetric potential for Xe within the thermally accessible distance range from the center of the cage. This reduces the problem of obtaining the solution of a diatomic rovibrational problem. In the second approach, first-principles classical molecular dynamics on the density functional potential energy hypersurface is used to produce the dynamical trajectory for the whole system, including the dynamic cage. Snapshots from the trajectory are used for calculations of the dynamic contribution to the absorption 129Xe chemical shift. The calculated nonrelativistic Xe shift is found to be highly sensitive to the optimized molecular structure and to the choice of the exchange-correlation functional. Relativistic and dynamic effects are significant and represent each about 10% of the nonrelativistic static shift at the minimum structure. While the role of the Xe dynamics inside of the rigid cage is negligible, the cage dynamics turns out to be responsible for most of the dynamical correction to the 129Xe shift. Solvent effects evaluated with a polarized continuum model are found to be very small.

Precipitating auroral electrons and lower thermospheric nitric oxide densities: SNOE, POLAR, SAMPEX, and NOAA/POES Comparisons for Geomagnetic Storms in 1998-2001

NASA Astrophysics Data System (ADS)

Baker, D. N.; Fisher, T. A.; Barth, C. A.; Mankoff, K. D.; Kanekal, S. G.; Bailey, S. M.; Petrinec, S. M.; Luhmann, J. G.; Mason, G. M.; Mazur, J. E.; Evans, D. S.

2002-05-01

Nitric oxide (NO) densities measured at altitudes between 97 and 150 km have been acquired using the UVS sensor onboard the Student Nitric Oxide Explorer (SNOE) spacecraft during the years 1998-2001. These data are compared with energetic electron fluxes (E>25 keV) measured concurrently using a sensitive sensor system (LICA) onboard the Solar, Anomalous, and Magnetospheric Particle Explorer (SAMPEX) spacecraft. Geomagnetic storm intervals are examined to determine altitude and latitude variations of NO density as it compares to energetic electron precipitation. A broader statistical analysis is then carried out using daily averages of peak NO densities (at 106 km altitudes) and electron intensities measured by SAMPEX/LICA and by the TED sensor system onboard the NOAA/Polar Orbiting Environmental Satellite (POES) spacecraft. We also use the PIXIE instrument onboard POLAR to obtain global views of 2-12 keV x-rays emanating from the upper atmosphere. This gives a broad synoptic measure of relatively low-energy electron precipitation into the atmosphere. Latitude versus time displays of the UVS, PIXIE, LICA and TED data show excellent temporal and spatial correlations of the data sets. More detailed comparisons help us to assess spectral and local time relationships between auroral particle inputs and lower thermospheric chemical responses. These results are potentially quite important since past modeling has shown that particle inputs are significant for changing the chemistry and subsequent dynamics of the atmosphere.

Two color interferometric electron density measurement in an axially blown arc

NASA Astrophysics Data System (ADS)

Stoller, Patrick; Carstensen, Jan; Galletti, Bernardo; Doiron, Charles; Sokolov, Alexey; Salzmann, René; Simon, Sandor; Jabs, Philipp

2016-09-01

High voltage circuit breakers protect the power grid by interrupting the current in case of a short circuit. To do so an arc is ignited between two contacts as they separate; transonic gas flow is used to cool and ultimately extinguish the arc at a current-zero crossing of the alternating current. A detailed understanding of the arc interruption process is needed to improve circuit breaker design. The conductivity of the partially ionized gas remaining after the current-zero crossing, a key parameter in determining whether the arc will be interrupted or not, is a function of the electron density. The electron density, in turn, is a function of the detailed dynamics of the arc cooling process, which does not necessarily occur under local thermodynamic equilibrium (LTE) conditions. In this work, we measure the spatially resolved line-integrated index of refraction in a near-current-zero arc stabilized in an axial flow of synthetic air with two nanosecond pulsed lasers at wavelengths of 532 nm and 671 nm. Generating a stable, cylindrically symmetric arc enables us to determine the three-dimensional index of refraction distribution using Abel inversion. Due to the wavelength dependence of the component of the index of refraction related to the free electrons, the information at two different wavelengths can be used to determine the electron density. This information allows us to determine how important it is to take into account non-equilibrium effects for accurate modeling of the physics of decaying arcs.

Real-time decay of a highly excited charge carrier in the one-dimensional Holstein model

NASA Astrophysics Data System (ADS)

Dorfner, F.; Vidmar, L.; Brockt, C.; Jeckelmann, E.; Heidrich-Meisner, F.

2015-03-01

We study the real-time dynamics of a highly excited charge carrier coupled to quantum phonons via a Holstein-type electron-phonon coupling. This is a prototypical example for the nonequilibrium dynamics in an interacting many-body system where excess energy is transferred from electronic to phononic degrees of freedom. We use diagonalization in a limited functional space (LFS) to study the nonequilibrium dynamics on a finite one-dimensional chain. This method agrees with exact diagonalization and the time-evolving block-decimation method, in both the relaxation regime and the long-time stationary state, and among these three methods it is the most efficient and versatile one for this problem. We perform a comprehensive analysis of the time evolution by calculating the electron, phonon and electron-phonon coupling energies, and the electronic momentum distribution function. The numerical results are compared to analytical solutions for short times, for a small hopping amplitude and for a weak electron-phonon coupling. In the latter case, the relaxation dynamics obtained from the Boltzmann equation agrees very well with the LFS data. We also study the time dependence of the eigenstates of the single-site reduced density matrix, which defines the so-called optimal phonon modes. We discuss their structure in nonequilibrium and the distribution of their weights. Our analysis shows that the structure of optimal phonon modes contains very useful information for the interpretation of the numerical data.

Electron transfer beyond the static picture: A TDDFT/TD-ZINDO study of a pentacene dimer

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

Reslan, Randa; Lopata, Kenneth; Arntsen, Christopher

2012-12-14

We use time-dependent density functional theory and time-dependent ZINDO (a semi-empirical method) to study transfer of an extra electron between a pair of pentacene molecules. A measure of the electronic transfer integral is computed in a dynamic picture via the vertical excitation energy from a delocalized anionic ground state. With increasing dimer separation, this dynamical measurement of charge transfer is shown to be significantly larger than the commonly used static approximation (i.e., LUMO+1–LUMO of the neutral dimer, or HOMO–LUMO of the charged dimer), up to an order of magnitude higher at 6 Å. These results offer a word of cautionmore » for calculations involving large separations, as in organic photovoltaics, where care must be taken when using a static picture to model charge transfer.« less

Electron transfer beyond the static picture: A TDDFT/TD-ZINDO study of a pentacene dimer

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

Reslan, Randa; Lopata, Kenneth A.; Arntsen, Christopher D.

2012-12-14

We use time-dependent density functional theory and time-dependent ZINDO (a semi-empirical method) to study transfer of an extra electron between a pair of pentacene dimers. A measure of the electronic transfer integral is computed in a dynamic picture via the vertical excitation energy from a delocalized anionic ground state. With increasing dimer separation, this dynamical measurement of charge transfer is shown to be significantly larger than the commonly used static approximation (i.e., LUMO+1 - LUMO of the neutral dimer, or HOMO - LUMO of the charged dimer), up to an order of magnitude higher at 6 Å. These results offermore » a word of caution for calculations involving large separations, as in organic photovoltaics, where care must be taken when using a static picture to model charge transfer.« less

Electron-Cloud Build-Up: Theory and Data

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

Furman, M. A.

We present a broad-brush survey of the phenomenology, history and importance of the electron-cloud effect (ECE). We briefly discuss the simulation techniques used to quantify the electron-cloud (EC) dynamics. Finally, we present in more detail an effective theory to describe the EC density build-up in terms of a few effective parameters. For further details, the reader is encouraged to refer to the proceedings of many prior workshops, either dedicated to EC or with significant EC contents, including the entire 'ECLOUD' series. In addition, the proceedings of the various flavors of Particle Accelerator Conferences contain a large number of EC-related publications.more » The ICFA Beam Dynamics Newsletter series contains one dedicated issue, and several occasional articles, on EC. An extensive reference database is the LHC website on EC.« less

The dynamic behavior of a liquid ethanol-water mixture: a perspective from quantum chemical topology.

PubMed

Mejía, Sol M; Mills, Matthew J L; Shaik, Majeed S; Mondragon, Fanor; Popelier, Paul L A

2011-05-07

Quantum Chemical Topology (QCT) is used to reveal the dynamics of atom-atom interactions in a liquid. A molecular dynamics simulation was carried out on an ethanol-water liquid mixture at its azeotropic concentration (X(ethanol)=0.899), using high-rank multipolar electrostatics. A thousand (ethanol)(9)-water heterodecamers, respecting the water-ethanol ratio of the azeotropic mixture, were extracted from the simulation. Ab initio electron densities were computed at the B3LYP/6-31+G(d) level for these molecular clusters. A video shows the dynamical behavior of a pattern of bond critical points and atomic interaction lines, fluctuating over 1 ns. A bond critical point distribution revealed the fluctuating behavior of water and ethanol molecules in terms of O-H···O, C-H···O and H···H interactions. Interestingly, the water molecule formed one to six C-H···O and one to four O-H···O interactions as a proton acceptor. We found that the more localized a dynamical bond critical point distribution, the higher the average electron density at its bond critical points. The formation of multiple C-H···O interactions affected the shape of the oxygen basin of the water molecule, which is shown in three dimensions. The hydrogen atoms of water strongly preferred to form H···H interactions with ethanol's alkyl hydrogen atoms over its hydroxyl hydrogen. This journal is © the Owner Societies 2011

Thomson scattering from a three-component plasma.

PubMed

Johnson, W R; Nilsen, J

2014-02-01

A model for a three-component plasma consisting of two distinct ionic species and electrons is developed and applied to study x-ray Thomson scattering. Ions of a specific type are assumed to be identical and are treated in the average-atom approximation. Given the plasma temperature and density, the model predicts mass densities, effective ionic charges, and cell volumes for each ionic type, together with the plasma chemical potential and free-electron density. Additionally, the average-atom treatment of individual ions provides a quantum-mechanical description of bound and continuum electrons. The model is used to obtain parameters needed to determine the dynamic structure factors for x-ray Thomson scattering from a three-component plasma. The contribution from inelastic scattering by free electrons is evaluated in the random-phase approximation. The contribution from inelastic scattering by bound electrons is evaluated using the bound-state and scattering wave functions obtained from the average-atom calculations. Finally, the partial static structure factors for elastic scattering by ions are evaluated using a two-component version of the Ornstein-Zernike equations with hypernetted chain closure, in which electron-ion interactions are accounted for using screened ion-ion interaction potentials. The model is used to predict the x-ray Thomson scattering spectrum from a CH plasma and the resulting spectrum is compared with experimental results obtained by Feltcher et al. [Phys. Plasmas 20, 056316 (2013)].

FAST TRACK COMMUNICATION A DFT + DMFT approach for nanosystems

NASA Astrophysics Data System (ADS)

Turkowski, Volodymyr; Kabir, Alamgir; Nayyar, Neha; Rahman, Talat S.

2010-11-01

We propose a combined density-functional-theory-dynamical-mean-field-theory (DFT + DMFT) approach for reliable inclusion of electron-electron correlation effects in nanosystems. Compared with the widely used DFT + U approach, this method has several advantages, the most important of which is that it takes into account dynamical correlation effects. The formalism is illustrated through different calculations of the magnetic properties of a set of small iron clusters (number of atoms 2 <= N <= 5). It is shown that the inclusion of dynamical effects leads to a reduction in the cluster magnetization (as compared to results from DFT + U) and that, even for such small clusters, the magnetization values agree well with experimental estimations. These results justify confidence in the ability of the method to accurately describe the magnetic properties of clusters of interest to nanoscience.

Dynamics of streamer-to-leader transition at reduced air densities and its implications for propagation of lightning leaders and gigantic jets

NASA Astrophysics Data System (ADS)

da Silva, Caitano L.; Pasko, Victor P.

2013-12-01

In this paper we present modeling studies of air heating by electrical discharges in a wide range of pressures. The developed model is capable of quantifying the different contributions for heating of air at the particle level and rigorously accounts for the vibration-dissociation-vibration coupling. The model is validated by calculating the breakdown times of short air gaps and comparing to available experimental data. Detailed discussion on the role of electron detachment in the development of the thermal-ionizational instability that triggers the spark development in short air gaps is presented. The dynamics of fast heating by quenching of excited electronic states is discussed and the scaling of its main channels with ambient air density is quantified. The developed model is employed to study the streamer-to-leader transition process and to obtain its scaling with ambient air density. Streamer-to-leader transition is the name given to a sequence of events occurring in a thin plasma channel through which a relatively strong current is forced through, culminating in heating of ambient gas and increase of the electrical conductivity of the channel. This process occurs during the inception of leaders (from sharp metallic structures, from hydrometeors inside the thundercloud, or in virgin air) and during their propagation (at the leader head or during the growth of a space leader). The development of a thermal-ionizational instability that culminates in the leader formation and propagation is characterized by a change in air ionization mechanism from electron impact to associative ionization and by contraction of the plasma channel. The introduced methodology for estimation of leader speeds shows that the propagation of a leader is limited by the air heating of every newly formed leader section. It is demonstrated that the streamer-to-leader transition time has an inverse-squared dependence on the ambient air density at near-ground pressures, in agreement with similarity laws for Joule heating in a streamer channel. Model results indicate that a deviation from this similarity scaling occurs at very low air densities, where the rate of electronic power deposition is balanced by the channel expansion, and air heating from quenching of excited electronic states is very inefficient. These findings place a limit on the maximum altitude at which a hot and highly conducting lightning leader channel can be formed in the Earth's atmosphere, result which is important for understating of the gigantic jet (GJ) discharges between thundercloud tops and the lower ionosphere. Simulations of leader speeds at GJ altitudes demonstrate that initial speeds of GJs are consistent with the leader propagation mechanism. The simulation of a GJ, escaping upward from a thundercloud top, shows that the lengthening of the leader streamer zone, in a medium of exponentially decreasing air density, determines the existence of an altitude at which the streamer zones of GJs become so long that they dynamically extend (jump) all the way to the ionosphere.

Observation of multi-channel non-local transport in J-TEXT plasmas

NASA Astrophysics Data System (ADS)

Shi, Yuejiang; Chen, Zhongyong; Yang, Zhoujun; Shi, Peng; Zhao, Kaijun; Diamond, Patrick H.; Kwon, JaeMin; Yan, Wei; Zhou, Hao; Pan, Xiaoming; Cheng, Zhifeng; Chen, Zhiping; Yang, SeongMoo; Zhang, Chi; Li, Da; Dong, Yunbo; Wang, Lu; Ding, YongHua; Liang, Yunfeng; Hahn, SangHee; Jhang, HoGun; Na, Yong-Su

2018-04-01

In cold pulse experiments in J-TEXT, not only are rapid electron temperature increases in the core observed, but also steep rises in the inner density are found. Moreover, some evidence of acceleration of the core toroidal rotation is also observed during the non-local transport process of electron temperature. These new findings of cold pulse experiments in J-TEXT suggest that turbulence spreading is a possible mechanism for the non-local transport dynamics.

Defects and anharmonicity induced electron spectra of YBa2Cu3O7-δ superconductors

NASA Astrophysics Data System (ADS)

Singh, Anu; Indu, B. D.

2018-05-01

The effects of defects and anharmonicities on the electron density of states (EDOS) have been studied in high-temperature superconductors (HTS) adopting the many body quantum dynamical theory of electron Green's functions via a generalized Hamiltonian that includes the effects of electron-phonon interactions, anharmonicities and point impurities. The automatic emergence of pairons and temperature dependence of EDOS are appear as special feature of the theory. The results thus obtained and their numerical analysis for YBa2Cu3O7-δ superconductors clearly demonstrate that the presence of defects, anharmonicities and electron-phonon interactions modifies the behavior of EDOS over a wide range of temperature.

Segregation formation, thermal and electronic properties of ternary cubic CdZnTe clusters: MD simulations and DFT calculations

NASA Astrophysics Data System (ADS)

Kurban, Mustafa; Erkoç, Şakir

2017-04-01

Surface and core formation, thermal and electronic properties of ternary cubic CdZnTe clusters are investigated by using classical molecular dynamics (MD) simulations and density functional theory (DFT) calculations. In this work, MD simulations of the CdZnTe clusters are performed by means of LAMMPS by using bond order potential (BOP). MD simulations are carried out at different temperatures to study the segregation phenomena of Cd, Zn and Te atoms, and deviation of clusters and heat capacity. After that, using optimized geometries obtained, excess charge on atoms, dipole moments, highest occupied molecular orbitals, lowest unoccupied molecular orbitals, HOMO-LUMO gaps (Eg) , total energies, spin density and the density of states (DOS) have been calculated with DFT. Simulation results such as heat capacity and segregation formation are compared with experimental bulk and theoretical results.

SUPRATHERMAL ELECTRONS IN TITAN’S SUNLIT IONOSPHERE: MODEL–OBSERVATION COMPARISONS

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

Vigren, E.; Edberg, N. J. T.; Wahlund, J.-E.

2016-08-01

The dayside ionosphere of the Saturnian satellite Titan is generated mainly from photoionization of N{sub 2} and CH{sub 4}. We compare model-derived suprathermal electron intensities with spectra measured by the Cassini Plasma Spectrometer/Electron Spectrometer (CAPS/ELS) in Titan's sunlit ionosphere (altitudes of 970–1250 km) focusing on the T40, T41, T42, and T48 Titan flybys by the Cassini spacecraft. The model accounts only for photoelectrons and associated secondary electrons, with a main input being the impinging solar EUV spectra as measured by the Thermosphere Ionosphere Mesosphere Energy and Dynamics/Solar EUV Experiment and extrapolated to Saturn. Associated electron-impact electron production rates have beenmore » derived from ambient number densities of N{sub 2} and CH{sub 4} (measured by the Ion Neutral Mass Spectrometer/Closed Source Neutral mode) and related energy-dependent electron-impact ionization cross sections. When integrating up to electron energies of 60 eV, covering the bulk of the photoelectrons, the model-based values exceed the observationally based values typically by factors of ∼3 ± 1. This finding is possibly related to current difficulties in accurately reproducing the observed electron number densities in Titan's dayside ionosphere. We compare the utilized dayside CAPS/ELS spectra with ones measured in Titan's nightside ionosphere during the T55–T59 flybys. The investigated nightside locations were associated with higher fluxes of high-energy (>100 eV) electrons than the dayside locations. As expected, for similar neutral number densities, electrons with energies <60 eV give a higher relative contribution to the total electron-impact ionization rates on the dayside (due to the contribution from photoelectrons) than on the nightside.« less

Longitudinal bunch shaping of picosecond high-charge MeV electron beams

DOE PAGES

Beaudoin, B. L.; Thangaraj, J. C. T.; Edstrom, Jr., D.; ...

2016-10-20

With ever increasing demands for intensities in modern accelerators, the understanding of space-charge effects becomes crucial. Herein are presented measurements of optically shaped picosecond-long electron beams in a superconducting L-band linac over a wide range of charges, from 0.2 nC to 3.4 nC. At low charges, the shape of the electron beam is preserved, while at higher charge densities, modulations on the beam convert to energy modulations. Here, energy profile measurements using a spectrometer and time profile measurements using a streak camera reveal the dynamics of longitudinal space-charge on MeV-scale electron beams.

Superconducting gap in cuprate high temperature superconductors

NASA Astrophysics Data System (ADS)

Verma, Sanjeev K.; Kumari, Anita; Gupta, Anushri; Indu, B. D.

2018-05-01

The many body quantum dynamical evaluation of double time thermodynamic electron Green's functions followed by generalized electron density of states (EDOS) is used to study the superconducting gap (SG). The dependence of EDOS on defects, anharmonicity and electron-phonon interactions makes the problem quite complicated and challenging but furnishes the more realistic grounds to study the SG both in conventional and high temperature superconductors (HTS). For simplicity, only electron-phonon interaction has been taken up to evaluate the intricate integral to enumerate the SG for representative cuprate HTS: YBa2Cu3O7-δ and results show 2Δ/kBTc ⋍ 7.2.

Classical Coset Hamiltonian for the Electronic Motion and its Application to Anderson Localization and Hammett Equation

NASA Astrophysics Data System (ADS)

Xing, Guan; Wu, Guo-Zhen

2001-02-01

A classical coset Hamiltonian is introduced for the system of one electron in multi-sites. By this Hamiltonian, the dynamical behaviour of the electronic motion can be readily simulated. The simulation reproduces the retardation of the electron density decay in a lattice with site energies randomly distributed - an analogy with Anderson localization. This algorithm is also applied to reproduce the Hammett equation which relates the reaction rate with the property of the substitutions in the organic chemical reactions. The advantages and shortcomings of this algorithm, as contrasted with traditional quantum methods such as the molecular orbital theory, are also discussed.

Dynamic evolutions of electron properties: A theoretical study for condensed-phase β-HMX under shock loading

NASA Astrophysics Data System (ADS)

He, Zheng-Hua; Chen, Jun; Wu, Qiang; Ji, Guang-Fu

2017-11-01

We present the density functional theory (DFT) calculations for microscopic electron properties of β-HMX under shock loading. The metallization pressure is determined to be within 30-55 GPa. The frontier molecular orbitals mainly localize on N-NO2 groups initially and disperse with pressure increase, while HOMO and LUMO orbitals trend to aggregate with each other. The deformation of N-NO2 groups and enhanced hydrogen-bonding interactions cause the electron delocalization and lower the band gap, inducing the reaction initiation finally. Our results show that using the electron properties can reliably predict the initial decomposition of energetic materials under shock loading.

Electron dynamics in complex environments with real-time time dependent density functional theory in a QM-MM framework

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

Morzan, Uriel N.; Ramírez, Francisco F.; Scherlis, Damián A., E-mail: damian@qi.fcen.uba.ar, E-mail: mcgl@qb.ffyb.uba.ar

2014-04-28

This article presents a time dependent density functional theory (TDDFT) implementation to propagate the Kohn-Sham equations in real time, including the effects of a molecular environment through a Quantum-Mechanics Molecular-Mechanics (QM-MM) hamiltonian. The code delivers an all-electron description employing Gaussian basis functions, and incorporates the Amber force-field in the QM-MM treatment. The most expensive parts of the computation, comprising the commutators between the hamiltonian and the density matrix—required to propagate the electron dynamics—, and the evaluation of the exchange-correlation energy, were migrated to the CUDA platform to run on graphics processing units, which remarkably accelerates the performance of the code.more » The method was validated by reproducing linear-response TDDFT results for the absorption spectra of several molecular species. Two different schemes were tested to propagate the quantum dynamics: (i) a leap-frog Verlet algorithm, and (ii) the Magnus expansion to first-order. These two approaches were confronted, to find that the Magnus scheme is more efficient by a factor of six in small molecules. Interestingly, the presence of iron was found to seriously limitate the length of the integration time step, due to the high frequencies associated with the core-electrons. This highlights the importance of pseudopotentials to alleviate the cost of the propagation of the inner states when heavy nuclei are present. Finally, the methodology was applied to investigate the shifts induced by the chemical environment on the most intense UV absorption bands of two model systems of general relevance: the formamide molecule in water solution, and the carboxy-heme group in Flavohemoglobin. In both cases, shifts of several nanometers are observed, consistently with the available experimental data.« less

Electron dynamics in complex environments with real-time time dependent density functional theory in a QM-MM framework

NASA Astrophysics Data System (ADS)

Morzan, Uriel N.; Ramírez, Francisco F.; Oviedo, M. Belén; Sánchez, Cristián G.; Scherlis, Damián A.; Lebrero, Mariano C. González

2014-04-01

This article presents a time dependent density functional theory (TDDFT) implementation to propagate the Kohn-Sham equations in real time, including the effects of a molecular environment through a Quantum-Mechanics Molecular-Mechanics (QM-MM) hamiltonian. The code delivers an all-electron description employing Gaussian basis functions, and incorporates the Amber force-field in the QM-MM treatment. The most expensive parts of the computation, comprising the commutators between the hamiltonian and the density matrix—required to propagate the electron dynamics—, and the evaluation of the exchange-correlation energy, were migrated to the CUDA platform to run on graphics processing units, which remarkably accelerates the performance of the code. The method was validated by reproducing linear-response TDDFT results for the absorption spectra of several molecular species. Two different schemes were tested to propagate the quantum dynamics: (i) a leap-frog Verlet algorithm, and (ii) the Magnus expansion to first-order. These two approaches were confronted, to find that the Magnus scheme is more efficient by a factor of six in small molecules. Interestingly, the presence of iron was found to seriously limitate the length of the integration time step, due to the high frequencies associated with the core-electrons. This highlights the importance of pseudopotentials to alleviate the cost of the propagation of the inner states when heavy nuclei are present. Finally, the methodology was applied to investigate the shifts induced by the chemical environment on the most intense UV absorption bands of two model systems of general relevance: the formamide molecule in water solution, and the carboxy-heme group in Flavohemoglobin. In both cases, shifts of several nanometers are observed, consistently with the available experimental data.

Real-Time Quantum Dynamics of Long-Range Electronic Excitation Transfer in Plasmonic Nanoantennas.

PubMed

Ilawe, Niranjan V; Oviedo, M Belén; Wong, Bryan M

2017-08-08

Using large-scale, real-time, quantum dynamics calculations, we present a detailed analysis of electronic excitation transfer (EET) mechanisms in a multiparticle plasmonic nanoantenna system. Specifically, we utilize real-time, time-dependent, density functional tight binding (RT-TDDFTB) to provide a quantum-mechanical description (at an electronic/atomistic level of detail) for characterizing and analyzing these systems, without recourse to classical approximations. We also demonstrate highly long-range electronic couplings in these complex systems and find that the range of these couplings is more than twice the conventional cutoff limit considered by Förster resonance energy transfer (FRET)-based approaches. Furthermore, we attribute these unusually long-ranged electronic couplings to the coherent oscillations of conduction electrons in plasmonic nanoparticles. This long-range nature of plasmonic interactions has important ramifications for EET; in particular, we show that the commonly used "nearest-neighbor" FRET model is inadequate for accurately characterizing EET even in simple plasmonic antenna systems. These findings provide a real-time, quantum-mechanical perspective for understanding EET mechanisms and provide guidance in enhancing plasmonic properties in artificial light-harvesting systems.

Highly parallel implementation of non-adiabatic Ehrenfest molecular dynamics

NASA Astrophysics Data System (ADS)

Kanai, Yosuke; Schleife, Andre; Draeger, Erik; Anisimov, Victor; Correa, Alfredo

2014-03-01

While the adiabatic Born-Oppenheimer approximation tremendously lowers computational effort, many questions in modern physics, chemistry, and materials science require an explicit description of coupled non-adiabatic electron-ion dynamics. Electronic stopping, i.e. the energy transfer of a fast projectile atom to the electronic system of the target material, is a notorious example. We recently implemented real-time time-dependent density functional theory based on the plane-wave pseudopotential formalism in the Qbox/qb@ll codes. We demonstrate that explicit integration using a fourth-order Runge-Kutta scheme is very suitable for modern highly parallelized supercomputers. Applying the new implementation to systems with hundreds of atoms and thousands of electrons, we achieved excellent performance and scalability on a large number of nodes both on the BlueGene based ``Sequoia'' system at LLNL as well as the Cray architecture of ``Blue Waters'' at NCSA. As an example, we discuss our work on computing the electronic stopping power of aluminum and gold for hydrogen projectiles, showing an excellent agreement with experiment. These first-principles calculations allow us to gain important insight into the the fundamental physics of electronic stopping.

Electrons as probes of dynamics in molecules and clusters: A contribution from Time Dependent Density Functional Theory

NASA Astrophysics Data System (ADS)

Wopperer, P.; Dinh, P. M.; Reinhard, P.-G.; Suraud, E.

2015-02-01

There are various ways to analyze the dynamical response of clusters and molecules to electromagnetic perturbations. Particularly rich information can be obtained from measuring the properties of electrons emitted in the course of the excitation dynamics. Such an analysis of electron signals covers observables such as total ionization, Photo-Electron Spectra (PES), Photoelectron Angular Distributions (PAD), and ideally combined PES/PAD. It has a long history in molecular physics and was increasingly used in cluster physics as well. Recent progress in the design of new light sources (high intensity, high frequency, ultra short pulses) opens new possibilities for measurements and thus has renewed the interest on these observables, especially for the analysis of various dynamical scenarios, well beyond a simple access to electronic density of states. This, in turn, has motivated many theoretical investigations of the dynamics of electronic emission for molecules and clusters up to such a complex and interesting system as C60. A theoretical tool of choice is here Time-Dependent Density Functional Theory (TDDFT) propagated in real time and on a spatial grid, and augmented by a Self-Interaction Correction (SIC). This provides a pertinent, robust, and efficient description of electronic emission including the detailed pattern of PES and PAD. A direct comparison between experiments and well founded elaborate microscopic theories is thus readily possible, at variance with more demanding observables such as for example fragmentation or dissociation cross sections. The purpose of this paper is to describe the theoretical tools developed on the basis of real-time and real-space TDDFT and to address in a realistic manner the analysis of electronic emission following irradiation of clusters and molecules by various laser pulses. After a general introduction, we shall present in a second part the available experimental results motivating such studies, starting from the simplest total ionization signals to the more elaborate PES and PAD, possibly combining them and/or resolving them in time. This experimental discussion will be complemented in a third part by a presentation of available theoretical tools focusing on TDDFT and detailing the methods used to address ionization observables. We shall also discuss the shortcomings of standard versions of TDDFT, especially what concerns the SIC problem, and show how to improve formally and practically the theory on that aspect. A long fourth part will be devoted to representative results. We shall illustrate the use of total ionization in pump and probe scenarios with fs lasers for tracking ionic dynamics in clusters. More challenging from the experimental point of view is pump and probe setups using attosecond pulses. The effort there is more on the capability to define proper signals to be measured/computed at such a short time scale. TDDFT analysis provides here a valuable tool in the search for the most efficient observables. PES and PAD will allow one to address more directly electronic dynamics itself by means of fs or ns laser pulses. We shall in particular discuss the impact of the dynamical regime in PES and PAD. We shall end this fourth part by addressing the role of temperature in PES and PAD. When possible, the results will be directly compared to experiments. The fifth part of the paper will be devoted to future directions of investigations. From the rich choice of developments, we shall in particular address two aspects. We shall start to discuss the information content of energy/angular spectra of emitted electrons in case of excitation by swift and highly charged ions rather than lasers. The second issue concerns the account of dissipative effects in TDDFT to be able to consider longer laser pulses where the competition between direct electron emission and thermalization is known to play a role as, e.g., in experiments with C60. Although such questions have been superficially addressed in the simple case of alkaline clusters by means of semi-classical methods, no satisfying quantum formulation, compulsory for most realistic systems, is yet available. First encouraging results will be presented on that occasion. We shall finally give a short conclusion.

Spin-polarization dependent carrier recombination dynamics and spin relaxation mechanism in asymmetrically doped (110) n-GaAs quantum wells

NASA Astrophysics Data System (ADS)

Teng, Lihua; Jiang, Tianran; Wang, Xia; Lai, Tianshu

2018-05-01

Carrier recombination and electron spin relaxation dynamics in asymmetric n-doped (110) GaAs/AlGaAs quantum wells are investigated with time-resolved pump-probe spectroscopy. The experiment results reveal that the measured carrier recombination time depends strongly on the polarization of pump pulse. With the same pump photon flux densities, the recombination time of spin-polarized carriers is always longer than that of the spin-balanced carriers except at low pump photon flux densities, this anomaly originates from the polarization-sensitive nonlinear absorption effect. Differing from the traditional views, in the low carrier density regime, the D'yakonov-Perel' (DP) mechanism can be more important than the Bir-Aronov-Pikus (BAP) mechanism, since the DP mechanism takes effect, the spin relaxation time in (110) GaAs QWs is shortened obviously via asymmetric doping.

Ultrafast semi-metallic layer formation in detonating nitromethane

NASA Astrophysics Data System (ADS)

Reed, Evan; Manaa, M. Riad; Fried, Laurence; Glaesemann, Kurt; Joannopoulos, John

2008-03-01

We present the first quantum molecular dynamics simulations behind a detonation front (up to 0.2 ns) of the explosive nitromethane (CH3NO2) represented by the density-functional-based tight-binding method (DFTB). This simulation is enabled by our recently developed multi-scale shock wave molecular dynamics technique (MSST) that opens the door to longer duration simulations by several orders of magnitude. The electronic density of states around the Fermi energy initially increases as metastable material states are produced but then later decreases, perhaps unexpectedly. These changes indicate that the shock front is characterized by an increase in optical thickness and conductivity followed by a reduction around 100 picoseconds behind the front. We find that a significant population of intermediate metastable molecules are charged and charged species play an important role in the density of states evolution. The transient transformation to a semi-metallic state can be understood within the Anderson picture of metallization.

Tracking of an electron beam through the solar corona with LOFAR

NASA Astrophysics Data System (ADS)

Mann, G.; Breitling, F.; Vocks, C.; Aurass, H.; Steinmetz, M.; Strassmeier, K. G.; Bisi, M. M.; Fallows, R. A.; Gallagher, P.; Kerdraon, A.; Mackinnon, A.; Magdalenic, J.; Rucker, H.; Anderson, J.; Asgekar, A.; Avruch, I. M.; Bell, M. E.; Bentum, M. J.; Bernardi, G.; Best, P.; Bîrzan, L.; Bonafede, A.; Broderick, J. W.; Brüggen, M.; Butcher, H. R.; Ciardi, B.; Corstanje, A.; Gasperin, F. de; Geus, E. de; Deller, A.; Duscha, S.; Eislöffel, J.; Engels, D.; Falcke, H.; Fender, R.; Ferrari, C.; Frieswijk, W.; Garrett, M. A.; Grießmeier, J.; Gunst, A. W.; van Haarlem, M.; Hassall, T. E.; Heald, G.; Hessels, J. W. T.; Hoeft, M.; Hörandel, J.; Horneffer, A.; Juette, E.; Karastergiou, A.; Klijn, W. F. A.; Kondratiev, V. I.; Kramer, M.; Kuniyoshi, M.; Kuper, G.; Maat, P.; Markoff, S.; McFadden, R.; McKay-Bukowski, D.; McKean, J. P.; Mulcahy, D. D.; Munk, H.; Nelles, A.; Norden, M. J.; Orru, E.; Paas, H.; Pandey-Pommier, M.; Pandey, V. N.; Pizzo, R.; Polatidis, A. G.; Rafferty, D.; Reich, W.; Röttgering, H.; Scaife, A. M. M.; Schwarz, D. J.; Serylak, M.; Sluman, J.; Smirnov, O.; Stappers, B. W.; Tagger, M.; Tang, Y.; Tasse, C.; ter Veen, S.; Thoudam, S.; Toribio, M. C.; Vermeulen, R.; van Weeren, R. J.; Wise, M. W.; Wucknitz, O.; Yatawatta, S.; Zarka, P.; Zensus, J. A.

2018-03-01

The Sun's activity leads to bursts of radio emission, among other phenomena. An example is type-III radio bursts. They occur frequently and appear as short-lived structures rapidly drifting from high to low frequencies in dynamic radio spectra. They are usually interpreted as signatures of beams of energetic electrons propagating along coronal magnetic field lines. Here we present novel interferometric LOFAR (LOw Frequency ARray) observations of three solar type-III radio bursts and their reverse bursts with high spectral, spatial, and temporal resolution. They are consistent with a propagation of the radio sources along the coronal magnetic field lines with nonuniform speed. Hence, the type-III radio bursts cannot be generated by a monoenergetic electron beam, but by an ensemble of energetic electrons with a spread distribution in velocity and energy. Additionally, the density profile along the propagation path is derived in the corona. It agrees well with three-fold coronal density model by (1961, ApJ, 133, 983).

Characterization of swift heavy ion irradiation damage in ceria

DOE PAGES

Yablinsky, Clarissa A.; Devanathan, Ram; Pakarinen, Janne; ...

2015-03-04

Swift heavy ion induced radiation damage is investigated for ceria (CeO 2), which serves as a UO 2 fuel surrogate. Microstructural changes resulting from an irradiation with 940 MeV gold ions of 42 keV/nm electronic energy loss are investigated by means of electron microscopy accompanied by electron energy loss spectroscopy showing that there exists a small density reduction in the ion track core. While chemical changes in the ion track are not precluded, evidence of them was not observed. Classical molecular dynamics simulations of thermal spikes in CeO 2 with an energy deposition of 12 and 36 keV/nm show damagemore » consisting of isolated point defects at 12 keV/nm, and defect clusters at 36 keV/nm, with no amorphization at either energy. Furthermore, inferences are drawn from modeling about density changes in the ion track and the formation of interstitial loops that shed light on features observed by electron microscopy of swift heavy ion irradiated ceria.« less

Carrier thermalization dynamics in single zincblende and wurtzite InP Nanowires.

PubMed

Wang, Yuda; Jackson, Howard E; Smith, Leigh M; Burgess, Tim; Paiman, Suriati; Gao, Qiang; Tan, Hark Hoe; Jagadish, Chennupati

2014-12-10

Using transient Rayleigh scattering (TRS) measurements, we obtain photoexcited carrier thermalization dynamics for both zincblende (ZB) and wurtzite (WZ) InP single nanowires (NW) with picosecond resolution. A phenomenological fitting model based on direct band-to-band transition theory is developed to extract the electron-hole-plasma density and temperature as a function of time from TRS measurements of single nanowires, which have complex valence band structures. We find that the thermalization dynamics of hot carriers depends strongly on material (GaAs NW vs InP NW) and less strongly on crystal structure (ZB vs WZ). The thermalization dynamics of ZB and WZ InP NWs are similar. But a comparison of the thermalization dynamics in ZB and WZ InP NWs with ZB GaAs NWs reveals more than an order of magnitude slower relaxation for the InP NWs. We interpret these results as reflecting their distinctive phonon band structures that lead to different hot phonon effects. Knowledge of hot carrier thermalization dynamics is an essential component for effective incorporation of nanowire materials into electronic devices.

Time-resolved cathodoluminescence microscopy with sub-nanosecond beam blanking for direct evaluation of the local density of states.

PubMed

Moerland, Robert J; Weppelman, I Gerward C; Garming, Mathijs W H; Kruit, Pieter; Hoogenboom, Jacob P

2016-10-17

We show cathodoluminescence-based time-resolved electron beam spectroscopy in order to directly probe the spontaneous emission decay rate that is modified by the local density of states in a nanoscale environment. In contrast to dedicated laser-triggered electron-microscopy setups, we use commercial hardware in a standard SEM, which allows us to easily switch from pulsed to continuous operation of the SEM. Electron pulses of 80-90 ps duration are generated by conjugate blanking of a high-brightness electron beam, which allows probing emitters within a large range of decay rates. Moreover, we simultaneously attain a resolution better than λ/10, which ensures details at deep-subwavelength scales can be retrieved. As a proof-of-principle, we employ the pulsed electron beam to spatially measure excited-state lifetime modifications in a phosphor material across the edge of an aluminum half-plane, coated on top of the phosphor. The measured emission dynamics can be directly related to the structure of the sample by recording photon arrival histograms together with the secondary-electron signal. Our results show that time-resolved electron cathodoluminescence spectroscopy is a powerful tool of choice for nanophotonics, within reach of a large audience.

Multiple ion species fluid modeling of sprite halos and the role of electron detachment from O- in their dynamics

NASA Astrophysics Data System (ADS)

Liu, N.

2011-12-01

Sprite halos are brief descending glows appearing at the lower ionosphere boundary, which follow impulsive cloud-to-ground lightning discharges [e.g., Barrington-Leigh et al., JGR, 106, 1741, 2001, Wescott et al., JGR, 106, 10467, 2001; Pasko, JGR, 115, A00E35, 2010]. They last for a few milliseconds, with horizontal extension of tens of kilometers and vertical thickness of several kilometers. According to global survey of the occurrence of transient luminous events by the ISUAL instruments on the FORMOSAT-2 satellite, on average sprite halos occur once every minute on Earth [Chen et al., JGR, 113, A08306, 2008]. It has been established that sprite halos are caused by electron heating, and molecule excitation and ionization in the lower ionosphere due to lightning quasi-electrostatic field [e.g., Pasko et al., JGR, 102, 4529, 1997; Barrington-Leigh et al., 2001; Pasko, 2010]. Past modeling work on sprite halos was conducted using either a two dimensional (2D) model of at most three charged species or a zero dimensional model of multiple ion species. In this talk, we report a modeling study of sprite halos using a recently developed 2D fluid model of multiple charged species. The model charged species include the ion species set used in [Lehtinen and Inan, GRL, 34, L08804, 2007] to study the dynamics of ionization perturbations produced by gigantic jets in the middle and upper atmosphere. In addition, another charged species, O-, is added to this set, because electron detachment of O- can proceed very fast under moderate electric field [Rayment and Moruzzi, Int. J. Mass Spectrom., 26, 321, 1978], requiring a separate treatment from the other light negative ions. The modeling results of a sprite halo driven by positive cloud-to-ground lightning indicate that the halo can descend to lower altitude with much higher electron density behind its front when the O- detachment process is included. Electron density ahead of the halo front is not significantly reduced from the ambient value, so that there is no attachment "hole" forming in that region that is commonly observed in previous modeling work. According to recent work by Qin et al. [JGR, 116, A06305, 2011], electron density must be around 10^3 1/m^3 or less at sprite initiation altitude in order for individual streamers to form. This requires the ambient electron density at the sprite initiation altitude to be close to 10^3 1/m^3 from our results, because electron density is not greatly decreased below the halo front. In addition, the large downward extent of the halo shown by our results may offer an explanation for the initiation of sprite streamers at 65-70 km altitude observed previously.

Fundamental mechanisms of laser damage of dielectric crystals by ultrashort pulse: ionization dynamics for the Keldysh model

NASA Astrophysics Data System (ADS)

Gruzdev, Vitaly

2014-12-01

Laser-induced ionization is a major process that initiates and drives the initial stages of laser-induced damage (LID) of high-quality transparent solids. The ionization and its contribution to LID are characterized in terms of the time-dependent ionization rate and conduction-band electron density. Considering femtosecond pulses of various durations (from 35 to 706 fs) and variable peak irradiances (from 0.01 to 60 TW/cm2), we use a single-rate equation to simulate time variations of conduction-band electron density and rates of the photoionization and impact ionization. The photoionization rate is evaluated with the Keldysh equation. At low irradiance, the electron density and total ionization rate demonstrate power scaling characteristic of multiphoton ionization. With the increase of irradiance, there is observed a saturation of the photoionization rate due to photoionization suppression by the Keldysh-type singularity during the increase in the number of simultaneously absorbed photons by 1. A striking result is that the saturation is followed by a stepwise transition from the ionization regime which is completely dominated by the photoionization to a regime totally dominated by the impact ionization. The transition results in the increase of the electron density by a few orders of magnitude induced by a variation of peak laser irradiance by about 15% to 20%. The physical effects that are involved are discussed.

Kinetic model for the collisionless sheath of a collisional plasma

DOE PAGES

Tang, Xian-Zhu; Guo, Zehua

2016-08-04

Collisional plasmas typically have mean-free-path still much greater than the Debye length, so the sheath is mostly collisionless. Once the plasma density, temperature, and flow are specified at the sheath entrance, the profile variation of electron and ion density, temperature, flow speed, and conductive heat fluxes inside the sheath is set by collisionless dynamics, and can be predicted by an analytical kinetic model distribution. Finally, these predictions are contrasted in this paper with direct kinetic simulations, showing good agreement.

Advanced Packaging Materials and Techniques for High Power TR Module: Standard Flight vs. Advanced Packaging

NASA Technical Reports Server (NTRS)

Hoffman, James Patrick; Del Castillo, Linda; Miller, Jennifer; Jenabi, Masud; Hunter, Donald; Birur, Gajanana

2011-01-01

The higher output power densities required of modern radar architectures, such as the proposed DESDynI [Deformation, Ecosystem Structure, and Dynamics of Ice] SAR [Synthetic Aperture Radar] Instrument (or DSI) require increasingly dense high power electronics. To enable these higher power densities, while maintaining or even improving hardware reliability, requires advances in integrating advanced thermal packaging technologies into radar transmit/receive (TR) modules. New materials and techniques have been studied and compared to standard technologies.

Canonical angular momentum compression near the Brillouin limit

NASA Astrophysics Data System (ADS)

Jeong, E.; Gilson, E.; Fajans, J.

2000-10-01

Near the Brillouin limit, the angular momentum of a trapped, T=0, pure-electron plasma approaches zero. If the plasma expands axially, its density would appear to drop. However, the plasma's canonical angular momentum is not changed by an axial expansion, so the plasma must stay near the Brillouin limit; thus the plasma's density cannot change when it is expanded. The only way for the plasma density to remain constant as the plasma length increases is for the plasma radius to decrease. Dynamically, this decrease is caused by the polarization drift induced by a small decrease in the density. In this poster we present preliminary experimental evidence demonstrating this radial compression. This work was supported by the ONR.

Magnetic Fluctuations in Pair-Density-Wave Superconductors

NASA Astrophysics Data System (ADS)

Christensen, Morten H.; Jacobsen, Henrik; Maier, Thomas A.; Andersen, Brian M.

2016-04-01

Pair-density-wave superconductivity constitutes a novel electronic condensate proposed to be realized in certain unconventional superconductors. Establishing its potential existence is important for our fundamental understanding of superconductivity in correlated materials. Here we compute the dynamical magnetic susceptibility in the presence of a pair-density-wave ordered state and study its fingerprints on the spin-wave spectrum including the neutron resonance. In contrast to the standard case of d -wave superconductivity, we show that the pair-density-wave phase exhibits neither a spin gap nor a magnetic resonance peak, in agreement with a recent neutron scattering experiment on underdoped La1.905 Ba0.095 CuO4 [Z. Xu et al., Phys. Rev. Lett. 113, 177002 (2014)].

Revealing electronic open quantum systems with subsystem TDDFT

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

Krishtal, Alisa, E-mail: alisa.krishtal@rutgers.edu; Pavanello, Michele, E-mail: m.pavanello@rutgers.edu

2016-03-28

Open quantum systems (OQSs) are perhaps the most realistic systems one can approach through simulations. In recent years, describing OQSs with Density Functional Theory (DFT) has been a prominent avenue of research with most approaches based on a density matrix partitioning in conjunction with an ad-hoc description of system-bath interactions. We propose a different theoretical approach to OQSs based on partitioning of the electron density. Employing the machinery of subsystem DFT (and its time-dependent extension), we provide a novel way of isolating and analyzing the various terms contributing to the coupling between the system and the surrounding bath. To illustratemore » the theory, we provide numerical simulations on a toy system (a molecular dimer) and on a condensed phase system (solvated excimer). The simulations show that non-Markovian dynamics in the electronic system-bath interactions are important in chemical applications. For instance, we show that the superexchange mechanism of transport in donor-bridge-acceptor systems is a non-Markovian interaction between the donor-acceptor (OQS) with the bridge (bath) which is fully characterized by real-time subsystem time-dependent DFT.« less

Revealing electronic open quantum systems with subsystem TDDFT.

PubMed

Krishtal, Alisa; Pavanello, Michele

2016-03-28

Open quantum systems (OQSs) are perhaps the most realistic systems one can approach through simulations. In recent years, describing OQSs with Density Functional Theory (DFT) has been a prominent avenue of research with most approaches based on a density matrix partitioning in conjunction with an ad-hoc description of system-bath interactions. We propose a different theoretical approach to OQSs based on partitioning of the electron density. Employing the machinery of subsystem DFT (and its time-dependent extension), we provide a novel way of isolating and analyzing the various terms contributing to the coupling between the system and the surrounding bath. To illustrate the theory, we provide numerical simulations on a toy system (a molecular dimer) and on a condensed phase system (solvated excimer). The simulations show that non-Markovian dynamics in the electronic system-bath interactions are important in chemical applications. For instance, we show that the superexchange mechanism of transport in donor-bridge-acceptor systems is a non-Markovian interaction between the donor-acceptor (OQS) with the bridge (bath) which is fully characterized by real-time subsystem time-dependent DFT.

Revealing electronic open quantum systems with subsystem TDDFT

NASA Astrophysics Data System (ADS)

Krishtal, Alisa; Pavanello, Michele

2016-03-01

Open quantum systems (OQSs) are perhaps the most realistic systems one can approach through simulations. In recent years, describing OQSs with Density Functional Theory (DFT) has been a prominent avenue of research with most approaches based on a density matrix partitioning in conjunction with an ad-hoc description of system-bath interactions. We propose a different theoretical approach to OQSs based on partitioning of the electron density. Employing the machinery of subsystem DFT (and its time-dependent extension), we provide a novel way of isolating and analyzing the various terms contributing to the coupling between the system and the surrounding bath. To illustrate the theory, we provide numerical simulations on a toy system (a molecular dimer) and on a condensed phase system (solvated excimer). The simulations show that non-Markovian dynamics in the electronic system-bath interactions are important in chemical applications. For instance, we show that the superexchange mechanism of transport in donor-bridge-acceptor systems is a non-Markovian interaction between the donor-acceptor (OQS) with the bridge (bath) which is fully characterized by real-time subsystem time-dependent DFT.

Automatic Whistler Detector and Analyzer system: Implementation of the analyzer algorithm

NASA Astrophysics Data System (ADS)

Lichtenberger, JáNos; Ferencz, Csaba; Hamar, Daniel; Steinbach, Peter; Rodger, Craig J.; Clilverd, Mark A.; Collier, Andrew B.

2010-12-01

The full potential of whistlers for monitoring plasmaspheric electron density variations has not yet been realized. The primary reason is the vast human effort required for the analysis of whistler traces. Recently, the first part of a complete whistler analysis procedure was successfully automated, i.e., the automatic detection of whistler traces from the raw broadband VLF signal was achieved. This study describes a new algorithm developed to determine plasmaspheric electron density measurements from whistler traces, based on a Virtual (Whistler) Trace Transformation, using a 2-D fast Fourier transform transformation. This algorithm can be automated and can thus form the final step to complete an Automatic Whistler Detector and Analyzer (AWDA) system. In this second AWDA paper, the practical implementation of the Automatic Whistler Analyzer (AWA) algorithm is discussed and a feasible solution is presented. The practical implementation of the algorithm is able to track the variations of plasmasphere in quasi real time on a PC cluster with 100 CPU cores. The electron densities obtained by the AWA method can be used in investigations such as plasmasphere dynamics, ionosphere-plasmasphere coupling, or in space weather models.

Computational predictions of the new Gallium nitride nanoporous structures

NASA Astrophysics Data System (ADS)

Lien, Le Thi Hong; Tuoc, Vu Ngoc; Duong, Do Thi; Thu Huyen, Nguyen

2018-05-01

Nanoporous structural prediction is emerging area of research because of their advantages for a wide range of materials science and technology applications in opto-electronics, environment, sensors, shape-selective and bio-catalysis, to name just a few. We propose a computationally and technically feasible approach for predicting Gallium nitride nanoporous structures with hollows at the nano scale. The designed porous structures are studied with computations using the density functional tight binding (DFTB) and conventional density functional theory methods, revealing a variety of promising mechanical and electronic properties, which can potentially find future realistic applications. Their stability is discussed by means of the free energy computed within the lattice-dynamics approach. Our calculations also indicate that all the reported hollow structures are wide band gap semiconductors in the same fashion with their parent’s bulk stable phase. The electronic band structures of these nanoporous structures are finally examined in detail.

Investigation of thermodynamic equilibrium in laser-induced aluminum plasma using the H{sub α} line profiles and Thomson scattering spectra

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

Cvejić, M., E-mail: marko.cvejic@ipb.ac.rs, E-mail: krzysztof.dzierzega@uj.edu.pl; Faculty of Physics, Weizmann Institute of Science, Rehovot 7610001; Dzierżęga, K., E-mail: marko.cvejic@ipb.ac.rs, E-mail: krzysztof.dzierzega@uj.edu.pl

2015-07-13

We have studied isothermal equilibrium in the laser-induced plasma from aluminum pellets in argon at pressure of 200 mbar by using a method which combines the standard laser Thomson scattering and analysis of the H{sub α}, Stark-broadened, line profiles. Plasma was created using 4.5 ns, 4 mJ pulses from a Nd:YAG laser at 1064 nm. While electron density and temperature were determined from the electron feature of Thomson scattering spectra, the heavy particle temperature was obtained from the H{sub α} full profile applying computer simulation including ion-dynamical effects. We have found strong imbalance between these two temperatures during entire plasma evolution whichmore » indicates its non-isothermal character. At the same time, according to the McWhirter criterion, the electron density was high enough to establish plasma in local thermodynamic equilibrium.« less

{bold {ital Ab initio}} studies of the structural and electronic properties of solid cubane

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

Richardson, S.L.; Martins, J.L.

1998-12-01

In this paper, we report {ital ab initio} calculation of the structural and electronic properties of solid cubane (s-C{sub 8}H{sub 8}) in the local-density approximation. By using an {ital ab initio} constant pressure extended molecular dynamics method with variable cell shape proposed by Wentzcovitch, Martins, and Price, we compute a lattice parameter {ital a} and a bond angle {alpha} for the rhombohedral Bravais lattice and compare it with experimental x-ray data. We obtain bond lengths for the mononuclear C{sub 8}H{sub 8} unit of basis atoms, as well as a density of states and heat of formation. {copyright} {ital 1998} {italmore » The American Physical Society}« less

Hydrodynamic model for conductivity in graphene.

PubMed

Mendoza, M; Herrmann, H J; Succi, S

2013-01-01

Based on the recently developed picture of an electronic ideal relativistic fluid at the Dirac point, we present an analytical model for the conductivity in graphene that is able to describe the linear dependence on the carrier density and the existence of a minimum conductivity. The model treats impurities as submerged rigid obstacles, forming a disordered medium through which graphene electrons flow, in close analogy with classical fluid dynamics. To describe the minimum conductivity, we take into account the additional carrier density induced by the impurities in the sample. The model, which predicts the conductivity as a function of the impurity fraction of the sample, is supported by extensive simulations for different values of ε, the dimensionless strength of the electric field, and provides excellent agreement with experimental data.

Charge Separation and Triplet Exciton Formation Pathways in Small-Molecule Solar Cells as Studied by Time-Resolved EPR Spectroscopy

DOE PAGES

Thomson, Stuart A. J.; Niklas, Jens; Mardis, Kristy L.; ...

2017-09-13

Organic solar cells are a promising renewable energy technology, offering the advantages of mechanical flexibility and solution processability. An understanding of the electronic excited states and charge separation pathways in these systems is crucial if efficiencies are to be further improved. Here we use light induced electron paramagnetic resonance (LEPR) spectroscopy and density functional theory calculations (DFT) to study the electronic excited states, charge transfer (CT) dynamics and triplet exciton formation pathways in blends of the small molecule donors (DTS(FBTTh 2) 2, DTS(F2BTTh 2) 2, DTS(PTTh 2) 2, DTG(FBTTh 2) 2 and DTG(F2BTTh 2) 2) with the fullerene derivative PCmore » 61BM. Using high frequency EPR the g-tensor of the positive polaron on the donor molecules was determined. The experimental results are compared with DFT calculations which reveal that the spin density of the polaron is distributed over a dimer or trimer. Time-resolved EPR (TR-EPR) spectra attributed to singlet CT states were identified and the polarization patterns revealed similar charge separation dynamics in the four fluorobenzothiadiazole donors, while charge separation in the DTS(PTTh 2) 2 blend is slower. Using TR-EPR we also investigated the triplet exciton formation pathways in the blend. The polarization patterns reveal that the excitons originate from both intersystem crossing (ISC) and back electron transfer (BET) processes. The DTS(PTTh 2) 2 blend was found to contain substantially more triplet excitons formed by BET than the fluorobenzothiadiazole blends. As a result, the higher BET triplet exciton population in the DTS(PTTh 2) 2 blend is in accordance with the slower charge separation dynamics observed in this blend.« less

Investigation of the spectral properties and magnetism of BiFeO3 by dynamical mean-field theory

NASA Astrophysics Data System (ADS)

Paul, Souvik; Iuşan, Diana; Thunström, Patrik; Kvashnin, Yaroslav O.; Hellsvik, Johan; Pereiro, Manuel; Delin, Anna; Knut, Ronny; Phuyal, Dibya; Lindblad, Andreas; Karis, Olof; Sanyal, Biplab; Eriksson, Olle

2018-03-01

Using the local density approximation plus dynamical mean-field theory (LDA+DMFT), we have computed the valence-band photoelectron spectra and magnetic excitation spectra of BiFeO3, one of the most studied multiferroics. Within the DMFT approach, the local impurity problem is tackled by the exact diagonalization solver. The solution of the impurity problem within the LDA+DMFT method for the paramagnetic and magnetically ordered phases produces result in agreement with the experimental data on electronic and magnetic structures. For comparison, we also present results obtained by the LDA +U approach which is commonly used to compute the physical properties of this compound. Our LDA+DMFT derived electronic spectra match adequately with the experimental hard x-ray photoelectron spectroscopy and resonant photoelectron spectroscopy for Fe 3 d states, whereas the LDA +U method fails to capture the general features of the measured spectra. This indicates the importance of accurately incorporating the dynamical aspect of electronic correlation among Fe 3 d orbitals to reproduce the experimental excitation spectra. Specifically, the LDA+DMFT derived density of states exhibits a significant amount of Fe 3 d states at the position of Bi lone pairs, implying that the latter are not alone in the spectral scenario. This fact might modify our interpretation about the origin of ferroelectric polarization in this material. Our study demonstrates that the combination of orbital cross sections for the constituent elements and broadening schemes for the spectral functions are crucial to explain the detailed structures of the experimental electronic spectra. Our magnetic excitation spectra computed from the LDA+DMFT result conform well with the inelastic neutron scattering data.

Charge Separation and Triplet Exciton Formation Pathways in Small Molecule Solar Cells as Studied by Time-resolved EPR Spectroscopy.

PubMed

Thomson, Stuart A J; Niklas, Jens; Mardis, Kristy L; Mallares, Christopher; Samuel, Ifor D W; Poluektov, Oleg G

2017-10-19

Organic solar cells are a promising renewable energy technology, offering the advantages of mechanical flexibility and solution processability. An understanding of the electronic excited states and charge separation pathways in these systems is crucial if efficiencies are to be further improved. Here we use light induced electron paramagnetic resonance (LEPR) spectroscopy and density functional theory calculations (DFT) to study the electronic excited states, charge transfer (CT) dynamics and triplet exciton formation pathways in blends of the small molecule donors (DTS(FBTTh 2 ) 2 , DTS(F 2 BTTh 2 ) 2 , DTS(PTTh 2 ) 2 , DTG(FBTTh 2 ) 2 and DTG(F 2 BTTh 2 ) 2 ) with the fullerene derivative PC 61 BM. Using high frequency EPR the g-tensor of the positive polaron on the donor molecules was determined. The experimental results are compared with DFT calculations which reveal that the spin density of the polaron is distributed over a dimer or trimer. Time-resolved EPR (TR-EPR) spectra attributed to singlet CT states were identified and the polarization patterns revealed similar charge separation dynamics in the four fluorobenzothiadiazole donors, while charge separation in the DTS(PTTh 2 ) 2 blend is slower. Using TR-EPR we also investigated the triplet exciton formation pathways in the blend. The polarization patterns reveal that the excitons originate from both intersystem crossing (ISC) and back electron transfer (BET) processes. The DTS(PTTh 2 ) 2 blend was found to contain substantially more triplet excitons formed by BET than the fluorobenzothiadiazole blends. The higher BET triplet exciton population in the DTS(PTTh 2 ) 2 blend is in accordance with the slower charge separation dynamics observed in this blend.

Charge Separation and Triplet Exciton Formation Pathways in Small-Molecule Solar Cells as Studied by Time-Resolved EPR Spectroscopy

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

Thomson, Stuart A. J.; Niklas, Jens; Mardis, Kristy L.

Organic solar cells are a promising renewable energy technology, offering the advantages of mechanical flexibility and solution processability. An understanding of the electronic excited states and charge separation pathways in these systems is crucial if efficiencies are to be further improved. Here we use light induced electron paramagnetic resonance (LEPR) spectroscopy and density functional theory calculations (DFT) to study the electronic excited states, charge transfer (CT) dynamics and triplet exciton formation pathways in blends of the small molecule donors (DTS(FBTTh 2) 2, DTS(F2BTTh 2) 2, DTS(PTTh 2) 2, DTG(FBTTh 2) 2 and DTG(F2BTTh 2) 2) with the fullerene derivative PCmore » 61BM. Using high frequency EPR the g-tensor of the positive polaron on the donor molecules was determined. The experimental results are compared with DFT calculations which reveal that the spin density of the polaron is distributed over a dimer or trimer. Time-resolved EPR (TR-EPR) spectra attributed to singlet CT states were identified and the polarization patterns revealed similar charge separation dynamics in the four fluorobenzothiadiazole donors, while charge separation in the DTS(PTTh 2) 2 blend is slower. Using TR-EPR we also investigated the triplet exciton formation pathways in the blend. The polarization patterns reveal that the excitons originate from both intersystem crossing (ISC) and back electron transfer (BET) processes. The DTS(PTTh 2) 2 blend was found to contain substantially more triplet excitons formed by BET than the fluorobenzothiadiazole blends. As a result, the higher BET triplet exciton population in the DTS(PTTh 2) 2 blend is in accordance with the slower charge separation dynamics observed in this blend.« less

Picosecond Dynamics Of The GaAs (110) Surface Studied With Laser Photoemission

NASA Astrophysics Data System (ADS)

Haight, R.; Silberman, J. A.; Lilie, M. I.

1988-08-01

A novel laser system and detection scheme is described which has been developed to investigate the transient dynamics of photoexcited electrons at material surfaces and interfaces with photoemission. The excited carrier population on the surface of GaAs (110) and the related Cr/GaAs (110) surface has been studied with 1-2 picosecond time resolution. Studies reveal a rapid rise and fall of the photexcited carrier population at the clean semiconductor surface within 15 picoseconds of excitation. For times greater than 15 picoseconds the carrier density decays slowly. Studies of the photoexcited surface after deposition of small numbers of Cr atoms reveal a remarkable decrease in the carrier density observed at the surface for a coverage as low as .006 monolayer.

Ultrafast observation of lattice dynamics in laser-irradiated gold foils

DOE PAGES

Hartley, N. J.; Ozaki, Norimasa; Matsuoka, T.; ...

2017-02-13

Here, we have observed the lattice expansion before the onset of compression in an optical-laser-driven target, using diffraction of femtosecond X-ray beams generated by the SPring-8 Angstrom Compact Free-electron Laser. The change in diffraction angle provides a direct measure of the lattice spacing, allowing the density to be calculated with a precision of ±1%. From the known equation of state relations, this allows an estimation of the temperature responsible for the expansion as <1000 K. The subsequent ablation-driven compression was observed with a clear rise in density at later times. This demonstrates the feasibility of studying the dynamics of preheatingmore » and shock formation with unprecedented detail.« less

Ultrafast observation of lattice dynamics in laser-irradiated gold foils

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

Hartley, N. J.; Ozaki, Norimasa; Matsuoka, T.

Here, we have observed the lattice expansion before the onset of compression in an optical-laser-driven target, using diffraction of femtosecond X-ray beams generated by the SPring-8 Angstrom Compact Free-electron Laser. The change in diffraction angle provides a direct measure of the lattice spacing, allowing the density to be calculated with a precision of ±1%. From the known equation of state relations, this allows an estimation of the temperature responsible for the expansion as <1000 K. The subsequent ablation-driven compression was observed with a clear rise in density at later times. This demonstrates the feasibility of studying the dynamics of preheatingmore » and shock formation with unprecedented detail.« less

Electrical manipulation of dynamic magnetic impurity and spin texture of helical Dirac fermions

NASA Astrophysics Data System (ADS)

Wang, Rui-Qiang; Zhong, Min; Zheng, Shi-Han; Yang, Mou; Wang, Guang-Hui

2016-05-01

We have theoretically investigated the spin inelastic scattering of helical electrons off a high-spin nanomagnet absorbed on a topological surface. The nanomagnet is treated as a dynamic quantum spin and driven by the spin transfer torque effect. We proposed a mechanism to electrically manipulate the spin texture of helical Dirac fermions rather than by an external magnetic field. By tuning the bias voltage and the direction of impurity magnetization, we present rich patterns of spin texture, from which important fingerprints exclusively associated with the spin helical feature are obtained. Furthermore, it is found that the nonmagnetic potential can create the resonance state in the spin density with different physics as the previously reported resonance of charge density.

Understanding the impact of insulating and conducting endplate boundary conditions on turbulence in CSDX through nonlocal simulations

DOE PAGES

Vaezi, P.; Holland, C.; Thakur, S. C.; ...

2017-04-01

The Controlled Shear Decorrelation Experiment (CSDX) linear plasma device provides a unique platform for investigating the underlying physics of self-regulating drift-wave turbulence/zonal flow dynamics. A minimal model of 3D drift-reduced nonlocal cold ion fluid equations which evolves density, vorticity, and electron temperature fluctuations, with proper sheath boundary conditions, is used to simulate dynamics of the turbulence in CSDX and its response to changes in parallel boundary conditions. These simulations are then carried out using the BOUndary Turbulence (BOUT++) framework and use equilibrium electron density and temperature profiles taken from experimental measurements. The results show that density gradient-driven drift-waves are themore » dominant instability in CSDX. However, the choice of insulating or conducting endplate boundary conditions affects the linear growth rates and energy balance of the system due to the absence or addition of Kelvin-Helmholtz modes generated by the sheath-driven equilibrium E × B shear and sheath-driven temperature gradient instability. Moreover, nonlinear simulation results show that the boundary conditions impact the turbulence structure and zonal flow formation, resulting in less broadband (more quasi-coherent) turbulence and weaker zonal flow in conducting boundary condition case. These results are qualitatively consistent with earlier experimental observations.« less

New insights on boundary plasma turbulence and the Quasi-Coherent Mode in Alcator C-Mod using a Mirror Langmuir Probe

NASA Astrophysics Data System (ADS)

Labombard, Brian

2013-10-01

A ``Mirror Langmuir Probe'' (MLP) diagnostic has been used to interrogate edge plasma profiles and turbulence in Alcator C-Mod with unprecedented detail, yielding fundamental insights on the Quasi-Coherent Mode (QCM) - a mode that regulates plasma density and impurities in EDA H-modes without ELMs. The MLP employs a fast-switching, self-adapting bias scheme, recording density, electron temperature and plasma potential simultaneously at high bandwidth (~1 MHz) on each of four separate electrodes on a scanning probe. Temporal dynamics are followed in detail; wavenumber-frequency spectra and phase relationships are readily deduced. Poloidal field fluctuations are recorded separately with a two-coil, scanning probe. Results from ohmic L-mode and H-mode plasmas are reported, including key observations of the QCM: The QCM lives in a region of positive radial electric field, with a mode width (~3 mm) that spans open and closed field line regions. Remarkably large amplitude (~30%), sinusoidal bursts in density, electron temperature and plasma potential fluctuations are observed that are in phase; potential lags density by at most 10 degrees. Propagation velocity of the mode corresponds to the sum of local E × B and electron diamagnetic drift velocities - quantities that are deduced directly from time-averaged profiles. Poloidal magnetic field fluctuations project to parallel current densities of ~5 amps/cm2 in the mode layer, with significant parallel electromagnetic induction. Electron force balance is examined, unambiguously identifying the mode type. It is found that fluctuations in parallel electron pressure gradient are roughly balanced by the sum of electrostatic and electromotive forces. Thus the primary mode structure of the QCM is that of a drift-Alfven wave. Work supported by US DoE award DE-FC02-99ER54512.

The Role of the Dynamic Plasmapause on Outer Radiation Belt Electron Flux Enhancement and Three-Belt Structure Formation

NASA Astrophysics Data System (ADS)

Bruff, M.; Jaynes, A. N.; Zhao, H.; Malaspina, D.

2017-12-01

The plasmasphere is a highly dynamic toroidal region of cold, dense plasma around Earth. Plasma waves exist both inside and outside this region and can contribute to the loss and acceleration of high energy outer radiation belt electrons. Early observational studies found an apparent correlation on long time scales between the observed inner edge of the outer radiation belt and the simulated innermost plasmapause location. More recent work using high resolution Van Allen Probe satellite data has found a more complex relationship. The aim of this project was to provide a systematic study of the location and dynamics of the plasmapause compared to the MeV electrons in the outer radiation belt. We used spin-averaged electron flux data from the Relativistic Electron Proton Telescope (REPT) and density data derived from the EFW instrument on the Van Allen Probe satellites. We analyzed these data to determine the standoff distance of the location of peak electron flux of the outer belt MeV electrons from the plasmapause. We found that the location of peak flux was consistently outside but within ΔL=2.5 from the innermost location of the plasmapause at enhancement times, with an average standoff distance ΔL=1.0 +/- 0.5. This is consistent with the current model of chorus enhancement and previous observations of chorus activity. Finally, we identified "three-belt" structure events where a second outer belt formed and found a repeated pattern of plasmapause dynamics associated with specific changes in electron flux required to generate and sustain these structures. This study is significant to improving our understanding of how the plasmasphere under differing conditions can both shield Earth from or worsen the impacts of geomagnetic activity.

ICFA Beam Dynamics Newsletter

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

Pikin, A.

2017-11-21

Electron beam ion sources technology made significant progress since 1968 when this method of producing highly charged ions in a potential trap within electron beam was proposed by E. Donets. Better understanding of physical processes in EBIS, technological advances and better simulation tools determined significant progress in key EBIS parameters: electron beam current and current density, ion trap capacity, attainable charge states. Greatly increased the scope of EBIS and EBIT applications. An attempt is made to compile some of EBIS engineering problems and solutions and to demonstrate a present stage of understanding the processes and approaches to build a bettermore » EBIS.« less

Ionosphere of Mars observed by Mars Express.

NASA Astrophysics Data System (ADS)

Dubinin, Eduard; Fraenz, Markus; Andrews, Dave; Morgan, Dave

2016-04-01

The Martian ionosphere is studied at different solar zenith angles using the local electron number densities and total electron content (TEC) derived from the observations by MARSIS onboard Mars Express. The data are complemented by the ASPERA-3 observations which provide us with the information about upward/downward velocity of the low-energy ions and electron precipitation. We consider the Mars Express observations at different solar cycle intervals. Different factors which influence the ionosphere dynamics are analyzed. The focus is made on a role of the crustal magnetic field on the Martian ionosphere and its influence on ion escape.

Optical phonon effect in quasi-one-dimensional semiconductor quantum wires: Band-gap renormalization

NASA Astrophysics Data System (ADS)

Dan, Nguyen Trung; Bechstedt, F.

1996-02-01

We present theoretical studies of dynamical screening in quasi-one-dimensional semiconductor quantum wires including electron-electron and electron-LO-phonon interactions. Within the random-phase approximation we obtain analytical expressions for screened interaction potentials. These expressions can be used to calculate the band-gap renormalization of quantum wires, which depends on the free-carrier density and temperature. We find that the optical phonon interaction effect plays a significant role in band-gap renormalization of quantum wires. The numerical results are compared with some recent experiment measurements as well as available theories.

Combination of Wavefunction and Density Functional Approximations for Describing Electronic Correlation

NASA Astrophysics Data System (ADS)

Garza, Alejandro J.

Perhaps the most important approximations to the electronic structure problem in quantum chemistry are those based on coupled cluster and density functional theories. Coupled cluster theory has been called the ``gold standard'' of quantum chemistry due to the high accuracy that it achieves for weakly correlated systems. Kohn-Sham density functionals based on semilocal approximations are, without a doubt, the most widely used methods in chemistry and material science because of their high accuracy/cost ratio. The root of the success of coupled cluster and density functionals is their ability to efficiently describe the dynamic part of the electron correlation. However, both traditional coupled cluster and density functional approximations may fail catastrophically when substantial static correlation is present. This severely limits the applicability of these methods to a plethora of important chemical and physical problems such as, e.g., the description of bond breaking, transition states, transition metal-, lanthanide- and actinide-containing compounds, and superconductivity. In an attempt to tackle this problem, nonstandard (single-reference) coupled cluster-based techniques that aim to describe static correlation have been recently developed: pair coupled cluster doubles (pCCD) and singlet-paired coupled cluster doubles (CCD0). The ability to describe static correlation in pCCD and CCD0 comes, however, at the expense of important amounts of dynamic correlation so that the high accuracy of standard coupled cluster becomes unattainable. Thus, the reliable and efficient description of static and dynamic correlation in a simultaneous manner remains an open problem for quantum chemistry and many-body theory in general. In this thesis, different ways to combine pCCD and CCD0 with density functionals in order to describe static and dynamic correlation simultaneously (and efficiently) are explored. The combination of wavefunction and density functional methods has a long history in quantum chemistry (practical implementations have appeared in the literature since the 1970s). However, this kind of techniques have not achieved widespread use due to problems such as double counting of correlation and the symmetry dilemma--the fact that wavefunction methods respect the symmetries of Hamiltonian, while modern functionals are designed to work with broken symmetry densities. Here, particular mathematical features of pCCD and CCD0 are exploited to avoid these problems in an efficient manner. The two resulting families of approximations, denoted as pCCD+DFT and CCD0+DFT, are shown to be able to describe static and dynamic correlation in standard benchmark calculations. Furthermore, it is also shown that CCD0+DFT lends itself to combination with correlation from the direct random phase approximation (dRPA). Inclusion of dRPA in the long-range via the technique of range-separation allows for the description of dispersion correlation, the remaining part of the correlation. Thus, when combined with the dRPA, CCD0+DFT can account for all three-types of electron correlation that are necessary to accurately describe molecular systems. Lastly, applications of CCD0+DFT to actinide chemistry are considered in this work. The accuracy of CCD0+DFT for predicting equilibrium geometries and vibrational frequencies of actinide molecules and ions is assessed and compared to that of well-established quantum chemical methods. For this purpose, the f0 actinyl series (UO2 2+, NpO 23+, PuO24+, the isoelectronic NUN, and Thorium (ThO, ThO2+) and Nobelium (NoO, NoO2) oxides are studied. It is shown that the CCD0+DFT description of these species agrees with available experimental data and is comparable with the results given by the highest-level calculations that are possible for such heavy compounds while being, at least, an order of magnitude lower in computational cost.

Ultrafast Charge Transfer of a Valence Double Hole in Glycine Driven Exclusively by Nuclear Motion

NASA Astrophysics Data System (ADS)

Li, Zheng; Vendrell, Oriol; Santra, Robin

2015-10-01

We explore theoretically the ultrafast transfer of a double electron hole between the functional groups of glycine after K -shell ionization and subsequent Auger decay. Although a large energy gap of about 15 eV initially exists between the two electronic states involved and coherent electronic dynamics play no role in the hole transfer, we find that the double hole is transferred within 3 to 4 fs between both functional ends of the glycine molecule driven solely by specific nuclear displacements and non-Born-Oppenheimer effects. The nuclear displacements along specific vibrational modes are of the order of 15% of a typical chemical bond between carbon, oxygen, and nitrogen atoms and about 30% for bonds involving hydrogen atoms. The time required for the hole transfer corresponds to less than half a vibrational period of the involved nuclear modes. This finding challenges the common wisdom that nuclear dynamics of the molecular skeleton are unimportant for charge transfer processes at the few-femtosecond time scale and shows that they can even play a prominent role. It also indicates that in x-ray imaging experiments, in which ionization is unavoidable, valence electron redistribution caused by nuclear dynamics might be much faster than previously anticipated. Thus, non-Born-Oppenheimer effects may affect the apparent electron densities extracted from such measurements.

Stochastic analysis of surface roughness models in quantum wires

NASA Astrophysics Data System (ADS)

Nedjalkov, Mihail; Ellinghaus, Paul; Weinbub, Josef; Sadi, Toufik; Asenov, Asen; Dimov, Ivan; Selberherr, Siegfried

2018-07-01

We present a signed particle computational approach for the Wigner transport model and use it to analyze the electron state dynamics in quantum wires focusing on the effect of surface roughness. Usually surface roughness is considered as a scattering model, accounted for by the Fermi Golden Rule, which relies on approximations like statistical averaging and in the case of quantum wires incorporates quantum corrections based on the mode space approach. We provide a novel computational approach to enable physical analysis of these assumptions in terms of phase space and particles. Utilized is the signed particles model of Wigner evolution, which, besides providing a full quantum description of the electron dynamics, enables intuitive insights into the processes of tunneling, which govern the physical evolution. It is shown that the basic assumptions of the quantum-corrected scattering model correspond to the quantum behavior of the electron system. Of particular importance is the distribution of the density: Due to the quantum confinement, electrons are kept away from the walls, which is in contrast to the classical scattering model. Further quantum effects are retardation of the electron dynamics and quantum reflection. Far from equilibrium the assumption of homogeneous conditions along the wire breaks even in the case of ideal wire walls.

Ultrafast Charge Transfer of a Valence Double Hole in Glycine Driven Exclusively by Nuclear Motion.

PubMed

Li, Zheng; Vendrell, Oriol; Santra, Robin

2015-10-02

We explore theoretically the ultrafast transfer of a double electron hole between the functional groups of glycine after K-shell ionization and subsequent Auger decay. Although a large energy gap of about 15 eV initially exists between the two electronic states involved and coherent electronic dynamics play no role in the hole transfer, we find that the double hole is transferred within 3 to 4 fs between both functional ends of the glycine molecule driven solely by specific nuclear displacements and non-Born-Oppenheimer effects. The nuclear displacements along specific vibrational modes are of the order of 15% of a typical chemical bond between carbon, oxygen, and nitrogen atoms and about 30% for bonds involving hydrogen atoms. The time required for the hole transfer corresponds to less than half a vibrational period of the involved nuclear modes. This finding challenges the common wisdom that nuclear dynamics of the molecular skeleton are unimportant for charge transfer processes at the few-femtosecond time scale and shows that they can even play a prominent role. It also indicates that in x-ray imaging experiments, in which ionization is unavoidable, valence electron redistribution caused by nuclear dynamics might be much faster than previously anticipated. Thus, non-Born-Oppenheimer effects may affect the apparent electron densities extracted from such measurements.

Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate

PubMed Central

Coslovich, Giacomo; Kemper, Alexander F.; Behl, Sascha; Huber, Bernhard; Bechtel, Hans A.; Sasagawa, Takao; Martin, Michael C.; Lanzara, Alessandra; Kaindl, Robert A.

2017-01-01

The ability to probe symmetry-breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-terahertz response of the model stripe compound La1.75Sr0.25NiO4, yielding novel insight into its electronic and structural dynamics following an ultrafast optical quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen—as witnessed by time-delayed suppression of zone-folded Ni–O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. The hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry-breaking dynamics in solids. PMID:29202025

Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate

DOE PAGES

Coslovich, Giacomo; Kemper, Alexander F.; Behl, Sascha; ...

2017-11-24

The ability to probe symmetry-breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-terahertz response of the model stripe compound La 1.75Sr 0.25NiO 4, yielding novel insight into its electronic and structural dynamics following an ultrafast opticalmore » quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen—as witnessed by time-delayed suppression of zone-folded Ni–O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. As a result, the hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry-breaking dynamics in solids.« less

Ultrafast dynamics of vibrational symmetry breaking in a charge-ordered nickelate

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

Coslovich, Giacomo; Kemper, Alexander F.; Behl, Sascha

The ability to probe symmetry-breaking transitions on their natural time scales is one of the key challenges in nonequilibrium physics. Stripe ordering represents an intriguing type of broken symmetry, where complex interactions result in atomic-scale lines of charge and spin density. Although phonon anomalies and periodic distortions attest the importance of electron-phonon coupling in the formation of stripe phases, a direct time-domain view of vibrational symmetry breaking is lacking. We report experiments that track the transient multi-terahertz response of the model stripe compound La 1.75Sr 0.25NiO 4, yielding novel insight into its electronic and structural dynamics following an ultrafast opticalmore » quench. We find that although electronic carriers are immediately delocalized, the crystal symmetry remains initially frozen—as witnessed by time-delayed suppression of zone-folded Ni–O bending modes acting as a fingerprint of lattice symmetry. Longitudinal and transverse vibrations react with different speeds, indicating a strong directionality and an important role of polar interactions. As a result, the hidden complexity of electronic and structural coupling during stripe melting and formation, captured here within a single terahertz spectrum, opens new paths to understanding symmetry-breaking dynamics in solids.« less

CDW fluctuations and the pseudogap in the single-particle conductivity of quasi-1D Peierls CDW systems: II.

PubMed

Kupčić, I; Rukelj, Z; Barišić, S

2014-05-14

The current-dipole Kubo formula for the dynamical conductivity of interacting multiband electronic systems derived in Kupčić et al (2013 J. Phys.: Condens. Matter 25 145602) is illustrated on the Peierls model for quasi-one-dimensional systems with the charge-density-wave (CDW) instability. Using the microscopic representation of the Peierls model, it is shown in which way the scattering of conduction electrons by CDW fluctuations affects the dynamical conductivity at temperatures above and well below the CDW transition temperature. The generalized Drude formula for the intraband conductivity is derived in the ordered CDW state well below the transition temperature. The natural extension of this formula to the case where the intraband memory function is dependent on frequency and wave vectors is also presented. It is shown that the main adventage of such a memory-function conductivity model is that it can be easily extended to study the dynamical conductivity and the electronic Raman scattering in more complicated multiband electronic systems in a way consistent with the law of conservation of energy. The incoherent interband conductivity in the CDW pseudogap state is briefly discussed as well.

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

Morante, S., E-mail: morante@roma2.infn.it; Rossi, G.C., E-mail: rossig@roma2.infn.it; Centro Fermi-Museo Storico della Fisica e Centro Studi e Ricerche E. Fermi, Compendio del Viminale, Piazza del Viminale 1, I-00184 Rome

We give a novel and simple proof of the DFT expression for the interatomic force field that drives the motion of atoms in classical Molecular Dynamics, based on the observation that the ground state electronic energy, seen as a functional of the external potential, is the Legendre transform of the Hohenberg–Kohn functional, which in turn is a functional of the electronic density. We show in this way that the so-called Hellmann–Feynman analytical formula, currently used in numerical simulations, actually provides the exact expression of the interatomic force.

Microstructure refinement of cold-sprayed copper investigated by electron channeling contrast imaging.

PubMed

Zhang, Yinyin; Brodusch, Nicolas; Descartes, Sylvie; Chromik, Richard R; Gauvin, Raynald

2014-10-01

The electron channeling contrast imaging technique was used to investigate the microstructure of copper coatings fabricated by cold gas dynamic spray. The high velocity impact characteristics for cold spray led to the formation of many substructures, such as high density dislocation walls, dislocation cells, deformation twins, and ultrafine equiaxed subgrains/grains. A schematic model is proposed to explain structure refinement of Cu during cold spray, where an emphasis is placed on the role of dislocation configurations and twinning.

Ionospheric variations during sudden stratospheric warming in the high- and mid-latitude regions

NASA Astrophysics Data System (ADS)

Yasyukevich, Anna; Voeykov, Sergey; Mylnikova, Anna

2017-04-01

The ionospheric dynamic in the high- and middle-latitude regions during the periods of sudden stratospheric warmings (SSW) was studied by using the international network of phase dual-frequency GPS/GLONASS receivers and the vertical sounding data. Twelve SSW events that occurred in the Northern Hemisphere 2006 through 2013 were considered. In order to identify the possible response of the ionosphere to SSW events, we carried out the analysis of the total electron (TEC) and the F2-layer maximum electron density (NmF2) deviations from the background level. We have also studied changes of the level of total electron content (TEC) wave-like variations characterized by a special index WTEC. The index reflects the intensity of medium- and large-scale traveling ionospheric disturbances. The dynamics of the high- and middle-latitude ionosphere at the points near the SSW areas was found to differ from the regular. For a large number of events, it is shown that, despite quiet geomagnetic conditions, a noticeable decrease in the NmF2 and TEC values (by 5-10% relative to the background level) is observed during the SSW evolution and maximum stages. On the contrary, for 10-20 days after the SSW maxima, NmF2 and TEC significantly exceed the monthly averaged values. Moreover, these electron density changes are observed for both strong and weak stratospheric warmings, and are recorded mainly during daytime. The observed SSW effects in the polar and mid-latitude ionosphere are assumed to be probably associated with the changes in the neutral composition at the thermospheric heights that affect the F2-layer electron density. The study is supported by the Russian Foundation for Basic Research under Grant No. 16-35-60018, as well as by the RF President Grant of Public Support for RF Leading Scientific Schools (NSh-6894.2016.5).

a Time-Dependent Many-Electron Approach to Atomic and Molecular Interactions

NASA Astrophysics Data System (ADS)

Runge, Keith

A new methodology is developed for the description of electronic rearrangement in atomic and molecular collisions. Using the eikonal representation of the total wavefunction, time -dependent equations are derived for the electronic densities within the time-dependent Hartree-Fock approximation. An averaged effective potential which ensures time reversal invariance is used to describe the effect of the fast electronic transitions on the slower nuclear motions. Electron translation factors (ETF) are introduced to eliminate spurious asymptotic couplings, and a local ETF is incorporated into a basis of traveling atomic orbitals. A reference density is used to describe local electronic relaxation and to account for the time propagation of fast and slow motions, and is shown to lead to an efficient integration scheme. Expressions for time-dependent electronic populations and polarization parameters are given. Electronic integrals over Gaussians including ETFs are derived to extend electronic state calculations to dynamical phenomena. Results of the method are in good agreement with experimental data for charge transfer integral cross sections over a projectile energy range of three orders of magnitude in the proton-Hydrogen atom system. The more demanding calculations of integral alignment, state-to-state integral cross sections, and differential cross sections are found to agree well with experimental data provided care is taken to include ETFs in the calculation of electronic integrals and to choose the appropriate effective potential. The method is found to be in good agreement with experimental data for the calculation of charge transfer integral cross sections and state-to-state integral cross sections in the one-electron heteronuclear Helium(2+)-Hydrogen atom system and in the two-electron system, Hydrogen atom-Hydrogen atom. Time-dependent electronic populations are seen to oscillate rapidly in the midst of collision event. In particular, multiple exchanges of the electron are seen to occur in the proton-Hydrogen atom system at low collision energies. The concepts and results derived from the approach provide new insight into the dynamics of nuclear screening and electronic rearrangement in atomic collisions.

Dynamics of a high-current relativistic electron beam

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

Strelkov, P. S., E-mail: strelkov@fpl.gpi.ru; Tarakanov, V. P., E-mail: karat@gmail.ru; Ivanov, I. E., E-mail: iei@fpl.gpi.ru

2015-06-15

The dynamics of a high-current relativistic electron beam is studied experimentally and by numerical simulation. The beam is formed in a magnetically insulated diode with a transverse-blade explosive-emission cathode. It is found experimentally that the radius of a 500-keV beam with a current of 2 kA and duration of 500 ns decreases with time during the beam current pulse. The same effect was observed in numerical simulations. This effect is explained by a change in the shape of the cathode plasma during the current pulse, which, according to calculations, leads to a change in the beam parameters, such as themore » electron pitch angle and the spread over the longitudinal electron momentum. These parameters are hard to measure experimentally; however, the time evolution of the radial profile of the beam current density, which can be measured reliably, coincides with the simulation results. This allows one to expect that the behavior of the other beam parameters also agrees with numerical simulations.« less

Online, automatic, ionospheric maps: IRI-PLAS-MAP

NASA Astrophysics Data System (ADS)

Arikan, F.; Sezen, U.; Gulyaeva, T. L.; Cilibas, O.

2015-04-01

Global and regional behavior of the ionosphere is an important component of space weather. The peak height and critical frequency of ionospheric layer for the maximum ionization, namely, hmF2 and foF2, and the total number of electrons on a ray path, Total Electron Content (TEC), are the most investigated and monitored values of ionosphere in capturing and observing ionospheric variability. Typically ionospheric models such as International Reference Ionosphere (IRI) can provide electron density profile, critical parameters of ionospheric layers and Ionospheric electron content for a given location, date and time. Yet, IRI model is limited by only foF2 STORM option in reflecting the dynamics of ionospheric/plasmaspheric/geomagnetic storms. Global Ionospheric Maps (GIM) are provided by IGS analysis centers for global TEC distribution estimated from ground-based GPS stations that can capture the actual dynamics of ionosphere and plasmasphere, but this service is not available for other ionospheric observables. In this study, a unique and original space weather service is introduced as IRI-PLAS-MAP from http://www.ionolab.org

Dynamic polarizability of tungsten atoms reconstructed from fast electrical explosion of fine wires in vacuum

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

Sarkisov, G. S.; Rosenthal, S. E.; Struve, K. W.

For nanosecond electrical explosion of fine metal wires in vacuum generates calibrated, radially expanded gas cylinders of metal atoms are surrounded by low-density fast expanding plasma corona. Here, a novel integrated-phase technique, based on laser interferometry, provides the dynamic dipole polarizability of metal atoms. This data was previously unavailable for tungsten atoms. Furthermore, an extremely high melting temperature and significant pre-melt electronic emission make these measurements particularly complicated for this refractory metal.

Dynamic polarizability of tungsten atoms reconstructed from fast electrical explosion of fine wires in vacuum

DOE PAGES

Sarkisov, G. S.; Rosenthal, S. E.; Struve, K. W.

2016-10-12

For nanosecond electrical explosion of fine metal wires in vacuum generates calibrated, radially expanded gas cylinders of metal atoms are surrounded by low-density fast expanding plasma corona. Here, a novel integrated-phase technique, based on laser interferometry, provides the dynamic dipole polarizability of metal atoms. This data was previously unavailable for tungsten atoms. Furthermore, an extremely high melting temperature and significant pre-melt electronic emission make these measurements particularly complicated for this refractory metal.

Expectation-Based Control of Noise and Chaos

NASA Technical Reports Server (NTRS)

Zak, Michael

2006-01-01

A proposed approach to control of noise and chaos in dynamic systems would supplement conventional methods. The approach is based on fictitious forces composed of expectations governed by Fokker-Planck or Liouville equations that describe the evolution of the probability densities of the controlled parameters. These forces would be utilized as feedback control forces that would suppress the undesired diffusion of the controlled parameters. Examples of dynamic systems in which the approach is expected to prove beneficial include spacecraft, electronic systems, and coupled lasers.

Conformational dynamics of a crystalline protein from microsecond-scale molecular dynamics simulations and diffuse X-ray scattering.

PubMed

Wall, Michael E; Van Benschoten, Andrew H; Sauter, Nicholas K; Adams, Paul D; Fraser, James S; Terwilliger, Thomas C

2014-12-16

X-ray diffraction from protein crystals includes both sharply peaked Bragg reflections and diffuse intensity between the peaks. The information in Bragg scattering is limited to what is available in the mean electron density. The diffuse scattering arises from correlations in the electron density variations and therefore contains information about collective motions in proteins. Previous studies using molecular-dynamics (MD) simulations to model diffuse scattering have been hindered by insufficient sampling of the conformational ensemble. To overcome this issue, we have performed a 1.1-μs MD simulation of crystalline staphylococcal nuclease, providing 100-fold more sampling than previous studies. This simulation enables reproducible calculations of the diffuse intensity and predicts functionally important motions, including transitions among at least eight metastable states with different active-site geometries. The total diffuse intensity calculated using the MD model is highly correlated with the experimental data. In particular, there is excellent agreement for the isotropic component of the diffuse intensity, and substantial but weaker agreement for the anisotropic component. Decomposition of the MD model into protein and solvent components indicates that protein-solvent interactions contribute substantially to the overall diffuse intensity. We conclude that diffuse scattering can be used to validate predictions from MD simulations and can provide information to improve MD models of protein motions.

Spectroscopic diagnostics of plume rebound and shockwave dynamics of confined aluminum laser plasma plumes

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

Yeates, P.; Kennedy, E. T.; School of Physical Sciences, Dublin City University

2011-06-15

Generation and expansion dynamics of aluminum laser plasma plumes generated between parallel plates of varying separation ({Delta}Z = 2.0, 3.2, 4.0, and 5.6 mm), which confined plume expansion normal to the ablation surface, were diagnosed. Space and time resolved visible emission spectroscopy in the spectral range {lambda} = 355-470 nm and time gated visible imaging were employed to record emission spectra and plume dynamics. Space and time resolved profiles of N{sub e} (the electron density), T{sub e} (the electron temperature), and T{sub ionz} (the ionization temperature) were compared for different positions in the plasma plume. Significant modifications of the profilesmore » of the above parameters were observed for plasma-surface collisions at the inner surface of the front plate, which formed a barrier to the free expansion of the plasma plume generated by the laser light on the surface of the back plate. Shockwave generation at the collision interface resulted in delayed compression of the low-density plasma plume near the inner ablation surface, at late stages in the plasma history. Upon exiting the cavity formed by the two plates, through an aperture in the front plate, the plasma plume underwent a second phase of free expansion.« less

Towards a better comprehension of plasma formation and heating in high performances electron cyclotron resonance ion sources (invited)

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

Mascali, D.; Gammino, S.; Celona, L.

2012-02-15

Further improvements of electron cyclotron resonance ion sources (ECRIS) output currents and average charge state require a deep understanding of electron and ion dynamics in the plasma. This paper will discuss the most recent advances about modeling of non-classical evidences like the sensitivity of electron energy distribution function to the magnetic field detuning, the influence of plasma turbulences on electron heating and ion confinement, the coupling between electron and ion dynamics. All these issues have in common the non-homogeneous distribution of the plasma inside the source: the abrupt density drop at the resonance layer regulates the heating regimes (from collectivemore » to turbulent), the beam formation mechanism and emittance. Possible means to boost the performances of future ECRIS will be proposed. In particular, the use of Bernstein waves, in preliminary experiments performed at Laboratori Nazionali del Sud (LNS) on MDIS (microwave discharge ion sources)-type sources, has permitted to sustain largely overdense plasmas enhancing the warm electron temperature, which will make possible in principle the construction of sources for high intensity multicharged ions beams with simplified magnetic structures.« less

Picosecond Thermal Dynamics in an Underdense Plasma Measured with Thomson Scattering

NASA Astrophysics Data System (ADS)

Haberberger, D.; Katz, J.; Bucht, S.; Davies, A.; Bromage, J.; Zuegel, J. D.; Froula, D. H.; Trines, R.; Bingham, R.; Sadler, J.; Norreys, P. A.

2017-10-01

Field-ionized underdense plasmas have many promising applications within the laser-plasma interaction field: nuclear fusion, particle accelerators, x-ray sources, and laser-plasma amplification. Having complete knowledge of the plasma dynamics is essential to establishing optimal parameters for a given application. Here picosecond-resolved Thomson scattering measurements have been used to determine the electron thermal dynamics of an underdense ( 1019/cm) H2 plasma irradiated by a 60-ps, 1053-nm laser pulse with an intensity of 2 × 1014 W/cm2. The picosecond-resolved spectra were obtained with a novel pulse-front tilt compensated streaked optical spectrometer. The electron temperature was observed to rise from an initial 5 eV to a density-dependent plateau in 23 ps. Simulation results indicate that inverse bremsstrahlung heating, radiative cooling, and radial conduction cooling all play an important role in modeling the thermal dynamics. This material is based upon work supported by the Department of Energy National Nuclear Security Administration under Award Number DE-NA0001944.

Negative hydrogen ions in a linear helicon plasma device

NASA Astrophysics Data System (ADS)

Corr, Cormac; Santoso, Jesse; Samuell, Cameron; Willett, Hannah; Manoharan, Rounak; O'Byrne, Sean

2015-09-01

Low-pressure negative ion sources are of crucial importance to the development of high-energy (>1 MeV) neutral beam injection systems for the ITER experimental tokamak device. Due to their high power coupling efficiency and high plasma densities, helicon devices may be able to reduce power requirements and potentially remove the need for caesium. In helicon sources, the RF power can be coupled efficiently into the plasma and it has been previously observed that the application of a small magnetic field can lead to a significant increase in the plasma density. In this work, we investigate negative ion dynamics in a high-power (20 kW) helicon plasma source. The negative ion fraction is measured by probe-based laser photodetachment, electron density and temperature are determined by a Langmuir probe and tuneable diode laser absorption spectroscopy is used to determine the density of the H(n = 2) excited atomic state and the gas temperature. The negative ion density and excited atomic hydrogen density display a maximum at a low applied magnetic field of 3 mT, while the electron temperature displays a minimum. The negative ion density can be increased by a factor of 8 with the application of the magnetic field. Spatial and temporal measurements will also be presented. The Australian Research Grants Council is acknowledged for funding.