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Sample records for sub-femtosecond electron dynamics

  1. Progress in sub-femtosecond control of electron localization in ...

    Indian Academy of Sciences (India)

    2014-01-04

    Jan 4, 2014 ... Abstract. Recent advances in controlled generation of intense, ultrashort laser pulses in the ... We discuss the origin of the idea and various ..... generation. 2.3 Electron localization using a combination of many-cycle IR pulse and an attosecond pulse train. Unlike both the above techniques which required ...

  2. Progress in sub-femtosecond control of electron localization in ...

    Indian Academy of Sciences (India)

    2014-01-04

    Jan 4, 2014 ... Recent advances in controlled generation of intense, ultrashort laser pulses in the femtosecond and attosecond time-scales have pushed new avenues of research in the coherent control of ... We discuss the origin of the idea and various mechanisms to achieve electron localization in small molecules.

  3. Sub-Femtosecond Correlated Dynamics Explored with Antiprotons

    CERN Document Server

    Ullrich, J; Fischer, D; Moshammer, R; Najjari, B; Schulz, M; Voitkiv, A; Welsch, C P

    2005-01-01

    Ionizing collisions of antiprotons with atoms or molecules at energies between a few keV up to about one MeV provide a unique tool to explore correlated dynamics of electrons at large perturbations on a time scale between several femtoseconds (1 fs = 10−15 s) down to some tens of attoseconds (1 as = 10−18 s). Exploiting and developing many‐particle imaging methods — Reaction‐Microscopes — integrated into a novel ultra‐low energy storage ring (USR) for slow antiprotons will enable to access for the first time fully differential cross sections for single and multiple ionization in such collisions. Moreover, the formation of antiprotonic atoms, molecules or of protonium might be explored in kinematically complete experiments yielding unprecedented information on (n,l)‐distributions of captured antiprotons as well as precise spectroscopic data of the respective energy levels. In this contribution the present status on single and double ionization by antiproton and ion impact is highlighted pointin...

  4. Capturing atomic-scale carrier dynamics with electrons

    Science.gov (United States)

    Baum, Peter; Krausz, Ferenc

    2017-09-01

    Light-driven electronic motion unfolds on times as short as the cycle period of light and on length scales as small as the distance between two neighboring atoms in a molecule. Visualizing fundamental light-matter interactions therefore requires access to attosecond and picometer dimensions. Here we report on a potential unification of electron diffraction and microscopy with attosecond technology, which could provide a full space-time access to elementary electronic processes in matter and materials. We review recent progress in ultrafast diffraction and microscopy towards temporal resolutions approaching 10 fs by use of state-of-the-art microwave technology and discuss our latest findings on all-optical compression approaches for reaching sub-femtosecond, sub-optical-cycle resolution. Four-dimensional electron diffraction with attosecond-picometer resolution will access all dynamics outside the atomic core, offering an all-embracing insight into fundamental electron-nuclear dynamics of complex materials.

  5. Toward sub-femtosecond pump-probe experiments: a dispersionless autocorrelator with attosecond resolution

    Energy Technology Data Exchange (ETDEWEB)

    Constant, E.; Mevel, E.; Zair, A.; Bagnoud, V.; Salin, F. [Bordeaux-1 Univ., Talence (FR). Centre Lasers Intenses et Applications (CELIA)

    2001-07-01

    We designed a dispersionless autocorrelator with a sub-femtosecond resolution suitable for the characterization of ultrashort X-UV pulses. We present a proof of feasibility experiment with 11 fs infrared pulses. (orig.)

  6. Electronic Spectroscopy & Dynamics

    Energy Technology Data Exchange (ETDEWEB)

    Mark Maroncelli, Nancy Ryan Gray

    2010-06-08

    The Gordon Research Conference (GRC) on Electronic Spectroscopy and Dynamics was held at Colby College, Waterville, NH from 07/19/2009 thru 07/24/2009. The Conference was well-attended with participants (attendees list attached). The attendees represented the spectrum of endeavor in this field coming from academia, industry, and government laboratories, both U.S. and foreign scientists, senior researchers, young investigators, and students. The GRC on Electronic Spectroscopy & Dynamics showcases some of the most recent experimental and theoretical developments in electronic spectroscopy that probes the structure and dynamics of isolated molecules, molecules embedded in clusters and condensed phases, and bulk materials. Electronic spectroscopy is an important tool in many fields of research, and this GRC brings together experts having diverse backgrounds in physics, chemistry, biophysics, and materials science, making the meeting an excellent opportunity for the interdisciplinary exchange of ideas and techniques. Topics covered in this GRC include high-resolution spectroscopy, biological molecules in the gas phase, electronic structure theory for excited states, multi-chromophore and single-molecule spectroscopies, and excited state dynamics in chemical and biological systems.

  7. Hydrated-electron population dynamics

    NARCIS (Netherlands)

    Pshenichnikov, MS; Baltuska, A; Wiersma, DA; Pshenichnikov, Maxim S.; Baltuška, Andrius

    2004-01-01

    A detailed frequency-resolved pump-probe study of hydrated electron dynamics, performed with 5-fs pulses, is presented. We show that the experimental data can be successfully described with a model in which the excited state lifetime is similar to50 fs in regular water and similar to70 A in heavy

  8. Realization of dynamical electronic systems

    Directory of Open Access Journals (Sweden)

    Hammari Elena

    2014-04-01

    Full Text Available This article gives an overview of a methodology for building dynamical electronic systems. As an example a part of a system for epileptic seizure prediction is used, which monitors EEG signals and continuously calculates the largest short-term Lyapunov exponents. In dynamical electronic systems, the cost of exploitation, for instance energy consumption, may vary substantially with the values of input signals. In addition, the functions describing the variations are not known at the time the system is designed. As a result, the architecture of the system must accommodate for the worst case exploitation costs, which rapidly exceed the available resources (for instance battery life when accumulated over time. The presented system scenario methodology solves these challenges by identifying at design time groups of possible exploitation costs, called system scenarios, and implementing a mechanism to detect system scenarios at run time and re-configure the system to cost-efficiently accommodate them. During reconfiguration, the optimized system architecture settings for the active system scenario are selected and the total exploitation cost is reduced. When the dynamic behavior is due to input data variables with a large number of possible values, current techniques for bottom-up scenario identification and detection becomes too complex. A new top-down technique, based on polygonal regions, is presented in this paper. The results for the example system indicate that with 10 system scenarios the average energy consumption of the system can be reduced by 28% and brought within 5% of the theoretically best solution.

  9. Ultrafast dynamics of correlated electrons

    Energy Technology Data Exchange (ETDEWEB)

    Rettig, Laurenz

    2012-07-09

    This work investigates the ultrafast electron dynamics in correlated, low-dimensional model systems using femtosecond time- and angle-resolved photoemission spectroscopy (trARPES) directly in the time domain. In such materials, the strong electron-electron (e-e) correlations or coupling to other degrees of freedom such as phonons within the complex many-body quantum system lead to new, emergent properties that are characterized by phase transitions into broken-symmetry ground states such as magnetic, superconducting or charge density wave (CDW) phases. The dynamical processes related to order like transient phase changes, collective excitations or the energy relaxation within the system allow deeper insight into the complex physics governing the emergence of the broken-symmetry state. In this work, several model systems for broken-symmetry ground states and for the dynamical charge balance at interfaces have been studied. In the quantum well state (QWS) model system Pb/Si(111), the charge transfer across the Pb/Si interface leads to an ultrafast energetic stabilization of occupied QWSs, which is the result of an increase of the electronic confinement to the metal film. In addition, a coherently excited surface phonon mode is observed. In antiferromagnetic (AFM) Fe pnictide compounds, a strong momentum-dependent asymmetry of electron and hole relaxation rates allows to separate the recovery dynamics of the AFM phase from electron-phonon (e-ph) relaxation. The strong modulation of the chemical potential by coherent phonon modes demonstrates the importance of e-ph coupling in these materials. However, the average e-ph coupling constant is found to be small. The investigation of the excited quasiparticle (QP) relaxation dynamics in the high-T{sub c}4 superconductor Bi{sub 2}Sr{sub 2}CaCu{sub 2}O{sub 8+δ} reveals a striking momentum and fluence independence of the QP life times. In combination with the momentum-dependent density of excited QPs, this demonstrates the

  10. Nonadiabatic electron wavepacket dynamics behind molecular autoionization.

    Science.gov (United States)

    Matsuoka, Takahide; Takatsuka, Kazuo

    2018-01-07

    A theoretical method for real-time dynamics of nonadiabatic reorganization of electronic configurations in molecules is developed, with dual aim that the intramolecular electron dynamics can be probed by means of direct and/or indirect photoionizations and that the physical origins behind photoionization signals attained in the time domain can be identified in terms of the language of time-dependent quantum chemistry. In doing so, we first formulate and implement a new computational scheme for nonadiabatic electron dynamics associated with molecular ionization, which well fits in the general theory of nonadiabatic electron dynamics. In this method, the total nonadiabatic electron wavepackets are propagated in time directly with complex natural orbitals without referring to Hartree-Fock molecular orbitals, and the amount of electron flux from a molecular region leading to ionization is evaluated in terms of the relevant complex natural orbitals. In the second half of this paper, we apply the method to electron dynamics in the elementary processes consisting of the Auger decay to demonstrate the methodological significance. An illustrative example is taken from an Auger decay starting from the 2a1 orbital hole-state of H2O+. The roles of nuclear momentum (kinetic) couplings in electronic-state mixing during the decay process are analyzed in terms of complex natural orbitals, which are schematically represented in the conventional language of molecular symmetry of the Hartree-Fock orbitals.

  11. Nonadiabatic electron wavepacket dynamics behind molecular autoionization

    Science.gov (United States)

    Matsuoka, Takahide; Takatsuka, Kazuo

    2018-01-01

    A theoretical method for real-time dynamics of nonadiabatic reorganization of electronic configurations in molecules is developed, with dual aim that the intramolecular electron dynamics can be probed by means of direct and/or indirect photoionizations and that the physical origins behind photoionization signals attained in the time domain can be identified in terms of the language of time-dependent quantum chemistry. In doing so, we first formulate and implement a new computational scheme for nonadiabatic electron dynamics associated with molecular ionization, which well fits in the general theory of nonadiabatic electron dynamics. In this method, the total nonadiabatic electron wavepackets are propagated in time directly with complex natural orbitals without referring to Hartree-Fock molecular orbitals, and the amount of electron flux from a molecular region leading to ionization is evaluated in terms of the relevant complex natural orbitals. In the second half of this paper, we apply the method to electron dynamics in the elementary processes consisting of the Auger decay to demonstrate the methodological significance. An illustrative example is taken from an Auger decay starting from the 2a1 orbital hole-state of H2O+. The roles of nuclear momentum (kinetic) couplings in electronic-state mixing during the decay process are analyzed in terms of complex natural orbitals, which are schematically represented in the conventional language of molecular symmetry of the Hartree-Fock orbitals.

  12. Dynamics of a photoexcited hydrated electron

    NARCIS (Netherlands)

    Pshenichnikov, M.S.; Baltuška, A.; Wiersma, D.A.; Kärtner, F.X.

    2004-01-01

    Combining photon-echo and frequency-resolved pump-probe techniques with extremely short laser pulses that consist of only few optical cycles, we investigate the dynamics of the equilibrated hydrated electron. The pure dephasing time of the hydrated electron deduced from the photon-echo measurements

  13. Dynamic aspects of electronic predissociation

    DEFF Research Database (Denmark)

    Grønager, Michael; Henriksen, Niels Engholm

    1996-01-01

    We consider electronic excitation induced with a continuous wave laser to an excited bound state which can predissociate due to a radiationless transition to a dissociative state. The conditions for a separation of the process into the preparation of a vibrational eigenstate which subsequently di...

  14. Electron dynamics controlled via self-interaction

    CERN Document Server

    Tamburini, Matteo; Di Piazza, Antonino

    2013-01-01

    The dynamics of an electron in a strong laser field can be significantly altered by radiation reaction. This usually results in a strongly damped motion, with the electron losing a large fraction of its initial energy. Here we show that the electron dynamics in a bichromatic laser pulse can be indirectly controlled by a comparatively small radiation reaction force through its interplay with the Lorentz force. By changing the relative phase between the two frequency components of the bichromatic laser field, an ultrarelativistic electron bunch colliding head-on with the laser pulse can be deflected in a controlled way, with the deflection angle being independent of the initial electron energy. The effect is predicted to be observable with intensities available at upcoming laser facilities.

  15. Hot electron dynamics in graphene

    Energy Technology Data Exchange (ETDEWEB)

    Ling, Meng-Chieh [Iowa State Univ., Ames, IA (United States)

    2011-01-01

    Graphene, a two-dimensional (2D) honeycomb structure allotrope of carbon atoms, has a long history since the invention of the pencil [Petroski (1989)] and the linear dispersion band structure proposed by Wallace [Wal]; however, only after Novoselov et al. successively isolated graphene from graphite [Novoselov et al. (2004)], it has been studied intensively during the recent years. It draws so much attentions not only because of its potential application in future electronic devices but also because of its fundamental properties: its quasiparticles are governed by the two-dimensional Dirac equation, and exhibit a variety of phenomena such as the anomalous integer quantum Hall effect (IQHE) [Novoselov et al. (2005)] measured experimentally, a minimal conductivity at vanishing carrier concentration [Neto et al. (2009)], Kondo effect with magnetic element doping [Hentschel and Guinea (2007)], Klein tunneling in p-n junctions [Cheianov and Fal’ko (2006), Beenakker (2008)], Zitterbewegung [Katsnelson (2006)], and Schwinger pair production [Schwinger (1951); Dora and Moessner (2010)]. Although both electron-phonon coupling and photoconductivity in graphene also draws great attention [Yan et al. (2007); Satou et al. (2008); Hwang and Sarma (2008); Vasko and Ryzhii (2008); Mishchenko (2009)], the nonequilibrium behavior based on the combination of electronphonon coupling and Schwinger pair production is an intrinsic graphene property that has not been investigated. Our motivation for studying clean graphene at low temperature is based on the following effect: for a fixed electric field, below a sufficiently low temperature linear eletric transport breaks down and nonlinear transport dominates. The criteria of the strength of this field [Fritz et al. (2008)] is eE = T2/~vF (1.1) For T >√eE~vF the system is in linear transport regime while for T <√eE~vF the system is in nonlinear transport regime. From the scaling’s point of view, at the nonlinear transport regime

  16. Protein electron transfer: Dynamics and statistics.

    Science.gov (United States)

    Matyushov, Dmitry V

    2013-07-14

    Electron transfer between redox proteins participating in energy chains of biology is required to proceed with high energetic efficiency, minimizing losses of redox energy to heat. Within the standard models of electron transfer, this requirement, combined with the need for unidirectional (preferably activationless) transitions, is translated into the need to minimize the reorganization energy of electron transfer. This design program is, however, unrealistic for proteins whose active sites are typically positioned close to the polar and flexible protein-water interface to allow inter-protein electron tunneling. The high flexibility of the interfacial region makes both the hydration water and the surface protein layer act as highly polar solvents. The reorganization energy, as measured by fluctuations, is not minimized, but rather maximized in this region. Natural systems in fact utilize the broad breadth of interfacial electrostatic fluctuations, but in the ways not anticipated by the standard models based on equilibrium thermodynamics. The combination of the broad spectrum of static fluctuations with their dispersive dynamics offers the mechanism of dynamical freezing (ergodicity breaking) of subsets of nuclear modes on the time of reaction/residence of the electron at a redox cofactor. The separation of time-scales of nuclear modes coupled to electron transfer allows dynamical freezing. In particular, the separation between the relaxation time of electro-elastic fluctuations of the interface and the time of conformational transitions of the protein caused by changing redox state results in dynamical freezing of the latter for sufficiently fast electron transfer. The observable consequence of this dynamical freezing is significantly different reorganization energies describing the curvature at the bottom of electron-transfer free energy surfaces (large) and the distance between their minima (Stokes shift, small). The ratio of the two reorganization energies

  17. Ab Initio molecular dynamics with excited electrons

    NARCIS (Netherlands)

    Alavi, A.; Kohanoff, J.; Parrinello, M.; Frenkel, D.

    1994-01-01

    A method to do ab initio molecular dynamics suitable for metallic and electronically hot systems is described. It is based on a density functional which is costationary with the finite-temperature functional of Mermin, with state being included with possibly fractional occupation numbers.

  18. Ultrafast Electron Dynamics in Solar Energy Conversion.

    Science.gov (United States)

    Ponseca, Carlito S; Chábera, Pavel; Uhlig, Jens; Persson, Petter; Sundström, Villy

    2017-08-23

    Electrons are the workhorses of solar energy conversion. Conversion of the energy of light to electricity in photovoltaics, or to energy-rich molecules (solar fuel) through photocatalytic processes, invariably starts with photoinduced generation of energy-rich electrons. The harvesting of these electrons in practical devices rests on a series of electron transfer processes whose dynamics and efficiencies determine the function of materials and devices. To capture the energy of a photogenerated electron-hole pair in a solar cell material, charges of opposite sign have to be separated against electrostatic attractions, prevented from recombining and being transported through the active material to electrodes where they can be extracted. In photocatalytic solar fuel production, these electron processes are coupled to chemical reactions leading to storage of the energy of light in chemical bonds. With the focus on the ultrafast time scale, we here discuss the light-induced electron processes underlying the function of several molecular and hybrid materials currently under development for solar energy applications in dye or quantum dot-sensitized solar cells, polymer-fullerene polymer solar cells, organometal halide perovskite solar cells, and finally some photocatalytic systems.

  19. Structural dynamics of electronic and photonic systems

    CERN Document Server

    Suhir, Ephraim; Steinberg, David S

    2011-01-01

    The proposed book will offer comprehensive and versatile methodologies and recommendations on how to determine dynamic characteristics of typical micro- and opto-electronic structural elements (printed circuit boards, solder joints, heavy devices, etc.) and how to design a viable and reliable structure that would be able to withstand high-level dynamic loading. Particular attention will be given to portable devices and systems designed for operation in harsh environments (such as automotive, aerospace, military, etc.)  In-depth discussion from a mechanical engineer's viewpoint will be conducte

  20. Electron Dynamics in Finite Quantum Systems

    Science.gov (United States)

    McDonald, Christopher R.

    The multiconfiguration time-dependent Hartree-Fock (MCTDHF) and multiconfiguration time-dependent Hartree (MCTDH) methods are employed to investigate nonperturbative multielectron dynamics in finite quantum systems. MCTDHF is a powerful tool that allows for the investigation of multielectron dynamics in strongly perturbed quantum systems. We have developed an MCTDHF code that is capable of treating problems involving three dimensional (3D) atoms and molecules exposed to strong laser fields. This code will allow for the theoretical treatment of multielectron phenomena in attosecond science that were previously inaccessible. These problems include complex ionization processes in pump-probe experiments on noble gas atoms, the nonlinear effects that have been observed in Ne atoms in the presence of an x-ray free-electron laser (XFEL) and the molecular rearrangement of cations after ionization. An implementation of MCTDH that is optimized for two electrons, each moving in two dimensions (2D), is also presented. This implementation of MCTDH allows for the efficient treatment of 2D spin-free systems involving two electrons; however, it does not scale well to 3D or to systems containing more that two electrons. Both MCTDHF and MCTDH were used to treat 2D problems in nanophysics and attosecond science. MCTDHF is used to investigate plasmon dynamics and the quantum breathing mode for several electrons in finite lateral quantum dots. MCTDHF is also used to study the effects of manipulating the potential of a double lateral quantum dot containing two electrons; applications to quantum computing are discussed. MCTDH is used to examine a diatomic model molecular system exposed to a strong laser field; nonsequential double ionization and high harmonic generation are studied and new processes identified and explained. An implementation of MCTDHF is developed for nonuniform tensor product grids; this will allow for the full 3D implementation of MCTDHF and will provide a means to

  1. Single-shot dynamic transmission electron microscopy

    Science.gov (United States)

    LaGrange, T.; Armstrong, M. R.; Boyden, K.; Brown, C. G.; Campbell, G. H.; Colvin, J. D.; DeHope, W. J.; Frank, A. M.; Gibson, D. J.; Hartemann, F. V.; Kim, J. S.; King, W. E.; Pyke, B. J.; Reed, B. W.; Shirk, M. D.; Shuttlesworth, R. M.; Stuart, B. C.; Torralva, B. R.; Browning, N. D.

    2006-07-01

    A dynamic transmission electron microscope (DTEM) has been designed and implemented to study structural dynamics in condensed matter systems. The DTEM is a conventional in situ transmission electron microscope (TEM) modified to drive material processes with a nanosecond laser, "pump" pulse and measure it shortly afterward with a 30-ns-long probe pulse of ˜107 electrons. An image with a resolution of <20nm may be obtained with a single pulse, largely eliminating the need to average multiple measurements and enabling the study of unique, irreversible events with nanosecond- and nanometer-scale resolution. Space charge effects, while unavoidable at such a high current, may be kept to reasonable levels by appropriate choices of operating parameters. Applications include the study of phase transformations and defect dynamics at length and time scales difficult to access with any other technique. This single-shot approach is complementary to stroboscopic TEM, which is capable of much higher temporal resolution but is restricted to the study of processes with a very high degree of repeatability.

  2. Dynamical electronic nematicity from Mott physics

    Energy Technology Data Exchange (ETDEWEB)

    Okamoto, Satoshi [ORNL; Senechal, D. [University of Sherbrooke; Civelli, M. [Institut Laue-Langevin (ILL); Tremblay, A.-M. [University of Sherbrooke

    2010-01-01

    Very large anisotropies in transport quantities have been observed in the presence of very small in-plane structural anisotropy in many strongly correlated electron materials. By studying the two-dimensional Hubbard model with dynamical-mean-field theory for clusters, we show that such large anisotropies can be induced without static stripe order if the interaction is large enough to yield a Mott transition. Anisotropy decreases at large frequency. The maximum effect on conductivity anisotropy occurs in the underdoped regime, as observed in high temperature superconductors.

  3. Nonadiabatic effects in electronic and nuclear dynamics

    Directory of Open Access Journals (Sweden)

    Martin P. Bircher

    2017-11-01

    Full Text Available Due to their very nature, ultrafast phenomena are often accompanied by the occurrence of nonadiabatic effects. From a theoretical perspective, the treatment of nonadiabatic processes makes it necessary to go beyond the (quasi static picture provided by the time-independent Schrödinger equation within the Born-Oppenheimer approximation and to find ways to tackle instead the full time-dependent electronic and nuclear quantum problem. In this review, we give an overview of different nonadiabatic processes that manifest themselves in electronic and nuclear dynamics ranging from the nonadiabatic phenomena taking place during tunnel ionization of atoms in strong laser fields to the radiationless relaxation through conical intersections and the nonadiabatic coupling of vibrational modes and discuss the computational approaches that have been developed to describe such phenomena. These methods range from the full solution of the combined nuclear-electronic quantum problem to a hierarchy of semiclassical approaches and even purely classical frameworks. The power of these simulation tools is illustrated by representative applications and the direct confrontation with experimental measurements performed in the National Centre of Competence for Molecular Ultrafast Science and Technology.

  4. Dynamically programmable electronic pill dispenser system.

    Science.gov (United States)

    Boquete, Luciano; Rodriguez-Ascariz, Jose Manuel; Artacho, Irene; Cantos-Frontela, Joaquin; Peixoto, Nathalia

    2010-06-01

    Compliance in medicine dispensation has proven critical for dosage control, diagnosis, and treatment. We have designed, manufactured, and characterized a novel dynamically programmable e-pill dispensing system. Our system is initially programmed remotely through a cell phone. After programming, the system may be reconfigured in order to adapt pill dispensation to new conditions. In this paper we describe the mechanics, electronics, control, and communication protocols implemented. Our dyn-e-pill devices can be actuated for over 350 h with two pill retrievals per hour. We challenged the charging circuit and demonstrated that the system has a lifetime longer than 6 h with a 30 min charging cycle, while it lasts for 14 h of uninterrupted use with a full charge.

  5. XXIII International Conference on Nonlinear Dynamics of Electronic Systems

    CERN Document Server

    Stoop, Ruedi; Stramaglia, Sebastiano

    2017-01-01

    This book collects contributions to the XXIII international conference “Nonlinear dynamics of electronic systems”. Topics range from non-linearity in electronic circuits to synchronisation effects in complex networks to biological systems, neural dynamics and the complex organisation of the brain. Resting on a solid mathematical basis, these investigations address highly interdisciplinary problems in physics, engineering, biology and biochemistry.

  6. Electron trapping in amorphous silicon: A quantum molecular dynamics study

    Energy Technology Data Exchange (ETDEWEB)

    Yang, Lin H.; Kalia, R.K.; Vashishta, P.

    1990-12-01

    Quantum molecular dynamics (QMD) simulations provide the real-time dynamics of electrons and ions through numerical solutions of the time-dependent Schrodinger and Newton equations, respectively. Using the QMD approach we have investigated the localization behavior of an excess electron in amorphous silicon at finite temperatures. For time scales on the order of a few picoseconds, we find the excess electron is localized inside a void of radius {approximately}3 {Angstrom} at finite temperatures. 12 refs.

  7. Electron cloud dynamics in the Cornell Electron Storage Ring Test Accelerator wiggler

    Directory of Open Access Journals (Sweden)

    C. M. Celata

    2011-04-01

    Full Text Available The interference of stray electrons (also called “electron clouds” with accelerator beams is important in modern intense-beam accelerators, especially those with beams of positive charge. In magnetic wigglers, used, for instance, for transverse emittance damping, the intense synchrotron radiation produced by the beam can generate an electron cloud of relatively high density. In this paper the complicated dynamics of electron clouds in wigglers is examined using the example of a wiggler in the Cornell Electron Storage Ring Test Accelerator experiment at the Cornell Electron Storage Ring. Three-dimensional particle-in-cell simulations with the WARP-POSINST computer code show different density and dynamics for the electron cloud at locations near the maxima of the vertical wiggler field when compared to locations near the minima. Dynamics in these regions, the electron cloud distribution vs longitudinal position, and the beam coherent tune shift caused by the wiggler electron cloud will be discussed.

  8. Ultrafast electronic dynamics in laser-excited crystalline bismuth

    Directory of Open Access Journals (Sweden)

    Chekalin S.

    2013-03-01

    Full Text Available Femtosecond spectroscopy was applied to capture complex dynamics of non equilibrium electrons in bismuth. Data analysis reveals significant wavevector dependence of electron-hole and electron-phonon coupling strength along the Γ-T direction of the Brillouin zone

  9. Dynamic pricing models for electronic business

    Indian Academy of Sciences (India)

    R. Narasimhan (Krishtel eMaging) 1461 1996 Oct 15 13:05:22

    Abstract. Dynamic pricing is the dynamic adjustment of prices to consumers depending upon the value these customers attribute to a product or service. Today's digital economy is ready for dynamic pricing; however recent research has shown that the prices will have to be adjusted in fairly sophisticated ways, based on.

  10. Dynamic pricing models for electronic business

    Indian Academy of Sciences (India)

    Dynamic pricing is the dynamic adjustment of prices to consumers depending upon the value these customers attribute to a product or service. Today's digital economy is ready for dynamic pricing; however recent research has shown that the prices will have to be adjusted in fairly sophisticated ways, based on sound ...

  11. Study of Electron Polarization Dynamics in the JLEIC at Jlab

    Energy Technology Data Exchange (ETDEWEB)

    Lin, Fanglei [Thomas Jefferson National Accelerator Facility (TJNAF), Newport News, VA (United States); Derbenev, Yaroslav [Thomas Jefferson National Accelerator Facility (TJNAF), Newport News, VA (United States); Morozov, Vasiliy [Thomas Jefferson National Accelerator Facility (TJNAF), Newport News, VA (United States); Zhang, Yuhong [Thomas Jefferson National Accelerator Facility (TJNAF), Newport News, VA (United States); Barber, Desmond P. [Deutsches Elektronen-Synchrotron (DESY), Hamburg (Germany)

    2017-05-01

    The design of an electron polarization scheme in the Jefferson Lab Electron-Ion Collider (JLEIC) aims to attain a high longitudinal electron polarization (over 70%) at collision points as required by the nuclear physics program. Comprehensive strategies for achieving this goal have been considered and developed including injection of highly polarized electrons from CEBAF, mechanisms for manipulation and preservation of the polarization in the JLEIC collider ring and measurement of the electron polarization. In particular, maintaining a sufficiently long polarization lifetime is crucial for accumulation of adequate experimental statistics. The chosen electron polarization configuration, based on the unique figure-8 geometry of the ring, removes the electron spin-tune energy dependence. This significantly simplifies the control of the electron polarization and suppresses the synchrotron sideband resonances. This paper reports recent studies and simulations of the electron polarization dynamics in the JLEIC electron collider ring.

  12. Generation of attosecond electron bunches in a laser-plasma accelerator using a plasma density upramp

    Energy Technology Data Exchange (ETDEWEB)

    Weikum, M.K., E-mail: maria.weikum@desy.de [Deutsches Elektronensynchrotron (DESY), Bdg. 30b, Notkestr. 85, 22607 Hamburg (Germany); Department of Physics, University of Strathclyde, G4 0NG Glasgow (United Kingdom); Li, F.Y. [Department of Physics, University of Strathclyde, G4 0NG Glasgow (United Kingdom); Assmann, R.W. [Deutsches Elektronensynchrotron (DESY), Bdg. 30b, Notkestr. 85, 22607 Hamburg (Germany); Sheng, Z.M. [Department of Physics, University of Strathclyde, G4 0NG Glasgow (United Kingdom); Laboratory for Laser Plasmas and Department of Physics and Astronomy, Shanghai Jiao Tong University, Shanghai 200240 (China); Jaroszynski, D. [Department of Physics, University of Strathclyde, G4 0NG Glasgow (United Kingdom)

    2016-09-01

    Attosecond electron bunches and attosecond radiation pulses enable the study of ultrafast dynamics of matter in an unprecedented regime. In this paper, the suitability for the experimental realization of a novel scheme producing sub-femtosecond duration electron bunches from laser-wakefield acceleration in plasma with self-injection in a plasma upramp profile has been investigated. While it has previously been predicted that this requires laser power above a few hundred terawatts typically, here we show that the scheme can be extended with reduced driving laser powers down to tens of terawatts, generating accelerated electron pulses with minimum length of around 166 attoseconds and picocoulombs charge. Using particle-in-cell simulations and theoretical models, the evolution of the accelerated electron bunch within the plasma as well as simple scalings of the bunch properties with initial laser and plasma parameters are presented. - Highlights: • LWFA with an upramp density profile can trap and accelerate sub-fs electron beams. • A reduction of the necessary threshold laser intensity by a factor 4 is presented. • Electron properties are tuned by varying initial laser and plasma parameters. • Simulations predict electron bunch lengths below 200 attoseconds with pC charge. • Strong bunch evolution effects and a large energy spread still need to be improved.

  13. Electron Dynamics by Inelastic X-Ray Scattering

    CERN Document Server

    Schülke, Winfried

    2007-01-01

    The book offers the first comprehensive review of experimental methods, theory, and successful applications of synchrotron radiation based inelastic X-ray scattering (IXS) spectroscopy, which enables the investigation of electron dynamics in condensed matter (correlated motion and excitation).

  14. Theory of molecular nonadiabatic electron dynamics in condensed phases

    Science.gov (United States)

    Takatsuka, Kazuo

    2017-11-01

    In light of the rapid progress of ultrafast chemical dynamics driven by the pulse lasers having width as short as several tens of attoseconds, we herein develop a theory of nonadiabatic electron wavepacket dynamics in condensed phases, with which to directly track the dynamics of electronic-state mixing such as electron transfer in liquid solvents. Toward this goal, we combine a theory of path-branching representation for nonadiabatic electron wavepacket dynamics in vacuum {a mixed quantum-classical representation, Yonehara and Takatsuka [J. Chem. Phys. 129, 134109 (2008)]} and a theory of entropy functional to treat chemical dynamics in condensed phases {a mixed dynamical-statistical representation, Takatsuka and Matsumoto [Phys. Chem. Chem. Phys. 18, 1771 (2016)]}. Difficulty and complexity in the present theoretical procedure arise in embedding the Schrödinger equation into classically treated statistical environment. Nevertheless, the resultant equations of motion for electronic-state mixing due to the intrinsic nonadiabatic interactions and solute-solvent interactions, along with the force matrix that drives nuclear branching paths, both turn out to be clear enough to make it possible to comprehend the physical meanings behind. We also discuss briefly the nonvalidness of naive application of the notion of nonadiabatic transition dynamics among free energy surfaces.

  15. Theory of molecular nonadiabatic electron dynamics in condensed phases.

    Science.gov (United States)

    Takatsuka, Kazuo

    2017-11-07

    In light of the rapid progress of ultrafast chemical dynamics driven by the pulse lasers having width as short as several tens of attoseconds, we herein develop a theory of nonadiabatic electron wavepacket dynamics in condensed phases, with which to directly track the dynamics of electronic-state mixing such as electron transfer in liquid solvents. Toward this goal, we combine a theory of path-branching representation for nonadiabatic electron wavepacket dynamics in vacuum {a mixed quantum-classical representation, Yonehara and Takatsuka [J. Chem. Phys. 129, 134109 (2008)]} and a theory of entropy functional to treat chemical dynamics in condensed phases {a mixed dynamical-statistical representation, Takatsuka and Matsumoto [Phys. Chem. Chem. Phys. 18, 1771 (2016)]}. Difficulty and complexity in the present theoretical procedure arise in embedding the Schrödinger equation into classically treated statistical environment. Nevertheless, the resultant equations of motion for electronic-state mixing due to the intrinsic nonadiabatic interactions and solute-solvent interactions, along with the force matrix that drives nuclear branching paths, both turn out to be clear enough to make it possible to comprehend the physical meanings behind. We also discuss briefly the nonvalidness of naive application of the notion of nonadiabatic transition dynamics among free energy surfaces.

  16. Particle dynamics during electronic sputtering of solid krypton

    DEFF Research Database (Denmark)

    Dutkiewicz, L.; Pedrys, R.; Schou, Jørgen

    1995-01-01

    We have modeled electronic sputtering of solid krypton by excimer production with molecular dynamics. Both excimer evolution in the solid and deexcitation processes have been incorporated in the simulation. The excimer dynamics in the lattice has been analyzed: the excimers formed near the surface...

  17. Radiation Belt Electron Dynamics: Modeling Atmospheric Losses

    Science.gov (United States)

    Selesnick, R. S.

    2003-01-01

    The first year of work on this project has been completed. This report provides a summary of the progress made and the plan for the coming year. Also included with this report is a preprint of an article that was accepted for publication in Journal of Geophysical Research and describes in detail most of the results from the first year of effort. The goal for the first year was to develop a radiation belt electron model for fitting to data from the SAMPEX and Polar satellites that would provide an empirical description of the electron losses into the upper atmosphere. This was largely accomplished according to the original plan (with one exception being that, for reasons described below, the inclusion of the loss cone electrons in the model was deferred). The main concerns at the start were to accurately represent the balance between pitch angle diffusion and eastward drift that determines the dominant features of the low altitude data, and then to accurately convert the model into simulated data based on the characteristics of the particular electron detectors. Considerable effort was devoted to achieving these ends. Once the model was providing accurate results it was applied to data sets selected from appropriate periods in 1997, 1998, and 1999. For each interval of -30 to 60 days, the model parameters were calculated daily, thus providing good short and long term temporal resolution, and for a range of radial locations from L = 2.7 to 3.9. .

  18. A single-electron approach for many-electron dynamics in high-order harmonic generation

    CERN Document Server

    Schild, Axel

    2016-01-01

    We present a novel ab-initio single-electron approach to correlated electron dynamics in strong laser fields. By writing the electronic wavefunction as a product of a marginal one-electron wavefunction and a conditional wavefunction, we show that the exact harmonic spectrum can be obtained from a single-electron Schr\\"odinger equation. To obtain the one-electron potential in practice, we propose an adiabatic approximation, i.e. a potential is generated that depends only on the position of one electron. This potential, together with the laser interaction, is then used to obtain the dynamics of the system. For a model Helium atom in a laser field, we show that by using our approach, the high-order harmonic generation spectrum can be obtained to a good approximation.

  19. Ultrafast dynamics of electrons at interfaces

    Energy Technology Data Exchange (ETDEWEB)

    McNeill, Jason Douglas [Univ. of California, Berkeley, CA (United States)

    1999-05-03

    Electronic states of a thin layer of material on a surface possess unique physical and chemical properties. Some of these properties arise from the reduced dimensionality of the thin layer with respect to the bulk or the properties of the electric field where two materials of differing dielectric constants meet at an interface. Other properties are related to the nature of the surface chemical bond. Here, the properties of excess electrons in thin layers of Xenon, Krypton, and alkali metals are investigated, and the bound state energies and effective masses of the excess electrons are determined using two-photon photoemission. For Xenon, the dependence of bound state energy, effective mass, and lifetime on layer thickness from one to nine layers is examined. Not all quantities were measured at each coverage. The two photon photoemission spectra of thin layers of Xenon on a Ag(111) substrate exhibit a number of sharp, well-defined peaks. The binding energy of the excess electronic states of Xenon layers exhibited a pronounced dependence on coverage. A discrete energy shift was observed for each additional atomic layer. At low coverage, a series of states resembling a Rydberg series is observed. This series is similar to the image state series observed on clean metal surfaces. Deviations from image state energies can be described in terms of the dielectric constant of the overlayer material and its effect on the image potential. For thicker layers of Xe (beyond the first few atomic layers), the coverage dependence of the features begins to resemble that of quantum well states. Quantum well states are related to bulk band states. However, the finite thickness of the layer restricts the perpendicular wavevector to a discrete set of values. Therefore, the spectrum of quantum well states contains a series of peaks which correspond to the various allowed values of the perpendicular wavevector. Analysis of the quantum well spectrum yields electronic band structure

  20. Dynamical backaction cooling with free electrons.

    Science.gov (United States)

    Niguès, A; Siria, A; Verlot, P

    2015-09-18

    The ability to cool single ions, atomic ensembles, and more recently macroscopic degrees of freedom down to the quantum ground state has generated considerable progress and perspectives in fundamental and technological science. These major advances have been essentially obtained by coupling mechanical motion to a resonant electromagnetic degree of freedom in what is generally known as laser cooling. Here, we experimentally demonstrate the first self-induced coherent cooling mechanism that is not mediated by an electromagnetic resonance. Using a focused electron beam, we report a 50-fold reduction of the motional temperature of a nanowire. Our result primarily relies on the sub-nanometre confinement of the electron beam and generalizes to any delayed and spatially confined interaction, with important consequences for near-field microscopy and fundamental nanoscale dissipation mechanisms.

  1. Mixed quantum-classical dynamics using collective electronic variables: A better alternative to electronic friction theories

    CERN Document Server

    Ryabinkin, Ilya G

    2016-01-01

    An accurate description of nonadiabatic dynamics of molecular species on metallic surfaces poses a serious computational challenge associated with a multitude of closely-spaced electronic states. We propose a mixed quantum-classical scheme that addresses this challenge by introducing collective electronic variables. These variables are defined through analytic block-diagonalization applied to the time-dependent Hamiltonian matrix governing the electronic dynamics. We compare our scheme with the Ehrenfest approach and with a full-memory electronic friction model on a one-dimensional "adatom + atomic chain" model. Our simulations demonstrate that collective-mode dynamics with only few (2-3) electronic variables is robust and can describe a variety of situations: from a chemisorbed atom on an insulator to an atom on a metallic surface. Our molecular model also reveals that the friction approach is prone to unpredictable and catastrophic failures.

  2. Electron Dynamics in Nanostructures in Strong Laser Fields

    Energy Technology Data Exchange (ETDEWEB)

    Kling, Matthias

    2014-09-11

    The goal of our research was to gain deeper insight into the collective electron dynamics in nanosystems in strong, ultrashort laser fields. The laser field strengths will be strong enough to extract and accelerate electrons from the nanoparticles and to transiently modify the materials electronic properties. We aimed to observe, with sub-cycle resolution reaching the attosecond time domain, how collective electronic excitations in nanoparticles are formed, how the strong field influences the optical and electrical properties of the nanomaterial, and how the excitations in the presence of strong fields decay.

  3. Electronic Predetermination of Ethylene Fragmentation Dynamics

    Directory of Open Access Journals (Sweden)

    Xinhua Xie

    2014-04-01

    Full Text Available We experimentally investigate the dependence of the fragmentation behavior of the ethylene dication on the intensity and duration of the laser pulses that initiate the fragmentation dynamics by strong-field double ionization. Using coincidence momentum imaging for the detection of ionic fragments, we disentangle the different contributions of ionization from lower-valence orbitals and field-driven excitation dynamics to the population of certain dissociative excited ionic states that are connected to one of several possible fragmentation pathways towards a given set of fragment ions. We find that the excitation probability to a particular excited state and therewith the outcome of the fragmentation reaction strongly depend on the parameters of the laser pulse. This, in turn, opens up new possibilities for controlling the outcome of fragmentation reactions of polyatomic molecules in that it may allow one to selectively enhance or suppress individual fragmentation channels, which was not possible in previous attempts of controlling fragmentation processes of polyatomic molecules with strong laser fields.

  4. Special issue on ultrafast electron and molecular dynamics

    Science.gov (United States)

    Hishikawa, Akiyoshi; Martin, Fernando; Vrakking, Marc

    2013-07-01

    Your invitation to submit. Journal of Physics. B: Atomic Molecular and Optical Physics (JPhysB) is delighted to announce a forthcoming special issue on ultrafast electron and molecular dynamics to appear in 2014, and invites you to submit a paper. Within the last decade, a number of novel approaches have emerged, both experimental and theoretical, that allow the investigation of (time-resolved) molecular dynamics in novel ways not anticipated before. Experimentally, the introduction of novel light sources such as high-harmonic generation and XUV/x-ray free electron lasers, and the emergence of novel detection strategies, such as time-resolved electron/x-ray diffraction and the fully coincident detection of electrons and fragment ions in reaction microscopes, has significantly expanded the arsenal of available techniques, and has taken studies of molecular dynamics into new domains of spectroscopic, spatial and temporal resolution, the latter including first explorations into the attosecond domain. Along the way, particular types of molecular dynamics, such as dynamics around conical intersections, have gained an increased prominence, sparked by an emerging realization about the essential role that this dynamics plays in relaxation pathways in important bio-molecular systems. The progress on the theoretical side has been no less impressive. Novel generations of supercomputers and a series of novel computational strategies have allowed nearly exact calculations in small molecules, as well as highly successful approximate calculations in large, polyatomic molecules. Frequent and intensive collaborations involving both theory and experiment have been essential for the progress that has been accomplished. The special issue 'Ultrafast electron and molecular dynamics' seeks to provide an overview of some of the most important developments in the field, while at the same time indicating how studies of (time-resolved) molecular dynamics are likely to evolve in the coming

  5. Dynamics of Dissociative Electron Attachment to Methane

    Science.gov (United States)

    Rescigno, T. N.; Douguet, N.; Fonseca, S.; Orel, A. E.; Slaughter, D. S.; Belkacem, A.

    2015-05-01

    We present the results of a theoretical ad experimental study of dissociative electron attachment (DEA) to CH4. The total DEA cross section is dominated by a single broad peak centered near 10 eV, leading predominantly to H-/CH4 and CH2-/CH4dissociation channels. We will present evidence that both of these ion channels result from excitation of a triply degenerate Feshbach resonance (doubly excited negative ion state) of 2T2 symmetry whose parent is the lowest excited triplet state of the neutral molecule. We will present calculated angular distributions based on analysis of the entrance amplitudes obtained from the results of complex Kohn scattering calculations along with experimentally measured angular distributions obtained using the COLTRIMS method. Work performed under the auspices of the US DOE by the LBNL and supported by the U.S. DOE Office of Basic Energy Sciences, Division of Chemical Sciences.

  6. Ultrafast Control of Electron Dynamics in 3D Topological Insulator

    Science.gov (United States)

    Azar Oliaei Motlagh, S.; Wu, Jhih-Sheng; Apalkov, Vadym; Stockman, Mark I.

    2017-10-01

    We theoretically study the coherent dynamics of Dirac fermions at the surface of a 3D topological insulator (Bi2Se3) in the field of an ultrafast laser pulse. In the presence of the ultrafast pulse, which has a femtosecond time scale that is less than the characteristic electron scattering time in these materials, the electron dynamics is coherent. Because of the gapless dispersion relation, the electrons dynamics is highly irreversible, which is dramatically different from dielectrics (fused silica, quartz, and sapphire). Due to irreversibility, finite conduction band population does exist after the pulse ends. Within two-band k.p Hamiltonian, which includes cubic momentum hexagonal warping terms, the residual conduction band (RCB) population in the reciprocal space is highly anisotropic. The distribution of RCB population in the reciprocal space strongly depends on the polarization of the ultrafast laser pulse.

  7. Dynamics and reactivity of trapped electrons on supported ice crystallites.

    Science.gov (United States)

    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

  8. Kinetic modelling of runaway electrons in dynamic scenarios

    CERN Document Server

    Stahl, A; Papp, G; Landreman, M; Fülöp, T

    2016-01-01

    Improved understanding of runaway-electron formation and decay processes are of prime interest for the safe operation of large tokamaks, and the dynamics of the runaway electrons during dynamical scenarios such as disruptions are of particular concern. In this paper, we present kinetic modelling of scenarios with time-dependent plasma parameters; in particular, we investigate hot-tail runaway generation during a rapid drop in plasma temperature. With the goal of studying runaway-electron generation with a self-consistent electric-field evolution, we also discuss the implementation of a conservative collision operator and demonstrate its properties. An operator for avalanche runaway-electron generation, which takes the energy dependence of the scattering cross section and the runaway distribution into account, is investigated. We show that the simpler avalanche model of Rosenbluth & Putvinskii [Nucl. Fusion 37, 1355 (1997)] can give very inaccurate results for the avalanche growth rate (either lower or hig...

  9. Phase-space dynamics of runaway electrons in magnetic fields

    Science.gov (United States)

    Guo, Zehua; McDevitt, Christopher J.; Tang, Xian-Zhu

    2017-04-01

    Dynamics of runaway electrons in magnetic fields are governed by the competition of three dominant physics: parallel electric field acceleration, Coulomb collision, and synchrotron radiation. Examination of the energy and pitch-angle flows reveals that the presence of local vortex structure and global circulation is crucial to the saturation of primary runaway electrons. Models for the vortex structure, which has an O-point to X-point connection, and the bump of runaway electron distribution in energy space have been developed and compared against the simulation data. Identification of these velocity-space structures opens a new venue to re-examine the conventional understanding of runaway electron dynamics in magnetic fields.

  10. Imaging the dynamics of free-electron Landau states.

    Science.gov (United States)

    Schattschneider, P; Schachinger, Th; Stöger-Pollach, M; Löffler, S; Steiger-Thirsfeld, A; Bliokh, K Y; Nori, Franco

    2014-08-08

    Landau levels and states of electrons in a magnetic field are fundamental quantum entities underlying the quantum Hall and related effects in condensed matter physics. However, the real-space properties and observation of Landau wave functions remain elusive. Here we report the real-space observation of Landau states and the internal rotational dynamics of free electrons. States with different quantum numbers are produced using nanometre-sized electron vortex beams, with a radius chosen to match the waist of the Landau states, in a quasi-uniform magnetic field. Scanning the beams along the propagation direction, we reconstruct the rotational dynamics of the Landau wave functions with angular frequency ~100 GHz. We observe that Landau modes with different azimuthal quantum numbers belong to three classes, which are characterized by rotations with zero, Larmor and cyclotron frequencies, respectively. This is in sharp contrast to the uniform cyclotron rotation of classical electrons, and in perfect agreement with recent theoretical predictions.

  11. Large amplitude femtosecond electron dynamics in metal clusters

    CERN Document Server

    Daligault, J

    2003-01-01

    We present a theoretical model that allows us to study linear and non-linear aspects of the femtosecond electron dynamics in metal clusters. The theoretical approach consists in the classical limit of the time-dependent Kohn-Sham equations. The electrons are described by a phase-space distribution function which satisfies a Vlasov-like equation while the ions are treated classically. This allows simulations for clusters containing several hundreds of atoms and extending up to several hundreds of femtoseconds during which the description conserves the fermionic character of the electron distribution. This semi-quantal approach compares very well with the purely quantal treatment. As an application of this approach, we show the prominent role of the electron dynamics during and after the interaction with an intense femtosecond laser pulse.

  12. Electron spin dynamics in cubic GaN

    Science.gov (United States)

    Buß, J. H.; Schupp, T.; As, D. J.; Brandt, O.; Hägele, D.; Rudolph, J.

    2016-12-01

    The electron spin dynamics in cubic GaN is comprehensively investigated by time-resolved magneto-optical Kerr-rotation spectroscopy over a wide range of temperatures, magnetic fields, and doping densities. The spin dynamics is found to be governed by the interplay of spin relaxation of localized electrons and Dyakonov-Perel relaxation of delocalized electrons. Localized electrons significantly contribute to spin relaxation up to room temperature at moderate doping levels, while Dyakonov-Perel relaxation dominates for high temperatures or degenerate doping levels. Quantitative agreement to Dyakonov-Perel theory requires a larger value of the spin-splitting constant than theoretically predicted. Possible reasons for this discrepancy are discussed, including the role of charged dislocations.

  13. Ultrafast electron dynamics in GeSi nanostructures

    Science.gov (United States)

    Cavill, S. A.; Potenza, A.; Dhesi, S. S.

    2012-01-01

    The relaxation dynamics of photoexcited hot carriers in GexSi1-x islands grown on Si(111)-(7×7) have been studied with the spatial and temporal resolution of time-resolved two-photon photoemission electron microscopy. The relaxation dynamics of the excited electronic states within the Ge-rich GexSi1-x dots and the surrounding Si-rich wetting layer are found to vary significantly below the conduction-band minimum. These differences are ascribed to faster hot-carrier-diffusion rates for the islands compared to those for the wetting layer.

  14. Spin dynamics in electron synchrotrons; Spindynamik in Elektronensynchrotronen

    Energy Technology Data Exchange (ETDEWEB)

    Schmidt, Jan Felix

    2017-07-14

    Providing spin polarized particle beams with circular accelerators requires the consideration of depolarizing resonances which may significantly reduce the desired degree of polarization at specific beam energies. The corresponding spin dynamical effects are typically analyzed with numerical methods. In case of electron beams the influence of the emission of synchrotron radiation has to be taken into account. On short timescales, as in synchrotrons with a fast energy ramp or in damping rings, spin dynamics are investigated with spin tracking algorithms. This thesis presents the spin tracking code Polematrix as a versatile tool to study the impact of synchrotron radiation on spin dynamics. Spin tracking simulations have been performed based on the well established particle tracking code Elegant. The numerical studies demonstrate effects which are responsible for beam depolarization: Synchrotron side bands of depolarizing resonances and decoherence of spin precession. Polematrix can be utilized for any electron accelerator with minimal effort as it imports lattice files from the tracking programs MAD-X or Elegant. Polematrix has been published as open source software. Currently, the Electron Stretcher Accelerator ELSA at Bonn University is the only electron synchrotron worldwide providing a polarized beam. Integer and intrinsic depolarizing resonances are compensated with dedicated countermeasures during the fast energy ramp. Polarization measurements from ELSA demonstrate the particular spin dynamics of electrons and confirm the results of the spin tracking code Polematrix.

  15. Space-charge dynamics of polymethylmethacrylate under electron beam irradiation

    CERN Document Server

    Gong, H; Ong, C K

    1997-01-01

    Space-charge dynamics of polymethylmethacrylate (PMMA) under electron beam irradiation has been investigated employing a scanning electron microscope. Assuming a Gaussian space-charge distribution, the distribution range (sigma) has been determined using a time-resolved current method in conjunction with a mirror image method. sigma is found to increase with irradiation time and eventually attain a stationary value. These observations have been discussed by taking into account radiation-induced conductivity and charge mobility. (author)

  16. Special issue on ultrafast electron and molecular dynamics

    Science.gov (United States)

    Martin, Fernando; Hishikawa, Akiyoshi; Vrakking, Marc

    2014-06-01

    In the last few years, the advent of novel experimental and theoretical approaches has made possible the investigation of (time-resolved) molecular dynamics in ways not anticipated before. Experimentally, the introduction of novel light sources such as high-harmonic generation (HHG) and XUV/x-ray free electron lasers, and the emergence of novel detection strategies, such as time-resolved electron/x-ray diffraction and the fully coincident detection of electrons and fragment ions in reaction microscopes, has significantly expanded the arsenal of available techniques, and has taken studies of molecular dynamics into new domains of spectroscopic, spatial and temporal resolution, the latter including first explorations into the attosecond domain, thus opening completely new avenues for imaging electronic and nuclear dynamics in molecules. Along the way, particular types of molecular dynamics, e.g., dynamics around conical intersections, have gained an increased prominence, sparked by the realization of the essential role that this dynamics plays in relaxation pathways in important bio-molecular systems. In the short term, this will allow one to uncover and control the dynamics of elementary chemical processes such as, e.g., ultrafast charge migration, proton transfer, isomerization or multiple ionization, and to address new key questions about the role of attosecond coherent electron dynamics in chemical reactivity. The progress on the theoretical side has been no less impressive. Novel generations of supercomputers and a series of novel computational strategies have allowed nearly exact calculations in small molecules, as well as highly successful approximate calculations in large, polyatomic molecules, including biomolecules. Frequent and intensive collaborations involving both theory and experiment have been essential for the progress that has been accomplished. The special issue 'Ultrafast electron and molecular dynamics' seeks to provide an overview of the current

  17. Influence of the dynamic screening on single-electron ionization of multi-electron atoms

    Energy Technology Data Exchange (ETDEWEB)

    Monti, J M; Fojon, O A; Rivarola, R D [Instituto de FIsica Rosario (CONICET-UNR) and Facultad de Ciencias Exactas, IngenierIa y Agrimensura, Universidad Nacional de Rosario, Avenida Pellegrini 250, 2000 Rosario (Argentina); Hanssen, J, E-mail: monti@ifir-conicet.gov.a [Institut de Chimie, Physique et Materiaux, Laboratoire de Physique Moleculaire et des Collisions, Universite Paul Verlaine - Metz, 1 Bv. Arago, 57078 Metz Cedex 3 (France)

    2010-10-28

    A complete formulation of the post-version of the continuum distorted wave-eikonal initial state model to investigate single-electron ionization of multi-electron atoms by fast bare ion beams is considered. The influence of the non-ionized electrons on the dynamic evolution of the ejected electron is analysed showing that the corresponding interaction plays a main role in the determination of double differential cross sections. It is demonstrated that its inclusion as an additional term in the perturbative potential of the exit channel avoids discrepancies between the pre- and post-versions of the studied distorted wave model.

  18. High-Harmonic Generation Enhanced by Dynamical Electron Correlation

    Science.gov (United States)

    Tikhomirov, Iliya; Sato, Takeshi; Ishikawa, Kenichi L.

    2017-05-01

    We theoretically study multielectron effects in high-harmonic generation (HHG), using all-electron first-principles simulations for a one-dimensional model atom. In addition to the usual plateau and cutoff (from a cation in the present case, since the neutral is immediately ionized), we find a prominent resonance peak far above the plateau and a second plateau extended beyond the first cutoff. These features originate from the dication response enhanced by orders of magnitude due to the action of the Coulomb force from the rescattering electron, and, hence, are a clear manifestation of electron correlation. Although the present simulations are done in 1D, the physical mechanism underlying the dramatic enhancement is expected to hold also for three-dimensional real systems. This will provide new possibilities to explore dynamical electron correlation in intense laser fields using HHG, which is usually considered to be of single-electron nature in most cases.

  19. Attosecond-correlated dynamics of two electrons in argon

    Indian Academy of Sciences (India)

    2014-01-11

    correlated dynamics of two electrons in argon. V Sharma N Camus B Fischer M Kremer A Rudenko B Bergues M Kuebel N G Johnson M F Kling T Pfeifer J Ullrich R Moshammer. Invited Talks Volume 82 Issue 1 January 2014 ...

  20. Lattice dynamics during electronic sputtering of solid Ne

    DEFF Research Database (Denmark)

    Dutkiewicz, L.; Pedrys, R.; Schou, Jørgen

    1997-01-01

    Electronic sputtering of solid neon has been studied with molecular dynamics. The cavity formation around an excited atom and particle migration in the surface region, as well as the sputtering process have been studied. A single atomic exciton has been observed to produce a desorption of up...

  1. Effect of strong coupling on interfacial electron transfer dynamics in ...

    Indian Academy of Sciences (India)

    Transient absorption studies on TPP-cat/TiO2 system exciting both the Soret band at 400 nm and the Q-band at 800 nm have been carried out to determine excitation wavelength-dependence on ET dynamics. The reaction channel for the electron-injection process has been found to be different for both the excitation ...

  2. Femtosecond electron-bunch dynamics in laser wakefields and vacuum

    NARCIS (Netherlands)

    Khachatryan, A.G.; Irman, A.; van Goor, F.A.; Boller, Klaus J.

    2007-01-01

    Recent advances in laser wakefield acceleration demonstrated the generation of extremely short (with a duration of a few femtoseconds) relativistic electron bunches with relatively low (of the order of couple of percent) energy spread. In this article we study the dynamics of such bunches in drift

  3. Structural preablation dynamics of graphite observed by ultrafast electron crystallography

    NARCIS (Netherlands)

    Carbone, Fabrizio; Baum, Peter; Rudolf, Petra; Zewail, Ahmed H.

    2008-01-01

    By means of time-resolved electron crystallography, we report direct observation of the structural dynamics of graphite, providing new insights into the processes involving coherent lattice motions and ultrafast graphene ablation. When graphite is excited by an ultrashort laser pulse, the excited

  4. Comparison of solvation dynamics of electrons in four polyols

    Energy Technology Data Exchange (ETDEWEB)

    Lampre, I.; Pernot, P.; Bonin, J. [Laboratoire de Chimie Physique/ELYSE, Universite Paris-Sud 11, UMR 8000, Bat. 349, Orsay F-91405 (France); CNRS, Orsay F-91405 (France); Mostafavi, M. [Laboratoire de Chimie Physique/ELYSE, Universite Paris-Sud 11, UMR 8000, Bat. 349, Orsay F-91405 (France); CNRS, Orsay F-91405 (France)], E-mail: mehran.mostafavi@lcp.u-psud.fr

    2008-10-15

    Using pump-probe transient absorption spectroscopy, we studied the solvation dynamics of the electron in liquid polyalcohols: ethane-1,2-diol, propane-1,2-diol, propane-1,3-diol and propane-1,2,3-triol. Time-resolved absorption spectra ranging from 440 to 720 nm were measured. Our study shows that the excess electron in the diols presents an intense and wide absorption band in the visible and near-IR spectral domain at early time after two-photon ionization of the neat solvent. Then, for the first tens of picoseconds, the electron spectrum shifts toward the blue domain and its bandwidth decreases as the red part of the initial spectrum rapidly drops, while the blue part hardly evolves. In contrast, in the triol, the absorption spectrum of the electron is early situated in the visible range after the pump pulse and then solely evolves in the red part. The Bayesian data analysis of the observed picosecond solvation dynamics with different models is in favor of a heterogeneous continuous relaxation. That is corroborated by the analogy between the change in the absorption band with increasing time or decreasing temperature. That tends to indicate a similar organization disorder of the solvent. Moreover, the electron solvation dynamics is very fast in propane-1,2,3-triol despite its high viscosity and highlight the role of the OH-group in that process.

  5. Phase-space Dynamics of Runaway Electrons In Tokamaks

    Energy Technology Data Exchange (ETDEWEB)

    Xiaoyin Guan, Hong Qin, and Nathaniel J. Fisch

    2010-08-31

    The phase-space dynamics of runaway electrons is studied, including the influence of loop voltage, radiation damping, and collisions. A theoretical model and a numerical algorithm for the runaway dynamics in phase space are developed. Instead of standard integrators, such as the Runge-Kutta method, a variational symplectic integrator is applied to simulate the long-term dynamics of a runaway electron. The variational symplectic integrator is able to globally bound the numerical error for arbitrary number of time-steps, and thus accurately track the runaway trajectory in phase space. Simulation results show that the circulating orbits of runaway electrons drift outward toward the wall, which is consistent with experimental observations. The physics of the outward drift is analyzed. It is found that the outward drift is caused by the imbalance between the increase of mechanical angular momentum and the input of toroidal angular momentum due to the parallel acceleration. An analytical expression of the outward drift velocity is derived. The knowledge of trajectory of runaway electrons in configuration space sheds light on how the electrons hit the first wall, and thus provides clues for possible remedies.

  6. Femtosecond electron diffraction: heralding the era of atomically resolved dynamics

    Science.gov (United States)

    Sciaini, Germán; Miller, R. J. Dwayne

    2011-09-01

    One of the great dream experiments in Science is to directly observe atomic motions as they occur. Femtosecond electron diffraction provided the first 'light' of sufficient intensity to achieve this goal by attaining atomic resolution to structural changes on the relevant timescales. This review covers the technical progress that made this new level of acuity possible and gives a survey of the new insights gained from an atomic level perspective of structural dynamics. Atomic level views of the simplest possible structural transition, melting, are discussed for a number of systems in which both thermal and purely electronically driven atomic displacements can be correlated with the degree of directional bonding. Optical manipulation of charge distributions and effects on interatomic forces/bonding can be directly observed through the ensuing atomic motions. New phenomena involving strongly correlated electron-lattice systems are also discussed in which optically induced changes in the potential energy landscape lead to ballistic structural changes. Concepts such as the structural order parameters are now directly observable at the atomic level of inspection to give a remarkable view of the extraordinary degree of cooperativity involved in strongly correlated electron-lattice systems. These recent examples, in combination with time-resolved real space imaging now possible with electron probes, are truly defining an emerging field that holds great promise to make a significant impact in how we understand structural dynamics. This article is dedicated to the memory of Professor David John Hugh Cockayne, a world leader in electron microscopy, who sadly passed away in December.

  7. Photocathode Optimization for a Dynamic Transmission Electron Microscope: Final Report

    Energy Technology Data Exchange (ETDEWEB)

    Ellis, P; Flom, Z; Heinselman, K; Nguyen, T; Tung, S; Haskell, R; Reed, B W; LaGrange, T

    2011-08-04

    The Dynamic Transmission Electron Microscope (DTEM) team at Harvey Mudd College has been sponsored by LLNL to design and build a test setup for optimizing the performance of the DTEM's electron source. Unlike a traditional TEM, the DTEM achieves much faster exposure times by using photoemission from a photocathode to produce electrons for imaging. The DTEM team's work is motivated by the need to improve the coherence and current density of the electron cloud produced by the electron gun in order to increase the image resolution and contrast achievable by DTEM. The photoemission test setup is nearly complete and the team will soon complete baseline tests of electron gun performance. The photoemission laser and high voltage power supply have been repaired; the optics path for relaying the laser to the photocathode has been finalized, assembled, and aligned; the internal setup of the vacuum chamber has been finalized and mostly implemented; and system control, synchronization, and data acquisition has been implemented in LabVIEW. Immediate future work includes determining a consistent alignment procedure to place the laser waist on the photocathode, and taking baseline performance measurements of the tantalum photocathode. Future research will examine the performance of the electron gun as a function of the photoemission laser profile, the photocathode material, and the geometry and voltages of the accelerating and focusing components in the electron gun. This report presents the team's progress and outlines the work that remains.

  8. Molecular Dynamics Simulation of Electron-Ion Temperature Relaxation in Dense Hydrogen: Electronic Quantum Effects

    Science.gov (United States)

    Ma, Qian; Dai, Jiayu; Zhao, Zengxiu

    2016-10-01

    The electron-ion temperature relaxation is an important non-equilibrium process in the generation of dense plasmas, particularly in Inertial Confinement Fusion. Classical molecular dynamics considers electrons as point charges, ignoring important quantum processes. We use an Electron Force Field (EFF) method to study the temperature relaxation processes, considering the nuclei as semi-classical point charges and assume electrons as Gaussian wave packets which includes the influences of the size and the radial motion of electrons. At the same time, a Pauli potential is used to describe the electronic exchange effect. At this stage, quantum effects such as exchange, tunneling can be included in this model. We compare the results from EFF and classical molecular dynamics, and find that the relaxation time is much longer with including quantum effects, which can be explained directly by the deference of collision cross sections between quantum particles and classical particles. Further, the final thermal temperature of electron and ion is different compared with classical results that the electron quantum effects cannot be neglected.

  9. Spatiotemporal Observation of Electron-Impact Dynamics in Photovoltaic Materials Using 4D Electron Microscopy

    KAUST Repository

    Shaheen, Basamat

    2017-05-17

    Understanding light-triggered charge carrier dynamics near photovoltaic-material surfaces and at interfaces has been a key element and one of the major challenges for the development of real-world energy devices. Visualization of such dynamics information can be obtained using the one-of-a-kind methodology of scanning ultrafast electron microscopy (S-UEM). Here, we address the fundamental issue of how the thickness of the absorber layer may significantly affect the charge carrier dynamics on material surfaces. Time-resolved snapshots indicate that the dynamics of charge carriers generated by electron impact in the electron-photon dynamical probing regime is highly sensitive to the thickness of the absorber layer, as demonstrated using CdSe films of different thicknesses as a model system. This finding not only provides the foundation for potential applications of S-UEM to a wide range of devices in the fields of chemical and materials research, but also has impact on the use and interpretation of electron beam-induced current for optimization of photoactive materials in these devices.

  10. Spatiotemporal Observation of Electron-Impact Dynamics in Photovoltaic Materials Using 4D Electron Microscopy.

    Science.gov (United States)

    Shaheen, Basamat S; Sun, Jingya; Yang, Ding-Shyue; Mohammed, Omar F

    2017-06-01

    Understanding light-triggered charge carrier dynamics near photovoltaic-material surfaces and at interfaces has been a key element and one of the major challenges for the development of real-world energy devices. Visualization of such dynamics information can be obtained using the one-of-a-kind methodology of scanning ultrafast electron microscopy (S-UEM). Here, we address the fundamental issue of how the thickness of the absorber layer may significantly affect the charge carrier dynamics on material surfaces. Time-resolved snapshots indicate that the dynamics of charge carriers generated by electron impact in the electron-photon dynamical probing regime is highly sensitive to the thickness of the absorber layer, as demonstrated using CdSe films of different thicknesses as a model system. This finding not only provides the foundation for potential applications of S-UEM to a wide range of devices in the fields of chemical and materials research, but also has impact on the use and interpretation of electron beam-induced current for optimization of photoactive materials in these devices.

  11. Molecular dynamics simulations of electron irradiated PVDF nanofibers

    Science.gov (United States)

    Miao, Jiayuan; Bhatta, Ram; Kisielowski, Christian; Lolla, Dinesh; Reneker, Darrell; Tsige, Mesfin; Taylor, Philip

    2014-03-01

    High-resolution, aberration corrected transmission electron microscopy was used to observe morphological changes and segmental motion of electrospun poly(vinylidene fluoride) nanofibers in an 80 kilovolt electron beam. Atomic and molecular scale high-resolution images of fibers were made with an aberration corrected electron microscope. Chemical and morphological changes, which include the breaking of the fiber, loss of fluorine atoms and cross-linking of chains, caused by the high-energy electron beam were observed. We present the results of molecular dynamics (MD) simulations of such atomic and molecular level observations. The calculational models include the influence of chain scission, chain recoiling, and torsional defects on the morphology of a nanofiber. The effects of the loss of fluorine atoms and the applied tension on the morphology of the fibers were also investigated. Work supported by the Petroleum Research Fund of the American Chemical Society.

  12. Extraction dynamics of electrons from magneto-optically trapped atoms

    Science.gov (United States)

    Fedchenko, Olena; Chernov, Sergii; McCulloch, Andrew; Vielle-Grosjean, Mélissa; Comparat, Daniel; Schönhense, Gerd

    2017-07-01

    Pulsed photoionization of laser-cooled atoms in a magneto-optical trap (MOT) has the potential to create cold electron beams of few meV bandwidths and few ps pulse lengths. Such a source would be highly attractive for the study of fast low-energy processes like coherent phonon excitation. To study the suitability of MOT-based sources for the production of simultaneously cold and fast electrons, we study the photoionization dynamics of trapped Cs atoms. A momentum-microscope-like setup with a delay-line detector allows for the simultaneous measurement of spatial and temporal electron distributions. The measured patterns are complex, due to the Lorentz force inducing spiral trajectories. Ray-tracing simulations reproduce the main features. We find that the production of electron bunches with bandwidths of a few meV is straightforward; however, pulses in the ps-range are more demanding and require beam blanking or partial blocking.

  13. Electron-impact-ionization dynamics of S F6

    Science.gov (United States)

    Bull, James N.; Lee, Jason W. L.; Vallance, Claire

    2017-10-01

    A detailed understanding of the dissociative electron ionization dynamics of S F6 is important in the modeling and tuning of dry-etching plasmas used in the semiconductor manufacture industry. This paper reports a crossed-beam electron ionization velocity-map imaging study on the dissociative ionization of cold S F6 molecules, providing complete, unbiased kinetic energy distributions for all significant product ions. Analysis of these distributions suggests that fragmentation following single ionization proceeds via formation of S F5 + or S F3 + ions that then dissociate in a statistical manner through loss of F atoms or F2, until most internal energy has been liberated. Similarly, formation of stable dications is consistent with initial formation of S F4 2 + ions, which then dissociate on a longer time scale. These data allow a comparison between electron ionization and photoionization dynamics, revealing similar dynamical behavior. In parallel with the ion kinetic energy distributions, the velocity-map imaging approach provides a set of partial ionization cross sections for all detected ionic fragments over an electron energy range of 50-100 eV, providing partial cross sections for S2 +, and enables the cross sections for S F4 2 + from S F+ to be resolved.

  14. Dissipation and energy balance in electronic dynamics of Na clusters

    Science.gov (United States)

    Vincendon, Marc; Suraud, Eric; Reinhard, Paul-Gerhard

    2017-06-01

    We investigate the impact of dissipation on the energy balance in the electron dynamics of metal clusters excited by strong electro-magnetic pulses. The dynamics is described theoretically by Time-Dependent Density-Functional Theory (TDDFT) at the level of Local Density Approximation (LDA) augmented by a self interaction correction term and a quantum collision term in Relaxation-Time Approximation (RTA). We evaluate the separate contributions to the total excitation energy, namely energy exported by electron emission, potential energy due to changing charge state, intrinsic kinetic and potential energy, and collective flow energy. The balance of these energies is studied as function of the laser parameters (frequency, intensity, pulse length) and as function of system size and charge. We also look at collisions with a highly charged ion and here at the dependence on the impact parameter (close versus distant collisions). Dissipation turns out to be small where direct electron emission prevails namely for laser frequencies above any ionization threshold and for slow electron extraction in distant collisions. Dissipation is large for fast collisions and at low laser frequencies, particularly at resonances. Contribution to the Topical Issue "Dynamics of Systems at the Nanoscale", edited by Andrey Solov'yov and Andrei Korol.

  15. Ultrafast studies of electron dynamics at metal-dielectric interfaces

    Energy Technology Data Exchange (ETDEWEB)

    Ge, Nien-Hui [Univ. of California, Berkeley, CA (United States)

    1998-10-01

    Femtosecond time- and angle-resolved two-photon photoemission spectroscopy has been used to study fundamental aspects of excited electron dynamics at metal-dielectric interfaces, including layer-by-layer evolution of electronic structure and two-dimensional electron localization. On bare Ag(111), the lifetimes of image states are dominated by their position with respect to the projected bulk band structure. The n = 2 state has a shorter lifetime than the n = 1 state due to degeneracy with the bulk conduction band. As the parallel momentum of the n = 1 image electron increases, the lifetime decreases. With decreasing temperatures, the n = 1 image electrons, with zero or nonzero parallel momentum, all become longer lived. Adsorption of one to three layers of n-heptane results in an approximately exponential increase in lifetime as a function of layer thickness. This results from the formation of a tunneling barrier through which the interfacial electrons must decay, consistent with the repulsive bulk electron affinity of n-alkanes. The lifetimes of the higher quantum states indicate that the presence of the monolayer significantly reduces coupling of the image states to the bulk band structure. These results are compared with predictions of a dielectric continuum model. The study of electron lateral motion shows that optical excitation creates interfacial electrons in quasifree states for motion parallel to the n-heptane/Ag(111) interface. These initially delocalized electrons decay into a localized state within a few hundred femtoseconds. The localized electrons then decay back to the metal by tunneling through the adlayer potential barrier. The localization time depends strongly on the electron's initial parallel momentum and exhibits a non-Arrhenius temperature dependence. The experimental findings are consistent with a 2-D self-trapping process in which electrons become localized by interacting with the topmost plane of the alkane layer. The energy

  16. Dynamics of two-electron excitations in helium

    Energy Technology Data Exchange (ETDEWEB)

    Caldwell, C.D.; Menzel, A.; Frigo, S.P. [Univ. of Central Florida, Orlando, FL (United States)] [and others

    1997-04-01

    Excitation of both electrons in helium offers a unique window for studying electron correlation at the most basic level in an atom in which these two electrons and the nucleus form a three-body system. The authors utilized the first light available at the U-8 undulator-SGM monochromator beamline to investigate the dynamic parameters, partial cross sections, differential cross sections, and photoelectron angular distribution parameters ({beta}), with a high resolving power for the photon beam and at the highly differential level afforded by the use of their electron spectrometer. In parallel, they carried out detailed calculations of the relevant properties by a theoretical approach that is based on the hyperspherical close-coupling method. Partial photoionization cross sections {sigma}{sub n}, and photoelectron angular distributions {beta}{sub n} were measured for all possible final ionic states He{sup +}(n) in the region of the double excitations N(K,T){sup A} up to the N=5 threshold. At a photon energy bandpass of 12 meV below the thresholds N=3, 4, and 5, this level of differentiation offers the most critical assessment of the dynamics of the two-electron excitations to date. The experimental data were seen to be very well described by the most advanced theoretical calculations.

  17. Reaction dynamics of electronically excited alkali atoms with simple molecules

    Energy Technology Data Exchange (ETDEWEB)

    Weiss, P.S.; Mestdagh, J.; Schmidt, H.; Vernon, M.F. Covinsky, M.H.; Balko, B.A.; Lee, Y.T.

    1985-09-01

    The reactions of electronically excited sodium atoms with simple molecules have been studied in crossed molecular beams experiments. Electronically excited Na(3/sup 2/P/sub 3/2/,4/sup 2/D/sub 5/2/, and 5/sup 2/S/sub 1/2) were produced by optical pumping using single frequency dye lasers. The effects of the symmetry, and the orientation and alignment of the excited orbital on the chemical reactivity, and detailed information on the reaction dynamics were derived from measurements of the product angular and velocity distributions.

  18. Reaction dynamics of electronically excited alkali atoms with simpler molecules

    Science.gov (United States)

    Weiss, P. S.; Mestdagh, J. M.; Schmidt, H.; Vernon, M. F.; Covinsky, M. H.; Balko, B. A.; Lee, Y. T.

    1985-05-01

    The reactions of electronically excited sodium atoms with simple molecules have been studied in crossed molecular beams experiments. Electronically excited Na(3(2)P(sub 3/2), 4(2)D(sub 5/2), and 5(2)S(sub 1/2) were produced by optical pumping using single frequency dye lasers. The effects of the symmetry, and the orientation and alignment of the excited orbital on the chemical reactivity, and detailed information on the reaction dynamics were derived from measurements of the product angular and velocity distributions.

  19. Electron spin dynamics due to hyperfine coupling in quantum dots

    Science.gov (United States)

    Woods, L. M.; Reinecke, T. L.; Rajagopal, A. K.

    2008-02-01

    The dynamics of spins in semiconductor quantum dots often is controlled by their hyperfine coupling to nuclear spins. We develop a straightforward and efficient approach to describe the dynamics and the effective decoherence of the electron spins due to hyperfine coupling in realistic quantum dots. Systems with a large number of nuclei and an arbitrary initial nuclear polarization for which the number of nuclei initially flipped over is much less than the total number of nuclei are treated. This treatment employs a pole approximation within a Schrödinger equation of motion for the state of the coupled electron and nuclear spin system, and it allows us to treat systems with arbitrary initial conditions. We find that typical time scales for the effective spin decoherence are on the order of tens of microseconds.

  20. Electron bremstrahlung recovery in ATLAS tracking using Dynamic Noise Adjustment

    CERN Document Server

    Kartvelishvili, V

    2007-01-01

    A number of approaches are being used in ATLAS reconstruction software, aiming to improve electron momentum measurement by taking into account the effects due to bremsstrahlung at various stages. One of them, designed and implemented in ATLAS, is covered in this talk. The method applies Dynamic Noise Adjustment (DNA) during the track fitting process based on the Kalman filter, and is both fast and efficient

  1. Electron dynamics during substorm dipolarization in Mercury's magnetosphere

    Directory of Open Access Journals (Sweden)

    D. C. Delcourt

    2005-11-01

    Full Text Available We examine the nonlinear dynamics of electrons during the expansion phase of substorms at Mercury using test particle simulations. A simple model of magnetic field line dipolarization is designed by rescaling a magnetic field model of the Earth's magnetosphere. The results of the simulations demonstrate that electrons may be subjected to significant energization on the time scale (several seconds of the magnetic field reconfiguration. In a similar manner to ions in the near-Earth's magnetosphere, it is shown that low-energy (up to several tens of eV electrons may not conserve the second adiabatic invariant during dipolarization, which leads to clusters of bouncing particles in the innermost magnetotail. On the other hand, it is found that, because of the stretching of the magnetic field lines, high-energy electrons (several keVs and above do not behave adiabatically and possibly experience meandering (Speiser-type motion around the midplane. We show that dipolarization of the magnetic field lines may be responsible for significant, though transient, (a few seconds precipitation of energetic (several keVs electrons onto the planet's surface. Prominent injections of energetic trapped electrons toward the planet are also obtained as a result of dipolarization. These injections, however, do not exhibit short-lived temporal modulations, as observed by Mariner-10, which thus appear to follow from a different mechanism than a simple convection surge.

  2. Consideration of Relativistic Dynamics in High-Energy Electron Coolers

    CERN Document Server

    Bruhwiler, David L

    2005-01-01

    A proposed electron cooler for RHIC would use ~55 MeV electrons to cool fully-ionized 100 GeV/nucleon gold ions.* At two locations in the collider ring, the electrons and ions will co-propagate for ~13 m, with velocities close to c and gamma>100. To lowest-order, one can Lorentz transform all physical quantities into the beam frame and calculate the dynamical friction forces assuming a nonrelativisitc, electrostatic plasma. However, we show that nonlinear space charge forces of the bunched electron beam on the ions must be calculated relativistically, because an electrostatic beam-frame calculation is not valid for such short interaction times. The validity of nonrelativistic friction force calculations must also be considered. Further, the transverse thermal velocities of the high-charge (~20 nC) electron bunch are large enough that some electrons have marginally relativistic velocities, even in the beam frame. Hence, we consider relativistic binary collisions – treating the model problem of ...

  3. Simulation of electron beam dynamics in a high-energy electron cooler

    Energy Technology Data Exchange (ETDEWEB)

    Ivanov, A.V. [BINP, Acad.Lavrentiev, 11, BudkerINP, Novosibirsk, 630090 (Russian Federation)]. E-mail: a.v.ivanov@inp.nsk.su; Panasyuk, V.M. [BINP, Acad.Lavrentiev, 11, BudkerINP, Novosibirsk, 630090 (Russian Federation); Parkhomchuk, V.V. [BINP, Acad.Lavrentiev, 11, BudkerINP, Novosibirsk, 630090 (Russian Federation); Reva, V.B. [BINP, Acad.Lavrentiev, 11, BudkerINP, Novosibirsk, 630090 (Russian Federation); Tiunov, M.A. [BINP, Acad.Lavrentiev, 11, BudkerINP, Novosibirsk, 630090 (Russian Federation)

    2006-03-01

    Electron cooling is now a standard tool for improvement of ion beam parameters in storage rings. In BINP, after successful development of several low-energy electron cooling devices, a project involving a high-energy electron cooler for GSI has been proposed. This cooler has a classical electrostatic scheme with electron energy of up to 8 MeV. Here we present results of numerical simulations of electron beam formation, acceleration and collection for this project. Special attention is paid to a description of the new codes developed in BINP. The electron gun and collector are simulated by the 2D USAM code. This code is modified to calculate collector performance with consideration of secondary emission. The BEAM code is used for simulation of dynamics in the accelerating section. A new 3D electrostatic code, ELEC3D, developed for the simulation of beam dynamics in bends with electrostatic compensation of the centrifugal drift, is described. This code is combined with the existing MAG3D magnetostatic code to provide a universal tool for 3D static calculations.

  4. The Delicate Balance of Static and Dynamic Electron Correlation

    CERN Document Server

    Stein, Christopher J; Reiher, Markus

    2016-01-01

    Multi-configurational approaches yield universal wave function parameterizations that can qualitatively well describe electronic structures along reaction pathways. For quantitative results, multi-reference perturbation theory is required to capture dynamic electron correlation from the otherwise neglected virtual orbitals. Still, the overall accuracy suffers from the finite size and choice of the active orbital space and peculiarities of the perturbation theory. Fortunately, the electronic wave functions at equilibrium structures of reactants and products can often be well described by single-reference methods and hence are accessible to accurate coupled cluster calculations. Here, we calculate the heterolytic double dissociation energy of four 3d-metallocenes with the complete active space self-consistent field method and compare to highly accurate coupled cluster data. Our coupled cluster data are well within the experimental error bars. This accuracy can also be approached by complete active space calcula...

  5. Time Resolved Phase Transitions via Dynamic Transmission Electron Microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Reed, B W; Armstrong, M R; Blobaum, K J; Browning, N D; Burnham, A K; Campbell, G H; Gee, R; Kim, J S; King, W E; Maiti, A; Piggott, W T; Torralva, B R

    2007-02-22

    The Dynamic Transmission Electron Microscope (DTEM) project is developing an in situ electron microscope with nanometer- and nanosecond-scale resolution for the study of rapid laser-driven processes in materials. We report on the results obtained in a year-long LDRD-supported effort to develop DTEM techniques and results for phase transitions in molecular crystals, reactive multilayer foils, and melting and resolidification of bismuth. We report the first in situ TEM observation of the HMX {beta}-{delta} phase transformation in sub-{micro}m crystals, computational results suggesting the importance of voids and free surfaces in the HMX transformation kinetics, and the first electron diffraction patterns of intermediate states in fast multilayer foil reactions. This project developed techniques which are applicable to many materials systems and will continue to be employed within the larger DTEM effort.

  6. Delocalization of Electrons in Strong Insulators at High Dynamic Pressures

    Directory of Open Access Journals (Sweden)

    William J. Nellis

    2011-06-01

    Full Text Available Systematics of material responses to shock flows at high dynamic pressures are discussed. Dissipation in shock flows drives structural and electronic transitions or crossovers, such as used to synthesize metallic liquid hydrogen and most probably Al2O3 metallic glass. The term “metal” here means electrical conduction in a degenerate system, which occurs by band overlap in degenerate condensed matter, rather than by thermal ionization in a non-degenerate plasma. Since H2 and probably disordered Al2O3 become poor metals with minimum metallic conductivity (MMC virtually all insulators with intermediate strengths do so as well under dynamic compression. That is, the magnitude of strength determines the split between thermal energy and disorder, which determines material response. These crossovers occur via a transition from insulators with electrons localized in chemical bonds to poor metals with electron energy bands. For example, radial extents of outermost electrons of Al and O atoms are 7 a0 and 4 a0, respectively, much greater than 1.7 a0 needed for onset of hybridization at 300 GPa. All such insulators are Mott insulators, provided the term “correlated electrons” includes chemical bonds.

  7. Structure, dynamics, and reactivity of hydrated electrons by ab initio molecular dynamics.

    Science.gov (United States)

    Marsalek, Ondrej; Uhlig, Frank; VandeVondele, Joost; Jungwirth, Pavel

    2012-01-17

    Understanding the properties of hydrated electrons, which were first observed using pulse radiolysis of water in 1962, is crucial because they are key species in many radiation chemistry processes. Although time-resolved spectroscopic studies and molecular simulations have shown that an electron in water (prepared, for example, by water photoionization) relaxes quickly to a localized, cavity-like structure ∼2.5 Å in radius, this picture has recently been questioned. In another experimental approach, negatively charged water clusters of increasing size were studied with photoelectron and IR spectroscopies. Although small water clusters can bind an excess electron, their character is very different from bulk hydrated species. As data on electron binding in liquid water have become directly accessible experimentally, the cluster-to-bulk extrapolations have become a topic of lively debate. Quantum electronic structure calculations addressing experimental measurables have, until recently, been largely limited to small clusters; extended systems were approached mainly with pseudopotential calculations combining a classical description of water with a quantum mechanical treatment of the excess electron. In this Account, we discuss our investigations of electrons solvated in water by means of ab initio molecular dynamics simulations. This approach, applied to a model system of a negatively charged cluster of 32 water molecules, allows us to characterize structural, dynamical, and reactive aspects of the hydrated electron using all of the system's valence electrons. We show that under ambient conditions, the electron localizes into a cavity close to the surface of the liquid cluster. This cavity is, however, more flexible and accessible to water molecules than an analogous area around negatively charged ions. The dynamical process of electron attachment to a neutral water cluster is strongly temperature dependent. Under ambient conditions, the electron relaxes in the

  8. Laser-induced electron diffraction for dynamic imaging of molecules

    Science.gov (United States)

    Lin, Chii-Dong

    2017-04-01

    Electron diffraction is the well-established tool for probing the structure of gas-phase molecules near the equilibrium geometry. To study chemical dynamics ultrashort electron pulses below a few tens of femtoseconds are needed. Laser-induced electron diffraction (LIED) is a method where molecules can be probed with femtosecond temporal resolution and sub-angstrom spatial resolution. In LIED, molecules are exposed to an intense femtosecond laser pulse. The electrons that have been previously removed by the laser field can be driven back later to rescatter with the parent molecular ion. Using diffraction images from large-angle backscattered events, sub-angstrom spatial resolution can be achieved with tens to hundreds eV electrons. Recent LIED experimental results showing bond breaking in molecules will be illustrated. Practical issues related to the retrieval of diffraction images from LIED on aligned molecules and possibilities of real-time imaging of dissociating molecules using LIED will be presented. US Department of Energy. This work is performed in collaboration with Anh Thu Le (Kansas State University) and the experimental group of Jens Biegert (ICFO, Barcelona).

  9. Pulsed Power for a Dynamic Transmission Electron Microscope

    Energy Technology Data Exchange (ETDEWEB)

    dehope, w j; browning, n; campbell, g; cook, e; king, w; lagrange, t; reed, b; stuart, b; Shuttlesworth, R; Pyke, B

    2009-06-25

    Lawrence Livermore National Laboratory (LLNL) has converted a commercial 200kV transmission electron microscope (TEM) into an ultrafast, nanoscale diagnostic tool for material science studies. The resulting Dynamic Transmission Electron Microscope (DTEM) has provided a unique tool for the study of material phase transitions, reaction front analyses, and other studies in the fields of chemistry, materials science, and biology. The TEM's thermionic electron emission source was replaced with a fast photocathode and a laser beam path was provided for ultraviolet surface illumination. The resulting photoelectron beam gives downstream images of 2 and 20 ns exposure times at 100 and 10 nm spatial resolution. A separate laser, used as a pump pulse, is used to heat, ignite, or shock samples while the photocathode electron pulses, carefully time-synchronized with the pump, function as probe in fast transient studies. The device functions in both imaging and diffraction modes. A laser upgrade is underway to make arbitrary cathode pulse trains of variable pulse width of 10-1000 ns. Along with a fast e-beam deflection scheme, a 'movie mode' capability will be added to this unique diagnostic tool. This talk will review conventional electron microscopy and its limitations, discuss the development and capabilities of DTEM, in particularly addressing the prime and pulsed power considerations in the design and fabrication of the DTEM, and conclude with the presentation of a deflector and solid-state pulser design for Movie-Mode DTEM.

  10. Complex formation dynamics in a single-molecule electronic device.

    Science.gov (United States)

    Wen, Huimin; Li, Wengang; Chen, Jiewei; He, Gen; Li, Longhua; Olson, Mark A; Sue, Andrew C-H; Stoddart, J Fraser; Guo, Xuefeng

    2016-11-01

    Single-molecule electronic devices offer unique opportunities to investigate the properties of individual molecules that are not accessible in conventional ensemble experiments. However, these investigations remain challenging because they require (i) highly precise device fabrication to incorporate single molecules and (ii) sufficient time resolution to be able to make fast molecular dynamic measurements. We demonstrate a graphene-molecule single-molecule junction that is capable of probing the thermodynamic and kinetic parameters of a host-guest complex. By covalently integrating a conjugated molecular wire with a pendent crown ether into graphene point contacts, we can transduce the physical [2]pseudorotaxane (de)formation processes between the electron-rich crown ether and a dicationic guest into real-time electrical signals. The conductance of the single-molecule junction reveals two-level fluctuations that are highly dependent on temperature and solvent environments, affording a nondestructive means of quantitatively determining the binding and rate constants, as well as the activation energies, for host-guest complexes. The thermodynamic processes reveal the host-guest binding to be enthalpy-driven and are consistent with conventional 1 H nuclear magnetic resonance titration experiments. This electronic device opens up a new route to developing single-molecule dynamics investigations with microsecond resolution for a broad range of chemical and biochemical applications.

  11. Electron beam dynamics in an ultrafast transmission electron microscope with Wehnelt electrode

    Energy Technology Data Exchange (ETDEWEB)

    Bücker, K.; Picher, M.; Crégut, O. [Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504 CNRS, Université de Strasbourg, 23 rue du Loess, 67034 Strasbourg (France); LaGrange, T. [Interdisciplinary Centre for Electron Microscopy, École Polytechnique Fédérale de Lausanne, 1015 Lausanne (Switzerland); Reed, B.W.; Park, S.T.; Masiel, D.J. [Integrated Dynamic Electron Solutions, Inc., 5653 Stoneridge Drive 117, Pleasanton, CA 94588 (United States); Banhart, F., E-mail: florian.banhart@ipcms.unistra.fr [Institut de Physique et Chimie des Matériaux de Strasbourg, UMR 7504 CNRS, Université de Strasbourg, 23 rue du Loess, 67034 Strasbourg (France)

    2016-12-15

    High temporal resolution transmission electron microscopy techniques have shown significant progress in recent years. Using photoelectron pulses induced by ultrashort laser pulses on the cathode, these methods can probe ultrafast materials processes and have revealed numerous dynamic phenomena at the nanoscale. Most recently, the technique has been implemented in standard thermionic electron microscopes that provide a flexible platform for studying material's dynamics over a wide range of spatial and temporal scales. In this study, the electron pulses in such an ultrafast transmission electron microscope are characterized in detail. The microscope is based on a thermionic gun with a Wehnelt electrode and is operated in a stroboscopic photoelectron mode. It is shown that the Wehnelt bias has a decisive influence on the temporal and energy spread of the picosecond electron pulses. Depending on the shape of the cathode and the cathode-Wehnelt distance, different emission patterns with different pulse parameters are obtained. The energy spread of the pulses is determined by space charge and Boersch effects, given by the number of electrons in a pulse. However, filtering effects due to the chromatic aberrations of the Wehnelt electrode allow the extraction of pulses with narrow energy spreads. The temporal spread is governed by electron trajectories of different length and in different electrostatic potentials. High temporal resolution is obtained by excluding shank emission from the cathode and aberration-induced halos in the emission pattern. By varying the cathode-Wehnelt gap, the Wehnelt bias, and the number of photoelectrons in a pulse, tradeoffs between energy and temporal resolution as well as beam intensity can be made as needed for experiments. Based on the characterization of the electron pulses, the optimal conditions for the operation of ultrafast TEMs with thermionic gun assembly are elaborated. - Highlights: • A detailed characterization of electron

  12. Modern aspects of Josephson dynamics and superconductivity electronics

    CERN Document Server

    Askerzade, Iman; Cantürk, Mehmet

    2017-01-01

    In this book new experimental investigations of properties of Josephson junctions and systems are explored with the help of recent developments in superconductivity. The theory of the Josephson effect is presented taking into account the influence of multiband and anisotropy effects in new superconducting compounds. Anharmonicity effects in current-phase relation on Josephson junctions dynamics are discussed. Recent studies in analogue and digital superconductivity electronics are presented. Topics of special interest include resistive single flux quantum logic in digital electronics. Application of Josephson junctions in quantum computing as superconducting quantum bits are analyzed. Particular attention is given to understanding chaotic behaviour of Josephson junctions and systems. The book is written for graduate students and researchers in the field of applied superconductivity.

  13. Electron dynamics in RF sources with a laser controlled emission

    CERN Document Server

    Khodak, I V; Metrochenko, V V

    2001-01-01

    Photoemission radiofrequency (RF) electron sources are sources of electron beams with extremely high brightness. Beam bunching processes in such devices are well studied in case when laser pulse duration is much lower of rf oscillation period.At the same time photoemission RF guns have some merits when operating in 'long-pulse' mode. In this case the laser pulse duration is much higher of rf oscillation period but much lower of rise time of oscillations in a gun cavity. Beam parameters at the gun output are compared for photoemission and thermoemission cathode applications. The paper presents results of a beam dynamics simulation in such guns with different resonance structures. Questions connected with defining of the current pulse peak value that can be obtained in such guns are discussed.

  14. Electron density and plasma dynamics of a colliding plasma experiment

    Energy Technology Data Exchange (ETDEWEB)

    Wiechula, J., E-mail: wiechula@physik.uni-frankfurt.de; Schönlein, A.; Iberler, M.; Hock, C.; Manegold, T.; Bohlender, B.; Jacoby, J. [Plasma Physics Group, Institute of Applied Physics, Goethe University, 60438 Frankfurt am Main (Germany)

    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 of 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.

  15. Machine Learning of Dynamic Electron Correlation Energies from Topological Atoms.

    Science.gov (United States)

    McDonagh, James L; Silva, Arnaldo F; Vincent, Mark A; Popelier, Paul L A

    2017-12-06

    We present an innovative method for predicting the dynamic electron correlation energy of an atom or a bond in a molecule utilizing topological atoms. Our approach uses the machine learning method Kriging (Gaussian Process Regression with a non-zero mean function) to predict these dynamic electron correlation energy contributions. The true energy values are calculated by partitioning the MP2 two-particle density-matrix via the Interacting Quantum Atoms (IQA) procedure. To our knowledge, this is the first time such energies have been predicted by a machine learning technique. We present here three important proof-of-concept cases: the water monomer, the water dimer, and the van der Waals complex H2···He. These cases represent the final step toward the design of a full IQA potential for molecular simulation. This final piece will enable us to consider situations in which dispersion is the dominant intermolecular interaction. The results from these examples suggest a new method by which dispersion potentials for molecular simulation can be generated.

  16. Dynamic Electronic Junctions in Organic-Inorganic Hybrid Perovskites.

    Science.gov (United States)

    Wang, Xi; Ling, Yichuan; Chiu, Yu-Che; Du, Yijun; Barreda, Jorge Luis; Perez-Orive, Fernando; Ma, Biwu; Xiong, Peng; Gao, Hanwei

    2017-08-09

    Organic-inorganic hybrid perovskites have shown great potential as building blocks for low-cost optoelectronics for their exceptional optical and electrical properties. Despite the remarkable progress in device demonstration, fundamental understanding of the physical processes in halide perovskites remains limited, especially the unusual electronic behaviors such as the current-voltage hysteresis and the switchable photovoltaic effect. These phenomena are of particular interests for being closely related to device functionalities and performance. In this work, a microscopic picture of electric fields in halide perovskite thin films was obtained using scanning laser microscopy. Unlike conventional semiconductors, distribution of the built-in electric fields in the halide perovskite evolves dynamically under the stimulation of external biases. The observations can be well explained using a model based on field-assisted ion migration, indicating that the mechanism responsible for the evolving charge transport observed in this material is not purely electronic. The anomalous dynamic responses to the applied bias are found to be effectively suppressed by operating the devices at reduced temperature or processing the materials at elevated temperature, which provide potential strategies for designing and creating halide perovskites with more stable charge transport properties in the development of viable perovskite-based optoelectronics.

  17. Femtosecond electron-bunch dynamics in laser wakefields and vacuum

    Directory of Open Access Journals (Sweden)

    A. G. Khachatryan

    2007-12-01

    Full Text Available Recent advances in laser wakefield acceleration demonstrated the generation of extremely short (with a duration of a few femtoseconds relativistic electron bunches with relatively low (of the order of couple of percent energy spread. In this article we study the dynamics of such bunches in drift space (vacuum and in channel-guided laser wakefields. Analytical solutions were found for the transverse coordinate of an electron and for the bunch envelope in the wakefield in the case of arbitrary change in the energy. Our results show strong bunch dynamics already on a millimeter scale propagation distance both in plasma and in vacuum. When the bunch propagates in vacuum, its transverse sizes grow considerably; the same is observed for the normalized bunch emittance that worsens the focusability of the bunch. A scheme of two-stage laser wakefield accelerator with small drift space between the stages is proposed. It is found that fast longitudinal betatron phase mixing occurs in a femtosecond bunch when it propagates along the wakefield axis. When bunch propagates off axis, strong bunch decoherence and fast emittance degradation due to the finite bunch length was observed.

  18. Femtosecond electron diffraction. Next generation electron sources for atomically resolved dynamics

    Energy Technology Data Exchange (ETDEWEB)

    Hirscht, Julian

    2015-08-15

    Three instruments for femtosecond electron diffraction (FED) experiments were erected, partially commissioned and used for first diffraction experiments. The Relativistic Electron Gun for Atomic Exploration (REGAE) was completed by beamline elements including supports, a specimen chamber and dark current or electron beam collimating elements such that the commissioning process, including first diffraction experiments in this context, could be started. The temporal resolution of this machine is simulated to be 25 fs (fwhm) short, while a transverse coherence length of 30 nm (fwhm) is feasible to resolve proteins on this scale. Whether this machine is capable of meeting these predictions or whether the dynamics of the electron beam will stay limited by accelerator components, is not finally determined by the end of this work, because commissioning and improvement of accelerator components is ongoing. Simultaneously, a compact DC electron diffraction apparatus, the E-Gun 300, designed for solid and liquid specimens and a target electron energy of 300 keV, was built. Fundamental design issues of the high potential carrying and beam generating components occurred and are limiting the maximum potential and electron energy to 120 keV. Furthermore, this is limiting the range of possible applications and consequently the design and construction of a brand new instrument began. The Femtosecond Electron Diffraction CAmera for Molecular Movies (FED-CAMM) bridges the performance problems of very high electric potentials and provides optimal operational conditions for all applied electron energies up to 300 keV. The variability of gap spacings and optimized manufacturing of the high voltage electrodes lead to the best possible electron pulse durations obtainable with a compact DC setup, that does not comprise of rf-structures. This third apparatus possesses pulse durations just a few tenth femtoseconds apart from the design limit of the highly relativistic REGAE and combines the

  19. Slow dynamics of electron glasses: The role of disorder

    Science.gov (United States)

    Ovadyahu, Z.

    2017-04-01

    We examine in this work the role of disorder in contributing to the sluggish relaxation observed in intrinsic electron glasses. Our approach is guided by several empirical observations: First and foremost, Anderson localization is a pre-requisite for observing these nonequilibrium phenomena. Secondly, sluggish relaxation appears to favor Anderson insulators with relatively large Fermi energies (hence proportionally large disorder). These observations motivated us to consider a way to measure the underlying disorder in a realistic Anderson insulator. Optical studies using a series of amorphous indium oxide (InxO ) establish a simple connection between carrier concentration and the disorder necessary to approach the metal-insulator transition from the insulating side. This is used to estimate the typical magnitude of the quenched potential fluctuation in the electron-glass phase of this system. The implications of our findings on the slow dynamics of Anderson insulators are discussed. In particular, the reason for the absence of a memory dip and the accompanying electron-glass effects in lightly-doped semiconductors emerges as a natural consequence of their weak disorder.

  20. Organic (opto)electronic materials: understanding charge carrier dynamics

    Science.gov (United States)

    Ostroverkhova, Oksana

    2008-05-01

    There is growing interest in using organic (opto)electronic materials for applications in electronics and photonics. In particular, organic semiconductor thin films offer several advantages over traditional silicon technology, including low-cost processing, the potential for large-area flexible devices, high-efficiency light emission, and widely tunable properties through functionalization of the molecules. Over the past decade, remarkable progress in materials design and purification has been made, which led to applications of organic semiconductors in light-emitting diodes, polymer lasers, photovoltaic cells, high-speed photodetectors, organic thin-film transistors, and many others. Most of the applications envisioned for organic semiconductors rely on their conductive or photoconductive properties. However, despite remarkable progress in organic electronics and photonics, the nature of charge carrier photogeneration and transport in organic semiconductors is not completely understood and remains controversial, partly due to difficulties in assessing intrinsic properties that are often masked by impurities, grain boundaries, etc. Measurements of charge carrier dynamics at picosecond time scales after excitation reveal the intrinsic nature of mobile charge carriers before they are trapped at defect sites. In this presentation, I will review the current state of the field and summarize our recent results on photoconductivity of novel high-performance organic semiconductors (such as functionalized pentacene and anthradithiophene thin films) from picoseconds to seconds after photoexcitation. Photoluminescent properties of these novel materials will also be discussed.

  1. Spin dynamics of equilibrium electrons in gallium arsenide

    Energy Technology Data Exchange (ETDEWEB)

    Mueller, Georg Martin

    2010-12-08

    In this dissertation, spin noise spectroscopy is applied to study spin dynamics in GaAs based semiconductor structures close to thermal equilibrium. Semiconductor spin noise spectroscopy measures the stochastic spin polarization of the electron ensemble via off-resonant Faraday rotation. Correspondingly, no energy has to be deposited in the sample system contrary to other experimental techniques, in which the dephasing or the depolarization of an artificially injected spin polarization is measured. Since the spin fluctuations are measured in real-time, spin noise spectroscopy had been hitherto limited to frequencies below 1 GHz. This thesis introduces the experimental advancement of ultrafast spin noise spectroscopy, in which the fluctuations are probed by pulsed light, and detection of spin noise at frequencies up to 16 GHz is demonstrated. These frequencies exceed the bandwidth of the photoreceiver by a factor of around 200. To further explore the limitations of the finite bandwidth of the detection system, electrical frequency mixing is applied for down-conversion of the electrical spin noise signal. Furthermore, spin noise measurements are simulated revealing that also ultrafast digitizers with low resolution can be utilized for spectral analysis in spin noise spectroscopy without any significant loss of sensitivity. The spin dynamics in a symmetrically grown, modulation-doped, (110)-oriented GaAs/AlGaAs multiple quantum well structure are investigated in this work. This experiment represents the first spin noise measurements on a semiconductor system of reduced effective dimensionality. The Dyakonov-Perel mechanism that usually dominates spin dephasing of free electrons in GaAs is ineffective in (110)-oriented structures for spins along the growth direction. Nevertheless, the correspondingly anticipated long spin dephasing times in (110) GaAs/AlGaAs quantum wells at low temperatures are not accessible with conventional experiments that rely on optical spin

  2. Dynamics of a nanodroplet under a transmission electron microscope

    Energy Technology Data Exchange (ETDEWEB)

    Leong, Fong Yew, E-mail: leongfy@ihpc.a-star.edu.sg [A-STAR Institute of High Performance Computing, 1 Fusionopolis Way, Connexis, Singapore 138632 (Singapore); Mirsaidov, Utkur M. [Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore 117551 (Singapore); Center for BioImaging Sciences, National University of Singapore, Science Drive 4, Singapore 117543 (Singapore); Matsudaira, Paul [Center for BioImaging Sciences, National University of Singapore, Science Drive 4, Singapore 117543 (Singapore); MechanoBiology Institute, National University of Singapore, 5A Engineering Drive 1, Singapore 117411 (Singapore); Department of Biological Sciences, National University of Singapore, 14 Science Drive 4, Singapore 117543 (Singapore); Singapore-MIT Alliance for Research and Technology Center, Science Drive 2, Singapore 117543 (Singapore); Mahadevan, L. [School of Engineering and Applied Sciences, Harvard University, Cambridge, Massachusetts 02138, USA and Department of Physics, Harvard University, Cambridge, Massachusetts 02138 (United States)

    2014-01-15

    We investigate the cyclical stick-slip motion of water nanodroplets on a hydrophilic substrate viewed with and stimulated by a transmission electron microscope. Using a continuum long wave theory, we show how the electrostatic stress imposed by non-uniform charge distribution causes a pinned convex drop to deform into a toroidal shape, with the shape characterized by the competition between the electrostatic stress and the surface tension of the drop, as well as the charge density distribution which follows a Poisson equation. A horizontal gradient in the charge density creates a lateral driving force, which when sufficiently large, overcomes the pinning induced by surface heterogeneities in the substrate disjoining pressure, causing the drop to slide on the substrate via a cyclical stick-slip motion. Our model predicts step-like dynamics in drop displacement and surface area jumps, qualitatively consistent with experimental observations.

  3. Surface electronic excitations and dynamic spectral properties of adsorbates

    Science.gov (United States)

    Gumhalter, B.

    Many-body aspects of screening and relaxation mechanisms encountered in spectroscopic studies of the electronic structure of adsorbates have recently attracted considerable attention from both experimental and theoretical physicists. Interest in these phenomena has also been augmented by the rapid improvement of experimental techniques which have enabled better resolution and analysis of various subtile components of the adsorbate spectra. Many of these spectral features have until recently been ascribed to purely chemical and initial state effects. One of the first major advances of the theoretical development in this field was to seek and attribute the origin of these structures to the many-body properties of adsorption systems and, secondly, to predict how the many-body effects would manifest themselves in surface spectroscopies. We start with a rather detailed description of the formalism of the surface electronic response and discuss the properties of the surface excitation spectrum of idealized and real metals. This formalism is then successively applied to set up a model of screening firstly in the nonbonding levels of mainly physisorbed adsorbates and later in the core and valence levels of chemisorbed species. Various modifications of the model enable a dynamic description of the final state relaxation and shake-up effects typical of spectroscopic measurements. To treat the particularly complicated problem of dynamic relaxation in the adsorbate valence levels a special perturbational approach based on Mayer's cluster expansion is developed in §5. The characteristics, and some limitations of this approach, which may also prove useful in other physical problems, are described in detail and discussed within the context of the interaction of localized adsorbate charge fluctuations with bosonic surface excitations. Experimental support for the presented theoretical framework and its applications has been very important. A qualitative comparison with the

  4. Electron dynamics in MoS2-graphite heterostructures.

    Science.gov (United States)

    Zhang, Xinwu; He, Dawei; Yi, Lixin; Zhao, Siqi; He, Jiaqi; Wang, Yongsheng; Zhao, Hui

    2017-10-05

    The electron dynamics in heterostructures formed by multilayer graphite and monolayer or bulk MoS2 were studied by femtosecond transient absorption measurements. Samples of monolayer MoS2-multilayer graphite and bulk MoS2-multilayer graphite were fabricated by exfoliation and dry transfer techniques. Ultrafast laser pulses were used to inject electron-hole pairs into monolayer or bulk MoS2. The transfer of these photocarriers to the adjacent multilayer graphite was time resolved by measuring the differential reflection of a probe pulse. We found that photocarriers injected into monolayer MoS2 transfer to graphite on an ultrafast time scale shorter than 400 fs. Such an efficient charge transfer is key to the development of high performance optoelectronic devices with MoS2 as the light absorbing layer and graphite as electrodes. The absorption coefficient of monolayer MoS2 can be controlled by the carriers in graphite. This process can be used for interlayer coupling and control. In a bulk MoS2-graphite heterostructure, the photocarrier transfer time is about 220 ps, due to the inefficient interlayer charge transport in bulk MoS2. These results provide useful information for developing optoelectronic devices based on MoS2-graphite heterostructures.

  5. Dynamic electronic institutions in agent oriented cloud robotic systems.

    Science.gov (United States)

    Nagrath, Vineet; Morel, Olivier; Malik, Aamir; Saad, Naufal; Meriaudeau, Fabrice

    2015-01-01

    The dot-com bubble bursted in the year 2000 followed by a swift movement towards resource virtualization and cloud computing business model. Cloud computing emerged not as new form of computing or network technology but a mere remoulding of existing technologies to suit a new business model. Cloud robotics is understood as adaptation of cloud computing ideas for robotic applications. Current efforts in cloud robotics stress upon developing robots that utilize computing and service infrastructure of the cloud, without debating on the underlying business model. HTM5 is an OMG's MDA based Meta-model for agent oriented development of cloud robotic systems. The trade-view of HTM5 promotes peer-to-peer trade amongst software agents. HTM5 agents represent various cloud entities and implement their business logic on cloud interactions. Trade in a peer-to-peer cloud robotic system is based on relationships and contracts amongst several agent subsets. Electronic Institutions are associations of heterogeneous intelligent agents which interact with each other following predefined norms. In Dynamic Electronic Institutions, the process of formation, reformation and dissolution of institutions is automated leading to run time adaptations in groups of agents. DEIs in agent oriented cloud robotic ecosystems bring order and group intellect. This article presents DEI implementations through HTM5 methodology.

  6. Electron momentum spectroscopy of dimethyl ether taking account of nuclear dynamics in the electronic ground state

    Science.gov (United States)

    Morini, Filippo; Watanabe, Noboru; Kojima, Masataka; Deleuze, Michael Simon; Takahashi, Masahiko

    2015-10-01

    The influence of nuclear dynamics in the electronic ground state on the (e,2e) momentum profiles of dimethyl ether has been analyzed using the harmonic analytical quantum mechanical and Born-Oppenheimer molecular dynamics approaches. In spite of fundamental methodological differences, results obtained with both approaches consistently demonstrate that molecular vibrations in the electronic ground state have a most appreciable influence on the momentum profiles associated to the 2b1, 6a1, 4b2, and 1a2 orbitals. Taking this influence into account considerably improves the agreement between theoretical and newly obtained experimental momentum profiles, with improved statistical accuracy. Both approaches point out in particular the most appreciable role which is played by a few specific molecular vibrations of A1, B1, and B2 symmetries, which correspond to C-H stretching and H-C-H bending modes. In line with the Herzberg-Teller principle, the influence of these molecular vibrations on the computed momentum profiles can be unraveled from considerations on the symmetry characteristics of orbitals and their energy spacing.

  7. Invisible Electronic States and Their Dynamics Revealed by Perturbations

    Science.gov (United States)

    Merer, Anthony J.

    2011-06-01

    Sooner or later everyone working in the field of spectroscopy encounters perturbations. These can range in size from a small shift of a single rotational level to total destruction of the vibrational and rotational patterns of an electronic state. To some workers perturbations are a source of terror, but to others they are the most fascinating features of molecular spectra, because they give information about molecular dynamics, and about states that would otherwise be invisible as a result of unfavorable selection rules. An example of the latter is the essentially complete characterization of the tilde{b}^3A_2 state of SO_2 from the vibronic perturbations it causes in the tilde{a}^3B_1 state. The S_1-trans state of acetylene is a beautiful example of dynamics in action. The level patterns of the three bending vibrations change dramatically with increasing vibrational excitation as a result of the vibrational angular momentum and the approach to the isomerization barrier. Several vibrational levels of the S_1-cis isomer, previously thought to be unobservable, can now be assigned. They obtain their intensity through interactions with nearby levels of the trans isomer.

  8. Magnetic dynamics studied by high-resolution electron spectroscopy and time-resolved electron microscopy

    Science.gov (United States)

    Jayaraman, Rajeswari

    Future information technology requires an increased magnetically encoded data density and novel electromagnetic modes of data transfer. While to date magnetic properties are observed and characterized mostly statically, the need emerges to monitor and capture their fast dynamics. In this talk, I will focus on the spin dynamics i.e. spin wave excitations and the dynamics of a new topological distribution of spins termed ``skyrmions''. Wave packets of spin waves offer the unique capability to transport a quantum bit, the spin, without the transport of charge or mass. Here, large wave-vector spin waves are of particular interest as they admit spin localization within a few nanometers. By using our recently developed electron energy loss spectrometer, we could study such spin waves in ultrathin films with an unprecedented energy resolution of 4 meV. By virtue of the finite penetration depth of low energy electrons, spin waves localized at interfaces between a substrate and a thin capping layer can be been studied yielding information about the exchange coupling between atoms at the interface. The quantization of spin waves with wave vectors perpendicular to the film gives rise to standing modes to which EELS has likewise access. Such studies when carried out as function of the film thickness again yield information on the layer dependence of the exchange coupling. Magnetic skyrmions are promising candidates as information carriers in logic or storage devices. Currently, little is known about the influence of disorder, defects, or external stimuli on the spatial distribution and temporal evolution of the skyrmion lattice. In this talk, I will describe the dynamical role of disorder in a large and flat thin film of Cu2OSeO3, exhibiting a skyrmion phase in an insulating material. We image up to 70,000 skyrmions by means of cryo-Lorentz Transmission Electron Microscopy as a function of the applied magnetic field. In the skyrmion phase, dislocations are shown to cause the

  9. Electron cyclotron heating and supra-thermal electron dynamics in the TCV Tokamak

    Energy Technology Data Exchange (ETDEWEB)

    Gnesin, S.

    2011-10-15

    This thesis is concerned with the physics of supra-thermal electrons in thermonuclear, magnetically confined plasmas. Under a variety of conditions, in laboratory as well as space plasmas, the electron velocity distribution function is not in thermodynamic equilibrium owing to internal or external drives. Accordingly, the distribution function departs from the equilibrium Maxwellian, and in particular generally develops a high-energy tail. In tokamak plasmas, this occurs especially as a result of injection of high-power electromagnetic waves, used for heating and current drive, as well as a result of internal magnetohydrodynamic (MHD) instabilities. The physics of these phenomena is intimately tied to the properties and dynamics of this supra-thermal electron population. This motivates the development of instrumental apparatus to measure its properties as well as of numerical codes to simulate their dynamics. Both aspects are reflected in this thesis work, which features advanced instrumental development and experimental measurements as well as numerical modeling. The instrumental development consisted of the complete design of a spectroscopic and tomographic system of four multi-detector hard X-ray (HXR) cameras for the TCV tokamak. The goal is to measure bremsstrahlung emission from supra-thermal electrons with energies in the 10-300 keV range, with the ultimate aim of providing the first full tomographic reconstruction at these energies in a noncircular plasma. In particular, supra-thermal electrons are generated in TCV by a high-power electron cyclotron heating (ECH) system and are also observed in the presence of MHD events, such as sawtooth oscillations and disruptive instabilities. This diagnostic employs state-of-the-art solid-state detectors and is optimized for the tight space requirements of the TCV ports. It features a novel collimator concept that combines compactness and flexibility as well as full digital acquisition of the photon pulses, greatly

  10. Enhanced dynamic electron paramagnetic resonance imaging of in vivo physiology

    Science.gov (United States)

    Redler, Gage

    It is well established that low oxygen concentration (hypoxia) in tumors strongly affects their malignant state and resistance to therapy. The importance of tumor oxygenation status has led to increased interest in the development of robust oxygen imaging modalities. One such method is electron paramagnetic resonance imaging (EPRI). EPRI has provided a non-invasive, quantitative imaging modality with sensitivity deep in tissues, capable of investigating static oxygen concentration (pO2) in vivo and has helped to corroborate the correlation between chronic states of hypoxia and tumor malignancy. However, when studying the complicated physiology of a living animal, the situation tends to be inherently dynamic. It has been found that in certain tumor regions there may exist steady states of hypoxia, or chronic hypoxia, whereas in other regions there may exist transient states of hypoxia, or acute hypoxia. It has been postulated that the negative prognostic implications associated with hypoxic tumors may be amplified for acutely hypoxic tumors. However, controversial data and a current lack in methods with the capability to noninvasively image tumor pO2 in vivo with sufficient spatial, temporal, and pO 2 resolution preclude definitive conclusions on the relationships between the different forms of hypoxia and the differences in their clinical implications. A particularly promising oxygen imaging modality that can help to study both chronic and acute hypoxia and elucidate important physiological and clinical differences is rapid Dynamic EPRI. The focus of this work is the development of methods enabling Dynamic EPRI of in vivo physiology as well as its potential applications. This work describes methods which enhance various aspects of EPRI in order to establish a more robust Dynamic EPRI capable of noninvasively studying and quantifying acute hypoxia in vivo. These enhancements are achieved through improvements that span from methods for the acquisition of individual

  11. Time-resolved imaging of purely valence-electron dynamics during a chemical reaction

    DEFF Research Database (Denmark)

    Hockett, Paul; Bisgaard, Christer Z.; Clarkin, Owen J.

    2011-01-01

    the non-adiabatic photodissociation of carbon disulphide demonstrate how the purely electronic rearrangements of the valence electrons can be projected from inherently coupled electronic-vibrational dynamics. Combined with ongoing efforts in molecular frame alignment(20) and orientation(21,22), TRMFPADs...... offer the promise of directly imaging valence-electron dynamics during molecular processes without involving the use of strong, highly perturbing laser fields(23)....

  12. Complex dynamics in planar two-electron quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Schroeter, Sebastian Josef Arthur

    2013-06-25

    Quantum dots play an important role in a wide range of recent experimental and technological developments. In particular they are promising candidates for realisations of quantum bits and further applications in quantum information theory. The harmonically confined Hooke's atom model is experimentally verified and separates in centre-of-mass and relative coordinates. Findings that are contradictory to this separability call for an extension of the model, in particular changing the confinement potential. In order to study effects of an anharmonic confinement potential on spectral properties of planar two-electron quantum dots a sophisticated numerical approach is developed. Comparison between the Helium atom, Hooke's atom and an anharmonic potential model are undertaken in order to improve the description of quantum dots. Classical and quantum features of complexity and chaos are investigated and used to characterise the dynamics of the system to be mixed regular-chaotic. Influence of decoherence can be described by quantum fidelity, which measures the effect of a perturbation on the time evolution. The quantum fidelity of eigenstates of the system depends strongly on the properties of the perturbation. Several methods for solving the time-dependent Schrödinger equation are implemented and a high level of accuracy for long time evolutions is achieved. The concept of offset entanglement, the entanglement of harmonic models in the noninteracting limit, is introduced. This concept explains different questions raised in the literature for harmonic quantum dot models, recently. It shows that only in the groundstate the electrons are not entangled in the fermionic sense. The applicability, validity, and origin of Hund's first rule in general quantum dot models is further addressed. In fact Hund's first rule is only applicable, and in this case also valid, for one pair of singlet and triplet states in Hooke's atom. For more realistic models of two-electron

  13. Ring polymer molecular dynamics beyond the linear response regime: Excess electron injection and trapping in liquids.

    Science.gov (United States)

    Menzeleev, Artur R; Miller, Thomas F

    2010-01-21

    Ring polymer molecular dynamics (RPMD) is used to directly simulate the injection and relaxation of excess electrons into supercritical helium fluid and ambient liquid water. A method for modulating the initial energy of the excess electron in the RPMD model is presented and used to study both low-energy (cold) and high-energy (hot) electron injections. For cold injection into both solvents, the RPMD model recovers electronically adiabatic dynamics with the excess electron in its ground state, whereas for hot electron injection, the model predicts slower relaxation dynamics associated with electronic transitions between solvent cavities. The analysis of solvent dynamics during electron localization reveals the formation of an outgoing solvent compression wave in helium that travels for over 2 nm and the delayed formation of water solvation shells on the timescale of 300 fs. Various system-size effects that are intrinsic to the simulation of excess electron injection are discussed. Comparison of the RPMD simulations with previous mixed quantum-classical dynamics simulations finds general agreement for both the mechanisms and timescales for electron localization, although the electron localization dynamics in the RPMD model is essentially completed within 400 fs in helium and 150 fs in water.

  14. Vlasov simulations of electron hole dynamics in inhomogeneous magnetic field

    Science.gov (United States)

    Kuzichev, Ilya; Vasko, Ivan; Agapitov, Oleksiy; Mozer, Forrest; Artemyev, Anton

    2017-04-01

    Electron holes (EHs) or phase space vortices are solitary electrostatic waves existing due to electrons trapped within EH electrostatic potential. Since the first direct observation [1], EHs have been widely observed in the Earth's magnetosphere: in reconnecting current sheets [2], injection fronts [3], auroral region [4], and many other space plasma systems. EHs have typical spatial scales up to tens of Debye lengths, electric field amplitudes up to hundreds of mV/m and propagate along magnetic field lines with velocities of about electron thermal velocity [5]. The role of EHs in energy dissipation and supporting of large-scale potential drops is under active investigation. The accurate interpretation of spacecraft observations requires understanding of EH evolution in inhomogeneous plasma. The critical role of plasma density gradients in EH evolution was demonstrated in [6] using PIC simulations. Interestingly, up to date no studies have addressed a role of magnetic field gradients in EH evolution. In this report, we use 1.5D gyrokinetic Vlasov code to demonstrate the critical role of magnetic field gradients in EH dynamics. We show that EHs propagating into stronger (weaker) magnetic field are decelerated (accelerated) with deceleration (acceleration) rate dependent on the magnetic field gradient. Remarkably, the reflection points of decelerating EHs are independent of the average magnetic field gradient in the system and depend only on the EH parameters. EHs are decelerated (accelerated) faster than would follow from the "quasi-particle" concept assuming that EH is decelerated (accelerated) entirely due to the mirror force acting on electrons trapped within EH. We demonstrate that EH propagation in inhomogeneous magnetic fields results in development of a net potential drop along an EH, which depends on the magnetic field gradient. The revealed features will be helpful for interpreting spacecraft observations and results of advanced particle simulations. In

  15. Problems in single-particle dynamics specific to electrons

    CERN Document Server

    Renieri, A

    1977-01-01

    The author investigates the specific problems related to the electron motion in a circular high-energy accelerator. The main difference between electrons and protons (or other heavy particles) is the synchrotron radiation energy loss. This phenomenon is negligible for heavy particles, but not for electrons. (5 refs).

  16. First-principles electron dynamics control simulation of diamond under femtosecond laser pulse train irradiation.

    Science.gov (United States)

    Wang, Cong; Jiang, Lan; Wang, Feng; Li, Xin; Yuan, Yanping; Xiao, Hai; Tsai, Hai-Lung; Lu, Yongfeng

    2012-07-11

    A real-time and real-space time-dependent density functional is applied to simulate the nonlinear electron-photon interactions during shaped femtosecond laser pulse train ablation of diamond. Effects of the key pulse train parameters such as the pulse separation, spatial/temporal pulse energy distribution and pulse number per train on the electron excitation and energy absorption are discussed. The calculations show that photon-electron interactions and transient localized electron dynamics can be controlled including photon absorption, electron excitation, electron density, and free electron distribution by the ultrafast laser pulse train.

  17. Three-dimensional simulations of ion dynamics in an Electron Cyclotron Resonance Ion Source

    NARCIS (Netherlands)

    Beijers, J. P. M.; Mironov, V.

    We present a three-dimensional simulation of the ion dynamics in an electron cyclotron resonance ion source. Ion trajectories in the min-B field of the source are calculated taking ion-ion and electron-ion collisions into account. The electrons are not tracked but considered as a neutralizing

  18. Hydrated Electron Transfer to Nucleobases in Aqueous Solutions Revealed by Ab Initio Molecular Dynamics Simulations.

    Science.gov (United States)

    Zhao, Jing; Wang, Mei; Fu, Aiyun; Yang, Hongfang; Bu, Yuxiang

    2015-08-03

    We present an ab initio molecular dynamics (AIMD) simulation study into the transfer dynamics of an excess electron from its cavity-shaped hydrated electron state to a hydrated nucleobase (NB)-bound state. In contrast to the traditional view that electron localization at NBs (G/A/C/T), which is the first step for electron-induced DNA damage, is related only to dry or prehydrated electrons, and a fully hydrated electron no longer transfers to NBs, our AIMD simulations indicate that a fully hydrated electron can still transfer to NBs. We monitored the transfer dynamics of fully hydrated electrons towards hydrated NBs in aqueous solutions by using AIMD simulations and found that due to solution-structure fluctuation and attraction of NBs, a fully hydrated electron can transfer to a NB gradually over time. Concurrently, the hydrated electron cavity gradually reorganizes, distorts, and even breaks. The transfer could be completed in about 120-200 fs in four aqueous NB solutions, depending on the electron-binding ability of hydrated NBs and the structural fluctuation of the solution. The transferring electron resides in the π*-type lowest unoccupied molecular orbital of the NB, which leads to a hydrated NB anion. Clearly, the observed transfer of hydrated electrons can be attributed to the strong electron-binding ability of hydrated NBs over the hydrated electron cavity, which is the driving force, and the transfer dynamics is structure-fluctuation controlled. This work provides new insights into the evolution dynamics of hydrated electrons and provides some helpful information for understanding the DNA-damage mechanism in solution. © 2015 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.

  19. Dynamics of interacting electrons under effect of a Morse potential

    Science.gov (United States)

    dos Santos, J. L. L.; Sales, M. O.; Neto, A. Ranciaro; de Moura, F. A. B. F.

    2017-05-01

    We consider interacting electrons moving in a nonlinear Morse lattice. We set the initial conditions as follows: electrons were initially localized at the center of the chain and a solitonic deformation was produced by an impulse excitation on the center of the chain. By solving quantum and classical equations for this system numerically, we found that a fraction of electronic wave function was trapped by the solitonic excitation, and trapping specificities depend on the degree of interaction among electrons. Also, there is evidence that the effective electron velocity depends on Coulomb interaction and electron-phonon coupling in a nontrivial way. This association is explained in detail along this work. In addition, we briefly discuss the dependence of our results with the type of initial condition we choose for the electrons and lattice.

  20. Electron quantum dynamics in atom-ion interaction.

    Science.gov (United States)

    Sabzyan, H; 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, which 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.

  1. Mean field ring polymer molecular dynamics for electronically nonadiabatic reaction rates.

    Science.gov (United States)

    Duke, Jessica Ryan; Ananth, Nandini

    2016-12-22

    We present a mean field ring polymer molecular dynamics method to calculate the rate of electron transfer (ET) in multi-state, multi-electron condensed-phase processes. Our approach involves calculating a transition state theory (TST) estimate to the rate using an exact path integral in discrete electronic states and continuous Cartesian nuclear coordinates. A dynamic recrossing correction to the TST rate is then obtained from real-time dynamics simulations using mean field ring polymer molecular dynamics. We employ two different reaction coordinates in our simulations and show that, despite the use of mean field dynamics, the use of an accurate dividing surface to compute TST rates allows us to achieve remarkable agreement with Fermi's golden rule rates for nonadiabatic ET in the normal regime of Marcus theory. Further, we show that using a reaction coordinate based on electronic state populations allows us to capture the turnover in rates for ET in the Marcus inverted regime.

  2. Dynamics of electron injection in a laser-wakefield accelerator

    Science.gov (United States)

    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.

  3. Electron and nuclear dynamics following ionisation of modified bismethylene-adamantane.

    Science.gov (United States)

    Vacher, Morgane; Albertani, Fabio E A; Jenkins, Andrew J; Polyak, Iakov; Bearpark, Michael J; Robb, Michael A

    2016-12-16

    We have simulated the coupled electron and nuclear dynamics using the Ehrenfest method upon valence ionisation of modified bismethylene-adamantane (BMA) molecules where there is an electron transfer between the two π bonds. We have shown that the nuclear motion significantly affects the electron dynamics after a few fs when the electronic states involved are close in energy. We have also demonstrated how the non-stationary electronic wave packet determines the nuclear motion, more precisely the asymmetric stretching of the two π bonds, illustrating "charge-directed reactivity". Taking into account the nuclear wave packet width results in the dephasing of electron dynamics with a half-life of 8 fs; this eventually leads to the equal delocalisation of the hole density over the two methylene groups and thus symmetric bond lengths.

  4. Quantum Nuclear Extension of Electron Nuclear Dynamics on Folded Effective-Potential Surfaces

    DEFF Research Database (Denmark)

    Hall, B.; Deumens, E.; Ohrn, Y.

    2014-01-01

    A perennial problem in quantum scattering calculations is accurate theoretical treatment of low energy collisions. We propose a method of extracting a folded, nonadiabatic, effective potential energy surface from electron nuclear dynamics (END) trajectories; we then perform nuclear wave packet dy...... dynamics on that surface and calculate differential cross sections for two-center, one (active) electron systems.......A perennial problem in quantum scattering calculations is accurate theoretical treatment of low energy collisions. We propose a method of extracting a folded, nonadiabatic, effective potential energy surface from electron nuclear dynamics (END) trajectories; we then perform nuclear wave packet...

  5. Attosecond Electron Correlation Dynamics in Double Ionization of Benzene Probed with Two-Electron Angular Streaking

    Science.gov (United States)

    Winney, Alexander H.; Lee, Suk Kyoung; Lin, Yun Fei; Liao, Qing; Adhikari, Pradip; Basnayake, Gihan; Schlegel, H. Bernhard; Li, Wen

    2017-09-01

    With a novel three-dimensional electron-electron coincidence imaging technique and two-electron angular streaking method, we show that the emission time delay between two electrons can be measured from tens of attoseconds to more than 1 fs. Surprisingly, in benzene, the double ionization rate decays as the time delay between the first and second electron emission increases during the first 500 as. This is further supported by the decay of the Coulomb repulsion in the direction perpendicular to the laser polarization. This result reveals that laser-induced electron correlation plays a major role in strong field double ionization of benzene driven by a nearly circularly polarized field.

  6. Elucidating the Ultrafast Dynamics of Photoinduced Charge Separation in Metalloporphyrin-Fullerene Dyads Across the Electromagnetic Spectrum

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, J.; Pápai, M.; Hirsch, A.; Jennings, G.; Kurtz, C. A.; Møller, K. B.; Lomoth, R.; Gosztola, D.; Zhang, X.; Canton, S. E.

    2016-09-08

    Metalloporphyrins are prominent building blocks in the synthetic toolbox of advanced photodriven molecular devices. When the central ion is paramagnetic, the relaxation pathways within the manifold of excited states are highly intricate so that unravelling the intramolecular energy and electron transfer processes is usually a very complex task. This fact is critically hampering the development of applications based on the enhanced coupling offered by the electronic exchange interaction. In this work, the dynamics of charge separation in a copper porphyrin-fullerene are studied with several complementary spectroscopic tools across the electromagnetic spectrum (from near infra-red to X-ray wavelengths), each of them providing specific diagnostics. Correlating the various rates clearly demonstrates that the lifetime of the photoinduced charge-separated state exceeds by about 10 fold that of the isolated photoexcited CuII porphyrin. As revealed by the spectral modifications in the XANES region, this stabilization is accompanied by a transient change in covalency around the CuII center, which is induced by an enhanced interaction with the C60 moiety. This experimental finding is further confirmed by state-of-the art calculations using DFT and TD-DFT including dispersion effects that explain the electrostatic and structural origins of this interaction, as the CuIIP cation becomes ruffled and approaches closer to the fullerene in the charge-separated state. From a methodological point of view, these results exemplify the potential of multielectron excitation features in transient X-ray spectra as future diagnostics of sub-femtosecond electronic dynamics. From a practical point of view, this work is paving the way for elucidating out-of-equilibrium electron transfer events coupled to magnetic interaction processes on their intrinsic time-scales.

  7. Final Report: Vibrational Dynamics in Photoinduced Electron Transfer

    Energy Technology Data Exchange (ETDEWEB)

    Kenneth G. Spears

    2006-04-19

    The objective of this grant was to understand how molecular vibrational states (geometry distortions) are involved in photoinduced electron transfer rates of molecules. This subject is an important component of understanding how molecular absorbers of light convert that energy into charge separation. This is important because the absorption usually excites molecular vibrations in a new electronic state prior to electron transfer to other molecules or semiconductor nanoparticles, as in some types of solar cells. The speeds of charge separation and charge recombination are key parameters that require experiments such as those in this work to test the rules governing electron transfer rates. Major progress was made on this goal. Some of the molecular structures selected for developing experimental data were bimolecular charge transfer complexes that contained metals of cobalt or vanadium. The experiments used the absorption of an ultrafast pulse of light to directly separate charges onto the two different molecular parts of the complex. The charge recombination then proceeds naturally, and one goal was to measure the speed of this recombination for different types of molecular vibrations. We used picosecond and femtosecond duration pulses with tunable colors at infrared wavelengths to directly observe vibrational states and their different rates of charge recombination (also called electron transfer). We discovered that different contact geometries in the complexes had very different electron transfer rates, and that one geometry had a significant dependence on the amount of vibration in the complex. This is the first and only measurement of such rates, and it allowed us to confirm our interpretation with a number of molecular models and test the sensitivity of electron transfer to vibrational states. This led us to develop a general theory, where we point out how molecular distortions can change the electron transfer rates to be much faster than prior theories

  8. Dynamical local connector approximation for electron addition and removal spectra

    OpenAIRE

    Vanzini, Marco; Reining, Lucia; Gatti, Matteo

    2017-01-01

    Realistic calculations of electron addition and removal spectra rely most often on Green's functions and complex, non-local self-energies. We introduce a shortcut to obtain the spectral function directly from a local and frequency-dependent, yet real, potential. We calculate this potential in the homogeneous electron gas (HEG), and we design a connector which prescribes the use of the HEG results to calculate spectral functions of real materials. Benchmark results for several solids demonstra...

  9. Dynamical Mean Field Theory and Electronic Structure Calculations

    OpenAIRE

    Chitra, R.; Kotliar, G.

    1999-01-01

    We formulate the dynamical mean field theory directly in the continuum. For a given definition of the local Green's function, we show the existence of a unique functional, whose stationary point gives the physical local Green's function of the solid. We present the diagrammatic rules to calculate it perturbatively in the interaction. Inspired by the success of dynamical mean field calculations for model Hamiltonian systems, we present approximations to the exact saddle point equations which m...

  10. Capturing Structural Dynamics in Crystalline Silicon Using Chirped Electrons from a Laser Wakefield Accelerator.

    Science.gov (United States)

    He, Z-H; Beaurepaire, B; Nees, J A; Gallé, G; Scott, S A; Pérez, J R Sánchez; Lagally, M G; Krushelnick, K; Thomas, A G R; Faure, J

    2016-11-08

    Recent progress in laser wakefield acceleration has led to the emergence of a new generation of electron and X-ray sources that may have enormous benefits for ultrafast science. These novel sources promise to become indispensable tools for the investigation of structural dynamics on the femtosecond time scale, with spatial resolution on the atomic scale. Here, we demonstrate the use of laser-wakefield-accelerated electron bunches for time-resolved electron diffraction measurements of the structural dynamics of single-crystal silicon nano-membranes pumped by an ultrafast laser pulse. In our proof-of-concept study, we resolve the silicon lattice dynamics on a picosecond time scale by deflecting the momentum-time correlated electrons in the diffraction peaks with a static magnetic field to obtain the time-dependent diffraction efficiency. Further improvements may lead to femtosecond temporal resolution, with negligible pump-probe jitter being possible with future laser-wakefield-accelerator ultrafast-electron-diffraction schemes.

  11. The dynamics of electron and ion holes in a collisionless plasma

    OpenAIRE

    Eliasson, B.; Shukla, P. K.

    2005-01-01

    International audience; We present a review of recent analytical and numerical studies of the dynamics of electron and ion holes in a collisionless plasma. The new results are based on the class of analytic solutions which were found by Schamel more than three decades ago, and which here work as initial conditions to numerical simulations of the dynamics of ion and electron holes and their interaction with radiation and the background plasma. Our analytic and numerical studies reveal that ion...

  12. Development of a model electronic Hamiltonian for understanding electronic relaxation dynamics of [Fe(bpy){sub 3}]{sup 2+} through molecular dynamics simulations

    Energy Technology Data Exchange (ETDEWEB)

    Iuchi, Satoru; Koga, Nobuaki [Graduate School of Information Science, Nagoya University, Furo-cho, Chikusa-ku, Nagoya 464-8601 (Japan)

    2015-12-31

    A model electronic Hamiltonian of [Fe(bpy){sub 3}]{sup 2+}, which was recently refined for use in molecular dynamics simulations, is reviewed with some additional results. In particular, the quality of the refined model Hamiltonian is examined in terms of the vibrational frequencies and solvation structures of the lowest singlet and quintet states.

  13. Electron-magnetohydrodynamic simulations of electron scale current sheet dynamics in the Vineta.II guide field reconnection experiment

    Science.gov (United States)

    Jain, Neeraj; von Stechow, Adrian; Muñoz, Patricio A.; Büchner, Jörg; Grulke, Olaf; Klinger, Thomas

    2017-09-01

    Three dimensional electron-magnetohydrodynamic (EMHD) simulations of electron current sheet dynamics in a background of stationary and unmagnetized ions and the subsequent generation of electromagnetic fluctuations are carried out. The physical parameters and initial magnetic configuration in the simulations are chosen to be similar to those in the Vineta.II magnetic reconnection experiment. Consistent with the experimental results, our 3D EMHD simulations show the formation of an elongated electron scale current sheet together with the excitation of electromagnetic fluctuations within this sheet. The fluctuations in the simulations are generated by an electron shear flow instability growing on the in-plane (perpendicular to the direction of the main current in the sheet) electron shear flow (or current) developed during the current sheet evolution. Similar to the experiments, the magnetic field fluctuations perpendicular to the guide magnetic field exhibit a broadband frequency spectrum following a power law and a positive correlation with the axial current density. Although the experimental results show that ions influence the spectral properties of the fluctuations, the simulations suggest that the electron dynamics, even in the absence of ion motion, primarily determines the formation of the current sheet and the generation of electromagnetic fluctuations observed in the experiments.

  14. High dynamic range isotope ratio measurements using an analog electron multiplier

    Czech Academy of Sciences Publication Activity Database

    Williams, P.; Lorinčík, Jan; Franzreb, K.; Herwig, R.

    2013-01-01

    Roč. 45, č. 1 (2013), s. 549-552 ISSN 0142-2421 R&D Projects: GA MŠk ME 894 Institutional support: RVO:67985882 Keywords : Isotope ratios * electron multiplier * dynamic range Subject RIV: JA - Electronics ; Optoelectronics, Electrical Engineering Impact factor: 1.393, year: 2013

  15. Picosecond electron injection dynamics in dye-sensitized oxides in the presence of electrolyte

    NARCIS (Netherlands)

    Pijpers, J.J.H.; Ulbricht, R.; Derossi, S.; Reek, J.N.H.; Bonn, M.

    2011-01-01

    We employ time-resolved terahertz (THz) spectroscopy (TRTS) to directly monitor the picosecond dynamics of electron transfer in dye-sensitized oxides in the presence of an electrolyte phase. Understanding the time scale on which electrons are injected from the dye into the oxide phase in the

  16. Dynamics of the dissociative electron attachment in H 2 O and D 2 O ...

    Indian Academy of Sciences (India)

    The dynamics of the formation and decay of negative ion resonance of A1 symmetry at 8.5 eV electron energy in the dissociative electron attachment (DEA) process in H2O and D2O are investigated using the velocity slice imaging technique. While the highest energy hydride ions formed by DEA show angular distributions ...

  17. Adjoint Fokker-Planck equation and runaway electron dynamics

    Energy Technology Data Exchange (ETDEWEB)

    Liu, Chang; Brennan, Dylan P.; Bhattacharjee, Amitava [Princeton University, Princeton, New Jersey 08544 (United States); Boozer, Allen H. [Columbia University, New York, New York 10027 (United States)

    2016-01-15

    The adjoint Fokker-Planck equation method is applied to study the runaway probability function and the expected slowing-down time for highly relativistic runaway electrons, including the loss of energy due to synchrotron radiation. In direct correspondence to Monte Carlo simulation methods, the runaway probability function has a smooth transition across the runaway separatrix, which can be attributed to effect of the pitch angle scattering term in the kinetic equation. However, for the same numerical accuracy, the adjoint method is more efficient than the Monte Carlo method. The expected slowing-down time gives a novel method to estimate the runaway current decay time in experiments. A new result from this work is that the decay rate of high energy electrons is very slow when E is close to the critical electric field. This effect contributes further to a hysteresis previously found in the runaway electron population.

  18. Electron injection dynamics in high-potential porphyrin photoanodes.

    Science.gov (United States)

    Milot, Rebecca L; Schmuttenmaer, Charles A

    2015-05-19

    There is a growing need to utilize carbon neutral energy sources, and it is well known that solar energy can easily satisfy all of humanity's requirements. In order to make solar energy a viable alternative to fossil fuels, the problem of intermittency must be solved. Batteries and supercapacitors are an area of active research, but they currently have relatively low energy-to-mass storage capacity. An alternative and very promising possibility is to store energy in chemical bonds, or make a solar fuel. The process of making solar fuel is not new, since photosynthesis has been occurring on earth for about 3 billion years. In order to produce any fuel, protons and electrons must be harvested from a species in its oxidized form. Photosynthesis uses the only viable source of electrons and protons on the scale needed for global energy demands: water. Because artificial photosynthesis is a lofty goal, water oxidation, which is a crucial step in the process, has been the initial focus. This Account provides an overview of how terahertz spectroscopy is used to study electron injection, highlights trends from previously published reports, and concludes with a future outlook. It begins by exploring similarities and differences between dye-sensitized solar cells (DSSCs) for producing electricity and a putative device for splitting water and producing a solar fuel. It then identifies two important problems encountered when adapting DSSC technology to water oxidation-improper energy matching between sensitizer energy levels with the potential for water oxidation and the instability of common anchoring groups in water-and discusses steps to address them. Emphasis is placed on electron injection from sensitizers to metal oxides because this process is the initial step in charge transport. Both the rate and efficiency of electron injection are analyzed on a sub-picosecond time scale using time-resolved terahertz spectroscopy (TRTS). Bio-inspired pentafluorophenyl porphyrins are

  19. Electron dynamics in metals and semiconductors in strong THz fields

    DEFF Research Database (Denmark)

    Jepsen, Peter Uhd

    2017-01-01

    Semiconductors and metals respond to strong electric fields in a highly nonlinear fashion. Using single-cycle THz field transients it is possible to investigate this response in regimes not accessible by transport-based measurements. Extremely high fields can be applied without material damage......, intrinsic, undoped materials can be studied, and field-induced electron emission into free space can be investigated in detail, thereby offering new knowledge about material response to strong THz-frequency fields relevant for near-future generations of electronic circuitry....

  20. Attosecond pre-determination of reaction dynamics in polyatomic molecules

    Science.gov (United States)

    Kitzler, Markus

    2014-05-01

    An important aim of Ultrafast Laser Science and Attosecond Physics is the measurement of valence electron dynamics in molecules during complex restructuring and fragmentation reactions. Such reactions may be triggered by the removal of electrons, e.g., by ionization with intense, ultrashort laser pulses. Depending on the valence-shell from which the electrons are removed, the molecular ion might be put into a binding state or a certain dissociative state. With control over the ionization process it might thus be possible to gain control over the subsequent restructuring and fragmentation processes on a purely electronic level. Detailed insight into the process of electron removal can be obtained from interferometric measurements using two bound state wavepackets released at different times within a sub-cycle of a laser field. I will present results of experiments that exploit this kind of electron wavepacket interferometry with sub-10 attosecond resolution for tracing the evolution of the phase of the bound state of an atom or molecule during the removal of an electron. I will furthermore present two conceptually similar schemes that allow pre-determining the outcome of molecular restructuring and fragmentation processes in polyatomic molecules on sub-femtosecond time-scales by gaining control over the process of electron removal. The first method involves recollision double ionization in intense few-cycle laser fields with a known carrier-envelope phase (CEP). Tuning of the CEP allows controlling the removal of inner-valence electrons and the controlled population of dissociative excited states. Using this method I will show experimental CEP-control over various fragmentation reactions of a series of polyatomic molecules. The second control scheme uses the strong preponderance of ionization from specific molecular orbitals to the alignment of the molecular axis with respect to the laser polarization direction for determining which valence level the electrons are

  1. Quantum fluctuation of electronic wave-packet dynamics coupled with classical nuclear motions.

    Science.gov (United States)

    Amano, Michiko; Takatsuka, Kazuo

    2005-02-22

    An ab initio electronic wave-packet dynamics coupled with the simultaneous classical dynamics of nuclear motions in a molecule is studied. We first survey the dynamical equations of motion for the individual components. Reflecting the nonadiabatic dynamics that electrons can respond to nuclear motions only with a finite speed, the equations of motion for nuclei include a force arising from the kinematic (nuclear momentum) coupling from electron cloud. To materialize these quantum effects in the actual ab initio calculations, we study practical implementation of relevant electronic matrix elements that are related to the derivatives with respect to the nuclear coordinates. Applications of the present scheme are performed in terms of the configuration state functions (CSF) using the canonical molecular orbitals as basis functions without transformation to particular diabatic basis. In the CSF representation, the nonadiabatic interaction due to the kinematic coupling is anticipated to be rather small, and instead it should be well taken into account through the off-diagonal elements of the electronic Hamiltonian matrix. Therefore it is expected that the nonadiabatic dynamics based on this CSF basis neglecting the kinematic coupling may work. To verify this anticipation and to quantify the actual effects of the kinematic coupling, we compare the dynamics with and without the kinematic-coupling terms using the same CSF set. Applications up to the fifth electronically excited states in a nonadiabatic collision between H(2) and B(+) shows that the overall behaviors of these two calculations are surprisingly similar to each other in an average sense except for a fast fluctuation reflecting the electronic time scale. However, at the same time, qualitative differences in the collision events are sometimes observed. Therefore it turns out after all that the kinematic-coupling terms cannot be neglected in the CSF-basis representation. The present applications also demonstrate

  2. The dynamics of electron and ion holes in a collisionless plasma

    Directory of Open Access Journals (Sweden)

    B. Eliasson

    2005-01-01

    Full Text Available We present a review of recent analytical and numerical studies of the dynamics of electron and ion holes in a collisionless plasma. The new results are based on the class of analytic solutions which were found by Schamel more than three decades ago, and which here work as initial conditions to numerical simulations of the dynamics of ion and electron holes and their interaction with radiation and the background plasma. Our analytic and numerical studies reveal that ion holes in an electron-ion plasma can trap Langmuir waves, due the local electron density depletion associated with the negative ion hole potential. Since the scale-length of the ion holes are on a relatively small Debye scale, the trapped Langmuir waves are Landau damped. We also find that colliding ion holes accelerate electron streams by the negative ion hole potentials, and that these streams of electrons excite Langmuir waves due to a streaming instability. In our Vlasov simulation of two colliding ion holes, the holes survive the collision and after the collision, the electron distribution becomes flat-topped between the two ion holes due to the ion hole potentials which work as potential barriers for low-energy electrons. Our study of the dynamics between electron holes and the ion background reveals that standing electron holes can be accelerated by the self-created ion cavity owing to the positive electron hole potential. Vlasov simulations show that electron holes are repelled by ion density minima and attracted by ion density maxima. We also present an extension of Schamel's theory to relativistically hot plasmas, where the relativistic mass increase of the accelerated electrons have a dramatic effect on the electron hole, with an increase in the electron hole potential and in the width of the electron hole. A study of the interaction between electromagnetic waves with relativistic electron holes shows that electromagnetic waves can be both linearly and nonlinearly

  3. Dynamics of a single-atom electron pump

    Science.gov (United States)

    van der Heijden, J.; Tettamanzi, G. C.; Rogge, S.

    2017-01-01

    Single-electron pumps based on isolated impurity atoms have recently been experimentally demonstrated. In these devices the Coulomb potential of an atom creates a localised electron state with a large charging energy and considerable orbital level spacings, enabling robust charge capturing processes. In contrast to the frequently used gate-defined quantum dot pumps, which experience a strongly time-dependent potential, the confinement potential in these single-atom pumps is hardly affected by the periodic driving of the system. Here we describe the behaviour and performance of an atomic, single parameter, electron pump. This is done by considering the loading, isolating and unloading of one electron at the time, on a phosphorous atom embedded in a silicon double gate transistor. The most important feature of the atom pump is its very isolated ground state, which is populated through the fast loading of much higher lying excited states and a subsequent fast relaxation process. This leads to a substantial increase in pumping accuracy, and is opposed to the adverse role of excited states observed for quantum dot pumps due to non-adiabatic excitations. The pumping performance is investigated as a function of dopant position, revealing a pumping behaviour robust against the expected variability in atomic position. PMID:28295055

  4. Attosecond photoelectron spectroscopy of electron transport in solids

    Energy Technology Data Exchange (ETDEWEB)

    Magerl, Elisabeth

    2011-03-31

    Time-resolved photoelectron spectroscopy of condensed matter systems in the attosecond regime promises new insights into excitation mechanisms and transient dynamics of electrons in solids. This timescale became accessible directly only recently with the development of the attosecond streak camera and of laser systems providing few-cycle, phase-controlled laser pulses in the near-infrared, which are used to generate isolated, sub-femtosecond extreme-ultraviolet pulses with a well-defined timing with respect to the near-infrared pulse. Employing these pulses, the attosecond streak camera offers time resolutions as short as a few 10 attoseconds. In the framework of this thesis, a new, versatile experimental apparatus combining attosecond pulse generation in gases with state of the art surface science techniques is designed, constructed, and commissioned. Employing this novel infrastructure and the technique of the attosecond transient recorder, we investigate transport phenomena occurring after photoexcitation of electrons in tungsten and rhenium single crystals and show that attosecond streaking is a unique method for resolving extremely fast electronic phenomena in solids. It is demonstrated that electrons originating from different energy levels, i.e. from the conduction band and the 4f core level, are emitted from the crystal surface at different times. The origin of this time delay, which is below 150 attoseconds for all studied systems, is investigated by a systematic variation of several experimental parameters, in particular the photon energy of the employed attosecond pulses. These experimental studies are complemented by theoretical studies of the group velocity of highly-excited electrons based on ab initio calculations. While the streaking technique applied on single crystals can provide only information about the relative time delay between two types of photoelectrons, the absolute transport time remains inaccessible. We introduce a scheme of a reference

  5. Electronic dynamics due to exchange interaction with holes in GaAs

    Science.gov (United States)

    Schneider, Hans Christian; Krauß, Michael

    2010-02-01

    We present an investigation of electron-spin dynamics in p-doped bulk GaAs due to the electron-hole exchange interaction, aka the Bir-Aronov-Pikus mechanism. We discuss under which conditions a spin relaxation times for this mechanism is, in principle, accessible to experimental techniques, in particular to 2-photon photoemission, but also Faraday/Kerr effect measurements. We give numerical results for the spin relaxation time for a range of p-doping densities and temperatures. We then go beyond the relaxation time approximation and calculate numerically the spin-dependent electron dynamics by including the spin-flip electron-hole exchange scattering and spin-conserving carrier Coulomb scattering at the level of Boltzmann scattering integrals. We show that the electronic dynamics deviates from the simple spin-relaxation dynamics for electrons excited at high energies where the thermalization does not take place faster than the spin relaxation time. We also present a derivation of the influence of screening on the electron-hole exchange scattering and conclude that it can be neglected for the case of GaAs, but may become important for narrow-gap semiconductors.

  6. Ultrafast electronic relaxation and vibrational dynamics in a polyacetylene derivative

    Science.gov (United States)

    Kobayashi, Takayoshi; Iiyama, Tsugumasa; Okamura, Kotaro; Du, Juan; Masuda, Toshio

    2013-04-01

    Real-time vibrational spectra in a polyacetylene derivative, poly[o-TFMPA([o-(trifluoromethyl) phenyl]acetylene)] in a broad electronic spectral region were observed using a sub-7-fs laser. Using the frequencies and initial phases of vibrational modes obtained by the spectroscopy, the assignment of the wavepackets was made. From the first moment, Huang-Rhys parameters were determined for six most prominent modes, which characterize the potential hypersurface composed of multi-dimensional vibrational mode spaces.

  7. Radiation Belt Electron Dynamics Driven by Large-Amplitude Whistlers

    Science.gov (United States)

    Khazanov, G. V.; Tel'nikhin, A. A.; Kronberg, T. K.

    2013-01-01

    Acceleration of radiation belt electrons driven by oblique large-amplitude whistler waves is studied. We show analytically and numerically that this is a stochastic process; the intensity of which depends on the wave power modified by Bessel functions. The type of this dependence is determined by the character of the nonlinear interaction due to coupling between action and phase. The results show that physically significant quantities have a relatively weak dependence on the wave power.

  8. Time Resolved Broadband Terahertz Relaxation Dynamics of Electron in Water

    DEFF Research Database (Denmark)

    Wang, Tianwu; Iwaszczuk, Krzysztof; Cooke, David G.

    We investigated the transient response of the solvated electron in water ejected by photodetachment from potassium ferrocyanide using time resolved terahertz spectroscopy (TSTS). Ultrabroadband THz transients are generated and detected by a two-color femtosecond-induced air plasma and air biased...... coherent detection, respectively. We find that the measured frequency dependent conductivity can be well described by a Drude-Smith model, supplemented by a Lorentz model oscillating near 5 THz....

  9. Electron and proton kinetics and dynamics in flaring atmospheres

    CERN Document Server

    Zharkova, Valentina

    2012-01-01

    This timely book presents new research results on high-energy particle physics related to solar flares, covering the theory and applications of the reconnection process in a clear and comprehensible way. It investigates particle kinetics and dynamics in flaring atmospheres and their diagnostics from spectral observations, while providing an analysis of the observation data and techniques and comparing various models. Written by an internationally acclaimed expert, this is vital reading for all solar, astro-, and plasma physicists working in the field.

  10. New algorithm for dynamical friction of ions in a magnetized electron beam

    Science.gov (United States)

    Bruhwiler, David L.; Webb, Stephen D.

    2017-03-01

    Relativistic magnetized electron cooling in untested parameter regimes is essential to achieve the ion luminosity requirements of proposed electron-ion collider designs. Therefore, accurate calculations of magnetized dynamic friction are required, with the ability to include all relevant physics that might increase the cooling time, including space charge forces, field errors and complicated phase space distributions of imperfectly magnetized electron beams. We present a fundamentally new analytic treatment of momentum transfer from a single magnetized electron to a drifting ion, with arbitrary initial conditions and arbitrary interaction time. The map describing such collisions, which is derived from a Hamiltonian and conserves momentum, removes any need to numerically integrate the complicated Larmor trajectories. This important result, made possible by effectively exploiting the perturbative nature of the problem, will enable rapid semi-analytic calculations of dynamic friction on ions in magnetized cooling systems for arbitrary electron distributions.

  11. Influence of non-collisional laser heating on the electron dynamics in dielectric materials

    CERN Document Server

    Barilleau, L; Chimier, B; Geoffroy, G; Tikhonchuk, V

    2016-01-01

    The electron dynamics in dielectric materials induced by intense femtosecond laser pulses is theoretically addressed. The laser driven temporal evolution of the energy distribution of electrons in the conduction band is described by a kinetic Boltzmann equation. In addition to the collisional processes for energy transfer such as electron-phonon-photon and electron-electron interactions, a non-collisional process for photon absorption in the conduction band is included. It relies on direct transitions between sub-bands of the conduction band through multiphoton absorption. This mechanism is shown to significantly contribute to the laser heating of conduction electrons for large enough laser intensities. It also increases the time required for the electron distribution to reach the equilibrium state as described by the Fermi-Dirac statistics. Quantitative results are provided for quartz irradiated by a femtosecond laser pulse with a wavelength of 800 nm and for intensities in the range of tens of TW/cm$^2$, lo...

  12. Attosecond electron-electron collision dynamics of the four-electron escape in Be close to threshold

    CERN Document Server

    Emmanouilidou, A

    2012-01-01

    We explore the escape geometry of four electrons a few eV above threshold following single-photon absorption from the ground state of Be. We find that the four electrons leave the atom on the vertices of a pyramid instead of a previously-predicted tetrahedron. To illustrate the physical mechanisms of quadruple ionization we use a momentum transferring attosecond collision scheme which we show to be in accord with the pyramid break-up pattern.

  13. Dissociation dynamics of transient anion formed via electron attachment to sulfur dioxide

    Science.gov (United States)

    Gope, K.; Prabhudesai, V. S.; Mason, N. J.; Krishnakumar, E.

    2017-08-01

    We report the molecular dynamics of dissociative electron attachment to sulfur dioxide (SO2) by measuring the momentum distribution of fragment anions using the velocity slice imaging technique in the electron energy range of 2-10 eV. The S- channel results from symmetric dissociation which exhibits competition between the stretch mode and bending mode of vibration in the excited parent anion. The asymmetric dissociation of parent anions leads to the production of O- and SO- channels where the corresponding neutral fragments are formed in their ground as well as excited electronic states. We also identify that internal excitation of SO- is responsible for its low yield at higher electron energies.

  14. Studies of dynamics of electron clouds in STAR silicon drift detectors

    CERN Document Server

    Bellwied, R; Brandon, N; Caines, H; Chen, W; Dimassimo, D; Dyke, H; Hall, J R; Hardtke, D; Hoffmann, G W; Humanic, T J; Kotova, A I; Kotov, I V; Kraner, H W; Li, Z; Lynn, D; Middelkamp, P; Ott, G; Pandey, S U; Pruneau, C A; Rykov, V L; Schambach, J; Sedlmeir, J; Sugarbaker, E R; Takahashi, J; Wilson, W K

    2000-01-01

    The dynamics of electrons generated in silicon drift detectors was studied using an IR LED. Electrons were generated at different drift distances. In this way, the evolution of the cloud as a function of drift time was measured. Two methods were used to measure the cloud size. The method of cumulative functions was used to extract the electron cloud profiles. Another method obtains the cloud width from measurements of the charge collected on a single anode as a function of coordinate of the light spot. The evolution of the electron cloud width with drift time is compared with theoretical calculations. Experimental results agreed with theoretical expectations.

  15. Ultrafast structural and electronic dynamics of the metallic phase in a layered manganite

    Directory of Open Access Journals (Sweden)

    L. Piazza

    2014-01-01

    Full Text Available The transition between different states in manganites can be driven by various external stimuli. Controlling these transitions with light opens the possibility to investigate the microscopic path through which they evolve. We performed femtosecond (fs transmission electron microscopy on a bi-layered manganite to study its response to ultrafast photoexcitation. We show that a photoinduced temperature jump launches a pressure wave that provokes coherent oscillations of the lattice parameters, detected via ultrafast electron diffraction. Their impact on the electronic structure are monitored via ultrafast electron energy loss spectroscopy, revealing the dynamics of the different orbitals in response to specific structural distortions.

  16. Dynamic Pricing in Electronic Commerce Using Neural Network

    Science.gov (United States)

    Ghose, Tapu Kumar; Tran, Thomas T.

    In this paper, we propose an approach where feed-forward neural network is used for dynamically calculating a competitive price of a product in order to maximize sellers’ revenue. In the approach we considered that along with product price other attributes such as product quality, delivery time, after sales service and seller’s reputation contribute in consumers purchase decision. We showed that once the sellers, by using their limited prior knowledge, set an initial price of a product our model adjusts the price automatically with the help of neural network so that sellers’ revenue is maximized.

  17. Role of solvent dynamics in ultrafast photoinduced proton-coupled electron transfer reactions in solution.

    Science.gov (United States)

    Hazra, Anirban; Soudackov, Alexander V; Hammes-Schiffer, Sharon

    2010-09-30

    A theoretical formulation for modeling photoinduced nonequilibrium proton-coupled electron transfer (PCET) reactions in solution is presented. In this formulation, the PCET system is described by donor and acceptor electron-proton vibronic free energy surfaces that depend on a single collective solvent coordinate. Dielectric continuum theory is used to obtain a generalized Langevin equation of motion for this collective solvent coordinate. The terms in this equation depend on the solvent properties, such as the dielectric constants, relaxation time, and molecular moment of inertia, as well as the solute properties characterizing the vibronic surfaces. The ultrafast dynamics following photoexcitation is simulated using a surface hopping method in conjunction with the Langevin equation of motion. This methodology is used to examine a series of model photoinduced PCET systems, where the initial nonequilibrium state is prepared by vertical photoexcitation from the ground electronic state to the donor electronic state. Analysis of the dynamical trajectories provides insight into the interplay between the solvent dynamics and the electron-proton transfer for these types of processes. In addition, these model studies illustrate how the coupling between the electron-proton transfer and the solvent dynamics can be tuned by altering the solute and solvent properties.

  18. Dynamics and pathway of electron tunneling in repair of damaged DNA by photolyase

    Science.gov (United States)

    Liu, Zheyun; Guo, Xunmin; Tan, Chuang; Li, Jiang; Kao, Ya-Ting; Wang, Lijuan; Sancar, Aziz; Zhong, Dongping

    2013-03-01

    Through electron tunneling, photolyase, a photoenzyme, restores damaged DNA into normal bases. Here, we report our systematic characterization and analyses of three electron transfer processes in thymine dimer restoration by following the entire dynamical evolution during enzymatic repair with femtosecond resolution. Using (deoxy)uracil and thymine as dimer substrates, we unambiguously determined the electron tunneling pathways for the forward electron transfer to initiate repairing and for the final electron return to restore the active cofactor and complete the repair photocycle. Significantly, we found that the adenine moiety of the unusual bent cofactor is essential to mediating all electron-transfer dynamics through a super-exchange mechanism, leading to a delicate balance of time scales. The active-site structural integrity, unique electron tunneling pathways and the critical role of adenine assure these elementary dynamics in synergy in this complex photorepair machinery to achieve the maximum repair efficiency close to unity. The authors thank Drs. Chaitanya Sexana, Yi Yang, and Chen Zang for the initial help with experiment, and Prof. Sherwin Singer and Dr. Ali Hassanali for discussion.

  19. [The innovative dynamic of the mechanics, electronics and materials subsystem].

    Science.gov (United States)

    Maldonado, José; Gadelha, Carlos Augusto Grabois; Costa, Laís Silveira; Vargas, Marco

    2012-12-01

    The mechanics, electronics and materials subsystem, one of the subsystems of the health care productive complex, encompasses different activities, usually clustered in what is called the medical, hospital and dental equipment and materials industry. This is a strategic area for health care, since it represents a continuous source of changes in care practices, and influences the provision of health care services. It has, moreover, potential for promoting the progress of Brazil's system of innovation and for increasing the competitiveness of the industry as a whole, given that it articulates future technologies. Despite the significant growth of this industry in Brazil in recent years, such equipment and materials have been presenting a growing deficit in the balance of trade. This incompatibility between national health care needs and the productive and innovative basis of the industry points to structural fragilities in the system. Using the framework of political economy, the article aims to discuss the development of this industry in Brazil and its challenges.

  20. Understanding Dynamic Competitive Technology Diffusion in Electronic Markets

    Science.gov (United States)

    Zhang, Cheng; Song, Peijian; Xu, Yunjie; Xue, Ling

    The extant literature on information technology (IT) diffusion has largely treated technology diffusion as a generic and independent process. This study, in contrast, examines the diffusion of different IT products with brand differentiation and competition. Drawing upon existing theories of product diffusion, we propose a research model to capture the dynamics of the competitive diffusion of web-based IT products and validate it with longitudinal field data of e-business platforms. Our findings suggest that IT product diffusion can be better predicted by a competitive model than by an independent-diffusion-process model. This research extends IT research to the context of competitive diffusion and provides practitioners an effective model to predict the dissemination of their products. The research also suggests the existence of asymmetric interactions among competing products, prompting scholars and practitioners to pay attention to the influence of competing products when making forecast of their product market.

  1. Radiation belt seed population and its association with the relativistic electron dynamics: A statistical study

    Science.gov (United States)

    Tang, C. L.; Wang, Y. X.; Ni, B.; Zhang, J.-C.; Reeves, G. D.; Su, Z. P.; Baker, D. N.; Spence, H. E.; Funsten, H. O.; Blake, J. B.

    2017-05-01

    Using the particle data measured by Van Allen Probe A from October 2012 to March 2016, we investigate in detail the radiation belt seed population and its association with the relativistic electron dynamics during 74 geomagnetic storms. The period of the storm recovery phase was limited to 72 h. The statistical study shows that geomagnetic storms and substorms play important roles in the radiation belt seed population (336 keV electrons) dynamics. Based on the flux changes of 1 MeV electrons before and after the storm peak, these storm events are divided into two groups of "large flux enhancement" and "small flux enhancement." For large flux enhancement storm events, the correlation coefficients between the peak flux location of the seed population and those of relativistic electrons (592 keV, 1 MeV, 1.8 MeV, and 2.1 MeV) during the storm recovery phase decrease with electron kinetic energy, being 0.92, 0.68, 0.49, and 0.39, respectively. The correlation coefficients between the peak flux of the seed population and those of relativistic electrons are 0.92, 0.81, 0.75, and 0.73. For small flux enhancement storm events, the correlation coefficients between the peak flux location of the seed population and those of relativistic electrons are relatively smaller, while the peak flux of the seed population is well correlated with those of relativistic electrons (correlation coefficients >0.84). It is suggested that during geomagnetic storms there is a good correlation between the seed population and ≤1 MeV electrons and the seed population is important to the relativistic electron dynamics.

  2. Verlet-like algorithms for Car-Parrinello molecular dynamics with unequal electronic occupations

    Science.gov (United States)

    Castañeda Medina, Arcesio; Schmid, Rochus

    2017-09-01

    The ab initio molecular dynamics simulations of metallic, charged, and electrochemical systems require, in principle, the inclusion of unequally occupied electronic states. In this contribution, the general approach to work with fixed but arbitrary occupations within the Car-Parrinello molecular dynamics scheme is revisited, focusing on the procedure which is required to maintain the orthonormality constraints in the commonly used position-Verlet integrator. Expressions to constrain also the orbital velocities, as it is demanded by a velocity-Verlet integrator, are then derived. The generalized unequal-occupation SHAKE algorithm is compared with the standard procedure for damped dynamics (energy optimization) of systems including fully unoccupied electronic states. In turn, the proposed unequal-occupation RATTLE algorithm is validated by the corresponding microcanonical ensemble simulations. It is shown that only with the proper orthogonalization method, a correct ordering of states and energy conserving dynamics can be achieved.

  3. Semiclassical (SC) Description of Electronically Non-AdiabaticDynamics via the Initial Value Representation (IVR)

    Energy Technology Data Exchange (ETDEWEB)

    Ananth, V.; Venkataraman, C.; Miller, W.H.

    2007-06-22

    The initial value representation (IVR) of semiclassical (SC) theory is used in conjunction with the Meyer-Miller/Stock-Thoss description of electronic degrees of freedom in order to treat electronically non-adiabatic processes. It is emphasized that the classical equations of motion for the nuclear and electronic degrees of freedom that emerge in this description are precisely the Ehrenfest equations of motion (the force on the nuclei is the force averaged over the electronic wavefunction), but that the trajectories given by these equations of motion do not have the usual shortcomings of the traditional Ehrenfest model when they are used within the SC-IVR framework. For example, in the traditional Ehrenfest model (a mixed quantum-classical approach) the nuclear motion emerges from a non-adiabatic encounter on an average potential energy surface (a weighted average according to the population in the various electronic states), while the SC-IVR describes the correct correlation between electronic and nuclear dynamics, i.e., the nuclear motion is on one potential energy surface or the other depending on the electronic state. Calculations using forward-backward versions of SC-IVR theory (FB-IVR) are presented to illustrate this behavior. An even more approximate version of the SC-IVR, the linearized approximation (LSC-IVR), is slightly better than the traditional Ehrenfest model, but since it cannot describe quantum coherence effects, the LSC-IVR is also not able to describe the correct correlation between nuclear and electronic dynamics.

  4. Molecular Dynamics and Electron Density Studies of Siderophores and Peptides.

    Science.gov (United States)

    Fidelis, Krzysztof Andrzej

    1990-08-01

    The dissertation comprises three separate studies of siderophores and peptides. In the first of these studies the relative potential energies for a series of diastereomers of a siderophore neocoprogen I are evaluated with molecular mechanics force field methods. Charges on the hydroxamate moiety are determined with a synthetic model siderophore compound using valence population refinements, and alternatively, with the theoretical ab initio/ESP calculations. The single diastereomer found in the crystal structure is among four characterized by the low potential energy, while prevalence of Delta vs. Lambda configuration about the iron is found to be a property of the entire series. In the second study the crystal structure of a ferrichrome siderophore ferrirhodin is reported. The crystal structure conformation of the molecular backbone as well as the iron coordination geometry compare well with other ferrichrome structures. The differences between the acyl groups of ferrirubin and ferrirhodin are explored using the methods of molecular mechanics. The third study a 300 ps, 300 K, in vacuo molecular dynamics simulation of didemnin A and B yields distinct molecular conformers, which are different from the one found in the crystal structure or modeled in solution, using the Nuclear Overhauser Effect data. Evaluations of the relative potential energy are performed with short 10 ps simulations in solution. Didemnins are natural depsipeptides isolated from a Caribbean tunicate and characterized by particularly potent antiproliferative and immunomodulatory activity. Conformationally rigid and flexible regions of the molecule are described. A short review of the molecular mechanics methodology is given in the introduction.

  5. Probing interfacial electron dynamics with time-resolved X-ray spectroscopy

    Science.gov (United States)

    Neppl, Stefan

    2015-05-01

    Time-resolved core-level spectroscopy techniques using laser pulses to initiate and short X-ray pulses to probe photo-induced processes have the potential to provide electronic state- and atomic site-specific insight into fundamental electron dynamics at complex interfaces. We describe the implementation of femto- and picosecond time-resolved photoelectron spectroscopy at the Linac Coherent Light Source (LCLS) and at the Advanced Light Source (ALS) in order to follow light-driven electron dynamics at dye-semiconductor interfaces on femto- to nanosecond timescales, and from the perspective of individual atomic sites. A distinct transient binding-energy shift of the Ru3d photoemission lines originating from the metal centers of N3 dye-molecules adsorbed on nanoporous ZnO is observed 500 fs after resonant HOMO-LUMO excitation with a visible laser pulse. This dynamical chemical shift is accompanied by a characteristic surface photo-voltage response of the semiconductor substrate. The two phenomena and their correlation will be discussed in the context of electronic bottlenecks for efficient interfacial charge-transfer and possible charge recombination and relaxation pathways leading to the neutralization of the transiently oxidized dye following ultrafast electron injection. First steps towards in operando time-resolved X-ray absorption spectroscopy techniques to monitor interfacial chemical dynamics will be presented.

  6. Transformation dynamics of Ni clusters into NiO rings under electron beam irradiation

    Energy Technology Data Exchange (ETDEWEB)

    Knez, Daniel, E-mail: daniel.knez@felmi-zfe.at [Institute of Electron Microscopy and Nanoanalysis, Graz University of Technology, Steyrergasse 17, 8010 Graz (Austria); Graz Centre for Electron Microscopy, Steyrergasse 17, 8010 Graz (Austria); Thaler, Philipp; Volk, Alexander [Institute of Experimental Physics, Graz University of Technology, Petersgasse 16, 8010 Graz (Austria); Kothleitner, Gerald [Institute of Electron Microscopy and Nanoanalysis, Graz University of Technology, Steyrergasse 17, 8010 Graz (Austria); Graz Centre for Electron Microscopy, Steyrergasse 17, 8010 Graz (Austria); Ernst, Wolfgang E. [Institute of Experimental Physics, Graz University of Technology, Petersgasse 16, 8010 Graz (Austria); Hofer, Ferdinand [Institute of Electron Microscopy and Nanoanalysis, Graz University of Technology, Steyrergasse 17, 8010 Graz (Austria); Graz Centre for Electron Microscopy, Steyrergasse 17, 8010 Graz (Austria)

    2017-05-15

    We report the transformation of nickel clusters into NiO rings by an electron beam induced nanoscale Kirkendall effect. High-purity nickel clusters consisting of a few thousand atoms have been used as precursors and were synthesized with the superfluid helium droplet technique. Aberration-corrected, analytical scanning transmission electron microscopy was applied to oxidise and simultaneously analyse the nanostructures. The transient dynamics of the oxidation could be documented by time lapse series using high-angle annular dark-field imaging and electron energy-loss spectroscopy. A two-step Cabrera-Mott oxidation mechanism was identified. It was found that water adsorbed adjacent to the clusters acts as oxygen source for the electron beam induced oxidation. The size-dependent oxidation rate was estimated by quantitative EELS measurements combined with molecular dynamics simulations. Our findings could serve to better control sample changes during examination in an electron microscope, and might provide a methodology to generate other metal oxide nanostructures. - Highlights: • Beam induced conversion of Ni clusters into crystalline NiO rings has been observed. • Ni clusters were grown with the superfluid He-droplet technique. • oxidizeSTEM was utilized to investigate and simultaneously oxidize these clusters. • Oxidation dynamics was captured in real-time. • Cluster sizes and the oxidation rate were estimated via EELS and molecular dynamics.

  7. Dissociation dynamics of transient anion formed via electron attachment to sulfur dioxide

    OpenAIRE

    Gope, K.; Prabhudesai, V. S.; Mason, N. J.; Krishnakumar, E.

    2017-01-01

    We report the molecular dynamics of dissociative electron attachment to sulfur dioxide (SO2) by measuring the momentum distribution of fragment anions using the velocity slice imaging technique in the electron energy range of 2–10 eV. The S- channel results from symmetric dissociation which exhibits competition between the stretch mode and bending mode of vibration in the excited parent anion. The asymmetric dissociation of parent anions leads to the production of O- and SO- channels where th...

  8. Electron spin dynamics in GaAsN and InGaAsN structures

    Energy Technology Data Exchange (ETDEWEB)

    Lagarde, D.; Lombez, L.; Marie, X.; Balocchi, A.; Amand, T. [Laboratoire de Nanophysique, Magnetisme et Optoelectronique, INSA 135 avenue de Rangueil 31077 Toulouse Cedex 4 (France); Kalevich, V.K.; Shiryaev, A.; Ivchenko, E.; Egorov, A. [A.F. Ioffe Physico-Technical Institute, 194021 St-Petersburg (Russian Federation)

    2007-01-15

    We report on optical orientation experiments in undoped GaAsN epilayers and InGaAsN quantum wells (QW), showing that a strong electron spin polarisation can persist at room temperature. We demonstrate that the spin dynamics in these dilute nitride structures is governed by a spin-dependent recombination process of free conduction electrons on deep paramagnetic centres. (copyright 2007 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  9. Electron Dynamics of Interatomic Coulombic Decay in Quantum Dots: Singlet Initial State

    Directory of Open Access Journals (Sweden)

    Cederbaum Lorenz S.

    2013-03-01

    Full Text Available In this paper we investigated the interatomic Coulombic decay (ICD of a resonance singlet state in a model potential for two few-electron semiconductor quantum dots (QDs by means of electron dynamics. We demonstrate that ICD is the major decay process of the resonance for the singlet wave function and compare the total and partial decay widths as a function of the QD separation with that from our previous study on the corresponding triplet states [1].

  10. Target Surface Area Effects on Hot Electron Dynamics from High Intensity Laser-Plasma Interactions

    Science.gov (United States)

    2016-08-19

    sheath field confinement on electron dynamics. X-ray emission due to energetic electrons was imaged using a aK imaging crystal. Electronswere observed to...laser conversion efficiency into particle andfield energy. Previous efforts tominimize this effect have primarily focused on small, isolated targets...leading to enhanced fields [12] improved conversion efficiency [13] and enhanced proton energies [14]with laser pulse durations of hundreds of fs

  11. 2012 ELECTRONIC SPECTROSCOPY & DYNAMICS GORDON RESEARCH CONFERENCE, JULY 22-27, 2012

    Energy Technology Data Exchange (ETDEWEB)

    Kohler, Bern

    2012-07-27

    Topics covered in this GRC include high-resolution spectroscopy, coherent electronic energy transport in biology, excited state theory and dynamics, excitonics, electronic spectroscopy of cold and ultracold molecules, and the spectroscopy of nanostructures. Several sessions will highlight innovative techniques such as time-resolved x-ray spectroscopy, frequency combs, and liquid microjet photoelectron spectroscopy that have forged stimulating new connections between gas-phase and condensed-phase work.

  12. Influence of cathode geometry on electron dynamics in an ultrafast electron microscope

    Directory of Open Access Journals (Sweden)

    Shaozheng Ji

    2017-09-01

    Full Text Available Efforts to understand matter at ever-increasing spatial and temporal resolutions have led to the development of instruments such as the ultrafast transmission electron microscope (UEM that can capture transient processes with combined nanometer and picosecond resolutions. However, analysis by UEM is often associated with extended acquisition times, mainly due to the limitations of the electron gun. Improvements are hampered by tradeoffs in realizing combinations of the conflicting objectives for source size, emittance, and energy and temporal dispersion. Fundamentally, the performance of the gun is a function of the cathode material, the gun and cathode geometry, and the local fields. Especially shank emission from a truncated tip cathode results in severe broadening effects and therefore such electrons must be filtered by applying a Wehnelt bias. Here we study the influence of the cathode geometry and the Wehnelt bias on the performance of a photoelectron gun in a thermionic configuration. We combine experimental analysis with finite element simulations tracing the paths of individual photoelectrons in the relevant 3D geometry. Specifically, we compare the performance of guard ring cathodes with no shank emission to conventional truncated tip geometries. We find that a guard ring cathode allows operation at minimum Wehnelt bias and improve the temporal resolution under realistic operation conditions in an UEM. At low bias, the Wehnelt exhibits stronger focus for guard ring than truncated tip cathodes. The increase in temporal spread with bias is mainly a result from a decrease in the accelerating field near the cathode surface. Furthermore, simulations reveal that the temporal dispersion is also influenced by the intrinsic angular distribution in the photoemission process and the initial energy spread. However, a smaller emission spot on the cathode is not a dominant driver for enhancing time resolution. Space charge induced temporal broadening

  13. Influence of cathode geometry on electron dynamics in an ultrafast electron microscope

    Science.gov (United States)

    Ji, Shaozheng; Piazza, Luca; Cao, Gaolong; Park, Sang Tae; Reed, Bryan W.; Masiel, Daniel J.; Weissenrieder, Jonas

    2017-01-01

    Efforts to understand matter at ever-increasing spatial and temporal resolutions have led to the development of instruments such as the ultrafast transmission electron microscope (UEM) that can capture transient processes with combined nanometer and picosecond resolutions. However, analysis by UEM is often associated with extended acquisition times, mainly due to the limitations of the electron gun. Improvements are hampered by tradeoffs in realizing combinations of the conflicting objectives for source size, emittance, and energy and temporal dispersion. Fundamentally, the performance of the gun is a function of the cathode material, the gun and cathode geometry, and the local fields. Especially shank emission from a truncated tip cathode results in severe broadening effects and therefore such electrons must be filtered by applying a Wehnelt bias. Here we study the influence of the cathode geometry and the Wehnelt bias on the performance of a photoelectron gun in a thermionic configuration. We combine experimental analysis with finite element simulations tracing the paths of individual photoelectrons in the relevant 3D geometry. Specifically, we compare the performance of guard ring cathodes with no shank emission to conventional truncated tip geometries. We find that a guard ring cathode allows operation at minimum Wehnelt bias and improve the temporal resolution under realistic operation conditions in an UEM. At low bias, the Wehnelt exhibits stronger focus for guard ring than truncated tip cathodes. The increase in temporal spread with bias is mainly a result from a decrease in the accelerating field near the cathode surface. Furthermore, simulations reveal that the temporal dispersion is also influenced by the intrinsic angular distribution in the photoemission process and the initial energy spread. However, a smaller emission spot on the cathode is not a dominant driver for enhancing time resolution. Space charge induced temporal broadening shows a close to

  14. Dynamic correlation in the electron angular distribution in ionization of helium by ion impact

    Energy Technology Data Exchange (ETDEWEB)

    Monti, J M; Fojon, O A; Rivarola, R D [Instituto de Fisica Rosario (CONICET-UNR) and Facultad de Ciencias Exactas, IngenierIa y Agrimensura, Universidad Nacional de Rosario, Avenida Pellegrini 250, 2000 Rosario (Argentina); Hanssen, J, E-mail: rivarola@fceia.unr.edu.ar [Institut de Chimie, Physique et Materiaux, Laboratoire de Physique Moleculaire et des Collisions, Universite Paul Verlaine - Metz, 1 Bv. Arago, 57078 Metz Cedex 3 (France)

    2011-04-01

    Single ionization of helium by proton impact is investigated in terms of a four-body distorted wave model. In this approximation both electrons are considered as active, being one of them ionized whereas the other remains in a residual target bound state. The influence of dynamic correlation between electrons is investigated by comparison with a four-body uncorrelated distorted wave model. Double differential cross sections as a function of the emission angle for fixed electron energies and different collision energies are presented.

  15. Beam dynamics analysis in pulse compression using electron beam compact simulator for Heavy Ion Fusion

    Directory of Open Access Journals (Sweden)

    Kikuchi Takashi

    2013-11-01

    Full Text Available In a final stage of an accelerator system for heavy ion inertial fusion (HIF, pulse shaping and beam current increase by bunch compression are required for effective pellet implosion. A compact simulator with an electron beam was constructed to understand the beam dynamics. In this study, we investigate theoretically and numerically the beam dynamics for the extreme bunch compression in the final stage of HIF accelerator complex. The theoretical and numerical results implied that the compact experimental device simulates the beam dynamics around the stagnation point for initial low temperature condition.

  16. Structure and Dynamics of Electron Injection and Charge Recombination in i-Motif DNA Conjugates.

    Science.gov (United States)

    Fujii, Taiga; K Thazhathveetil, Arun; Yildirim, Ilyas; Young, Ryan M; Wasielewski, Michael R; Schatz, George C; Lewis, Frederick D

    2017-08-31

    The dynamics of electron injection have been investigated in intramolecular i-motif conjugates possessing stilbenediether (Sd) and perylenediimide (PDI) chromophores separated by either four or six hemiprotonated cytosine C-C base pairs assembled with synthetic loops. Circular dichroism spectra are consistent with the formation of i-motif structures in the absence or presence of Sd and PDI chromophores. The fluorescence of the Sd chromophore is essentially completely quenched by neighboring C-C base pairs, consistent with their function as an electron donor and electron acceptor, respectively. However, the fluorescence of the PDI chromophore is only partially quenched. The dynamics of electron injection from singlet Sd into the i-motif and subsequent charge recombination has been determined by femtosecond transient absorption (fsTA) spectroscopy and compared with the results for electron injection and charge recombination in Sd-linked hairpins possessing cytosine-guanine (C-G) or 5-fluorouracil-adenine (F-A) base pairs. While charge injection is ultrafast (electron trap is not observed. The absence of electron transport is related to the structure of the stacked C-C base pairs in the i-motif.

  17. The effects of magnetospheric processes on relativistic electron dynamics in the Earth's outer radiation belt

    Science.gov (United States)

    Tang, C. L.; Wang, Y. X.; Ni, B.; Su, Z. P.; Reeves, G. D.; Zhang, J.-C.; Baker, D. N.; Spence, H. E.; Funsten, H. O.; Blake, J. B.

    2017-10-01

    Using the electron phase space density (PSD) data measured by Van Allen Probe A from January 2013 to April 2015, we investigate the effects of magnetospheric processes on relativistic electron dynamics in the Earth's outer radiation belt during 50 geomagnetic storms. A statistical study shows that the maximum electron PSDs for various μ (μ = 630, 1096, 2290, and 3311 MeV/G) at L* 4.0 after the storm peak have good correlations with storm intensity (cc 0.70). This suggests that the occurrence and magnitude of geomagnetic storms are necessary for relativistic electron enhancements at the inner edge of the outer radiation belt (L* = 4.0). For moderate or weak storm events (SYM-Hmin > -100 nT) with weak substorm activity (AEmax 0.77). For storm events with intense substorms after the storm peak, relativistic electron enhancements at L* = 4.5 and 5.0 are observed. This shows that intense substorms during the storm recovery phase are crucial to relativistic electron enhancements in the heart of the outer radiation belt. Our statistics study suggests that magnetospheric processes during geomagnetic storms have a significant effect on relativistic electron dynamics.

  18. Mapping Carrier Dynamics on Material Surfaces in Space and Time using Scanning Ultrafast Electron Microscopy

    KAUST Repository

    Sun, Jingya

    2016-02-25

    Selectively capturing the ultrafast dynamics of charge carriers on materials surfaces and at interfaces is crucial to the design of solar cells and optoelectronic devices. Despite extensive research efforts over the past few decades, information and understanding about surface-dynamical processes, including carrier trapping and recombination remains extremely limited. A key challenge is to selectively map such dynamic processes, a capability that is hitherto impractical by time-resolved laser techniques, which are limited by the laser’s relatively large penetration depth and consequently they record mainly bulk information. Such surface dynamics can only be mapped in real space and time by applying four-dimensional (4D) scanning ultrafast electron microscopy (S-UEM), which records snapshots of materials surfaces with nanometer spatial and sub-picosecond temporal resolutions. In this method, the secondary electron (SE) signal emitted from the sample’s surface is extremely sensitive to the surface dynamics and is detected in real time. In several unique applications, we spatially and temporally visualize the SE energy gain and loss, the charge carrier dynamics on the surface of InGaN nanowires and CdSe single crystals and its powder film. We also provide the mechanisms for the observed dynamics, which will be the foundation for future potential applications of S-UEM to a wide range of studies on material surfaces and device interfaces.

  19. Electron-phonon scattering from Green’s function transport combined with molecular dynamics

    DEFF Research Database (Denmark)

    Markussen, Troels; Palsgaard, Mattias Lau Nøhr; Stradi, Daniele

    2017-01-01

    We present a conceptually simple method for treating electron-phonon scattering and phonon limited mobilities. By combining Green’s function based transport calculations and molecular dynamics, we obtain a temperature dependent transmission from which we evaluate the mobility. We validate our...

  20. Modeling radiation belt electron dynamics during GEM challenge intervals with the DREAM3D diffusion model

    NARCIS (Netherlands)

    W. Tu (Weichao); G.S. Cunningham; Y. Chen; M.G. Henderson; E. Camporeale (Enrico); G.D. Reeves (Geoffrey)

    2013-01-01

    textabstractAs a response to the Geospace Environment Modeling (GEM) “Global Radiation Belt Modeling Challenge,” a 3D diffusion model is used to simulate the radiation belt electron dynamics during two intervals of the Combined Release and Radiation Effects Satellite (CRRES) mission, 15 August to 15

  1. Nonadiabatic dynamics of photoinduced proton-coupled electron transfer: comparison of explicit and implicit solvent simulations.

    Science.gov (United States)

    Auer, Benjamin; Soudackov, Alexander V; Hammes-Schiffer, Sharon

    2012-07-05

    Theoretical approaches for simulating the ultrafast dynamics of photoinduced proton-coupled electron transfer (PCET) reactions in solution are developed and applied to a series of model systems. These processes are simulated by propagating nonadiabatic surface hopping trajectories on electron-proton vibronic surfaces that depend on the solute and solvent nuclear coordinates. The PCET system is represented by a four-state empirical valence bond model, and the solvent is treated either as explicit solvent molecules or as a dielectric continuum, in which case the solvent dynamics is described in terms of two collective solvent coordinates corresponding to the energy gaps associated with electron and proton transfer. The explicit solvent simulations reveal two distinct solvent relaxation time scales, where the faster time scale relaxation corresponds to librational motions of solvent molecules in the first solvation shell, and the slower time scale relaxation corresponds to the bulk solvent dielectric response. The charge transfer dynamics is strongly coupled to both the fast and slow time scale solvent dynamics. The dynamical multistate continuum theory is extended to include the effects of two solvent relaxation time scales, and the resulting coupled generalized Langevin equations depend on parameters that can be extracted from equilibrium molecular dynamics simulations. The implicit and explicit solvent approaches lead to qualitatively similar charge transfer and solvent dynamics for model PCET systems, suggesting that the implicit solvent treatment captures the essential elements of the nonequilibrium solvent dynamics for many systems. A combination of implicit and explicit solvent approaches will enable the investigation of photoinduced PCET processes in a variety of condensed phase systems.

  2. Nanosecond time-resolved investigations using the in situ of dynamic transmission electron microscope (DTEM).

    Science.gov (United States)

    LaGrange, Thomas; Campbell, Geoffrey H; Reed, B W; Taheri, Mitra; Pesavento, J Bradley; Kim, Judy S; Browning, Nigel D

    2008-10-01

    Most biological processes, chemical reactions and materials dynamics occur at rates much faster than can be captured with standard video rate acquisition methods in transmission electron microscopes (TEM). Thus, there is a need to increase the temporal resolution in order to capture and understand salient features of these rapid materials processes. This paper details the development of a high-time resolution dynamic transmission electron microscope (DTEM) that captures dynamics in materials with nanosecond time resolution. The current DTEM performance, having a spatial resolution <10nm for single-shot imaging using 15ns electron pulses, will be discussed in the context of experimental investigations in solid state reactions of NiAl reactive multilayer films, the study of martensitic transformations in nanocrystalline Ti and the catalytic growth of Si nanowires. In addition, this paper will address the technical issues involved with high current, electron pulse operation and the near-term improvements to the electron optics, which will greatly improve the signal and spatial resolutions, and to the laser system, which will allow tailored specimen and photocathode drive conditions.

  3. Dynamic tunneling force microscopy for characterizing electronic trap states in non-conductive surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Wang, R.; Williams, C. C., E-mail: clayton@physics.utah.edu [Department of Physics and Astronomy, University of Utah, Salt Lake City, Utah 84112 (United States)

    2015-09-15

    Dynamic tunneling force microscopy (DTFM) is a scanning probe technique for real space mapping and characterization of individual electronic trap states in non-conductive films with atomic scale spatial resolution. The method is based upon the quantum mechanical tunneling of a single electron back and forth between a metallic atomic force microscopy tip and individual trap states in completely non-conducting surface. This single electron shuttling is measured by detecting the electrostatic force induced on the probe tip at the shuttling frequency. In this paper, the physical basis for the DTFM method is unfolded through a physical model and a derivation of the dynamic tunneling signal as a function of several experimental parameters is shown. Experimental data are compared with the theoretical simulations, showing quantitative consistency and verifying the physical model used. The experimental system is described and representative imaging results are shown.

  4. Nonadiabatic study of dynamic electronic effects during brittle fracture of silicon.

    Science.gov (United States)

    Theofanis, Patrick L; Jaramillo-Botero, Andres; Goddard, William A; Xiao, Hai

    2012-01-27

    It has long been observed that brittle fracture of materials can lead to emission of high energy electrons and UV photons, but an atomistic description of the origin of such processes has lacked. We report here on simulations using a first-principles-based electron force field methodology with effective core potentials to describe the nonadiabatic quantum dynamics during brittle fracture in silicon crystal. Our simulations replicate the correct response of the crack tip velocity to the threshold critical energy release rate, a feat that is inaccessible to quantum mechanics methods or conventional force-field-based molecular dynamics. We also describe the crack induced voltages, current bursts, and charge carrier production observed experimentally during fracture but not previously captured in simulations. We find that strain-induced surface rearrangements and local heating cause ionization of electrons at the fracture surfaces.

  5. Imaging Magnetic Vortices Dynamics Using Lorentz Electron Microscopy with GHz Excitations

    Science.gov (United States)

    Zhu, Yimei

    2015-03-01

    Magnetic vortices in thin films are naturally formed spiral spin configurations with a core polarization pointing out of the film plane. They typically represent ground states with high structural and thermal stability as well as four different chirality-polarity combinations, offering great promise in the development of spin-based devices. For applications to spin oscillators, non-volatile memory and logic devices, the fundamental understanding and precise control of vortex excitations and dynamic switching behavior are essential. The compact dimensionality and fast spin dynamics set grand challenges for direct imaging technologies. Recently, we have developed a unique method to directly visualize the dynamic magnetic vortex motion using advanced Lorentz electron microscopy combined with GHz electronic excitations. It enables us to map the orbit of a magnetic vortex core in a permalloy square with Material Sciences and Engineering Division, under Contract No. DE-AC02-98CH10886.

  6. Ultrafast XUV spectroscopy: Unveiling the nature of electronic couplings in molecular dynamics

    Science.gov (United States)

    Timmers, Henry Robert

    Molecules are traditionally treated quantum mechanically using the Born-Oppenheimer formalism. In this formalism, different electronic states of the molecule are treated independently. However, most photo-initiated phenomena occurring in nature are driven by the couplings between different electronic states in both isolated molecules and molecular aggregates, and therefore occur beyond the Born-Oppenheimer formalism. These couplings are relevant in reactions relating to the perception of vision in the human eye, the oxidative damage and repair of DNA, the harvesting of light in photosynthesis, and the transfer of charge across large chains of molecules. While these reaction dynamics have traditionally been studied with visible and ultraviolet spectroscopy, attosecond XUV pulses formed through the process of high harmonic generation form a perfect tool for probing coupled electronic dynamics in molecules. In this thesis, I will present our work in using ultrafast, XUV spectroscopy to study these dynamics in molecules of increasing complexity. We begin by probing the relaxation dynamics of superexcited states in diatomic O 2. These states can relax via two types of electronic couplings, either through autoionization or neutral dissociation. We find that our pump-probe scheme can disentangle the two relaxation mechanisms and independently measure their contributing lifetimes. Next, we present our work in observing a coherent electron hole wavepacket initiated by the ionization of polyatomic CO 2 near a conical intersection. The electron-nuclear couplings near the conical intersection drive the electron hole between different orbital configurations. We find that we can not only measure the lifetime of quantum coherence in the electron hole wavepacket, but also control its evolution with a strong, infrared probing field. Finally, we propose an experiment to observe the migration of an electron hole across iodobenzene on the few-femtosecond timescale. We present

  7. Femtochemistry in the electronic ground state: Dynamic Stark control of vibrational dynamics

    DEFF Research Database (Denmark)

    Shu, Chuan-Cun; Thomas, Esben Folger; Henriksen, Niels Engholm

    2017-01-01

    We study the interplay of vibrational and rotational excitation in a diatomic molecule due to the non-resonant dynamic Stark effect. With a fixed peak intensity, optimal Gaussian pulse durations for maximizing vibrational or rotational transitions are obtained analytically and confirmed numerically...

  8. Practical Considerations for High Spatial and Temporal Resolution Dynamic Transmission Electron Microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Armstrong, M; Boyden, K; Browning, N D; Campbell, G H; Colvin, J D; DeHope, B; Frank, A M; Gibson, D J; Hartemann, F; Kim, J S; King, W E; LaGrange, T B; Pyke, B J; Reed, B W; Shuttlesworth, R M; Stuart, B C; Torralva, B R

    2006-05-01

    Although recent years have seen significant advances in the spatial resolution possible in the transmission electron microscope (TEM), the temporal resolution of most microscopes is limited to video rate at best. This lack of temporal resolution means that our understanding of dynamic processes in materials is extremely limited. High temporal resolution in the TEM can be achieved, however, by replacing the normal thermionic or field emission source with a photoemission source. In this case the temporal resolution is limited only by the ability to create a short pulse of photoexcited electrons in the source, and this can be as short as a few femtoseconds. The operation of the photo-emission source and the control of the subsequent pulse of electrons (containing as many as 5 x 10{sup 7} electrons) create significant challenges for a standard microscope column that is designed to operate with a single electron in the column at any one time. In this paper, the generation and control of electron pulses in the TEM to obtain a temporal resolution <10{sup -6} s will be described and the effect of the pulse duration and current density on the spatial resolution of the instrument will be examined. The potential of these levels of temporal and spatial resolution for the study of dynamic materials processes will also be discussed.

  9. Photoinduced Interfacial Electron Injection Dynamics in Dye-Sensitized Solar Cells under Photovoltaic Operating Conditions.

    Science.gov (United States)

    Teuscher, Joël; Décoppet, Jean-David; Punzi, Angela; Zakeeruddin, Shaik M; Moser, Jacques-E; Grätzel, Michael

    2012-12-20

    We report a pump-probe spectroscopy study of electron injection rates in dye-sensitized solar cell (DSSC) devices. We examine the case of working devices employing an N719 ruthenium sensitizer and an iodide electrolyte. Electron injection is found to occur mainly on a sub-100 fs time scale, followed by a slower component with a lifetime of 26.9 ps, in accordance with previous reports on model samples. The amplitude of this latter component varies with electrolyte composition from 25 to 9%. The appearance of slower components in the electron injection dynamics may be attributed to an aggregated or weakly bound state of the surface-adsorbed N719 sensitizer. Further measurements are reported varying the cell light bias and load conditions, revealing no influence on electron injection dynamics. No other electron injection event is found to occur up to 1 ns. These results show no evidence for a slowdown of electron injection under working conditions compared to model systems for the electrolytes examined in this study.

  10. Practical considerations for high spatial and temporal resolution dynamic transmission electron microscopy

    Energy Technology Data Exchange (ETDEWEB)

    Armstrong, Michael R. [Materials Science and Technology Division, Chemistry and Materials Science Directorate, Lawrence Livermore National Laboratory, P.O. Box 808, L-356, Livermore, CA 94550 (United States)], E-mail: armstrong30@llnl.gov; Boyden, Ken [Materials Science and Technology Division, Chemistry and Materials Science Directorate, Lawrence Livermore National Laboratory, P.O. Box 808, L-356, Livermore, CA 94550 (United States); Browning, Nigel D. [Materials Science and Technology Division, Chemistry and Materials Science Directorate, Lawrence Livermore National Laboratory, P.O. Box 808, L-356, Livermore, CA 94550 (United States); Department of Chemical Engineering and Materials Science, University of California-Davis, One Shields Avenue, Davis, CA 95616 (United States); Campbell, Geoffrey H.; Colvin, Jeffrey D.; De Hope, William J.; Frank, Alan M. [Materials Science and Technology Division, Chemistry and Materials Science Directorate, Lawrence Livermore National Laboratory, P.O. Box 808, L-356, Livermore, CA 94550 (United States); Gibson, David J.; Hartemann, Fred [N Division, Physics and Advanced Technologies Directorate, Lawrence Livermore National Laboratory, P.O. Box 808, L-280, Livermore, CA 94550 (United States); Kim, Judy S. [Materials Science and Technology Division, Chemistry and Materials Science Directorate, Lawrence Livermore National Laboratory, P.O. Box 808, L-356, Livermore, CA 94550 (United States); Department of Chemical Engineering and Materials Science, University of California-Davis, One Shields Avenue, Davis, CA 95616 (United States); King, Wayne E.; La Grange, Thomas B.; Pyke, Ben J.; Reed, Bryan W.; Shuttlesworth, Richard M.; Stuart, Brent C.; Torralva, Ben R. [Materials Science and Technology Division, Chemistry and Materials Science Directorate, Lawrence Livermore National Laboratory, P.O. Box 808, L-356, Livermore, CA 94550 (United States)

    2007-04-15

    Although recent years have seen significant advances in the spatial resolution possible in the transmission electron microscope (TEM), the temporal resolution of most microscopes is limited to video rate at best. This lack of temporal resolution means that our understanding of dynamic processes in materials is extremely limited. High temporal resolution in the TEM can be achieved, however, by replacing the normal thermionic or field emission source with a photoemission source. In this case the temporal resolution is limited only by the ability to create a short pulse of photoexcited electrons in the source, and this can be as short as a few femtoseconds. The operation of the photo-emission source and the control of the subsequent pulse of electrons (containing as many as 5x10{sup 7} electrons) create significant challenges for a standard microscope column that is designed to operate with a single electron in the column at any one time. In this paper, the generation and control of electron pulses in the TEM to obtain a temporal resolution <10{sup -6} s will be described and the effect of the pulse duration and current density on the spatial resolution of the instrument will be examined. The potential of these levels of temporal and spatial resolution for the study of dynamic materials processes will also be discussed.

  11. Cryo-electron microscopy for structural analysis of dynamic biological macromolecules.

    Science.gov (United States)

    Murata, Kazuyoshi; Wolf, Matthias

    2018-02-01

    Since the introduction of what became today's standard for cryo-embedding of biological macromolecules at native conditions more than 30years ago, techniques and equipment have been drastically improved and the structure of biomolecules can now be studied at near atomic resolution by cryo-electron microscopy (cryo-EM) while capturing multiple dynamic states. Here we review the recent progress in cryo-EM for structural studies of dynamic biological macromolecules. We provide an overview of the cryo-EM method and introduce contemporary studies to investigate biomolecular structure and dynamics, including examples from the recent literature. Cryo-EM is a powerful tool for the investigation of biological macromolecular structures including analysis of their dynamics by using advanced image-processing algorithms. The method has become even more widely applicable with present-day single particle analysis and electron tomography. The cryo-EM method can be used to determine the three-dimensional structure of biomacromolecules in near native condition at close to atomic resolution, and has the potential to reveal conformations of dynamic molecular complexes. This article is part of a Special Issue entitled "Biophysical Exploration of Dynamical Ordering of Biomolecular Systems" edited by Dr. Koichi Kato. Copyright © 2017 The Authors. Published by Elsevier B.V. All rights reserved.

  12. Spin dynamics in Kapitza-Dirac scattering of electrons from bichromatic laser fields

    CERN Document Server

    Dellweg, Matthias M; Müller, Carsten

    2016-01-01

    Kapitza-Dirac scattering of nonrelativistic electrons from counterpropagating bichromatic laser waves of linear polarization i s studied. The focus lies on the electronic spin dynamics in the Bragg regime when the laser fields possess a frequency ratio of two. To this end, the time-dependent Pauli equation is solved numerically, both in coordinate space and momentum space. Our numerical results are corroborated by analytical derivations. We demonstrate that, for certain incident electron momenta, the scattering crucially relies on the electron spin which undergo es characteristic Rabi-like oscillations. A parameter regime is identified where the Rabi oscillations reach maximum amplitude. We also briefly discuss spin-dependent Kapitza-Dirac scattering of protons.

  13. Simulating electron wave dynamics in graphene superlattices exploiting parallel processing advantages

    Science.gov (United States)

    Rodrigues, Manuel J.; Fernandes, David E.; Silveirinha, Mário G.; Falcão, Gabriel

    2018-01-01

    This work introduces a parallel computing framework to characterize the propagation of electron waves in graphene-based nanostructures. The electron wave dynamics is modeled using both "microscopic" and effective medium formalisms and the numerical solution of the two-dimensional massless Dirac equation is determined using a Finite-Difference Time-Domain scheme. The propagation of electron waves in graphene superlattices with localized scattering centers is studied, and the role of the symmetry of the microscopic potential in the electron velocity is discussed. The computational methodologies target the parallel capabilities of heterogeneous multi-core CPU and multi-GPU environments and are built with the OpenCL parallel programming framework which provides a portable, vendor agnostic and high throughput-performance solution. The proposed heterogeneous multi-GPU implementation achieves speedup ratios up to 75x when compared to multi-thread and multi-core CPU execution, reducing simulation times from several hours to a couple of minutes.

  14. A variational approach to nonsmooth dynamics applications in unilateral mechanics and electronics

    CERN Document Server

    Adly, Samir

    2017-01-01

    This brief examines mathematical models in nonsmooth mechanics and nonregular electrical circuits, including evolution variational inequalities, complementarity systems, differential inclusions, second-order dynamics, Lur'e systems and Moreau's sweeping process. The field of nonsmooth dynamics is of great interest to mathematicians, mechanicians, automatic controllers and engineers. The present volume acknowledges this transversality and provides a multidisciplinary view as it outlines fundamental results in nonsmooth dynamics and explains how to use them to study various problems in engineering. In particular, the author explores the question of how to redefine the notion of dynamical systems in light of modern variational and nonsmooth analysis. With the aim of bridging between the communities of applied mathematicians, engineers and researchers in control theory and nonlinear systems, this brief outlines both relevant mathematical proofs and models in unilateral mechanics and electronics.

  15. Freezing hot electrons. Electron transfer and solvation dynamics at D{sub 2}O and NH{sub 3}-metal interfaces

    Energy Technology Data Exchange (ETDEWEB)

    Staehler, A.J.

    2007-05-15

    The present work investigates the electron transfer and solvation dynamics at the D{sub 2}O/Cu(111), D{sub 2}O/Ru(001), and NH{sub 3}/Cu(111) interfaces using femtosecond time-resolved two-photon photoelectron spectroscopy. Within this framework, the influence of the substrate, adsorbate structure and morphology, solvation site, coverage, temperature, and solvent on the electron dynamics are studied, yielding microscopic insight into the underlying fundamental processes. Transitions between different regimes of ET, substrate-dominated, barrier-determined, strong, and weak coupling are observed by systematic variation of the interfacial properties and development of empirical model descriptions. It is shown that the fundamental steps of the interfacial electron dynamics are similar for all investigated systems: Metal electrons are photoexcited to unoccupied metal states and transferred into the adlayer via the adsorbate's conduction band. The electrons localize at favorable sites and are stabilized by reorientations of the surrounding polar solvent molecules. Concurrently, they decay back two the metal substrate, as it offers a continuum of unoccupied states. However, the detailed characteristics vary for the different investigated interfaces: For amorphous ice-metal interfaces, the electron transfer is initially, right after photoinjection, dominated by the substrate's electronic surface band structure. With increasing solvation, a transient barrier evolves at the interface that increasingly screens the electrons from the substrate. Tunneling through this barrier becomes the rate-limiting step for ET. The competition of electron decay and solvation leads to lifetimes of the solvated electrons in the order of 100 fs. Furthermore, it is shown that the electrons bind in the bulk of the ice layers, but on the edges of adsorbed D{sub 2}O clusters and that the ice morphology strongly influences the electron dynamics. For the amorphous NH{sub 3}/Cu(111

  16. Correlated electron dynamics and memory in time-dependent density functional theory

    Energy Technology Data Exchange (ETDEWEB)

    Thiele, Mark

    2009-07-28

    Time-dependent density functional theory (TDDFT) is an exact reformulation of the time-dependent many-electron Schroedinger equation, where the problem of many interacting electrons is mapped onto the Kohn-Sham system of noninteracting particles which reproduces the exact electronic density. In the Kohn-Sham system all non-classical many-body effects are incorporated in the exchange-correlation potential which is in general unknown and needs to be approximated. It is the goal of this thesis to investigate the connection between memory effects and correlated electron dynamics in strong and weak fields. To this end one-dimensional two-electron singlet systems are studied. At the same time these systems include the onedimensional helium atom model, which is an established system to investigate the crucial effects of correlated electron dynamics in external fields. The studies presented in this thesis show that memory effects are negligible for typical strong field processes. Here the approximation of the spatial nonlocality is of primary importance. For the photoabsorption spectra on the other hand the neglect of memory effects leads to qualitative and quantitative errors, which are shown to be connected to transitions of double excitation character. To develop a better understanding of the conditions under which memory effects become important quantum fluid dynamics has been found to be especially suitable. It represents a further exact reformulation of the quantum mechanic many-body problem which is based on hydrodynamic quantities such as density and velocity. Memory effects are shown to be important whenever the velocity field develops strong gradients and dissipative effects contribute. (orig.)

  17. Correlated electron-nuclear dynamics in above-threshold multiphoton ionization of asymmetric molecule

    Science.gov (United States)

    Wang, Zhuo; Li, Min; Zhou, Yueming; Lan, Pengfei; Lu, Peixiang

    2017-02-01

    The partition of the photon energy into the subsystems of molecules determines many photon-induced chemical and physical dynamics in laser-molecule interactions. The electron-nuclear energy sharing from multiphoton ionization of molecules has been used to uncover the correlated dynamics of the electron and fragments. However, most previous studies focus on symmetric molecules. Here we study the electron-nuclear energy sharing in strong-field photoionization of HeH2+ by solving the one-dimensional time-dependent Schrödinger equation (TDSE). Compared with symmetric molecules, the joint electron-nuclear energy spectrum (JES) of HeH2+ reveals an anomalous energy shift at certain nuclear energies, while it disappears at higher and lower nuclear energies. Through tracing the time evolution of the wavepacket of bound states, we identify that this energy shift originates from the joint effect of the Stark shift, associated with the permanent dipole, and the Autler-Townes effect due to the coupling of the 2pσ and 2sσ states in strong fields. The energy shift in the JES appears at certain nuclear distances only when both Stark effect and Autler-Townes effect play important roles. We further demonstrate that the electron-nuclei energy sharing can be controlled by varying laser intensity for asymmetric molecules, providing alternative approaches to manipulate photochemical reactions for more complex molecules.

  18. Poisson-distributed electron-transfer dynamics from single quantum dots to C60 molecules.

    Science.gov (United States)

    Song, Nianhui; Zhu, Haiming; Jin, Shengye; Zhan, Wei; Lian, Tianquan

    2011-01-25

    Functional quantum dot (QD)-based nanostructures are often constructed through the self-assembly of QDs with binding partners (molecules or other nanoparticles), a process that leads to a statistical distribution of the number of binding partners. Using single QD fluorescence spectroscopy, we probe this distribution and its effect on the function (electron-transfer dynamics) in QD-C60 complexes. Ensemble-averaged transient absorption and fluorescence decay as well as single QD fluorescence decay measurements show that the QD exciton emission was quenched by electron transfer from the QD to C60 molecules and the electron-transfer rate increases with the C60-to-QD ratio. The electron-transfer rate of single QD-C60 complexes fluctuates with time and varies among different QDs. The standard deviation increases linearly with the average of electron-transfer rates of single QD-C60 complexes, and the distributions of both quantities obey Poisson statistics. The observed distributions of single QD-C60 complexes and ensemble-averaged fluorescence decay kinetics can be described by a model that assumes a Poisson distribution of the number of adsorbed C60 molecules per QD. Our findings suggest that, in self-assembled QD nanostructures, the statistical distribution of the number of adsorbed partners can dominate the distributions of the averages and standard deviation of their interfacial dynamical properties.

  19. Charge transfer dynamics from adsorbates to surfaces with single active electron and configuration interaction based approaches

    Energy Technology Data Exchange (ETDEWEB)

    Ramakrishnan, Raghunathan, E-mail: r.ramakrishnan@unibas.ch [Institute of Physical Chemistry, National Center for Computational Design and Discovery of Novel Materials (MARVEL), Department of Chemistry, University of Basel, Klingelbergstrasse 80, CH-4056 Basel (Switzerland); Nest, Mathias [Theoretische Chemie, Technische Universität München, Lichtenbergstr. 4, 85747 Garching (Germany)

    2015-01-13

    Highlights: • We model electron dynamics across cyano alkanethiolates attached to gold cluster. • We present electron transfer time scales from TD-DFT and TD-CI based simulations. • Both DFT and CI methods qualitatively predict the trend in time scales. • TD-CI predicts the experimental relative time scale very accurately. - Abstract: We employ wavepacket simulations based on many-body time-dependent configuration interaction (TD-CI), and single active electron theories, to predict the ultrafast molecule/metal electron transfer time scales, in cyano alkanethiolates bonded to model gold clusters. The initial states represent two excited states where a valence electron is promoted to one of the two virtual π{sup ∗} molecular orbitals localized on the cyanide fragment. The ratio of the two time scales indicate the efficiency of one charge transfer channel over the other. In both our one-and many-electron simulations, this ratio agree qualitatively with each other as well as with the previously reported experimental time scales (Blobner et al., 2012), measured for a macroscopic metal surface. We study the effect of cluster size and the description of electron correlation on the charge transfer process.

  20. Radiation belt electron dynamics at low L (Van Allen Probes era versus previous two solar cycles

    Science.gov (United States)

    Li, X.; Baker, D. N.; Zhao, H.; Zhang, K.; Jaynes, A. N.; Schiller, Q.; Kanekal, S. G.; Blake, J. B.; Temerin, M.

    2017-05-01

    Long-term (>2 solar cycles) measurements reveal that MeV electron fluxes, solar wind speed, and geomagnetic activity have been extremely low during this current solar cycle, including years before and during the Van Allen Probes era. This study examines solar wind speed, the geomagnetic storm index (Dst), >2 MeV electrons at geostationary orbit, and 2 MeV electrons across various L shells measured by Solar Anomalous Magnetospheric Particle Explorer in low Earth orbit (LEO) and by the Van Allen Probes/Relativistic Electron and Proton Telescope (REPT) in a geotransfer-like orbit; the latter measurements are normalized to LEO based on comparison with Colorado Student Space Weather Experiment/Relativistic Electron and Proton Telescope integrated little experiment (REPTile) measurements in LEO. The average ratio of REPTile/REPT varies in a systematic manner with L, 16% at L = 2.7, decreasing with L and reaching 0.7% at L = 4.7, and increasing again with L though with greater uncertainty. We show that there have been no 2 MeV electron enhancements inside L 2.6 since 2006, prior to which numerous penetrations of 2 MeV electrons into L Van Allen Probes, which have been providing the finest measurements but in operation during a quiet solar activity period, may not be representative of radiation belt dynamics, particularly for the inner edge of the outer belt, during other solar cycle phases.

  1. Dynamical characteristics of Rydberg electrons released by a weak electric field

    CERN Document Server

    Diesen, Elias; Richter, Martin; Kunitski, Maksim; Dörner, Reinhard; Rost, Jan M

    2015-01-01

    The dynamics of ultra-slow electrons in the combined potential of an ionic core and a static electric field is discussed. With state-of-the-art detection it is possible to create such electrons through strong intense-field photo-absorption and to detect them via high-resolution time-of-flight spectroscopy despite their very low kinetic energy. The characteristic feature of their momentum spectrum, which emerges at the same position for different laser orientations, is derived and could be revealed experimentally with an energy resolution of the order of 1meV.

  2. Direct Measurement of the Electron Energy Relaxation Dynamics in Metallic Wires

    Science.gov (United States)

    Pinsolle, Edouard; Rousseau, Alexandre; Lupien, Christian; Reulet, Bertrand

    2016-06-01

    We present measurements of the dynamical response of thermal noise to an ac excitation in conductors at low temperature. From the frequency dependence of this response function—the (noise) thermal impedance—in the range 1 kHz-1 GHz we obtain direct determinations of the inelastic relaxation times relevant in metallic wires at low temperature: the electron-phonon scattering time and the diffusion time of electrons along the wires. Combining these results with that of resistivity provides a measurement of heat capacity of samples made of thin film. The simplicity and reliability of this technique makes it very promising for future applications in other systems.

  3. Centrifugal separation and equilibration dynamics in an electron-antiproton plasma

    CERN Document Server

    Andresen, G B; Baquero-Ruiz, Marcelo; Bertsche, William; Bowe, Paul D; Butler, Eoin; Cesar, Claudio L; Chapman, Steven; Charlton, Michael; Deller, A; Eriksson, S; Fajans, Joel; Friesen, Tim; Fujiwara, Makoto C; Gill, David R; Gutierrez, A; Hangst, Jeffrey S; Hardy, Walter N; Hayden, Michael E; Humphries, Andrew J; Hydomako, Richard; Jonsell, Svante; Madsen, Niels; Menary, Scott; Nolan, Paul; Olin, Art; Povilus, Alexander; Pusa, Petteri; Robicheaux, Francis; Sarid, Eli; Silveira, Daniel M; So, Chukman; Storey, James W; Thompson, Robert I; van der Werf, Dirk P; Wurtele, Jonathan S; Yamazaki, Yasunori

    2011-01-01

    Charges in cold, multiple-species, non-neutral plasmas separate radially by mass, forming centrifugally-separated states. Here, we report the first detailed measurements of such states in an electron-antiproton plasma, and the first observations of the separation dynamics in any centrifugally-separated system. While the observed equilibrium states are expected and in agreement with theory, the equilibration time is approximately constant over a wide range of parameters, a surprising and as yet unexplained result. Electron-antiproton plasmas play a crucial role in antihydrogen trapping experiments.

  4. Vlasov Fokker Planck Study of Electron Dynamics in the Scrape Off Layer with Expander Divertor

    Science.gov (United States)

    Gupta, S.; Yushmanov, P.; Tae Team, The; Barnes, D. C.

    2017-10-01

    Control of electron heat losses in the open field region surrounding a Field Reversed Configuration (FRC) is important for sustaining higher temperatures in the FRC core, for favorable beam energy deposition, and for reducing loads on divertor plates. At TAE, a magnetic expander will be used to attain these objectives in the new C-2W machine and to comprehensively study expander divertor physics. The electron dynamics and electrostatic potential formation in the expanding magnetic field is analyzed using a 3-D (2 velocity and 1 spatial) Vlasov Fokker Planck code (Ksol). Numerical results showing the effect of collisionality, current, Zeff, incoming distribution etc., on the formation of electrostatic potentials will be presented.

  5. Transient mid-IR study of electron dynamics in TiO2 conduction band.

    Science.gov (United States)

    Sá, Jacinto; Friedli, Peter; Geiger, Richard; Lerch, Philippe; Rittmann-Frank, Mercedes H; Milne, Christopher J; Szlachetko, Jakub; Santomauro, Fabio G; van Bokhoven, Jeroen A; Chergui, Majed; Rossi, Michel J; Sigg, Hans

    2013-04-07

    The dynamics of TiO2 conduction band electrons were followed with a novel broadband synchrotron-based transient mid-IR spectroscopy setup. The lifetime of conduction band electrons was found to be dependent on the injection method used. Direct band gap excitation results in a lifetime of 2.5 ns, whereas indirect excitation at 532 nm via Ru-N719 dye followed by injection from the dye into TiO2 results in a lifetime of 5.9 ns.

  6. Cryo-electron microscopy snapshots of the spliceosome: structural insights into a dynamic ribonucleoprotein machine.

    Science.gov (United States)

    Fica, Sebastian M; Nagai, Kiyoshi

    2017-10-05

    The spliceosome excises introns from pre-messenger RNAs using an RNA-based active site that is cradled by a dynamic protein scaffold. A recent revolution in cryo-electron microscopy (cryo-EM) has led to near-atomic-resolution structures of key spliceosome complexes that provide insight into the mechanism of activation, splice site positioning, catalysis, protein rearrangements and ATPase-mediated dynamics of the active site. The cryo-EM structures rationalize decades of observations from genetic and biochemical studies and provide a molecular framework for future functional studies.

  7. Dynamic covalent bond from first principles: Diarylbibenzofuranone structural, electronic, and oxidation studies.

    Science.gov (United States)

    Schleder, Gabriel R; Fazzio, Adalberto; Arantes, Jeverson T

    2017-12-05

    A structure that can self-heal under standard conditions is a challenge faced nowadays and is one of the most promising areas in smart materials science. This can be achieved by dynamic bonds, of which diarylbibenzofuranone (DABBF) dynamic covalent bond is an appealing solution. In this report, we studied the DABBF bond formation against arylbenzofuranone (ABF) and O 2 reaction (autoxidation). Our results show that the barrierless DABBF bond formation is preferred over autoxidation due to the charge transfer process that results in the weakly bonded superoxide. We calculated the electronic and structural properties using total energy density functional theory. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.

  8. Nonradiative Relaxation in Real-Time Electronic Dynamics OSCF2: Organolead Triiodide Perovskite.

    Science.gov (United States)

    Nguyen, Triet S; Parkhill, John

    2016-09-01

    We apply our recently developed nonequilibrium real-time time-dependent density functional theory (OSCF2) to investigate the transient spectrum and relaxation dynamics of the tetragonal structure of methylammonium lead triiodide perovskite (MAPbI3). We obtain an estimate of the interband relaxation kinetics and identify multiple ultrafast cooling channels for hot electrons and hot holes that largely corroborate the dual valence-dual conduction model. The computed relaxation rates and absorption spectra are in good agreement with the existing experimental data. We present the first ab initio simulations of the perovskite transient absorption (TA) spectrum, substantiating the assignment of induced bleaches and absorptions including a Pauli-bleach signal. This paper validates both OSCF2 as a good qualitative model of electronic dynamics, and the dominant interpretation of the TA spectrum of this material.

  9. Reduced electron exposure for energy-dispersive spectroscopy using dynamic sampling

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Yan; Godaliyadda, G. M. Dilshan; Ferrier, Nicola; Gulsoy, Emine B.; Bouman, Charles A.; Phatak, Charudatta

    2018-01-01

    Analytical electron microscopy and spectroscopy of biological specimens, polymers, and other beam sensitive materials has been a challenging area due to irradiation damage. There is a pressing need to develop novel imaging and spectroscopic imaging methods that will minimize such sample damage as well as reduce the data acquisition time. The latter is useful for high-throughput analysis of materials structure and chemistry. In this work, we present a novel machine learning based method for dynamic sparse sampling of EDS data using a scanning electron microscope. Our method, based on the supervised learning approach for dynamic sampling algorithm and neural networks based classification of EDS data, allows a dramatic reduction in the total sampling of up to 90%, while maintaining the fidelity of the reconstructed elemental maps and spectroscopic data. We believe this approach will enable imaging and elemental mapping of materials that would otherwise be inaccessible to these analysis techniques.

  10. Quantum-classical transition in the electron dynamics of thin metal films

    Energy Technology Data Exchange (ETDEWEB)

    Jasiak, R; Manfredi, G; Hervieux, P-A [Institut de Physique et Chimie des Materiaux, CNRS and Universite de Strasbourg, BP 43, F-67034 Strasbourg (France); Haefele, M [INRIA Nancy Grand-Est and Institut de Recherche en Mathematiques Avancees, 7 rue Rene Descartes, F-67084 Strasbourg (France)], E-mail: Giovanni.Manfredi@ipcms.u-strasbg.fr

    2009-06-15

    The quantum electrons dynamics in a thin metal film is studied numerically using the self-consistent Wigner-Poisson equations. The initial equilibrium is computed from the Kohn-Sham equations at finite temperature, and then mapped into the phase-space Wigner function. The time-dependent results are compared systematically with those obtained previously with a classical approach (Vlasov-Poisson equations). It is found that, for large excitations, the quantum and classical dynamics display the same low-frequency oscillations due to ballistic electrons bouncing back and forth on the film surfaces. However, below a certain excitation energy (roughly corresponding to one quantum of plasmon energy {Dirac_h}{omega}{sub p}), the quantum and classical results diverge, and the ballistic oscillations are no longer observed. These results provide an example of a quantum-classical transition that may be observed with current pump-probe experiments on thin metal films.

  11. Dynamical Birefringence: Electron-Hole Recollisions as Probes of Berry Curvature

    Directory of Open Access Journals (Sweden)

    Hunter B. Banks

    2017-11-01

    Full Text Available The direct measurement of Berry phases is still a great challenge in condensed-matter systems. The bottleneck has been the ability to adiabatically drive an electron coherently across a large portion of the Brillouin zone in a solid where the scattering is strong and complicated. We break through this bottleneck and show that high-order sideband generation (HSG in semiconductors is intimately affected by Berry phases. Electron-hole recollisions and HSG occur when a near-band-gap laser beam excites a semiconductor that is driven by sufficiently strong terahertz-frequency electric fields. We carry out experimental and theoretical studies of HSG from three GaAs/AlGaAs quantum wells. The observed HSG spectra contain sidebands up to the 90th order, to our knowledge the highest-order optical nonlinearity reported in solids. The highest-order sidebands are associated with electron-hole pairs driven coherently across roughly 10% of the Brillouin zone around the Γ point. The principal experimental claim is a dynamical birefringence: the intensity and polarization of the sidebands depend on the relative polarization of the exciting near-infrared (NIR and the THz electric fields, as well as on the relative orientation of the laser fields with the crystal. We explain dynamical birefringence by generalizing the three-step model for high-order harmonic generation. The hole accumulates Berry phases due to variation of its internal state as the quasimomentum changes under the THz field. Dynamical birefringence arises from quantum interference between time-reversed pairs of electron-hole recollision pathways. We propose a method to use dynamical birefringence to measure Berry curvature in solids.

  12. Temporal Dynamics and Electronic Nose Detection of Stink Bug-Induced Volatile Emissions from Cotton Bolls

    OpenAIRE

    Degenhardt, David C.; Greene, Jeremy K.; Ahmad Khalilian

    2012-01-01

    Management decisions for stink bugs (Pentatomidae) in Bt cotton are complicated by time-consuming sampling methods, and there is a need for more efficient detection tools. Volatile compounds are released from cotton bolls in response to feeding by stink bugs, and electronic nose (E-nose) technology may be useful for detecting boll damage. In this study, we investigated the temporal dynamics of volatile emissions in response to feeding by stink bugs and tested the ability of E-nose to discrimi...

  13. Tunable superlattice amplifiers based on dynamics of miniband electrons in electric and magnetic fields

    OpenAIRE

    Hyart, T. (Timo)

    2009-01-01

    Abstract The most important paradigms in quantum mechanics are probably a twolevel system, a harmonic oscillator and an ideal (infinite) periodic potential. The first two provide a starting point for understanding the phenomena in systems where the spectrum of energy levels is discrete, whereas the last one results in continuous energy bands. Here an attempt is made to study the dynamics of the electrons in a narrow miniband of a semiconductor superlattice under electric and magnetic field...

  14. The Atmospheric Scanning Electron Microscope with open sample space observes dynamic phenomena in liquid or gas

    Energy Technology Data Exchange (ETDEWEB)

    Suga, Mitsuo, E-mail: msuga@jeol.co.jp [Clair Project, JEOL Ltd., 3-1-2, Musashino, Akishima, Tokyo 196-8558 (Japan); Nishiyama, Hidetoshi; Konyuba, Yuji [Clair Project, JEOL Ltd., 3-1-2, Musashino, Akishima, Tokyo 196-8558 (Japan); Iwamatsu, Shinnosuke; Watanabe, Yoshiyuki [Yamagata Research Institute of Technology, 2-2-1, Matsuei, Yamagata, 990-2473 (Japan); Yoshiura, Chie; Ueda, Takumi [Graduate School of Pharmaceutical Sciences, The University of Tokyo, Hongo, Bunkyo-ku, Tokyo 113-0033 (Japan); Sato, Chikara, E-mail: ti-sato@aist.go.jp [Biomedical Research Institute, National Institute of Advanced Industrial Science and Technology (AIST), 1-1-4, Umezono, Tsukuba 305-8568 (Japan)

    2011-12-15

    Although conventional electron microscopy (EM) requires samples to be in vacuum, most chemical and physical reactions occur in liquid or gas. The Atmospheric Scanning Electron Microscope (ASEM) can observe dynamic phenomena in liquid or gas under atmospheric pressure in real time. An electron-permeable window made of pressure-resistant 100 nm-thick silicon nitride (SiN) film, set into the bottom of the open ASEM sample dish, allows an electron beam to be projected from underneath the sample. A detector positioned below captures backscattered electrons. Using the ASEM, we observed the radiation-induced self-organization process of particles, as well as phenomena accompanying volume change, including evaporation-induced crystallization. Using the electrochemical ASEM dish, we observed tree-like electrochemical depositions on the cathode. In silver nitrate solution, we observed silver depositions near the cathode forming incidental internal voids. The heated ASEM dish allowed observation of patterns of contrast in melting and solidifying solder. Finally, to demonstrate its applicability for monitoring and control of industrial processes, silver paste and solder paste were examined at high throughput. High resolution, imaging speed, flexibility, adaptability, and ease of use facilitate the observation of previously difficult-to-image phenomena, and make the ASEM applicable to various fields. -- Highlights: Black-Right-Pointing-Pointer Atmospheric SEM (ASEM) observes dynamic phenomena in liquid or gas in open ASEM dish. Black-Right-Pointing-Pointer Random motion and radiation-induced self-organization were observed. Black-Right-Pointing-Pointer Tree-like electrochemical deposition of gold was observed on an electrode in situ. Black-Right-Pointing-Pointer Temperature-dependent phase transitions of solder were dynamically observed in air. Black-Right-Pointing-Pointer Silver and solder pastes were easily and rapidly observed in air for process control.

  15. Dynamics of a Rydberg hydrogen atom near a metal surface in the electron-extraction scheme

    Energy Technology Data Exchange (ETDEWEB)

    Iñarrea, Manuel [Área de Física Aplicada, Universidad de La Rioja, Logroño (Spain); Lanchares, Víctor [Departamento de Matemáticas y Computación, Universidad de La Rioja, Logroño, La Rioja (Spain); Palacián, Jesús [Departamento de Ingeniería Matemática e Informática, Universidad Pública de Navarra, Pamplona (Spain); Pascual, Ana I. [Departamento de Matemáticas y Computación, Universidad de La Rioja, Logroño, La Rioja (Spain); Salas, J. Pablo, E-mail: josepablo.salas@unirioja.es [Área de Física Aplicada, Universidad de La Rioja, Logroño (Spain); Yanguas, Patricia [Departamento de Ingeniería Matemática e Informática, Universidad Pública de Navarra, Pamplona (Spain)

    2015-01-23

    We study the classical dynamics of a Rydberg hydrogen atom near a metal surface in the presence of a constant electric field in the electron-extraction situation [1], e.g., when the field attracts the electron to the vacuum. From a dynamical point of view, this field configuration provides a dynamics richer than in the usual ion-extraction scheme, because, depending on the values of field and the atom–surface distance, the atom can be ionized only towards the metal surface, only to the vacuum or to the both sides. The evolution of the phase space structure as a function of the atom–surface distance is explored in the bound regime of the atom. In the high energy regime, the ionization mechanism is also investigated. We find that the classical results of this work are in good agreement with the results obtained in the wave-packet propagation study carried out by So et al. [1]. - Highlights: • We study a classical hydrogen atom near a metal surface plus a electric field. • We explore the phase space structure as a function of the field strength. • We find most of the electronic orbits are oriented along the field direction. • We study the ionization of the atom for several atom–surface distances. • This classical study is in good agreement with the quantum results.

  16. Coupled electron-nuclear quantum dynamics through and around a conical intersection

    Science.gov (United States)

    Albert, Julian; Hader, Kilian; Engel, Volker

    2017-08-01

    In solving the time-dependent Schrödinger equation for a coupled electron-nuclear system, we study the motion of wave packets in a model which exhibits a conical intersection (CoIn) of adiabatic potential energy surfaces. Three different situations are studied. In the first case, an efficient non-adiabatic transition takes place while the wave packet passes the region of the CoIn. It is demonstrated that during these times, the nuclear probability density retains its Gaussian shape and the electronic density remains approximately constant. Second, dynamics are regarded where non-adiabatic transitions do not take place, and the nuclear dynamics follows a circle around the location of the CoIn. During this motion, the electronic density is shown to rotate. The comparison with the Born-Oppenheimer nuclear dynamics reveals the geometrical phase being associated with the circular motion. This phase is clearly revealed by an analysis of time-dependent autocorrelation functions and spectra obtained from the numerically exact and the Born-Oppenheimer calculation. The intermediate situation with a small non-adiabatic transition probability is characterized by wave-packet splitting into several fractions.

  17. The Effect of Magnetic Field Errors on Dynamical Friction in Electron Coolers

    CERN Document Server

    Bruhwiler, David L; Busby, Richard; Fedotov, Alexei V; Litvinenko, Vladimir N; Veitzer, Seth A

    2005-01-01

    A proposed luminosity upgrade to the Relativistic Heavy Ion Collider (RHIC) includes a novel electron cooling section,* which would use ~55 MeV electrons to cool fully-ionized 100 GeV/nucleon gold ions. A strong (1-5 T) solenoidal field will be used to magnetize the electrons and thus enhance the dynamical friction force on the ions. The physics of magnetized friction is being simulated for RHIC parameters, using the VORPAL code.** Most theoretical treatments for magnetized dynamical friction do not consider the effect of magnetic field errors, except in a parametric fashion.*** However, field errors can in some cases dramatically reduce the velocity drag and corresponding cooling rate. We present a simple analytical model for the magnetic field errors, which must be Lorentz transformed into the beam frame for use in our simulations. The simulated dynamical friction for the case of a perfect solenoidal field will be compared with results from this new model, for parameters relevant to RHIC.

  18. Direct simulation of proton-coupled electron transfer reaction dynamics and mechanisms

    Science.gov (United States)

    Kretchmer, Joshua S.; Miller, Thomas F., III

    2014-03-01

    Proton-coupled electron transfer (PCET) reactions, in which both an electron and an associated proton undergo reactive transfer, play an important role in many chemical and biological systems. Due to the complexity of this class of reactions, a variety of different mechanisms fall under the umbrella of PCET. However, the physical driving forces that determine the preferred mechanism in a given system still remain poorly understood. Towards this end, we extend ring polymer molecular dynamics (RPMD), a path-integral quantum dynamics method, to enable the direct simulation and characterization of PCET reaction dynamics in both fully atomistic and system-bath models of organometallic catalysts. In addition to providing validation for the simulation method via extensive comparison with existing PCET rate theories, we analyze the RPMD trajectories to investigate the competition between the concerted and sequential reaction mechanisms for PCET, elucidating the large role of the solvent in controlling the preferred mechanism. We further employ RPMD to determine the kinetics and mechanistic features of concerted PCET reactions across different regimes of electronic and vibrational coupling, providing evidence for a new and distinct PCET reaction mechanism.

  19. Photoinduced Electron Transfer in DNA: Charge Shift Dynamics Between 8-Oxo-Guanine Anion and Adenine.

    Science.gov (United States)

    Zhang, Yuyuan; Dood, Jordan; Beckstead, Ashley A; Li, Xi-Bo; Nguyen, Khiem V; Burrows, Cynthia J; Improta, Roberto; Kohler, Bern

    2015-06-18

    Femtosecond time-resolved IR spectroscopy is used to investigate the excited-state dynamics of a dinucleotide containing an 8-oxoguanine anion at the 5'-end and neutral adenine at the 3'-end. UV excitation of the dinucleotide transfers an electron from deprotonated 8-oxoguanine to its π-stacked neighbor adenine in less than 1 ps, generating a neutral 8-oxoguanine radical and an adenine radical anion. These species are identified by the excellent agreement between the experimental and calculated IR difference spectra. The quantum efficiency of this ultrafast charge shift reaction approaches unity. Back electron transfer from the adenine radical anion to the 8-oxguanine neutral radical occurs in 9 ps, or approximately 6 times faster than between the adenine radical anion and the 8-oxoguanine radical cation (Zhang, Y. et al. Proc. Natl. Acad. Sci. U.S.A. 2014, 111, 11612-11617). The large asymmetry in forward and back electron transfer rates is fully rationalized by semiclassical nonadiabatic electron transfer theory. Forward electron transfer is ultrafast because the driving force is nearly equal to the reorganization energy, which is estimated to lie between 1 and 2 eV. Back electron transfer is highly exergonic and takes place much more slowly in the Marcus inverted region.

  20. High Dynamic Range Pixel Array Detector for Scanning Transmission Electron Microscopy.

    Science.gov (United States)

    Tate, Mark W; Purohit, Prafull; Chamberlain, Darol; Nguyen, Kayla X; Hovden, Robert; Chang, Celesta S; Deb, Pratiti; Turgut, Emrah; Heron, John T; Schlom, Darrell G; Ralph, Daniel C; Fuchs, Gregory D; Shanks, Katherine S; Philipp, Hugh T; Muller, David A; Gruner, Sol M

    2016-02-01

    We describe a hybrid pixel array detector (electron microscope pixel array detector, or EMPAD) adapted for use in electron microscope applications, especially as a universal detector for scanning transmission electron microscopy. The 128×128 pixel detector consists of a 500 µm thick silicon diode array bump-bonded pixel-by-pixel to an application-specific integrated circuit. The in-pixel circuitry provides a 1,000,000:1 dynamic range within a single frame, allowing the direct electron beam to be imaged while still maintaining single electron sensitivity. A 1.1 kHz framing rate enables rapid data collection and minimizes sample drift distortions while scanning. By capturing the entire unsaturated diffraction pattern in scanning mode, one can simultaneously capture bright field, dark field, and phase contrast information, as well as being able to analyze the full scattering distribution, allowing true center of mass imaging. The scattering is recorded on an absolute scale, so that information such as local sample thickness can be directly determined. This paper describes the detector architecture, data acquisition system, and preliminary results from experiments with 80-200 keV electron beams.

  1. Beam Dynamics Simulation of Photocathode RF Electron Gun at the PBP-CMU Linac Laboratory

    Science.gov (United States)

    Buakor, K.; Rimjaem, S.

    2017-09-01

    Photocathode radio-frequency (RF) electron guns are widely used at many particle accelerator laboratories due to high quality of produced electron beams. By using a short-pulse laser to induce the photoemission process, the electrons are emitted with low energy spread. Moreover, the photocathode RF guns are not suffered from the electron back bombardment effect, which can cause the limited electron current and accelerated energy. In this research, we aim to develop the photocathode RF gun for the linac-based THz radiation source. Its design is based on the existing gun at the PBP-CMU Linac Laboratory. The gun consists of a one and a half cell S-band standing-wave RF cavities with a maximum electric field of about 60 MV/m at the centre of the full cell. We study the beam dynamics of electrons traveling through the electromagnetic field inside the RF gun by using the particle tracking program ASTRA. The laser properties i.e. transverse size and injecting phase are optimized to obtain low transverse emittance. In addition, the solenoid magnet is applied for beam focusing and emittance compensation. The proper solenoid magnetic field is then investigated to find the optimum value for proper emittance conservation condition.

  2. Electron dynamics during substorm dipolarization in Mercury's magnetosphere

    Directory of Open Access Journals (Sweden)

    D. C. Delcourt

    2005-11-01

    Full Text Available We examine the nonlinear dynamics of electrons during the expansion phase of substorms at Mercury using test particle simulations. A simple model of magnetic field line dipolarization is designed by rescaling a magnetic field model of the Earth's magnetosphere. The results of the simulations demonstrate that electrons may be subjected to significant energization on the time scale (several seconds of the magnetic field reconfiguration. In a similar manner to ions in the near-Earth's magnetosphere, it is shown that low-energy (up to several tens of eV electrons may not conserve the second adiabatic invariant during dipolarization, which leads to clusters of bouncing particles in the innermost magnetotail. On the other hand, it is found that, because of the stretching of the magnetic field lines, high-energy electrons (several keVs and above do not behave adiabatically and possibly experience meandering (Speiser-type motion around the midplane. We show that dipolarization of the magnetic field lines may be responsible for significant, though transient, (a few seconds precipitation of energetic (several keVs electrons onto the planet's surface. Prominent injections of energetic trapped electrons toward the planet are also obtained as a result of dipolarization. These injections, however, do not exhibit short-lived temporal modulations, as observed by Mariner-10, which thus appear to follow from a different mechanism than a simple convection surge.

  3. Mechanism and Dynamics of Electron Injection and Charge Recombination in DNA. Dependence on Neighboring Pyrimidines.

    Science.gov (United States)

    Gorczak, Natalie; Fujii, Taiga; Mishra, Ashutosh Kumar; Houtepen, Arjan J; Grozema, Ferdinand C; Lewis, Frederick D

    2015-06-18

    The mechanism and dynamics of photoinduced electron injection and charge recombination have been investigated for several series of DNA hairpins. The hairpins possess a stilbenediether linker, which serves as an electron donor and base pair stems that possess different pyrimidine bases adjacent to the linker. Hairpins with adjacent thymine-adenine (T-A) base pairs undergo fast electron injection and relatively slow charge recombination with rate constants that are not strongly dependent upon the following base pair. Hairpins with adjacent cytosine-guanine (C-G) base pairs undergo reversible electron injection and much faster charge recombination than those with adjacent T-A base pairs. Hairpins with 5-fluorouracil or other halogenated pyrimidines in their first and second base pair undergo fast electron injection and multiexponential charge recombination. The difference in kinetic behavior for the different series of hairpins and its implications for the formation of long-lived charge-separated states are discussed and compared to results reported previously for other electron-donor chromophores.

  4. Dynamic motions of ion acoustic waves in plasmas with superthermal electrons

    Energy Technology Data Exchange (ETDEWEB)

    Saha, Asit, E-mail: asit_saha123@rediffmail.com [Department of Mathematics, Sikkim Manipal Institute of Technology (India); Chatterjee, Prasanta [Department of Mathematics, Siksha Bhavana, Visva Bharati University (India); Wong, C.S. [Plasma Technology Research Centre, Department of Physics, University of Malaya, Kuala Lampur (Malaysia)

    2015-12-15

    The dynamic motions of ion acoustic waves an unmagnetized plasma with superthermal (q-non extensive) electrons are investigated employing the bifurcation theory of planar dynamical systems through direct approach. Using traveling wave transformation and initial conditions, basic equations are transformed to a planar dynamical system. Using numerical computations, all possible phase portraits of the dynamical system are presented. Corresponding to homoclinic and periodic orbits of the phase portraits, two new analytical forms of solitary and periodic wave solutions are derived depending on the non extensive parameter q and speed v of the traveling wave. Considering an external periodic perturbation, the quasiperiodic and chaotic motions of ion acoustic waves are presented. Depending upon different ranges of non extensive parameter q, the effect of q is shown on quasiperiodic and chaotic motions of ion acoustic waves with fixed value of v. It is seen that the unperturbed dynamical system has the solitary and periodic wave solutions, but the perturbed dynamical system has the quasiperiodic and chaotic motions with same values of parameters q and v. (author)

  5. Dynamics of single or double ionization of small systems from coincidence electron impact experiments

    Energy Technology Data Exchange (ETDEWEB)

    Lahmam-Bennani, A; Staicu Casagrande, E M; Naja, A, E-mail: azzedine.bennani@u-psud.f [Laboratoire des Collisions Atomiques et Moleculaires (LCAM, UMR8625), Universite Paris-Sud 11, F-91405 Orsay cedex (France)

    2010-06-01

    In this brief review, we illustrate the potentialities and the power of electron-electron coincidence studies to investigate the dynamics of single ionization SI [(e,2e) case] or double ionization DI [(e,3e) case] processes. An example for (e,2e) SI of rare gas atoms is presented with a new insight into the behaviour of the recoil versus the binary intensity. A second example for (e,2e) SI of molecules is used to illustrate the observation of a purely molecular effect, namely the signature of interference effects due to the two-center nature of the H{sub 2} molecule. The third example discusses an unprecedented triple coincidence study involving the scattered - ejected - Auger electrons emitted from an argon target. It is shown that the method allows to disentangle the contribution of various DI mechanisms.

  6. Time-resolved ARPES at LACUS: Band Structure and Ultrafast Electron Dynamics of Solids.

    Science.gov (United States)

    Crepaldi, Alberto; Roth, Silvan; Gatti, Gianmarco; Arrell, Christopher A; Ojeda, José; van Mourik, Frank; Bugnon, Philippe; Magrez, Arnaud; Berger, Helmuth; Chergui, Majed; Grioni, Marco

    2017-05-31

    The manipulation of the electronic properties of solids by light is an exciting goal, which requires knowledge of the electronic structure with energy, momentum and temporal resolution. Time- and angle-resolved photoemission spectroscopy (tr-ARPES) is the most direct probe of the effects of an optical excitation on the band structure of a material. In particular, tr-ARPES in the extreme ultraviolet (VUV) range gives access to the ultrafast dynamics over the entire Brillouin zone. VUV tr-ARPES experiments can now be performed at the ASTRA (ARPES Spectrometer for Time-Resolved Applications) end station of Harmonium, at LACUS. Its capabilities are illustrated by measurements of the ultrafast electronic response of ZrSiTe, a novel topological semimetal characterized by linearly dispersing states located at the Brillouin zone boundary.

  7. Ultrafast unequilibrium electron dynamics of aluminium interacting with an ultra-intense x-ray pulse

    Science.gov (United States)

    Gao, Cheng; Zeng, Jiaolong; Yuan, Jianmin

    2017-10-01

    Ultrafast nonequilibrium dynamics of free electrons in an ultra-intense and ultrafast x-ray pulse interacting with a solid-density aluminium is investigated by solving Fokker-Planck equation. X-ray propagation through aluminium is determined by solving a one-dimensional radiative transfer equation which is coupled with a time-dependent rate equation. Although high energy electrons are evidently nonequilibrium, they account for a small population fraction in the total free electrons. The transmission of an ultra-intense x-ray pulse through a 1 um thick solid-density aluminium sample is calculated and compared with a recent experiment, where good agreement is found and saturable absorption is evidently observed.

  8. Photo-excited hot carrier dynamics in hydrogenated amorphous silicon imaged by 4D electron microscopy

    Science.gov (United States)

    Liao, Bolin; Najafi, Ebrahim; Li, Heng; Minnich, Austin J.; Zewail, Ahmed H.

    2017-09-01

    Charge carrier dynamics in amorphous semiconductors has been a topic of intense research that has been propelled by modern applications in thin-film solar cells, transistors and optical sensors. Charge transport in these materials differs fundamentally from that in crystalline semiconductors owing to the lack of long-range order and high defect density. Despite the existence of well-established experimental techniques such as photoconductivity time-of-flight and ultrafast optical measurements, many aspects of the dynamics of photo-excited charge carriers in amorphous semiconductors remain poorly understood. Here, we demonstrate direct imaging of carrier dynamics in space and time after photo-excitation in hydrogenated amorphous silicon (a-Si:H) by scanning ultrafast electron microscopy (SUEM). We observe an unexpected regime of fast diffusion immediately after photoexcitation, together with spontaneous electron-hole separation and charge trapping induced by the atomic disorder. Our findings demonstrate the rich dynamics of hot carrier transport in amorphous semiconductors that can be revealed by direct imaging based on SUEM.

  9. Dynamical Processes in Open Quantum Systems from a TDDFT Perspective: Resonances and Electron Photoemission.

    Science.gov (United States)

    Larsen, Ask Hjorth; De Giovannini, Umberto; Rubio, Angel

    2016-01-01

    We present a review of different computational methods to describe time-dependent phenomena in open quantum systems and their extension to a density-functional framework. We focus the discussion on electron emission processes in atoms and molecules addressing excited-state lifetimes and dissipative processes. Initially we analyze the concept of an electronic resonance, a central concept in spectroscopy associated with a metastable state from which an electron eventually escapes (electronic lifetime). Resonances play a fundamental role in many time-dependent molecular phenomena but can be rationalized from a time-independent context in terms of scattering states. We introduce the method of complex scaling, which is used to capture resonant states as localized states in the spirit of usual bound-state methods, and work on its extension to static and time-dependent density-functional theory. In a time-dependent setting, complex scaling can be used to describe excitations in the continuum as well as wave packet dynamics leading to electron emission. This process can also be treated by using open boundary conditions which allow time-dependent simulations of emission processes without artificial reflections at the boundaries (i.e., borders of the simulation box). We compare in detail different schemes to implement open boundaries, namely transparent boundaries using Green functions, and absorbing boundaries in the form of complex absorbing potentials and mask functions. The last two are regularly used together with time-dependent density-functional theory to describe the electron emission dynamics of atoms and molecules. Finally, we discuss approaches to the calculation of energy and angle-resolved time-dependent pump-probe photoelectron spectroscopy of molecular systems.

  10. PREFACE: 19th International Conference on Electron Dynamics in Semiconductors, Optoelectronics and Nanostructures (EDISON'19)

    Science.gov (United States)

    González, T.; Martín-Martínez, M. J.; Mateos, J.

    2015-10-01

    The 19th International Conference on Electron Dynamics in Semiconductors, Optoelectronics and Nanostructures (EDISON'19) was held at the Hospedería Fonseca (Universidad de Salamanca, Spain), on 29 June - 2 July, 2015, and was organized by the Electronics Area from the University of Salamanca. The Conference is held biannually and covers the recent progress in the field of electron dynamics in solid-state materials and devices. This was the 19th meeting of the international conference series formerly named Hot Carriers in Semiconductors (HCIS), first held in Modena in 1973. In the edition of 1997 in Berlin the name of the conference changed to International Conference on Nonequilibrium Carrier Dynamics in Semiconductors, keeping the same acronym, HCIS; and finally in the edition of Montpellier in 2009 the name was again changed to the current one, International Conference on Electron Dynamics in Semiconductors, Optoelectronics and Nanostructures (EDISON). The latest editions took place in Santa Barbara, USA, in 2011 and Matsue, Japan, in 2013. Research work on electron dynamics involves quite different disciplines, and requires both fundamental and technological scientific efforts. Attendees to the conference come mostly from academic institutions, belonging to both theoretical and experimental groups working in a variety of fields, such as solid-state physics, electronics, optics, electrical engineering, material science, laser physics, etc. In this framework, events like the EDISON conference become a basic channel for the progress in the field. Here, researchers working in different areas can meet, present their latest advances and exchange their ideas. The program of EDISON'19 included 13 invited papers, 61 oral contributions and 73 posters. These contributions originated from scientists in more than 30 different countries. The Conference gathered 140 participants, coming from 24 different countries, most from Europe, but also with a significant participation

  11. New insights into electron spin dynamics in the presence of correlated noise.

    Science.gov (United States)

    Spezia, S; Adorno, D Persano; Pizzolato, N; Spagnolo, B

    2012-02-08

    The changes in the spin depolarization length in zinc-blende semiconductors when an external component of correlated noise is added to a static driving electric field are analyzed for different values of field strength, noise amplitude and correlation time. Electron dynamics is simulated by a Monte Carlo procedure which takes into account all the possible scattering phenomena of the hot electrons in the medium and includes the evolution of spin polarization. Spin depolarization is studied by examining the decay of the initial spin polarization of the conduction electrons through the D'yakonov-Perel process, the only relevant relaxation mechanism in III-V crystals. Our results show that, for electric field amplitudes lower than the Gunn field, the dephasing length shortens with increasing noise intensity. Moreover, a nonmonotonic behavior of spin depolarization length with the noise correlation time is found, characterized by a maximum variation for values of noise correlation time comparable with the dephasing time. Instead, in high field conditions, we find that, critically depending on the noise correlation time, external fluctuations can positively affect the relaxation length. The influence of the inclusion of the electron-electron scattering mechanism is also shown and discussed.

  12. Femtosecond few- to single-electron point-projection microscopy for nanoscale dynamic imaging

    Directory of Open Access Journals (Sweden)

    A. R. Bainbridge

    2016-03-01

    Full Text Available Femtosecond electron microscopy produces real-space images of matter in a series of ultrafast snapshots. Pulses of electrons self-disperse under space-charge broadening, so without compression, the ideal operation mode is a single electron per pulse. Here, we demonstrate femtosecond single-electron point projection microscopy (fs-ePPM in a laser-pump fs-e-probe configuration. The electrons have an energy of only 150 eV and take tens of picoseconds to propagate to the object under study. Nonetheless, we achieve a temporal resolution with a standard deviation of 114 fs (equivalent to a full-width at half-maximum of 269 ± 40 fs combined with a spatial resolution of 100 nm, applied to a localized region of charge at the apex of a nanoscale metal tip induced by 30 fs 800 nm laser pulses at 50 kHz. These observations demonstrate real-space imaging of reversible processes, such as tracking charge distributions, is feasible whilst maintaining femtosecond resolution. Our findings could find application as a characterization method, which, depending on geometry, could resolve tens of femtoseconds and tens of nanometres. Dynamically imaging electric and magnetic fields and charge distributions on sub-micron length scales opens new avenues of ultrafast dynamics. Furthermore, through the use of active compression, such pulses are an ideal seed for few-femtosecond to attosecond imaging applications which will access sub-optical cycle processes in nanoplasmonics.

  13. Configurable Electronics with Low Noise and 14-bit Dynamic Range for Photodiode-based Photon Detectors

    CERN Document Server

    Müller, H; Yin, Z; Zhou, D; Cao, X; Li, Q; Liu, Y; Zou, F; Skaali, B; Awes, T C

    2006-01-01

    We describe the principles and measured performance characteristics of custom configurable 32-channel shaper/digitizer Front End Electronics (FEE) cards with 14-bit dynamic range for use with gain-adjustable photon detectors. The electronics has been designed for the PHOS calorimeter of ALICE with avalanche photodiode (APD) readout operated at -25 C ambient temperature and a signal shaping time of $1 {\\mu}s$. The electronics has also been adopted by the EMCal detector of ALICE with the same APD readout, but operated at an ambient temperature of +20 C and with a shaping time of 100ns. The CR-RC2 signal shapers on the FEE cards are implemented in discrete logic on a 10-layer board with two shaper sections for each input channel. The two shaper sections with gain ratio of 16:1 are digitized by 10-bit ADCs and provide an effective dynamic range of 14 bits. Gain adjustment for each individual APD is available through 32 bias voltage control registers of 10-bit range. The fixed gains and shaping times of the pole-z...

  14. Generalized GW+Boltzmann Approach for the Description of Ultrafast Electron Dynamics in Topological Insulators

    Science.gov (United States)

    Battiato, Marco; Sánchez-Barriga, Jaime

    2017-01-01

    Quantum-phase transitions between trivial insulators and topological insulators differ from ordinary metal-insulator transitions in that they arise from the inversion of the bulk band structure due to strong spin–orbit coupling. Such topological phase transitions are unique in nature as they lead to the emergence of topological surface states which are characterized by a peculiar spin texture that is believed to play a central role in the generation and manipulation of dissipationless surface spin currents on ultrafast timescales. Here, we provide a generalized GW+Boltzmann approach for the description of ultrafast dynamics in topological insulators driven by electron–electron and electron–phonon scatterings. Taking the prototypical insulator Bi2Te3 as an example, we test the robustness of our approach by comparing the theoretical prediction to results of time- and angle-resolved photoemission experiments. From this comparison, we are able to demonstrate the crucial role of the excited spin texture in the subpicosecond relaxation of transient electrons, as well as to accurately obtain the magnitude and strength of electron–electron and electron–phonon couplings. Our approach could be used as a generalized theory for three-dimensional topological insulators in the bulk-conducting transport regime, paving the way for the realization of a unified theory of ultrafast dynamics in topological materials. PMID:28773171

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

    Science.gov (United States)

    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.

  16. Charge constrained density functional molecular dynamics for simulation of condensed phase electron transfer reactions.

    Science.gov (United States)

    Oberhofer, Harald; Blumberger, Jochen

    2009-08-14

    We present a plane-wave basis set implementation of charge constrained density functional molecular dynamics (CDFT-MD) for simulation of electron transfer reactions in condensed phase systems. Following the earlier work of Wu and Van Voorhis [Phys. Rev. A 72, 024502 (2005)], the density functional is minimized under the constraint that the charge difference between donor and acceptor is equal to a given value. The classical ion dynamics is propagated on the Born-Oppenheimer surface of the charge constrained state. We investigate the dependence of the constrained energy and of the energy gap on the definition of the charge and present expressions for the constraint forces. The method is applied to the Ru2+-Ru3+ electron self-exchange reaction in aqueous solution. Sampling the vertical energy gap along CDFT-MD trajectories and correcting for finite size effects, a reorganization free energy of 1.6 eV is obtained. This is 0.1-0.2 eV lower than a previous estimate based on a continuum model for solvation. The smaller value for the reorganization free energy can be explained by the fact that the Ru-O distances of the divalent and trivalent Ru hexahydrates are predicted to be more similar in the electron transfer complex than for the separated aqua ions.

  17. The Role of Electronic Excitations on Chemical Reaction Dynamics at Metal, Semiconductor and Nanoparticle Surfaces

    Energy Technology Data Exchange (ETDEWEB)

    Tully, John C. [Yale Univ., New Haven, CT (United States)

    2017-06-10

    Chemical reactions are often facilitated and steered when carried out on solid surfaces, essential for applications such as heterogeneous catalysis, solar energy conversion, corrosion, materials processing, and many others. A critical factor that can determine the rates and pathways of chemical reactions at surfaces is the efficiency and specificity of energy transfer; how fast does energy move around and where does it go? For reactions on insulator surfaces energy transfer generally moves in and out of vibrations of the adsorbed molecule and the underlying substrate. By contrast, on metal surfaces, metallic nanoparticles and semiconductors, another pathway for energy flow opens up, excitation and de-excitation of electrons. This so-called “nonadiabatic” mechanism often dominates the transfer of energy and can directly impact the course of a chemical reaction. Conventional computational methods such as molecular dynamics simulation do not account for this nonadiabatic behavior. The current DOE-BES funded project has focused on developing the underlying theoretical foundation and the computational methodology for the prediction of nonadiabatic chemical reaction dynamics at surfaces. The research has successfully opened up new methodology and new applications for molecular simulation. In particular, over the last three years, the “Electronic Friction” theory, pioneered by the PI, has now been developed into a stable and accurate computational method that is sufficiently practical to allow first principles “on-the-fly” simulation of chemical reaction dynamics at metal surfaces.

  18. Multidimensional electron-nuclear wavepacket dynamics via Time-, Energy- and Angle-resolved Photoelectron Spectroscopy

    Science.gov (United States)

    Veyrinas, K.; Makhija, V.; Boguslavskiy, A. E.; Forbes, R.; Wilkinson, I.; Moffatt, D.; Lausten, R.; Stolow, A.

    2017-04-01

    Generating and probing a coherent superposition of coupled vibrational-electronic (vibronic) states - a multidimensional wavepacket - remains a challenging problem in molecular dynamics. Here, we present recent results using time-resolved photoelectron velocity map imaging (VMI) of complex vibronic wavepacket dynamics in the NO molecule following femtosecond single photon excitation in the vacuum ultraviolet (VUV) range (λpump = 160 nm, 80 fs). The induced ultrafast dynamics, involving highly excited valence and Rydberg states, is probed by single photon ionization (λprobe = 400 nm, 40 fs). Varying the pump-probe time delay, the emitted photoelectrons are detected in a VMI spectrometer for time-, energy- and angle-resolved photoelectron spectroscopy. We observe that the different final vibrational states of the NO+ (X 1Σ+) cation, onto which this evolving vibronic wavepacket is projected, reveal different time dependences for the kinetic energy distribution and the laboratory frame photoelectron angular distribution (LFPAD). In particular, we observe unusually strong oscillations in the β4 asymmetry parameter, indicating sensitivity to the higher angular momentum components of the electronic aspect of this complex vibronic wavepacket.

  19. Dynamic Structural Response and Deformations of Monolayer MoS2 Visualized by Femtosecond Electron Diffraction.

    Science.gov (United States)

    Mannebach, Ehren M; Li, Renkai; Duerloo, Karel-Alexander; Nyby, Clara; Zalden, Peter; Vecchione, Theodore; Ernst, Friederike; Reid, Alexander Hume; Chase, Tyler; Shen, Xiaozhe; Weathersby, Stephen; Hast, Carsten; Hettel, Robert; Coffee, Ryan; Hartmann, Nick; Fry, Alan R; Yu, Yifei; Cao, Linyou; Heinz, Tony F; Reed, Evan J; Dürr, Hermann A; Wang, Xijie; Lindenberg, Aaron M

    2015-10-14

    Two-dimensional materials are subject to intrinsic and dynamic rippling that modulates their optoelectronic and electromechanical properties. Here, we directly visualize the dynamics of these processes within monolayer transition metal dichalcogenide MoS2 using femtosecond electron scattering techniques as a real-time probe with atomic-scale resolution. We show that optical excitation induces large-amplitude in-plane displacements and ultrafast wrinkling of the monolayer on nanometer length-scales, developing on picosecond time-scales. These deformations are associated with several percent peak strains that are fully reversible over tens of millions of cycles. Direct measurements of electron-phonon coupling times and the subsequent interfacial thermal heat flow between the monolayer and substrate are also obtained. These measurements, coupled with first-principles modeling, provide a new understanding of the dynamic structural processes that underlie the functionality of two-dimensional materials and open up new opportunities for ultrafast strain engineering using all-optical methods.

  20. Dynamic footprint measurement collection technique and intrarater reliability: ink mat, paper pedography, and electronic pedography.

    Science.gov (United States)

    Fascione, Jeanna M; Crews, Ryan T; Wrobel, James S

    2012-01-01

    Identifying the variability of footprint measurement collection techniques and the reliability of footprint measurements would assist with appropriate clinical foot posture appraisal. We sought to identify relationships between these measures in a healthy population. On 30 healthy participants, midgait dynamic footprint measurements were collected using an ink mat, paper pedography, and electronic pedography. The footprints were then digitized, and the following footprint indices were calculated with photo digital planimetry software: footprint index, arch index, truncated arch index, Chippaux-Smirak Index, and Staheli Index. Differences between techniques were identified with repeated-measures analysis of variance with post hoc test of Scheffe. In addition, to assess practical similarities between the different methods, intraclass correlation coefficients (ICCs) were calculated. To assess intrarater reliability, footprint indices were calculated twice on 10 randomly selected ink mat footprint measurements, and the ICC was calculated. Dynamic footprint measurements collected with an ink mat significantly differed from those collected with paper pedography (ICC, 0.85-0.96) and electronic pedography (ICC, 0.29-0.79), regardless of the practical similarities noted with ICC values (P = .00). Intrarater reliability for dynamic ink mat footprint measurements was high for the footprint index, arch index, truncated arch index, Chippaux-Smirak Index, and Staheli Index (ICC, 0.74-0.99). Footprint measurements collected with various techniques demonstrate differences. Interchangeable use of exact values without adjustment is not advised. Intrarater reliability of a single method (ink mat) was found to be high.

  1. Dynamic optical modulation of an electron beam on a photocathode RF gun: Toward intensity-modulated radiation therapy (IMRT)

    Energy Technology Data Exchange (ETDEWEB)

    Kondoh, Takafumi [Osaka University, 8-1 Mihogaoka, Ibaraki, Osaka 567-0047 (Japan)], E-mail: t-kondo@sanken.osaka-u.ac.jp; Kashima, Hiroaki; Yang, Jinfeng; Yoshida, Yoichi; Tagawa, Seiichi [Osaka University, 8-1 Mihogaoka, Ibaraki, Osaka 567-0047 (Japan)

    2008-10-15

    In intensity-modulated radiation therapy (IMRT), the aim is to deliver reduced doses of radiation to normal tissue. As a step toward IMRT, we examined dynamic optical modulation of an electron beam produced by a photocathode RF gun. Images on photomasks were transferred onto a photocathode by relay imaging. The resulting beam was controlled by a remote mirror. The modulated electron beam maintained its shape on acceleration, had a fine spatial resolution, and could be moved dynamically by optical methods.

  2. Visualization of carrier dynamics in p(n)-type GaAs by scanning ultrafast electron microscopy.

    Science.gov (United States)

    Cho, Jongweon; Hwang, Taek Yong; Zewail, Ahmed H

    2014-02-11

    Four-dimensional scanning ultrafast electron microscopy is used to investigate doping- and carrier-concentration-dependent ultrafast carrier dynamics of the in situ cleaved single-crystalline GaAs(110) substrates. We observed marked changes in the measured time-resolved secondary electrons depending on the induced alterations in the electronic structure. The enhancement of secondary electrons at positive times, when the electron pulse follows the optical pulse, is primarily due to an energy gain involving the photoexcited charge carriers that are transiently populated in the conduction band and further promoted by the electron pulse, consistent with a band structure that is dependent on chemical doping and carrier concentration. When electrons undergo sufficient energy loss on their journey to the surface, dark contrast becomes dominant in the image. At negative times, however, when the electron pulse precedes the optical pulse (electron impact), the dynamical behavior of carriers manifests itself in a dark contrast which indicates the suppression of secondary electrons upon the arrival of the optical pulse. In this case, the loss of energy of material's electrons is by collisions with the excited carriers. These results for carrier dynamics in GaAs(110) suggest strong carrier-carrier scatterings which are mirrored in the energy of material's secondary electrons during their migration to the surface. The approach presented here provides a fundamental understanding of materials probed by four-dimensional scanning ultrafast electron microscopy, and offers possibilities for use of this imaging technique in the study of ultrafast charge carrier dynamics in heterogeneously patterned micro- and nanostructured material surfaces and interfaces.

  3. Dynamics, magnetic properties, and electron binding energies of H2O2 in water.

    Science.gov (United States)

    C Cabral, Benedito J

    2017-06-21

    Results for the magnetic properties and electron binding energies of H2O2 in liquid water are presented. The adopted methodology relies on the combination of Born-Oppenheimer molecular dynamics and electronic structure calculations. The Keal-Tozer functional was applied for predicting magnetic shieldings and H2O2 intramolecular spin-spin coupling constants. Electron binding energies were calculated with electron propagator theory. In water, H2O2 is a better proton donor than proton acceptor, and the present results indicate that this feature is important for understanding magnetic properties in solution. In comparison with the gas-phase, H2O2 atoms are deshielded in water. For oxygen atoms, the deshielding is mainly determined by structural/conformational changes. Hydrogen-bond interactions explain the deshielding of protons in water. The predicted chemical shift for the H2O2 protons in water (δ∼11.8 ppm) is in good agreement with experimental information (δ=11.2 ppm). The two lowest electron binding energies of H2O2 in water (10.7±0.5 and 11.2±0.5 eV) are in reasonable agreement with experiment. In keeping with data from photoelectron spectroscopy, an ∼1.6 eV red-shift of the two first ionisation energies relative to the gas-phase is observed in water. The strong dependence of magnetic properties on changes of the electronic density in the nuclei environment is illustrated by a correlation between the σ(17O) magnetic shielding constant and the energy gap between the [2a] lowest valence and [1a] core orbitals of H2O2.

  4. Dynamics, magnetic properties, and electron binding energies of H2O2 in water

    Science.gov (United States)

    C. Cabral, Benedito J.

    2017-06-01

    Results for the magnetic properties and electron binding energies of H2O2 in liquid water are presented. The adopted methodology relies on the combination of Born-Oppenheimer molecular dynamics and electronic structure calculations. The Keal-Tozer functional was applied for predicting magnetic shieldings and H2O2 intramolecular spin-spin coupling constants. Electron binding energies were calculated with electron propagator theory. In water, H2O2 is a better proton donor than proton acceptor, and the present results indicate that this feature is important for understanding magnetic properties in solution. In comparison with the gas-phase, H2O2 atoms are deshielded in water. For oxygen atoms, the deshielding is mainly determined by structural/conformational changes. Hydrogen-bond interactions explain the deshielding of protons in water. The predicted chemical shift for the H2O2 protons in water (δ ˜11.8 ppm) is in good agreement with experimental information (δ =11.2 ppm). The two lowest electron binding energies of H2O2 in water (10.7 ±0.5 and 11.2 ±0.5 eV) are in reasonable agreement with experiment. In keeping with data from photoelectron spectroscopy, an ˜1.6 eV red-shift of the two first ionisation energies relative to the gas-phase is observed in water. The strong dependence of magnetic properties on changes of the electronic density in the nuclei environment is illustrated by a correlation between the σ(17O) magnetic shielding constant and the energy gap between the [2a] lowest valence and [1a] core orbitals of H2O2.

  5. Tuning the Electronic and Dynamical Properties of a Molecule by Atom Trapping Chemistry.

    Science.gov (United States)

    Pham, Van Dong; Repain, Vincent; Chacon, Cyril; Bellec, Amandine; Girard, Yann; Rousset, Sylvie; Abad, Enrique; Dappe, Yannick J; Smogunov, Alexander; Lagoute, Jérôme

    2017-11-28

    The ability to trap adatoms with an organic molecule on a surface has been used to obtain a range of molecular functionalities controlled by the choice of the molecular trapping site and local deprotonation. The tetraphenylporphyrin molecule used in this study contains three types of trapping sites: two carbon rings (phenyl and pyrrole) and the center of a macrocycle. Catching a gold adatom on the carbon rings leads to an electronic doping of the molecule, whereas trapping the adatom at the macrocycle center with single deprotonation leads to a molecular rotor and a second deprotonation leads to a molecular jumper. We call "atom trapping chemistry" the control of the structure, electronic, and dynamical properties of a molecule achieved by trapping metallic atoms with a molecule on a surface. In addition to the examples previously described, we show that more complex structures can be envisaged.

  6. Effect of Atmosphere on Recovery Dynamics of Polyimide Film Damaged by Electron Radiation

    Science.gov (United States)

    Plis, E.; Engelhart, D. P.; Cooper, R.; Humagain, S.; Brunetti, M.; Koch, A.; Greenbaum, S.; Ferguson, D.; Hoffmann, R.

    2017-09-01

    Since electrons are the primary charged particles at the geosynchronous Earth orbit (GEO), understanding of their interactions with spacecraft materials, such as polyimide (PI, Kapton-H®), is important. Understanding of the chemical nature of electron damage and its effect on PI’s electrical and optical properties is still limited. Thus, predictive spacecraft models (electrical charging, thermal, etc) are restricted to only pristine material properties. This is a major source of error in spacecraft construction and anomaly resolution, since material properties change after exposure to the space environment. Ground based measurements are critical to understanding the dynamics of spacecraft materials however it will be shown in this work that standard material handling practice and exposure to air are unacceptable for these studies.

  7. Dynamic Estimation of the Probability of Patient Readmission to the ICU using Electronic Medical Records.

    Science.gov (United States)

    Caballero, Karla; Akella, Ram

    2015-01-01

    In this paper, we propose a framework to dynamically estimate the probability that a patient is readmitted after he is discharged from the ICU and transferred to a lower level care. We model this probability as a latent state which evolves over time using Dynamical Linear Models (DLM). We use as an input a combination of numerical and text features obtained from the patient Electronic Medical Records (EMRs). We process the text from the EMRs to capture different diseases, symptoms and treatments by means of noun phrases and ontologies. We also capture the global context of each text entry using Statistical Topic Models. We fill out the missing values using a Expectation Maximization based method (EM). Experimental results show that our method outperforms other methods in the literature terms of AUC, sensitivity and specificity. In addition, we show that the combination of different features (numerical and text) increases the prediction performance of the proposed approach.

  8. Single-Molecule Electronic Measurements of the Dynamic Flexibility of Histone Deacetylases

    Science.gov (United States)

    Froberg, James; You, Seungyong; Yu, Junru; Haldar, Manas; Sedigh, Abbas; Mallik, Sanku; Srivastava, D. K.; Choi, Yongki

    Due to their involvement in epigenetic regulation, histone deacetylases (HDACs) have gained considerable interest in designing drugs for treatment of a variety of human diseases including cancers. Recently, we applied a label-free, electronic single-molecule nano-circuit technique to gain insight into the contribution of the dynamic flexibility in HDACs structure during the course of substrates/ ligands binding and catalysis. We observed that HDAC8 has two major (dynamically interconvertible) conformational states, ``ground (catalytically unfavorable)'' and ``transition (catalytically favorable)''. In addition, we found that its cognate substrates/ligands reciprocally catalyze the transition of the ground to the transition state conformation of HDAC8. Thus, we propose that both enzymes and their substrates/ligands serve as ``catalysts'' in facilitating the structural changes of each other and promoting the overall chemical transformation reaction. Such new information provides the potential for designing a new class of mechanism-based inhibitors and activators of HDAC8 for treating human diseases.

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

    Science.gov (United States)

    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.

  10. Beam dynamics analysis of femtosecond microbunches produced by the staged electron laser acceleration experiment

    Directory of Open Access Journals (Sweden)

    F. Zhou

    2003-05-01

    Full Text Available Preservation of the femtosecond (fs microbunches, created during laser acceleration, is a crucial step to enable staging of the laser acceleration process. This paper focuses on the optimization of the beam dynamics of fs microbunches transported through the staged electron laser acceleration (STELLA-II experiment being carried out at the Brookhaven National Laboratory Accelerator Test Facility. STELLA-II consists of an inverse free electron laser (IFEL untapered undulator, which acts as an electron beam energy modulator; a magnetic chicane, which acts as a buncher; a second IFEL tapered undulator, which acts as an accelerator; and a dipole, which serves as an energy spectrometer. When the energy-modulated macrobunch traverses through the chicane and a short drift space, microbunches of order fs in duration (i.e., ∼3  fs FWHM are formed. The 3-fs microbunches are accelerated by interacting with a high-power CO_{2} laser beam in the following tapered undulator. These extremely short microbunches may experience significant space charge and coherent synchrotron radiation effects when traversing the STELLA-II transport line. These effects are analyzed and the safe operating conditions are determined. With less than 0.5-pC microbunch charge, both microbunch debunching and emittance growth are negligible, and the energy-spread increase is less than 5%. These results are also useful for the laser electron acceleration project at SLAC and in possible future programs where the fs microbunches are employed for other purposes.

  11. Multi-time scale dynamics in power electronics-dominated power systems

    Science.gov (United States)

    Yuan, Xiaoming; Hu, Jiabing; Cheng, Shijie

    2017-09-01

    Electric power infrastructure has recently undergone a comprehensive transformation from electromagnetics to semiconductors. Such a development is attributed to the rapid growth of power electronic converter applications in the load side to realize energy conservation and on the supply side for renewable generations and power transmissions using high voltage direct current transmission. This transformation has altered the fundamental mechanism of power system dynamics, which demands the establishment of a new theory for power system control and protection. This paper presents thoughts on a theoretical framework for the coming semiconducting power systems.

  12. Coalescence dynamics of size-selected gold clusters studied by time-resolved transmission electron microscopy

    Science.gov (United States)

    Liu, J.; Foster, D.; Li, Z. Y.; Wilkinson, N.; Yuan, J.

    2017-09-01

    Coalescence dynamics of size-selected gold (Au) clusters (each with nominal 923 atoms), on amorphous Si3N4 substrate at room temperature, has been studied via time-resolved transmission electron microscopy (TEM). We found that the clusters approached each other in two stages. In the first stage, the drift velocity was independent of the particle separation and could be attributed to beam-induced random motion. In the second stage, the clusters were found to jump into contact with a much higher final averaged speed. This is independent of beam dose rates and is attributed to the van der Waal attraction.

  13. Quantum corrected Langevin dynamics for adsorbates on metal surfaces interacting with hot electrons

    DEFF Research Database (Denmark)

    Olsen, Thomas; Schiøtz, Jakob

    2010-01-01

    We investigate the importance of including quantized initial conditions in Langevin dynamics for adsorbates interacting with a thermal reservoir of electrons. For quadratic potentials the time evolution is exactly described by a classical Langevin equation and it is shown how to rigorously obtain...... mechanical master equation approach. With CO on Cu(100) as an example, we demonstrate the effect for a system with ab initio frictional tensor and potential energy surfaces and show that quantizing the initial conditions can have a large impact on both the desorption probability and the distribution...

  14. The Generalized Coherent State ansatz: Application to quantum electron-vibrational dynamics

    Energy Technology Data Exchange (ETDEWEB)

    Borrelli, Raffaele, E-mail: raffaele.borrelli@unito.it [DISAFA, Università di Torino, I-10095 Grugliasco (Italy); Gelin, Maxim F. [Departement of Chemistry, Technische Universität München, D-85747 Garching (Germany)

    2016-12-20

    A new ansatz for molecular vibronic wave functions based on a superposition of time-dependent Generalized Coherent States is developed and analysed. The methodology is specifically tailored to describe the time evolution of the wave function of a system in which several interacting electronic states are coupled to a bath of harmonic oscillators. The equations of motion for the wave packet parameters are obtained by using the Dirac–Frenkel time-dependent variational principle. The methodology is used to describe the quantum dynamical behavior of a model polaron system and its scaling and convergence properties are discussed and compared with numerically exact results.

  15. Hydrodynamic theory for quantum plasmonics: Linear-response dynamics of the inhomogeneous electron gas

    DEFF Research Database (Denmark)

    Yan, Wei

    2015-01-01

    We investigate the hydrodynamic theory of metals, offering systematic studies of the linear-response dynamics for an inhomogeneous electron gas. We include the quantum functional terms of the Thomas-Fermi kinetic energy, the von Weizsa¨cker kinetic energy, and the exchange-correlation Coulomb...... energies under the local density approximation. The advantages, limitations, and possible improvements of the hydrodynamic theory are transparently demonstrated. The roles of various parameters in the theory are identified. We anticipate that the hydrodynamic theory can be applied to investigate the linear...

  16. Electron correlation dynamics of strong-field double ionization of atoms below recollision threshold

    Energy Technology Data Exchange (ETDEWEB)

    Liu Yunquan; Gong Qihuang [Department of Physics and State Key Laboratory for Mesoscopic Physics, Peking University, Beijing 100871 (China); Ye Difa; Liu Jie [Center for Applied Physics and Technology, Peking University, 100084 Beijing (China); Rudenko, A; Tschuch, S; Duerr, M; Moshammer, R; Ullrich, J [Max-Planck-Institut fuer Kernphysik, D-69117 Heidelberg (Germany); Siegel, M; Morgner, U, E-mail: yunquan.liu@pku.edu.cn [Leibniz Universitaet Hannover, Welfengarten 1, D-30167 Hannover (Germany)

    2011-02-01

    In recent combined experimental and theoretical study we have explored nonsequential double ionization of neon and argon atoms in the infrared light field (800nm) below the recollision threshold. We find that the two-electron correlation dynamics depends on atomic structure- 'side-by-side emission' (correlation) for Ne and 'back-to-back emission' (anticorrelation) for argon atoms. This can be explained theoretically within our three dimensional classical model calculation including tunnelling effect. The multiple recollisions as well as recollision-induced-excitation-tunnelling (RIET) effect dominate the anticorrelation of argon, whereas the laser-assisted instantaneous recollision dominates the correlation of neon.

  17. Direct observation of graphene growth and associated copper substrate dynamics by in situ scanning electron microscopy.

    Science.gov (United States)

    Wang, Zhu-Jun; Weinberg, Gisela; Zhang, Qiang; Lunkenbein, Thomas; Klein-Hoffmann, Achim; Kurnatowska, Michalina; Plodinec, Milivoj; Li, Qing; Chi, Lifeng; Schloegl, R; Willinger, Marc-Georg

    2015-02-24

    This work highlights the importance of in situ experiments for an improved understanding of graphene growth on copper via metal-catalyzed chemical vapor deposition (CVD). Graphene growth inside the chamber of a modified environmental scanning electron microscope under relevant low-pressure CVD conditions allows visualizing structural dynamics of the active catalyst simultaneously with graphene nucleation and growth in an unparalleled way. It enables the observation of a complete CVD process from substrate annealing through graphene nucleation and growth and, finally, substrate cooling in real time and nanometer-scale resolution without the need of sample transfer. A strong dependence of surface dynamics such as sublimation and surface premelting on grain orientation is demonstrated, and the influence of substrate dynamics on graphene nucleation and growth is presented. Insights on the growth mechanism are provided by a simultaneous observation of the growth front propagation and nucleation rate. Furthermore, the role of trace amounts of oxygen during growth is discussed and related to graphene-induced surface reconstructions during cooling. Above all, this work demonstrates the potential of the method for in situ studies of surface dynamics on active metal catalysts.

  18. Dynamical effects in strain measurements by dark-field electron holography

    Energy Technology Data Exchange (ETDEWEB)

    Javon, E. [CEMES-CNRS and Université de Toulouse, 29 rue Jeanne Marvig, F-31055 Toulouse (France); EMAT, University of Antwerp, Groenenborgerlaan 171, 2020 Antwerp (Belgium); Lubk, A. [CEMES-CNRS and Université de Toulouse, 29 rue Jeanne Marvig, F-31055 Toulouse (France); EMAT, University of Antwerp, Groenenborgerlaan 171, 2020 Antwerp (Belgium); Institute of Structure Physics, Technische Universität Dresden, 01062 Dresden (Germany); Cours, R. [CEMES-CNRS and Université de Toulouse, 29 rue Jeanne Marvig, F-31055 Toulouse (France); Reboh, S. [CEMES-CNRS and Université de Toulouse, 29 rue Jeanne Marvig, F-31055 Toulouse (France); CEA, LETI, Minatec Campus, 17 rue de Martyrs, 38054 Grenoble (France); Cherkashin, N.; Houdellier, F.; Gatel, C.; Hÿtch, M.J. [CEMES-CNRS and Université de Toulouse, 29 rue Jeanne Marvig, F-31055 Toulouse (France)

    2014-12-15

    Here, we study the effect of dynamic scattering on the projected geometric phase and strain maps reconstructed using dark-field electron holography (DFEH) for non-uniformly strained crystals. The investigated structure consists of a {SiGe/Si} superlattice grown on a (001)-Si substrate. The three-dimensional strain field within the thin TEM lamella is modelled by the finite element method. The observed projected strain is simulated in two ways by multiplying the strain at each depth in the crystal by a weighting function determined from a recently developed analytical two-beam dynamical theory, and by simply taking the average value. We demonstrate that the experimental results need to be understood in terms of the dynamical theory and good agreement is found between the experimental and simulated results. Discrepancies do remain for certain cases and are likely to be from an imprecision in the actual two-beam diffraction conditions, notably the deviation parameter, and points to limitations in the 2-beam approximation. Finally, a route towards a 3D reconstruction of strain fields is proposed. - Highlights: • We explain DFEH strain map thanks to a recent theoretical development. • The projection measured by DFEH is a weighted average of the strain along the e-beam. • The weighting function depends on diffracted beam, thickness and sample orientation. • The weighting functions were included in FEM simulation and compared to DFEH results. • Kinematic conditions avoid the dynamical effects and lead to the average strain value.

  19. On the adiabatic representation of Meyer-Miller electronic-nuclear dynamics.

    Science.gov (United States)

    Cotton, Stephen J; Liang, Ruibin; Miller, William H

    2017-08-14

    The Meyer-Miller (MM) classical vibronic (electronic + nuclear) Hamiltonian for electronically non-adiabatic dynamics-as used, for example, with the recently developed symmetrical quasiclassical (SQC) windowing model-can be written in either a diabatic or an adiabatic representation of the electronic degrees of freedom, the two being a canonical transformation of each other, thus giving the same dynamics. Although most recent applications of this SQC/MM approach have been carried out in the diabatic representation-because most of the benchmark model problems that have exact quantum results available for comparison are typically defined in a diabatic representation-it will typically be much more convenient to work in the adiabatic representation, e.g., when using Born-Oppenheimer potential energy surfaces (PESs) and derivative couplings that come from electronic structure calculations. The canonical equations of motion (EOMs) (i.e., Hamilton's equations) that come from the adiabatic MM Hamiltonian, however, in addition to the common first-derivative couplings, also involve second-derivative non-adiabatic coupling terms (as does the quantum Schrödinger equation), and the latter are considerably more difficult to calculate. This paper thus revisits the adiabatic version of the MM Hamiltonian and describes a modification of the classical adiabatic EOMs that are entirely equivalent to Hamilton's equations but that do not involve the second-derivative couplings. The second-derivative coupling terms have not been neglected; they simply do not appear in these modified adiabatic EOMs. This means that SQC/MM calculations can be carried out in the adiabatic representation, without approximation, needing only the PESs and the first-derivative coupling elements. The results of example SQC/MM calculations are presented, which illustrate this point, and also the fact that simply neglecting the second-derivative couplings in Hamilton's equations (and presumably also in the Schr

  20. Investigation of the photodetached electronic wave packet dynamics in a magnetic field near a surface

    Science.gov (United States)

    Chen, Zhaohang; Wang, Dehua; Cheng, Shaohao

    2017-05-01

    The electronic wave packet dynamics photodetached from H- ion in a magnetic field near an elastic surface has been studied by using the time-dependent perturbation theory combined with the semiclassical closed orbit theory for the first time. Firstly, we put forward an analytic formula for calculating the autocorrelation function of this system. Then we calculate and analyze the autocorrelation function in great detail. It is demonstrated that the quantum wave packet revival phenomenon is significant when the laser pulse width is far less than the period of the detached electron's closed orbit. As the pulse width is close to the period of the detached electron's closed orbit, the quantum wave packet revival phenomenon becomes weakened. When the laser pulse width is bigger than the period of the closed orbit of the detached electron, the adjacent revival peaks in the autocorrelation function begin to merge and the quantum revival phenomenon disappears. In addition, the magnetic field strength can also affect the autocorrelation function of this system. As the magnetic field strength is relatively small, the quantum wave packet revival phenomenon is weak. With the increase of the magnetic field strength, the number of the reviving peaks in the autocorrelation function becomes increased and the quantum wave packet revival phenomenon becomes significant. Therefore, we can control the quantum wave packet revival in the autocorrelation function of this system by changing the laser pulse width and the external magnetic field strength. This study can guide the future experimental research on the wave packet dynamics of atoms or ions in the external fields or surfaces.

  1. First and second one-​electron reduction of lumiflavin in water - A first principles molecular dynamics study

    NARCIS (Netherlands)

    Kılıç, M.; Ensing, B.

    2013-01-01

    Flavins are ubiquitously found in nature as cofactors in proteins that regulate electron and proton transfer reactions. The electron and proton affinities of flavins are modulated by their molecular environment. Using density functional theory based molecular dynamics simulations, we have studied

  2. Integrated analysis of DFIG drive-train and power electronics dynamics during electrical AC faults and wind disturbances

    DEFF Research Database (Denmark)

    Barahona Garzón, Braulio; Sørensen, Poul Ejnar; Anaya-Lara, Olimpo

    2013-01-01

    The dynamics of a 2 MW DFIG wind turbine are studied during electrical AC faults, and wind disturbances. A simulation platform that couples HAWC2, and Matlab/Simulink was used. High frequencies of the gear box, and power electronics are neglected. It was shown that the dynamics of the dc...

  3. Simulation of Electron Beam Dynamics in the 22 MeV Accelerator for a Coherent Electron Cooling Proof of Principle Experiment

    Energy Technology Data Exchange (ETDEWEB)

    Owen, Justin [Stony Brook Univ., NY (United States)

    2013-12-01

    Coherent electron cooling (CeC) offers a potential new method of cooling hadron beams in colliders such as the Relativistic Heavy Ion Collider (RHIC) or the future electron ion collider eRHIC. A 22 MeV linear accelerator is currently being built as part of a proof of principle experiment for CeC at Brookhaven National Laboratory (BNL). In this thesis we present a simulation of electron beam dynamics including space charge in the 22 MeV CeC proof of principle experiment using the program ASTRA (A Space charge TRacking Algorithm).

  4. Optical Response of Warm Dense Matter Using Real-Time Electron Dynamics

    Science.gov (United States)

    Baczewski, Andrew; Shulenburger, Luke; Desjarlais, Michael; Magyar, Rudolph

    2014-03-01

    The extreme temperatures and solid-like densities in warm dense matter present a unique challenge for theory, wherein neither conventional models from condensed matter nor plasma physics capture all of the relevant phenomenology. While Kubo-Greenwood DFT calculations have proven capable of reproducing optical properties of WDM, they require a significant number of virtual orbitals to reach convergence due to their perturbative nature. Real-time TDDFT presents a complementary framework with a number of computationally favorable properties, including reduced cost complexity and better scalability, and has been used to reproduce the optical response of finite and ordered extended systems. We will describe the use of Ehrenfest-TDDFT to evolve coupled electron-nuclear dynamics in WDM systems, and the subsequent evaluation of optical response functions from the real-time electron dynamics. The advantages and disadvantages of this approach will be discussed relative to the current state-of-the-art. 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.

  5. Exploring the vibrational fingerprint of the electronic excitation energy via molecular dynamics

    Energy Technology Data Exchange (ETDEWEB)

    Deyne, Andy Van Yperen-De; Pauwels, Ewald; Ghysels, An; Waroquier, Michel; Van Speybroeck, Veronique; Hemelsoet, Karen, E-mail: karen.hemelsoet@ugent.be [Center for Molecular Modeling (CMM), Ghent University, Technologiepark 903, 9052 Zwijnaarde (Belgium); De Meyer, Thierry [Center for Molecular Modeling (CMM), Ghent University, Technologiepark 903, 9052 Zwijnaarde (Belgium); Department of Textiles, Ghent University, Technologiepark 907, 9052 Zwijnaarde (Belgium); De Clerck, Karen [Department of Textiles, Ghent University, Technologiepark 907, 9052 Zwijnaarde (Belgium)

    2014-04-07

    A Fourier-based method is presented to relate changes of the molecular structure during a molecular dynamics simulation with fluctuations in the electronic excitation energy. The method implies sampling of the ground state potential energy surface. Subsequently, the power spectrum of the velocities is compared with the power spectrum of the excitation energy computed using time-dependent density functional theory. Peaks in both spectra are compared, and motions exhibiting a linear or quadratic behavior can be distinguished. The quadratically active motions are mainly responsible for the changes in the excitation energy and hence cause shifts between the dynamic and static values of the spectral property. Moreover, information about the potential energy surface of various excited states can be obtained. The procedure is illustrated with three case studies. The first electronic excitation is explored in detail and dominant vibrational motions responsible for changes in the excitation energy are identified for ethylene, biphenyl, and hexamethylbenzene. The proposed method is also extended to other low-energy excitations. Finally, the vibrational fingerprint of the excitation energy of a more complex molecule, in particular the azo dye ethyl orange in a water environment, is analyzed.

  6. The reaction dynamics of alkali dimer molecules and electronically excited alkali atoms with simple molecules

    Energy Technology Data Exchange (ETDEWEB)

    Hou, Hongtao [Univ. of California, Berkeley, CA (United States). Dept. of Chemistry

    1995-12-01

    This dissertation presents the results from the crossed molecular beam studies on the dynamics of bimolecular collisions in the gas phase. The primary subjects include the interactions of alkali dimer molecules with simple molecules, and the inelastic scattering of electronically excited alkali atoms with O2. The reaction of the sodium dimers with oxygen molecules is described in Chapter 2. Two reaction pathways were observed for this four-center molecule-molecule reaction, i.e. the formations of NaO2 + Na and NaO + NaO. NaO2 products exhibit a very anisotropic angular distribution, indicating a direct spectator stripping mechanism for this reaction channel. The NaO formation follows the bond breaking of O2, which is likely a result of a charge transfer from Na2 to the excited state orbital of O2-. The scattering of sodium dimers from ammonium and methanol produced novel molecules, NaNH3 and Na(CH3OH), respectively. These experimental observations, as well as the discussions on the reaction dynamics and the chemical bonding within these molecules, will be presented in Chapter 3. The lower limits for the bond dissociation energies of these molecules are also obtained. Finally, Chapter 4 describes the energy transfer between oxygen molecules and electronically excited sodium atoms.

  7. Dynamics and control of gold-encapped gallium arsenide nanowires imaged by 4D electron microscopy.

    Science.gov (United States)

    Chen, Bin; Fu, Xuewen; Tang, Jau; Lysevych, Mykhaylo; Tan, Hark Hoe; Jagadish, Chennupati; Zewail, Ahmed H

    2017-11-20

    Eutectic-related reaction is a special chemical/physical reaction involving multiple phases, solid and liquid. Visualization of a phase reaction of composite nanomaterials with high spatial and temporal resolution provides a key understanding of alloy growth with important industrial applications. However, it has been a rather challenging task. Here, we report the direct imaging and control of the phase reaction dynamics of a single, as-grown free-standing gallium arsenide nanowire encapped with a gold nanoparticle, free from environmental confinement or disturbance, using four-dimensional (4D) electron microscopy. The nondestructive preparation of as-grown free-standing nanowires without supporting films allows us to study their anisotropic properties in their native environment with better statistical character. A laser heating pulse initiates the eutectic-related reaction at a temperature much lower than the melting points of the composite materials, followed by a precisely time-delayed electron pulse to visualize the irreversible transient states of nucleation, growth, and solidification of the complex. Combined with theoretical modeling, useful thermodynamic parameters of the newly formed alloy phases and their crystal structures could be determined. This technique of dynamical control aided by 4D imaging of phase reaction processes on the nanometer-ultrafast time scale opens new venues for engineering various reactions in a wide variety of other systems. Copyright © 2017 the Author(s). Published by PNAS.

  8. Topological Properties of Chemical Bonds from Static and Dynamic Electron Densities.

    Science.gov (United States)

    Jagannatha Prathapa, Siriyara; Held, Jeanette; van Smaalen, Sander

    2013-09-01

    Dynamic and static electron densities (EDs) based on the independent spherical atom model (IAM) and multipole (MP) models of crambin were successfully computed, holding no series-termination effects. The densities are compared to EDs of small biological molecules at diverse temperatures. It is outlined that proteins exhibit an intrinsic flexibility, present as frozen disorder at 100 K, in contrast to small molecules. The flexibility of the proteins is reflected by atomic displacement parameters (B-factors), which are considerably larger than for small molecules at 298 K. Thus, an optimal deconvolution of deformation density and thermal motion is not guaranteed, which prevents a free refinement of MP parameters but allows an application of transferable, fixed MP parameters. The analysis of the topological properties, such as the density at bond critical points (BCPs) and the Laplacian, reveals systematic differences between static and dynamic EDs. Zero-point-vibrations, yet present in dynamic EDs at low temperature, affect but marginally the EDs of small molecules. The zero-point-vibrations cause a smearing of the ED, which becomes more pronounced with increasing temperature. Topological properties, primarily the Laplacian, of covalent bonds appear to be more sensitive to effects by temperature and the polarity of the bonds. However, dynamic EDs at ca. 20 K based on MP models provide a good characterization of chemical bonding. Both the density at BCPs and the Laplacian of hydrogen bonds constitute similar values from static and dynamic EDs for all studied temperatures. Deformation densities demonstrate the necessity of the employment of MP parameters in order to comprise the nature of covalent bonds. The character of hydrogen bonds can be roughly pictured by IAM, whereas MP parameters are recommended for a classification of hydrogen bonds beyond a solely interpretation of topological properties.

  9. Space dependent, full orbit effects on runaway electron dynamics in tokamak plasmas

    Science.gov (United States)

    Carbajal, L.; del-Castillo-Negrete, D.; Spong, D.; Seal, S.; Baylor, L.

    2017-04-01

    The dynamics of RE (runaway electrons) in fusion plasmas span a wide range of temporal scales, from the fast gyro-motion, ˜ 10 - 11 s, to the observational time scales, ˜ 10 - 2 → 1 s. To cope with this scale separation, RE are usually studied within the bounce-average or the guiding center approximations. Although these approximations have yielded valuable insights, a study with predictive capabilities of RE in fusion plasmas calls for the incorporation of full orbit effects in configuration space in the presence of three-dimensional magnetic fields. We present numerical results on this problem using the Kinetic Orbit Runaway electrons Code that follows relativistic electrons in general electric and magnetic fields under the full Lorentz force, collisions, and radiation losses. At relativistic energies, the main energy loss is due to radiation damping, which we incorporate using the Landau-Lifshitz formulation of the Abraham-Lorentz-Dirac force. The main focus is on full orbit effects on synchrotron radiation. It is shown that even in the absence of magnetic field stochasticty, neglecting orbit dynamics can introduce significant errors in the computation of the total radiated power and the synchrotron spectra. The statistics of collisionless (i.e., full orbit induced) pitch angle dispersion, and its key role played on synchrotron radiation, are studied in detail. Numerical results are also presented on the pitch angle dependence of the spatial confinement of RE and on full orbit effects on the competition of electric field acceleration and radiation damping. Finally, full orbit calculations are used to explore the limitations of gyro-averaging in the relativistic regime. To explore the practical impact of the results, DIII-D and ITER-like parameters are used in the simulations.

  10. Elucidating energy and electron transfer dynamics within molecular assemblies for solar energy conversion

    Science.gov (United States)

    Morseth, Zachary Aaron

    The use of sunlight to make chemical fuels (i.e. solar fuels) is an attractive approach in the quest to develop sustainable energy sources. Using nature as a guide, assemblies for artificial photosynthesis will need to perform multiple functions. They will need to be able to harvest light across a broad region of the solar spectrum, transport excited-state energy to charge-separation sites, and then transport and store redox equivalents for use in the catalytic reactions that produce chemical fuels. This multifunctional behavior will require the assimilation of multiple components into a single macromolecular system. A wide variety of different architectures including porphyrin arrays, peptides, dendrimers, and polymers have been explored, with each design posing unique challenges. Polymer assemblies are attractive due to their relative ease of production and facile synthetic modification. However, their disordered nature gives rise to stochastic dynamics not present in more ordered assemblies. The rational design of assemblies requires a detailed understanding of the energy and electron transfer events that follow light absorption, which can occur on timescales ranging from femtoseconds to hundreds of microseconds, necessitating the use of sophisticated techniques. We have used a combination of time-resolved absorption and emission spectroscopies with observation times that span nine orders of magnitude to follow the excited-state evolution within single-site and polymer-based molecular assemblies. We complement experimental observations with electronic structure calculations, molecular dynamics simulations, and kinetic modeling to develop a microscopic view of these dynamics. This thesis provides an overview of work on single-site molecular assemblies and polymers decorated with pendant chromophores, both in solution and on surfaces. This work was made possible through extensive collaboration with Dr. Kirk Schanze's and Dr. John Reynolds' research groups who

  11. Quantifying Transient States in Materials with the Dynamic Transmission Electron Microscope

    Energy Technology Data Exchange (ETDEWEB)

    Campbell, G; LaGrange, T; Kim, J; Reed, B; Browning, N

    2009-09-21

    The Dynamic Transmission Electron Microscope (DTEM) offers a means of capturing rapid evolution in a specimen through in-situ microscopy experiments by allowing 15 ns electron micrograph exposure times. The rapid exposure time is enabled by creating a burst of electrons at the emitter by ultraviolet pulsed laser illumination. This burst arrives a specified time after a second laser initiates the specimen reaction. The timing of the two Q-switched lasers is controlled by high-speed pulse generators with a timing error much less than the pulse duration. Both diffraction and imaging experiments can be performed, just as in a conventional TEM. The brightness of the emitter and the total current control the spatial and temporal resolutions. We have demonstrated 7 nm spatial resolution in single 15 ns pulsed images. These single-pulse imaging experiments have been used to study martensitic transformations, nucleation and crystallization of an amorphous metal, and rapid chemical reactions. Measurements have been performed on these systems that are possible by no other experimental approaches currently available.

  12. Studying Dynamic Processes of Nano-sized Objects in Liquid using Scanning Transmission Electron Microscopy.

    Science.gov (United States)

    Hermannsdörfer, Justus; de Jonge, Niels

    2017-02-05

    Samples fully embedded in liquid can be studied at a nanoscale spatial resolution with Scanning Transmission Electron Microscopy (STEM) using a microfluidic chamber assembled in the specimen holder for Transmission Electron Microscopy (TEM) and STEM. The microfluidic system consists of two silicon microchips supporting thin Silicon Nitride (SiN) membrane windows. This article describes the basic steps of sample loading and data acquisition. Most important of all is to ensure that the liquid compartment is correctly assembled, thus providing a thin liquid layer and a vacuum seal. This protocol also includes a number of tests necessary to perform during sample loading in order to ensure correct assembly. Once the sample is loaded in the electron microscope, the liquid thickness needs to be measured. Incorrect assembly may result in a too-thick liquid, while a too-thin liquid may indicate the absence of liquid, such as when a bubble is formed. Finally, the protocol explains how images are taken and how dynamic processes can be studied. A sample containing AuNPs is imaged both in pure water and in saline.

  13. Interaction of 3d transition metal atoms with charged ion projectiles from Electron Nuclear Dynamics computation

    Science.gov (United States)

    Hagelberg, Frank

    2003-03-01

    Computational results on atomic scattering between charged projectiles and transition metal target atoms are presented. This work aims at obtaining detailed information about charge, spin and energy transfer processes that occur between the interacting particles. An in-depth understanding of these phenomena is expected to provide a theoretical basis for the interpretation of various types of ion beam experiments, ranging from gas phase chromatography to spectroscopic observations of fast ions in ferromagnetic media. This contribution focuses on the scattering of light projectiles ranging from He to O, that are prepared in various initial charge states, by 3d transition metal atoms. The presented computations are performed in the framework of Electron Nuclear Dynamics (END)^1 theory which incorporates the coupling between electronic and nuclear degrees of freedom without reliance on the computationally cumbersome and frequently intractable determination of potential energy surfaces. In the present application of END theory to ion - transition metal atom scattering, a supermolecule approach is utilized in conjunction with a spin-unrestricted single determinantal wave function describing the electronic system. Integral scattering, charge and spin exchange cross sections are discussed as functions of the elementary parameters of the problem, such as projectile and target atomic numbers as well as projectile charge and initial kinetic energy. ^1 E.Deumens, A.Diz, R.Longo, Y.Oehrn, Rev.Mod.Phys. 66, 917 (1994)

  14. An Evaluation of Dynamic Partial Reconfiguration for Signal and Image Processing in Professional Electronics Applications

    Directory of Open Access Journals (Sweden)

    Philippe Manet

    2009-02-01

    Full Text Available Signal and image processing applications require a lot of computing resources. For low-volume applications like in professional electronics applications, FPGA are used in combination with DSP and GPP in order to reach the performances required by the product roadmaps. Nevertheless, FPGA designs are static, which raises a flexibility issue with new complex or software defined applications like software-defined radio (SDR. In this scope, dynamic partial reconfiguration (DPR is used to bring a virtualization layer upon the static hardware of FPGA. During the last decade, DPR has been widely studied in academia. Nevertheless, there are very few real applications using it, and therefore, there is a lack of feedback providing relevant issues to address in order to improve its applicability. This paper evaluates the interest and limitations when using DPR in professional electronics applications and provides guidelines to improve its applicability. It makes a fair evaluation based on experiments made on a set of signal and image processing applications. It identifies the missing elements of the design flow to use DPR in professional electronics applications. Finally, it introduces a fast reconfiguration manager providing an 84-time improvement compared to the vendor solution.

  15. Imaging surface acoustic wave dynamics in semiconducting polymers by scanning ultrafast electron microscopy.

    Science.gov (United States)

    Najafi, Ebrahim; Liao, Bolin; Scarborough, Timothy; Zewail, Ahmed

    2018-01-01

    Understanding the mechanical properties of organic semiconductors is essential to their electronic and photovoltaic applications. Despite a large volume of research directed toward elucidating the chemical, physical and electronic properties of these materials, little attention has been directed toward understanding their thermo-mechanical behavior. Here, we report the ultrafast imaging of surface acoustic waves (SAWs) on the surface of the Poly(3-hexylthiophene-2,5-diyl) (P3HT) thin film at the picosecond and nanosecond timescales. We then use these images to measure the propagation velocity of SAWs, which we then employ to determine the Young's modulus of P3HT. We further validate our experimental observation by performing a semi-empirical transient thermoelastic finite element analysis. Our findings demonstrate the potential of ultrafast electron microscopy to not only probe charge carrier dynamics in materials as previously reported, but also to measure their mechanical properties with great accuracy. This is particularly important when in situ characterization of stiffness for thin devices and nanomaterials is required. Copyright © 2017 Elsevier B.V. All rights reserved.

  16. An Evaluation of Dynamic Partial Reconfiguration for Signal and Image Processing in Professional Electronics Applications

    Directory of Open Access Journals (Sweden)

    Aulagnier Denis

    2008-01-01

    Full Text Available Abstract Signal and image processing applications require a lot of computing resources. For low-volume applications like in professional electronics applications, FPGA are used in combination with DSP and GPP in order to reach the performances required by the product roadmaps. Nevertheless, FPGA designs are static, which raises a flexibility issue with new complex or software defined applications like software-defined radio (SDR. In this scope, dynamic partial reconfiguration (DPR is used to bring a virtualization layer upon the static hardware of FPGA. During the last decade, DPR has been widely studied in academia. Nevertheless, there are very few real applications using it, and therefore, there is a lack of feedback providing relevant issues to address in order to improve its applicability. This paper evaluates the interest and limitations when using DPR in professional electronics applications and provides guidelines to improve its applicability. It makes a fair evaluation based on experiments made on a set of signal and image processing applications. It identifies the missing elements of the design flow to use DPR in professional electronics applications. Finally, it introduces a fast reconfiguration manager providing an 84-time improvement compared to the vendor solution.

  17. Effect of picosecond magnetic pulse on dynamics of electron's subbands in semiconductor bilayer nanowire

    Science.gov (United States)

    Chwiej, T.

    2017-10-01

    We report on possibility of charge current generation in nanowire made of two tunnel coupled one-dimensional electron waveguides by means of single magnetic pulse lasting up to 20 ps. Existence of interlayer tunnel coupling plays a crucial role in the effect described here as it allows for hybridization of the wave functions localized in different layers which can be dynamically modified by applying a time changeable in-plane magnetic field. Results of time-dependent DFT calculations performed for a bilayer nanowire confining many electrons show that the effect of such magnetic hybridization relies on tilting of electrons' energy subbands, to the left or to the right, depending on a sign of time derivative of oscillating magnetic field due to the Faraday law. Consequently, the tilted subbands become a source of charge flow along the wire. Strength of such magneto-induced current oscillations may achieve even 0.6 μA but it depends on duration of magnetic pulse as well as on charge density confined in nanowire which has to be unequally distributed between both transport layers to observe this effect.

  18. Spin noise spectroscopy in GaAs (110) quantum wells: access to intrinsic spin lifetimes and equilibrium electron dynamics.

    Science.gov (United States)

    Müller, Georg M; Römer, Michael; Schuh, Dieter; Wegscheider, Werner; Hübner, Jens; Oestreich, Michael

    2008-11-14

    In this Letter, the first spin noise spectroscopy measurements in semiconductor systems of reduced effective dimensionality are reported. The nondemolition measurement technique gives access to the otherwise concealed intrinsic, low temperature electron spin relaxation time of n-doped GaAs (110) quantum wells and to the corresponding low temperature anisotropic spin relaxation. The Brownian motion of the electrons within the spin noise probe laser spot becomes manifest in a modification of the spin noise line width. Thereby, the spatially resolved observation of the stochastic spin polarization uniquely allows to study electron dynamics at equilibrium conditions with a vanishing total momentum of the electron system.

  19. Local Dynamic Stability Assessment of Motion Impaired Elderly Using Electronic Textile Pants.

    Science.gov (United States)

    Liu, Jian; Lockhart, Thurmon E; Jones, Mark; Martin, Tom

    2008-10-01

    A clear association has been demonstrated between gait stability and falls in the elderly. Integration of wearable computing and human dynamic stability measures into home automation systems may help differentiate fall-prone individuals in a residential environment. The objective of the current study was to evaluate the capability of a pair of electronic textile (e-textile) pants system to assess local dynamic stability and to differentiate motion-impaired elderly from their healthy counterparts. A pair of e-textile pants comprised of numerous e-TAGs at locations corresponding to lower extremity joints was developed to collect acceleration, angular velocity and piezoelectric data. Four motion-impaired elderly together with nine healthy individuals (both young and old) participated in treadmill walking with a motion capture system simultaneously collecting kinematic data. Local dynamic stability, characterized by maximum Lyapunov exponent, was computed based on vertical acceleration and angular velocity at lower extremity joints for the measurements from both e-textile and motion capture systems. Results indicated that the motion-impaired elderly had significantly higher maximum Lyapunov exponents (computed from vertical acceleration data) than healthy individuals at the right ankle and hip joints. In addition, maximum Lyapunov exponents assessed by the motion capture system were found to be significantly higher than those assessed by the e-textile system. Despite the difference between these measurement techniques, attaching accelerometers at the ankle and hip joints was shown to be an effective sensor configuration. It was concluded that the e-textile pants system, via dynamic stability assessment, has the potential to identify motion-impaired elderly.

  20. Local Dynamic Stability Assessment of Motion Impaired Elderly Using Electronic Textile Pants

    Science.gov (United States)

    Liu, Jian; Lockhart, Thurmon E.; Jones, Mark; Martin, Tom

    2010-01-01

    A clear association has been demonstrated between gait stability and falls in the elderly. Integration of wearable computing and human dynamic stability measures into home automation systems may help differentiate fall-prone individuals in a residential environment. The objective of the current study was to evaluate the capability of a pair of electronic textile (e-textile) pants system to assess local dynamic stability and to differentiate motion-impaired elderly from their healthy counterparts. A pair of e-textile pants comprised of numerous e-TAGs at locations corresponding to lower extremity joints was developed to collect acceleration, angular velocity and piezoelectric data. Four motion-impaired elderly together with nine healthy individuals (both young and old) participated in treadmill walking with a motion capture system simultaneously collecting kinematic data. Local dynamic stability, characterized by maximum Lyapunov exponent, was computed based on vertical acceleration and angular velocity at lower extremity joints for the measurements from both e-textile and motion capture systems. Results indicated that the motion-impaired elderly had significantly higher maximum Lyapunov exponents (computed from vertical acceleration data) than healthy individuals at the right ankle and hip joints. In addition, maximum Lyapunov exponents assessed by the motion capture system were found to be significantly higher than those assessed by the e-textile system. Despite the difference between these measurement techniques, attaching accelerometers at the ankle and hip joints was shown to be an effective sensor configuration. It was concluded that the e-textile pants system, via dynamic stability assessment, has the potential to identify motion-impaired elderly. PMID:20953265

  1. Dynamics of energetic electrons interacting with sub-packet chorus emissions in the magnetosphere

    Science.gov (United States)

    Hiraga, R.; Omura, Y.

    2016-12-01

    The recent study has revealed RTA and URA processes, the acceleration of relativistic electrons by interaction with chorus emissions. The wave model, however, is found to require some updates based on the recent observations. We develop a new wave model compatible with the observations and study the particle motion under the influence of this new wave model. The most distinctive feature of the new model is its amplitude growth manner. The wave is excited near the equator and grows in amplitude as an absolute instability as a function of time. This amplitude growth is bounded by the optimum and threshold amplitudes. When the amplitude grows to reach the optimum amplitude, it drops down to the threshold value and repeats the growth with a saw-like shape defined as sub-packet wave. The sub-packet wave generated near the equator experiences the convective amplitude growth propagating to the higher latitude region. Since the group velocity of the wave propagation is a function of its frequency, a wave source generated and released from the equator at a certain time and a group velocity could be overtaken by another wave released at a later timing and hence a faster group velocity. In sub-packet case, this frequency value is further affected by the sub-packet amplitude wave form to make the process more complex. Into this new wave form, energetic electrons are inserted and their motions are examined. For example, a resonant electron can be entrapped by the wave, being accelerated and normally detrapped after a certain period of time, but there can be a possibility that the following sub-packet wave in a complex propagation manner coincidently entraps the electron to provide multiple accelerations. We injected a large number of electrons over a wide energy range from 10kev to 10Mev into the sub-packet wave to simulate the nonlinear dynamics of RTA and URA. The electrons motion or more precisely entrapping and detrapping processes are examined under various conditions.

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

    Science.gov (United States)

    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.

  3. Electronic and lattice dynamical properties of II-IV-N{sub 2} semiconductors

    Energy Technology Data Exchange (ETDEWEB)

    Punya, Atchara; Paudel, Tula R.; Lambrecht, Walter R.L. [Department of Physics, Case Western Reserve University, Cleveland, OH 444106-7079 (United States)

    2011-07-15

    The II-IV-N2 semiconductors constitute a family of heterovalent ternary semiconductors with properties closely related to those of the III-Nitrides. We here focus on Zn-IV-N2 semiconductors with the group IV-element Si, Ge and Sn. We present results on their electronic band structures obtained with the quasiparticle self-consistent GW method and the full-potential linearized muffin-tin orbital method. The latter is also used to calculate the energies of formation of these compounds from the constituent elements. The lattice dynamical properties were presented earlier in a series of papers and the main properties are briefly reviewed here. We emphasize the trends in the family of materials compared to those of the III-N and discuss the experimental data for the phonons. (copyright 2011 WILEY-VCH Verlag GmbH and Co. KGaA, Weinheim) (orig.)

  4. Electronic fine structure and recombination dynamics in single InAs quantum dots

    Energy Technology Data Exchange (ETDEWEB)

    Seguin, R.

    2008-01-28

    In the work at hand single InAs/GaAs quantum dots (QDs) are examined via cathodoluminescence spectroscopy. A thorough analysis of the spectra leads to an unambiguous assignment of the lines to the decay of specific excitonic complexes. A special aspect of the Coulomb interaction, the exchange interaction, gives rise to a fine structure in the initial and final states of an excitonic decay. This leads to a fine structure in the emission spectra that again is unique for every excitonic complex. The exchange interaction is discussed in great detail in this work.QDs of different sizes are investigated and the influence on the electronic properties is monitored. Additionally, the structure is modified ex situ by a thermal annealing process. The changes of the spectra under different annealing temperatures are traced. Finally, recombination dynamics of different excitonic complexes are examined by performing time-resolved cathodoluminescence spectroscopy. (orig.)

  5. Conditioned spin and charge dynamics of a single-electron quantum dot

    Science.gov (United States)

    Greplova, Eliska; Laird, Edward A.; Briggs, G. Andrew D.; Mølmer, Klaus

    2017-11-01

    In this article we describe the incoherent and coherent spin and charge dynamics of a single-electron quantum dot. We use a stochastic master equation to model the state of the system, as inferred by an observer with access to only the current signal through a quantum point contact, acting as a charge sensor. Measurements obtained during an interval of time contribute, by a past quantum state analysis, to our knowledge about the system at any time t within that interval. Such analysis permits precise estimation of physical parameters and we propose and test a modification of the classical Baum-Welch parameter reestimation method to systems driven by both coherent and incoherent processes.

  6. Multiple bunch longitudinal dynamics measurements at the Cornell Electron-Positron Storage Ring

    Directory of Open Access Journals (Sweden)

    R. Holtzapple

    2001-01-01

    Full Text Available The Cornell Electron-Positron Storage Ring (CESR has a longitudinal dipole-coupled-bunch instability that limits the total amount of current that can be stored in the ring without feedback. As a result, it is one of the major limitations for higher stored current and luminosity. This paper reports the measurements of multiple bunch longitudinal dynamics done on CESR with a streak camera. The camera was used to measure the dependence of the bunch distribution on current and accelerating rf voltage, for multiple bunches stored in CESR, as well as the effects of the longitudinal instability on the bunch distribution. Measurements of the beam's longitudinal bunch distribution with multiple bunches present in the ring help give an understanding of the instability, how it affects the bunch distribution, and possibly give insight into a cure of the instability.

  7. Electron-beam dynamics for an advanced flash-radiography accelerator

    Energy Technology Data Exchange (ETDEWEB)

    Ekdahl, Carl August Jr. [Los Alamos National Laboratory

    2015-06-22

    Beam dynamics issues were assessed for a new linear induction electron accelerator. Special attention was paid to equilibrium beam transport, possible emittance growth, and beam stability. Especially problematic would be high-frequency beam instabilities that could blur individual radiographic source spots, low-frequency beam motion that could cause pulse-to-pulse spot displacement, and emittance growth that could enlarge the source spots. Beam physics issues were examined through theoretical analysis and computer simulations, including particle-in cell (PIC) codes. Beam instabilities investigated included beam breakup (BBU), image displacement, diocotron, parametric envelope, ion hose, and the resistive wall instability. Beam corkscrew motion and emittance growth from beam mismatch were also studied. It was concluded that a beam with radiographic quality equivalent to the present accelerators at Los Alamos will result if the same engineering standards and construction details are upheld.

  8. SYSTEM DYNAMICS MODEL FOR EVALUATION OF REUSE OF ELECTRONIC WASTE ORIGINATED FROM PERSONAL COMPUTERS

    Directory of Open Access Journals (Sweden)

    Eugênio Simonetto

    2016-11-01

    Full Text Available Information and Communication Technologies (ICT are part of the day to day activities of a large part of world population, however its use involves a growing generation of electronic waste (ewaste. Due to the increasing technological innovation, it occurs that in a short time, the products become obsolete and have their life cycle reduced. The article aims to present the development, verification and validation of models of computational simulation for assessment of environmental and financial impacts caused by the extension of the life cycle of personal computers (PC through their remanufacturing. For the system modeling the System Dynamics theory was used. Results generated by the simulation model, show that the remanufacturing is a viable alternative for the reutilization of discarded computers and that it is possible, in advance, to discuss, assess and decide necessary measures for a better financial and environmental performance in the acquisition and use of ICT.

  9. Glassy Dynamics in Disordered Electronic Systems Reveal Striking Thermal Memory Effects

    Science.gov (United States)

    Eisenbach, A.; Havdala, T.; Delahaye, J.; Grenet, T.; Amir, A.; Frydman, A.

    2016-09-01

    Memory is one of the unique qualities of a glassy system. The relaxation of a glass to equilibrium contains information on the sample's excitation history, an effect often refer to as "aging." We demonstrate that under the right conditions a glass can also possess a different type of memory. We study the conductance relaxation of electron glasses that are fabricated at low temperatures. Remarkably, the dynamics are found to depend not only on the ambient measurement temperature but also on the maximum temperature to which the system was exposed. Hence the system "remembers" its highest temperature. This effect may be qualitatively understood in terms of energy barriers and local minima in configuration space and therefore may be a general property of the glass state.

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

    Energy Technology Data Exchange (ETDEWEB)

    Dabhi, Shweta D. [Department of Physics, Maharaja Krishnakumarsinhji Bhavnagar University, Bhavnagar 364001 (India); Gupta, Sanjay D. [V. B. Institute of Science, Department of Physics, C. U. Shah University, Wadhwan City - 363030, Surendranagar (India); Jha, Prafulla K., E-mail: prafullaj@yahoo.com [Department of Physics, Faculty of Science, The Maharaja Sayajirao University of Baroda, Vadodara-390002 (India)

    2014-05-28

    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.

  11. Modeling of temperature profiles in an environmental transmission electron microscope using computational fluid dynamics

    DEFF Research Database (Denmark)

    Mortensen, Peter Mølgaard; Jensen, Anker Degn; Hansen, Thomas Willum

    2015-01-01

    The temperature and velocity field, pressure distribution, and the temperature variation across the sample region inside an environmental transmission electron microscope (ETEM) have been modeled by means of computational fluid dynamics (CFD). Heating the sample area by a furnace type TEM holder ...... difference over the TEM grid is less than 5. °C, at what must be considered typical conditions, and it is concluded that the conditions on the sample grid in the ETEM can be considered as isothermal during general use....... gives rise to temperature gradients over the sample area. Three major mechanisms have been identified with respect to heat transfer in the sample area: radiation from the grid, conduction in the grid, and conduction in the gas. A parameter sensitivity analysis showed that the sample temperature...

  12. Tracking the charge and spin dynamics of electronic excited states in inorganic complexes

    Science.gov (United States)

    Gaffney, Kelly

    2015-03-01

    Inorganic complexes have many advantageous properties for solar energy applications, including strong visible absorption and photocatalytic activity. Whether used as a photocatalyst or a photosensitizer, the lifetime of electronic excited states and the earth abundance of the molecular components represent a key property for solar energy applications. These dual needs have undermined the usefulness of many coordination compounds. Isoelectronic iron and ruthenium based complexes represent a clear example. Ru-polypyridal based molecules have been the workhorse of solar energy related research and dye sensitized solar cells for decades, but the replacement of low abundance Ru with Fe leads to million-fold reductions in metal to ligand charge transfer (MLCT) excited state lifetimes. Understanding the origin of this million-fold reduction in lifetime and how to control excited state relaxation in 3d-metal complexes motivates the work I will discuss. We have used the spin sensitivity of hard x-ray fluorescence spectroscopy and the intense femtosecond duration pulses generated by the LCLS x-ray laser to probe the spin dynamics in a series of electronically excited [Fe(CN)6-2N(2,2'-bipyridine)N]2 N - 4 complexes, with N = 1-3. These femtosecond resolution measurements demonstrate that modification of the solvent and ligand environment can lengthen the MLCT excited state lifetime by more than two orders of magnitude. They also verify the role of triplet ligand field excited states in the spin crossover dynamics from singlet to quintet spin configurations. Work supported by the AMOS program within the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences, Office of Science, U.S. Department of Energy.

  13. Structural, Dynamical, and Electronic Transport Properties of Modified DNA Duplexes Containing Size-Expanded Nucleobases

    Energy Technology Data Exchange (ETDEWEB)

    Fuentes-Cabrera, Miguel A [ORNL; Orozco, Modesto [Institut de Recerca Biomedica, Parc Cientific de Barcelona, Barcelona, Spain; Luque, Javier [Universitat de Barcelona; Sumpter, Bobby G [ORNL; Blas, Jose [Universidad de Castilla-La Mancha; Ordejon, Pablo J [ORNL; Huertas, Oscar [Universitat de Barcelona; Tabares, Carolina [Universitat de Barcelona

    2011-01-01

    Among the distinct strategies proposed to expand the genetic alphabet, sizeexpanded nucleobases are promising for the development of modified DNA duplexes with improved biotechnological properties. In particular, duplexes built up by replacing canonical bases with the corresponding benzo-fused counterparts could be valuable as molecular nanowires. In this context, this study reports the results of classical molecular dynamics simulations carried out to examine the structural and dynamical features of size-expanded DNAs, including both hybrid duplexes containing mixed pairs of natural and benzo-fused bases (xDNA) and pure size-expanded (xxDNA) duplexes. Furthermore, the electronic structure of both natural and size-expanded duplexes is examined by means of density functional computations. The results confirm that the structural and flexibility properties of the canonical DNA are globally little affected by the presence of benzo-fused bases. Themost relevant differences are found in the enhanced size of the grooves, and the reduction in the twist. However, the analysis also reveals subtle structural effects related to the nature and sequence of benzo-fused bases in the duplex. On the other hand, electronic structure calculations performed for xxDNAs confirm the reduction in the HOMOLUMO gap predicted from the analysis of the natural bases and their size-expanded counterparts, which suggests that pure size-expanded DNAs can be good conductors. A more complex situation is found for xDNAs, where fluctuations in the electrostatic interaction between base pairs exerts a decisive influence on the modulation of the energy gap.

  14. Structure, Dynamics, and Electronic Properties of Lithium Disilicate Melt and Glass

    Energy Technology Data Exchange (ETDEWEB)

    Du, Jincheng; Corrales, Louis R.

    2006-09-18

    Ab initio molecular dynamics simulations within the framework of density functional theory (DFT) have been performed to study the structural, dynamic and electronic properties of lithium disilicate melt and the glass derived from quenching the melt. It is found that lithium ions have a much higher diffusion coefficient and show different diffusion mechanism than the network forming silicon and oxygen ions in the melt. The simulated lithium disilicate glass structure has 100% four coordinated silicon, close to theoretical non-bridging oxygen (NBO) to bridging oxygen (BO) ratio (2:3), and a Qn distribution of 20.8%, 58.4% and 20.8% for n=2,3,4 respectively. In the melt there are considerable amount (10-15%) of silicon coordination defects; however, the average silicon coordination number remains about 4, similar to that in the glass. The lithium ion coordination number increases from 3.7 in the glass to 4.4 in the melt mainly due to the increase of bridging oxygen in the first coordination shell. The bond length and bond angle distributions, vibrational density of states, and static structure factors of the simulated glass were determined where the latter was found to be in good agreement with experiment. Atomic charges were obtained based on Bader and Hirshfeld population analyses. The average Bader charges found in lithium disilicate glass were –1.729, 3.419, and 0.915 for oxygen, silicon and lithium, respectively. The corresponding Hirshfeld charges were –0.307, 0.550, and 0.229. The electronic density of states of the melt and glass were calculated and compared with those of crystalline lithium disilicate. Battelle operates PNNL for the USDOE

  15. Laser-induced electron dynamics including photoionization: A heuristic model within time-dependent configuration interaction theory.

    Science.gov (United States)

    Klinkusch, Stefan; Saalfrank, Peter; Klamroth, Tillmann

    2009-09-21

    We report simulations of laser-pulse driven many-electron dynamics by means of a simple, heuristic extension of the time-dependent configuration interaction singles (TD-CIS) approach. The extension allows for the treatment of ionizing states as nonstationary states with a finite, energy-dependent lifetime to account for above-threshold ionization losses in laser-driven many-electron dynamics. The extended TD-CIS method is applied to the following specific examples: (i) state-to-state transitions in the LiCN molecule which correspond to intramolecular charge transfer, (ii) creation of electronic wave packets in LiCN including wave packet analysis by pump-probe spectroscopy, and, finally, (iii) the effect of ionization on the dynamic polarizability of H(2) when calculated nonperturbatively by TD-CIS.

  16. Separation of electron and hole dynamics in the semimetal LaSb

    Energy Technology Data Exchange (ETDEWEB)

    Han, F.; Xu, J.; Botana, A. S.; Xiao, Z. L.; Wang, Y. L.; Yang, W. G.; Chung, D. Y.; Kanatzidis, M. G.; Norman, M. R.; Crabtree, G. W.; Kwok, W. K.

    2017-09-01

    We report investigations on the magnetotransport in LaSb, which exhibits extremely large magnetoresistance (XMR). Foremost, we demonstrate that the resistivity plateau can be explained without invoking topological protection. We then determine the Fermi surface from Shubnikov–de Haas (SdH) quantum oscillation measurements and find good agreement with the bulk Fermi pockets derived from first-principles calculations. Using a semiclassical theory and the experimentally determined Fermi pocket anisotropies, we quantitatively describe the orbital magnetoresistance, including its angle dependence.We show that the origin of XMR in LaSb lies in its high mobility with diminishing Hall effect, where the high mobility leads to a strong magnetic-field dependence of the longitudinal magnetoconductance. Unlike a one-band material, when a system has two or more bands (Fermi pockets) with electron and hole carriers, the added conductance arising from the Hall effect is reduced, hence revealing the latent XMR enabled by the longitudinal magnetoconductance. With diminishing Hall effect, the magnetoresistivity is simply the inverse of the longitudinal magnetoconductivity, enabling the differentiation of the electron and hole contributions to the XMR, which varies with the strength and orientation of the magnetic field. This work demonstrates a convenient way to separate the dynamics of the charge carriers and to uncover the origin of XMR in multiband materials with anisotropic Fermi surfaces. Our approach can be readily applied to other XMR materials.

  17. Separation of electron and hole dynamics in the semimetal LaSb

    Science.gov (United States)

    Han, F.; Xu, J.; Botana, A. S.; Xiao, Z. L.; Wang, Y. L.; Yang, W. G.; Chung, D. Y.; Kanatzidis, M. G.; Norman, M. R.; Crabtree, G. W.; Kwok, W. K.

    2017-09-01

    We report investigations on the magnetotransport in LaSb, which exhibits extremely large magnetoresistance (XMR). Foremost, we demonstrate that the resistivity plateau can be explained without invoking topological protection. We then determine the Fermi surface from Shubnikov-de Haas (SdH) quantum oscillation measurements and find good agreement with the bulk Fermi pockets derived from first-principles calculations. Using a semiclassical theory and the experimentally determined Fermi pocket anisotropies, we quantitatively describe the orbital magnetoresistance, including its angle dependence. We show that the origin of XMR in LaSb lies in its high mobility with diminishing Hall effect, where the high mobility leads to a strong magnetic-field dependence of the longitudinal magnetoconductance. Unlike a one-band material, when a system has two or more bands (Fermi pockets) with electron and hole carriers, the added conductance arising from the Hall effect is reduced, hence revealing the latent XMR enabled by the longitudinal magnetoconductance. With diminishing Hall effect, the magnetoresistivity is simply the inverse of the longitudinal magnetoconductivity, enabling the differentiation of the electron and hole contributions to the XMR, which varies with the strength and orientation of the magnetic field. This work demonstrates a convenient way to separate the dynamics of the charge carriers and to uncover the origin of XMR in multiband materials with anisotropic Fermi surfaces. Our approach can be readily applied to other XMR materials.

  18. Effect of self-interstitial diffusion anisotropy in electron-irradiated zirconium: A cluster dynamics modeling

    Science.gov (United States)

    Christien, F.; Barbu, A.

    2005-11-01

    A model based on the cluster dynamics approach was proposed in [A. Hardouin Duparc, C. Moingeon, N. Smetniansky-de-Grande, A. Barbu, J. Nucl. Mater. 302 (2002) 143] to describe point defect agglomeration in metals under irradiation. This model is restricted to materials where point defect diffusion is isotropic and is thus not applicable to anisotropic metals such as zirconium. Following the approach proposed by Woo [C.H. Woo, J. Nucl. Mater. 159 (1988) 237], we extended in this work the model to the case where self-interstitial atoms (SIA) diffusion is anisotropic. The model was then applied to the loop microstructure evolution of a zirconium thin foil irradiated with electrons in a high-voltage microscope. First, the inputs were validated by comparing the numerical results with Hellio et al. experimental results [C. Hellio, C.H. de Novion, L. Boulanger, J. Nucl. Mater. 159 (1988) 368]. Further calculations were made to evidence the effect of the thin foil orientation on the dislocation loop microstructure under irradiation. The result is that it is possible to reproduce for certain orientations the 'unexpected' vacancy loop growth experimentally observed in electron-irradiated zirconium [M. Griffiths, M.H. Loretto, R.E. Sallmann, J. Nucl. Mater. 115 (1983) 313; J. Nucl. Mater. 115 (1983) 323; Philos. Mag. A 49 (1984) 613]. This effect is directly linked to SIA diffusion anisotropy.

  19. Unified Approach towards the Dynamics of Optical and Electron Vortex Beams.

    Science.gov (United States)

    Bandyopadhyay, Pratul; Basu, Banasri; Chowdhury, Debashree

    2016-04-08

    We have proposed a unified framework towards the dynamics of optical and electron vortex beams from the perspective of the geometric phase and the associated Hall effects. The unification is attributed to the notion that the spin degrees of freedom of a relativistic particle, either massive or massless, are associated with a vortex line. Based on a cylindrical coordinate formulation, which leads to a local vortex structure related to orbital angular momentum (OAM), it can be shown that, when electron vortex beams (EVBs) move in an external electric field, paraxial beams give rise to an OAM Hall effect, and nonparaxial beams with tilted vortices initiate a spin Hall effect in free space as well as in an external field. A similar analysis reveals that the paraxial optical vortex beams (OVBs) in an inhomogeneous medium induce an OAM Hall effect, whereas nonparaxial beams with tilted vortices drive the spin Hall effect. Moreover, both OVBs and EVBs with tilted vortices give rise to OAM states with an arbitrary fractional value.

  20. Diagnosis and dynamics in a simple low energy medium current electron beam channel

    Science.gov (United States)

    Marghitu, S.; Marghitu, O.; Oproiu, C.; Marin, G.; Scarlat, Fl.

    2004-05-01

    We present a simple experimental setup and an associated method enabling both the non-destructive diagnosis and the calculation of the beam evolution in a low energy medium current electron beam channel, where the space-charge and emittance effects are comparable. The diagnosis makes use of an axially symmetric magnetic lens while a second lens is added to increase the flexibility in the beam processing. The paper emphasizes the three steps involved in the method: the evaluation of the lenses' magnetic field by numerical simulation, the beam diagnosis, and the computation of the beam envelope. The calculation of the magnetic field is based on the finite element method. Subsequently, the beam parameters at the electron source exit - emittance and cross-over radius and position - are found with the modified three gradient method. Finally, the beam dynamics are modeled with the K-V equation adapted for the particular case of axial symmetry. The results obtained in this paper can be used to optimize technological processes, such as welding, hardening, cladding, and surface alloying.

  1. Batch crystallization of rhodopsin for structural dynamics using an X-ray free-electron laser

    Energy Technology Data Exchange (ETDEWEB)

    Wu, Wenting; Nogly, Przemyslaw; Rheinberger, Jan; Kick, Leonhard M.; Gati, Cornelius; Nelson, Garrett; Deupi, Xavier; Standfuss, Jörg; Schertler, Gebhard; Panneels, Valérie, E-mail: valerie.panneels@psi.ch [Paul Scherrer Institute, OFLC/103, 5232 Villigen-PSI (Switzerland)

    2015-06-27

    A new batch preparation method is presented for high-density micrometre-sized crystals of the G protein-coupled receptor rhodopsin for use in time-resolved serial femtosecond crystallography at an X-ray free-electron laser using a liquid jet. Rhodopsin is a membrane protein from the G protein-coupled receptor family. Together with its ligand retinal, it forms the visual pigment responsible for night vision. In order to perform ultrafast dynamics studies, a time-resolved serial femtosecond crystallography method is required owing to the nonreversible activation of rhodopsin. In such an approach, microcrystals in suspension are delivered into the X-ray pulses of an X-ray free-electron laser (XFEL) after a precise photoactivation delay. Here, a millilitre batch production of high-density microcrystals was developed by four methodical conversion steps starting from known vapour-diffusion crystallization protocols: (i) screening the low-salt crystallization conditions preferred for serial crystallography by vapour diffusion, (ii) optimization of batch crystallization, (iii) testing the crystal size and quality using second-harmonic generation (SHG) imaging and X-ray powder diffraction and (iv) production of millilitres of rhodopsin crystal suspension in batches for serial crystallography tests; these crystals diffracted at an XFEL at the Linac Coherent Light Source using a liquid-jet setup.

  2. Atomic and electronic structures of a-SiC:H from tight-binding molecular dynamics

    CERN Document Server

    Ivashchenko, V I; Shevchenko, V I; Ivashchenko, L A; Rusakov, G V

    2003-01-01

    The atomic and electronic properties of amorphous unhydrogenated (a-SiC) and hydrogenated (a-SiC:H) silicon carbides are studied using an sp sup 3 s sup * tight-binding force model with molecular dynamics simulations. The parameters of a repulsive pairwise potential are determined from ab initio pseudopotential calculations. Both carbides are generated from dilute vapours condensed from high temperature, with post-annealing at low temperature for a-SiC:H. A plausible model for the inter-atomic correlations and electronic states in a-SiC:H is suggested. According to this model, the formation of the amorphous network is weakly sensitive to the presence of hydrogen. Hydrogen passivates effectively only the weak bonds of threefold-coordinated atoms. Chemical ordering is very much affected by the cooling rate and the structure of the high-temperature vapour. The as-computed characteristics are in rather good agreement with the results for a-SiC and a-Si:H from ab initio calculations.

  3. Dynamical mean-field theory and path integral renormalisation group calculations of strongly correlated electronic states

    Energy Technology Data Exchange (ETDEWEB)

    Heilmann, D.B.

    2007-02-15

    The two-plane HUBBARD model, which is a model for some electronic properties of undoped YBCO superconductors as well as displays a MOTT metal-to-insulator transition and a metal-to-band insulator transition, is studied within Dynamical Mean-Field Theory using HIRSCH-FYE Monte Carlo. In order to find the different transitions and distinguish the types of insulator, we calculate the single-particle spectral densities, the self-energies and the optical conductivities. We conclude that there is a continuous transition from MOTT to band insulator. In the second part, ground state properties of a diagonally disordered HUBBARD model is studied using a generalisation of Path Integral Renormalisation Group, a variational method which can also determine low-lying excitations. In particular, the distribution of antiferromagnetic properties is investigated. We conclude that antiferromagnetism breaks down in a percolation-type transition at a critical disorder, which is not changed appreciably by the inclusion of correlation effects, when compared to earlier studies. Electronic and excitation properties at the system sizes considered turn out to primarily depend on the geometry. (orig.)

  4. Modeling of temperature profiles in an environmental transmission electron microscope using computational fluid dynamics

    Energy Technology Data Exchange (ETDEWEB)

    Mølgaard Mortensen, Peter [Department of Chemical and Biochemical Engineering, Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Willum Hansen, Thomas [Center for Electron Nanoscopy, Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Birkedal Wagner, Jakob, E-mail: jakob.wagner@cen.dtu.dk [Center for Electron Nanoscopy, Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark); Degn Jensen, Anker, E-mail: aj@kt.dtu.dk [Department of Chemical and Biochemical Engineering, Technical University of Denmark, DK-2800 Kgs. Lyngby (Denmark)

    2015-05-15

    The temperature and velocity field, pressure distribution, and the temperature variation across the sample region inside an environmental transmission electron microscope (ETEM) have been modeled by means of computational fluid dynamics (CFD). Heating the sample area by a furnace type TEM holder gives rise to temperature gradients over the sample area. Three major mechanisms have been identified with respect to heat transfer in the sample area: radiation from the grid, conduction in the grid, and conduction in the gas. A parameter sensitivity analysis showed that the sample temperature was affected by the conductivity of the gas, the emissivity of the sample grid, and the conductivity of the grid. Ideally the grid should be polished and made from a material with good conductivity, e.g. copper. With hydrogen gas, which has the highest conductivity of the gases studied, the temperature difference over the TEM grid is less than 5 °C, at what must be considered typical conditions, and it is concluded that the conditions on the sample grid in the ETEM can be considered as isothermal during general use. - Highlights: • Computational fluid dynamics used for mapping flow and temperature in ETEM setup. • Temperature gradient across TEM grid in furnace based heating holder very small in ETEM. • Conduction from TEM grid and gas in addition to radiation from TEM grid most important. • Pressure drop in ETEM limited to the pressure limiting apertures.

  5. Molecular dynamics-based refinement and validation for sub-5 Å cryo-electron microscopy maps

    Science.gov (United States)

    Singharoy, Abhishek; Teo, Ivan; McGreevy, Ryan; Stone, John E; Zhao, Jianhua; Schulten, Klaus

    2016-01-01

    Two structure determination methods, based on the molecular dynamics flexible fitting (MDFF) paradigm, are presented that resolve sub-5 Å cryo-electron microscopy (EM) maps with either single structures or ensembles of such structures. The methods, denoted cascade MDFF and resolution exchange MDFF, sequentially re-refine a search model against a series of maps of progressively higher resolutions, which ends with the original experimental resolution. Application of sequential re-refinement enables MDFF to achieve a radius of convergence of ~25 Å demonstrated with the accurate modeling of β-galactosidase and TRPV1 proteins at 3.2 Å and 3.4 Å resolution, respectively. The MDFF refinements uniquely offer map-model validation and B-factor determination criteria based on the inherent dynamics of the macromolecules studied, captured by means of local root mean square fluctuations. The MDFF tools described are available to researchers through an easy-to-use and cost-effective cloud computing resource on Amazon Web Services. DOI: http://dx.doi.org/10.7554/eLife.16105.001 PMID:27383269

  6. Ribosome dynamics and tRNA movement by time-resolved electron cryomicroscopy.

    Science.gov (United States)

    Fischer, Niels; Konevega, Andrey L; Wintermeyer, Wolfgang; Rodnina, Marina V; Stark, Holger

    2010-07-15

    The translocation step of protein synthesis entails large-scale rearrangements of the ribosome-transfer RNA (tRNA) complex. Here we have followed tRNA movement through the ribosome during translocation by time-resolved single-particle electron cryomicroscopy (cryo-EM). Unbiased computational sorting of cryo-EM images yielded 50 distinct three-dimensional reconstructions, showing the tRNAs in classical, hybrid and various novel intermediate states that provide trajectories and kinetic information about tRNA movement through the ribosome. The structures indicate how tRNA movement is coupled with global and local conformational changes of the ribosome, in particular of the head and body of the small ribosomal subunit, and show that dynamic interactions between tRNAs and ribosomal residues confine the path of the tRNAs through the ribosome. The temperature dependence of ribosome dynamics reveals a surprisingly flat energy landscape of conformational variations at physiological temperature. The ribosome functions as a Brownian machine that couples spontaneous conformational changes driven by thermal energy to directed movement.

  7. Structural, Dynamical, and Electronic Properties of Liquid Water: A Hybrid Functional Study.

    Science.gov (United States)

    Ambrosio, Francesco; Miceli, Giacomo; Pasquarello, Alfredo

    2016-08-04

    We study structural, dynamical, and electronic properties of liquid water through ab initio molecular dynamics (MD) simulations based on a hybrid functional which includes nonlocal van der Waals (vdW) interactions. The water dimer, the water hexamer, and two phases of ice are studied as benchmark cases. The hydrogen-bond energy depends on the balance between Fock exchange and vdW interactions. Moreover, the energetic competition between extended and compact structural motifs is found to be well described by theory provided vdW interactions are accounted for. Applied to the hydrogen-bond network of liquid water, the dispersion interactions favor more compact structural motifs, bring the density closer to the experimental value, and improve the agreement with experimental observables such as radial distribution functions. The description of the self-diffusion coefficient is also found to improve upon the combined consideration of Fock exchange and vdW interactions. The band gap and the band edges are found to agree with experiment within 0.1 eV.

  8. Dynamic analysis and electronic circuit implementation of a novel 3D autonomous system without linear terms

    Science.gov (United States)

    Kengne, J.; Jafari, S.; Njitacke, Z. T.; Yousefi Azar Khanian, M.; Cheukem, A.

    2017-11-01

    Mathematical models (ODEs) describing the dynamics of almost all continuous time chaotic nonlinear systems (e.g. Lorenz, Rossler, Chua, or Chen system) involve at least a nonlinear term in addition to linear terms. In this contribution, a novel (and singular) 3D autonomous chaotic system without linear terms is introduced. This system has an especial feature of having two twin strange attractors: one ordinary and one symmetric strange attractor when the time is reversed. The complex behavior of the model is investigated in terms of equilibria and stability, bifurcation diagrams, Lyapunov exponent plots, time series and Poincaré sections. Some interesting phenomena are found including for instance, period-doubling bifurcation, antimonotonicity (i.e. the concurrent creation and annihilation of periodic orbits) and chaos while monitoring the system parameters. Compared to the (unique) case previously reported by Xu and Wang (2014) [31], the system considered in this work displays a more 'elegant' mathematical expression and experiences richer dynamical behaviors. A suitable electronic circuit (i.e. the analog simulator) is designed and used for the investigations. Pspice based simulation results show a very good agreement with the theoretical analysis.

  9. High-speed nanoscale characterization of dewetting via dynamic transmission electron microscopy

    Science.gov (United States)

    Hihath, Sahar; Santala, Melissa K.; Campbell, Geoffrey; van Benthem, Klaus

    2016-08-01

    The dewetting of thin films can occur in either the solid or the liquid state for which different mass transport mechanisms are expected to control morphological changes. Traditionally, dewetting dynamics have been examined on time scales between several seconds to hours, and length scales ranging between nanometers and millimeters. The determination of mass transport mechanisms on the nanoscale, however, requires nanoscale spatial resolution and much shorter time scales. This study reports the high-speed observation of dewetting phenomena for kinetically constrained Ni thin films on crystalline SrTiO3 substrates. Movie-mode Dynamic Transmission Electron Microscopy (DTEM) was used for high-speed image acquisition during thin film dewetting at different temperatures. DTEM imaging confirmed that the initial stages of film agglomeration include edge retraction, hole formation, and growth. Finite element modeling was used to simulate temperature distributions within the DTEM samples after laser irradiation with different energies. For pulsed laser irradiation at 18 μJ, experimentally observed hole growth suggests that Marangoni flow dominates hole formation in the liquid nickel film. After irradiation with 13.8 μJ, however, the observations suggest that dewetting was initiated by nucleation of voids followed by hole growth through solid-state surface diffusion.

  10. Graphene on Ni(111): Electronic Corrugation and Dynamics from Helium Atom Scattering.

    Science.gov (United States)

    Tamtögl, Anton; Bahn, Emanuel; Zhu, Jianding; Fouquet, Peter; Ellis, John; Allison, William

    2015-11-19

    Using helium atom scattering, we have studied the structure and dynamics of a graphene layer prepared in situ on a Ni(111) surface. Graphene/Ni(111) exhibits a helium reflectivity of ∼20% for a thermal helium atom beam and a particularly small surface electron density corrugation ((0.06 ± 0.02) Å peak to peak height). The Debye-Waller attenuation of the elastic diffraction peaks of graphene/Ni(111) and Ni(111) was measured at surface temperatures between 150 and 740 K. A surface Debye temperature of θD = (784 ± 14) K is determined for the graphene/Ni(111) system and θD = (388 ± 7) K for Ni(111), suggesting that the interlayer interaction between graphene and the Ni substrate is intermediary between those for strongly interacting systems like graphene/Ru(0001) and weakly interacting systems like graphene/Pt(111). In addition we present measurements of low frequency surface phonon modes on graphene/Ni(111) where the phonon modes of the Ni(111) substrate can be clearly observed. The similarity of these findings with the graphene/Ru(0001) system indicates that the bonding of graphene to a metal substrate alters the dynamic properties of the graphene surface strongly and is responsible for the high helium reflectivity of these systems.

  11. Optically Controlled Electron-Transfer Reaction Kinetics and Solvation Dynamics: Effect of Franck-Condon States.

    Science.gov (United States)

    Gupta, Kriti; Patra, Aniket; Dhole, Kajal; Samanta, Alok Kumar; Ghosh, Swapan K

    2017-09-21

    Experimental results for optically controlled electron-transfer reaction kinetics (ETRK) and nonequilibrium solvation dynamics (NESD) of Coumarin 480 in DMPC vesicle show their dependence on excitation wavelength λex. However, the celebrated Marcus theory and linear-response-theory-based approaches for ETRK and NESD, respectively, predict both of the processes to be independent of λex. The above said lacuna in these theories prompted us to develop a novel theory in 1D space, where the effect of innumerable Franck-Condon states is included through λex. The present theory not only sheds light on the origin of failure of the existing theories but also gives the correct trend for the effect of λex on ETRK and NESD. More importantly, the calculated results of NESD are in excellent agreement with the experimental results for different values of λex. The new theory will therefore advance the knowledge of scientific community on the dynamics of photoinduced nonequilibrium processes.

  12. Moving solvated electrons with light: nonadiabatic mixed quantum/classical molecular dynamics simulations of the relocalization of photoexcited solvated electrons in tetrahydrofuran (THF).

    Science.gov (United States)

    Bedard-Hearn, Michael J; Larsen, Ross E; Schwartz, Benjamin J

    2006-11-21

    Motivated by recent ultrafast spectroscopic experiments [Martini et al., Science 293, 462 (2001)], which suggest that photoexcited solvated electrons in tetrahydrofuran (THF) can relocalize (that is, return to equilibrium in solvent cavities far from where they started), we performed a series of nonequilibrium, nonadiabatic, mixed quantum/classical molecular dynamics simulations that mimic one-photon excitation of the THF-solvated electron. We find that as photoexcited THF-solvated electrons relax to their ground states either by continuous mixing from the excited state or via nonadiabatic transitions, approximately 30% of them relocalize into cavities that can be over 1 nm away from where they originated, in close agreement with the experiments. A detailed investigation shows that the ability of excited THF-solvated electrons to undergo photoinduced relocalization stems from the existence of preexisting cavity traps that are an intrinsic part of the structure of liquid THF. This explains why solvated electrons can undergo photoinduced relocalization in solvents like THF but not in solvents like water, which lack the preexisting traps necessary to stabilize the excited electron in other places in the fluid. We also find that even when they do not ultimately relocalize, photoexcited solvated electrons in THF temporarily visit other sites in the fluid, explaining why the photoexcitation of THF-solvated electrons is so efficient at promoting recombination with nearby scavengers. Overall, our study shows that the defining characteristic of a liquid that permits the photoassisted relocalization of solvated electrons is the existence of nascent cavities that are attractive to an excess electron; we propose that other such liquids can be found from classical computer simulations or neutron diffraction experiments.

  13. Pump-probe reflectivity study of ultrafast dynamics of strongly correlated 5f electrons inUO2

    Energy Technology Data Exchange (ETDEWEB)

    Au, Yongqiang Q [Los Alamos National Laboratory; Taylor, Antoinette J [Los Alamos National Laboratory; Durakiewicz, Tomasz [Los Alamos National Laboratory; Rodriguez, George [Los Alamos National Laboratory

    2010-01-01

    5f electrons in the Mott insulator UO{sub 2} produce intriguing electronic states and dynamics, such as strong correlation and f-f excitations. We have performed femtosecond pump-probe reflectivity measurements on a single crystal UO{sub 2} at temperatures 5-300 K to study the ultrafast dynamics of photoexcited 5f electrons. The laser pulses at 400 nm pump 5 f electrons across the Mott gap, while those at 800 nm probe the pump-induced change of reflectivity. We find temperature-dependent excitation and relaxation processes and long-lived acoustic phonons, and extract picosecond risetimes and microsecond relaxation times at low temperatures. The observed slow relaxation is ascribed to the decay of Hubbard excitons formed by U{sup 3+}-U{sup 5+} pairs.

  14. Electron arc therapy: design, implementation and evaluation of a dynamic multi-vane collimator system.

    Science.gov (United States)

    Leavitt, D D; Stewart, J R; Moeller, J H; Lee, W L; Takach, G A

    1989-11-01

    Innovative techniques in motion control technology have been applied to the design and implementation of a portable computer-controlled multi-vane collimator for use in electron arc therapy. The collimator, consisting of 18 independently controlled vanes, is inserted into the standard accessory mount assembly of a linear accelerator, in the same fashion as standard field shaping blocks. Power is supplied to the collimator vane motors via a self-contained battery system. The range of motion of the vanes, symmetrically mounted nine on each side, provides a variable aperture width projected to isocenter of 2 cm minimum to 8 cm maximum. The projected length of the aperture at isocenter is 38 cm. The transition time between vane positions is less than 1 second, corresponding to gantry movement of less than 1 degree. The movement of each of the 18 vanes is monitored and controlled by six individually addressed three axis processors that are shielded from the electron beam. A table of collimator vane positions versus gantry angle, as determined by dose optimization calculations, is stored in a data file. The desired collimator vane position corresponding to the current arc segment is conveyed from the control console to each vane controller via packets within a token passing network. Communication between the computer in the console area and the vane controllers is accomplished through encoded infra-red pulse transmission, eliminating the need for additional communication lines between the console and the accelerator. This dynamic collimator offers improved dose uniformity while simplifying the delivery of electron arc therapy.

  15. Electron cyclotron resonance near the axis of the gas-dynamic trap

    Science.gov (United States)

    Bagulov, D. S.; Kotelnikov, I. A.

    2012-08-01

    Propagation of an extraordinary electromagnetic wave in the vicinity of electron cyclotron resonance surface in an open linear trap is studied analytically, taking into account inhomogeneity of the magnetic field in paraxial approximation. Ray trajectories are derived from a reduced dispersion equation that makes it possible to avoid the difficulty associated with a transition from large propagation angles to the case of strictly longitudinal propagation. Our approach is based on the theory, originally developed by Zvonkov and Timofeev [Sov. J. Plasma Phys. 14, 743 (1988)], who used the paraxial approximation for the magnetic field strength, but did not consider the slope of the magnetic field lines, which led to considerable error, as has been recently noted by Gospodchikov and Smolyakova [Plasma Phys. Rep. 37, 768-774 (2011)]. We have found ray trajectories in analytic form and demonstrated that the inhomogeneity of both the magnetic field strength and the field direction can qualitatively change the picture of wave propagation and significantly affect the efficiency of electron cyclotron heating of a plasma in a linear magnetic trap. Analysis of the ray trajectories has revealed a criterion for the resonance point on the axis of the trap to be an attractor for the ray trajectories. It is also shown that a family of ray trajectories can still reach the resonance point on the axis if the latter generally repels the ray trajectories. As an example, results of general theory are applied to the electron cyclotron resonance heating experiment which is under preparation on the gas dynamic trap in the Budker Institute of Nuclear Physics [Shalashov et al., Phys. Plasmas 19, 052503 (2012)].

  16. Time-dependent density-functional theory simulation for electron-ion dynamics in molecules under intense laser pulses.

    Science.gov (United States)

    Kawashita, Y; Nakatsukasa, T; Yabana, K

    2009-02-11

    We have developed a simulation method to describe three-dimensional dynamics of electrons and ions in a molecule based on the time-dependent density-functional theory. We solve the time-dependent Kohn-Sham equation for electrons employing the real-space and real-time method, while the ion dynamics are described in classical mechanics by the Ehrenfest method. For an efficient calculation in massively parallel computers, the code is parallelized dividing the spatial grid points. We apply the method to the Coulomb explosion of the H(2)S molecule under an intense and ultrashort laser pulse and investigate the mechanism of the process.

  17. Operation of a quantum dot in the finite-state machine mode: Single-electron dynamic memory

    Energy Technology Data Exchange (ETDEWEB)

    Klymenko, M. V. [Department of Chemistry, University of Liège, B4000 Liège (Belgium); Klein, M. [The Fritz Haber Center for Molecular Dynamics and the Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 91904 (Israel); Levine, R. D. [The Fritz Haber Center for Molecular Dynamics and the Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 91904 (Israel); Crump Institute for Molecular Imaging and Department of Molecular and Medical Pharmacology, David Geffen School of Medicine and Department of Chemistry and Biochemistry, University of California, Los Angeles, California 90095 (United States); Remacle, F., E-mail: fremacle@ulg.ac.be [Department of Chemistry, University of Liège, B4000 Liège (Belgium); The Fritz Haber Center for Molecular Dynamics and the Institute of Chemistry, The Hebrew University of Jerusalem, Jerusalem 91904 (Israel)

    2016-07-14

    A single electron dynamic memory is designed based on the non-equilibrium dynamics of charge states in electrostatically defined metallic quantum dots. Using the orthodox theory for computing the transfer rates and a master equation, we model the dynamical response of devices consisting of a charge sensor coupled to either a single and or a double quantum dot subjected to a pulsed gate voltage. We show that transition rates between charge states in metallic quantum dots are characterized by an asymmetry that can be controlled by the gate voltage. This effect is more pronounced when the switching between charge states corresponds to a Markovian process involving electron transport through a chain of several quantum dots. By simulating the dynamics of electron transport we demonstrate that the quantum box operates as a finite-state machine that can be addressed by choosing suitable shapes and switching rates of the gate pulses. We further show that writing times in the ns range and retention memory times six orders of magnitude longer, in the ms range, can be achieved on the double quantum dot system using experimentally feasible parameters, thereby demonstrating that the device can operate as a dynamic single electron memory.

  18. Molecular dynamics and simulations study on the vibrational and electronic solvatochromism of benzophenone

    Energy Technology Data Exchange (ETDEWEB)

    Ravi Kumar, Venkatraman; Umapathy, Siva, E-mail: umapathy@ipc.iisc.ernet.in, E-mail: chandra@bii.a-star.edu.sg [Inorganic and Physical Chemistry Department, Indian Institute of Science, Bangalore 560012 (India); Verma, Chandra, E-mail: umapathy@ipc.iisc.ernet.in, E-mail: chandra@bii.a-star.edu.sg [Bioinformatics Institute - A*STAR, 30 Biopolis Street, # 07-01 Matrix, Singapore 138671 (Singapore); School of Biological Sciences, Nanyang Technological University, 60 Nanyang Drive, Singapore 637551 (Singapore); Department of Biological Sciences, National University of Singapore, 14 Science Drive 4, Singapore 117543 (Singapore)

    2016-02-14

    Solvent plays a key role in diverse physico-chemical and biological processes. Therefore, understanding solute-solvent interactions at the molecular level of detail is of utmost importance. A comprehensive solvatochromic analysis of benzophenone (Bzp) was carried out in various solvents using Raman and electronic spectroscopy, in conjunction with Density Functional Theory (DFT) calculations of supramolecular solute-solvent clusters generated using classical Molecular Dynamics Simulations (c-MDSs). The >C=O stretching frequency undergoes a bathochromic shift with solvent polarity. Interestingly, in protic solvents this peak appears as a doublet: c-MDS and ad hoc explicit solvent ab initio calculations suggest that the lower and higher frequency peaks are associated with the hydrogen bonded and dangling carbonyl group of Bzp, respectively. Additionally, the dangling carbonyl in methanol (MeOH) solvent is 4 cm{sup −1} blue-shifted relative to acetonitrile solvent, despite their similar dipolarity/polarizability. This suggests that the cybotactic region of the dangling carbonyl group in MeOH is very different from its bulk solvent structure. Therefore, we propose that this blue-shift of the dangling carbonyl originates in the hydrophobic solvation shell around it resulting from extended hydrogen bonding network of the protic solvents. Furthermore, the 1{sup 1}nπ{sup ∗} (band I) and 1{sup 1}ππ{sup ∗} (band II) electronic transitions show a hypsochromic and bathochromic shift, respectively. In particular, these shifts in protic solvents are due to differences in their excited state-hydrogen bonding mechanisms. Additionally, a linear relationship is obtained for band I and the >C=O stretching frequency (cm{sup −1}), which suggests that the different excitation wavelengths in band I correspond to different solvation states. Therefore, we hypothesize that the variation in excitation wavelengths in band I could arise from different solvation states leading to

  19. The near ultraviolet photodissociation dynamics of 2- and 3-substituted thiophenols: Geometric vs. electronic structure effects

    Science.gov (United States)

    Marchetti, Barbara; Karsili, Tolga N. V.; Cipriani, Maicol; Hansen, Christopher S.; Ashfold, Michael N. R.

    2017-07-01

    The near ultraviolet spectroscopy and photodissociation dynamics of two families of asymmetrically substituted thiophenols (2- and 3-YPhSH, with Y = F and Me) have been investigated experimentally (by H (Rydberg) atom photofragment translational spectroscopy) and by ab initio electronic structure calculations. Photoexcitation in all cases populates the 11ππ* and/or 11πσ* excited states and results in S-H bond fission. Analyses of the experimentally obtained total kinetic energy release (TKER) spectra yield the respective parent S-H bond strengths, estimates of ΔE(A ˜ -X ˜ ), the energy splitting between the ground (X ˜ ) and first excited (A ˜ ) states of the resulting 2-(3-)YPhS radicals, and reveal a clear propensity for excitation of the C-S in-plane bending vibration in the radical products. The companion theory highlights roles for both geometric (e.g., steric effects and intramolecular H-bonding) and electronic (i.e., π (resonance) and σ (inductive)) effects in determining the respective parent minimum energy geometries, and the observed substituent and position-dependent trends in S-H bond strength and ΔE(A ˜ -X ˜ ). 2-FPhSH shows some clear spectroscopic and photophysical differences. Intramolecular H-bonding ensures that most 2-FPhSH molecules exist as the syn rotamer, for which the electronic structure calculations return a substantial barrier to tunnelling from the photoexcited 11ππ* state to the 11πσ* continuum. The 11ππ* ← S0 excitation spectrum of syn-2-FPhSH thus exhibits resolved vibronic structure, enabling photolysis studies with a greater parent state selectivity. Structure apparent in the TKER spectrum of the H + 2-FPhS products formed when exciting at the 11ππ* ← S0 origin is interpreted by assuming unintended photoexcitation of an overlapping resonance associated with syn-2-FPhSH(v33 = 1) molecules. The present data offer tantalising hints that such out-of-plane motion influences non-adiabatic coupling in the vicinity

  20. Matching sub-fs electron bunches for laser-driven plasma acceleration at SINBAD

    Energy Technology Data Exchange (ETDEWEB)

    Zhu, J., E-mail: jun.zhu@desy.de [Deutsches Elektronen-Synchrotron, DESY, Hamburg (Germany); Universität Hamburg, Hamburg (Germany); Assmann, R.W.; Dorda, U.; Marchetti, B. [Deutsches Elektronen-Synchrotron, DESY, Hamburg (Germany)

    2016-09-01

    We present theoretical and numerical studies of matching sub-femtosecond space-charge-dominated electron bunch into the Laser-plasma Wake Field Accelerator (LWFA) foreseen at the SINBAD facility. The longitudinal space-charge (SC) effect induced growths of the energy spread and longitudinal phase-space chirp are major issues in the matching section, which will result in bunch elongation, emittance growth and spot size dilution. In addition, the transverse SC effect would lead to a mismatch of the beam optics if it were not compensated for. Start-to-end simulations and preliminary optimizations were carried out in order to understand the achievable beam parameters at the entrance of the plasma accelerator.

  1. Dynamic response of a two-dimensional electron gas: Effect of short-range correlations in the ladder approximation

    Science.gov (United States)

    Takayanagi, K.; Lipparini, E.

    1996-09-01

    The Dyson equation for the particle-hole Green's function, including exchange matrix elements, has been solved exactly for the effective interaction between two electrons in a two-dimensional electron gas. The effective interaction is obtained numerically by solving the Bethe-Goldstone integral equation in a two-dimensional electron gas. The effect of short-range correlations on static and dynamic dielectric functions is studied. Results are compared with the normal random-phase approximation, local-field theories, and recent quantum Monte Carlo results.

  2. Ultrafast electron spin dynamics in ZnO and Zn1-xCoxO sol-gel thin films

    Directory of Open Access Journals (Sweden)

    Leitenstorfer A.

    2013-03-01

    Full Text Available We probe the electron spin dynamics in ZnO and Zn1-xCoxO sol-gel films with time-resolved Faraday rotation spectroscopy. Dephasing times T2* on the order of nanoseconds are observed at room temperature due to charge-separated states. In ZnCoO the effective electron Landé g factor rises with increasing Co2+ concentration, providing the mean-field electron-Co2+ exchange energy N0α = +0.25 ± 0.02 eV.

  3. High-throughput rear-surface drilling of microchannels in glass based on electron dynamics control using femtosecond pulse trains.

    Science.gov (United States)

    Jiang, Lan; Liu, Pengjun; Yan, Xueliang; Leng, Ni; Xu, Chuancai; Xiao, Hai; Lu, Yongfeng

    2012-07-15

    This study proposes a rear-surface ablation enhancement approach to fabricate high-aspect-ratio microchannels by temporally shaping femtosecond laser pulse trains. In the case study of K9 glass, enhancements of up to a 56 times higher material removal rate and a three times greater maximum drilling depth are obtained by the proposed method, as compared with conventional femtosecond laser drilling at the same processing parameters. The improvements are due to the changes of photon-electron interactions by shaping femtosecond pulse train, which can effectively adjust the photon absorption and localized transient material properties by changing electron dynamics such as free electron densities.

  4. The role of protein dynamics and thermal fluctuations in regulating cytochrome c/cytochrome c oxidase electron transfer.

    Science.gov (United States)

    Alvarez-Paggi, Damian; Zitare, Ulises; Murgida, Daniel H

    2014-07-01

    In this overview we present recent combined electrochemical, spectroelectrochemical, spectroscopic and computational studies from our group on the electron transfer reactions of cytochrome c and of the primary electron acceptor of cytochrome c oxidase, the CuA site, in biomimetic complexes. Based on these results, we discuss how protein dynamics and thermal fluctuations may impact on protein ET reactions, comment on the possible physiological relevance of these results, and finally propose a regulatory mechanism that may operate in the Cyt/CcO electron transfer reaction in vivo. This article is part of a Special Issue entitled: 18th European Bioenergetic Conference. Copyright © 2014 Elsevier B.V. All rights reserved.

  5. Electron-spin dynamics in Mn-doped GaAs using time-resolved magneto-optical techniques

    Science.gov (United States)

    Akimov, I. A.; Dzhioev, R. I.; Korenev, V. L.; Kusrayev, Yu. G.; Zhukov, E. A.; Yakovlev, D. R.; Bayer, M.

    2009-08-01

    We study the electron-spin dynamics in p -type GaAs doped with magnetic Mn acceptors by means of time-resolved pump-probe and photoluminescence techniques. Measurements in transverse magnetic fields show a long spin-relaxation time of 20 ns that can be uniquely related to electrons. Application of weak longitudinal magnetic fields above 100 mT extends the spin-relaxation times up to microseconds which is explained by suppression of the Bir-Aronov-Pikus spin relaxation for the electron on the Mn acceptor.

  6. Can Excited State Electronic Coherence Be Tuned via Molecular Structural Modification? A First-Principles Quantum Electronic Dynamics Study of Pyrazolate-Bridged Pt(II) Dimers

    Energy Technology Data Exchange (ETDEWEB)

    Lingerfelt, David B.; Lestrange, Patrick J.; Radler, Joseph J.; Brown-Xu, Samantha E.; Kim, Pyosang; Castellano, Felix N.; Chen, Lin X.; Li, Xiaosong

    2017-02-24

    Materials and molecular systems exhibiting long-lived electronic coherence can facilitate coherent transport, opening the door to efficient charge and energy transport beyond traditional methods. Recently, signatures of a possible coherent, recurrent electronic motion were identified in femtosecond pump-probe spectroscopy experiments on a binuclear platinum complex, where a persistent periodic beating in the transient absorption signal’s anisotropy was observed. In this study, we investigate the excitonic dynamics that underlie the suspected electronic coherence for a series of binuclear platinum complexes exhibiting a range of interplatinum distances. Results suggest that the long-lived coherence can only result when competitive electronic couplings are in balance. At longer Pt-Pt distances, the electronic couplings between the two halves of the binuclear system weaken, and exciton localization and recombination is favored on short time scales. For short Pt-Pt distances, electronic couplings between the states in the coherent superposition are stronger than the coupling with other excitonic states, leading to long-lived coherence.

  7. Can Excited State Electronic Coherence Be Tuned via Molecular Structural Modification? A First-Principles Quantum Electronic Dynamics Study of Pyrazolate-Bridged Pt(II) Dimers.

    Science.gov (United States)

    Lingerfelt, David B; Lestrange, Patrick J; Radler, Joseph J; Brown-Xu, Samantha E; Kim, Pyosang; Castellano, Felix N; Chen, Lin X; Li, Xiaosong

    2017-03-09

    Materials and molecular systems exhibiting long-lived electronic coherence can facilitate coherent transport, opening the door to efficient charge and energy transport beyond traditional methods. Recently, signatures of a possible coherent, recurrent electronic motion were identified in femtosecond pump-probe spectroscopy experiments on a binuclear platinum complex, where a persistent periodic beating in the transient absorption signal's anisotropy was observed. In this study, we investigate the excitonic dynamics that underlie the suspected electronic coherence for a series of binuclear platinum complexes exhibiting a range of interplatinum distances. Results suggest that the long-lived coherence can only result when competitive electronic couplings are in balance. At longer Pt-Pt distances, the electronic couplings between the two halves of the binuclear system weaken, and exciton localization and recombination is favored on short time scales. For short Pt-Pt distances, electronic couplings between the states in the coherent superposition are stronger than the coupling with other excitonic states, leading to long-lived coherence.

  8. Dynamic investigation of electron trapping and charge decay in electron-irradiated Al sub 2 O sub 3 in a scanning electron microscope: Methodology and mechanisms

    CERN Document Server

    Fakhfakh, S; Belhaj, M; Fakhfakh, Z; Kallel, A; Rau, E I

    2002-01-01

    The charging and discharging of polycrystalline Al sub 2 O sub 3 submitted to electron-irradiation in a scanning electron microscope (SEM) are investigated by means of the displacement current method. To circumvent experimental shortcomings inherent to the use of the basic sample holder, a redesign of the latter is proposed and tests are carried out to verify its operation. The effects of the primary beam accelerating voltage on charging, flashover and discharging phenomena during and after electron-irradiation are studied. The experimental results are then analyzed. In particular, the divergence between the experimental data and those predicted by the total electron emission yield approach (TEEYA) is discussed. A partial discharge was observed immediately after the end of the electron-irradiation exposure. The experimental data suggests, that the discharge is due to the evacuation to the ground, along the insulator surface, of released electrons from shallow traps at (or in the close vicinity of) the insulat...

  9. Dynamics of a Low-Dimensional Model for Short Pulse Mode Locking

    Directory of Open Access Journals (Sweden)

    Edward D. Farnum

    2015-08-01

    Full Text Available Emerging ultra-fast mode-locked lasers are now capable of generating pulses in the few to sub-femtosecond regime. Using recent theoretical innovations around the short pulse equation, we characterize the mode locking dynamics using a low-dimensional representation of the pulse parameters. The theory is formulated using a variational approach, since linearization of the exact solution is not tractable. The dominant dynamics can be characterized in a geometrical way using phase-plane analysis. Of note is our ability to determine the underlying bifurcations that occur due to changes in the fiber laser cavity parameters, including the onset of the multi-pulsing instability. The theory can aid in design principles for generating robust and highly-stable mode-locked pulses.

  10. Electron and photon reconstruction and performance in ATLAS using a dynamical, topological cell clustering-based approach

    CERN Document Server

    The ATLAS collaboration

    2017-01-01

    The electron and photon reconstruction in ATLAS has moved towards the use of a dynamical, topo- logical cell-based approach for cluster building, owing to advancements in the calibration procedure which allow for such a method to be applied. The move to this new technique allows for improved measurements of electron and photon energies, particularly in situations where an electron radiates a bremsstrahlung photon, or a photon converts to an electron-poistron pair. This note details the changes to the ATLAS electron and photon reconstruction software, and assesses its performance under current LHC luminosity conditions using simulated data. Changes to the converted photon reconstruction are also detailed, which improve the reconstruction efficiency of double-track converted photons, as well as reducing the reconstruction of spurious one-track converted photons. The performance of the new reconstruction algorithm is also presented in a number of important topologies relevant to precision Standard Model physics,...

  11. Dynamics and Control of Switched Electronic Systems Advanced Perspectives for Modeling, Simulation and Control of Power Converters

    CERN Document Server

    Iannelli, Luigi

    2012-01-01

    The increased efficiency and quality constraints imposed on electrical energy systems have inspired a renewed research interest in the study of formal approaches to the analysis and control of power electronics converters. Switched systems represent a useful framework for modeling these converters and the peculiarities of their operating conditions and control goals justify the specific classification of “switched electronic systems”. Indeed, idealized switched models of power converters introduce problems not commonly encountered when analyzing generic switched models or non-switched electrical networks. In that sense the analysis of switched electronic systems represents a source for new ideas and benchmarks for switched and hybrid systems generally. Dynamics and Control of Switched Electronic Systems draws on the expertise of an international group of expert contributors to give an overview of recent advances in the modeling, simulation and control of switched electronic systems. The reader is provided...

  12. Unravelling the structure and dynamics of concentrated aqueous proton defects using simulations incorporating both nuclear and electronic quantum effects

    Science.gov (United States)

    Markland, Thomas

    Aqueous proton defects give rise to a range of structural and dynamical environments that vary with concentration. These manifest as a continuum of infra-red and Raman spectral features. However, assigning spectral features to the underlying structures formed in solution and their dynamical interconversion remains an area of significant debate. In this talk I will show how path integral ab initio molecular dynamics simulations, where the electronic structure is computed on the fly using density functional theory and nuclear quantum effects are included explicitly via path integral molecular dynamics, can be used to accurately describe the spectroscopic properties of liquid water and systems with aqueous proton defects. These simulations, which have previously been computationally intractable for such large condensed phase systems, are now possible due to our recent path integral developments. I will discuss how these simulations can be used to elucidate the linear and multidimensional spectroscopy of concentrated acid systems and the dynamics and structures that give rise to them.

  13. Dynamic response of a two-dimensional electron gas: Exact treatment of Coulomb exchange in the random-phase approximation

    Science.gov (United States)

    Takayanagi, K.; Lipparini, E.

    1995-07-01

    The Dyson equation for the particle-hole Green's function, including Coulomb exchange matrix elements, has been solved exactly for a two-dimensional electron gas. Static and dynamic dielectric functions have been calculated and compared with normal random-phase-approximation and recent quantum Monte Carlo results.

  14. Dynamic shock compaction of a ZrO2-RuO2 electronic nanocomposite: toward functionally graded materials

    NARCIS (Netherlands)

    van Zyl, W.E.; Carton, Erik P.; Raming, T.P.; ten Elshof, Johan E.; Verweij, H.

    2005-01-01

    An electronic ZrO2-RuO2 nanocomposite was fabricated by dynamic compaction (DC) at 1.5 GPa resulting in a maximum relative density of 88% in the material. The DC process formed pristine elongated conical-shaped compacts 3 cm in length. The compacts retained their original nanometer-sized grains (~20

  15. Strong impact of lattice vibrations on electronic and magnetic properties of paramagnetic Fe revealed by disordered local moments molecular dynamics

    NARCIS (Netherlands)

    Alling, B.; Kormann, F.H.W.; Grabowski, B; Glensk, A; Abrikosov, I.A.

    2016-01-01

    We study the impact of lattice vibrations on magnetic and electronic properties of paramagnetic bcc and fcc iron at finite temperature, employing the disordered local moments molecular dynamics (DLM-MD) method. Vibrations strongly affect the distribution of local magnetic moments at finite

  16. A method for geometrical verification of dynamic intensity modulated radiotherapy using a scanning electronic portal imaging device

    NARCIS (Netherlands)

    Ploeger, Lennert S.; Smitsmans, Monique H. P.; Gilhuijs, Kenneth G. A.; van Herk, Marcel

    2002-01-01

    In order to guarantee the safe delivery of dynamic intensity modulated radiotherapy (IMRT), verification of the leaf trajectories during the treatment is necessary. Our aim in this study is to develop a method for on-line verification of leaf trajectories using an electronic portal imaging device

  17. An infrared free-electron laser for the Chemical Dynamics Research Laboratory

    Energy Technology Data Exchange (ETDEWEB)

    Vaughan, D. (comp.)

    1992-04-01

    This document describes a free-electron laser (FEL) proposed as part of the Chemical Dynamics Research Laboratory (CDRL), a user facility that also incorporates several advanced lasers of conventional design and two beamlines for the ALS. The FEL itself addresses the needs of the chemical sciences community for a high-brightness, tunable source covering a broad region of the infrared spectrum -- from 3 to 50 {mu}m. All of these sources, together with a variety of sophisticated experimental stations, will be housed in a new building to be located adjacent to the ALS. The radiation sources can be synchronized to permit powerful two-color, pump-probe experiments that will further our fundamental understanding of chemical dynamics at the molecular level, especially those aspects relevant to practical issues in combustion chemistry. The technical approach adopted in this design makes use of superconducting radiofrequency (SCRF) accelerating structures. The primary motivation for adopting this approach was to meet the user requirement for wavelength stability equal to one part in 10{sup 4}. Previous studies concluded that a wavelength stability of only one part in 10{sup 3} could be achieved with currently available room-temperature technology. In addition, the superconducting design operates in a continuous-wave (cw) mode and hence offers considerably higher average optical output power. It also allows for various pulse-gating configurations that will permit simultaneous multiuser operations. A summary of the comparative performance attainable with room-temperature and superconducting designs is given. The FEL described in this report provides a continuous train of 30-ps micropulses, with 100{mu}J of optical energy per micropulse, at a repetition rate of 6.1 MHz. The device can also deliver pulses at a cw repetition rate of 12.2 MHz, with a peak power of 50 {mu}J per micropulse. 70 ref.

  18. An infrared free-electron laser for the Chemical Dynamics Research Laboratory. Design report

    Energy Technology Data Exchange (ETDEWEB)

    Vaughan, D. [comp.

    1992-04-01

    This document describes a free-electron laser (FEL) proposed as part of the Chemical Dynamics Research Laboratory (CDRL), a user facility that also incorporates several advanced lasers of conventional design and two beamlines for the ALS. The FEL itself addresses the needs of the chemical sciences community for a high-brightness, tunable source covering a broad region of the infrared spectrum -- from 3 to 50 {mu}m. All of these sources, together with a variety of sophisticated experimental stations, will be housed in a new building to be located adjacent to the ALS. The radiation sources can be synchronized to permit powerful two-color, pump-probe experiments that will further our fundamental understanding of chemical dynamics at the molecular level, especially those aspects relevant to practical issues in combustion chemistry. The technical approach adopted in this design makes use of superconducting radiofrequency (SCRF) accelerating structures. The primary motivation for adopting this approach was to meet the user requirement for wavelength stability equal to one part in 10{sup 4}. Previous studies concluded that a wavelength stability of only one part in 10{sup 3} could be achieved with currently available room-temperature technology. In addition, the superconducting design operates in a continuous-wave (cw) mode and hence offers considerably higher average optical output power. It also allows for various pulse-gating configurations that will permit simultaneous multiuser operations. A summary of the comparative performance attainable with room-temperature and superconducting designs is given. The FEL described in this report provides a continuous train of 30-ps micropulses, with 100{mu}J of optical energy per micropulse, at a repetition rate of 6.1 MHz. The device can also deliver pulses at a cw repetition rate of 12.2 MHz, with a peak power of 50 {mu}J per micropulse. 70 ref.

  19. The Primary Care Electronic Library: RSS feeds using SNOMED-CT indexing for dynamic content delivery.

    Science.gov (United States)

    Robinson, Judas; de Lusignan, Simon; Kostkova, Patty; Madge, Bruce; Marsh, A; Biniaris, C

    2006-01-01

    Rich Site Summary (RSS) feeds are a method for disseminating and syndicating the contents of a website using extensible mark-up language (XML). The Primary Care Electronic Library (PCEL) distributes recent additions to the site in the form of an RSS feed. When new resources are added to PCEL, they are manually assigned medical subject headings (MeSH terms), which are then automatically mapped to SNOMED-CT terms using the Unified Medical Language System (UMLS) Metathesaurus. The library is thus searchable using MeSH or SNOMED-CT. Our syndicate partner wished to have remote access to PCEL coronary heart disease (CHD) information resources based on SNOMED-CT search terms. To pilot the supply of relevant information resources in response to clinically coded requests, using RSS syndication for transmission between web servers. Our syndicate partner provided a list of CHD SNOMED-CT terms to its end-users, a list which was coded according to UMLS specifications. When the end-user requested relevant information resources, this request was relayed from our syndicate partner's web server to the PCEL web server. The relevant resources were retrieved from the PCEL MySQL database. This database is accessed using a server side scripting language (PHP), which enables the production of dynamic RSS feeds on the basis of Source Asserted Identifiers (CODEs) contained in UMLS. Retrieving resources using SNOMED-CT terms using syndication can be used to build a functioning application. The process from request to display of syndicated resources took less than one second. The results of the pilot illustrate that it is possible to exchange data between servers using RSS syndication. This method could be utilised dynamically to supply digital library resources to a clinical system with SNOMED-CT data used as the standard of reference.

  20. Comparison of the ultrafast hot electron dynamics of titanium nitride and gold for plasmonic applications

    Science.gov (United States)

    Doiron, Brock; Li, Yi; Mihai, Andrei P.; Cohen, Lesley F.; Petrov, Peter K.; Alford, Neil M.; Oulton, Rupert F.; Maier, Stefan A.

    2017-08-01

    With similar optical properties to gold and high thermal stability, titanium nitride continues to prove itself as a promising plasmonic material for high-temperature applications in the visible and near-infrared. In this work, we use transient pump probe differential reflection measurements to compare the electron energy decay channels in titanium nitride and gold thin films. Using an extended two temperature model to incorporate the photoexcited electrons, it is possible to separate the electron-electron and electron-phonon scattering contributions immediately following the arrival of the pump pulse. This model allows for incredibly accurate determination of the internal electronic properties using only optical measurements. As the electronic properties are key in hot electron applications, we show that titanium nitide has substantially longer electron thermalization and electron-phonon scattering times. With this, we were also able to resolve electron thermal conduction in the film using purely optical measurements.

  1. Molecular Dynamics Simulation of Strong Shock Waves Propagating in Dense Deuterium With the Effect of Excited Electrons

    CERN Document Server

    Liu, Hao; Kang, Wei; Zhang, Ping; Duan, Huiling; He, X T

    2016-01-01

    We present a molecular dynamics simulation of shock waves propagating in dense deuterium with the electron force field method [J. T. Su and W. A. Goddard, Phys. Rev. Lett. 99, 185003 (2007)], which explicitly takes the excitation of electrons into consideration. Non-equilibrium features associated with the excitation of electrons are systematically investigated. We show that chemical bonds in D$_2$ molecules lead to a more complicated shock wave structure near the shock front, compared with the results of classical molecular dynamics simulation. Charge separation can bring about accumulation of net charges on the large scale, instead of the formation of a localized dipole layer, which might cause extra energy for the shock wave to propagate. In addition, the simulations also display that molecular dissociation at the shock front is the major factor corresponding to the "bump" structure in the principal Hugoniot. These results could help to build a more realistic picture of shock wave propagation in fuel mater...

  2. Non-perturbation theory of electronic dynamic conductivity for two-barrier resonance tunnel nano-structure

    Directory of Open Access Journals (Sweden)

    O.M. Voitsekhivska

    2011-12-01

    Full Text Available The non-perturbation theory of electronic dynamic conductivity for open two-barrier resonance tunnel structure is established for the first time within the model of rectangular potentials and different effective masses of electrons in the elements of nano-structure and the wave function linear over the intensity of electromagnetic field. It is proven that the results of the theory of dynamic conductivity, developed earlier in weak signal approximation within the perturbation method, qualitatively and quantitatively correlate with the obtained results. The advantage of non-perturbation theory is that it can be extended to the case of electronic currents interacting with strong electromagnetic fields in open multi-shell resonance tunnel nano-structures, as active elements of quantum cascade lasers and detectors.

  3. Beyond the electronic textbook model: software techniques to make on-line educational content dynamic.

    Science.gov (United States)

    Frank, M S; Dreyer, K

    2001-06-01

    We describe a working software technology that enables educators to incorporate their expertise and teaching style into highly interactive and Socratic educational material for distribution on the world wide web. A graphically oriented interactive authoring system was developed to enable the computer novice to create and store within a database his or her domain expertise in the form of electronic knowledge. The authoring system supports and facilitates the input and integration of several types of content, including free-form, stylized text, miniature and full-sized images, audio, and interactive questions with immediate feedback. The system enables the choreography and sequencing of these entities for display within a web page as well as the sequencing of entire web pages within a case-based or thematic presentation. Images or segments of text can be hyperlinked with point-and-click to other entities such as adjunctive web pages, audio, or other images, cases, or electronic chapters. Miniature (thumbnail) images are automatically linked to their full-sized counterparts. The authoring system contains a graphically oriented word processor, an image editor, and capabilities to automatically invoke and use external image-editing software such as Photoshop. The system works in both local area network (LAN) and internet-centric environments. An internal metalanguage (invisible to the author but stored with the content) was invented to represent the choreographic directives that specify the interactive delivery of the content on the world wide web. A database schema was developed to objectify and store both this electronic knowledge and its associated choreographic metalanguage. A database engine was combined with page-rendering algorithms in order to retrieve content from the database and deliver it on the web in a Socratic style, assess the recipient's current fund of knowledge, and provide immediate feedback, thus stimulating in-person interaction with a human expert

  4. Multidimensional treatment of stochastic solvent dynamics in photoinduced proton-coupled electron transfer processes: sequential, concerted, and complex branching mechanisms.

    Science.gov (United States)

    Soudackov, Alexander V; Hazra, Anirban; Hammes-Schiffer, Sharon

    2011-10-14

    A theoretical approach for the multidimensional treatment of photoinduced proton-coupled electron transfer (PCET) processes in solution is presented. This methodology is based on the multistate continuum theory with an arbitrary number of diabatic electronic states representing the relevant charge distributions in a general PCET system. The active electrons and transferring proton(s) are treated quantum mechanically, and the electron-proton vibronic free energy surfaces are represented as functions of multiple scalar solvent coordinates corresponding to the single electron and proton transfer reactions involved in the PCET process. A dynamical formulation of the dielectric continuum theory is used to derive a set of coupled generalized Langevin equations of motion describing the time evolution of these collective solvent coordinates. The parameters in the Langevin equations depend on the solvent properties, such as the dielectric constants, relaxation time, and molecular moment of inertia, as well as the solute properties. The dynamics of selected intramolecular nuclear coordinates, such as the proton donor-acceptor distance or a torsional angle within the PCET complex, may also be included in this formulation. A surface hopping method in conjunction with the Langevin equations of motion is used to simulate the nonadiabatic dynamics on the multidimensional electron-proton vibronic free energy surfaces following photoexcitation. This theoretical treatment enables the description of both sequential and concerted mechanisms, as well as more complex processes involving a combination of these mechanisms. The application of this methodology to a series of model systems corresponding to collinear and orthogonal PCET illustrates fundamental aspects of these different mechanisms and elucidates the significance of proton vibrational relaxation and nonequilibrium solvent dynamics. © 2011 American Institute of Physics

  5. Antwerp Advanced Study Institute on Electronic Structure, Dynamics and Quantum Structural Properties of Condensed Matter

    CERN Document Server

    Camp, Piet

    1985-01-01

    The 1984 Advanced Study Institute on "Electronic Structure, Dynamics and Quantum Structural Properties of Condensed Matter" took place at the Corsendonk Conference Center, close to the City of Antwerpen, from July 16 till 27, 1984. This NATO Advanced Study Institute was motivated by the research in my Institute, where, in 1971, a project was started on "ab-initio" phonon calculations in Silicon. I~ is my pleasure to thank several instances and people who made this ASI possible. First of all, the sponsor of the Institute, the NATO Scientific Committee. Next, the co-sponsors: Agfa-Gevaert, Bell Telephone Mfg. Co. N.V., C & A, Esso Belgium·, CDC Belgium, Janssens Pharmaceutica, Kredietbank and the Scientific Office of the U.S. Army. Special thanks are due to Dr. P. Van Camp and Drs. H. Nachtegaele, who, over several months, prepared the practical aspects of the ASI with the secretarial help of Mrs. R.-M. Vandekerkhof. I also like to. thank Mrs. M. Cuyvers who prepared and organized the subject and material ...

  6. Hildebrand and Hansen solubility parameters from molecular dynamics with applications to electronic nose polymer sensors.

    Science.gov (United States)

    Belmares, M; Blanco, M; Goddard, W A; Ross, R B; Caldwell, G; Chou, S-H; Pham, J; Olofson, P M; Thomas, Cristina

    2004-11-30

    We introduce the Cohesive Energy Density (CED) method, a multiple sampling Molecular Dynamics computer simulation procedure that may offer higher consistency in the estimation of Hildebrand and Hansen solubility parameters. The use of a multiple sampling technique, combined with a simple but consistent molecular force field and quantum mechanically determined atomic charges, allows for the precise determination of solubility parameters in a systematic way (sigma = 0.4 hildebrands). The CED method yields first-principles Hildebrand parameter predictions in good agreement with experiment [root-mean-square (rms) = 1.1 hildebrands]. We apply the CED method to model the Caltech electronic nose, an array of 20 polymer sensors. Sensors are built with conducting leads connected through thin-film polymers loaded with carbon black. Odorant detection relies on a change in electric resistivity of the polymer film as function of the amount of swelling caused by the odorant compound. The amount of swelling depends upon the chemical composition of the polymer and the odorant molecule. The pattern is unique, and unambiguously identifies the compound. Experimentally determined changes in relative resistivity of seven polymer sensors upon exposure to 24 solvent vapors were modeled with the CED estimated Hansen solubility components. Predictions of polymer sensor responses result in Pearson R2 coefficients between 0.82 and 0.99. Copyright 2004 Wiley Periodicals, Inc.

  7. Three-body dynamical interference in electron and positron collision with positronium atom

    Directory of Open Access Journals (Sweden)

    E Ghanbari Adivi

    2010-12-01

    Full Text Available In this project, the Faddeev-Watson-Lovelace (FWL formalism is generalized to large scattering angles. The angular range includes 0-180 degrees. Using this method, the charge transfer differential cross-sections are calculated, in a second-order approximation, for collision of energetic positrons and electrons with neutral positronium atoms. In this approximation, the rearrangement amplitude contains two first-order and three second-order partial amplitudes. The first first-order term is the Born amplitude in a first-order approximation. The second one corresponds to capturing the transferred particle without perturbing the state of this particle. This term, in fact, describes a knock-on process. Since the masses of the particles and the absolute values of their charges are equal, one expects that the second-order terms be similar in magnitude. This aspect causes the instructive interference of the partial amplitudes in some angles and destructive interference in some others. However, it is predicted that these amplitudes have local maxima in direction of the recoiling of the projectile. In order to investigate this situation, the second-order partial amplitudes are calculated and their relations with the parity of the initial and final states of the scattering system are analyzed. In particular, the role of dynamical interference of these partial amplitudes in creation of the kinematical peak and the peak corresponding to the knock-on scattering in angular distribution of the differential cross sections is investigated.

  8. Direct observation of photocarrier electron dynamics in C60 films on graphite by time-resolved two-photon photoemission

    Science.gov (United States)

    Shibuta, Masahiro; Yamamoto, Kazuo; Ohta, Tsutomu; Nakaya, Masato; Eguchi, Toyoaki; Nakajima, Atsushi

    2016-01-01

    Time-resolved two-photon photoemission (TR-2PPE) spectroscopy is employed to probe the electronic states of a C60 fullerene film formed on highly oriented pyrolytic graphite (HOPG), acting as a model two-dimensional (2D) material for multi-layered graphene. Owing to the in-plane sp2-hybridized nature of the HOPG, the TR-2PPE spectra reveal the energetics and dynamics of photocarriers in the C60 film: after hot excitons are nascently formed in C60 via intramolecular excitation by a pump photon, they dissociate into photocarriers of free electrons and the corresponding holes, and the electrons are subsequently detected by a probe photon as photoelectrons. The decay rate of photocarriers from the C60 film into the HOPG is evaluated to be 1.31 × 1012 s−1, suggesting a weak van der Waals interaction at the interface, where the photocarriers tentatively occupy the lowest unoccupied molecular orbital (LUMO) of C60. The photocarrier electron dynamics following the hot exciton dissociation in the organic thin films has not been realized for any metallic substrates exhibiting strong interactions with the overlayer. Furthermore, the thickness dependence of the electron lifetime in the LUMO reveals that the electron hopping rate in C60 layers is 3.3 ± 1.2 × 1013 s−1. PMID:27775005

  9. Dynamics of coupled electron-nuclei-systems in laser fields; Dynamik gekoppelter Elektronen-Kern-Systeme in Laserfeldern

    Energy Technology Data Exchange (ETDEWEB)

    Falge, Mirjam

    2012-07-01

    This work aimed at the theoretical analysis of high harmonic generation in molecules and the influence of coupled electron and nuclear dynamics on ultra-short pulse ionization processes. In the first part of this thesis, the isotope effect and influence of vibrational excitation on high harmonic generation were investigated for the isotope pairs H{sub 2}O/D{sub 2}O and H{sub 2}/D{sub 2}. It was shown that on the one hand high harmonic intensities strongly depend on the vibrational quantum number of the initial state of the water molecule and on the other hand the spectra of H{sub 2}O and D{sub 2}O exhibit a clear isotope effect for certain vibrationally excited states. Also it was shown that high harmonics of vibrationally excited states show an even more pronounced isotope effect than the ground state. The second and third part of this work treats the influence of coupled electron and nuclear dynamics on photoelectron spectra. In order to facilitate a numerically exact description of this dynamics, a simple one-dimensional model system (Shin-Metiu model) was used. It consists of only a single electronic and nuclear degree-of-freedom and allows for a switching between adiabatic and strongly non-adiabatic dynamics by its parameterization. This model served for the analysis of the dynamics of three different cases ranging from weak over intermediate to strong electron-nuclear coupling. To investigate the influence of non-adiabatic effects on photoelectron spectra, time-resolved photoelectron spectra were calculated applying two methods: a numerically exact treatment and an adiabatic approach neglecting the electron-nuclear coupling. Subsequently, the dependence of the efficiency of a non-adiabatic transition on the nuclear mass was analysed. To this end, the population dynamics and photoelectron spectra were calculated numerically exactly for a strong electron and nuclear coupling. Thereafter the asymmetry in forward and backward direction of time

  10. Electron Lenses for Experiments on Nonlinear Dynamics with Wide Stable Tune Spreads in the Fermilab Integrable Optics Test Accelerator

    Energy Technology Data Exchange (ETDEWEB)

    Stancari, G. [Fermilab; Carlson, K. [Fermilab; McGee, M. W. [Fermilab; Nobrega, L. E. [Fermilab; Romanov, A. L. [Fermilab; Ruan, J. [Fermilab; Valishev, A. [Fermilab; Noll, D. [Frankfurt U.

    2015-06-01

    Recent developments in the study of integrable Hamiltonian systems have led to nonlinear accelerator lattice designs with two transverse invariants. These lattices may drastically improve the performance of high-power machines, providing wide tune spreads and Landau damping to protect the beam from instabilities, while preserving dynamic aperture. To test the feasibility of these concepts, the Integrable Optics Test Accelerator (IOTA) is being designed and built at Fermilab. One way to obtain a nonlinear integrable lattice is by using the fields generated by a magnetically confined electron beam (electron lens) overlapping with the circulating beam. The parameters of the required device are similar to the ones of existing electron lenses. We present theory, numerical simulations, and first design studies of electron lenses for nonlinear integrable optics.

  11. Visualizing the non-equilibrium dynamics of photoinduced intramolecular electron transfer with femtosecond X-ray pulses

    DEFF Research Database (Denmark)

    Canton, Sophie E.; Kjær, Kasper S.; Vankó, György

    2015-01-01

    spectroscopy with ultrafast X-ray emission spectroscopy and diffuse X-ray scattering at the SACLA facility to track the non-equilibrated electronic and structural dynamics within a bimetallic donor–acceptor complex that contains an optically dark centre. Exploiting the 100-fold increase in temporal resolution...... as compared with storage ring facilities, these measurements constitute the first X-ray-based visualization of a non-equilibrated intramolecular electron transfer process over large interatomic distances. Experimental and theoretical results establish that mediation through electronically excited molecular...... states is a key mechanistic feature. The present study demonstrates the extensive potential of femtosecond X-ray techniques as diagnostics of non-adiabatic electron transfer processes in synthetic and biological systems, and some directions for future studies, are outlined....

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

    Science.gov (United States)

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

    2015-08-07

    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.

  13. Dynamic evaluation of swallowing disorders with electron-beam tomography; Funktionelle Schluckaktuntersuchungen mit der Elektronenstrahlcomputertomographie

    Energy Technology Data Exchange (ETDEWEB)

    Raith, J. [Universitaetsklinik fuer Radiologie, Graz (Austria); Lindbichler, F. [Universitaetsklinik fuer Radiologie, Graz (Austria); Kern, R. [Universitaetsklinik fuer Radiologie, Graz (Austria); Groell, R. [Universitaetsklinik fuer Radiologie, Graz (Austria); Rienmueller, R. [Universitaetsklinik fuer Radiologie, Graz (Austria)

    1996-03-01

    Three cases preselected by videofluorography were studied to evaluate whether electron beam tomography (EBT) permits more detailed dynamic imaging of swallowing disorders focusing on the mesonasopharyngeal segment, the hypopharynx and the upper esophageal sphincter (UES). Immediately after videofluorographic examination of the oropharyngeal deglutition, EBT is performed. The patient is in a supine position and while the patient swallows a 20 ml bolus of water or diluted iodine containing contrast agent, a sequence of 20 images per level is scanned. The levels, which are determined by using the scout view, are oriented parallel to the hard palate either at the level of the hard palate to image the mesonasopharyngel segment or just above the hyoid bone to focus on the hypopharynx or at the location of the USE. The scan technique is a single-slice cinemode with a slice thickness of 3 mm (exposure time 100 ms, interscan delay 16 ms, 130 kV, 620 mA). The following structural interactions that we have so far been unable to image can be clearly demonstrated with EBT: During normal swallowing, the mesonasopharyngeal segment is completely and symmetrically closed by the soft palate and Passavant`s cushion; lateral hypopharyngeal pouches can be located more precisely; and disorders of the UES can be differentiated into functional or morphologically caused disorders (e.g., goiter or cervical osteophytes). Videofluorography and cinematography are still the gold standard in functional evaluation of swallowing disorders. However, EBT permits dynamic imaging of pharyngeal deglutition in a preselected transverse plane and can give useful additional information concerning functional anatomical changes in the pharynx during swallowing. Further clinical evaluation is needed. (orig.) [Deutsch] Videofluorographie und Kinematographie gelten derzeit als Goldstandard fuer die Abklaerung von Schluckstoerungen. Methodisch bedingt ist jedoch keine ueberlagerungsfreie Darstellung der

  14. Dynamical electron-phonon coupling, G W self-consistency, and vertex effect on the electronic band gap of ice and liquid water

    Science.gov (United States)

    Ziaei, Vafa; Bredow, Thomas

    2017-06-01

    We study the impact of dynamical electron-phonon (el-ph) effects on the electronic band gap of ice and liquid water by accounting for frequency-dependent Fan contributions in the el-ph mediated self-energy within the many-body perturbation theory (MBPT). We find that the dynamical el-ph coupling effects greatly reduce the static el-ph band-gap correction of the hydrogen-rich molecular ice crystal from-2.46 to -0.23 eV in great contrast to the result of Monserrat et al. [Phys. Rev. B 92, 140302 (2015), 10.1103/PhysRevB.92.140302]. This is of particular importance as otherwise the static el-ph gap correction would considerably reduce the electronic band gap, leading to considerable underestimation of the intense peaks of optical absorption spectra of ice which would be in great disagreement to experimental references. By contrast, the static el-ph gap correction of liquid water is very moderate (-0.32 eV), and inclusion of dynamical effects slightly reduces the gap correction to -0.19 eV. Further, we determine the diverse sensitivity of ice and liquid water to the G W self-consistency and show that the energy-only self-consistent approach (GnWn ) exhibits large implicit vertex character in comparison to the quasiparticle self-consistent approach, for which an explicit calculation of vertex corrections is necessary for good agreement with experiment.

  15. Three-body recombination and dynamics of electrons and excited states in the low-pressure argon afterglow

    Science.gov (United States)

    Tsankov, Tsanko Vaskov; Johnsen, Rainer; Czarnetzki, Uwe

    2016-09-01

    The afterglow phase occurs naturally during the power-off period in pulsed low-pressure plasmas and in atmospheric pressure ns discharges. During that period the electron energy rapidly declines and the charged particles are lost due to diffusion and recombination. In low-pressure discharges the dominant process is three-body recombination (TBR) of Ar+ ions with electrons. It leads to complex dynamics of the excited states, dominated by collisional-radiative cascades that eventually repopulate the metastable states. In this contribution the afterglow dynamics of an argon discharge is analyzed in detail to elucidate the roles played by the various processes. An analytical model for the fast drop of the electron energy by evaporative cooling and electron-ion collisions is combined with a time-dependent collisional radiative model for the atomic excited states that numerically solves the electron energy and density balance equations. By including further gas heating and cooling, the model leads to excellent agreement with experiments utilizing different diagnostic techniques, and hence gives insight into the interplay of the various processes in the afterglow. Work Supported by the DFG (Grant No. TS 307/1-1).

  16. Protection of DNA against low-energy electrons by amino acids: a first-principles molecular dynamics study.

    Science.gov (United States)

    Gu, Bin; Smyth, Maeve; Kohanoff, Jorge

    2014-11-28

    Using first-principles molecular dynamics simulations, we have investigated the notion that amino acids can play a protective role when DNA is exposed to excess electrons produced by ionizing radiation. In this study we focus on the interaction of glycine with the DNA nucleobase thymine. We studied thymine-glycine dimers and a condensed phase model consisting of one thymine molecule solvated in amorphous glycine. Our results show that the amino acid acts as a protective agent for the nucleobase in two ways. If the excess electron is initially captured by the thymine, then a proton is transferred in a barrier-less way from a neighboring hydrogen-bonded glycine. This stabilizes the excess electron by reducing the net partial charge on the thymine. In the second mechanism the excess electron is captured by a glycine, which acts as a electron scavenger that prevents electron localization in DNA. Both these mechanisms introduce obstacles to further reactions of the excess electron within a DNA strand, e.g. by raising the free energy barrier associated with strand breaks.

  17. Molecular dynamics simulations give insight into the conformational change, complex formation, and electron transfer pathway for cytochrome P450 reductase

    Science.gov (United States)

    Sündermann, Axel; Oostenbrink, Chris

    2013-01-01

    Cytochrome P450 reductase (CYPOR) undergoes a large conformational change to allow for an electron transfer to a redox partner to take place. After an internal electron transfer over its cofactors, it opens up to facilitate the interaction and electron transfer with a cytochrome P450. The open conformation appears difficult to crystallize. Therefore, a model of a human CYPOR in the open conformation was constructed to be able to investigate the stability and conformational change of this protein by means of molecular dynamics simulations. Since the role of the protein is to provide electrons to a redox partner, the interactions with cytochrome P450 2D6 (2D6) were investigated and a possible complex structure is suggested. Additionally, electron pathway calculations with a newly written program were performed to investigate which amino acids relay the electrons from the FMN cofactor of CYPOR to the HEME of 2D6. Several possible interacting amino acids in the complex, as well as a possible electron transfer pathway were identified and open the way for further investigation by site directed mutagenesis studies. PMID:23832577

  18. Dynamics of dust grains in an electron-dust plasma induced by solar radiation under microgravity conditions

    Energy Technology Data Exchange (ETDEWEB)

    Fortov, V E [Institute for High Energy Densities, Russian Academy of Sciences, Izhorskaya 13/19, 127412, Moscow (Russian Federation); Nefedov, A P [Institute for High Energy Densities, Russian Academy of Sciences, Izhorskaya 13/19, 127412, Moscow (Russian Federation); Vaulina, O S [Institute for High Energy Densities, Russian Academy of Sciences, Izhorskaya 13/19, 127412, Moscow (Russian Federation); Petrov, O F [Institute for High Energy Densities, Russian Academy of Sciences, Izhorskaya 13/19, 127412, Moscow (Russian Federation); Dranzhevski, I E [Institute for High Energy Densities, Russian Academy of Sciences, Izhorskaya 13/19, 127412, Moscow (Russian Federation); Lipaev, A M [Institute for High Energy Densities, Russian Academy of Sciences, Izhorskaya 13/19, 127412, Moscow (Russian Federation); Semenov, Yu P [Russian Space Corporation ' Energiya' , Korolev, Moscow oblast, 141070 (Russian Federation)

    2003-07-01

    In this paper the results of experimental investigation of the dynamic behaviour of macroparticles charged via photoemission are presented. The experimental data have been obtained for bronze particles subjected to solar radiation under conditions of microgravity (on board the Mir space station). The distribution of velocity, temperatures and charge, as well as the friction coefficient and diffusion constants, have been found. The analysis of the results obtained has shown that the polarization effects of opposite charges may appreciably influence the transport processes in a two-component electron-dust plasma, consisting of positively charged dust and emitted electrons.

  19. Size-dependent ultrafast ionization dynamics of nanoscale samples in intense femtosecond x-ray free-electron-laser pulses.

    Science.gov (United States)

    Schorb, Sebastian; Rupp, Daniela; Swiggers, Michelle L; Coffee, Ryan N; Messerschmidt, Marc; Williams, Garth; Bozek, John D; Wada, Shin-Ichi; Kornilov, Oleg; Möller, Thomas; Bostedt, Christoph

    2012-06-08

    All matter exposed to intense femtosecond x-ray pulses from the Linac Coherent Light Source free-electron laser is strongly ionized on time scales competing with the inner-shell vacancy lifetimes. We show that for nanoscale objects the environment, i.e., nanoparticle size, is an important parameter for the time-dependent ionization dynamics. The Auger lifetimes of large Ar clusters are found to be increased compared to small clusters and isolated atoms, due to delocalization of the valence electrons in the x-ray-induced nanoplasma. As a consequence, large nanometer-sized samples absorb intense femtosecond x-ray pulses less efficiently than small ones.

  20. Micellar aggregates of saponins from Chenopodium quinoa: characterization by dynamic light scattering and transmission electron microscopy.

    Science.gov (United States)

    Verza, S G; de Resende, P E; Kaiser, S; Quirici, L; Teixeira, H F; Gosmann, G; Ferreira, F; Ortega, G G

    2012-04-01

    Entire seeds of Chenopodium quinoa Willd are a rich protein source and are also well-known for their high saponin content. Due to their amphiphily quinoa saponins are able to form intricate micellar aggregates in aqueous media. In this paper we study the aggregates formed by self-association of these compounds from two quinoa saponin fractions (FQ70 and FQ90) as well as several distinctive nanostructures obtained after their complexation with different ratios of cholesterol (CHOL) and phosphatidylcholine (PC). The FQ70 and FQ90 fractions were obtained by reversed-phase preparative chromatography. The structural features of their resulting aggregates were determined by Dynamic Light Scattering (DLS) and Transmission Electron Microscopy (TEM). Novel nanosized spherical vesicles formed by self-association with mean diameter about 100-200 nm were observed in FQ70 aqueous solutions whereas worm-like micelles an approximate width of 20 nm were detected in FQ90 aqueous solutions. Under experimental conditions similar to those reported for the preparation of Quillaja saponaria ISCOM matrices, tubular and ring-like micelles arose from FQ70:CHOL:PC and FQ90:CHOL:PC formulations, respectively. However, under these conditions no cage-like ISCOM matrices were observed. The saponin composition of FQ70 and FQ90 seems to determine the nanosized structures viewed by TEM. Phytolaccagenic acid, predominant in FQ70 and FQ90 fractions, is accountable for the formation of the nanosized vesicles and tubular structures observed by TEM in the aqueous solutions of both samples. Conversely, ring-like micelles observed in FQ90:CHOL:PC complexes can be attributed to the presence of less polar saponins present in FQ90, in particular those derived from oleanolic acid.

  1. X-rays in the Cryo-Electron Microscopy Era: Structural Biology's Dynamic Future.

    Science.gov (United States)

    Shoemaker, Susannah C; Ando, Nozomi

    2018-01-23

    Over the past several years, single-particle cryo-electron microscopy (cryo-EM) has emerged as a leading method for elucidating macromolecular structures at near-atomic resolution, rivaling even the established technique of X-ray crystallography. Cryo-EM is now able to probe proteins as small as hemoglobin (64 kDa) while avoiding the crystallization bottleneck entirely. The remarkable success of cryo-EM has called into question the continuing relevance of X-ray methods, particularly crystallography. To say that the future of structural biology is either cryo-EM or crystallography, however, would be misguided. Crystallography remains better suited to yield precise atomic coordinates of macromolecules under a few hundred kilodaltons in size, while the ability to probe larger, potentially more disordered assemblies is a distinct advantage of cryo-EM. Likewise, crystallography is better equipped to provide high-resolution dynamic information as a function of time, temperature, pressure, and other perturbations, whereas cryo-EM offers increasing insight into conformational and energy landscapes, particularly as algorithms to deconvolute conformational heterogeneity become more advanced. Ultimately, the future of both techniques depends on how their individual strengths are utilized to tackle questions at the frontiers of structural biology. Structure determination is just one piece of a much larger puzzle: a central challenge of modern structural biology is to relate structural information to biological function. In this perspective, we share insight from several leaders in the field and examine the unique and complementary ways in which X-ray methods and cryo-EM can shape the future of structural biology.

  2. Triplet state spectra and dynamics of peridinin analogs having different extents of pi-electron conjugation.

    Science.gov (United States)

    Kaligotla, Shanti; Doyle, Sara; Niedzwiedzki, Dariusz M; Hasegawa, Shinji; Kajikawa, Takayuki; Katsumura, Shigeo; Frank, Harry A

    2010-03-01

    The Peridinin-Chlorophyll a-Protein (PCP) complex has both an exceptionally efficient light-harvesting ability and a highly effective protective capacity against photodynamic reactions involving singlet oxygen. These functions can be attributed to presence of a substantial amount of the highly-substituted and complex carotenoid, peridinin, in the protein and the facts that the low-lying singlet states of peridinin are higher in energy than those of chlorophyll (Chl) a, but the lowest-lying triplet state of peridinin is below that of Chl a. Thus, singlet energy can be transferred from peridinin to Chl a, but the Chl a triplet state is quenched before it can sensitize the formation of singlet oxygen. The present investigation takes advantage of Chl a as an effective triplet state donor to peridinin and explores the triplet state spectra and dynamics of a systematic series of peridinin analogs having different numbers of conjugated carbon-carbon double bonds. The carotenoids investigated are peridinin, which has a C(37) carbon skeleton and eight conjugated carbon-carbon double bonds, and three synthetic analogs: C(33)-peridinin, having two less double bonds than peridinin, C(35)-peridinin which has one less double bond than peridinin, and C(39)-peridinin which has one more double bond than peridinin. In this study, the behavior of the triplet state spectra and kinetics exhibited by these molecules has been investigated in polar and nonpolar solvents and reveals a substantial effect of both pi-electron conjugated chain length and solvent environment on the spectral lineshapes. However, only a small dependence of these factors is observed on the kinetics of triplet energy transfer from Chl a and on carotenoid triplet state deactivation to the ground state.

  3. Field calculations, single-particle tracking, and beam dynamics with space charge in the electron lens for the Fermilab Integrable Optics Test Accelerator

    Energy Technology Data Exchange (ETDEWEB)

    Noll, Daniel [Goethe Univ., Frankfurt (Germany); Stancari, Giulio [Fermi National Accelerator Lab. (FNAL), Batavia, IL (United States)

    2015-11-17

    An electron lens is planned for the Fermilab Integrable Optics Test Accelerator as a nonlinear element for integrable dynamics, as an electron cooler, and as an electron trap to study space-charge compensation in rings. We present the main design principles and constraints for nonlinear integrable optics. A magnetic configuration of the solenoids and of the toroidal section is laid out. Singleparticle tracking is used to optimize the electron path. Electron beam dynamics at high intensity is calculated with a particle-in-cell code to estimate current limits, profile distortions, and the effects on the circulating beam. In the conclusions, we summarize the main findings and list directions for further work.

  4. Development of a simulation method for dynamics of electrons ejected from DNA molecules irradiated with X-rays.

    Science.gov (United States)

    Kai, Takeshi; Higuchi, Mariko; Fujii, Kentaro; Watanabe, Ritsuko; Yokoya, Akinari

    2012-12-01

    To develop a method for simulating the dynamics of the photoelectrons and Auger electrons ejected from DNA molecules irradiated with pulsed monochromatic X-rays. A 30-base-pair (bp) DNA molecule was used as the target model, and the X-rays were assumed to have a Gaussian-shaped time distribution. Photoionization and Auger decay were considered as the atomic processes. The atoms from which the photoelectrons or Auger electrons were emitted were specified in the DNA molecule (or DNA ion) using the Monte Carlo method, and the trajectory of each electron in the electric field formed around the positively charged DNA molecule was calculated with a Newtonian equation. The kinetics of the electrons produced by irradiation with X-rays at an intensity ranging from 1 × 10(12) to 1 × 10(16) photons/mm(2) and energies of 380 eV (below the carbon K-edge), 435 eV (above the nitrogen K-edge), and 560 eV (above the oxygen K-edge) were evaluated. It was found that at an X-ray intensity of 1 × 10(14) photons/mm(2) or less, all the produced electrons escaped from the target. However, above an X-ray intensity of 1 × 10(15) photons/mm(2) and an energy of 560 eV, some photoelectrons that were ejected from the oxygen atoms were trapped near the target DNA. A simulation method for studying the trajectories of electrons ejected from a 30-bp DNA molecule irradiated with pulsed monochromatic X-rays has been developed. The present results show that electron dynamics are strongly dependent on the charged density induced in DNA by pulsed X-ray irradiation.

  5. How good is the generalized Langevin equation to describe the dynamics of photo-induced electron transfer in fluid solution?

    Science.gov (United States)

    Angulo, Gonzalo; Jedrak, Jakub; Ochab-Marcinek, Anna; Pasitsuparoad, Pakorn; Radzewicz, Czesław; Wnuk, Paweł; Rosspeintner, Arnulf

    2017-06-01

    The dynamics of unimolecular photo-triggered reactions can be strongly affected by the surrounding medium for which a large number of theoretical descriptions have been used in the past. An accurate description of these reactions requires knowing the potential energy surface and the friction felt by the reactants. Most of these theories start from the Langevin equation to derive the dynamics, but there are few examples comparing it with experiments. Here we explore the applicability of a Generalized Langevin Equation (GLE) with an arbitrary potential and a non-Markovian friction. To this end, we have performed broadband fluorescence measurements with sub-picosecond time resolution of a covalently linked organic electron donor-acceptor system in solvents of changing viscosity and dielectric permittivity. In order to establish the free energy surface (FES) of the reaction, we resort to stationary electronic spectroscopy. On the other hand, the dynamics of a non-reacting substance, Coumarin 153, provide the calibrating tool for the non-Markovian friction over the FES, which is assumed to be solute independent. A simpler and computationally faster approach uses the Generalized Smoluchowski Equation (GSE), which can be derived from the GLE for pure harmonic potentials. Both approaches reproduce the measurements in most of the solvents reasonably well. At long times, some differences arise from the errors inherited from the analysis of the stationary solvatochromism and at short times from the excess excitation energy. However, whenever the dynamics become slow, the GSE shows larger deviations than the GLE, the results of which always agree qualitatively with the measured dynamics, regardless of the solvent viscosity or dielectric properties. The method applied here can be used to predict the dynamics of any other reacting system, given the FES parameters and solvent dynamics are provided. Thus no fitting parameters enter the GLE simulations, within the applicability

  6. Single-shot mega-electronvolt ultrafast electron diffraction for structure dynamic studies of warm dense matter

    Energy Technology Data Exchange (ETDEWEB)

    Mo, M. Z., E-mail: mmo09@slac.stanford.edu; Shen, X.; Chen, Z.; Li, R. K.; Dunning, M.; Zheng, Q.; Weathersby, S. P.; Reid, A. H.; Coffee, R.; Makasyuk, I.; Edstrom, S.; McCormick, D.; Jobe, K.; Hast, C.; Glenzer, S. H.; Wang, X. [SLAC National Accelerator Laboratory, 2575 Sand Hill Road, Menlo Park, California 94025 (United States); Sokolowski-Tinten, K. [Faculty of Physics and Centre for Nanointegration Duisburg-Essen, University of Duisburg-Essen, Lotharstrasse 1, D-47048 Duisburg (Germany)

    2016-11-15

    We have developed a single-shot mega-electronvolt ultrafast-electron-diffraction system to measure the structural dynamics of warm dense matter. The electron probe in this system is featured by a kinetic energy of 3.2 MeV and a total charge of 20 fC, with the FWHM pulse duration and spot size at sample of 350 fs and 120 μm respectively. We demonstrate its unique capability by visualizing the atomic structural changes of warm dense gold formed from a laser-excited 35-nm freestanding single-crystal gold foil. The temporal evolution of the Bragg peak intensity and of the liquid signal during solid-liquid phase transition are quantitatively determined. This experimental capability opens up an exciting opportunity to unravel the atomic dynamics of structural phase transitions in warm dense matter regime.

  7. Conserving approximations for strongly correlated electron systems - Bethe-Salpeter equation and dynamics for the two-dimensional Hubbard model

    Science.gov (United States)

    Bickers, N. E.; Scalapino, D. J.; White, S. R.

    1989-01-01

    A semianalytical approach is described for strongly correlated electronic systems which satisfies microscopic conservation laws, treats strong frequency and momentum dependences, and provides information on both static and dynamic properties. This approach may be used to treat large systems and temperatures lower than those currently accessible to finite-temperature quantum Monte Carlo techniques. Examples of such systems include heavy-electron compounds, organic Bechegaard salts, bis-(ethylenedithiolo)-TTF superconductors, and the oxide superconductors. The technique is based on the derivation and self-consistent solution of infinite-order conserving approximations. The technique is used to derive a low-temperature phase diagram and dynamic correlation functions for the two-dimensional Hubbard lattice model.

  8. Dynamics of the microstructure of current channels and the generation of high-energy electrons in nanosecond discharges in air

    Energy Technology Data Exchange (ETDEWEB)

    Karelin, V. I.; Trenkin, A. A., E-mail: trenkin@ntc.vniief.ru; Fedoseev, I. G. [Russian Federal Nuclear Center VNIIEF (Russian Federation)

    2015-12-15

    The results of the three-dimensional numerical simulation of the dynamics of the microstructure of high-voltage nanosecond discharges in air at atmospheric pressure are presented. It is established that the fast (at a time of ≈10 ns) broadening and significant decrease in the gas concentration in the microchannels occur as a result of the ohmic heating of microchannels with the diameter of 1–30 μm. It was shown that the broadening of microchannels in a nanosecond diffusive discharge provides an increase in the ratio of the electric field strength to the gas concentration in microchannels to values sufficient for the generation highenergy electron beams and X-ray bremsstrahlung in them. Features of the dynamics of the system of microchannels and its effect on the efficiency of the generation of high-energy electrons in discharges developing in the microstructuring regime of the current channels are considered.

  9. Electronic band structure, optical, dynamical and thermodynamic properties of cesium chloride (CsCl from first-principles

    Directory of Open Access Journals (Sweden)

    Bingol Suat

    2015-01-01

    Full Text Available The geometric structural optimization, electronic band structure, total density of states for valence electrons, density of states for phonons, optical, dynamical, and thermodynamical features of cesium chloride have been investigated by linearized augmented plane wave method using the density functional theory under the generalized gradient approximation. Ground state properties of cesium chloride are studied. The calculated ground state properties are consistent with experimental results. Calculated band structure indicates that the cesium chloride structure has an indirect band gap value of 5.46 eV and is an insulator. From the obtained phonon spectra, the cesium chloride structure is dynamically stable along the various directions in the Brillouin zone. Temperature dependent thermodynamic properties are studied using the harmonic approximation model.

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

    Directory of Open Access Journals (Sweden)

    Linlin Wei

    2017-07-01

    Full Text Available 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.

  11. Nuclear dynamics investigation of the initial electron transfer in the cyclobutane pyrimidine dimer lesion repair process by photolyases

    CERN Document Server

    Joubert-Doriol, Loic; Olivucci, Massimo; Izmaylov, Artur F

    2016-01-01

    Photolyases are proteins capable of harvesting the sunlight to repair DNA damages caused by UV light. In this work we focus on the first step in the repair process of the cyclobutane pyrimidine dimer photoproduct (CPD) lesion, which is an electron transfer (ET) from a flavine cofactor to CPD, and study the role of various nuclear degrees of freedom (DOF) in this step. The ET step has been experimentally studied using transient spectroscopy and the corresponding data provide excellent basis for testing the quality of quantum dynamical models. Based on previous theoretical studies of electronic structure and conformations of the protein active site, we present a procedure to build a diabatic Hamiltonian for simulating the ET reaction in a molecular complex mimicking the enzyme's active site. We generate a reduced nuclear dimensional model that provides a first non-empirical quantum dynamical description of the structural features influencing the ET rate. By varying the nuclear DOF parametrization in the model t...

  12. Beam Dynamics in an Electron Lens with the Warp Particle-in-cell Code

    CERN Document Server

    Stancari, Giulio; Redaelli, Stefano

    2014-01-01

    Electron lenses are a mature technique for beam manipulation in colliders and storage rings. In an electron lens, a pulsed, magnetically confined electron beam with a given current-density profile interacts with the circulating beam to obtain the desired effect. Electron lenses were used in the Fermilab Tevatron collider for beam-beam compensation, for abort-gap clearing, and for halo scraping. They will be used in RHIC at BNL for head-on beam-beam compensation, and their application to the Large Hadron Collider for halo control is under development. At Fermilab, electron lenses will be implemented as lattice elements for nonlinear integrable optics. The design of electron lenses requires tools to calculate the kicks and wakefields experienced by the circulating beam. We use the Warp particle-in-cell code to study generation, transport, and evolution of the electron beam. For the first time, a fully 3-dimensional code is used for this purpose.

  13. Study of the anode plasma dynamics under the action of a high-power electron beam on epoxy resin

    Science.gov (United States)

    Ananyev, S. S.; Bagdasarov, G. A.; Gasilov, V. A.; Dan'ko, S. A.; Demidov, B. A.; Kazakov, E. D.; Kalinin, Yu. G.; Kurilo, A. A.; Ol'khovskaya, O. G.; Strizhakov, M. G.; Tkachenko, S. I.

    2017-07-01

    Results are presented from experimental studies of plasma dynamics in a diode gap under the action of a high-current relativistic electron beam on epoxy resin at energy densities in the range of 170-860 J/cm2. The plasma expansion was studied by means of an optical streak camera. Three-dimensional numerical simulations in the one-temperature hydrodynamic approximation were also performed. The experimental data are compared with the results of numerical simulations.

  14. Full-Potential Electronic Structure Method Energy and Force Calculations with Density Functional and Dynamical Mean Field Theory

    CERN Document Server

    Wills, John M; Andersson, Per; Delin, Anna; Grechnyev, Oleksiy; Alouani, Mebarek

    2010-01-01

    This book covers the theory of electronic structure of materials, with special emphasis on the usage of linear muffin-tin orbitals. Methodological aspects are given in detail as are examples of the method when applied to various materials. Different exchange and correlation functionals are described and how they are implemented within the basis of linear muffin-tin orbitals. Functionals covered are the local spin density approximation, generalised gradient approximation, self-interaction correction and dynamical mean field theory.

  15. Statistical properties of plasmaspheric hiss derived from Van Allen Probes data and their Effects on radiation belt electron dynamics

    OpenAIRE

    Li, W; Ma, Q; Thorne, RM; Bortnik, J; Kletzing, CA; Kurth, WS; Hospodarsky, GB; Nishimura, Y

    2015-01-01

    ©2015. American Geophysical Union. Plasmaspheric hiss is known to play an important role in controlling the overall structure and dynamics of radiation belt electrons inside the plasmasphere. Using newly available Van Allen Probes wave data, which provide excellent coverage in the entire inner magnetosphere, we evaluate the global distribution of the hiss wave frequency spectrum and wave intensity for different levels of substorm activity. Our statistical results show that observed hiss peak ...

  16. Benchmark of Dynamic Electron Correlation Models for Seniority-Zero Wave Functions and Their Application to Thermochemistry.

    Science.gov (United States)

    Boguslawski, Katharina; Tecmer, Paweł

    2017-10-03

    Wave functions restricted to electron-pair states are promising models to describe static/nondynamic electron correlation effects encountered, for instance, in bond-dissociation processes and transition-metal and actinide chemistry. To reach spectroscopic accuracy, however, the missing dynamic electron correlation effects that cannot be described by electron-pair states need to be included a posteriori. In this Article, we extend the previously presented perturbation theory models with an Antisymmetric Product of 1-reference orbital Geminal (AP1roG) reference function that allows us to describe both static/nondynamic and dynamic electron correlation effects. Specifically, our perturbation theory models combine a diagonal and off-diagonal zero-order Hamiltonian, a single-reference and multireference dual state, and different excitation operators used to construct the projection manifold. We benchmark all proposed models as well as an a posteriori Linearized Coupled Cluster correction on top of AP1roG against CR-CC(2,3) reference data for reaction energies of several closed-shell molecules that are extrapolated to the basis set limit. Moreover, we test the performance of our new methods for multiple bond breaking processes in the homonuclear N2, C2, and F2 dimers as well as the heteronuclear BN, CO, and CN(+) dimers against MRCI-SD, MRCI-SD+Q, and CR-CC(2,3) reference data. Our numerical results indicate that the best performance is obtained from a Linearized Coupled Cluster correction as well as second-order perturbation theory corrections employing a diagonal and off-diagonal zero-order Hamiltonian and a single-determinant dual state. These dynamic corrections on top of AP1roG provide substantial improvements for binding energies and spectroscopic properties obtained with the AP1roG approach, while allowing us to approach chemical accuracy for reaction energies involving closed-shell species.

  17. Electronic structure and lattice dynamics of rhombohedral BiAlO{sub 3} from first-principles

    Energy Technology Data Exchange (ETDEWEB)

    Kaczkowski, J., E-mail: kaczkowski@ifmpan.poznan.pl

    2016-07-01

    The structural, elastic, electronic, dynamical (zone-center phonon modes and Born effective charge tensors), and ferroelectric properties of the rhombohedral BiAlO{sub 3} were calculated within various exchange-correlation functionals. The standard local-density (LDA) and generalized gradient (GGA) approximations, and nonlocal hybrid Heyd-Scuseria-Ernzerhof (HSE) were used. We have also performed the electronic structure calculations with meta-GGA Tran-Blaha functional. BiAlO{sub 3} is indirect band gap semiconductor with the value of band gap: 2.87 eV (GGA), 4.14 eV (HSE), and 3.78 eV (TB-mBJ). The calculated spontaneous polarization is 81 μC/cm{sup 2} (87 μC/cm{sup 2}) for GGA (HSE). The vibrational spectrum including LO-TO splitting was calculated within GGA. The zone-center phonon modes with LO-TO splitting for BiAlO{sub 3} were compared with those in isostructural BiFeO{sub 3}. - Highlights: • Electronic structure of the rhombohedral phase of BiAlO{sub 3} were calculated. • Structural, elastic, dynamical, and ferroelectric properties were investigated. • Calculations were done within GGA, hybrid HSE, and TB-mBJ functionals. • The lattice dynamics with LO-TO splitting were investigated within GGA functional.

  18. Materials Properties and Solvated Electron Dynamics of Isolated Nanoparticles and Nanodroplets Probed with Ultrafast Extreme Ultraviolet Beams.

    Science.gov (United States)

    Ellis, Jennifer L; Hickstein, Daniel D; Xiong, Wei; Dollar, Franklin; Palm, Brett B; Keister, K Ellen; Dorney, Kevin M; Ding, Chengyuan; Fan, Tingting; Wilker, Molly B; Schnitzenbaumer, Kyle J; Dukovic, Gordana; Jimenez, Jose L; Kapteyn, Henry C; Murnane, Margaret M

    2016-02-18

    We present ultrafast photoemission measurements of isolated nanoparticles in vacuum using extreme ultraviolet (EUV) light produced through high harmonic generation. Surface-selective static EUV photoemission measurements were performed on nanoparticles with a wide array of compositions, ranging from ionic crystals to nanodroplets of organic material. We find that the total photoelectron yield varies greatly with nanoparticle composition and provides insight into material properties such as the electron mean free path and effective mass. Additionally, we conduct time-resolved photoelectron yield measurements of isolated oleylamine nanodroplets, observing that EUV photons can create solvated electrons in liquid nanodroplets. Using photoemission from a time-delayed 790 nm pulse, we observe that a solvated electron is produced in an excited state and subsequently relaxes to its ground state with a lifetime of 151 ± 31 fs. This work demonstrates that femotosecond EUV photoemission is a versatile surface-sensitive probe of the properties and ultrafast dynamics of isolated nanoparticles.

  19. Dynamics of Coupled Electron-Boson Systems with the Multiple Davydov D1Ansatz and the Generalized Coherent State.

    Science.gov (United States)

    Chen, Lipeng; Borrelli, Raffaele; Zhao, Yang

    2017-11-22

    The dynamics of a coupled electron-boson system is investigated by employing a multitude of the Davydov D 1 trial states, also known as the multi-D 1 Ansatz, and a second trial state based on a superposition of the time-dependent generalized coherent state (GCS Ansatz). The two Ansätze are applied to study population dynamics in the spin-boson model and the Holstein molecular crystal model, and a detailed comparison with numerically exact results obtained by the (multilayer) multiconfiguration time-dependent Hartree method and the hierarchy equations of motion approach is drawn. It is found that the two methodologies proposed here have significantly improved over that with the single D 1 Ansatz, yielding quantitatively accurate results even in the critical cases of large energy biases and large transfer integrals. The two methodologies provide new effective tools for accurate, efficient simulation of many-body quantum dynamics thanks to a relatively small number of parameters which characterize the electron-nuclear wave functions. The wave-function-based approaches are capable of tracking explicitly detailed bosonic dynamics, which is absent by construct in approaches based on the reduced density matrix. The efficiency and flexibility of our methods are also advantages as compared with numerically exact approaches such as QUAPI and HEOM, especially at low temperatures and in the strong coupling regime.

  20. Dynamics of electron-capture-to-continuum (ECC) formation in slow ion-atom collisions

    Energy Technology Data Exchange (ETDEWEB)

    Afaneh, F [Physics Department, The Hashemite University, PO Box 150459, Zarqa 13115 (Jordan); Schmidt, L Ph H [Institut fuer Kernphysik, Max-von-Laue-Str. 1, 60438 Frankfurt (Germany); Schoeffler, M [Institut fuer Kernphysik, Max-von-Laue-Str. 1, 60438 Frankfurt (Germany); Stiebing, K E [Institut fuer Kernphysik, Max-von-Laue-Str. 1, 60438 Frankfurt (Germany); Al-Jundi, J [Physics Department, The Hashemite University, PO Box 150459, Zarqa 13115 (Jordan); Schmidt-Boecking, H [Institut fuer Kernphysik, Max-von-Laue-Str. 1, 60438 Frankfurt (Germany); Doerner, R [Institut fuer Kernphysik, Max-von-Laue-Str. 1, 60438 Frankfurt (Germany)

    2007-05-28

    The zero-degree ejected-electron spectrum for protons incident on He at 25 keV is examined experimentally using the COLTRIMS technique. The momentum distribution of the emitted electrons for the transfer ionization (TI) reaction channel is measured in coincidence with the momentum vectors of the recoil ion and the scattered projectile. The momentum distribution of the electrons emitted around zero degree in the forward direction for the TI reaction channel shows two prominent structures: the electron-capture-to-the-continuum (ECC) peak and the saddle-point peak. From the measured fully differential electron emission cross sections with respect to the scattering plane we can deduce that the main ECC formation mechanism is electron promotion via quasimolecular orbitals.

  1. Relativistic quantum dynamics in strong fields: Photon emission from heavy, few-electron ions

    Energy Technology Data Exchange (ETDEWEB)

    Fritzsche, S. [Kassel Univ. (Germany). Inst. fuer Physik; Indelicato, P. [Lab. Kastler Brossel, Ecole Normale Superieure et Universite Pierre et Marie Curie, Paris (France); Stoehlker, T. [Frankfurt Univ. (Germany). Inst. fuer Kernphysik

    2005-03-01

    Recent progress in the study of the photon emission from highly-charged heavy ions is reviewed. These investigations show that high-Z ions provide a unique tool for improving the understanding of the electron-electron and electron-photon interaction in the presence of strong fields. Apart from the bound-state transitions, which are accurately described in the framework of quantum electrodynamics, much information has been obtained also from the radiative capture of (quasi-) free electrons by high-Z ions. Many features in the observed spectra hereby confirm the inherently relativistic behavior of even the simplest compound quantum systems in nature. (orig.)

  2. Influence of environment induced correlated fluctuations in electronic coupling on coherent excitation energy transfer dynamics in model photosynthetic systems.

    Science.gov (United States)

    Huo, Pengfei; Coker, David F

    2012-03-21

    Two-dimensional photon-echo experiments indicate that excitation energy transfer between chromophores near the reaction center of the photosynthetic purple bacterium Rhodobacter sphaeroides occurs coherently with decoherence times of hundreds of femtoseconds, comparable to the energy transfer time scale in these systems. The original explanation of this observation suggested that correlated fluctuations in chromophore excitation energies, driven by large scale protein motions could result in long lived coherent energy transfer dynamics. However, no significant site energy correlation has been found in recent molecular dynamics simulations of several model light harvesting systems. Instead, there is evidence of correlated fluctuations in site energy-electronic coupling and electronic coupling-electronic coupling. The roles of these different types of correlations in excitation energy transfer dynamics are not yet thoroughly understood, though the effects of site energy correlations have been well studied. In this paper, we introduce several general models that can realistically describe the effects of various types of correlated fluctuations in chromophore properties and systematically study the behavior of these models using general methods for treating dissipative quantum dynamics in complex multi-chromophore systems. The effects of correlation between site energy and inter-site electronic couplings are explored in a two state model of excitation energy transfer between the accessory bacteriochlorophyll and bacteriopheophytin in a reaction center system and we find that these types of correlated fluctuations can enhance or suppress coherence and transfer rate simultaneously. In contrast, models for correlated fluctuations in chromophore excitation energies show enhanced coherent dynamics but necessarily show decrease in excitation energy transfer rate accompanying such coherence enhancement. Finally, for a three state model of the Fenna-Matthews-Olsen light

  3. Coupled electron-phonon transport from molecular dynamics with quantum baths

    DEFF Research Database (Denmark)

    Lu, Jing Tao; Wang, J. S.

    2009-01-01

    -classical approximation. Both charge and energy transport and their interplay can be studied. We compare the MD results with those of a fully quantum mechanical nonequilibrium Green's function (NEGF) approach for the electron currents. We find a ballistic to diffusive transition of the electron conduction in one...

  4. Charge and spin control of ultrafast electron and hole dynamics in single CdSe/ZnSe quantum dots

    Science.gov (United States)

    Hinz, C.; Gumbsheimer, P.; Traum, C.; Holtkemper, M.; Bauer, B.; Haase, J.; Mahapatra, S.; Frey, A.; Brunner, K.; Reiter, D. E.; Kuhn, T.; Seletskiy, D. V.; Leitenstorfer, A.

    2018-01-01

    We study the dynamics of photoexcited electrons and holes in single negatively charged CdSe/ZnSe quantum dots with two-color femtosecond pump-probe spectroscopy. An initial characterization of the energy level structure is performed at low temperatures and magnetic fields of up to 5 T. Emission and absorption resonances are assigned to specific transitions between few-fermion states by a theoretical model based on a configuration interaction approach. To analyze the dynamics of individual charge carriers, we initialize the quantum system into excited trion states with defined energy and spin. Subsequently, the time-dependent occupation of the trion ground state is monitored by spectrally resolved differential transmission measurements. We observe subpicosecond dynamics for a hole excited to the D shell. The energy dependence of this D -to-S shell intraband transition is investigated in quantum dots of varying size. Excitation of an electron-hole pair in the respective p shells leads to the formation of singlet and triplet spin configurations. Relaxation of the p -shell singlet is observed to occur on a time scale of a few picoseconds. Pumping of p -shell triplet transitions opens up two pathways with distinctly different scattering times. These processes are shown to be governed by the mixing of singlet and triplet states due to exchange interactions enabling simultaneous electron and hole spin flips. To isolate the relaxation channels, we align the spin of the residual electron by a magnetic field and employ laser pulses of defined helicity. This step provides ultrafast preparation of a fully inverted trion ground state of the quantum dot with near unity probability, enabling deterministic addition of a single photon to the probe pulse. Therefore our experiments represent a significant step towards using single quantum emitters with well-controled inversion to manipulate the photon statistics of ultrafast light pulses.

  5. Relativistic electron dynamics produced by azimuthally localized poloidal mode ULF waves: Boomerang-shaped pitch angle evolutions

    Science.gov (United States)

    Hao, Y. X.; Zong, Q.-G.; Zhou, X.-Z.; Rankin, R.; Chen, X. R.; Liu, Y.; Fu, S. Y.; Spence, H. E.; Blake, J. B.; Reeves, G. D.

    2017-08-01

    We present an analysis of "boomerang-shaped" pitch angle evolutions of outer radiation belt relativistic electrons observed by the Van Allen Probes after the passage of an interplanetary shock on 7 June 2014. The flux at different pitch angles is modulated by Pc5 waves, with equatorially mirroring electrons reaching the satellite first. For 90° pitch angle electrons, the phase change of the flux modulations across energy exceeds 180° and increasingly tilts with time. Using estimates of the arrival time of particles of different pitch angles at the spacecraft location, a scenario is investigated in which shock-induced ULF waves interact with electrons through the drift resonance mechanism in a localized region westward of the spacecraft. Numerical calculations on particle energy gain with the modified ULF wavefield reproduce the observed boomerang stripes and modulations in the electron energy spectrogram. The study of boomerang stripes and their relationship to drift resonance taking place at a location different from the observation point adds new understanding of the processes controlling the dynamics of the outer radiation belt.

  6. Ultrafast Gap Dynamics and Electronic Interactions in a Photoexcited Cuprate Superconductor

    Directory of Open Access Journals (Sweden)

    S. Parham

    2017-10-01

    Full Text Available We perform time- and angle-resolved photoemission spectroscopy (trARPES on optimally doped Bi_{2}Sr_{2}CaCu_{2}O_{8+δ} (BSCCO-2212 using sufficient energy resolution (9 meV to resolve the k-dependent near-nodal gap structure on time scales where the concept of an electronic pseudotemperature is a useful quantity, i.e., after electronic thermalization has occurred. We study the ultrafast evolution of this gap structure, uncovering a very rich landscape of decay rates as a function of angle, temperature, and energy. We explicitly focus on the quasiparticle states at the gap edge as well as on the spectral weight inside the gap that “fills” the gap—understood as an interaction, or self-energy effect—and we also make high resolution measurements of the nodal states, enabling a direct and accurate measurement of the electronic temperature (or pseudotemperature of the electrons in the system. Rather than the standard method of interpreting these results using individual quasiparticle scattering rates that vary significantly as a function of angle, temperature, and energy, we show that the entire landscape of relaxations can be understood by modeling the system as following a nonequilibrium, electronic pseudotemperature that controls all electrons in the zone. Furthermore, this model has zero free parameters, as we obtain the crucial information of the SC gap Δ and the gap-filling strength Γ_{TDoS} by connecting to static ARPES measurements. The quantitative and qualitative agreement between data and model suggests that the critical parameters and interactions of the system, including the pairing interactions, follow parametrically from the electronic pseudotemperature. We expect that this concept will be relevant for understanding the ultrafast response of a great variety of electronic materials, even though the electronic pseudotemperature may not be directly measurable.

  7. Steering the Electron in H2+ by Nuclear Wave Packet Dynamics

    Science.gov (United States)

    Fischer, Bettina; Kremer, Manuel; Pfeifer, Thomas; Feuerstein, Bernold; Sharma, Vandana; Thumm, Uwe; Schröter, Claus Dieter; Moshammer, Robert; Ullrich, Joachim

    2010-11-01

    By combining carrier-envelope phase (CEP) stable light fields and the traditional method of optical pump-probe spectroscopy we study electron localization in dissociating H2+ molecular ions. Localization and localizability of electrons is observed to strongly depend on the time delay between the two CEP-stable laser pulses with a characteristic periodicity corresponding to the oscillating molecular wave packet. Variation of the pump-probe delay time allows us to uncover the underlying physical mechanism for electron localization, which are two distinct sets of interfering dissociation channels that exhibit specific temporal signatures in their asymmetry response.

  8. Beam dynamics performances and applications of a low-energy electron-beam magnetic bunch compressor

    Energy Technology Data Exchange (ETDEWEB)

    Prokop, C. R.; Piot, P.; Carlsten, B. E.; Church, M.

    2013-08-01

    Many front-end applications of electron linear accelerators rely on the production of temporally compressed bunches. The shortening of electron bunches is often realized with magnetic bunch compressors located in high-energy sections of accelerators. Magnetic compression is subject to collective effects including space charge and self interaction via coherent synchrotron radiation. In this paper we explore the application of magnetic compression to low-energy (~40MeV), high-charge (nC) electron bunches with low normalized transverse emittances (<5@mm).

  9. Beam dynamics in an initial part of a high Brightness electron linac

    CERN Document Server

    Ayzatsky, M I; Dovbnya-Kushnir, V A

    2001-01-01

    The paper is focused on problems of obtained a bright electron beam in a system that includes a grid-controlled electron gun,a klystron type type subharmonical buncher, a standing wave fundamental buncher with increasing accelerating field and a short travelling wave accelerating section. Beam focusing is provided by a longitudinal solenoidal magnetic field.It was shown that the proposed system can provide electron bunches with a peak current more than 100 A and normalized r.m.s. emittance no more than phi centre dot mm centre dot mrad.

  10. Dynamic-Stark-effect-induced coherent mixture of virtual paths in laser-dressed helium: energetic electron impact excitation

    Science.gov (United States)

    Agueny, Hicham; Makhoute, Abdelkader; Dubois, Alain

    2017-06-01

    We theoretically investigate quantum virtual path interference caused by the dynamic Stark effect in bound-bound electronic transitions. The effect is studied in an intermediate resonant region and in connection with the energetic electron impact excitation of a helium atom embedded in a weak low-frequency laser field. The process under investigation is dealt with via a Born-Floquet approach. Numerical calculations show a resonant feature in laser-assisted cross sections. The latter is found to be sensitive to the intensity of the laser field dressing. We show that this feature is a signature of quantum beats which result from the coherent mixture of different quantum virtual pathways, and that excitation may follow in order to end up with a common final channel. This mixture arises from the dynamic Stark effect, which produces a set of avoided crossings in laser-dressed states. The effect allows one to coherently control quantum virtual path interference by varying the intensity of the laser field dressing. Our findings suggest that the combination of an energetic electron and a weak laser field is a useful tool for the coherent control of nonadiabatic transitions in an intermediate resonant region.

  11. Electron induced break-up of helium. Benchmark experiments on a dynamical four-body Coulomb system

    Energy Technology Data Exchange (ETDEWEB)

    Duerr, M.

    2006-07-05

    This work presents an experimental study of fragmentation of helium by electron impact, in which absolute fully differential cross sections for single ionization, ionization-excitation and double ionization were determined. By applying a charged-particle imaging technique, the so-called 'reaction microscope', a large fraction of the final-state momentum space is covered, and the major limitations of previous experimental methods applied in this field could be overcome. Decisive modifications of the previous reaction microscope were undertaken, the most important one being the arrangement of the projectile beam parallel to the imaging-fields. For single ionization on helium an enhanced electron emission outside the projectile scattering plane is observed at both considered impact energies (102 eV and 1 keV), which is similar to the result found for ion-impact (M. Schulz et al., Nature (London) 422, 48 (2003)). The angle resolved cross sections obtained for double ionization at 105 eV impact energy reveal, that the process is dominated by the mutual repulsion of the three final-state continuum electrons. However, signatures of more complex dynamics are also observed. The data provide an ultimate benchmark for recently developed theories treating the dynamical three- and four-body Coulomb problem. (orig.)

  12. Ballistic dynamics of a relativistic electron beam for mapping of the magnetosphere

    Science.gov (United States)

    Greklek-McKeon, Michael; Powis, Andrew T.; Kaganovich, Igor D.; Porazik, Peter; Johnson, Jay; Willard, Jake; Sanchez, Ennio

    2017-10-01

    Relativistic electrons fired from an orbiting satellite will propagate along the field lines of the magnetosphere. When the electrons impact the Earth's atmosphere, they produce a characteristic signature that is detectable by ground stations. Such a diagnostic would enable direct validation of magnetospheric models, and assist in answering outstanding questions on auroral arcs. We determine the loss cone of a relativistic electron beam at various injection points within the Earth's magnetosphere during the stages of a prominent geomagnetic event. We then study the degree of beam spreading during propagation to determine the viability of signal detection at the top of the atmosphere. This verification, using realistic magnetic field data, demonstrates that an electron beam emitted from a satellite can be fired into the loss cone of the Earth's atmosphere and create an observable signal on the ground. This work is supported by the US DOE Contract No. DE-AC02-09CH11466.

  13. Dynamics of electron acceleration in laser-driven wakefields. Acceleration limits and asymmetric plasma waves

    Energy Technology Data Exchange (ETDEWEB)

    Popp, Antonia

    2011-12-16

    The experiments presented in this thesis study several aspects of electron acceleration in a laser-driven plasma wave. High-intensity lasers can efficiently drive a plasma wave that sustains electric fields on the order of 100 GV/m. Electrons that are trapped in this plasma wave can be accelerated to GeV-scale energies. As the accelerating fields in this scheme are 3-4 orders of magnitude higher than in conventional radio-frequency accelerators, the necessary acceleration distance can be reduced by the same factor, turning laser-wakefield acceleration (LWFA) into a promising compact, and potentially cheaper, alternative. However, laser-accelerated electron bunches have not yet reached the parameter standards of conventional accelerators. This work will help to gain better insight into the acceleration process and to optimize the electron bunch properties. The 25 fs, 1.8 J-pulses of the ATLAS laser at the Max-Planck-Institute of Quantum Optics were focused into a steady-state flow gas cell. This very reproducible and turbulence-free gas target allows for stable acceleration of electron bunches. Thus the sensitivity of electron parameters to subtle changes of the experimental setup could be determined with meaningful statistics. At optimized experimental parameters, electron bunches of {approx}50 pC total charge were accelerated to energies up to 450 MeV with a divergence of {approx}2 mrad FWHM. As, in a new design of the gas cell, its length can be varied from 2 to 14 mm, the electron bunch energy could be evaluated after different acceleration distances, at two different electron densities. From this evolution important acceleration parameters could be extracted. At an electron density of 6.43. 10{sup 18} cm{sup -3} the maximum electric field strength in the plasma wave was determined to be {approx}160 GV/m. The length after which the relativistic electrons outrun the accelerating phase of the electric field and are decelerated again, the so-called dephasing length

  14. SYSTEM DYNAMICS MODEL FOR EVALUATION OF REUSE OF ELECTRONIC WASTE ORIGINATED FROM PERSONAL COMPUTERS

    National Research Council Canada - National Science Library

    Eugênio Simonetto; Osvaldo Quelhas; Vesna Spasojević Brkić; Goran Putnik; Cátia Alves; Hélio Castro

    2016-01-01

    Information and Communication Technologies (ICT) are part of the day to day activities of a large part of world population, however its use involves a growing generation of electronic waste (ewaste...

  15. U31: vehicle stability and dynamics electronic stability control final report.

    Science.gov (United States)

    2011-09-01

    A team led by NTRCI is working to improve the roll and yaw stability of heavy duty combination trucks through developing stability algorithms, assembling demonstration hardware, and investigating robust wireless communication. : Modern electronic sta...

  16. Selforganisation and dynamics peculiarities of intense electron beams in compact crossed fields systems

    CERN Document Server

    Agafonov, A V; Fedorov, V M

    2001-01-01

    The review of the results of computer simulations of electron flow self-organisation inside magnetically isolated coaxial diodes (magnetron gun) is given. Magnetron guns of usual and inverted polarities are considered.

  17. Nonlocal Electron-Phonon Interaction as a Source of Dynamic Charge Stripes in the Cuprates

    Directory of Open Access Journals (Sweden)

    Claus Falter

    2012-01-01

    small pockets with reduced doping. We argue that the incompressibility of the orbital and simultaneously the compressibility of the orbital in the pseudogap state seem to be required to nucleate dynamic stripes.

  18. Studying Dynamic Processes of Nano-sized Objects in Liquid using Scanning Transmission Electron Microscopy

    OpenAIRE

    Hermannsd?rfer, Justus; de Jonge, Niels

    2017-01-01

    Samples fully embedded in liquid can be studied at a nanoscale spatial resolution with Scanning Transmission Electron Microscopy (STEM) using a microfluidic chamber assembled in the specimen holder for Transmission Electron Microscopy (TEM) and STEM. The microfluidic system consists of two silicon microchips supporting thin Silicon Nitride (SiN) membrane windows. This article describes the basic steps of sample loading and data acquisition. Most important of all is to ensure that the liquid c...

  19. Symmetry-constrained Analysis of Pulsed Double Electron-Electron Resonance (DEER) Spectroscopy Reveals the Dynamic Nature of the KcsA Activation Gate

    Science.gov (United States)

    Dalmas, Olivier; Hyde, H. Clark; Hulse, Raymond E.; Perozo, Eduardo

    2013-01-01

    Distance determination from an echo intensity modulation obtained by pulsed double electron-electron resonance (DEER) experiment is a mathematically ill-posed problem. Tikhonov regularization yields distance distributions that can be difficult to interpret, especially in system with multiple discrete distance distributions. Here, we show that by using geometric fit constraints in symmetric homo-oligomeric protein systems, we were able to increase the accuracy of a model-based fit solution based on a sum of Gaussian distributions. Our approach was validated on two different ion channels of known oligomeric states, KcsA (a tetramer) and CorA (a pentamer). Statistical analysis of the resulting fits was integrated within our method to help the experimenter evaluate the significance of a symmetry-constrained vs. standard model distribution fit and to examine multi-distance confidence regions. This approach was used to quantitatively evaluate the role of the C-terminal domain (CTD) on the flexibility and conformation of the activation gate of the K+ channel KcsA. Our analysis reveals a significant increase in the dynamics of the inner bundle gate upon opening. Also, it explicitly demonstrates the degree to which the CTD restricts the motion of the lower gate at rest and during activation gating. PMID:22946877

  20. Effect of the lattice dynamics on the electronic structure of paramagnetic NiO within the disordered local moment picture

    Science.gov (United States)

    Mozafari, Elham; Alling, Björn; Belov, Maxim P.; Abrikosov, Igor A.

    2018-01-01

    Using the disordered local moments approach in combination with the ab initio molecular dynamics method, we simulate the behavior of a paramagnetic phase of NiO at finite temperatures to investigate the effect of magnetic disorder, thermal expansion, and lattice vibrations on its electronic structure. In addition, we study its lattice dynamics. We verify the reliability of our theoretical scheme via comparison of our results with available experiment and earlier theoretical studies carried out within static approximations. We present the phonon dispersion relations for the paramagnetic rock-salt (B1) phase of NiO and demonstrate that it is dynamically stable. We observe that including the magnetic disorder to simulate the paramagnetic phase has a small yet visible effect on the band gap. The amplitude of the local magnetic moment of Ni ions from our calculations for both antiferromagnetic and paramagnetic phases agree well with other theoretical and experimental values. We demonstrate that the increase of temperature up to 1000 K does not affect the electronic structure strongly. Taking into account the lattice vibrations and thermal expansion at higher temperatures have a major impact on the electronic structure, reducing the band gap from ˜3.5 eV at 600 K to ˜2.5 eV at 2000 K. We conclude that static lattice approximations can be safely employed in simulations of the paramagnetic state of NiO up to relatively high temperatures (˜1000 K), but as we get closer to the melting temperature vibrational effects become quite large and therefore should be included in the calculations.

  1. Crystallization kinetics of the phase change material GeSb6Te measured with dynamic transmission electron microscopy.

    Science.gov (United States)

    Winseck, M M; Cheng, H-Y; Campbell, G H; Santala, M K

    2016-06-14

    GeSb6Te is a chalcogenide-based phase change material that has shown great ptoential for use in solid-state memory devices. The crystallization kinetics of amorphous thin films of GeSb6Te during laser crystallization were followed with dynamic transmission electron microscopy, a photo-emission electron microscopy technique with nanosecond-scale time resolution. Nine-frame movies of crystal growth were taken during laser crystallization. The nucleation rate is observed to be very low and the growth rates are very high, up to 10.8 m s(-1) for amorphous as-deposited films and significantly higher for an amorphous film subject to sub-threshold laser annealing before crystallization. The measured growth rates exceed any directly measured growth rate of a phase change material. The crystallization is reminiscent of explosive crystallization of elemental semiconductors both in the magnitude of the growth rate and in the resulting crystalline microstructures.

  2. Resonant inelastic X-ray scattering as a probe of molecular structure and electron dynamics in solutions

    Energy Technology Data Exchange (ETDEWEB)

    Lange, Kathrin M. [Joint Ultrafast Dynamics Lab in Solutions and at Interfaces (JULiq), Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Strasse 15, 12489 Berlin (Germany); Freie Universität Berlin, FB Physik, Arnimallee 14, D-14195 Berlin (Germany); Max-Born-Institut, Max Born Straße 2A, 12489 Berlin (Germany); Suljoti, Edlira [Joint Ultrafast Dynamics Lab in Solutions and at Interfaces (JULiq), Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Strasse 15, 12489 Berlin (Germany); Freie Universität Berlin, FB Physik, Arnimallee 14, D-14195 Berlin (Germany); Aziz, Emad F., E-mail: Emad.Aziz@fu-berlin.de [Joint Ultrafast Dynamics Lab in Solutions and at Interfaces (JULiq), Helmholtz-Zentrum Berlin für Materialien und Energie, Albert-Einstein-Strasse 15, 12489 Berlin (Germany); Freie Universität Berlin, FB Physik, Arnimallee 14, D-14195 Berlin (Germany)

    2013-06-15

    Resonant inelastic X-ray scattering (RIXS) technique is applied to gain insight into the local electronic structure in liquid phase. The approach combines a liquid micro-jet and an X-ray emission spectrometer (XES) both installed in the recently developed LiXEdrom experimental station. Here we demonstrate how the combined approach enables investigation of the hydrogen bonding network in water and of chemical bonding in different solvents. In addition, the probe of energy transfer and electron dynamics at the metal–solvent interface is achieved by comparing the integrated RIXS intensities of the different radiative decay channels of the 2p core-hole of 3d transition-metals. The integrated RIXS intensities build the partial and the inverse partial X-ray fluorescence yields that allow for absorption measurements free from background signal of other elements or saturation effects.

  3. Assessment of Time-dependent Unrestricted Hartree-Fock Method for Electron Dynamics in Intense Laser Fields

    Science.gov (United States)

    Sato, Takeshi; Ishikawa, Kenichi L.

    Time-dependent restricted and unrestricted Hartree-Fock (TD-RHF and TD-UHF) methods are comparatively assessed for the description of the electron dynamics in intense laser fields. These methods are applied to the one-dimensional H2 molecule exposed to an intense laser field, and compared to the results from the time-dependent Schrödinger (TDSE) equation. Around the equilibrium interatomic distance, where the initial RHF and UHF wavefunctions coincide, TD-UHF keeps an initial closed-shell, thus underestimates large amplitude electron motions. At a longer interatomic distance, where the UHF wavefunction differs from the RHF one, TD-UHF better reprodeces the TDSE result than TD-RHF does.

  4. Drop-on-Demand Inkjet Printhead Performance Enhancement by Dynamic Lumped Element Modeling for Printable Electronics Fabrication

    Directory of Open Access Journals (Sweden)

    Maowei He

    2014-01-01

    Full Text Available The major challenge in printable electronics fabrication is the print resolution and accuracy. In this paper, the dynamic lumped element model (DLEM is proposed to directly simulate an inkjet-printed nanosilver droplet formation process and used for predictively controlling jetting characteristics. The static lumped element model (LEM previously developed by the authors is extended to dynamic model with time-varying equivalent circuits to characterize nonlinear behaviors of piezoelectric printhead. The model is then used to investigate how performance of the piezoelectric ceramic actuator influences jetting characteristics of nanosilver ink. Finally, the proposed DLEM is applied to predict the printing quality using nanosilver ink. Experimental results show that, compared to other analytic models, the proposed DLEM has a simpler structure with the sufficient simulation and prediction accuracy.

  5. A wide dynamic range BF{sub 3} neutron monitor with front-end electronics based on a logarithmic amplifier

    Energy Technology Data Exchange (ETDEWEB)

    Ferrarini, M., E-mail: michele.ferrarini@polimi.i [Politecnico di Milano, Dipartimento Energia, via G. Ponzio 34/3, I-20133 Milano (Italy); Fondazione CNAO, via Caminadella 16, 20123 Milano (Italy); Varoli, V. [Politecnico di Milano, Dipartimento Energia, via G. Ponzio 34/3, I-20133 Milano (Italy); Favalli, A. [European Commission, Joint Research Centre, Institute for the Protection and Security of Citizen, TP 800, Via E. Fermi, 21027 Ispra (Vatican City State, Holy See) (Italy); Caresana, M. [Politecnico di Milano, Dipartimento Energia, via G. Ponzio 34/3, I-20133 Milano (Italy); Pedersen, B. [European Commission, Joint Research Centre, Institute for the Protection and Security of Citizen, TP 800, Via E. Fermi, 21027 Ispra (Italy)

    2010-02-01

    This paper describes a wide dynamic range neutron monitor based on a BF{sub 3} neutron detector. The detector is used in current mode, and front-end electronics based on a logarithmic amplifier are used in order to have a measurement capability ranging over many orders of magnitude. The system has been calibrated at the Polytechnic of Milan, CESNEF, with an AmBe neutron source, and has been tested in a pulsed field at the PUNITA facility at JRC, Ispra. The detector has achieved a dynamic range of over 6 orders of magnitude, being able to measure single neutron pulses and showing saturation-free response for a reaction rate up to 10{sup 6} s{sup -1}. It has also proved effective in measuring the PUNITA facility pulse integral fluence.

  6. Dynamic Processes in Biology, Chemistry, and Materials Science: Opportunities for UltraFast Transmission Electron Microscopy - Workshop Summary Report

    Energy Technology Data Exchange (ETDEWEB)

    Kabius, Bernd C.; Browning, Nigel D.; Thevuthasan, Suntharampillai; Diehl, Barbara L.; Stach, Eric A.

    2012-07-25

    This report summarizes a 2011 workshop that addressed the potential role of rapid, time-resolved electron microscopy measurements in accelerating the solution of important scientific and technical problems. A series of U.S. Department of Energy (DOE) and National Academy of Science workshops have highlighted the critical role advanced research tools play in addressing scientific challenges relevant to biology, sustainable energy, and technologies that will fuel economic development without degrading our environment. Among the specific capability needs for advancing science and technology are tools that extract more detailed information in realistic environments (in situ or operando) at extreme conditions (pressure and temperature) and as a function of time (dynamic and time-dependent). One of the DOE workshops, Future Science Needs and Opportunities for Electron Scattering: Next Generation Instrumentation and Beyond, specifically addressed the importance of electron-based characterization methods for a wide range of energy-relevant Grand Scientific Challenges. Boosted by the electron optical advancement in the last decade, a diversity of in situ capabilities already is available in many laboratories. The obvious remaining major capability gap in electron microscopy is in the ability to make these direct in situ observations over a broad spectrum of fast (µs) to ultrafast (picosecond [ps] and faster) temporal regimes. In an effort to address current capability gaps, EMSL, the Environmental Molecular Sciences Laboratory, organized an Ultrafast Electron Microscopy Workshop, held June 14-15, 2011, with the primary goal to identify the scientific needs that could be met by creating a facility capable of a strongly improved time resolution with integrated in situ capabilities. The workshop brought together more than 40 leading scientists involved in applying and/or advancing electron microscopy to address important scientific problems of relevance to DOE’s research

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

    Energy Technology Data Exchange (ETDEWEB)

    Klinkusch, Stefan; Tremblay, Jean Christophe [Institute for Chemistry and Biochemistry, Freie Universität Berlin, Takustr. 3, D-14195 Berlin (Germany)

    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.

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

    Science.gov (United States)

    Klinkusch, Stefan; Tremblay, Jean Christophe

    2016-05-01

    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.

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

    Energy Technology Data Exchange (ETDEWEB)

    Maitra, Neepa [Hunter College City University of New York, New York, NY (United States)

    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.

  10. Electron spin resonance investigation of Mn^{2+} ions and their dynamics in manganese doped SrTiO_3

    OpenAIRE

    Laguta, V. V.; Kondakova, I. V.; Bykov, I. P.; Glinchuk, M. D.; Vilarinho, P M; Tkach, A; L. Jastrabik

    2007-01-01

    Using electron spin resonance, lattice position and dynamic properties of Mn2+ ions were studied in 0.5 and 2 % manganese doped SrTiO3 ceramics prepared by conventional mixed oxide method. The measurements showed that Mn2+ ions substitute preferably up to 97 % for Sr if the ceramics is prepared with a deficit of Sr ions. Motional narrowing of the Mn2+ ESR spectrum was observed when temperature increases from 120 K to 240-250 K that was explained as a manifestation of off-center position of th...

  11. Characterising thermal resistances and capacitances of GaN high-electron-mobility transistors through dynamic electrothermal measurements

    DEFF Research Database (Denmark)

    Wei, Wei; Mikkelsen, Jan H.; Jensen, Ole Kiel

    2014-01-01

    This study presents a method to characterise thermal resistances and capacitances of GaN high-electron-mobility transistors (HEMTs) through dynamic electrothermal measurements. A measured relation between RF gain and the channel temperature (Tc) is formed and used for indirect measurements...... method ensures that trapping effects have insignificant impact on the measurements of Tc responses, which makes this method suitable for GaN HEMT characterisation. The applicability of this method is demonstrated by characterising thermal resistances and capacitances of a CREE CGH40006P GaN HEMT....

  12. Modeling and simulation of longitudinal dynamics for Low Energy Ring–High Energy Ring at the Positron-Electron Project

    Directory of Open Access Journals (Sweden)

    C. Rivetta

    2007-02-01

    Full Text Available A time domain dynamic modeling and simulation tool for beam-cavity interactions in the Low Energy Ring (LER and High Energy Ring (HER at the Positron-Electron Project (PEP-II is presented. Dynamic simulation results for PEP-II are compared to measurements of the actual machine. The motivation for this tool is to explore the stability margins and performance limits of PEP-II radio-frequency (RF systems at future higher currents and upgraded RF configurations. It also serves as a test bed for new control algorithms and can define the ultimate limits of the low-level RF (LLRF architecture. The time domain program captures the dynamic behavior of the beam-cavity-LLRF interaction based on a reduced model. The ring current is represented by macrobunches. Multiple RF stations in the ring are represented via one or two macrocavities. Each macrocavity captures the overall behavior of all the 2 or 4 cavity RF stations. Station models include nonlinear elements in the klystron and signal processing. This enables modeling the principal longitudinal impedance control loops interacting via the longitudinal beam model. The dynamics of the simulation model are validated by comparing the measured growth rates for the LER with simulation results. The simulated behavior of the LER at increased operation currents is presented via low-mode instability growth rates. Different control strategies are compared and the effects of both the imperfections in the LLRF signal processing and the nonlinear drivers and klystrons are explored.

  13. Modeling and Simulation of Longitudinal Dynamics for Low Energy Ring_High Energy Ring at the Positron-Electron Project

    Energy Technology Data Exchange (ETDEWEB)

    Rivetta, Claudio; Mastorides, T.; Fox, J.D.; Teytelman, D.; Van Winkle, D.; /SLAC

    2007-03-06

    A time domain dynamic modeling and simulation tool for beam-cavity interactions in the Low Energy Ring (LER) and High Energy Ring (HER) at the Positron-Electron Project (PEP-II) is presented. Dynamic simulation results for PEP-II are compared to measurements of the actual machine. The motivation for this tool is to explore the stability margins and performance limits of PEP-II radio-frequency (RF) systems at future higher currents and upgraded RF configurations. It also serves as a test bed for new control algorithms and can define the ultimate limits of the low-level RF (LLRF) architecture. The time domain program captures the dynamic behavior of the beam-cavity-LLRF interaction based on a reduced model. The ring current is represented by macrobunches. Multiple RF stations in the ring are represented via one or two macrocavities. Each macrocavity captures the overall behavior of all the 2 or 4 cavity RF stations. Station models include nonlinear elements in the klystron and signal processing. This enables modeling the principal longitudinal impedance control loops interacting via the longitudinal beam model. The dynamics of the simulation model are validated by comparing the measured growth rates for the LER with simulation results. The simulated behavior of the LER at increased operation currents is presented via low-mode instability growth rates. Different control strategies are compared and the effects of both the imperfections in the LLRF signal processing and the nonlinear drivers and klystrons are explored.

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

    Science.gov (United States)

    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.

  15. Particle Dynamics at and Near the Electron and Ion Diffusion Regions

    Science.gov (United States)

    Giles, B. L.; Burch, J. L.; Torbert, R. B.; Phan, T.; Fuselier, S. A.; Avanov, L. A.; Boardsen, S. A.; Chandler, M. O.; Chen, L. J.; Coffey, V. N.; Dorelli, J.; Ergun, R.; Genestreti, K. J.; Gershman, D. J.; Lavraud, B.; Mackler, D. A.; Moore, T. E.; Paterson, W. R.; Pollock, C.; Rager, A. C.; Russell, C.; Saito, Y.; Schiff, C.; Shuster, J. R.; Smith, S. E.; Strangeway, R. J.; Vinas, A. F.; Wang, S.; Webster, J. M.; Wilder, F. D.; Zesta, E.

    2016-12-01

    At the dayside magnetopause, magnetic reconnection often occurs in thin sheets of plasma carrying electrical currents and rotating magnetic fields. Charged particles interact strongly with the magnetic field and simultaneously their motions modify the fields. Researchers are able to simulate the macroscopic interactions between the two plasma domains on both sides of the magnetopause and — for precise results —must include individual particle motions to better describe microscopic scales. For this presentation, plasma ion and electron distributions are examined for a high-shear asymmetric reconnection event observed by MMS on Oct. 16, 2015. As previously reported for this event, the opening of field lines was observed in the electron distributions by all four spacecraft as the transition from a perpendicular nongyrotropic crescent distribution to a parallel crescent distribution. The parallel crescents observed were flowing toward the Earth along reconnected field lines. On further examination, the higher energy magnetospheric electrons were simultaneously observed flowing away from the Earth along with an embedded narrow beam of electrons. A strong ion jet reversal was observed through the electron diffusion region at which the ions had very low energies as compared to the jets. Several of the structures noted have been demonstrated in simulations and others have not been predicted or explained to date. We report on these observations and their persistence at similar encounters with asymmetric reconnection

  16. Dynamic electron correlation in interactions of light with matter formulated in b ⃗ space

    Science.gov (United States)

    Kaplan, Lev; McGuire, J. H.

    2015-09-01

    Scattering of beams of light and matter from multielectron atomic targets is formulated in the position representation of quantum mechanics. This yields expressions for the probability amplitude a (b ⃗) for a wide variety of processes. Here the spatial parameter b ⃗ is the distance of closest approach of incoming particles traveling on a straight line with the center of the atomic target. The correlated probability amplitude a (b ⃗) reduces to a relatively simple product of single-electron probability amplitudes in the widely used independent electron approximation limit, where the correlation effects of the Coulomb interactions between the atomic electrons disappear. As an example in which a (b ⃗) has an explicit dependence on b ⃗, we consider transversely finite vortex beams of twisted photons that lack the translational invariance of infinite plane-wave beams. Relatively simple calculations, illustrating the b ⃗ dependence in transition probabilities for photon beams interacting with a two-state degenerate single-electron atomic target, are included. Further application for many-electron systems is discussed. Possible practical uses are briefly considered.

  17. Proton-coupled electron transfer dynamics in the catalytic mechanism of a [NiFe]-hydrogenase.

    Science.gov (United States)

    Greene, Brandon L; Wu, Chang-Hao; McTernan, Patrick M; Adams, Michael W W; Dyer, R Brian

    2015-04-08

    The movement of protons and electrons is common to the synthesis of all chemical fuels such as H2. Hydrogenases, which catalyze the reversible reduction of protons, necessitate transport and reactivity between protons and electrons, but a detailed mechanism has thus far been elusive. Here, we use a phototriggered chemical potential jump method to rapidly initiate the proton reduction activity of a [NiFe] hydrogenase. Coupling the photochemical initiation approach to nanosecond transient infrared and visible absorbance spectroscopy afforded direct observation of interfacial electron transfer and active site chemistry. Tuning of intramolecular proton transport by pH and isotopic substitution revealed distinct concerted and stepwise proton-coupled electron transfer mechanisms in catalysis. The observed heterogeneity in the two sequential proton-associated reduction processes suggests a highly engineered protein environment modulating catalysis and implicates three new reaction intermediates; Nia-I, Nia-D, and Nia-SR(-). The results establish an elementary mechanistic understanding of catalysis in a [NiFe] hydrogenase with implications in enzymatic proton-coupled electron transfer and biomimetic catalyst design.

  18. Width dependent collisionless electron dynamics in the static fields of the shock ramp, 1, Single particle behavior and implications for downstream distribution

    Directory of Open Access Journals (Sweden)

    M. Gedalin

    1997-01-01

    Full Text Available We study the collisionless dynamics of electrons in the shock ramp using the numerical trajectory analysis in the model electric and magnetic fields of the shock. Even with very modest assumptions about the cross-shock potential the electron trajectories are very sensitive to the width of the ramp. The character of electron motion changes from the fully adiabatic (with conservation of v2  /B when the ramp is wide, to the nonadiabatic one, when the ramp becomes sufficiently narrow. The downstream electron distribution also changes drastically, although this change depends on the initial electron temperature.

  19. Ultrafast Relaxation Dynamics of Photoexcited Heme Model Compounds: Observation of Multiple Electronic Spin States and Vibrational Cooling.

    Science.gov (United States)

    Govind, Chinju; Karunakaran, Venugopal

    2017-04-13

    Hemin is a unique model compound of heme proteins carrying out variable biological functions. Here, the excited state relaxation dynamics of heme model compounds in the ferric form are systematically investigated by changing the axial ligand (Cl/Br), the peripheral substituent (vinyl/ethyl-meso), and the solvent (methanol/DMSO) using femtosecond pump-probe spectroscopy upon excitation at 380 nm. The relaxation time constants of these model compounds are obtained by global analysis. Excited state deactivation pathway of the model compounds comprising the decay of the porphyrin excited state (S*) to ligand to metal charge transfer state (LMCT, τ 1 ), back electron transfer from metal to ligand (MLCT, τ 2 ), and relaxation to the ground state through different electronic spin states of iron (τ 3 and τ 4 ) are proposed along with the vibrational cooling processes. This is based on the excited state absorption spectral evolution, similarities between the transient absorption spectra of the ferric form and steady state absorption spectra of the low-spin ferrous form, and the data analysis. The observation of an increase of all the relaxation time constants in DMSO compared to the methanol reflects the stabilization of intermediate states involved in the electronic relaxation. The transient absorption spectra of met-myoglobin are also measured for comparison. Thus, the transient absorption spectra of these model compounds reveal the involvement of multiple iron spin states in the electronic relaxation dynamics, which could be an alternative pathway to the ground state beside the vibrational cooling processes and associated with the inherent features of the heme b type.

  20. Nonadiabatic dynamics of electron transfer in solution: explicit and implicit solvent treatments that include multiple relaxation time scales.

    Science.gov (United States)

    Schwerdtfeger, Christine A; Soudackov, Alexander V; Hammes-Schiffer, Sharon

    2014-01-21

    The development of efficient theoretical methods for describing electron transfer (ET) reactions in condensed phases is important for a variety of chemical and biological applications. Previously, dynamical dielectric continuum theory was used to derive Langevin equations for a single collective solvent coordinate describing ET in a polar solvent. In this theory, the parameters are directly related to the physical properties of the system and can be determined from experimental data or explicit molecular dynamics simulations. Herein, we combine these Langevin equations with surface hopping nonadiabatic dynamics methods to calculate the rate constants for thermal ET reactions in polar solvents for a wide range of electronic couplings and reaction free energies. Comparison of explicit and implicit solvent calculations illustrates that the mapping from explicit to implicit solvent models is valid even for solvents exhibiting complex relaxation behavior with multiple relaxation time scales and a short-time inertial response. The rate constants calculated for implicit solvent models with a single solvent relaxation time scale corresponding to water, acetonitrile, and methanol agree well with analytical theories in the Golden rule and solvent-controlled regimes, as well as in the intermediate regime. The implicit solvent models with two relaxation time scales are in qualitative agreement with the analytical theories but quantitatively overestimate the rate constants compared to these theories. Analysis of these simulations elucidates the importance of multiple relaxation time scales and the inertial component of the solvent response, as well as potential shortcomings of the analytical theories based on single time scale solvent relaxation models. This implicit solvent approach will enable the simulation of a wide range of ET reactions via the stochastic dynamics of a single collective solvent coordinate with parameters that are relevant to experimentally accessible

  1. High-speed multiframe dynamic transmission electron microscope image acquisition system with arbitrary timing

    Energy Technology Data Exchange (ETDEWEB)

    Reed, Bryan W.; DeHope, William J.; Huete, Glenn; LaGrange, Thomas B.; Shuttlesworth, Richard M.

    2015-10-20

    An electron microscope is disclosed which has a laser-driven photocathode and an arbitrary waveform generator (AWG) laser system ("laser"). The laser produces a train of temporally-shaped laser pulses of a predefined pulse duration and waveform, and directs the laser pulses to the laser-driven photocathode to produce a train of electron pulses. An image sensor is used along with a deflector subsystem. The deflector subsystem is arranged downstream of the target but upstream of the image sensor, and has two pairs of plates arranged perpendicular to one another. A control system controls the laser and a plurality of switching components synchronized with the laser, to independently control excitation of each one of the deflector plates. This allows each electron pulse to be directed to a different portion of the image sensor, as well as to be provided with an independently set duration and independently set inter-pulse spacings.

  2. High-speed multiframe dynamic transmission electron microscope image acquisition system with arbitrary timing

    Science.gov (United States)

    Reed, Bryan W.; Dehope, William J; Huete, Glenn; LaGrange, Thomas B.; Shuttlesworth, Richard M

    2016-06-21

    An electron microscope is disclosed which has a laser-driven photocathode and an arbitrary waveform generator (AWG) laser system ("laser"). The laser produces a train of temporally-shaped laser pulses of a predefined pulse duration and waveform, and directs the laser pulses to the laser-driven photocathode to produce a train of electron pulses. An image sensor is used along with a deflector subsystem. The deflector subsystem is arranged downstream of the target but upstream of the image sensor, and has two pairs of plates arranged perpendicular to one another. A control system controls the laser and a plurality of switching components synchronized with the laser, to independently control excitation of each one of the deflector plates. This allows each electron pulse to be directed to a different portion of the image sensor, as well as to be provided with an independently set duration and independently set inter-pulse spacings.

  3. High-speed multi-frame dynamic transmission electron microscope image acquisition system with arbitrary timing

    Energy Technology Data Exchange (ETDEWEB)

    Reed, Bryan W.; DeHope, William J.; Huete, Glenn; LaGrange, Thomas B.; Shuttlesworth, Richard M.

    2016-02-23

    An electron microscope is disclosed which has a laser-driven photocathode and an arbitrary waveform generator (AWG) laser system ("laser"). The laser produces a train of temporally-shaped laser pulses each being of a programmable pulse duration, and directs the laser pulses to the laser-driven photocathode to produce a train of electron pulses. An image sensor is used along with a deflector subsystem. The deflector subsystem is arranged downstream of the target but upstream of the image sensor, and has a plurality of plates. A control system having a digital sequencer controls the laser and a plurality of switching components, synchronized with the laser, to independently control excitation of each one of the deflector plates. This allows each electron pulse to be directed to a different portion of the image sensor, as well as to enable programmable pulse durations and programmable inter-pulse spacings.

  4. LASER-driven fast electron dynamics in gaseous media under the influence of large electric fields

    Science.gov (United States)

    Batani, D.; Baton, S. D.; Manclossi, M.; Piazza, D.; Koenig, M.; Benuzzi-Mounaix, A.; Popescu, H.; Rousseaux, C.; Borghesi, M.; Cecchetti, C.; Schiavi, A.

    2009-03-01

    We present the results of experiments performed at the LULI laboratory, using the 100 TW laser facility, on the study of the propagation of fast electrons in gas targets. The implemented diagnostics included chirped shadowgraphy and proton imaging. Proton images showed the presence of very large fields in the gas (produced by charge separation). In turn, these imply a strong inhibition of propagation, and a slowing down of the fast electron cloud as it penetrates in the gas. Indeed chirped shadowgraphy images show a reduction in time of the velocity of the electron cloud from the initial value, of the order of a fraction of c, over a time scale of a few picoseconds.

  5. Electron dynamics and plasma jet formation in a helium atmospheric pressure dielectric barrier discharge jet

    Energy Technology Data Exchange (ETDEWEB)

    Algwari, Q. Th. [Centre for Plasma Physics, School of Maths and Physics, Queen' s University Belfast, University Road, Belfast, Northern Ireland BT7 1NN (United Kingdom); Electronic Department, College of Electronics Engineering, Mosul University, Mosul 41002 (Iraq); O' Connell, D. [Centre for Plasma Physics, School of Maths and Physics, Queen' s University Belfast, University Road, Belfast, Northern Ireland BT7 1NN (United Kingdom); York Plasma Institute, Department of Physics, University of York, York YO10 5DD (United Kingdom)

    2011-09-19

    The excitation dynamics within the main plasma production region and the plasma jets of a kHz atmospheric pressure dielectric barrier discharge (DBD) jet operated in helium was investigated. Within the dielectric tube, the plasma ignites as a streamer-type discharge. Plasma jets are emitted from both the powered and grounded electrode end; their dynamics are compared and contrasted. Ignition of these jets are quite different; the jet emitted from the powered electrode is ignited with a slight time delay to plasma ignition inside the dielectric tube, while breakdown of the jet at the grounded electrode end is from charging of the dielectric and is therefore dependent on plasma production and transport within the dielectric tube. Present streamer theories can explain these dynamics.

  6. The VENUS/NWChem Software Package. Tight Coupling Between Chemical Dynamics Simulations and Electronic Structure Theory

    Energy Technology Data Exchange (ETDEWEB)

    Lourderaj, Upakarasamy; Sun, Rui; De Jong, Wibe A.; Windus, Theresa L.; Hase, William L.

    2014-03-01

    The interface for VENUS and NWChem, and the resulting software package for direct dynamics simulations are described. The coupling of the two codes is considered to be a tight coupling. The two codes are compiled and linked together and act as one executable with data being passed between the two codes through routine calls. The advantages of this type of coupling are discussed. The interface has been designed to have as little interference as possible with the core codes of both VENUS and NWChem. VENUS is the code that propagates the direct dynamics trajectories and, therefore, is the program that drives the overall execution of VENUS/NWChem. VENUS has remained an essentially sequential code, which uses the highly parallel structure of NWChem. Subroutines of the interface which accomplish the data transmission and communication between the two computer programs are described. Recent examples of the use of VENUS/NWChem for direct dynamics simulations are summarized.

  7. Ultrafast electron diffraction optimized for studying structural dynamics in thin films and monolayers

    Directory of Open Access Journals (Sweden)

    D. S. Badali

    2016-05-01

    Full Text Available A compact electron source specifically designed for time-resolved diffraction studies of free-standing thin films and monolayers is presented here. The sensitivity to thin samples is achieved by extending the established technique of ultrafast electron diffraction to the “medium” energy regime (1–10 kV. An extremely compact design, in combination with low bunch charges, allows for high quality diffraction in a lensless geometry. The measured and simulated characteristics of the experimental system reveal sub-picosecond temporal resolution, while demonstrating the ability to produce high quality diffraction patterns from atomically thin samples.

  8. Critical Electron-Paramagnetic-Resonance Spin Dynamics in NiCl2

    DEFF Research Database (Denmark)

    Birgeneau, R.J.; Rupp, L.W.; Guggenheim, H.J.

    1973-01-01

    We have studied the critical behavior of the electron-paramagnetic-resonance linewidth in the planar XY antiferromagnet NiCl2; it is found that the linewidth diverges like ξ∼(T-TN)-0.7 rather than ξ5/2 predicted by the current random-phase-approximation theory.......We have studied the critical behavior of the electron-paramagnetic-resonance linewidth in the planar XY antiferromagnet NiCl2; it is found that the linewidth diverges like ξ∼(T-TN)-0.7 rather than ξ5/2 predicted by the current random-phase-approximation theory....

  9. Electron spin dynamics in heavily Mn-doped (Ga,Mn)As

    Science.gov (United States)

    Zhu, Yonggang; Han, Lifen; Chen, Lin; Zhang, Xinhui; Zhao, Jianhua

    2010-12-01

    Electron spin relaxation and related mechanisms in heavily Mn-doped (Ga,Mn)As are studied by performing time-resolved magneto-optical Kerr effect measurements. At low temperature, s-d exchange scattering dominates electron spin relaxation, whereas the Bir-Aronov-Pikus mechanism and Mn impurity scattering play important roles at high temperature. The temperature-dependent spin relaxation time exhibits an anomaly around the Curie temperature (Tc) that implies that thermal fluctuation is suppressed by short-range correlated spin fluctuation above Tc.

  10. Electrons as probes of dynamics in molecules and clusters: A contribution from Time Dependent Density Functional Theory

    Science.gov (United States)

    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

  11. Structural dynamics of gas-phase molybdenum nanoclusters : A transmission electron microscopy study

    NARCIS (Netherlands)

    Vystavel, T; Koch, SA; Palasantzas, G; De Hosson, JTM

    2005-01-01

    In this paper we study structural aspects of molybdenum clusters by transmission electron microscopy. The deposited clusters with sizes 4 nm or larger show a body-centered crystal (bcc) structure. The clusters are self-assembled from smaller structural units and form cuboids with a typical size of 4

  12. Electronic structures and population dynamics of excited states of xanthione and its derivatives

    Science.gov (United States)

    Fedunov, Roman G.; Rogozina, Marina V.; Khokhlova, Svetlana S.; Ivanov, Anatoly I.; Tikhomirov, Sergei A.; Bondarev, Stanislav L.; Raichenok, Tamara F.; Buganov, Oleg V.; Olkhovik, Vyacheslav K.; Vasilevskii, Dmitrii A.

    2017-09-01

    A new compound, 1,3-dimethoxy xanthione (DXT), has been synthesized and its absorption (stationary and transient) and luminescence spectra have been measured in n-hexane and compared with xanthione (XT) spectra. The pronounced broadening of xanthione vibronic absorption band related to the electronic transition to the second singlet excited state has been observed. Distinctions between the spectra of xanthione and its methoxy derivatives are discussed. Quantum chemical calculations of these compounds in the ground and excited electronic states have been accomplished to clarify the nature of electronic spectra changes due to modification of xanthione by methoxy groups. Appearance of a new absorption band of DXT caused by symmetry changes has been discussed. Calculations of the second excited state structure of xanthione and its methoxy derivatives confirm noticeable charge transfer (about 0.1 of the charge of an electron) from the methoxy group to thiocarbonyl group. Fitting of the transient spectra of XT and DXT has been fulfilled and the time constants of internal conversion S2 →S1 and intersystem crossing S1 →T1 have been determined. A considerable difference between the time constants of internal conversion S2 →S1 in XT and DXT is uncovered.

  13. Electronic Bottleneck and Coherent Vibrational Effect on Relaxation Dynamics of Photoexcited Ions in Crystals

    National Research Council Canada - National Science Library

    Alfano, R. R

    2000-01-01

    .... The nonequilibrium population of a local mode of 765 cm(sup -1) in Cr(sup 4+):Mg2SiO4 was found to build up during the transition through an electronic bottleneck and decay by interaction with a restricted number of phonon modes...

  14. Annealing effect on the electron spin dynamics in heavily Mn-doped (Ga,Mn)As

    Energy Technology Data Exchange (ETDEWEB)

    Yue, Han; Chen, Lin; Gao, Haixia; Zhao, Jianhua; Zhang, Xinhui [Institute of Semiconductors, Chinese Academy of Sciences, Beijing (China)

    2014-05-15

    A temperature- and photo-excitation-density-dependent electron spin dephasing process has been studied by time-resolved magneto-optical Kerr effect (TR-MOKE) measurements for heavily-doped (Ga,Mn)As after appropriate annealing treatment. Unlike the as-grown (Ga,Mn)As in which s-d scattering is dominant for spin dephasing at low temperature, the exchange scattering induced by Mn ions is efficiently suppressed after annealing. For annealed (Ga,Mn)As, the p-d exchange coupling proves to be important for the electron spin dephasing process. Moreover, the Coulomb scattering arising from the weakly-localized holes and Mn impurities is revealed to play an important role in the electron spin dephasing after annealing. Our results demonstrate that the impurity induced disorder plays a significant role in the electron spin-dephasing process in (Ga,Mn)As when Mn is over doped by as much as 15%, which is a critical issue that needs to be considered to achieve high-quality (Ga,Mn)As thin films with a higher Curie temperature T{sub C} and better functionality.

  15. Modeling Radiation Belt Electron Dynamics with the DREAM3D Diffusion Model

    Energy Technology Data Exchange (ETDEWEB)

    Tu, Weichao [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Cunningham, Gregory S. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Chen, Yue [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Henderson, Michael G. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Morley, Steven K. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Reeves, Geoffrey D. [Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Blake, Bernard J. [The Aerospace Corporation, El Segundo, CA (United States); Baker, Daniel N. [Lab. for Atmospheric and Space Physics, Boulder, CO (United States); Spence, Harlan [Univ. of New Hampshire, Durham, NH (United States)

    2014-02-14

    The simulation results from our 3D diffusion model on the CRRES era suggest; our model captures the general variations of radiation belt electrons, including the dropouts and the enhancements; the overestimations inside the plasmapause can be improved by increasing the PA diffusion from hiss waves; and that better DLL and wave models are required.

  16. Electron paramagnetic resonance and dynamic nuclear polarization of char suspensions: surface science and oximetry

    DEFF Research Database (Denmark)

    Clarkson, R B; Odintsov, B M; Ceroke, P J

    1998-01-01

    Carbon chars have been synthesized in our laboratory from a variety of starting materials, by means of a highly controlled pyrolysis technique. These chars exhibit electron paramagnetic resonance (EPR) line shapes which change with the local oxygen concentration in a reproducible and stable fashion...

  17. Time-resolved microplasma electron dynamics in a pulsed microwave discharge

    Science.gov (United States)

    Monfared, S. K.; Hoskinson, A. R.; Hopwood, J.

    2013-10-01

    Microwave-driven microplasmas are typically operated in a steady-state mode in which the electron temperature is constant in time. Transient measurements of excitation temperature and helium emission lines, however, suggest that short microwave pulses can be used to increase the electron energy by 20-30%. Time-resolved optical emission spectrometry reveals an initial burst of light emission from the igniting microplasma. This emission overshoot is also correlated with a measured increase in excitation temperature. Excimer emission lags atomic emission, however, and does not overshoot. A simple model shows that an increase in electron temperature is responsible for the overshoot of atomic optical emission at the beginning of each microwave pulse. The formation of dimers and subsequent excimer emission requires slower three-body collisions with the excited rare gas atoms, which is why excimer emission does not overshoot the steady-state values. Similar results are observed in argon gas. The overshoot in electron temperature may be used to manipulate the collisional production of species in microplasmas using short, low-duty cycle microwave pulses.

  18. Approaches to structure and dynamics of biological systems by electron-paramagnetic-resonance spectroscopy

    NARCIS (Netherlands)

    Scarpelli, Francesco

    2009-01-01

    Proteins and enzymes play a key role in all biological systems. Understanding the mechanism of biological functions and reactions in which proteins and enzymes are involved requires a detailed characterization of protein structure and dynamics. Structure refers to geometrical structure, as a result

  19. The Primary Care Electronic Library: RSS feeds using SNOMED-CT indexing for dynamic content delivery

    Directory of Open Access Journals (Sweden)

    Judas Robinson

    2006-12-01

    Conclusion The results of the pilot illustrate that it is possible to exchange data between servers using RSS syndication. This method could be utilised dynamically to supply digital library resources to a clinical system with SNOMED-CTdata used as the standard of reference.

  20. On the importance of excited state dynamic response electron correlation in polarizable embedding methods

    DEFF Research Database (Denmark)

    Eriksen, Janus J.; Sauer, Stephan P. A.; Mikkelsen, Kurt Valentin

    2012-01-01

    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 (SCF) level within the Polarizable Embedding (PE) formalism. We formulate HF based PE within the linear response theory...

  1. Toward Highlighting the Ultrafast Electron Transfer Dynamics at the Optically Dark Sites of Photocatalysts

    DEFF Research Database (Denmark)

    Canton, Sophie E.; Zhang, Xiaoyi; Zhang, Jianxin

    2013-01-01

    Building a detailed understanding of the structure–function relationship is a crucial step in the optimization of molecular photocatalysts employed in water splitting schemes. The optically dark nature of their active sites usually prevents a complete mapping of the photoinduced dynamics. In this...

  2. The effects of different substrates on the electron stimulated desorption dynamics of O - from physisorbed O2

    Science.gov (United States)

    Hedhili, M. N.; Parenteau, L.; Huels, M. A.; Azria, R.; Tronc, M.; Sanche, L.

    1997-11-01

    We report condensed phase measurements of kinetic energy (Ek) distributions of O-, produced by dissociative electron attachment (DEA) at 6 eV incident electron energy; they are obtained under identical experimental conditions from submonolayer quantities of 16O2 deposited on disordered multilayer substrates of 18O2, Ar, Kr, Xe, CH4, and C2H6, all condensed at 20 K on polycrystalline platinum (Pt). The results suggest that the desorption dynamics of O- DEA fragments is, in part, determined by large angle elastic scattering of O- prior to desorption, as well as the net image charge potential (Ep) induced in the condensed dielectric solid and the Pt metal. The measurements also indicate that, particularly at small Kr substrate thicknesses, the Ep may not necessarily be uniform across the surface, but may fluctuate due to surface roughness. Thus, in addition to energy losses in the substrate prior to, and during, DEA, these effects may influence the dissociation dynamics of the O2- resonance itself, as well as the desorption of the DEA O- fragment.

  3. Statistics and kinetics of single-molecule electron transfer dynamics in complex environments: a simulation model study.

    Science.gov (United States)

    Paula, Luciana C; Wang, Jin; Leite, Vitor B P

    2008-12-14

    Dynamics of the environments of complex systems such as biomolecules, polar solvents, and glass plays an important role in controlling electron transfer reactions. The kinetics is determined by the nature of a complex multidimensional landscape. By quantifying the mean and high-order statistics of the first-passage time and the associated ratios, the dynamics in electron transfer reactions controlled by the environments can be revealed. We consider real experimental conditions with finite observation time windows. At high temperatures, exponential kinetics is observed and there are multiple kinetic paths leading to the product state. At and below an intermediate temperature, nonexponential kinetics starts to appear, revealing the nature of the distribution of local traps on the landscape. Discrete kinetic paths emerge. At very low temperatures, nonexponential kinetics continues to be observed. We point out that the size of the observational time window is crucial in revealing the intrinsic nature of the real kinetics. The mean first-passage time is defined as a characteristic time. Only when the observational time window is significantly larger than this characteristic time does one have the opportunity to collect enough statistics to capture rare statistical fluctuations and characterize the kinetics accurately.

  4. Spin dynamics in high-mobility two-dimensional electron systems embedded in GaAs/AlGaAs quantum wells

    Energy Technology Data Exchange (ETDEWEB)

    Griesbeck, Michael

    2012-11-22

    Since many years there has been great effort to explore the spin dynamics in low-dimensional electron systems embedded in GaAs/AlGaAs based heterostructures for the purpose of quantum computation and spintronics applications. Advances in technology allow for the design of high quality and well-defined two-dimensional electron systems (2DES), which are perfectly suited for the study of the underlying physics that govern the dynamics of the electron spin system. In this work, spin dynamics in high-mobility 2DES is studied by means of the all-optical time-resolved Kerr/Faraday rotation technique. In (001)-grown 2DES, a strong in-plane spin dephasing anisotropy is studied, resulting from the interference of comparable Rashba and Dresselhaus contributions to the spin-orbit field (SOF). The dependence of this anisotropy on parameters like the confinement length of the 2DES, the sample temperature, as well as the electron density is demonstrated. Furthermore, coherent spin dynamics of an ensemble of ballistically moving electrons is studied without and within an applied weak magnetic field perpendicular to the sample plane, which forces the electrons to move on cyclotron orbits. Finally, strongly anisotropic spin dynamics is investigated in symmetric (110)-grown 2DES, using the resonant spin amplification method. Here, extremely long out-of-plane spin dephasing times can be achieved, in consequence of the special symmetry of the Dresselhaus SOF.

  5. Von Neumann entropy in a Rashba-Dresselhaus nanodot; dynamical electronic spin-orbit entanglement

    Science.gov (United States)

    Safaiee, Rosa; Golshan, Mohammad Mehdi

    2017-06-01

    The main purpose of the present article is to report the characteristics of von Neumann entropy, thereby, the electronic hybrid entanglement, in the heterojunction of two semiconductors, with due attention to the Rashba and Dresselhaus spin-orbit interactions. To this end, we cast the von Neumann entropy in terms of spin polarization and compute its time evolution; with a vast span of applications. It is assumed that gate potentials are applied to the heterojunction, providing a two dimensional parabolic confining potential (forming an isotropic nanodot at the junction), as well as means of controlling the spin-orbit couplings. The spin degeneracy is also removed, even at electronic zero momentum, by the presence of an external magnetic field which, in turn, leads to the appearance of Landau states. We then proceed by computing the time evolution of the corresponding von Neumann entropy from a separable (spin-polarized) initial state. The von Neumann entropy, as we show, indicates that electronic hybrid entanglement does occur between spin and two-dimensional Landau levels. Our results also show that von Neumann entropy, as well as the degree of spin-orbit entanglement, periodically collapses and revives. The characteristics of such behavior; period, amplitude, etc., are shown to be determined from the controllable external agents. Moreover, it is demonstrated that the phenomenon of collapse-revivals' in the behavior of von Neumann entropy, equivalently, electronic hybrid entanglement, is accompanied by plateaus (of great importance in quantum computation schemes) whose durations are, again, controlled by the external elements. Along these lines, we also make a comparison between effects of the two spin-orbit couplings on the entanglement (von Neumann entropy) characteristics. The finer details of the electronic hybrid entanglement, which may be easily verified through spin polarization measurements, are also accreted and discussed. The novel results of the present

  6. Decay of MHD-scale Kelvin-Helmholtz vortices mediated by parasitic electron dynamics.

    Science.gov (United States)

    Nakamura, T K M; Hayashi, D; Fujimoto, M; Shinohara, I

    2004-04-09

    We have simulated nonlinear development of MHD-scale Kelvin-Helmholtz (KH) vortices by a two-dimensional two-fluid system including finite electron inertial effects. In the presence of moderate density jump across a shear layer, in striking contrast to MHD results, MHD KH vortices are found to decay by the time one eddy turnover is completed. The decay is mediated by smaller vortices that appear within the parent vortex and stays effective even when the shear layer width is made larger. It is shown that the smaller vortices are basically of MHD nature while the seeding for these is achieved by the electron inertial effect. Application of the results to the magnetotail boundary layer is discussed.

  7. Hall-Driven Effects in Electron-Magnetohydro- dynamic Z-Pinch-Like Implosions

    Science.gov (United States)

    Richardson, A. S.; Swanekamp, S. B.; Schumer, J. W.; Mosher, D.; Ottinger, P. F.

    2017-10-01

    In previous work, it has been shown that density gradients give rise to Hall-driven magnetic field penetration in electron-magnetohydrodynamics (EMHD). Here, we examine the effect of geometry on this Hall-driven penetration. It is found that in z-pinch-like geometries, the implosion velocity of a Hall-driven magnetic pinch depends on its distance from the axis, moving faster as it approaches the axis. We compare analytical and numerical results for the z-pinch geometry to previous results for a rectangular slab geometry. Similar effects are found in both geometries, including electron-inertia driven nonlinearities, a Kelvin-Helmoltz like instability, and the generation of vortices. The electric field in the vortices is also examined, to determine how much charge separation occurs. If the electric field becomes large enough, it could accelerate the background ions to very high energies. This work was supported by the Naval Research Laboratory Base Program.

  8. Dynamic flexibility in the light reactions of photosynthesis governed by both electron and proton transfer reactions.

    Science.gov (United States)

    Kramer, David M; Avenson, Thomas J; Edwards, Gerald E

    2004-07-01

    Plant photosynthesis performs the remarkable feat of converting light energy into usable chemical forms, which involves taming highly reactive intermediates without harming plant cells. This requires an apparatus that is not only efficient and robust but also flexible in its responses to changing environmental conditions. It also requires that the output of the energy-storing reactions be matched with the demands of metabolism. This article addresses the mechanisms by which this flexibility is achieved for short-term environmental changes. We argue that chloroplasts need two types of flexible mechanisms: one for modulating the output ratio of ATP:NADPH, which involves cyclic electron flux around photosystem I; and another for changing the regulatory sensitivity of the light-harvesting antenna to electron (and proton) flow.

  9. Multi-channel electronic and vibrational dynamics in polyatomic resonant high-order harmonic generation

    Science.gov (United States)

    Ferré, A.; Boguslavskiy, A. E.; Dagan, M.; Blanchet, V.; Bruner, B. D.; Burgy, F.; Camper, A.; Descamps, D.; Fabre, B.; Fedorov, N.; Gaudin, J.; Geoffroy, G.; Mikosch, J.; Patchkovskii, S.; Petit, S.; Ruchon, T.; Soifer, H.; Staedter, D.; Wilkinson, I.; Stolow, A.; Dudovich, N.; Mairesse, Y.

    2015-01-01

    High-order harmonic generation in polyatomic molecules generally involves multiple channels of ionization. Their relative contribution can be strongly influenced by the presence of resonances, whose assignment remains a major challenge for high-harmonic spectroscopy. Here we present a multi-modal approach for the investigation of unaligned polyatomic molecules, using SF6 as an example. We combine methods from extreme-ultraviolet spectroscopy, above-threshold ionization and attosecond metrology. Fragment-resolved above-threshold ionization measurements reveal that strong-field ionization opens at least three channels. A shape resonance in one of them is found to dominate the signal in the 20–26 eV range. This resonance induces a phase jump in the harmonic emission, a switch in the polarization state and different dynamical responses to molecular vibrations. This study demonstrates a method for extending high-harmonic spectroscopy to polyatomic molecules, where complex attosecond dynamics are expected. PMID:25608712

  10. Matrix photochemistry of small molecules: Influencing reaction dynamics on electronically excited hypersurfaces

    Energy Technology Data Exchange (ETDEWEB)

    Laursen, S.L.

    1990-01-01

    Investigations of chemical reactions on electronically excited reaction surfaces are presented. The role of excited-surface multiplicity is of particular interest, as are chemical reactivity and energy transfer in systems in which photochemistry is initiated through a metal atom sensitizer.'' Two approaches are employed: A heavy-atom matrix affords access to forbidden triplet reaction surfaces, eliminating the need for a potentially reactive sensitizer. Later, the role of the metal atom in the photosensitization process is examined directly.

  11. What Institutional Dynamics Guide Waste Electrical and Electronic Equipment Refurbishment and Reuse in Urban China?

    OpenAIRE

    Steuer, Benjamin

    2016-01-01

    For over two decades China has faced a veritable e-waste challenge due to the continuous increase in quantities of Waste Electrical and Electronic Equipment (WEEE) coming from foreign and domestic sources. Over more than a decade, the government’s response has been focussed on developing large-scale recycling facilities so as to recover the valuable materials within WEEE. Simultaneously, China is home to a vast, informal segment, which engages in the collection, refurbishment, and processing ...

  12. Applications and limitations of electron correlation microscopy to study relaxation dynamics in supercooled liquids

    Energy Technology Data Exchange (ETDEWEB)

    Zhang, Pei; He, Li [Department of Materials Science and Engineering, University of Wisconsin-Madison, Madison, WI 53706 (United States); Besser, Matthew F. [Materials Science and Engineering, Ames Laboratory, Iowa State University, Ames, IA 50011 (United States); Liu, Ze; Schroers, Jan [Department of Mechanical Engineering and Materials Science, Yale University, New Haven, CT 06511 (United States); Kramer, Matthew J. [Materials Science and Engineering, Ames Laboratory, Iowa State University, Ames, IA 50011 (United States); Voyles, Paul M., E-mail: paul.voyles@wisc.edu [Department of Materials Science and Engineering, University of Wisconsin-Madison, Madison, WI 53706 (United States)

    2017-07-15

    Electron correlation microscopy (ECM) is a way to measure structural relaxation times, τ, of liquids with nanometer-scale spatial resolution using coherent electron scattering equivalent of photon correlation spectroscopy. We have applied ECM with a 3.5 nm diameter probe to Pt{sub 57.5}Cu{sub 14.7}Ni{sub 5.3}P{sub 22.5} amorphous nanorods and Pd{sub 40}Ni{sub 40}P{sub 20} bulk metallic glass (BMG) heated inside the STEM into the supercooled liquid region. These data demonstrate that the ECM technique is limited by the characteristics of the time series, which must be at least 40τ to obtain a well-converged correlation function g{sub 2}(t), and the time per frame, which must be less than 0.1τ to obtain sufficient sampling. A high-speed direct electron camera enables fast acquisition and affords reliable g{sub 2}(t) data even with low signal per frame. - Highlights: • Electron Correlation Microscopy (ECM) technique was applied to measure structural relaxation times of supercooled liquids in metallic glass. • In Pt{sub 57.5}Cu{sub 14.7}Ni{sub 5.3}P{sub 22.5} nanowire, τ and β decreases over the measured supercooled liquid regime. • In Pd{sub 40}Ni{sub 40}P{sub 20} bulk alloy, τ decreases from T{sub g}+28 °C to T{sub g}+48 °C, then increases as the temperature approaches T{sub x}. • ECM experiment requires a length of time series at least 40 times the characteristic relaxation time and a time per diffraction pattern at most 0.1 times the relaxation time.

  13. Electron Dynamics During High-Power, Short-Pulsed Laser Interactions with Solids and Interfaces

    Science.gov (United States)

    2016-06-28

    phonon thermal conductivity of ferroelectric solids. The electric fields changed the ferroelastic domain states, which varied the phonon scattering rates...Adamo, C., Ye, L., Huey, B., Lee, S., Schlom, D.G., “Strain field and coherent domain wall effects on thermal conductivity and Kapitza conductance...temperature in bilayer and strain-released PZT thin films via modulation of the domain structure using applied electric fields ,” Electronic Materials

  14. Structure of the channeling electrons wave functions under dynamical chaos conditions

    Energy Technology Data Exchange (ETDEWEB)

    Shul’ga, N.F. [National Science Center “Kharkov Institute of Physics and Technology”, 1, Akademicheskaya St., Kharkov 61108 (Ukraine); V.N. Karazin National University, 4, Svodody Sq., Kharkov 61022 (Ukraine); Syshchenko, V.V., E-mail: syshch@yandex.ru [Belgorod National Research University, 85, Pobedy St., Belgorod 308015 (Russian Federation); Tarnovsky, A.I. [Belgorod National Research University, 85, Pobedy St., Belgorod 308015 (Russian Federation); Isupov, A.Yu. [Laboratory of High Energy Physics, Joint Institute for Nuclear Research, 141980 Dubna, Moscow region (Russian Federation)

    2016-03-01

    The stationary wave functions of fast electrons axially channeling in the silicon crystal near [1 1 0] direction have been found numerically for integrable and non-integrable cases, for which the classical motion is regular and chaotic, respectively. The nodal structure of the wave functions in the quasi-classical region, where the energy levels density is high, is agreed with quantum chaos theory predictions.

  15. Solving the Accelerator-Condenser Coupling Problem in a Nanosecond Dynamic Transmission Electron Microscope

    Energy Technology Data Exchange (ETDEWEB)

    Reed, B W; LaGrange, T; Shuttlesworth, R M; Gibson, D J; Campbell, G H; Browning, N D

    2009-12-29

    We describe a modification to a transmission electron microscope (TEM) that allows it to briefly (using a pulsed-laser-driven photocathode) operate at currents in excess of 10 mA while keeping the effects of condenser lens aberrations to a minimum. This modification allows real-space imaging of material microstructure with a resolution of order 10 nm over regions several {micro}m across with an exposure time of 15 ns. This is more than 6 orders of magnitude faster than typical video-rate TEM imaging. The key is the addition of a weak magnetic lens to couple the large-diameter high-current beam exiting the accelerator into the acceptance aperture of a conventional TEM condenser lens system. We show that the performance of the system is essentially consistent with models derived from ray tracing and finite element simulations. The instrument can also be operated as a conventional TEM by using the electron gun in a thermionic mode. The modification enables very high electron current densities in {micro}m-sized areas and could also be used in a non-pulsed system for high-throughput imaging and analytical TEM.

  16. Ultrafast electron, lattice and spin dynamics on rare earth metal surfaces. Investigated with linear and nonlinear optical techniques

    Energy Technology Data Exchange (ETDEWEB)

    Radu, I.E.

    2006-03-15

    This thesis presents the femtosecond laser-induced electron, lattice and spin dynamics on two representative rare-earth systems: The ferromagnetic gadolinium Gd(0001) and the paramagnetic yttrium Y(0001) metals. The employed investigation tools are the time-resolved linear reflectivity and second-harmonic generation, which provide complementary information about the bulk and surface/interface dynamics, respectively. The femtosecond laser excitation of the exchange-split surface state of Gd(0001) triggers simultaneously the coherent vibrational dynamics of the lattice and spin subsystems in the surface region at a frequency of 3 THz. The coherent optical phonon corresponds to the vibration of the topmost atomic layer against the underlying bulk along the normal direction to the surface. The coupling mechanism between phonons and magnons is attributed to the modulation of the exchange interaction J between neighbour atoms due to the coherent lattice vibration. This leads to an oscillatory motion of the magnetic moments having the same frequency as the lattice vibration. Thus these results reveal a new type of phonon-magnon coupling mediated by the modulation of the exchange interaction and not by the conventional spin-orbit interaction. Moreover, we show that coherent spin dynamics in the THz frequency domain is achievable, which is at least one order of magnitude faster than previously reported. The laser-induced (de)magnetization dynamics of the ferromagnetic Gd(0001) thin films have been studied. Upon photo-excitation, the nonlinear magneto-optics measurements performed in this work show a sudden drop in the spin polarization of the surface state by more than 50% in a <100 fs time interval. Under comparable experimental conditions, the time-resolved photoemission studies reveal a constant exchange splitting of the surface state. The ultrafast decrease of spin polarization can be explained by the quasi-elastic spin-flip scattering of the hot electrons among spin

  17. Photosystem II cycle activity and alternative electron transport in the diatom Phaeodactylum tricornutum under dynamic light conditions and nitrogen limitation.

    Science.gov (United States)

    Wagner, Heiko; Jakob, Torsten; Lavaud, Johann; Wilhelm, Christian

    2016-05-01

    Alternative electron sinks are an important regulatory mechanism to dissipate excessively absorbed light energy particularly under fast changing dynamic light conditions. In diatoms, the cyclic electron transport (CET) around Photosystem II (PS II) is an alternative electron transport pathway (AET) that contributes to avoidance of overexcitation under high light illumination. The combination of nitrogen limitation and high-intensity irradiance regularly occurs under natural conditions and is expected to force the imbalance between light absorption and the metabolic use of light energy. The present study demonstrates that under N limitation, the amount of AET and the activity of CETPSII in the diatom Phaeodactylum tricornutum were increased. Thereby, the activity of CETPSII was linearly correlated with the amount of AET rates. It is concluded that CETPSII significantly contributes to AET in P. tricornutum. Surprisingly, CETPSII was found to be activated already at the end of the dark period under N-limited conditions. This coincided with a significantly increased degree of reduction of the plastoquinone (PQ) pool. The analysis of the macromolecular composition of cells of P. tricornutum under N-limited conditions revealed a carbon allocation in favor of carbohydrates during the light period and their degradation during the dark phase. A possible linkage between the activity of CETPSII and degree of reduction of the PQ pool on the one side and the macromolecular changes on the other is discussed.

  18. Electron transfer dynamics of triphenylamine dyes bound to TiO2 nanoparticles from femtosecond stimulated Raman spectroscopy

    KAUST Repository

    Hoffman, David P.

    2013-04-11

    Interfacial electron transfer between sensitizers and semiconducting nanoparticles is a crucial yet poorly understood process. To address this problem, we have used transient absorption (TA) and femtosecond stimulated Raman spectroscopy (FSRS) to investigate the photoexcited dynamics of a series of triphenylamine-coumarin dye/TiO2 conjugates. The TA decay is multiexponential, spanning time scales from 100 fs to 100 ps, while the characteristic transient Raman spectrum of the radical cation decays biexponentially with a dominant ∼3 ps component. To explain these observations, we propose a model in which the decay of the TA is due to hot electrons migrating from surface trap states to the conduction band of TiO 2 while the decay of the Raman signature is due to internal conversion of the dye molecule. Furthermore, the S1 Raman spectrum of TPAC3, a dye wherein a vinyl group separates the triphenylamine and coumarin moieties, is similar to the S1 Raman spectrum of trans-stilbene; we conclude that their S1 potential energy surfaces and reactivity are also similar. This correlation suggests that dyes containing vinyl linkers undergo photoisomerization that competes with electron injection. © 2013 American Chemical Society.

  19. Photodissociation of HBr. 1. Electronic structure, photodissociation dynamics, and vector correlation coefficients.

    Science.gov (United States)

    Smolin, Andrey G; Vasyutinskii, Oleg S; Balint-Kurti, Gabriel G; Brown, Alex

    2006-04-27

    Ab initio potential energy curves, transition dipole moments, and spin-orbit coupling matrix elements are computed for HBr. These are then used, within the framework of time-dependent quantum-mechanical wave-packet calculations, to study the photodissociation dynamics of the molecule. Total and partial integral cross sections, the branching fraction for the formation of excited-state bromine atoms Br(2P(1/2)), and the lowest order anisotropy parameters, beta, for both ground and excited-state bromine are calculated as a function of photolysis energy and compared to experimental and theoretical data determined previously. Higher order anisotropy parameters are computed for the first time for HBr and compared to recent experimental measurements. A new expression for the Re[a1(3) (parallel, perpendicular)] parameter describing coherent parallel and perpendicular production of ground-state bromine in terms of the dynamical functions is given. Although good agreement is obtained between the theoretical predictions and the experimental measurements, the discrepancies are analyzed to establish how improvements might be achieved. Insight is obtained into the nonadiabatic dynamics by comparing the results of diabatic and fully adiabatic calculations.

  20. Femtosecond dynamics of electronic states in the Mott insulator 1T-TaS{sub 2} by time resolved photoelectron spectroscopy

    Energy Technology Data Exchange (ETDEWEB)

    Perfetti, L; Loukakos, P A; Lisowski, M; Bovensiepen, U; Wolf, M [Fachbereich Physik, Freie Universitaet Berlin, Arnimallee 14, 14195 Berlin (Germany); Berger, H [Institut de Physique de la Matiere Complexe, EPFL, CH-1015 Lausanne (Switzerland); Biermann, S; Georges, A [Centre de Physique Theorique, Ecole Polytechnique, 91128 Palaiseau Cedex (France)], E-mail: perfetti@physik.fu-berlin.de

    2008-05-15

    Photoexcitation of the Mott insulator 1T-TaS{sub 2} by an intense laser pulse leads to an ultrafast transition toward a gapless phase. Besides the collapse of the electronic gap, the sudden excitation of the charge density wave (CDW) mode results in periodic oscillations of the electronic states. We employ time resolved photoelectron spectroscopy to monitor the rich dynamics of electrons and phonons during the relaxation toward equilibrium. The qualitative difference between the oscillatory dynamics of the CDW and the monotonic recovery of the electronic gap proves that 1T-TaS{sub 2} is indeed a Mott insulator. Moreover the quasi-instantaneous build-up of mid gap states is in contrast with the retarded response expected from a Peierls insulating phase. Interestingly, the photoinduced electronic states in the midgap spectral region display a weak resonance that is reminiscent of a quasiparticle peak.

  1. Initial Beam Dynamics Simulations of a High-Average-Current Field-Emission Electron Source in a Superconducting RadioFrequency Gun

    Energy Technology Data Exchange (ETDEWEB)

    Mohsen, O. [Northern Illinois U.; Gonin, I. [Fermilab; Kephart, R. [Fermilab; Khabiboulline, T. [Fermilab; Piot, P. [Northern Illinois U.; Solyak, N. [Fermilab; Thangaraj, J. C. [Fermilab; Yakovlev, V. [Fermilab

    2018-01-05

    High-power electron beams are sought-after tools in support to a wide array of societal applications. This paper investigates the production of high-power electron beams by combining a high-current field-emission electron source to a superconducting radio-frequency (SRF) cavity. We especially carry out beam-dynamics simulations that demonstrate the viability of the scheme to form $\\sim$ 300 kW average-power electron beam using a 1+1/2-cell SRF gun.

  2. Experiments on current-driven three-dimensional ion sound turbulence. I - Return-current limited electron beam injection. II - Wave dynamics

    Science.gov (United States)

    Stenzel, R. L.

    1978-01-01

    Pulsed electron beam injection into a weakly collisional magnetized background plasma is investigated experimentally; properties of the electron beam and background plasma, as well as the low-frequency instabilities and wave dynamics, are discussed. The current of the injected beam closes via a field-aligned return current of background electrons. Through study of the frequency and wavenumber distribution, together with the electron distribution function, the low-frequency instabilities associated with the pulsed injection are identified as ion acoustic waves driven unstable by the return current. The frequency cut-off of the instabilities predicted from renormalized plasma turbulence theory, has been verified experimentally.

  3. Dynamic behavior of correlated electrons in the insulating doped semiconductor Si:P

    Energy Technology Data Exchange (ETDEWEB)

    Ritz, Elvira

    2009-06-04

    At low energy scales charge transport in the insulating Si:P is dominated by activated hopping between the localized donor electron states. Theoretical models for a disordered electronic system with a long-range Coulomb interaction are appropriate to interpret the electric conductivity spectra. With a novel and advanced method we perform broadband phase sensitive measurements of the reflection coefficient from 45 MHz up to 5 GHz, employing a vector network analyzer with a 2.4 mm coaxial sensor, which is terminated by the sample under test. While the material parameters (conductivity and permittivity) can be easily extracted from the obtained impedance data if the sample is metallic, no direct solution is possible if the material under investigation is an insulator. Focusing on doped semiconductors with largely varying conductivity and dielectric function, we present a closed calibration and evaluation procedure with an optimized theoretical and experimental complexity, based on the rigorous solution for the electromagnetic field inside the insulating sample, combined with the variational principle. Basically no limiting assumptions are necessary in a strictly defined parameter range. As an application of our new method, we have measured the complex broadband microwave conductivity of Si:P in a broad range of phosphorus concentration n/n{sub c} from 0.56 to 0.9 relative to the critical value n{sub c}=3.5 x 10{sup 18} cm{sup -3} of the metal-insulator transition driven by doping at temperatures down to 1.1 K, and studied unresolved issues of fundamental research concerning the electronic correlations and the metal-insulator transition. (orig.)

  4. The large-scale isolated disturbances dynamics in the main peak of electronic concentration of ionosphere

    Science.gov (United States)

    Kalinin, U. K.; Romanchuk, A. A.; Sergeenko, N. P.; Shubin, V. N.

    2003-07-01

    The vertical sounding data at chains of ionosphere stations are used to obtain relative variations of electron concentration in the F2 ionosphere region. Specific isolated traveling large-scale irregularities are distinguished in the diurnal succession of the fcF2 relative variations records. The temporal shifts of the irregularities at the station chains determine their motion velocity (of the order of speed of sound) and spatial scale (of order of 3000-5000km, the trajectory length being up to 10000km). The motion trajectories of large-scale isolated irregularities which had preceded the earthquakes are reconstructed.

  5. Structure and conformational dynamics of molecules in the excited electronic states: theory and experiment

    Science.gov (United States)

    Godunov, I. A.; Bataev, V. A.; Maslov, D. V.; Yakovlev, N. N.

    2017-01-01

    The structure of conformational non-rigid molecules in the excited electronic states are investigated by joint theoretical and experimental methods. The theoretical part of work consist of two stages. In first stage the ab initio quantum-chemical calculations are carried out using high level methods. In second stage the vibrational problems of the various dimensions are solved by variational method for vibrations of large amplitude. In experimental part of work the vibronic spectra are investigated: gas-phase absorption and also, fluorescence excitation spectra of jet-cooled molecules. Some examples are considered.

  6. Gas mixing system for imaging of nanomaterials under dynamic environments by environmental transmission electron microscopy.

    Science.gov (United States)

    Akatay, M Cem; Zvinevich, Yury; Baumann, Philipp; Ribeiro, Fabio H; Stach, Eric A

    2014-03-01

    A gas mixing manifold system that is capable of delivering a stable pressure stream of a desired composition of gases into an environmental transmission electron microscope has been developed. The system is designed to provide a stable imaging environment upon changes of either the composition of the gas mixture or upon switching from one gas to another. The design of the system is described and the response of the pressure inside the microscope, the sample temperature, and sample drift in response to flow and composition changes of the system are reported.

  7. Atomistic Control of the Dynamical Electronic Properties of 2D Materials and Beyond

    Science.gov (United States)

    Santos, Elton

    Two-dimensional (2D) materials, such as graphene, transition metal dichalcogenides and recently found 2D-perovskites, have attracted intense interest for their fascinating electronic properties, and exhibit strikingly different optoelectronic and mechanical features from their 3D-bulk counterparts. They are promising for a wide range of applications, including flexible, mechanically strong electronics such as transistors, memories, logic circuits, light emitters and photodetectors. In this presentation I will discuss different alternatives ranging from electric fields, strain, Ar-plasma treatment, to synthesis processes, to precisely control intrinsic material properties. I will describe several case studies where the synergy between in-silico predictions and experiments has driven smart devices with novel set of functional chemical and physical properties. Moreover, I will discuss some challenges at the forefront of 2D-perovskite materials as the few-layer limit is reached and new device-platforms for energy conversion applications. We acknowledge UKCP consortium (EPSRC Grant ref EP/K013564/1), Xsede network (NSF Grants Number TG-DMR120049 and TG-DMR150017), Sustainable Energy PRP (Queen's University Belfast), and Queen's Fellow Award (Grant Number M8407MPH).

  8. Electronic structure and dynamics of ordered clusters with ME or RE ions on oxide surface

    Energy Technology Data Exchange (ETDEWEB)

    Kulagin, N.A., E-mail: nkulagin@bestnet.kharkov.u [Kharkiv National University for Radio Electronics, Avenue Shakespeare 6-48, 61045 Kharkiv (Ukraine)

    2011-03-15

    Selected data of ab initio simulation of the electronic structure and spectral properties of either cluster with ions of iron, rare earth or actinium group elements have been presented here. Appearance of doped Cr{sup +4} ions in oxides, Cu{sup +2} in HTSC, Nd{sup +2} in solids has been discussed. Analysis of experimental data for plasma created ordered structures of crystallites with size of about 10{sup -9} m on surface of separate oxides are given, too. Change in the spectroscopic properties of clusters and nano-structures on surface of strontium titanate crystals discussed shortly using the X-ray line spectroscopy experimental results. - Research highlights: External influence and variation of technology induce changes in valence of nl ions in compounds. Wave function of cluster presented as anti-symmetrical set of ions wave functions. The main equation describes the self-consistent field depending on state of all electrons of cluster. Level scheme of Cr{sup 4+} ions in octo- and tetra-site corresponds to doped oxides spectra after treatment. Plasma treatment effects in appearance of systems of unit crystallites with size of about 10{sup -6}-10{sup -9} m.

  9. Momentum-resolved electron dynamics of image-potential states on Cu and Ag surfaces

    Science.gov (United States)

    Schubert, K.; Damm, A.; Eremeev, S. V.; Marks, M.; Shibuta, M.; Berthold, W.; Güdde, J.; Borisov, A. G.; Tsirkin, S. S.; Chulkov, E. V.; Höfer, U.

    2012-05-01

    The dependence of the inelastic lifetime of electrons in the first n=1 image-potential state of clean and rare-gas covered Ag(111), Cu(111), and Cu(100) surfaces on their momentum parallel to the surface has been studied experimentally by means of time- and angle-resolved two-photon photoemission spectroscopy (2PPE) and theoretically by calculations based on the many-body theory within the self-energy formalism. Similar to the previously studied clean Cu(100) surface, the theoretical results are in excellent agreement with the experiment findings for Cu(111). For Ag(111), the theory overestimates the decay rate and its momentum dependence, which is attributed to the neglect of surface plasmon excitations. With increasing parallel momentum, the n=1 state shifts out of the projected bulk band gap on both surfaces and turns into an image-potential resonance. This opens an additional decay channel by resonant electron transfer into the bulk, which is theoretically treated by the application of the wave packet propagation approach. The expected stronger increase of the decay rate upon crossing the edge of the band gap, however, is not observed in the experiment. The decoupling of the image-potential states from the metal surface upon adsorption of rare-gas layers results in a decrease of the decay rate as well as of its momentum dependence by a similar factor, which can be successfully explained by the change of interband and intraband contributions to the total decay rate.

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

    KAUST Repository

    Sun, Jingya

    2015-09-14

    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.

  11. Dynamic electron-ion collisions and nuclear quantum effects in quantum simulation of warm dense matter.

    Science.gov (United States)

    Kang, Dongdong; Dai, Jiayu

    2017-11-29

    The structural, thermodynamic and transport properties of warm dense matter (WDM) are crucial to the fields of astrophysical physics, 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 up to 10 times solid density and the temperature is between 0.1 and 100 eV. In the WDM regime, matter exhibits moderately or strongly coupled, partially degenerate. Therefore, the methods which used to deal with condensed matter and isolated atom should be validated for WDM properly. 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, \\ie, quantum Langevin molecular dynamics and first principles path integral molecular dynamics. The related applications for WDM are also included. © 2017 IOP Publishing Ltd.

  12. Efficient analysis of mode profiles in elliptical microcavity using dynamic-thermal electron-quantum medium FDTD method.

    Science.gov (United States)

    Khoo, E H; Ahmed, I; Goh, R S M; Lee, K H; Hung, T G G; Li, E P

    2013-03-11

    The dynamic-thermal electron-quantum medium finite-difference time-domain (DTEQM-FDTD) method is used for efficient analysis of mode profile in elliptical microcavity. The resonance peak of the elliptical microcavity is studied by varying the length ratio. It is observed that at some length ratios, cavity mode is excited instead of whispering gallery mode. This depicts that mode profiles are length ratio dependent. Through the implementation of the DTEQM-FDTD on graphic processing unit (GPU), the simulation time is reduced by 300 times as compared to the CPU. This leads to an efficient optimization approach to design microcavity lasers for wide range of applications in photonic integrated circuits.

  13. Wavelength dependence of sub-laser-cycle few-electron dynamics in strong-field multiple ionization

    Energy Technology Data Exchange (ETDEWEB)

    Herrwerth, O; Rudenko, A; Kremer, M; Jesus, V L B de; Fischer, B; Gademann, G; Simeonidis, K; Achtelik, A; Ergler, Th; Feuerstein, B; Schroeter, C D; Moshammer, R; Ullrich, J [Max-Planck-Institut fuer Kernphysik, Saupfercheckweg 1, D-69117 Heidelberg (Germany)], E-mail: Artem.Rudenko@mpi-hd.mpg.de

    2008-02-15

    Recoil-ion momentum distributions for double and triple ionization of Ne and Ar, as well as for double ionization of N{sub 2} molecule by intense (0.3-0.5 PW cm{sup -2}), short ({approx}35-40 fs) laser pulses have been recorded in a so far unexplored long laser-wavelength regime at 1300 nm. Compared to earlier results at 800 nm, the direct (e, ne) ionization pathway during recollision is strongly enhanced manifesting itself in a pronounced double-hump structure in the longitudinal ion momentum spectra not only for Ne, but also surprisingly distinct for Ar and, found for the first time, for molecules. Observed wavelength dependence of the sub-laser-cycle correlated few-electron dynamics might be of paramount importance for possible future applications in attosecond science, in particular, for imaging of ultrafast molecular processes via recollision-induced fragmentation.

  14. Measurement of dynamic patterns of an elastic membrane at bi-modal vibration using high speed electronic speckle pattern interferometry

    Energy Technology Data Exchange (ETDEWEB)

    Preciado, Jorge Sanchez; Lopez, Carlos Perez; Santoyo, Fernando Mendoza [Grupo de Metrología Optica, Centro de Investigaciones en Óptica, A. C. Loma del Bosque 115, Col. Lomas del Campestre, León, Guanajuato, 37150 (Mexico)

    2014-05-27

    Implementing a hybrid arrangement of Laser Doppler Vibrometry (LDV) and high speed Electronic Speckle Pattern Interferometry (ESPI) we were able to measure the dynamic patterns of a flat rectangular elastic membrane clamped at its edges stimulated with the sum of two resonance frequencies. ESPI is a versatile technique to analyze in real-time the deformation of a membrane since its low computational cost and easy implementation of the optical setup. Elastic membranes present nonlinear behaviors when stimulated with low amplitude signals. The elastic membrane under test, with several non rational related vibrating modals below the 200 Hz, was stimulated with two consecutives resonant frequencies. The ESPI patterns, acquired at high speed rates, shown a similar behavior for the dual frequency stimulation as in the case of patterns formed with the entrainment frequency. We think this may be related to the effects observed in the application of dual frequency stimulation in ultrasound.

  15. Probing ultrafast dynamics in electronic structure of epitaxial Gd(0 0 0 1) on W(1 1 0)

    Energy Technology Data Exchange (ETDEWEB)

    Beaulieu, Nathan [Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin BP 48, 91192 Gif-sur-Yvette Cedex (France); Malinowski, Gregory [Laboratoire de Physique des Solides, Université Paris Sud, Orsay (France); Bendounan, Azzedine; Silly, Mathieu G.; Chauvet, Christian [Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin BP 48, 91192 Gif-sur-Yvette Cedex (France); Krizmancic, Damjan [Instituto Officina dei Materiali (IOM)-CNR Laboratorio TASC, in Area Science Park S.S.14, Km 163.5, I-34149 Trieste (Italy); Sirotti, Fausto [Synchrotron SOLEIL, L’Orme des Merisiers, Saint-Aubin BP 48, 91192 Gif-sur-Yvette Cedex (France)

    2013-08-15

    Highlights: •Study of the magnetism of epitaxial Gd(0 0 0 1)/W(1 1 0). •Study of Gd(0 0 0 1) band structure as a function of the temperature. •Study of the Gd magnetism dynamics probing the M5 edge. -- Abstract: The electronic and magnetic properties of Gd have been studied using time- and angle-resolved photoelectron spectroscopy employing laser pump and synchrotron radiation probe pulses. The static temperature evolution of the valence band and more precisely, the 5d6s exchange splitting is reported. Ultrafast demagnetization is measured using dichroic resonant Auger spectroscopy. Remarkably, a complete demagnetization is observed followed up by a non-monotonic recovery that could be associated to magnetization oscillations.

  16. Probe of Multi-electron Dynamics in Xenon by Caustics in High Order Harmonic Generation

    CERN Document Server

    Faccialà, Davide; Bruner, Barry D; Ciriolo, Anna G; De Silvestri, Sandro; Devetta, Michele; Negro, Matteo; Soifer, Hadas; Stagira, Salvatore; Dudovich, Nirit; Vozzi, Caterina

    2016-01-01

    We investigated the giant resonance in Xenon by high-order harmonic generation spectroscopy driven by a two-color field. The addition of a non-perturbative second harmonic component parallel to the driving field breaks the symmetry between neighboring sub-cycles resulting in the appearance of spectral caustics at two distinct cut-off energies. By controlling the phase delay between the two color components it is possible to tailor the harmonic emission in order to amplify and isolate the spectral feature of interest. In this paper we demonstrate how this control scheme can be used to investigate the role of electron correlations that give birth to the giant resonance in Xenon. The collective excitations of the giant dipole resonance in Xenon combined with the spectral manipulation associated with the two color driving field allow to see features that are normally not accessible and to obtain a quantitative good agreement between the experimental results and the theoretical predictions.

  17. Ion dynamics in electron beam–plasma interaction: particle-in-cell simulations

    Directory of Open Access Journals (Sweden)

    K. Baumgärtel

    2014-08-01

    Full Text Available Electron beam–plasma interaction including ions is studied by particle-in-cell (PIC simulations using a one-dimensional, electrostatic code. Evidence for Langmuir wave decay is given for sufficiently energetic beams, as in previous Vlasov–Maxwell simulations. The mechanism for the generation of localized finite-amplitude ion density fluctuations is analyzed. Amplitude modulation due to interference between the beam-generated Langmuir waves causes random wave localization including strong transient spikes in field intensity which create bursty ion density structures via ponderomotive forces. More dense beams may quench the decay instability and generate low-frequency variations dominated by the wave number of the fastest growing Langmuir mode.

  18. Dynamics of vendor innovation capability: Evidence from the Electronics Manufacturing Services industry

    DEFF Research Database (Denmark)

    Perunovic, Zoran; Mefford, Robert; Christoffersen, Mads

    2012-01-01

    , by traditional manufacturing capabilities, such as cost, quality, delivery, and flexibility. Taking a vendor’s perspective in outsourcing, we develop and present a conceptual framework for studying vendor innovation capability. We propose to test this framework in the Electronic Manufacturing Services Industry.......Recent developments suggest that an increasing number of companies outsource manufacturing with the hope that vendors will help them improve innovativeness. Still, the growing research in the topic has not yet studied two important dimensions of the relationship between manufacturing outsourcing...... and innovation. The first is the realization that vendor capabilities have been recognized as one of the most important factors for the success of outsourcing. The second refers to the fact that, even though innovation capability is required, vendors are still being selected, and their performance evaluated...

  19. Implementation of Dynamically Corrected Gates on a Single Electron Spin in Diamond

    Science.gov (United States)

    Rong, Xing; Geng, Jianpei; Wang, Zixiang; Zhang, Qi; Ju, Chenyong; Shi, Fazhan; Duan, Chang-Kui; Du, Jiangfeng

    2014-02-01

    Precise control of an open quantum system is critical to quantum information processing but is challenging due to inevitable interactions between the quantum system and the environment. We demonstrated experimentally a type of dynamically corrected gates using only bounded-strength pulses on the nitrogen-vacancy centers in diamond. The infidelity of quantum gates caused by a nuclear-spin bath is reduced from being the second order to the sixth order of the noise-to-control-field ratio, which offers greater efficiency in reducing infidelity. The quantum gates have been protected to the limit essentially set by the spin-lattice relaxation time T1. Our work marks an important step towards fault-tolerant quantum computation in realistic systems.

  20. Challenging bullwhip effect dynamics with electronically enabled-supply chain management systems

    Directory of Open Access Journals (Sweden)

    Thokozani Patmond Mbhele

    2016-11-01

    Full Text Available The bullwhip effect shows the dynamics of accumulating order rate that exceeds the tentatively stable actual demand rate. This paper aimed to assess the relative role of e-SCM systems as consumer demand orders cascading upstream supply chain network. The study’s population, consisting of the managers (senior and functional levels including supervisory level (non-managerial from retail sales, logistics, warehousing, marketing, manufacturing and IT hubs organisations, comprised of 460 respondents. In order to achieve the paper’s objective, the researcher developed and distributed a survey questionnaire and collected and analysed the data using Statistical Package for the Social Sciences (SPSS. The empirical results from the study reveal that business-to-business information technology (B2BIT diffusion frequencies have an effect on supply chain performance and e-SCM implementation promotes connectivity among supply chain partners to entrench commitment of the exchanged demand order information to mitigate the bullwhip effect

  1. Hydrogen bond, electron donor-acceptor dimer, and residence dynamics in supercritical CO(2)-ethanol mixtures and the effect of hydrogen bonding on single reorientational and translational dynamics: A molecular dynamics simulation study.

    Science.gov (United States)

    Skarmoutsos, Ioannis; Guardia, Elvira; Samios, Jannis

    2010-07-07

    The hydrogen bonding and dynamics in a supercritical mixture of carbon dioxide with ethanol as a cosolvent (X(ethanol) approximately 0.1) were investigated using molecular dynamics simulation techniques. The results obtained reveal that the hydrogen bonds formed between ethanol molecules are significantly more in comparison with those between ethanol-CO(2) molecules and also exhibit much larger lifetimes. Furthermore, the residence dynamics in the solvation shells of ethanol and CO(2) have been calculated, revealing much larger residence times for ethanol molecules in the ethanol solvation shell. These results support strongly the ethanol aggregation effects and the slow local environment reorganization inside the ethanol solvation shell, reported in a previous publication of the authors [Skarmoutsos et al., J. Chem. Phys. 126, 224503 (2007)]. The formation of electron donor-acceptor dimers between the ethanol and CO(2) molecules has been also investigated and the calculated lifetimes of these complexes have been found to be similar to those corresponding to ethanol-CO(2) hydrogen bonds, exhibiting a slightly higher intermittent lifetime. However, the average number of these dimers is larger than the number of ethanol-CO(2) hydrogen bonds in the system. Finally, the effect of the hydrogen bonds formed between the individual ethanol molecules on their reorientational and translational dynamics has been carefully explored showing that the characteristic hydrogen bonding microstructure obtained exhibits sufficiently strong influence upon the behavior of them.

  2. Electron and excitation energy transfers in covalently linked donor-acceptor dyads: mechanisms and dynamics revealed using quantum chemistry.

    Science.gov (United States)

    Cupellini, Lorenzo; Giannini, Samuele; Mennucci, Benedetta

    2017-12-20

    Photoinduced electron transfer (ET), hole transfer (HT), charge recombination (CR) and energy transfer (EET) are fundamental mechanisms, which occur in both natural and artificial light harvesting systems. Here, we present a computational strategy which determines ET, HT, CR and EET rates in a consistent way and merges them in a kinetic model to reproduce the net excited state dynamics. The effects of the solvent are included in all steps of the calculations making the present strategy a useful tool for a rational design of charge and energy transfer processes in complex systems. An application to covalently linked zinc and free-base porphyrin-naphthalenediimide dyads is presented. For each of the two systems, ultrafast optical spectroscopy experiments have shown a specific photophysics with different processes taking place simultaneously. The model reveals that such a diversity is mainly due to the different relative stability of the charge-separated state, while the electronic couplings for charge and energy transfer processes are quite similar in the two dyads.

  3. Molecular dynamics simulations with electronic stopping can reproduce experimental sputtering yields of metals impacted by large cluster ions

    Science.gov (United States)

    Tian, Jiting; Zhou, Wei; Feng, Qijie; Zheng, Jian

    2018-03-01

    An unsolved problem in research of sputtering from metals induced by energetic large cluster ions is that molecular dynamics (MD) simulations often produce sputtering yields much higher than experimental results. Different from the previous simulations considering only elastic atomic interactions (nuclear stopping), here we incorporate inelastic electrons-atoms interactions (electronic stopping, ES) into MD simulations using a friction model. In this way we have simulated continuous 45° impacts of 10-20 keV C60 on a Ag(111) surface, and found that the calculated sputtering yields can be very close to the experimental results when the model parameter is appropriately assigned. Conversely, when we ignore the effect of ES, the yields are much higher, just like the previous studies. We further expand our research to the sputtering of Au induced by continuous keV C60 or Ar100 bombardments, and obtain quite similar results. Our study indicates that the gap between the experimental and the simulated sputtering yields is probably induced by the ignorance of ES in the simulations, and that a careful treatment of this issue is important for simulations of cluster-ion-induced sputtering, especially for those aiming to compare with experiments.

  4. Ultrafast Excited-State Dynamics of Diketopyrrolopyrrole (DPP)-Based Materials: Static versus Diffusion-Controlled Electron Transfer Process

    KAUST Repository

    Alsulami, Qana

    2015-06-25

    Singlet-to-triplet intersystem crossing (ISC) and photoinduced electron transfer (PET) of platinum(II) containing diketopyrrolopyrrole (DPP) oligomer in the absence and presence of strong electron-acceptor tetracyanoethylene (TCNE) were investigated using femtosecond and nanosecond transient absorption spectroscopy with broadband capabilities. The role of platinum(II) incorporation in those photophysical properties was evaluated by comparing the excited-state dynamics of DPP with and without the metal centers. The steady-state measurements reveal that platinum(II) incorporation facilitates dramatically the interactions between DPP-Pt(acac) and TCNE, resulting in charge transfer (CT) complex formation. The transient absorption spectra in the absence of TCNE reveal ultrafast ISC of DPP-Pt(acac) followed by their long-lived triplet state. In the presence of TCNE, PET from the excited DPP-Pt(acac) and DPP to TCNE, forming the radical ion pairs. The ultrafast PET which occurs statically from DPP-Pt(acac) to TCNE in picosecond regime, is much faster than that from DPP to TCNE (nanosecond time scale) which is diffusion-controlled process, providing clear evidence that PET rate is eventually controlled by the platinum(II) incorporation.

  5. Control of interspecies electron transfer flow during anaerobic digestion: dynamic diffusion reaction models for hydrogen gas transfer in microbial flocs.

    Science.gov (United States)

    Ozturk, S S; Palsson, B O; Thiele, J H

    1989-02-05

    Dynamic reaction diffusion models were used to analyze the consequences of aggregation for syntrophic reactions in methanogenic ecosystems. Flocs from a whey digestor were used to measure all model parameters under the in situ conditions of a particular defined biological system. Fermentation simulations without adjustable parameters could precisely predict the kinetics of H(2) gas production of digestor flocs during syntrophic methanogenesis from ethanol. The results demonstrated a kinetic compartmentalization of H(2) metabolism inside the flocs. The interspecies electron transfer reaction was mildly diffusion controlled. The H(2) gas profiles across the flocs showed high H (2) concentrations inside the flocs at any time. Simulations of the syntrophic metabolism at low substrate concentrations such as in digestors or sediments showed that it is impossible to achieve high H(2) gas turnovers at simultaneously low steady-state H(2) concentrations. This showed a mechanistic contradiction in the concept of postulated low H(2) microenvironments for the anaerobic digestion process. The results of the computer experiments support the conclusion that syntrophic H(2) production may only be a side reaction of H(2) independent interspecies electron transfer in methanogenic ecosystems.

  6. Study of molecular structure, anharmonic vibrational dynamic and electronic properties of sulindac using spectroscopic techniques integrated with quantum chemical calculations

    Science.gov (United States)

    Faizan, Mohd; Alam, Mohammad Jane; Ahmad, Shabbir

    2017-11-01

    In the present investigation, spectroscopic techniques (FTIR, FT-Raman and UV-Vis) and quantum chemical calculations are employed for exploring vibrational and electronic spectra of sulindac compound. The calculations are performed on most stable conformer of the sulindac molecule using density functional theory (DFT). Anharmonic corrections are made to frequencies using vibrational second-order perturbation theory (VPT2). The effect of intermolecular interactions on the vibrational dynamics has been analyzed using dimeric structure of sulindac molecule. Hirshfeld surface analysis and 2D fingerprint plots are utilized to investigate the nature of interaction present in the crystal system. To account for electronic spectra in different solvents, an integral equation formalism of polarizable continuum model (IEFPCM) at TD-DFT/B3LYP/6-31G(d,p) level of theory has been employed. An excellent agreement between the theoretical and experimental data over the entire spectral region is observed. In addition, natural bond orbital (NBO) analysis, frontier molecular orbitals, nonlinear optical properties (NLO) and molecular electrostatic potential (MEP) analysis are also reported.

  7. Dynamic nano-imaging of label-free living cells using electron beam excitation-assisted optical microscope

    Science.gov (United States)

    Fukuta, Masahiro; Kanamori, Satoshi; Furukawa, Taichi; Nawa, Yasunori; Inami, Wataru; Lin, Sheng; Kawata, Yoshimasa; Terakawa, Susumu

    2015-01-01

    Optical microscopes are effective tools for cellular function analysis because biological cells can be observed non-destructively and non-invasively in the living state in either water or atmosphere condition. Label-free optical imaging technique such as phase-contrast microscopy has been analysed many cellular functions, and it is essential technology for bioscience field. However, the diffraction limit of light makes it is difficult to image nano-structures in a label-free living cell, for example the endoplasmic reticulum, the Golgi body and the localization of proteins. Here we demonstrate the dynamic imaging of a label-free cell with high spatial resolution by using an electron beam excitation-assisted optical (EXA) microscope. We observed the dynamic movement of the nucleus and nano-scale granules in living cells with better than 100 nm spatial resolution and a signal-to-noise ratio (SNR) around 10. Our results contribute to the development of cellular function analysis and open up new bioscience applications. PMID:26525841

  8. Dynamic nano-imaging of label-free living cells using electron beam excitation-assisted optical microscope.

    Science.gov (United States)

    Fukuta, Masahiro; Kanamori, Satoshi; Furukawa, Taichi; Nawa, Yasunori; Inami, Wataru; Lin, Sheng; Kawata, Yoshimasa; Terakawa, Susumu

    2015-11-03

    Optical microscopes are effective tools for cellular function analysis because biological cells can be observed non-destructively and non-invasively in the living state in either water or atmosphere condition. Label-free optical imaging technique such as phase-contrast microscopy has been analysed many cellular functions, and it is essential technology for bioscience field. However, the diffraction limit of light makes it is difficult to image nano-structures in a label-free living cell, for example the endoplasmic reticulum, the Golgi body and the localization of proteins. Here we demonstrate the dynamic imaging of a label-free cell with high spatial resolution by using an electron beam excitation-assisted optical (EXA) microscope. We observed the dynamic movement of the nucleus and nano-scale granules in living cells with better than 100 nm spatial resolution and a signal-to-noise ratio (SNR) around 10. Our results contribute to the development of cellular function analysis and open up new bioscience applications.

  9. Towards Understanding the Solvent-Dynamic Control of the Transport and Heterogeneous Electron-Transfer Processes in Ionic Liquids.

    Science.gov (United States)

    Bhat, Mohsin Ahmad; Ingole, Pravin P; Randriamahazaka, Hyacinthe

    2017-02-17

    The impact of temperature-induced changes in solvent dynamics on the diffusion coefficient and standard rate constant k(0) for heterogeneous electron transfer (ET) of ethylferrocene (EFc) in 1-butyl-3-methylimidazolium hexafluorophosphate ([BMIM][PF6 ]) is investigated. The results are analysed to understand the impact of solvent-dynamic control, solute-solvent interactions and solvent friction on the transport of redox probes and k(0) . Concentration dependence of the diffusion coefficient of EFc in [BMIM][PF6 ] is observed. This is attributed to the solute-induced enhancement of the structural organisation of the ionic liquid (IL), which is supported by the concentration-dependent UV/Vis absorption and photoluminescence responses of EFc/[BMIM][PF6 ] solutions. Similar values of the activation energies for mass transport and ET and a linear relationship between the diffusion coefficient and the heterogeneous ET rate is observed. The ratio between the diffusion coefficient and the heterogeneous rate constant allows a characteristic length Ld , which is temperature-independent, to be introduced. The presented results clearly establish that mass transport and heterogeneous ET of redox probes are strongly correlated in ILs. It is proposed that the apparent kinetics of heterogeneous ET reactions in ILs can be explained in terms of their impact on thermal equilibration, energy dissipation and thermal excitation of redox-active probes. © 2017 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim.

  10. Electronic excitation induced hydrogen-bond adjustment and lattice control in organic-inorganic hybrid cubic perovskites: a fixed occupation molecular dynamics study.

    Science.gov (United States)

    Wang, Mo-Ran; Ren, Xiang-Yang; Li, Xian-Bin; Chen, Nian-Ke; Sun, Hong-Bo

    2017-10-04

    The organic-inorganic hybrid perovskite has become a new type of semiconductor for low cost and highly efficient solar cells. However, the mechanism of interactions between the organic cation and the inorganic framework is still not completely clear under optical electronic excitation. In this work, we employ first-principles molecular dynamics with electronic excitation effects to prove that the hydrogen-bond interaction between the molecular cation and the inorganic lattice can be readily adjusted by several-percentage-valence-electron excitations in cubic CH3NH3PbI3. While the hydrogen-bond interaction causes serious lattice distortions, the electronic excitation can recover the lattice symmetry largely by weakening hydrogen bonding. The study offers atomic dynamics to understand the excitation process in the organic-inorganic hybrid perovskite semiconductor.

  11. Time-resolved THz studies of carrier dynamics in semiconductors, superconductors, and strongly-correlated electron materials

    Energy Technology Data Exchange (ETDEWEB)

    Kaindl, Robert A.; Averitt, Richard D.

    2006-11-14

    materials occur at lower energies. The terahertz (THz) regime is particularly rich in such fundamental resonances. This includes ubiquitous lattice vibrations and low-energy collective oscillations of conduction charges. In nanoscale materials, band structure quantization also yields novel infrared and THz transitions, including intersubband absorption in quantum wells. The formation of excitons in turn leads to low-energy excitations analogous to inter-level transitions in atoms. In transition-metal oxides, fundamental excitation gaps arise from charge pairing into superconducting condensates and other correlated states. This motivates the use of ultrafast THz spectroscopy as a powerful tool to study light-matter interactions and microscopic processes in nanoscale and correlated-electron materials.A distinct advantage of coherent THz pulses is that the amplitude and phase of the electric field can be measured directly, as the THz fields are coherent with the fs pulses from which they are generated. Using THz time-domain spectroscopy (THz-TDS), both the real and imaginary parts of the response functions (such as the dielectric function) are obtained directly without the need for Kramers?Kronig transforms. The THz response can also be expressed in terms of absorption and refractive index, or as the optical conductivity. The optical conductivity describes the current response of a many-body system to an electric field, an ideal tool to study conducting systems. A second important advantage is the ultrafast time resolution that results from the short temporal duration of the THz time-domain sources. In particular, optical-pump THz-probe spectroscopy enables a delicate probe of the transient THz conductivity after optical photoexcitation. These experiments can provide insight into quasiparticle interactions, phase transitions, or nonequilibrium dynamics. In this chapter we will provide many such examples. Since THz spectroscopy of solids is a quickly expanding field

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

    Energy Technology Data Exchange (ETDEWEB)

    Morzan, Uriel N.; Ramírez, Francisco F.; Scherlis, Damián A., E-mail: damian@qi.fcen.uba.ar, E-mail: mcgl@qb.ffyb.uba.ar [Departamento de Química Inorgánica, Analítica y Química Física/INQUIMAE, Facultad de Ciencias Exactas y Naturales, Universidad de Buenos Aires, Ciudad Universitaria, Pab. II, Buenos Aires (C1428EHA) (Argentina); Oviedo, M. Belén; Sánchez, Cristián G. [Departamento de Matemática y Física, Facultad de Ciencias Químicas, INFIQC, Universidad Nacional de Córdoba, Ciudad Universitaria, X5000HUA Córdoba (Argentina); Lebrero, Mariano C. González, E-mail: damian@qi.fcen.uba.ar, E-mail: mcgl@qb.ffyb.uba.ar [Instituto de Química y Fisicoquímica Biológicas, IQUIFIB, CONICET (Argentina)

    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.

  13. Ultrafast harmonic rf kicker design and beam dynamics analysis for an energy recovery linac based electron circulator cooler ring

    Directory of Open Access Journals (Sweden)

    Yulu Huang

    2016-08-01

    Full Text Available An ultrafast kicker system is being developed for the energy recovery linac (ERL based electron circulator cooler ring (CCR in the proposed Jefferson Lab Electron Ion Collider (JLEIC, previously named MEIC. In the CCR, the injected electron bunches can be recirculated while performing ion cooling for 10–30 turns before the extraction, thus reducing the recirculation beam current in the ERL to 1/10−1/30 (150  mA-50  mA of the cooling beam current (up to 1.5 A. Assuming a bunch repetition rate of 476.3 MHz and a recirculating factor of 10 in the CCR, the kicker is required to operate at a pulse repetition rate of 47.63 MHz with pulse width of around 2 ns, so that only every 10th bunch in the CCR will experience a transverse kick while the rest of the bunches will not be disturbed. Such a kicker pulse can be synthesized by ten harmonic modes of the 47.63 MHz kicker pulse repetition frequency, using up to four quarter wavelength resonator (QWR based deflecting cavities. In this paper, several methods to synthesize such a kicker waveform will be discussed and a comparison of their beam dynamics performance is made using ELEGANT. Four QWR cavities are envisaged with high transverse shunt impedance requiring less than 100 W of total rf power for a Flat-Top kick pulse. Multipole fields due to the asymmetry of this type of cavity are analyzed. The transverse emittance growth due to the sextupole component is simulated in ELEGANT. Off-axis injection and extraction issues and beam optics using a multicavity kick-drift scheme will also be discussed.

  14. Live correlative light-electron microscopy to observe molecular dynamics in high resolution.

    Science.gov (United States)

    Kobayashi, Shouhei; Iwamoto, Masaaki; Haraguchi, Tokuko

    2016-08-01

    Fluorescence microscopy (FM) is a powerful tool for observing specific molecular components in living cells, but its spatial resolution is relatively low. In contrast, electron microscopy (EM) provides high-resolution information about cellular structures, but it cannot provide temporal information in living cells. To achieve molecular selectivity in imaging at high resolution, a method combining EM imaging with live-cell fluorescence imaging, known as live correlative light-EM (CLEM), has been developed. In this method, living cells are first observed by FM, fixed in situ during the live observation and then subjected to EM observation. Various fluorescence techniques and tools can be applied for FM, resulting in the generation of various modified methods that are useful for understanding cellular structure in high resolution. Here, we review the methods of CLEM and live-cell imaging associated with CLEM (live CLEM). Such methods can greatly advance the understanding of the function of cellular structures on a molecular level, and thus are useful for medical fields as well as for basic biology. © The Author 2016. Published by Oxford University Press on behalf of The Japanese Society of Microscopy. All rights reserved. For permissions, please e-mail: journals.permissions@oup.com.

  15. An approach for de novo structure determination of dynamic molecular assemblies by electron cryomicroscopy.

    Science.gov (United States)

    Sander, Bjoern; Golas, Monika M; Lührmann, Reinhard; Stark, Holger

    2010-06-09

    Single-particle electron cryomicroscopy is a powerful method for three-dimensional (3D) structure determination of macromolecular assemblies. Here we address the challenge of determining a 3D structure in the absence of reference models. The 3D structures are determined by alignment and weighted averaging of densities obtained by native cryo random conical tilt (RCT) reconstructions including consideration of missing data. Our weighted averaging scheme (wRCT) offers advantages for potentially heterogeneous 3D densities of low signal-to-noise ratios. Sets of aligned RCT structures can also be analyzed by multivariate statistical analysis (MSA) to provide insights into snapshots of the assemblies. The approach is used to compute 3D structures of the Escherichia coli 70S ribosome and the human U4/U6.U5 tri-snRNP under vitrified unstained cryo conditions, and to visualize by 3D MSA the L7/L12 stalk of the 70S ribosome and states of tri-snRNP. The approach thus combines de novo 3D structure determination with an analysis of compositional and conformational heterogeneity.

  16. Structural, dynamical & electronic properties of CaCuO{sub 2}

    Energy Technology Data Exchange (ETDEWEB)

    Agrawal, B.K.; Agrawal, S. [Allahabad Univ. (India)

    1994-12-31

    The scalar relativistic version of an accurate first principles full potential self- consistent linearized muffin tin orbital (LMTO) method has been employed for describing the physical properties of the parent system of the high-Tc oxide superconductors, i.e., CaCuO2. The presently employed modified version of the LMTO method is quite fast and goes beyond the usual LMTO-ASA method in the sense that it permits a completely general shape of the potential and the charge density. Also, in contrast to LMTO-ASA, the present method is also capable of treating distorted lattice structures accurately. The calculated values of the lattice parameters of pure CaCuO2 lie within 3% of the experimentally measured values for the Sr-doped system Ca(.86)Sr(.14)CuO(2). The computed electronic structures and the density of states is quite similar to those of the other oxide superconductors, except of their three- dimensional character because of the presence of strong coupling between the closely spaced CuO2 layers. The van Hove singularity peak appears slightly below the Fermi level and a small concentration of oxygenation /or/ substitutional doping may pin it as the Fermi level. The calculated frequencies for some symmetric frozen phonons for undoped CaCuO2 are quite near to the measured data for the Sr-doped CaCuO2.

  17. Dynamic molecular structure retrieval from low-energy laser-induced electron diffraction spectra

    Science.gov (United States)

    Vu, Dinh-Duy T.; Phan, Ngoc-Loan T.; Hoang, Van-Hung; Le, Van-Hoang

    2017-12-01

    A recently developed quantitative rescattering theory showed that a laser-free elastic cross section can be separated from laser-induced electron diffraction (LIED) spectra. Based upon this idea, Blaga et al investigated the possibility of reconstructing molecular structure from LIED spectra (2012 Nature 483 7388). In the above study, an independent atoms model (IAM) was used to interpret high-energy electron–molecule collisions induced by a mid-infrared laser. Our research aims to extend the application range of this structural retrieval method to low-energy spectra induced by more common near-infrared laser sources. The IAM is insufficient in this case, so we switch to a more comprehensive model—the multiple scattering (MS) theory. From the original version concerning only neutral targets, we upgrade the model so that it is compatible with electron–ion collisions at low energy. With available LIED experiment data of CO2 and O2, the upgraded MS is shown to be greatly effective as a tool for molecular imaging from spectra induced by a near-infrared laser. The captured image is at about 2 fs after the ionization, shorter than the period 4–6 fs by using the mid-infrared laser in Blaga’s experiment.

  18. Universal behaviour in the stock market: Time dynamics of the electronic orderbook

    Energy Technology Data Exchange (ETDEWEB)

    Kızılersü, Ayşe, E-mail: ayse.kizilersu@adelaide.edu.au [Special Research Centre for the Subatomic Structure of Matter (CSSM), Department of Physics, School of Chemistry and Physics, Adelaide University, 5005 (Australia); Kreer, Markus [phi-t products & services, Karlsruher Strasse 88, 76139 Karlsruhe (Germany); Thomas, Anthony W. [CoEPP and CSSM, Department of Physics, Adelaide University, SA 5005 (Australia); Feindt, Michael [Blue Yonder GmbH, Ohiostraße 8, 756139 Karlsruhe (Germany)

    2016-07-29

    A consequence of the digital revolution is that share trading at the stock exchange takes place via electronic order books which are accessed by traders and investors via the internet. Our empirical findings of the London Stock Exchange demonstrate that once ultra-high frequency manipulation on time scales less than around ten milliseconds is excluded, all relevant changes in the order book happen with time differences that are randomly distributed and well described by a left-truncated Weibull distribution with universal shape parameter (independent of time and same for all stocks). The universal shape parameter corresponds to maximum entropy of the distribution. - Highlights: • After the ultra-high frequency manipulation is excluded, all the time differences in the EOB described by a left-truncated Weibull distribution. • The Weibull shape parameter is universal i.e. independent of time and same for all stocks and it is equal to Euler–Mascheroni constant. • The universal shape parameter corresponds to maximum entropy of the distribution.

  19. Static and Dynamic Electronic (Hyperpolarizabilities of Dimethylnaphthalene Isomers: Characterization of Spatial Contributions by Density Analysis

    Directory of Open Access Journals (Sweden)

    Andrea Alparone

    2013-01-01

    Full Text Available Static and frequency-dependent electronic (hyperpolarizabilities of the dimethylnaphthalene (DMN isomers were computed in vacuum using the Coulomb-attenuating Density Functional Theory method. The nonlinear optical Second Harmonic Generation (SHG and Electro-Optical Pockels Effect (EOPE were investigated at the characteristic Nd:YAG laser wavelength of 1064 nm. The response electric properties especially the longitudinal polarizability, polarizability anisotropy, and first-order hyperpolarizability are significantly affected by the position of the methyl groups. The SHG and EOPE techniques can be potentially useful to discriminate the ,-DMN isomers (2,6-DMN < 2,7-DMN < 2,3-DMN as well as the ,-DMN isomers (1,5-DMN < 1,4-DMN < 1,8-DMN. The (hyperpolarizability differences among the investigated DMNs were elucidated through density analysis calculations. The predicted polarizabilities exhibit good linear relationships with the experimental first-order biomass-normalized rate coefficient, a physicochemical property connected to the rates of biodegradation processes of polycyclic aromatic hydrocarbons.

  20. Instrumentation and Beam Dynamics Study of Advanced Electron-Photon Facility in Indiana University

    Energy Technology Data Exchange (ETDEWEB)

    Luo, Tianhuan [Indiana Univ., Bloomington, IN (United States)

    2011-08-01

    The Advanced eLectron-PHoton fAcility (ALPHA) is a compact electron accelerator under construction and being commissioned at the Indiana University Center for Exploration of Energy and Matter (CEEM). In this thesis, we have studied the refurbished Cooler Injector Synchrotron (CIS) RF cavity using both the transmission line model and SUPERFISH simulation. Both low power and high power RF measurements have been carried out to characterize the cavity. Considering the performance limit of ferrite, we have designed a new ferrite loaded, co-axial quarter wave like cavity with similar structure but a more suitable ferrite material. We have also designed a traveling wave stripline kicker for fast extraction by POISSON and Microwave Studio. The strips geometry is trimmed to maximize the uniformity of the kicking field and match the impedance of the power cables. The time response simulation shows the kicker is fast enough for machine operation. The pulsed power supply requirement has also been specified. For the beam diagnosis in the longitudinal direction, we use a wideband Wall Gap Monitor (WGM) served in CIS. With proper shielding and amplification to get good WGM signal, we have characterized the injected and extracted beam signal in single pass commissioning, and also verified the debunching effect of the ALPHA storage ring. A modulation-demodulation signal processing method is developed to measure the current and longitudinal profile of injected beam. By scanning the dipole strength in the injection line, we have reconstructed the tomography of the longitudinal phase space of the LINAC beam. In the accumulation mode, ALPHA will be operated under a low energy and high current condition, where intra beam scattering (IBS) becomes a dominant effect on the beam emittance. A self consistent simulation, including IBS effect, gas scattering and linear coupling, has been carried out to calculate the emittance of the stored beam.