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Sample records for photocarrier dynamics electronic

  1. Direct observation of photocarrier electron dynamics in C60 films on graphite by time-resolved two-photon photoemission

    PubMed Central

    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

  2. Photocarrier dynamics in anatase TiO{sub 2} investigated by pump-probe absorption spectroscopy

    SciTech Connect

    Matsuzaki, H. E-mail: okamotoh@k.u-tokyo.ac.jp; Matsui, Y.; Uchida, R.; Yada, H.; Terashige, T.; Li, B.-S.; Sawa, A.; Kawasaki, M.; Tokura, Y.; Okamoto, H. E-mail: okamotoh@k.u-tokyo.ac.jp

    2014-02-07

    The dynamics of photogenerated electrons and holes in undoped anatase TiO{sub 2} were studied by femtosecond absorption spectroscopy from the visible to mid-infrared region (0.1–2.0 eV). The transient absorption spectra exhibited clear metallic responses, which were well reproduced by a simple Drude model. No mid-gap absorptions originating from photocarrier localization were observed. The reduced optical mass of the photocarriers obtained from the Drude-model analysis is comparable to theoretically expected one. These results demonstrate that both photogenerated holes and electrons act as mobile carriers in anatase TiO{sub 2}. We also discuss scattering and recombination dynamics of photogenerated electrons and holes on the basis of the time dependence of absorption changes.

  3. Deep subsurface electronic defect image contrast and resolution amplification in Si wafers using infrared photocarrier radiometry

    NASA Astrophysics Data System (ADS)

    Batista, Jerias; Mandelis, Andreas; Shaughnessy, Derrick; Li, Bincheng

    2004-09-01

    A photocarrier radiometry technique using a secondary subband-gap dc light source is introduced, along with the applications to deep subsurface electronic defect analysis in Si wafers. It is shown that the use of a dc light source, in addition to the modulated laser beam, drastically enhances the potential of the technique in resolving low-level damage otherwise virtually indistinguishable by conventional photothermal techniques. Using this methodology, the overall contrast enhancement was about 386% for amplitude and 5586% in phase over conventional photocarrier radiometry.

  4. Electronic transport characterization of silicon wafers by spatially resolved steady-state photocarrier radiometric imaging

    SciTech Connect

    Wang, Qian; Li, Bincheng

    2015-09-28

    Spatially resolved steady-state photocarrier radiometric (PCR) imaging technique is developed to characterize the electronic transport properties of silicon wafers. Based on a nonlinear PCR theory, simulations are performed to investigate the effects of electronic transport parameters (the carrier lifetime, the carrier diffusion coefficient, and the front surface recombination velocity) on the steady-state PCR intensity profiles. The electronic transport parameters of an n-type silicon wafer are simultaneously determined by fitting the measured steady-state PCR intensity profiles to the three-dimensional nonlinear PCR model. The determined transport parameters are in good agreement with the results obtained by the conventional modulated PCR technique with multiple pump beam radii.

  5. Temperature-dependent photocarrier recombination dynamics in Cu{sub 2}ZnSnS{sub 4} single crystals

    SciTech Connect

    Phuong, Le Quang; Kanemitsu, Yoshihiko; Okano, Makoto; Yamada, Yasuhiro; Nagaoka, Akira; Yoshino, Kenji

    2014-02-24

    Time-resolved photoluminescence (PL) measurements have been used to study the temperature-dependent photocarrier recombination dynamics in Cu{sub 2}ZnSnS{sub 4} (CZTS) single crystals. We found a significant change of nearly four orders of magnitude of the PL decay time, from microseconds at low temperatures to subnanoseconds at room temperature. The slow PL decay at low temperatures indicates localization of the photocarriers at the band tails. Due to the large band tail states, the PL decay time depends strongly on both the photon energy and excitation density. It is pointed out that the drastically enhanced nonradiative recombination at high temperatures is one of the main factors that determine the power conversion efficiency of CZTS-based solar cells.

  6. Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells.

    PubMed

    Vella, Eleonora; Li, Hao; Grégoire, Pascal; Tuladhar, Sachetan M; Vezie, Michelle S; Few, Sheridan; Bazán, Claudia M; Nelson, Jenny; Silva-Acuña, Carlos; Bittner, Eric R

    2016-01-01

    All-organic-based photovoltaic solar cells have attracted considerable attention because of their low-cost processing and short energy payback time. In such systems the primary dissociation of an optical excitation into a pair of photocarriers has been recently shown to be extremely rapid and efficient, but the physical reason for this remains unclear. Here, two-dimensional photocurrent excitation spectroscopy, a novel non-linear optical spectroscopy, is used to probe the ultrafast coherent decay of photoexcitations into charge-producing states in a polymer:fullerene based solar cell. The two-dimensional photocurrent spectra are interpreted by introducing a theoretical model for the description of the coupling of the electronic states of the system to an external environment and to the applied laser fields. The experimental data show no cross-peaks in the twodimensional photocurrent spectra, as predicted by the model for coherence times between the exciton and the photocurrent producing states of 20 fs or less. PMID:27412119

  7. Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells

    PubMed Central

    Vella, Eleonora; Li, Hao; Grégoire, Pascal; Tuladhar, Sachetan M.; Vezie, Michelle S.; Few, Sheridan; Bazán, Claudia M.; Nelson, Jenny; Silva-Acuña, Carlos; Bittner, Eric R.

    2016-01-01

    All-organic-based photovoltaic solar cells have attracted considerable attention because of their low-cost processing and short energy payback time. In such systems the primary dissociation of an optical excitation into a pair of photocarriers has been recently shown to be extremely rapid and efficient, but the physical reason for this remains unclear. Here, two-dimensional photocurrent excitation spectroscopy, a novel non-linear optical spectroscopy, is used to probe the ultrafast coherent decay of photoexcitations into charge-producing states in a polymer:fullerene based solar cell. The two-dimensional photocurrent spectra are interpreted by introducing a theoretical model for the description of the coupling of the electronic states of the system to an external environment and to the applied laser fields. The experimental data show no cross-peaks in the twodimensional photocurrent spectra, as predicted by the model for coherence times between the exciton and the photocurrent producing states of 20 fs or less. PMID:27412119

  8. Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells.

    PubMed

    Vella, Eleonora; Li, Hao; Grégoire, Pascal; Tuladhar, Sachetan M; Vezie, Michelle S; Few, Sheridan; Bazán, Claudia M; Nelson, Jenny; Silva-Acuña, Carlos; Bittner, Eric R

    2016-07-14

    All-organic-based photovoltaic solar cells have attracted considerable attention because of their low-cost processing and short energy payback time. In such systems the primary dissociation of an optical excitation into a pair of photocarriers has been recently shown to be extremely rapid and efficient, but the physical reason for this remains unclear. Here, two-dimensional photocurrent excitation spectroscopy, a novel non-linear optical spectroscopy, is used to probe the ultrafast coherent decay of photoexcitations into charge-producing states in a polymer:fullerene based solar cell. The two-dimensional photocurrent spectra are interpreted by introducing a theoretical model for the description of the coupling of the electronic states of the system to an external environment and to the applied laser fields. The experimental data show no cross-peaks in the twodimensional photocurrent spectra, as predicted by the model for coherence times between the exciton and the photocurrent producing states of 20 fs or less.

  9. Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells

    NASA Astrophysics Data System (ADS)

    Vella, Eleonora; Li, Hao; Grégoire, Pascal; Tuladhar, Sachetan M.; Vezie, Michelle S.; Few, Sheridan; Bazán, Claudia M.; Nelson, Jenny; Silva-Acuña, Carlos; Bittner, Eric R.

    2016-07-01

    All-organic-based photovoltaic solar cells have attracted considerable attention because of their low-cost processing and short energy payback time. In such systems the primary dissociation of an optical excitation into a pair of photocarriers has been recently shown to be extremely rapid and efficient, but the physical reason for this remains unclear. Here, two-dimensional photocurrent excitation spectroscopy, a novel non-linear optical spectroscopy, is used to probe the ultrafast coherent decay of photoexcitations into charge-producing states in a polymer:fullerene based solar cell. The two-dimensional photocurrent spectra are interpreted by introducing a theoretical model for the description of the coupling of the electronic states of the system to an external environment and to the applied laser fields. The experimental data show no cross-peaks in the twodimensional photocurrent spectra, as predicted by the model for coherence times between the exciton and the photocurrent producing states of 20 fs or less.

  10. Accurate determination of electronic transport properties of silicon wafers by nonlinear photocarrier radiometry with multiple pump beam sizes

    SciTech Connect

    Wang, Qian; Li, Bincheng

    2015-12-07

    In this paper, photocarrier radiometry (PCR) technique with multiple pump beam sizes is employed to determine simultaneously the electronic transport parameters (the carrier lifetime, the carrier diffusion coefficient, and the front surface recombination velocity) of silicon wafers. By employing the multiple pump beam sizes, the influence of instrumental frequency response on the multi-parameter estimation is totally eliminated. A nonlinear PCR model is developed to interpret the PCR signal. Theoretical simulations are performed to investigate the uncertainties of the estimated parameter values by investigating the dependence of a mean square variance on the corresponding transport parameters and compared to that obtained by the conventional frequency-scan method, in which only the frequency dependences of the PCR amplitude and phase are recorded at single pump beam size. Simulation results show that the proposed multiple-pump-beam-size method can improve significantly the accuracy of the determination of the electronic transport parameters. Comparative experiments with a p-type silicon wafer with resistivity 0.1–0.2 Ω·cm are performed, and the electronic transport properties are determined simultaneously. The estimated uncertainties of the carrier lifetime, diffusion coefficient, and front surface recombination velocity are approximately ±10.7%, ±8.6%, and ±35.4% by the proposed multiple-pump-beam-size method, which is much improved than ±15.9%, ±29.1%, and >±50% by the conventional frequency-scan method. The transport parameters determined by the proposed multiple-pump-beam-size PCR method are in good agreement with that obtained by a steady-state PCR imaging technique.

  11. Ultrafast Optical Reflectivity Study of Photo-Carrier Relaxation Dynamics in Perovskite Iridates

    NASA Astrophysics Data System (ADS)

    Chu, Hao; Zhao, Liuyan; Hogan, Tom; Wilson, Stephen; Hsieh, David; Caltech Collaboration; University of California, Santa Barbara Collaboration

    The Ruddlesden-Popper series of perovskite iridates Srn+1IrnO3n+1 lie close to a localization-delocalization boundary, evolving from a Mott-like magnetic insulator in the single layer (n=1) compound to a paramagnetic semi-metal in the infinite layer (n= ∞) compound. We will discuss the insulator-to-metal transition in perovskite iridates from the point of view of time-resolved optical reflectivity measurements. This technique probes the relaxation dynamics of photo-generated carriers, which are strongly affected by the presence of a charge gap.

  12. Depth profile reconstructions of electronic transport properties in H{sup +} MeV-energy ion-implanted n-Si wafers using photocarrier radiometry

    SciTech Connect

    Tai, Rui; Wang, Chinhua Hu, Jingpei; Mandelis, Andreas

    2014-07-21

    A depth profiling technique using photocarrier radiometry (PCR) is demonstrated and used for the reconstruction of continuously varying electronic transport properties (carrier lifetime and electronic diffusivity) in the interim region between the ion residence layer and the bulk crystalline layer in H{sup +} implanted semiconductor wafers with high implantation energies (∼MeV). This defect-rich region, which is normally assumed to be part of the homogeneous “substrate” in all existing two- and three-layer models, was sliced into many virtual thin layers along the depth direction so that the continuously and monotonically variable electronic properties across its thickness can be considered uniform within each virtual layer. The depth profile reconstruction of both carrier life time and diffusivity in H{sup +} implanted wafers with several implantation doses (3 × 10{sup 14}, 3 × 10{sup 15}, and 3 × 10{sup 16} cm{sup −2}) and different implantation energies (from 0.75 to 2.0 MeV) is presented. This all-optical PCR method provides a fast non-destructive way of characterizing sub-surface process-induced electronic defect profiles in devices under fabrication at any intermediate stage before final metallization and possibly lead to process correction and optimization well before electrical testing and defect diagnosis becomes possible.

  13. Photocarrier Radiometry for Noncontact Evaluation of Monocrystalline Silicon (c-Si) Solar Cell Irradiated by 1 MeV Electron Beams

    NASA Astrophysics Data System (ADS)

    Song, P.; Liu, J. Y.; Yuan, H. M.; Wang, F.; Wang, Y.

    2016-08-01

    In this paper, the monocrystalline silicon (c-Si) solar cell irradiated by 1 MeV electron beams was investigated using noncontact photocarrier radiometry (PCR). A theoretical 1D two-layer PCR model including the impedance effect of the p-n junction was used to characterize the transport properties (carrier lifetime, diffusion coefficient, and surface recombination velocities) of c-Si solar cells irradiated by 1 MeV electron beams with different fluences. The carrier transport parameters were derived by the best fit through PCR measurements. Furthermore, an Ev+0.56 eV trap was introduced into the band gap based on the minority carrier lifetime reduction. An I-V characteristic was obtained by both AFORS-HET simulation and experimental study, and the simulation results shows in good agreement with the experimental results. Moreover, the simulation and experiment results also indicate that the increase of fluences of electron beams results in the reduction of short-circuit current and open-circuit voltage.

  14. Photomodulation spectroscopy of photocarrier dynamics, electronic defects and morphology of conducting polymers

    SciTech Connect

    Vardeny, Z.V.

    1993-01-01

    A variety of techniques were used: CW photomodulation, photomodulation in femtosecond and picosecond time ranges, CW resonant Raman scattering, transient photoinduced Raman scattering, electro-absorption, degenerate four-wave mixing, spin dependent photomodulation, and absorption detected magnetic resonance. The following conducting polymers were studied: polyacetylene, polythiophene, polydiacetylene 4-BCMU, polydiethynylsilanes, polysilane embedded in a-Si:H matrix, and fullerenes.

  15. Spectrally resolved modulated infrared radiometry of photothermal, photocarrier, and photoluminescence response of CdSe crystals: Determination of optical, thermal, and electronic transport parameters

    NASA Astrophysics Data System (ADS)

    Pawlak, M.; Chirtoc, M.; Horny, N.; Pelzl, J.

    2016-03-01

    Spectrally resolved modulated infrared radiometry (SR-MIRR) with super-band gap photoexcitation is introduced as a self-consistent method for semiconductor characterization (CdSe crystals grown under different conditions). Starting from a theoretical model combining the contributions of the photothermal (PT) and photocarrier (PC) signal components, an expression is derived for the thermal-to-plasma wave transition frequency ftc which is found to be wavelength-independent. The deviation of the PC component from the model at high frequency is quantitatively explained by a quasi-continuous distribution of carrier recombination lifetimes. The integral, broad frequency band (0.1 Hz-1 MHz) MIRR measurements simultaneously yielded the thermal diffusivity a, the effective IR optical absorption coefficient βeff, and the bulk carrier lifetime τc. Spectrally resolved frequency scans were conducted with interchangeable IR bandpass filters (2.2-11.3 μm) in front of the detector. The perfect spectral match of the PT and PC components is the direct experimental evidence of the key assumption in MIRR that de-exciting carriers are equivalent to blackbody (Planck) radiators. The exploitation of the β spectrum measured by MIRR allowed determining the background (equilibrium) free carrier concentration n0. At the shortest wavelength (3.3 μm), the photoluminescence (PL) component supersedes the PC one and has distinct features. The average sample temperature influences the PC component but not the PT one.

  16. H{sup +} ion-implantation energy dependence of electronic transport properties in the MeV range in n-type silicon wafers using frequency-domain photocarrier radiometry

    SciTech Connect

    Wang Chinhua; Mandelis, Andreas; Tolev, Jordan; Burchard, Bernd; Meijer, Jan

    2007-06-15

    Industrial n-type Si wafers (resistivity of 5-10 {omega} cm) were H{sup +} ion implanted with energies between 0.75 and 2.00 MeV, and the electronic transport properties of the implanted layer (recombination lifetime, carrier diffusion coefficient, and front-surface and implanted-interface recombination velocities s{sub 1} and s{sub 2}) were studied using photocarrier radiometry (PCR). A quantitative fitting procedure to the diffusing photoexcited free-carrier density wave was introduced using a relatively simple two-layer PCR model in lieu of the more realistic but substantially more complicated three-layer model. The experimental trends in the transport properties of H{sup +}-implanted Si layers extracted from the PCR amplitude and phase data as functions of implantation energy corroborate a physical model of the implanted layer in which (a) overlayer damage due to the light H{sup +} ions decreases with increased depth of implantation at higher energies (b) the implanted region damage close to the interface is largely decoupled from the overlayer crystallinity, and (c) the concentration of implanted H{sup +} ions decreases at higher implantation energies at the interface, thus decreasing the degree of implantation damage at the interface proper.

  17. Electric-field dependence of photocarrier generation efficiency of organic photoconductors

    SciTech Connect

    Umeda, Minoru

    2015-03-07

    The electric-field dependence of photocarrier generation efficiency has been investigated in several different types of organic photoconductor for electrophotography to elucidate the controlling factors of light-to-electrical energy conversion. The rate-determining step in generating photocarriers has been considered to be the charge transfer between two neighboring molecules. Overall photocarrier generation efficiency has been determined using the charge transfer velocity at the rate-determining step as a function of electric-field-dependent activation energy, which is influenced by the symmetry factor α and the energy gap ΔE. The formula used successfully fits the experimental data for different types of organic photoconductor over a wide field strengths range. From the fitting results of high-sensitivity photoconductors, the zero-field activation energy is small and the reactant lifetime is long. In addition, ΔE is zero, which implies that the hole-electron interaction in the reactant is negligible at the rate-determining step. In contrast, for low-sensitivity photoconductors, the zero-field activation energy is large and the reactant lifetime is short; however, ΔE < 0 and α > 0.5, which suggest that the hole-electron interaction is not negligible. Consequently, the proposed formula well explains the electric-field dependence of photocarrier generation efficiency on the basis of its controlling factors.

  18. Exceptional and Anisotropic Transport Properties of Photocarriers in Black Phosphorus.

    PubMed

    He, Jiaqi; He, Dawei; Wang, Yongsheng; Cui, Qiannan; Bellus, Matthew Z; Chiu, Hsin-Ying; Zhao, Hui

    2015-06-23

    One key challenge in developing postsilicon electronic technology is to find ultrathin channel materials with high charge mobilities and sizable energy band gaps. Graphene can offer extremely high charge mobilities; however, the lack of a band gap presents a significant barrier. Transition metal dichalcogenides possess sizable and thickness-tunable band gaps; however, their charge mobilities are relatively low. Here we show that black phosphorus has room-temperature charge mobilities on the order of 10(4) cm(2) V(-1) s(-1), which are about 1 order of magnitude larger than silicon. We also demonstrate strong anisotropic transport in black phosphorus, where the mobilities along the armchair direction are about 1 order of magnitude larger than in the zigzag direction. A photocarrier lifetime as long as 100 ps is also determined. These results illustrate that black phosphorus is a promising candidate for future electronic and optoelectronic applications.

  19. Electronic Spectroscopy & Dynamics

    SciTech Connect

    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.

  20. Dynamic Transmission Electron Microscopy

    SciTech Connect

    Evans, James E.; Jungjohann, K. L.; Browning, Nigel D.

    2012-10-12

    Dynamic transmission electron microscopy (DTEM) combines the benefits of high spatial resolution electron microscopy with the high temporal resolution of ultrafast lasers. The incorporation of these two components into a single instrument provides a perfect platform for in situ observations of material processes. However, previous DTEM applications have focused on observing structural changes occurring in samples exposed to high vacuum. Therefore, in order to expand the pump-probe experimental regime to more natural environmental conditions, in situ gas and liquid chambers must be coupled with Dynamic TEM. This chapter describes the current and future applications of in situ liquid DTEM to permit time-resolved atomic scale observations in an aqueous environment, Although this chapter focuses mostly on in situ liquid imaging, the same research potential exists for in situ gas experiments and the successful integration of these techniques promises new insights for understanding nanoparticle, catalyst and biological protein dynamics with unprecedented spatiotemporal resolution.

  1. Individual identification of free hole and electron dynamics in CuIn{sub 1−x}Ga{sub x}Se{sub 2} thin films by simultaneous monitoring of two optical transitions

    SciTech Connect

    Okano, Makoto; Hagiya, Hideki; Sakurai, Takeaki; Akimoto, Katsuhiro; Shibata, Hajime; Niki, Shigeru; Kanemitsu, Yoshihiko

    2015-05-04

    The photocarrier dynamics of CuIn{sub 1−x}Ga{sub x}Se{sub 2} (CIGS) thin films were studied using white-light transient absorption (TA) measurements, as an understanding of this behavior is essential for improving the performance of solar cells composed of CIGS thin films. A characteristic double-peak structure due to the splitting of the valence bands in the CIGS was observed in the TA spectra under near-band-gap resonant excitation. From a comparison of the TA decay dynamics monitored at these two peaks, it was found that the slow-decay components of the electron and hole relaxation are on the nanosecond timescale. This finding is clear evidence of the long lifetimes of free photocarriers in polycrystalline CIGS thin films.

  2. Electron Cyclotron Resonances in Electron Cloud Dynamics

    SciTech Connect

    Celata, Christine; Celata, C.M.; Furman, Miguel A.; Vay, J.-L.; Yu, Jennifer W.

    2008-06-25

    We report a previously unknown resonance for electron cloud dynamics. The 2D simulation code"POSINST" was used to study the electron cloud buildup at different z positions in the International Linear Collider positron damping ring wiggler. An electron equilibrium density enhancement of up to a factor of 3 was found at magnetic field values for which the bunch frequency is an integral multiple of the electron cyclotron frequency. At low magnetic fields the effects of the resonance are prominent, but when B exceeds ~;;(2 pi mec/(elb)), with lb = bunch length, effects of the resonance disappear. Thus short bunches and low B fields are required for observing the effect. The reason for the B field dependence, an explanation of the dynamics, and the results of the 2D simulations and of a single-particle tracking code used to elucidate details of the dynamics are discussed.

  3. Optical pump-probe spectroscopy of photocarriers in rubrene single crystals

    NASA Astrophysics Data System (ADS)

    Tao, Shoichi; Matsuzaki, Hiroyuki; Uemura, Hirotaka; Yada, Hiroyuki; Uemura, Takafumi; Takeya, Jun; Hasegawa, Tatsuo; Okamoto, Hiroshi

    2011-02-01

    The photocarrier dynamics of rubrene, an organic molecular semiconductor, are investigated by transient absorption spectroscopy over a wide energy range (0.1-2.2 eV). By photoirradiation, we observed three kinds of absorption bands in the infrared region, which are attributable to induced absorptions of excitons, free carriers, and polarons. The results show that for photoirradiation with energies higher than ˜2.7 eV (˜0.4 eV higher than the lowest exciton energy), free carriers are photogenerated just after the photoirradiation. Some of those free carriers are stabilized as polarons and the others are relaxed to excitons. For the resonant excitation to the lowest-exciton, polarons can also be generated from the excitons. The temperature dependence of the decay dynamics of polarons reveals that polaron mobility increases with decreasing temperature, indicating bandlike transport of large polarons. Below 80 K, photocarriers are trapped by defects or impurities and their decay dynamics are dominated by the escape time from traps.

  4. Dynamic imaging with electron microscopy

    ScienceCinema

    Campbell, Geoffrey; McKeown, Joe; Santala, Melissa

    2016-07-12

    Livermore researchers have perfected an electron microscope to study fast-evolving material processes and chemical reactions. By applying engineering, microscopy, and laser expertise to the decades-old technology of electron microscopy, the dynamic transmission electron microscope (DTEM) team has developed a technique that can capture images of phenomena that are both very small and very fast. DTEM uses a precisely timed laser pulse to achieve a short but intense electron beam for imaging. When synchronized with a dynamic event in the microscope's field of view, DTEM allows scientists to record and measure material changes in action. A new movie-mode capability, which earned a 2013 R&D 100 Award from R&D Magazine, uses up to nine laser pulses to sequentially capture fast, irreversible, even one-of-a-kind material changes at the nanometer scale. DTEM projects are advancing basic and applied materials research, including such areas as nanostructure growth, phase transformations, and chemical reactions.

  5. Dynamic imaging with electron microscopy

    SciTech Connect

    Campbell, Geoffrey; McKeown, Joe; Santala, Melissa

    2014-02-20

    Livermore researchers have perfected an electron microscope to study fast-evolving material processes and chemical reactions. By applying engineering, microscopy, and laser expertise to the decades-old technology of electron microscopy, the dynamic transmission electron microscope (DTEM) team has developed a technique that can capture images of phenomena that are both very small and very fast. DTEM uses a precisely timed laser pulse to achieve a short but intense electron beam for imaging. When synchronized with a dynamic event in the microscope's field of view, DTEM allows scientists to record and measure material changes in action. A new movie-mode capability, which earned a 2013 R&D 100 Award from R&D Magazine, uses up to nine laser pulses to sequentially capture fast, irreversible, even one-of-a-kind material changes at the nanometer scale. DTEM projects are advancing basic and applied materials research, including such areas as nanostructure growth, phase transformations, and chemical reactions.

  6. Electron Dynamics in the Magnetotail

    NASA Technical Reports Server (NTRS)

    Schriver, David

    2001-01-01

    The goal of this research has been to study the effects of electrons on magnetotail dynamics and current sheet structure. The approach is to follow ion trajectories in a global model of the magnetotail, use a Boltzmann approximation to include electrons, and then to update the field model according to the currents that are generated by the cross-tail electric field and/or induced fields. Parallel (and perpendicular) electric fields that form are included through the Boltzmann relation. Transverse electron currents are to be included through adiabatic drift equations.

  7. Electron dynamics in Hall thruster

    NASA Astrophysics Data System (ADS)

    Marini, Samuel; Pakter, Renato

    2015-11-01

    Hall thrusters are plasma engines those use an electromagnetic fields combination to confine electrons, generate and accelerate ions. Widely used by aerospace industries those thrusters stand out for its simple geometry, high specific impulse and low demand for electric power. Propulsion generated by those systems is due to acceleration of ions produced in an acceleration channel. The ions are generated by collision of electrons with propellant gas atoms. In this context, we can realize how important is characterizing the electronic dynamics. Using Hamiltonian formalism, we derive the electron motion equation in a simplified electromagnetic fields configuration observed in hall thrusters. We found conditions those must be satisfied by electromagnetic fields to have electronic confinement in acceleration channel. We present configurations of electromagnetic fields those maximize propellant gas ionization and thus make propulsion more efficient. This work was supported by CNPq.

  8. Photomodulation spectroscopy of photocarrier dynamics, electronic defects and morphology of conducting polymers. Final progress report, October 1, 1989--March 31, 1993

    SciTech Connect

    Vardeny, Z.V.

    1993-03-01

    A variety of techniques were used: CW photomodulation, photomodulation in femtosecond and picosecond time ranges, CW resonant Raman scattering, transient photoinduced Raman scattering, electro-absorption, degenerate four-wave mixing, spin dependent photomodulation, and absorption detected magnetic resonance. The following conducting polymers were studied: polyacetylene, polythiophene, polydiacetylene 4-BCMU, polydiethynylsilanes, polysilane embedded in a-Si:H matrix, and fullerenes.

  9. Structural Dynamics of Electronic Systems

    NASA Astrophysics Data System (ADS)

    Suhir, E.

    2013-03-01

    The published work on analytical ("mathematical") and computer-aided, primarily finite-element-analysis (FEA) based, predictive modeling of the dynamic response of electronic systems to shocks and vibrations is reviewed. While understanding the physics of and the ability to predict the response of an electronic structure to dynamic loading has been always of significant importance in military, avionic, aeronautic, automotive and maritime electronics, during the last decade this problem has become especially important also in commercial, and, particularly, in portable electronics in connection with accelerated testing of various surface mount technology (SMT) systems on the board level. The emphasis of the review is on the nonlinear shock-excited vibrations of flexible printed circuit boards (PCBs) experiencing shock loading applied to their support contours during drop tests. At the end of the review we provide, as a suitable and useful illustration, the exact solution to a highly nonlinear problem of the dynamic response of a "flexible-and-heavy" PCB to an impact load applied to its support contour during drop testing.

  10. Electron dynamics in metallic nanoparticles

    NASA Astrophysics Data System (ADS)

    Bigot, J.-Y.; Halté, V.; Merle, J.-C.; Daunois, A.

    2000-01-01

    We studied the dynamics of electrons in copper and silver nanoparticles embedded in a transparent matrix, using the technique of pump-probe femtosecond spectroscopy. Comparative measurements are made in thin films of the same metals. In the case of the nanoparticles, the electron dynamics is strongly influenced by the surface at the boundary of the metal and the surrounding dielectric matrix. A detailed study of the pump-probe signals near the plasmon resonance of the nanoparticles reveals the importance of electron-electron scattering during several hundreds of femtoseconds. The influence of these scattering processes on the real and imaginary parts of the metal dielectric function is compared in the nanoparticles and thin films. In addition, the non-thermal component of the electrons and the heat transfer to the surrounding dielectric are measured. The results are analyzed with a model of effective medium, where the metal dielectric function is described in the random phase approximation, including the surface effects in a phenomenological way.

  11. Photoresponse enhancement in graphene/silicon infrared detector by controlling photocarrier collection

    NASA Astrophysics Data System (ADS)

    Tang, Xin; Zhang, Hengkai; Tang, Xiaobing; Lai, King W. C.

    2016-07-01

    Graphene/silicon junction based photodetectors have attracted great interest due to their superior characteristics like large photosensitive area, fast photocarrier collection and low dark current. Currently, the weak optical absorption and short photocarrier lifetime of graphene remain major limitations for detection of infrared light with wavelengths above 1.2 μm. Here, we elucidate the mechanism of photocarrier transport in graphene/silicon junction based photodetector and propose a theoretical model to study the design and effect of finger-electrode structures on the photocurrent in graphene. We demonstrate that the top finger-like electrode in graphene/silicon photodetector can be designed to enhance the photocarrier collection efficiency in graphene by reducing the average transport distance of photocarriers. Therefore, the photoresponsivity of the graphene/silicon junction based photodetector can be increased. Our results have successfully demonstrated that by optimizing the design of finger electrodes, 4 times enhancement of photocurrents in graphene can be obtained at room temperature.

  12. Dynamics of electrons and nuclei

    NASA Astrophysics Data System (ADS)

    Deumens, Erik; Öhrn, Yngve

    2010-11-01

    This paper presents the theory of Electron Nuclear Dynamics (END), which was developed and applied over the past 20 years or so in collaboration with a group of talented graduate students and postdoctoral associates. The Introduction presents the gist of this theoretical and computational approach to the study of molecular transformations. The next section outlines the major achievements of this time-dependent, direct, and non-adiabatic theory to the study of chemical change.

  13. Realization of dynamical electronic systems

    NASA Astrophysics Data System (ADS)

    Hammari, Elena; Catthoor, Francky; Iasemidis, Leonidas; Kjeldsberg, Per Gunnar; Huisken, Jos; Tsakalis, Konstantinos

    2014-04-01

    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.

  14. Dynamical effects in electron spectroscopy

    NASA Astrophysics Data System (ADS)

    Zhou, Jianqiang Sky; Kas, J. J.; Sponza, Lorenzo; Reshetnyak, Igor; Guzzo, Matteo; Giorgetti, Christine; Gatti, Matteo; Sottile, Francesco; Rehr, J. J.; Reining, Lucia

    2015-11-01

    One of the big challenges of theoretical condensed-matter physics is the description, understanding, and prediction of the effects of the Coulomb interaction on materials properties. In electronic spectra, the Coulomb interaction causes a renormalization of energies and change of spectral weight. Most importantly, it can lead to new structures, often called satellites. These can be linked to the coupling of excitations, also termed dynamical effects. State-of-the-art methods in the framework of many-body perturbation theory, in particular, the widely used GW approximation, often fail to describe satellite spectra. Instead, approaches based on a picture of electron-boson coupling such as the cumulant expansion are promising for the description of plasmon satellites. In this work, we give a unified derivation of the GW approximation and the cumulant expansion for the one-body Green's function. Using the example of bulk sodium, we compare the resulting spectral functions both in the valence and in the core region, and we discuss the dispersion of quasi-particles and satellites. We show that self-consistency is crucial to obtain meaningful results, in particular, at large binding energies. Very good agreement with experiment is obtained when the intrinsic spectral function is corrected for extrinsic and interference effects. Finally, we sketch how one can approach the problem in the case of the two-body Green's function, and we discuss the cancellation of various dynamical effects that occur in that case.

  15. Dynamical effects in electron spectroscopy

    SciTech Connect

    Zhou, Jianqiang Sky Reshetnyak, Igor; Giorgetti, Christine; Sottile, Francesco; Reining, Lucia; Kas, J. J.; Rehr, J. J.; Sponza, Lorenzo; Guzzo, Matteo; Gatti, Matteo

    2015-11-14

    One of the big challenges of theoretical condensed-matter physics is the description, understanding, and prediction of the effects of the Coulomb interaction on materials properties. In electronic spectra, the Coulomb interaction causes a renormalization of energies and change of spectral weight. Most importantly, it can lead to new structures, often called satellites. These can be linked to the coupling of excitations, also termed dynamical effects. State-of-the-art methods in the framework of many-body perturbation theory, in particular, the widely used GW approximation, often fail to describe satellite spectra. Instead, approaches based on a picture of electron-boson coupling such as the cumulant expansion are promising for the description of plasmon satellites. In this work, we give a unified derivation of the GW approximation and the cumulant expansion for the one-body Green’s function. Using the example of bulk sodium, we compare the resulting spectral functions both in the valence and in the core region, and we discuss the dispersion of quasi-particles and satellites. We show that self-consistency is crucial to obtain meaningful results, in particular, at large binding energies. Very good agreement with experiment is obtained when the intrinsic spectral function is corrected for extrinsic and interference effects. Finally, we sketch how one can approach the problem in the case of the two-body Green’s function, and we discuss the cancellation of various dynamical effects that occur in that case.

  16. Dynamical effects in electron spectroscopy.

    PubMed

    Zhou, Jianqiang Sky; Kas, J J; Sponza, Lorenzo; Reshetnyak, Igor; Guzzo, Matteo; Giorgetti, Christine; Gatti, Matteo; Sottile, Francesco; Rehr, J J; Reining, Lucia

    2015-11-14

    One of the big challenges of theoretical condensed-matter physics is the description, understanding, and prediction of the effects of the Coulomb interaction on materials properties. In electronic spectra, the Coulomb interaction causes a renormalization of energies and change of spectral weight. Most importantly, it can lead to new structures, often called satellites. These can be linked to the coupling of excitations, also termed dynamical effects. State-of-the-art methods in the framework of many-body perturbation theory, in particular, the widely used GW approximation, often fail to describe satellite spectra. Instead, approaches based on a picture of electron-boson coupling such as the cumulant expansion are promising for the description of plasmon satellites. In this work, we give a unified derivation of the GW approximation and the cumulant expansion for the one-body Green's function. Using the example of bulk sodium, we compare the resulting spectral functions both in the valence and in the core region, and we discuss the dispersion of quasi-particles and satellites. We show that self-consistency is crucial to obtain meaningful results, in particular, at large binding energies. Very good agreement with experiment is obtained when the intrinsic spectral function is corrected for extrinsic and interference effects. Finally, we sketch how one can approach the problem in the case of the two-body Green's function, and we discuss the cancellation of various dynamical effects that occur in that case. PMID:26567648

  17. Electron Dynamics in Perpendicular Shocks

    NASA Astrophysics Data System (ADS)

    Muschietti, L.; Roth, I.

    2003-12-01

    A full particle electromagnetic code in the Darwin approximation is used to investigate the dynamics of the electrons in a fast magnetosonic shock. We assume a perpendicular geometry where x points into the shock and the electromagnetic field structure is E=(Ex,E_y,0) and B=(0,0,Bz). The 1D3V code has open boundaries with upstream and downstream particles traversing the left and right boundaries, respectively, while the shock structure remains in the simulation box. Two shock strengths are considered, including a near critical shock with alfvenic Mach number Ma ˜ 2 and a supercritical shock with Ma ˜ 3--4. The simulation is initiated by loading the particles according to profiles modeled from conservation laws (Rankine-Hugoniot). Particles and fields are then left to evolve and, once the ion dynamics develops, a self-consistent shock structure forms. Importantly, due to the partial decoupling of ions and electrons which occurs in the magnetic ramp, the electrostatic field Ex builds up a large spike whose role is to slow down the ions. In the supercritical case a significant fraction of ions are reflected and accumulate in the foot, which leads to the process of cyclical shock reformation. We record the trajectories of selected electrons in order to analyse their behavior in the cross field structure of the ramp. We specially look for a possible ``superadiabatic heating'', a process described by previous authors [Balikhin and Gedalin (1994); Ball and Galloway (1998)]. The latter is expected to occur for extreme cases where the gradient of the electrostatic potential, which reflects the ions, is so strong that the electrons are accelerated across a large fraction of the ramp during one cyclotron gyration. The required potential difference across the ramp δ φ * depends upon its half width Δ , namely eδ φ*/mve^2≈(0.2/βe)~(Δ /λe; )2(r+1)2. Here, λ e is the electron inertia length c/ω pe and r is the compression ratio. Our study improves upon the above

  18. A General Design Rule to Manipulate Photocarrier Transport Path in Solar Cells and Its Realization by the Plasmonic-Electrical Effect

    NASA Astrophysics Data System (ADS)

    Sha, Wei E. I.; Zhu, Hugh L.; Chen, Luzhou; Chew, Weng Cho; Choy, Wallace C. H.

    2015-02-01

    It is well known that transport paths of photocarriers (electrons and holes) before collected by electrodes strongly affect bulk recombination and thus electrical properties of solar cells, including open-circuit voltage and fill factor. For boosting device performance, a general design rule, tailored to arbitrary electron to hole mobility ratio, is proposed to decide the transport paths of photocarriers. Due to a unique ability to localize and concentrate light, plasmonics is explored to manipulate photocarrier transport through spatially redistributing light absorption at the active layer of devices. Without changing the active materials, we conceive a plasmonic-electrical concept, which tunes electrical properties of solar cells via the plasmon-modified optical field distribution, to realize the design rule. Incorporating spectrally and spatially configurable metallic nanostructures, thin-film solar cells are theoretically modelled and experimentally fabricated to validate the design rule and verify the plasmonic-tunable electrical properties. The general design rule, together with the plasmonic-electrical effect, contributes to the evolution of emerging photovoltaics.

  19. A general design rule to manipulate photocarrier transport path in solar cells and its realization by the plasmonic-electrical effect.

    PubMed

    Sha, Wei E I; Zhu, Hugh L; Chen, Luzhou; Chew, Weng Cho; Choy, Wallace C H

    2015-01-01

    It is well known that transport paths of photocarriers (electrons and holes) before collected by electrodes strongly affect bulk recombination and thus electrical properties of solar cells, including open-circuit voltage and fill factor. For boosting device performance, a general design rule, tailored to arbitrary electron to hole mobility ratio, is proposed to decide the transport paths of photocarriers. Due to a unique ability to localize and concentrate light, plasmonics is explored to manipulate photocarrier transport through spatially redistributing light absorption at the active layer of devices. Without changing the active materials, we conceive a plasmonic-electrical concept, which tunes electrical properties of solar cells via the plasmon-modified optical field distribution, to realize the design rule. Incorporating spectrally and spatially configurable metallic nanostructures, thin-film solar cells are theoretically modelled and experimentally fabricated to validate the design rule and verify the plasmonic-tunable electrical properties. The general design rule, together with the plasmonic-electrical effect, contributes to the evolution of emerging photovoltaics. PMID:25686578

  20. A General Design Rule to Manipulate Photocarrier Transport Path in Solar Cells and Its Realization by the Plasmonic-Electrical Effect

    PubMed Central

    Sha, Wei E. I.; Zhu, Hugh L.; Chen, Luzhou; Chew, Weng Cho; Choy, Wallace C. H.

    2015-01-01

    It is well known that transport paths of photocarriers (electrons and holes) before collected by electrodes strongly affect bulk recombination and thus electrical properties of solar cells, including open-circuit voltage and fill factor. For boosting device performance, a general design rule, tailored to arbitrary electron to hole mobility ratio, is proposed to decide the transport paths of photocarriers. Due to a unique ability to localize and concentrate light, plasmonics is explored to manipulate photocarrier transport through spatially redistributing light absorption at the active layer of devices. Without changing the active materials, we conceive a plasmonic-electrical concept, which tunes electrical properties of solar cells via the plasmon-modified optical field distribution, to realize the design rule. Incorporating spectrally and spatially configurable metallic nanostructures, thin-film solar cells are theoretically modelled and experimentally fabricated to validate the design rule and verify the plasmonic-tunable electrical properties. The general design rule, together with the plasmonic-electrical effect, contributes to the evolution of emerging photovoltaics. PMID:25686578

  1. UV Laser Photocarrier Radiometry of c-Silicon with Surface Thin Hydrogenated Amorphous Si Film

    NASA Astrophysics Data System (ADS)

    Melnikov, A.; Mandelis, A.; Halliop, B.; Kherani, N. P.

    2015-06-01

    Photocarrier radiometry (PCR) with 355 nm laser excitation was used for the study of c-Si covered with intrinsic thin hydrogenated amorphous Si (i-a-Si:H) on one, or both, sides, with thicknesses ranging from 10 nm to 90 nm. Short wavelength excitation allows one to resolve the contribution of the upper i-a-S layer to the PCR signal due to the very small absorption depth (tens of nm) of the excitation beam. As a result, fundamental transport parameters of the composite structure can be evaluated from the PCR frequency dependence. A theoretical model has been developed to describe the diffuse carrier density wave (CDW) in this two-layer system. The model of the one-dimensional CDW fields for composite electronic solids involves front, interface, and back surface recombination velocities, the diffusion coefficient, recombination lifetimes in the upper and lower layers, and the unoccupied trap density at the interface. Simulations of the transport parameter influence on the PCR signal were performed, and the theoretical model was able to describe the experimental data accurately, therefore, making it possible to evaluate the transport parameters of i-a-Si:H and c-Si as well as to elucidate the role of interface electronic traps in the PCR frequency dependence under short wavelength excitation.

  2. AgI microplate monocrystals with polar {0001} facets: spontaneous photocarrier separation and enhanced photocatalytic activity.

    PubMed

    Kuang, Qin; Zheng, Xiaoli; Yang, Shihe

    2014-02-24

    Elucidating the facet-dependent photocatalytic activity of semiconductor photocatalysts is important in improving the overall efficiency of photocatalysis. Furthermore, combining facet control with selective deposition of oxidation and/or reduction cocatalysts on specific faces of semiconductor photocatalysts is potentially an effective strategy to synergistically optimize the functionality of photocatalysts. In the present study, high-purity wurtzite-type β-AgI platelet microcrystals with polar {0001} facets were prepared by a facile polyvinylpyrrolidone-assisted precipitation reaction. The polar-faceted AgI microplates were used as archetypes to demonstrate preferential diametric migration (i.e., effective separation) of photogenerated electrons and holes along the c axis. Such vectorial electron-hole separation stems from the asymmetric surface structures, which give rise to distinct photoexcited reaction behaviors on the ±(0001) polar facets of wurtzite-type semiconductors. Furthermore, on selective deposition of Ag and MnOx (1.5photocarriers. PMID:24449437

  3. Nonadiabatic evolution of electronic states by electron nuclear dynamics theory

    NASA Astrophysics Data System (ADS)

    Hagelberg, Frank

    The problem of how to determine the nonadiabatic content of any given dynamic process involving molecular motion is addressed in the context of Electron Nuclear Dynamics (END) theory. Specifically, it is proposed to cast the dynamic END wave function into the language of static electronic configurations with time dependent complex-valued amplitudes. This is achieved by adiabatic transport of an electronic basis along the classical nuclear trajectories of the studied molecular system, as yielded by END simulation. Projecting the dynamic wave function on this basis yields a natural distinction between adiabatic and nonadiabatic components of the motion considered. Tracing the evolution of the leading configurations is shown to be a helpful device for clarifying the physical nature of electronic excitation processes. For illustration of these concepts, dynamic configuration analysis is applied to the scattering of a proton by a lithium atom.

  4. Dynamical simulations of strongly correlated electron materials

    NASA Astrophysics Data System (ADS)

    Kress, Joel; Barros, Kipton; Batista, Cristian; Chern, Gia-Wei; Kotliar, Gabriel

    We present a formulation of quantum molecular dynamics that includes electron correlation effects via the Gutzwiller method. Our new scheme enables the study of the dynamical behavior of atoms and molecules with strong electron interactions. The Gutzwiller approach goes beyond the conventional mean-field treatment of the intra-atomic electron repulsion and captures crucial correlation effects such as band narrowing and electron localization. We use Gutzwiller quantum molecular dynamics to investigate the Mott transition in the liquid phase of a single-band metal and uncover intriguing structural and transport properties of the atoms.

  5. Probing photo-carrier collection efficiencies of individual silicon nanowire diodes on a wafer substrate

    NASA Astrophysics Data System (ADS)

    Schmitt, S. W.; Brönstrup, G.; Shalev, G.; Srivastava, S. K.; Bashouti, M. Y.; Döhler, G. H.; Christiansen, S. H.

    2014-06-01

    Vertically aligned silicon nanowire (SiNW) diodes are promising candidates for the integration into various opto-electronic device concepts for e.g. sensing or solar energy conversion. Individual SiNW p-n diodes have intensively been studied, but to date an assessment of their device performance once integrated on a silicon substrate has not been made. We show that using a scanning electron microscope (SEM) equipped with a nano-manipulator and an optical fiber feed-through for tunable (wavelength, power using a tunable laser source) sample illumination, the dark and illuminated current-voltage (I-V) curve of individual SiNW diodes on the substrate wafer can be measured. Surprisingly, the I-V-curve of the serially coupled system composed of SiNW/wafers is accurately described by an equivalent circuit model of a single diode and diode parameters like series and shunting resistivity, diode ideality factor and photocurrent can be retrieved from a fit. We show that the photo-carrier collection efficiency (PCE) of the integrated diode illuminated with variable wavelength and intensity light directly gives insight into the quality of the device design at the nanoscale. We find that the PCE decreases for high light intensities and photocurrent densities, due to the fact that considerable amounts of photo-excited carriers generated within the substrate lead to a decrease in shunting resistivity of the SiNW diode and deteriorate its rectification. The PCE decreases systematically for smaller wavelengths of visible light, showing the possibility of monitoring the effectiveness of the SiNW device surface passivation using the shown measurement technique. The integrated device was pre-characterized using secondary ion mass spectrometry (SIMS), TCAD simulations and electron beam induced current (EBIC) measurements to validate the properties of the characterized material at the single SiNW diode level.Vertically aligned silicon nanowire (SiNW) diodes are promising candidates for

  6. Trap State Effects in PbS Colloidal Quantum Dot Exciton Kinetics Using Photocarrier Radiometry Intensity and Temperature Measurements

    NASA Astrophysics Data System (ADS)

    Wang, Jing; Mandelis, Andreas; Melnikov, Alexander; Sun, Qiming

    2016-06-01

    Colloidal quantum dots (CQDs) have attracted significant interest for applications in electronic and optoelectronic devices such as photodetectors, light-emitting diodes, and solar cells. However, a poor understanding of charge transport in these nanocrystalline films hinders their practical applications. The photocarrier radiometry (PCR) technique, a frequency-domain photoluminescence method spectrally gated for monitoring radiative recombination photon emissions while excluding thermal infrared photons due to non-radiative recombination, has been applied to PbS CQD thin films for the analysis of charge transport properties. Linear excitation intensity responses of PCR signals were found in the reported experimental conditions. The type and influence of trap states in the coupled PbS CQD thin film were analyzed with PCR temperature- and time-dependent results.

  7. Probing photo-carrier collection efficiencies of individual silicon nanowire diodes on a wafer substrate.

    PubMed

    Schmitt, S W; Brönstrup, G; Shalev, G; Srivastava, S K; Bashouti, M Y; Döhler, G H; Christiansen, S H

    2014-07-21

    Vertically aligned silicon nanowire (SiNW) diodes are promising candidates for the integration into various opto-electronic device concepts for e.g. sensing or solar energy conversion. Individual SiNW p-n diodes have intensively been studied, but to date an assessment of their device performance once integrated on a silicon substrate has not been made. We show that using a scanning electron microscope (SEM) equipped with a nano-manipulator and an optical fiber feed-through for tunable (wavelength, power using a tunable laser source) sample illumination, the dark and illuminated current-voltage (I-V) curve of individual SiNW diodes on the substrate wafer can be measured. Surprisingly, the I-V-curve of the serially coupled system composed of SiNW/wafers is accurately described by an equivalent circuit model of a single diode and diode parameters like series and shunting resistivity, diode ideality factor and photocurrent can be retrieved from a fit. We show that the photo-carrier collection efficiency (PCE) of the integrated diode illuminated with variable wavelength and intensity light directly gives insight into the quality of the device design at the nanoscale. We find that the PCE decreases for high light intensities and photocurrent densities, due to the fact that considerable amounts of photo-excited carriers generated within the substrate lead to a decrease in shunting resistivity of the SiNW diode and deteriorate its rectification. The PCE decreases systematically for smaller wavelengths of visible light, showing the possibility of monitoring the effectiveness of the SiNW device surface passivation using the shown measurement technique. The integrated device was pre-characterized using secondary ion mass spectrometry (SIMS), TCAD simulations and electron beam induced current (EBIC) measurements to validate the properties of the characterized material at the single SiNW diode level.

  8. On electronic representations in molecular reaction dynamics

    NASA Astrophysics Data System (ADS)

    Killian, Benjamin J.

    For many decades, the field of chemical reaction dynamics has utilized computational methods that rely on potential energy surfaces that are constructed using stationary-state calculations. These methods are typically devoid of dynamical couplings between the electronic and nuclear degrees of freedom, a fact that can result in incorrect descriptions of dynamical processes. Often, non-adiabatic coupling expressions are included in these methodologies. The Electron-Nuclear Dynamics (END) formalism, in contrast, circumvents these deficiencies by calculating all intermolecular forces directly at each time step in the dynamics and by explicitly maintaining all electronic-nuclear couplings. The purpose of this work is to offer two new frameworks for implementing electronic representations in dynamical calculations. Firstly, a new schema is proposed for developing atomic basis sets that are consistent with dynamical calculations. Traditionally, basis sets have been designed for use in stationary-state calculations of the structures and properties of molecules in their ground states. As a consequence of common construction techniques that utilize energy optimization methods, the unoccupied orbitals bear little resemblance to physical virtual atomic orbitals. We develop and implement a method for basis set construction that relies upon physical properties of atomic orbitals and that results in meaningful virtual orbitals. These basis sets are shown to provide a significant improvement in the accuracy of calculated dynamical properties such as charge transfer probabilities. Secondly, the theoretical framework of END is expanded to incorporate a multi-configurational representation for electrons. This formalism, named Vector Hartree-Fock, is based in the theory of vector coherent states and utilizes a complete active space electronic representation. The Vector Hartree-Fock method is fully disclosed, with derivation of the equations of motion. The expressions for the equation

  9. Hot electron dynamics in graphene

    SciTech Connect

    Ling, Meng-Chieh

    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

  10. Electron and Proton Auroral Dynamics

    NASA Technical Reports Server (NTRS)

    Mende, S. B.; Frey, H. U.; Gerard, J. C.; Hubert, B.; Fuselier, S.; Spann, J. F., Jr.; Gladstone, R.; Burch, J. L.; Rose, M. Franklin (Technical Monitor)

    2000-01-01

    Data from the Wide-band Imaging Camera (WIC) sensitive to far ultraviolet auroras and from the Spectrographic Imager (SI) channel SI12, sensitive to proton precipitation induced Lyman alpha were analyzed during a high altitude orbit segment of the IMAGE spacecraft. This segment began during the expansive phase of a substorm. The aurora changed into a double oval configuration, consisting of a set of discrete pole-ward forms and a separate diffuse auroral oval equatorwards, Although IMF Bz was strongly southward considerable activity could be seen poleward of the discrete auroras in the region that was considered to be the polar cap. The SI12 Doppler shifted Lyman alpha signature of precipitating protons show that the proton aurora is on the equatorward side of the diffuse aurora. In the following several hours the IMF Bz field changed signed. Although the general character of the proton and electron aurora did not change, the dayside aurora moved equatorward when the Bz was negative and more bright aurora was seen in the central polar cap during periods of positive Bz.

  11. Electron correlation dynamics in atoms and molecules.

    PubMed

    Nest, M; Ludwig, M; Ulusoy, I; Klamroth, T; Saalfrank, P

    2013-04-28

    In this paper, we present quantum dynamical calculations on electron correlation dynamics in atoms and molecules using explicitly time-dependent ab initio configuration interaction theory. The goals are (i) to show that in which cases it is possible to switch off the electronic correlation by ultrashort laser pulses, and (ii) to understand the temporal evolution and the time scale on which it reappears. We characterize the appearance of correlation through electron-electron scattering when starting from an uncorrelated state, and we identify pathways for the preparation of a Hartree-Fock state from the correlated, true ground state. Exemplary results for noble gases, alkaline earth elements, and selected molecules are provided. For Mg we show that the uncorrelated state can be prepared using a shaped ultrashort laser pulse.

  12. Cyclotron Resonances in Electron Cloud Dynamics

    SciTech Connect

    Celata, C. M.; Furman, Miguel A.; Vay, J.-L.; Ng, J. S.T.; Grote, D. P.; Pivi, M. T. F.; Wang, L. F.

    2009-04-29

    A new set of resonances for electron cloud dynamics in the presence of a magnetic field has been found. For short beam bunch lengths and low magnetic fields where lb<< 2pi c/omega c (with lb = bunch length, omega c = non-relativistic cyclotron frequency) resonances between the bunch frequency and harmonics of the electron cyclotron frequency cause an increase in the electron cloud density in narrow ranges of magnetic field near the resonances. For ILC parameters the increase in the density is up to a factor ~;;3, and the spatial distribution of the electrons is broader near resonances, lacking the well-defined vertical density"stripes" found for non-resonant cases. Simulations with the 2D computer code POSINST, as well as a single-particle tracking code, were used to elucidate the physics of the dynamics. The existence of the resonances has been confirmed in experiments at PEP-II. The resonances are expected to affect the electron cloud dynamics in the fringe fields of conventional lattice magnets and in wigglers, where the magnetic fields are low. Results of the simulations and experimental observations, the reason for the bunch-length dependence, and details of the dynamics are discussed here.

  13. Electron Dynamics Near a Charged Radiator

    SciTech Connect

    Dufty, James W.; Wrighton, Jeffrey M.

    2008-10-22

    Time correlation functions for electron dynamics near a positively charged radiator are described by a mean field kinetic theory that is exact in the short time limit. The important case of the electric field autocorrelation function is examined and the dependence on radiator charge number is shown to be dominated by the bound states of the electron-ion potential. A very simple practical model is proposed and shown to be accurate over a wide range of electron-ion coupling conditions. The model is expected to be useful for more complex conditions confronted in recent theories for line shapes.

  14. Protein electron transfer: Dynamics and statistics

    NASA Astrophysics Data System (ADS)

    Matyushov, Dmitry V.

    2013-07-01

    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

  15. Cyclotron Resonances in Electron Cloud Dynamics

    SciTech Connect

    Celata, C M; Furman, M A; Vay, J L; Grote, D P; Ng, J T; Pivi, M F; Wang, L F

    2009-05-05

    A new set of resonances for electron cloud dynamics in the presence of a magnetic field has been found. For short beam bunch lengths and low magnetic fields where l{sub b} << 2{pi}{omega}{sub c}, (l{sub b} = bunch duration, {omega}{sub c} = non-relativistic cyclotron frequency) resonances between the bunch frequency and harmonics of the cyclotron frequency cause an increase in the electron cloud density in narrow ranges of magnetic field near the resonances. For ILC parameters the increase in the density is up to a factor {approx} 3, and the spatial distribution of the electrons is broader near resonances, lacking the well-defined density 'stripes' of multipactoring found for non-resonant cases. Simulations with the 2D computer code POSINST, as well as a single-particle tracking code, were used to elucidate the physics of the dynamics. The resonances are expected to affect the electron cloud dynamics in the fringe fields of conventional lattice magnets and in wigglers, where the magnetic fields are low. Results of the simulations, the reason for the bunch-length dependence, and details of the dynamics will be discussed.

  16. Electron dynamics and its control in molecules

    NASA Astrophysics Data System (ADS)

    de Vivie-Riedle, Regina

    2014-03-01

    The accessibility of few femtosecond or even attoseconds pulses opens the door to direct observation of electron dynamics. The idea to steer chemical reactions by localization of electronic wavepackets is intriguing, since electrons are directly involved in bond breaking and formation. The formation of a localized electronic wavepacket requires the superposition of two or more appropriate electronic states. Its guidance is only possible within the coherence time of the system and has to be synchronized with the vibrational molecular motions. In theoretical studies we elucidate the role of electron wavepacket motion for the control of molecular processes. We give three examples with direct connection to experiments. From our analysis, we extract the systems requirements defining the time window for intramolecular electronic coherence, the basis for efficient control. Based on these findings we map out a photoreaction that allows direct control by guiding electronic wavepackets. The carrier envelope of a femtosecond few cycle IR pulse is the control parameter that steers the photoreaction through a conical intersection.

  17. Dynamics of electron transfer in amine photooxidation

    SciTech Connect

    Peters, K.S.; Freilich, S.C.; Schaeffer, C.G.

    1980-08-13

    Studies were initiated utilizing picosecond (ps) absorption spectroscopy, to directly monitor the dynamics of electron transfer from 1,4-diazabicyclo(2.2.2)octane (Dabco) to the excited states of benzophenone and fluorenone. These two systems were chosen because of their contrasting photochemistry. The quantum yield for photoreduction of benzophenone in polar solvents is generally greater than 0.1, while that of fluorenone is zero. In polar solvents, the proposed mechanism dictates that an electron is transferred to the excited singlet state fluorenone, which then back-transfers the electron, regenerating ground-state fluorenone and amine. Photolysis of benzophenone in the presence of an amine transfers an electron to an excited triplet state, forming an ion pair that is stable relative to diffusional separation. The results of this study verify this proposal.

  18. Ultrafast electronic dynamics driven by nuclear motion

    NASA Astrophysics Data System (ADS)

    Vendrell, Oriol

    2016-05-01

    The transfer of electrical charge on a microscopic scale plays a fundamental role in chemistry, in biology, and in technological applications. In this contribution, we will discuss situations in which nuclear motion plays a central role in driving the electronic dynamics of photo-excited or photo-ionized molecular systems. In particular, we will explore theoretically the ultrafast transfer of a double electron hole between the functional groups of glycine after K-shell ionization and subsequent Auger decay. Although a large energy gap of about 15 eV initially exists between the two electronic states involved and coherent electronic dynamics play no role in the hole transfer, we will illustrate how the double hole can be transferred within 3 to 4 fs between both functional ends of the glycine molecule driven solely by specific nuclear displacements and non-Born-Oppenheimer effects. This finding challenges the common wisdom that nuclear dynamics of the molecular skeleton are unimportant for charge transfer processes at the few-femtosecond time scale and shows that they can even play a prominent role. We thank the Hamburg Centre for Ultrafast Imaging and the Volkswagen Foundation for financial support.

  19. Probing Structural and Electronic Dynamics with Ultrafast Electron Microscopy

    SciTech Connect

    Plemmons, DA; Suri, PK; Flannigan, DJ

    2015-05-12

    In this Perspective, we provide an overview,of the field of ultrafast electron microscopy (UEM). We begin by briefly discussing the emergence of methods for probing ultrafast structural dynamics and the information that can be obtained. Distinctions are drawn between the two main types a probes for femtosecond (fs) dynamics fast electrons and X-ray photons and emphasis is placed on hour the nature of charged particles is exploited in ultrafast electron-based' experiments:. Following this, we describe the versatility enabled by the ease with which electron trajectories and velocities can be manipulated with transmission electron microscopy (TEM): hardware configurations, and we emphasize how this is translated to the ability to measure scattering intensities in real, reciprocal, and energy space from presurveyed and selected rianoscale volumes. Owing to decades of ongoing research and development into TEM instrumentation combined with advances in specimen holder technology, comprehensive experiments can be conducted on a wide range of materials in various phases via in situ methods. Next, we describe the basic operating concepts, of UEM, and we emphasize that its development has led to extension of several of the formidable capabilities of TEM into the fs domain, dins increasing the accessible temporal parameter spade by several orders of magnitude. We then divide UEM studies into those conducted in real (imaging), reciprocal (diffraction), and energy (spectroscopy) spate. We begin each of these sections by providing a brief description of the basic operating principles and the types of information that can be gathered followed by descriptions of how these approaches are applied in UM, the type of specimen parameter space that can be probed, and an example of the types of dynamics that can be resolved. We conclude with an Outlook section, wherein we share our perspective on some future directions of the field pertaining to continued instrument development and

  20. Electron Dynamics in Finite Quantum Systems

    NASA Astrophysics Data System (ADS)

    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. Dynamics of Attosecond Electron Wave Packets

    NASA Astrophysics Data System (ADS)

    Mauritsson, Johan

    2005-05-01

    We present results from some of the first experimental studies of attosecond electron wave packets created via the absorption of ultrashort extreme ultraviolet (XUV) light pulses [1]. The pulses, made via high harmonic generation, form an attosecond pulse train (APT) whose properties we can manipulate by a combination of spatial and spectral filtering. For instance, we show that on-target attosecond pulses of 170 as duration, which is close to the single cycle limit, can be produced [2]. The electron wave packets created when such an APT is used to ionize an atom are different from the tunneling wave packets familiar from strong field ionization. We show how to measure the dynamics of these wave packets in a strong infrared (IR) field, where the absorption of energy above the ionization threshold is found to depend strongly on the APT-IR delay [3]. We also demonstrate that altering the properties of the initial electron wave packet by manipulating the APT changes the subsequent continuum electron dynamics. Finally, we show how the phase of a longer, femtosecond electron wave packet can be modulated by a moderately strong IR pulse with duration comparable to or shorter than that of the electron wave packet. This experiment reveals how the normal ponderomotive shift of an XUV ionization event is modified when the IR pulse is shorter than the XUV pulse.[1] The experiments were done at Lund Institute of Technology, Sweden.[2] R. López-Martens, et al., Phys. Rev. Lett. 94, 033001 (2005)[3] P. Johnsson, et al., submitted to Phys. Rev. Lett.

  2. Electron and hole dynamics in amorphous silicon

    SciTech Connect

    Werner, A.; Kunst, M.

    1988-07-01

    Charge carrier dynamics in doped and undoped hydrogenated amorphous silicon (a-Si:H) films is studied by contactless time-resolved photoconductivity measurements. Subband-gap and above band-gap excitation are used to generate excess mobile charge carriers. In undoped a-Si:H the electron decay at charge carrier concentrations larger than 10/sup 16/ cm/sup -3/ is mainly due to an electron-hole recombination which is controlled by hole dispersion. n doping introduces hole traps which increase the effective electron lifetime drastically as they quench this electron-hole recombination channel. At high n-doping levels the electron decay becomes faster due to an increase of the concentration of recombination centers upon doping. In lightly doped p-type samples the transient photoconductivity reflects the interaction of mobile holes with states in the valence-band tail. In heavily doped p- and n-type films the majority carriers decay by a second-order recombination process with trapped minority charge carriers. The transport parameters deduced agree with time-of-flight data.

  3. Ultrafast electronic dynamics in laser-excited crystalline bismuth

    NASA Astrophysics Data System (ADS)

    Melnikov, A.; Misochko, O.; Chekalin, S.

    2013-03-01

    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

  4. Dynamic spin susceptibility of interacting electron systems

    NASA Astrophysics Data System (ADS)

    Zyuzin, Vladimir; Maslov, Dmitrii

    2015-03-01

    We study the dynamic spin susceptibility of interacting electrons in spatial dimensions from one to three. In all cases, backscattering processes result in non-zero imaginary part of the spin susceptibility above the particle-hole continuum of non-interacting electrons. In one dimension, we employ the renormalization group to go beyond the second order and obtain a general expression for the spin susceptibility. In higher dimensions, we show that the imaginary part of the spin susceptibility arises from the same mechanism as non-analytic corrections to the Fermi-liquid theory. We relate the obtained results to the lifetime of collective spin modes. This work was supported by the National Science Foundation via Grant NSF DMR-1308972.

  5. Determination of photocarrier density under continuous photoirradiation using spectroscopic techniques as applied to polymer: Fullerene blend films

    SciTech Connect

    Kanemoto, Katsuichi Nakatani, Hitomi; Domoto, Shinya

    2014-10-28

    We propose a method to determine the density of photocarrier under continuous photoirradiation in conjugated polymers using spectroscopic signals obtained by photoinduced absorption (PIA) measurements. The bleaching signals in the PIA measurements of polymer films and the steady-state absorption signals of oxidized polymer solution are employed to determine the photocarrier density. The method is applied to photocarriers of poly (3-hexylthiophene) (P3HT) in a blended film consisting of P3HT and [6,6]-phenyl C61 butyric acid methyl ester (PCBM). The photocarrier density under continuous photoirradiation of 580 mW/cm{sup 2} is determined to be 3.5 × 10{sup 16 }cm{sup −3}. Using a trend of the carrier density increasing in proportion to the square root of photo-excitation intensity, we provide a general formula to estimate the photocarrier density under simulated 1 sun solar irradiation for the P3HT: PCBM film of an arbitrary thickness. We emphasize that the method proposed in this study enables an estimate of carrier density without measuring a current and can be applied to films with no electrodes as well as to devices.

  6. Noncontacting laser photocarrier radiometric depth profilometry of harmonically modulated band bending in the space-charge layer at doped SiO{sub 2}-Si interfaces

    SciTech Connect

    Mandelis, Andreas; Batista, Jerias; Gibkes, Juergen; Pawlak, Michael; Pelzl, Josef

    2005-04-15

    Laser infrared photocarrier radiometry (PCR) was used with a harmonically modulated low-power laser pump and a superposed dc superband-gap optical bias (a secondary laser beam) to control and monitor the space-charge-layer (SCL) width in oxidized p-Si-SiO{sub 2} and n-Si-SiO{sub 2} interfaces (wafers) exhibiting charged interface-state related band bending. Applying the theory of PCR-SCL dynamics [A. Mandelis, J. Appl. Phys. 97, 083508 (2005)] to the experiments yielded various transport parameters of the samples as well as depth profiles of the SCL exhibiting complete ( p-type Si) or partial (n-type Si) band flattening, to a degree controlled by widely different minority-carrier capture cross section at each interface. The uncompensated charge density at the interface was also calculated from the theory.

  7. Dynamically programmable electronic pill dispenser system.

    PubMed

    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. PMID:20503621

  8. Characterization of nano-depth junctions in silicon by using Photo-Carrier Radiometry (PCR)

    NASA Astrophysics Data System (ADS)

    Garcia, J. A.; Guo, X.; Mandelis, A.; Shaughnessy, D.; Nicolaides, L.; Salnik, A.

    2008-01-01

    Non-contact, non-intrusive Photo-Carrier Radiometry (PCR) was used for monitoring nano-depth junctions in industrial-grade silicon wafers. The silicon wafers were implanted with arsenic to the dose of 5E1014 cm-2. The junction depth was in the 30 nm to 100 nm range. Quantitative results for PCR sensitivity to the junction depth and implantation energies are presented. This laser-based carrier-wave technique monitors harmonically photo-excited and recombining carriers and shows great potential advantages for the characterization of multiple semiconductor processes such as ion implantation, ultra shallow junction (USJ) depth determination and other Si wafer process steps.

  9. Ionized impurity induced photocarrier generation in organic energy conversion systems

    NASA Astrophysics Data System (ADS)

    Popovic, Z. D.

    1982-07-01

    The present study has the objective to investigate the influence of the discrete nature of ionized impurities in a Schottky barrier on the field dependent carrier generation of an organic photovoltaic cell. Attention is given to the influence of the local ionized impurity field on the carrier generation, compared to the influence of the average field in the barrier. It is assumed that exciton dissociation into electron-hole pairs can be adequately described as a function of the local electric field. The proposal is made that thermal regeneration of ionized impurities can lead to continuous charge production based on the proposed mechanism. The study has been motivated by a significant discrepancy observed between the measured and calculated carrier generation efficiencies in x-metal-free phthalocyanine photovoltaic cells. The proposed mechanism of ionized impurity-assisted carrier generation offers an explanation for the observed enhancement in x-metal-free phthalocyanine photovoltaic cells.

  10. Origin of Photocarrier Losses in Iron Pyrite (FeS2) Nanocubes.

    PubMed

    Shukla, Sudhanshu; Xing, Guichuan; Ge, Hu; Prabhakar, Rajiv Ramanujam; Mathew, Sinu; Su, Zhenghua; Nalla, Venkatram; Venkatesan, Thirumalai; Mathews, Nripan; Sritharan, Thirumany; Sum, Tze Chien; Xiong, Qihua

    2016-04-26

    Iron pyrite has received significant attention due to its high optical absorption. However, the loss of open circuit voltage (Voc) prevents its further application in photovoltaics. Herein, we have studied the photophysics of pyrite by ultrafast laser spectroscopy to understand fundamental limitation of low Voc by quantifying photocarrier losses in high quality, stoichiometric, and phase pure {100} faceted pyrite nanocubes. We found that fast carrier localization of photoexcited carriers to indirect band edge and shallow trap states is responsible for major carrier loss. Slow relaxation component reflects high density of defects within the band gap which is consistent with the observed Mott-variable range hopping (VRH) conduction from transport measurements. Magnetic measurements strikingly show the magnetic ordering associated with phase inhomogeneity, such as FeS2-δ (0 ≤ δ ≤ 1). This implies that improvement of iron pyrite solar cell performance lies in mitigating the intrinsic defects (such as sulfur vacancies) by blocking the fast carrier localization process. Photocarrier generation and relaxation model is presented by comprehensive analysis. Our results provide insight into possible defects that induce midgap states and facilitate rapid carrier relaxation before collection. PMID:26962638

  11. Effective interface state effects in hydrogenated amorphous-crystalline silicon heterostructures using ultraviolet laser photocarrier radiometry

    NASA Astrophysics Data System (ADS)

    Melnikov, A.; Mandelis, A.; Halliop, B.; Kherani, N. P.

    2013-12-01

    Ultraviolet photocarrier radiometry (UV-PCR) was used for the characterization of thin-film (nanolayer) intrinsic hydrogenated amorphous silicon (i-a-Si:H) on c-Si. The small absorption depth (approximately 10 nm at 355 nm laser excitation) leads to strong influence of the nanolayer parameters on the propagation and recombination of the photocarrier density wave (CDW) within the layer and the substrate. A theoretical PCR model including the presence of effective interface carrier traps was developed and used to evaluate the transport parameters of the substrate c-Si as well as those of the i-a-Si:H nanolayer. Unlike conventional optoelectronic characterization methods such as photoconductance, photovoltage, and photoluminescence, UV-PCR can be applied to more complete quantitative characterization of a-Si:H/c-Si heterojunction solar cells, including transport properties and defect structures. The quantitative results elucidate the strong effect of a front-surface passivating nanolayer on the transport properties of the entire structure as the result of effective a-Si:H/c-Si interface trap neutralization through occupation. A further dramatic improvement of those properties with the addition of a back-surface passivating nanolayer is observed and interpreted as the result of the interaction of the increased excess bulk CDW with, and more complete occupation and neutralization of, effective front interface traps.

  12. Effective interface state effects in hydrogenated amorphous-crystalline silicon heterostructures using ultraviolet laser photocarrier radiometry

    SciTech Connect

    Melnikov, A.; Mandelis, A.; Halliop, B.; Kherani, N. P.

    2013-12-28

    Ultraviolet photocarrier radiometry (UV-PCR) was used for the characterization of thin-film (nanolayer) intrinsic hydrogenated amorphous silicon (i-a-Si:H) on c-Si. The small absorption depth (approximately 10 nm at 355 nm laser excitation) leads to strong influence of the nanolayer parameters on the propagation and recombination of the photocarrier density wave (CDW) within the layer and the substrate. A theoretical PCR model including the presence of effective interface carrier traps was developed and used to evaluate the transport parameters of the substrate c-Si as well as those of the i-a-Si:H nanolayer. Unlike conventional optoelectronic characterization methods such as photoconductance, photovoltage, and photoluminescence, UV-PCR can be applied to more complete quantitative characterization of a-Si:H/c-Si heterojunction solar cells, including transport properties and defect structures. The quantitative results elucidate the strong effect of a front-surface passivating nanolayer on the transport properties of the entire structure as the result of effective a-Si:H/c-Si interface trap neutralization through occupation. A further dramatic improvement of those properties with the addition of a back-surface passivating nanolayer is observed and interpreted as the result of the interaction of the increased excess bulk CDW with, and more complete occupation and neutralization of, effective front interface traps.

  13. Electronic Structure and Dynamics of Nitrosyl Porphyrins

    PubMed Central

    Scheidt, W. Robert; Barabanschikov, Alexander; Pavlik, Jeffrey W.; Silvernail, Nathan J.; Sage, J. Timothy

    2010-01-01

    fully successful at capturing the interaction between the axial NO and imidazole ligands. This supports previous conclusions that hemeNO complexes exhibit an unusual degree of variability with respect to computational method, and we speculate that this variability hints at a genuine electronic instability that a protein can exploit to tune reactivity. We anticipate that ongoing characterization of heme-NO complexes will deepen our understanding of their structure, dynamics, and reactivity. PMID:20666384

  14. Electron dynamics in a plasma focus. [electron acceleration

    NASA Technical Reports Server (NTRS)

    Hohl, F.; Gary, S. P.; Winters, P. A.

    1977-01-01

    Results are presented of a numerical integration of the three-dimensional relativistic equations of motion of electrons subject to given electric and magnetic fields deduced from experiments. Fields due to two different models are investigated. For the first model, the fields are those due to a circular distribution of axial current filaments. As the current filaments collapse toward the axis, large azimuthal magnetic and axial electric fields are induced. These fields effectively heat the electrons to a temperature of approximately 8 keV and accelerate electrons within the radius of the filaments to high axial velocities. Similar results are obtained for the current-reduction phase of focus formation. For the second model, the fields are those due to a uniform current distribution. Both the current-reduction and the compression phases were studied. These is little heating or acceleration of electrons during the compression phase because the electrons are tied to the magnetic field. However, during the current-reduction phase, electrons near the axis are accelerated toward the center electrode and reach energies of 100 keV. A criterion is obtained which limits the runaway electron current to about 400 A.

  15. Vibrational- and Laser-Driven Electronic Dynamics in the Molecules

    NASA Astrophysics Data System (ADS)

    Stolow, Albert

    2014-05-01

    Electronic dynamics within molecules can be driven by both motions of the atoms, via non-Born-Oppenheimer coupling, and by applied laser fields, driving electron motions on sub-cycle time scales. The challenging but most general case of Molecular Dynamics is where electronic and vibrational motions are fully coupled, the making and breaking of chemical bonds being the most prominent example. Time-Resolved Coincidence Imaging Spectroscopy (TRCIS) is a ultrafast photoelectron probe of Molecular Frame dynamics in polyatomic molecules. It makes use of full 3D recoil momentum vector determination of coincident photoions and photoelectrons as a function of time, permitting observations of coupled electronic-vibrational dynamics from the Molecular Frame rather than the Lab Frame point of view. Methods in non-resonant quantum control, based on the dynamic Stark effect, have also emerged as important tools for enhancing molecular dynamics studies. In particular, molecular alignment can fix the Molecular Frame within the Lab Frame, avoiding loss of information due to orientational averaging. Provided that the molecular dynamics are fast compared to rotational dephasing, this method also permits time-resolved Molecular Frame observations. As laser fields get stronger, a sub-cycle (attosecond) physics emerges, leading to new probes of driven multi-electron dynamics in polyatomic molecules. Understanding driven multi-electron responses will be central to advancing attosecond science towards polyatomic molecules and complex systems.

  16. Electronic and Ionic Transport Dynamics in Organolead Halide Perovskites.

    PubMed

    Li, Dehui; Wu, Hao; Cheng, Hung-Chieh; Wang, Gongming; Huang, Yu; Duan, Xiangfeng

    2016-07-26

    Ion migration has been postulated as the underlying mechanism responsible for the hysteresis in organolead halide perovskite devices. However, the electronic and ionic transport dynamics and how they impact each other in organolead halide perovskites remain elusive to date. Here we report a systematic investigation of the electronic and ionic transport dynamics in organolead halide perovskite microplate crystals and thin films using temperature-dependent transient response measurements. Our study reveals that thermally activated ionic and electronic conduction coexist in perovskite devices. The extracted activation energies suggest that the electronic transport is easier, but ions migrate harder in microplates than in thin films, demonstrating that the crystalline quality and grain boundaries can fundamentally modify electronic and ionic transport in perovskites. These findings offer valuable insight on the electronic and ionic transport dynamics in organolead halide perovskites, which is critical for optimizing perovskite devices with reduced hysteresis and improved stability and efficiency.

  17. Social Dynamics within Electronic Networks of Practice

    ERIC Educational Resources Information Center

    Mattson, Thomas A., Jr.

    2013-01-01

    Electronic networks of practice (eNoP) are special types of electronic social structures focused on discussing domain-specific problems related to a skill-based craft or profession in question and answer style forums. eNoP have implemented peer-to-peer feedback systems in order to motivate future contributions and to distinguish contribution…

  18. ELECTRON COUD DYNAMICS IN HIGH-INTENSITY RINGS.

    SciTech Connect

    WANG, L.; WEI, J.

    2005-05-16

    Electron cloud due to beam-induced multipacting is one of the main concerns for the high intensity. Electrons generated and accumulated inside the beam pipe form an ''electron cloud'' that interacts with the circulating charged particle beam. With sizeable amount of electrons, this interaction can cause beam instability, beam loss and emittance growth. At the same time, the vacuum pressure will rise due to electron desorption. This talk intends to provide an overview of the mechanism and dynamics of the typical electron multipacting in various magnetic fields and mitigation measures with different beams.

  19. Runaway electron dynamics in tokamak plasmas with high impurity content

    SciTech Connect

    Martín-Solís, J. R.; Loarte, A.; Lehnen, M.

    2015-09-15

    The dynamics of high energy runaway electrons is analyzed for plasmas with high impurity content. It is shown that modified collision terms are required in order to account for the collisions of the relativistic runaway electrons with partially stripped impurity ions, including the effect of the collisions with free and bound electrons, as well as the scattering by the full nuclear and the electron-shielded ion charge. The effect of the impurities on the avalanche runaway growth rate is discussed. The results are applied, for illustration, to the interpretation of the runaway electron behavior during disruptions, where large amounts of impurities are expected, particularly during disruption mitigation by massive gas injection. The consequences for the electron synchrotron radiation losses and the resulting runaway electron dynamics are also analyzed.

  20. Runaway electron dynamics in tokamak plasmas with high impurity content

    NASA Astrophysics Data System (ADS)

    Martín-Solís, J. R.; Loarte, A.; Lehnen, M.

    2015-09-01

    The dynamics of high energy runaway electrons is analyzed for plasmas with high impurity content. It is shown that modified collision terms are required in order to account for the collisions of the relativistic runaway electrons with partially stripped impurity ions, including the effect of the collisions with free and bound electrons, as well as the scattering by the full nuclear and the electron-shielded ion charge. The effect of the impurities on the avalanche runaway growth rate is discussed. The results are applied, for illustration, to the interpretation of the runaway electron behavior during disruptions, where large amounts of impurities are expected, particularly during disruption mitigation by massive gas injection. The consequences for the electron synchrotron radiation losses and the resulting runaway electron dynamics are also analyzed.

  1. Electron Spin Dynamics in Semiconductor Quantum Dots

    SciTech Connect

    Marie, X.; Belhadj, T.; Urbaszek, B.; Amand, T.; Krebs, O.; Lemaitre, A.; Voisin, P.

    2011-07-15

    An electron spin confined to a semiconductor quantum dot is not subject to the classical spin relaxation mechanisms known for free carriers but it strongly interacts with the nuclear spin system via the hyperfine interaction. We show in time resolved photoluminescence spectroscopy experiments on ensembles of self assembled InAs quantum dots in GaAs that this interaction leads to strong electron spin dephasing.

  2. Imaging the molecular dynamics of dissociative electron attachment to water

    SciTech Connect

    Adaniya, Hidihito; Rudek, B.; Osipov, Timur; Haxton, Dan; Weber, Thorsten; Rescigno, Thomas N.; McCurdy, C.W.; Belkacem, Ali

    2009-10-19

    Momentum imaging experiments on dissociative electron attachment to the water molecule are combined with ab initio theoretical calculations of the angular dependence of the quantum mechanical amplitude for electron attachment to provide a detailed picture of the molecular dynamics of dissociation attachment via the two lowest energy Feshbach resonances. The combination of momentum imaging experiments and theory can reveal dissociation dynamics for which the axial recoil approximation breaks down and thus provides a powerful reaction microscope for DEA to polyatomics.

  3. Ultrafast electronic and spin dynamics in thin iron films: electron-magnon and electron-phonon interactions

    NASA Astrophysics Data System (ADS)

    Carpene, E.; Mancini, E.; Dallera, C.; Brenna, M.; Puppin, E.; De Silvestri, S.

    The electronic and spin dynamics in thin iron films have been investigated by means of time-resolved reflectivity and magneto-optical Kerr effect. The electron-magnon and the electron-phonon coupling times are extrapolated and their influence is discussed.

  4. Entanglement Dynamics of Electrons and Photons

    NASA Astrophysics Data System (ADS)

    Wu, Xiang-Yao; Liu, Xiao-Jing; Lu, Jing-Bin; Li, Tian-Shun; Zhang, Si-Qi; Liang, Yu; Ma, Ji; Li, Hong

    2016-08-01

    Entanglement is a fundamental feature of quantum theory as well as a key resource for quantum computing and quantum communication, but the entanglement mechanism has not been found at present. We think when the two subsystems exist interaction directly or indirectly, they can be in entanglement state. such as, in the Jaynes-Cummings model, the entanglement between the atom and the light field comes from their interaction. In this paper, we have studied the entanglement mechanism of electron-electron and photon-photon, which are from the spin-spin interaction. We found their total entanglement states are relevant both space state and spin state. When two electrons or two photons are far away, their entanglement states should be disappeared even if their spin state is entangled.

  5. Lattice dynamics of neodymium: Influence of 4 f electron correlations

    NASA Astrophysics Data System (ADS)

    Waller, O.; Piekarz, P.; Bosak, A.; Jochym, P. T.; Ibrahimkutty, S.; Seiler, A.; Krisch, M.; Baumbach, T.; Parlinski, K.; Stankov, S.

    2016-07-01

    Incorporation of strong electron correlations into the density functional theory (DFT) for the electronic structure calculations of light lanthanides leads to a modification of interatomic forces and consequently the lattice dynamics. Using first-principles theory we demonstrate the substantial influence of the 4 f electron correlations on the phonon dispersion relations of Nd. The calculations are verified by an inelastic x-ray scattering experiment performed on a single-crystalline Nd(0001) film. We show that very good agreement between the calculated and measured data is achieved when electron-electron interactions are treated by the DFT +U approach.

  6. A model for electron nuclear dynamics of a monatomic chain

    NASA Astrophysics Data System (ADS)

    Calais, Jean-Louis; Deumens, Erik; Ohrn, Yngve

    1994-05-01

    The Electron Nuclear Dynamics (END) approach is developed for a linear chain in a parametrized model inspired by the PPP (Pariser-Parr-Pople) model. Particular attention is given to the model parameters, and the choice of basis functions in this time-dependent theory. The resulting equations of motion include electronic-vibrational couplings. Explicit analysis of the simplest model leads to coupling between the highest frequency longitudinal vibrational mode and the electrons.

  7. A model for electron nuclear dynamics of a monatomic chain

    NASA Astrophysics Data System (ADS)

    Calais, Jean-Louis; Deumens, Erik; Öhrn, Yngve

    1994-09-01

    The electron nuclear dynamics (END) approach is developed for a linear chain in a parametrized model inspired by the PPP (Pariser-Parr-Pople) model. Particular attention is given to the model parameters, and the choice of basis functions in this time-dependent theory. The resulting equations of motion include electronic-vibrational couplings. Explicit analysis of the simplest model leads to coupling between the highest frequency longitudinal vibrational mode and the electrons.

  8. Atomically resolved real-space imaging of hot electron dynamics

    PubMed Central

    Lock, D.; Rusimova, K. R.; Pan, T. L.; Palmer, R. E.; Sloan, P. A.

    2015-01-01

    The dynamics of hot electrons are central to understanding the properties of many electronic devices. But their ultra-short lifetime, typically 100 fs or less, and correspondingly short transport length-scale in the nanometre range constrain real-space investigations. Here we report variable temperature and voltage measurements of the nonlocal manipulation of adsorbed molecules on the Si(111)-7 × 7 surface in the scanning tunnelling microscope. The range of the nonlocal effect increases with temperature and, at constant temperature, is invariant over a wide range of electron energies. The measurements probe, in real space, the underlying hot electron dynamics on the 10 nm scale and are well described by a two-dimensional diffusive model with a single decay channel, consistent with 2-photon photo-emission (2PPE) measurements of the real time dynamics. PMID:26387703

  9. Atomically resolved real-space imaging of hot electron dynamics.

    PubMed

    Lock, D; Rusimova, K R; Pan, T L; Palmer, R E; Sloan, P A

    2015-09-21

    The dynamics of hot electrons are central to understanding the properties of many electronic devices. But their ultra-short lifetime, typically 100 fs or less, and correspondingly short transport length-scale in the nanometre range constrain real-space investigations. Here we report variable temperature and voltage measurements of the nonlocal manipulation of adsorbed molecules on the Si(111)-7 × 7 surface in the scanning tunnelling microscope. The range of the nonlocal effect increases with temperature and, at constant temperature, is invariant over a wide range of electron energies. The measurements probe, in real space, the underlying hot electron dynamics on the 10 nm scale and are well described by a two-dimensional diffusive model with a single decay channel, consistent with 2-photon photo-emission (2PPE) measurements of the real time dynamics.

  10. Dynamical backaction cooling with free electrons

    NASA Astrophysics Data System (ADS)

    Niguès, A.; Siria, A.; Verlot, P.

    2015-09-01

    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.

  11. Dynamical backaction cooling with free electrons

    PubMed Central

    Niguès, A.; Siria, A.; Verlot, P.

    2015-01-01

    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. PMID:26381454

  12. Dynamical backaction cooling with free electrons.

    PubMed

    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.

  13. Ultrafast dynamics of electrons at interfaces

    SciTech Connect

    McNeill, Jason D.

    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

  14. Quantum dynamics of secondary electron emission from nanographene

    NASA Astrophysics Data System (ADS)

    Ueda, Yoshihiro; Suzuki, Yasumitsu; Watanabe, Kazuyuki

    2016-07-01

    We have observed secondary electron emission (SEE) from nanographene by applying time-dependent density functional theory simulations in real-time and real-space to electron scattering on target graphene-flakes. We obtained the incident-electron energy dependence and bilayer effect on the amount of secondary electron (SE). The dynamics of SEE and collective density oscillations, which are electronic excitations induced by electron impact, were demonstrated numerically, and elucidated by the time-dependent occupation numbers of the Kohn-Sham electronic levels. The SE yields from graphene flakes are found to be ˜0.1 . The highest energy of SE is ˜20 eV, which is compatible with the characteristics observed in SEE experiments.

  15. Revealing Dissociative Electron Attachment Dynamics in Polyatomic Molecules Using Momentum Imaging Experiments and Electron Scattering Calculations

    NASA Astrophysics Data System (ADS)

    Belkacem, Ali; Slaughter, Daniel

    2015-05-01

    Understanding electron-driven chemical reactions is important for improving a variety of technological applications such as materials processing and the important role they play in the radiation damage in bulk matter. Furthermore, dissociative electron attachment often exhibits site-selective bond cleavage, which holds promise for prediction and precise control of electron-driven chemical reactions. Recent dynamical studies of these reactions have demonstrated that an understanding of anion dissociation dynamics beyond simple one-dimensional models is crucial in interpreting the measured fragment angular distributions. We combine ion fragment momentum imaging experiments with electron attachment entrance amplitude calculations to interrogate the non-Born-Oppenheimer dynamics of dissociative electron attachment in polyatomic molecules. We will report recent experimental developments in molecules of technological interest including methanol, methane and uracil. Work supported by Chemical Sciences, Geosciences and Biosciences division of BES/DOE.

  16. Electron Dynamics in Nanostructures in Strong Laser Fields

    SciTech Connect

    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.

  17. Dynamics of photoexcited quasiparticles in heavy electron compounds.

    PubMed

    Demsar, Jure; Sarrao, John L; Taylor, Antoinette J

    2006-04-26

    Femtosecond real-time spectroscopy is an emerging new tool for studying low energy electronic structure in correlated electron systems. Motivated by recent advances in understanding the nature of relaxation phenomena in various correlated electron systems (superconductors, density wave systems) the technique has been applied to heavy electron compounds in comparison with their non-magnetic counterparts. While the dynamics in their non-magnetic analogues are similar to the dynamics observed in noble metals (only weak temperature dependences are observed) and can be treated with a simple two-temperature model, the photoexcited carrier dynamics in heavy electron systems show dramatic changes as a function of temperature and excitation level. In particular, below some characteristic temperature the relaxation rate starts to decrease, dropping by more than two orders of magnitude upon cooling down to liquid He temperatures. This behaviour has been consistently observed in various heavy fermion metals as well as Kondo insulators, and is believed to be quite general. In order to account for the experimental observations, two theoretical models have been proposed. The first treats the heavy electron systems as simple metals with very flat electron dispersion near the Fermi level. An electron-phonon thermalization scenario can account for the observed slowing down of the relaxation provided that there exists a mechanism for suppression of electron-phonon scattering when both the initial and final electronic states lie in the region of flat dispersion. An alternative scenario argues that the relaxation dynamics in heavy electron systems are governed by the Rothwarf-Taylor bottleneck, where the dynamics are governed by the presence of a narrow gap in the density of states near the Fermi level. The so-called hybridization gap results from hybridization between localized moments and the conduction electron background. Remarkable agreement with the model suggests that carrier

  18. Electronic transport and dynamics in correlated heterostructures

    NASA Astrophysics Data System (ADS)

    Mazza, G.; Amaricci, A.; Capone, M.; Fabrizio, M.

    2015-05-01

    We investigate by means of the time-dependent Gutzwiller approximation the transport properties of a strongly correlated slab subject to Hubbard repulsion and connected with to two metallic leads kept at a different electrochemical potential. We focus on the real-time evolution of the electronic properties after the slab is connected to the leads and consider both metallic and Mott insulating slabs. When the correlated slab is metallic, the system relaxes to a steady state that sustains a finite current. The zero-bias conductance is finite and independent of the degree of correlations within the slab as long as the system remains metallic. On the other hand, when the slab is in a Mott insulating state, the external bias leads to currents that are exponentially activated by charge tunneling across the Mott-Hubbard gap, consistent with the Landau-Zener dielectric breakdown scenario.

  19. Beam Dynamics Considerations in Electron Ion Colliders

    NASA Astrophysics Data System (ADS)

    Krafft, Geoffrey

    2015-04-01

    The nuclear physics community is converging on the idea that the next large project after FRIB should be an electron-ion collider. Both Brookhaven National Lab and Thomas Jefferson National Accelerator Facility have developed accelerator designs, both of which need novel solutions to accelerator physics problems. In this talk we discuss some of the problems that must be solved and their solutions. Examples in novel beam optics systems, beam cooling, and beam polarization control will be presented. Authored by Jefferson Science Associates, LLC under U.S. DOE Contract No. DE-AC05-06OR23177. The U.S. Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce this manuscript for U.S. Government purposes.

  20. Dynamics of Dissociative Electron Attachment to Methane

    NASA Astrophysics Data System (ADS)

    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.

  1. Electron momentum spectroscopy of aniline taking account of nuclear dynamics in the initial electronic ground state

    NASA Astrophysics Data System (ADS)

    Farasat, M.; Shojaei, S. H. R.; Morini, F.; Golzan, M. M.; Deleuze, M. S.

    2016-04-01

    The electronic structure, electron binding energy spectrum and (e, 2e) momentum distributions of aniline have been theoretically predicted at an electron impact energy of 1.500 keV on the basis of Born-Oppenheimer molecular dynamical simulations, in order to account for thermally induced nuclear motions in the initial electronic ground state. Most computed momentum profiles are rather insensitive to thermally induced alterations of the molecular structure, with the exception of the profiles corresponding to two ionization bands at electron binding energies comprised between ˜10.0 and ˜12.0 eV (band C) and between ˜16.5 and ˜20.0 eV (band G). These profiles are found to be strongly influenced by nuclear dynamics in the electronic ground state, especially in the low momentum region. The obtained results show that thermal averaging smears out most generally the spectral fingerprints that are induced by nitrogen inversion.

  2. Direct observation of electron dynamics in the attosecond domain.

    PubMed

    Föhlisch, A; Feulner, P; Hennies, F; Fink, A; Menzel, D; Sanchez-Portal, D; Echenique, P M; Wurth, W

    2005-07-21

    Dynamical processes are commonly investigated using laser pump-probe experiments, with a pump pulse exciting the system of interest and a second probe pulse tracking its temporal evolution as a function of the delay between the pulses. Because the time resolution attainable in such experiments depends on the temporal definition of the laser pulses, pulse compression to 200 attoseconds (1 as = 10(-18) s) is a promising recent development. These ultrafast pulses have been fully characterized, and used to directly measure light waves and electronic relaxation in free atoms. But attosecond pulses can only be realized in the extreme ultraviolet and X-ray regime; in contrast, the optical laser pulses typically used for experiments on complex systems last several femtoseconds (1 fs = 10(-15) s). Here we monitor the dynamics of ultrafast electron transfer--a process important in photo- and electrochemistry and used in solid-state solar cells, molecular electronics and single-electron devices--on attosecond timescales using core-hole spectroscopy. We push the method, which uses the lifetime of a core electron hole as an internal reference clock for following dynamic processes, into the attosecond regime by focusing on short-lived holes with initial and final states in the same electronic shell. This allows us to show that electron transfer from an adsorbed sulphur atom to a ruthenium surface proceeds in about 320 as. PMID:16034414

  3. Identifying the Stern-Gerlach force of classical electron dynamics.

    PubMed

    Wen, Meng; Bauke, Heiko; Keitel, Christoph H

    2016-01-01

    Different classical theories are commonly applied in various branches of physics to describe the relativistic dynamics of electrons by coupled equations for the orbital motion and spin precession. Exemplarily, we benchmark the Frenkel model and the classical Foldy-Wouthuysen model with spin-dependent forces (Stern-Gerlach forces) to the quantum dynamics as predicted by the Dirac equation. Both classical theories can lead to different or even contradicting predictions how the Stern-Gerlach forces modify the electron's orbital motion, when the electron moves in strong electromagnetic field configurations of emerging high-intensity laser facilities. In this way, one may evaluate the validity and identify the limits of these classical theories via a comparison with possible experiments to provide a proper description of spin-induced dynamics. Our results indicate that the Foldy-Wouthuysen model is qualitatively in better agreement with the Dirac theory than the widely used Frenkel model. PMID:27546820

  4. The Dynamics of Dissociative Electron Attachment to Small Polyatomic Molecules

    NASA Astrophysics Data System (ADS)

    Rescigno, Thomas

    2013-09-01

    Dissociative electron attachment (DEA) is a resonant process in which an electron attaches to a molecule to form an unstable anion which subsequently fragments into stable products. DEA to small polyatomic molecules is often governed by complex electronic and nuclear dynamics that is intrinsically multi-dimensional. One-dimensional treatments of the dissociation dynamics based on resonance scattering theory, while often successful in modeling the energy dependence of total cross sections, can mask the complexity of post-attachment dynamics which is revealed by the observed angular dependence of the reaction products. The dissociation evolves on transient anion potential energy surfaces and often involves conical intersections which can result in a complete breakdown of the axial recoil approximation. I will use the examples of DEA to water, carbon dioxide and methanol to illustrate the discussion. Work performed under auspices of USDOE by LBNL under contract DE-AC02-05CH11231 and supported by OBES, Division of Chemical Sciences.

  5. Identifying the Stern-Gerlach force of classical electron dynamics.

    PubMed

    Wen, Meng; Bauke, Heiko; Keitel, Christoph H

    2016-08-22

    Different classical theories are commonly applied in various branches of physics to describe the relativistic dynamics of electrons by coupled equations for the orbital motion and spin precession. Exemplarily, we benchmark the Frenkel model and the classical Foldy-Wouthuysen model with spin-dependent forces (Stern-Gerlach forces) to the quantum dynamics as predicted by the Dirac equation. Both classical theories can lead to different or even contradicting predictions how the Stern-Gerlach forces modify the electron's orbital motion, when the electron moves in strong electromagnetic field configurations of emerging high-intensity laser facilities. In this way, one may evaluate the validity and identify the limits of these classical theories via a comparison with possible experiments to provide a proper description of spin-induced dynamics. Our results indicate that the Foldy-Wouthuysen model is qualitatively in better agreement with the Dirac theory than the widely used Frenkel model.

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

    PubMed

    Stähler, Julia; Gahl, Cornelius; Wolf, Martin

    2012-01-17

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

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

    PubMed

    Stähler, Julia; Gahl, Cornelius; Wolf, Martin

    2012-01-17

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

  8. Three-layer photocarrier radiometry model of ion-implanted silicon wafers

    NASA Astrophysics Data System (ADS)

    Li, Bincheng; Shaughnessy, Derrick; Mandelis, Andreas; Batista, Jerias; Garcia, Jose

    2004-06-01

    A three-dimensional three-layer model is presented for the quantitative understanding of the infrared photocarrier radiometry (PCR) response of ion-implanted semiconductors, specifically Si. In addition to the implanted layer and intact substrate normally assumed in all existing two-layer theoretical models to describe the photothermal response of ion-implanted semiconductors, a surface layer is considered in this three-layer model to represent a thin, less severally damaged region close to the surface. The effects on the PCR signal of several structural, transport, and optical properties of ion-implanted silicon wafers affected significantly by the ion implantation process (minority carrier lifetime, diffusion coefficient, optical absorption coefficient, thickness of the implanted layer, and front surface recombination velocity) are discussed. The dependence of the PCR signal on the ion implantation dose is theoretically calculated and compared to experimental results. Good agreement between experimental data and theoretical calculations is obtained. Both theoretical and experimental results show the PCR dependence on dose can be separated into four regions with the transition across each region defined by the implantation-induced electrical and optical degrees of damage, respectively, as the electrical and optical damage occurs at different dose ranges. It is also shown that the PCR amplitude decreases monotonically with increasing implantation dose. This monotonic dependence provides the potential of the PCR technique for industrial applications in semiconductor metrology.

  9. Influence of Carrier Transport on Diffraction Efficiency of Steady-State Photocarrier Grating

    NASA Astrophysics Data System (ADS)

    Sun, Q. M.; Wang, Y. F.; Gao, C. M.; Cui, H.

    2015-06-01

    A two-dimensional theoretical model of a diffractive steady-state photocarrier grating (SSPCG) has been developed. The carrier diffusion equation with a spatially periodic excitation source was solved, and an analytical expression of the carrier density distribution was obtained. Based on the band-filling theory and the Kramers-Kronig relation, the carrier-induced refractive index change of SSPCG was estimated, and the refractive index profile was determined. The diffraction efficiency of the SSPCG was calculated by multilevel rigorous coupled-wave analysis. Simulations were carried out to investigate the influence of the carrier transport properties on the diffraction efficiency of the SSPCG. The results show that a semiconductor material with a longer lifetime and a smaller diffusivity will have a higher diffraction efficiency. The spatial amplitude of the carrier density and the grating strength of the SSPCG are closely related to the grating period. For an InP-based SSPCG, the diffraction efficiency of the transmitted wave reaches its maximum value (25 %) when the grating provides a phase shift. The theoretical analysis and conclusions are helpful for material selection and experimental parameter determination of a diffractive SSPCG.

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

    PubMed

    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. Electron dynamics in nanostructures subjected to a laser field

    NASA Astrophysics Data System (ADS)

    Bubin, Sergiy; Driscoll, Joseph; Varga, Kalman

    2010-03-01

    Recent experiments (Zhu et al., J. Appl. Phys. 102, 114302 (2007); Gabor et al., Science, 325, 1367 (2009)) have shown that application of a laser field can significantly influence the electron dynamics in nanostructures. The study of such phenomena is vital both for fundamental understanding as well as for technological applications. We use time-dependent density functional theory to study how laser fields affect electron dynamics in nanostructures. Examples include the enhancement of field emission from carbon nanotubes (CNT) and effects on transport properties of a CNT-based nanowire.

  12. Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses

    NASA Astrophysics Data System (ADS)

    Calegari, F.; Ayuso, D.; Trabattoni, A.; Belshaw, L.; De Camillis, S.; Anumula, S.; Frassetto, F.; Poletto, L.; Palacios, A.; Decleva, P.; Greenwood, J. B.; Martín, F.; Nisoli, M.

    2014-10-01

    In the past decade, attosecond technology has opened up the investigation of ultrafast electronic processes in atoms, simple molecules, and solids. Here, we report the application of isolated attosecond pulses to prompt ionization of the amino acid phenylalanine and the subsequent detection of ultrafast dynamics on a sub-4.5-femtosecond temporal scale, which is shorter than the vibrational response of the molecule. The ability to initiate and observe such electronic dynamics in polyatomic molecules represents a crucial step forward in attosecond science, which is progressively moving toward the investigation of more and more complex systems.

  13. Kinetic modelling of runaway electrons in dynamic scenarios

    NASA Astrophysics Data System (ADS)

    Stahl, A.; Embréus, O.; Papp, G.; Landreman, M.; Fülöp, T.

    2016-11-01

    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 collision operator that conserves momentum and energy 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 simplified avalanche model of Rosenbluth and Putvinskii (1997 Nucl. Fusion 37 1355) can give inaccurate results for the avalanche growth rate (either lower or higher) for many parameters, especially when the average runaway energy is modest, such as during the initial phase of the avalanche multiplication. The developments presented pave the way for improved modelling of runaway-electron dynamics during disruptions or other dynamic events.

  14. Dynamic optometer. [for electronic recording of human lens anterior surface

    NASA Technical Reports Server (NTRS)

    Wilson, D. C.

    1974-01-01

    A dynamic optometer that electronically records the position of the anterior surface of the human lens is described. The geometrical optics of the eye and optometer, and the scattering of light from the lens, are closely examined to determine the optimum conditions for adjustment of the instrument. The light detector and associated electronics are also considered, and the operating conditions for obtaining the best signal-to-noise ratio are determined.

  15. Correlated electron ion dynamics: the excitation of atomic motion by energetic electrons

    NASA Astrophysics Data System (ADS)

    Horsfield, Andrew P.; Bowler, D. R.; Fisher, A. J.; Todorov, Tchavdar N.; Sánchez, Cristián G.

    2005-08-01

    Correlated electron-ion dynamics (CEID) is an extension of molecular dynamics that allows us to introduce in a correct manner the exchange of energy between electrons and ions. The formalism is based on a systematic approximation: small amplitude moment expansion. This formalism is extended here to include the explicit quantum spread of the ions and a generalization of the Hartree-Fock approximation for incoherent sums of Slater determinants. We demonstrate that the resultant dynamical equations reproduce analytically the selection rules for inelastic electron-phonon scattering from perturbation theory, which control the mutually driven excitations of the two interacting subsystems. We then use CEID to make direct numerical simulations of inelastic current-voltage spectroscopy in atomic wires, and to exhibit the crossover from ionic cooling to heating as a function of the relative degree of excitation of the electronic and ionic subsystems.

  16. Electronically Nonadiabatic Dynamics via Semiclassical Initial Value Methods

    SciTech Connect

    Miller, William H.

    2008-12-11

    In the late 1970's Meyer and Miller (MM) [J. Chem. Phys. 70, 3214 (1979)] presented a classical Hamiltonian corresponding to a finite set of electronic states of a molecular system (i.e., the various potential energy surfaces and their couplings), so that classical trajectory simulations could be carried out treating the nuclear and electronic degrees of freedom (DOF) in an equivalent dynamical framework (i.e., by classical mechanics), thereby describing non-adiabatic dynamics in a more unified manner. Much later Stock and Thoss (ST) [Phys. Rev. Lett. 78, 578 (1997)] showed that the MM model is actually not a 'model', but rather a 'representation' of the nuclear-electronic system; i.e., were the MMST nuclear-electronic Hamiltonian taken as a Hamiltonian operator and used in the Schroedinger equation, the exact (quantum) nuclear-electronic dynamics would be obtained. In recent years various initial value representations (IVRs) of semiclassical (SC) theory have been used with the MMST Hamiltonian to describe electronically non-adiabatic processes. Of special interest is the fact that though the classical trajectories generated by the MMST Hamiltonian (and which are the 'input' for an SC-IVR treatment) are 'Ehrenfest trajectories', when they are used within the SC-IVR framework the nuclear motion emerges from regions of non-adiabaticity on one potential energy surface (PES) or another, and not on an average PES as in the traditional Ehrenfest model. Examples are presented to illustrate and (hopefully) illuminate this behavior.

  17. Forecasting relativistic electron flux using dynamic multiple regression models

    NASA Astrophysics Data System (ADS)

    Wei, H.-L.; Billings, S. A.; Surjalal Sharma, A.; Wing, S.; Boynton, R. J.; Walker, S. N.

    2011-02-01

    The forecast of high energy electron fluxes in the radiation belts is important because the exposure of modern spacecraft to high energy particles can result in significant damage to onboard systems. A comprehensive physical model of processes related to electron energisation that can be used for such a forecast has not yet been developed. In the present paper a systems identification approach is exploited to deduce a dynamic multiple regression model that can be used to predict the daily maximum of high energy electron fluxes at geosynchronous orbit from data. It is shown that the model developed provides reliable predictions.

  18. Dynamics of coupled light waves and electron-acoustic waves.

    PubMed

    Shukla, P K; Stenflo, L; Hellberg, M

    2002-08-01

    The nonlinear interaction between coherent light waves and electron-acoustic waves in a two-electron plasma is considered. The interaction is governed by a pair of equations comprising a Schrödinger-like equation for the light wave envelope and a driven (by the light pressure) electron-acoustic wave equation. The newly derived nonlinear equations are used to study the formation and dynamics of envelope light wave solitons and light wave collapse. The implications of our investigation to space and laser-produced plasmas are pointed out.

  19. Electron nuclear dynamics of H + + H 2O collisions

    NASA Astrophysics Data System (ADS)

    Hedström, M.; Morales, J. A.; Deumens, E.; Öhrn, Y.

    1997-11-01

    Proton water collisions at 46 eV in the center of mass frame are studied within the electron nuclear dynamics theory (END). The electronic degrees of freedom are described with a coherent state formulation of determinantal wavefunctions. The nuclei are treated as classical particles but full nonadiabatic couplings are retained. The equations of motion are formulated in a generalized phase space and bypass the use of preconstructed potential energy surfaces. Differential cross sections for inelastic and electron transfer reactions as well as energy transfer are compared with experiment.

  20. Suprathermal electron dynamics and MHD instabilities in a tokamak

    NASA Astrophysics Data System (ADS)

    Kamleitner, J.; Coda, S.; Decker, J.; Graves, J. P.; the TCV Team

    2015-10-01

    The dynamics of suprathermal electrons in the presence of magnetohydrodynamics (MHD) activity and the excitation of MHD modes by suprathermal electrons are studied experimentally to improve the understanding of the interaction of fast particles with MHD instabilities in a tokamak. The study focuses on three different aspects of the internal kink mode with poloidal/toroidal mode number m/n=1/1 : the sawtooth instability, electron fishbones and coupled bursts alternating with sawtooth crashes (CAS), all located where the safety factor (q) profile approaches or takes the value q=1 . New quantitative results on suprathermal electron transport and an investigation of electron acceleration during sawtooth crashes are followed by the characterization of initial electron fishbone observations on the Tokamak à configuration variable (TCV). Finally, m/n=1/1 bursts associated with the sawtooth cycle, coupled to a persisting m/n=2/1 mode and alternating with sawtooth crashes, are discussed, in particular in view of the fast electron dynamics and their role in confinement degradation and mode excitation.

  1. Investigations of ultrafast dynamics in electronically excited alkylbenzenes

    NASA Astrophysics Data System (ADS)

    Liu, Y.; Gerber, T.; Radi, P.; Sych, Y.; Maksyutenko, P.; Knopp, G.

    2013-03-01

    We investigate ultrafast dynamics in electronically excited states of some typical alkylbenzenes by time-resolved two-colour four wave mixing and velocity map imaging as complementary methods. In this context an upgraded double-sided time-resolved velocity map imaging setup is also proposed.

  2. Calculation of Cross Sections in Electron-Nuclear Dynamics

    NASA Astrophysics Data System (ADS)

    Cabrera-Trujillo, R.; Sabin, John R.; Deumens, E.; Öhrn, Y.

    In this work, we present an overview of the study of total and differential cross section calculations within the electron-nuclear dynamics (END). END is a method to solve the time-dependent Schrödinger equation in a non-adiabatic approach to direct dynamics. The method takes advantage of a coherent state representation of the molecular wave function. A quantum-mechanical Lagrangian formulation is employed to approximate the Schrödinger equation, via the time-dependent variational principle, to a set of coupled first-order differential equations in time for the END. We obtain the final wave function for the system allowing the determination of collisional properties of interest, as for example, deflection functions, charge exchange probabilities and amplitudes, and differential cross sections. We discuss the use and selection of basis sets for both the electronic description of the colliding systems as well as for their importance in the description of electron capture. As quantum effects are important in many cases and lacking for classical nuclei, we discuss the Schiff methodology and its advantages over other traditional methods for including semiclassical corrections. Time-lapse rendering of the dynamics of the participating electrons and atomic nuclei provides for a detailed view of dynamical and reactive processes. Comparison to experimental and other theoretical results is provided where appropriate data are available.

  3. Dynamics Of Electronic Excitation Of Solids With Ultrashort Laser Pulse

    SciTech Connect

    Medvedev, Nikita; Rethfeld, Baerbel

    2010-10-08

    When ultrashort laser pulses irradiate a solid, photoabsorption by electrons in conduction band produces nonequilibrium highly energetic free electrons gas. We study the ionization and excitation of the electronic subsystem in a semiconductor and a metal (solid silicon and aluminum, respectively). The irradiating femtosecond laser pulse has a duration of 10 fs and a photon energy of h-bar {omega} = 38 eV. The classical Monte Carlo method is extended to take into account the electronic band structure and Pauli's principle for electrons excited to the conduction band. In the case of semiconductors this applies to the holes as well. Conduction band electrons and valence band holes induce secondary excitation and ionization processes which we simulate event by event. We discuss the transient electron dynamics with respect to the differences between semiconductors and metals. For metals the electronic distribution is split up into two branches: a low energy distribution as a slightly distorted Fermi-distribution and a long high energy tail. For the case of semiconductors it is split into two parts by the band gap. To thermalize, these excited electronic subsystems need longer times than the characteristic pulse duration. Therefore, the analysis of experimental data with femtosecond lasers must be based on non-equilibrium concepts.

  4. Identifying the Stern-Gerlach force of classical electron dynamics

    PubMed Central

    Wen, Meng; Bauke, Heiko; Keitel, Christoph H.

    2016-01-01

    Different classical theories are commonly applied in various branches of physics to describe the relativistic dynamics of electrons by coupled equations for the orbital motion and spin precession. Exemplarily, we benchmark the Frenkel model and the classical Foldy-Wouthuysen model with spin-dependent forces (Stern-Gerlach forces) to the quantum dynamics as predicted by the Dirac equation. Both classical theories can lead to different or even contradicting predictions how the Stern-Gerlach forces modify the electron’s orbital motion, when the electron moves in strong electromagnetic field configurations of emerging high-intensity laser facilities. In this way, one may evaluate the validity and identify the limits of these classical theories via a comparison with possible experiments to provide a proper description of spin-induced dynamics. Our results indicate that the Foldy-Wouthuysen model is qualitatively in better agreement with the Dirac theory than the widely used Frenkel model. PMID:27546820

  5. Ultrafast Electron-Ion Dynamics Near Aluminum Surfaces

    NASA Astrophysics Data System (ADS)

    Schleife, Andre; Wells, Kai; Knewstub, Sam

    Computational physics and materials research have greatly benefited from high-performance computing; modern first-principles simulations allow insight with unprecedented accuracy and detail. Here we use a recent highly parallel implementation of Ehrenfest molecular dynamics based on real-time time-dependent density functional theory to describe non-adiabatic ultrafast electron-ion dynamics using accurate first-principles calculations. We investigate aluminum subject to highly energetic particle radiation (hydrogen projectile) and study energy deposition due to the fast projectiles. Their high velocity makes it necessary to overcome the Born-Oppenheimer approximation. Using our first-principles calculations we study the behavior of fast ions near the surface of aluminum slabs and investigate, for instance, the influence of velocity and impact angle of the projectile ion. From the emerging non-adiabatic electron-ion dynamics we gain insight into the material on an atto-second time scale.

  6. Identifying the Stern-Gerlach force of classical electron dynamics

    NASA Astrophysics Data System (ADS)

    Wen, Meng; Bauke, Heiko; Keitel, Christoph H.

    2016-08-01

    Different classical theories are commonly applied in various branches of physics to describe the relativistic dynamics of electrons by coupled equations for the orbital motion and spin precession. Exemplarily, we benchmark the Frenkel model and the classical Foldy-Wouthuysen model with spin-dependent forces (Stern-Gerlach forces) to the quantum dynamics as predicted by the Dirac equation. Both classical theories can lead to different or even contradicting predictions how the Stern-Gerlach forces modify the electron’s orbital motion, when the electron moves in strong electromagnetic field configurations of emerging high-intensity laser facilities. In this way, one may evaluate the validity and identify the limits of these classical theories via a comparison with possible experiments to provide a proper description of spin-induced dynamics. Our results indicate that the Foldy-Wouthuysen model is qualitatively in better agreement with the Dirac theory than the widely used Frenkel model.

  7. Diagnostic techniques for measuring suprathermal electron dynamics in plasmas (invited)

    SciTech Connect

    Coda, S.

    2008-10-15

    Plasmas, both in the laboratory and in space, are often not in thermodynamic equilibrium, and the plasma electron distribution function is accordingly non-Maxwellian. Suprathermal electron tails can be generated by external drives, such as rf waves and electric fields, or internal ones, such as instabilities and magnetic reconnection. The variety and importance of the phenomena in which suprathermal electrons play a significant role explains an enduring interest in diagnostic techniques to investigate their properties and dynamics. X-ray bremsstrahlung emission has been studied in hot magnetized plasmas for well over two decades, flanked progressively by electron-cyclotron emission in geometries favoring the high-energy end of the distribution function (high-field-side, vertical, oblique emission), by electron-cyclotron absorption, by spectroscopic techniques, and at lower temperatures, by Langmuir probes and electrostatic analyzers. Continuous progress in detector technology and in measurement and analysis techniques, increasingly sophisticated layouts (multichannel and tomographic systems, imaging geometries), and highly controlled suprathermal generation methods (e.g., perturbative rf modulation) have all been brought to bear in recent years on an increasingly detailed, although far from complete, understanding of suprathermal electron dynamics.

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

    NASA Astrophysics Data System (ADS)

    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.

  9. The dynamics of highly excited electronic systems: Applications of the electron force field

    NASA Astrophysics Data System (ADS)

    Su, Julius T.; Goddard, William A.

    2009-12-01

    Highly excited heterogeneous complex materials are essential elements of important processes, ranging from inertial confinement fusion to semiconductor device fabrication. Understanding the dynamics of these systems has been challenging because of the difficulty in extracting mechanistic information from either experiment or theory. We describe here the electron force field (eFF) approximation to quantum mechanics which provides a practical approach to simulating the dynamics of such systems. eFF includes all the normal electrostatic interactions between electrons and nuclei and the normal quantum mechanical description of kinetic energy for the electrons, but contains two severe approximations: first, the individual electrons are represented as floating Gaussian wave packets whose position and size respond instantaneously to various forces during the dynamics; and second, these wave packets are combined into a many-body wave function as a Hartree product without explicit antisymmetrization. The Pauli principle is accounted for by adding an extra spin-dependent term to the Hamiltonian. These approximations are a logical extension of existing approaches to simulate the dynamics of fermions, which we review. In this paper, we discuss the details of the equations of motion and potentials that form eFF, and evaluate the ability of eFF to describe ground-state systems containing covalent, ionic, multicenter, and/or metallic bonds. We also summarize two eFF calculations previously reported on electronically excited systems: (1) the thermodynamics of hydrogen compressed up to ten times liquid density and heated up to 200 000 K; and (2) the dynamics of Auger fragmentation in a diamond nanoparticle, where hundreds of electron volts of excitation energy are dissipated over tens of femtoseconds. These cases represent the first steps toward using eFF to model highly excited electronic processes in complex materials.

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

    SciTech Connect

    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.

  11. Electron-phonon interaction within classical molecular dynamics

    DOE PAGESBeta

    Tamm, A.; Samolyuk, G.; Correa, A. A.; Klintenberg, M.; Aabloo, A.; Caro, A.

    2016-07-14

    Here, we present a model for nonadiabatic classical molecular dynamics simulations that captures with high accuracy the wave-vector q dependence of the phonon lifetimes, in agreement with quantum mechanics calculations. It is based on a local view of the e-ph interaction where individual atom dynamics couples to electrons via a damping term that is obtained as the low-velocity limit of the stopping power of a moving ion in a host. The model is parameter free, as its components are derived from ab initio-type calculations, is readily extended to the case of alloys, and is adequate for large-scale molecular dynamics computermore » simulations. We also show how this model removes some oversimplifications of the traditional ionic damped dynamics commonly used to describe situations beyond the Born-Oppenheimer approximation.« less

  12. Electron-phonon interaction within classical molecular dynamics

    NASA Astrophysics Data System (ADS)

    Tamm, A.; Samolyuk, G.; Correa, A. A.; Klintenberg, M.; Aabloo, A.; Caro, A.

    2016-07-01

    We present a model for nonadiabatic classical molecular dynamics simulations that captures with high accuracy the wave-vector q dependence of the phonon lifetimes, in agreement with quantum mechanics calculations. It is based on a local view of the e -ph interaction where individual atom dynamics couples to electrons via a damping term that is obtained as the low-velocity limit of the stopping power of a moving ion in a host. The model is parameter free, as its components are derived from ab initio-type calculations, is readily extended to the case of alloys, and is adequate for large-scale molecular dynamics computer simulations. We also show how this model removes some oversimplifications of the traditional ionic damped dynamics commonly used to describe situations beyond the Born-Oppenheimer approximation.

  13. Steering continuum electron dynamics by low-energy attosecond streaking

    NASA Astrophysics Data System (ADS)

    Geng, Ji-Wei; Xiong, Wei-Hao; Xiao, Xiang-Ru; Gong, Qihuang; Peng, Liang-You

    2016-08-01

    A semiclassical model is developed to understand the electronic dynamics in the low-energy attosecond streaking. Under a relatively strong infrared (IR) pulse, the low-energy part of photoelectrons initialized by a single attosecond pulse (SAP) can either rescatter with the ionic core and induce interferences structures in the momentum spectra of the ionized electrons or be recaptured into the Rydberg states. The Coulomb potential plays essential roles in both the electron rescattering and recapturing processes. We find that by changing the time delay between the SAP and the IR pulse, the photoelectrons yield or the population of the Rydberg states can be effectively controlled. The present study demonstrates a fascinating way to steer the electron motion in the continuum.

  14. Gated electron sharing within dynamic naphthalene diimide-based oligorotaxanes.

    PubMed

    Avestro, Alyssa-Jennifer; Gardner, Daniel M; Vermeulen, Nicolaas A; Wilson, Eleanor A; Schneebeli, Severin T; Whalley, Adam C; Belowich, Matthew E; Carmieli, Raanan; Wasielewski, Michael R; Stoddart, J Fraser

    2014-04-22

    The controlled self-assembly of well-defined and spatially ordered π-systems has attracted considerable interest because of their potential applications in organic electronics. An important contemporary pursuit relates to the investigation of charge transport across noncovalently coupled components in a stepwise fashion. Dynamic oligorotaxanes, prepared by template-directed methods, provide a scaffold for directing the construction of monodisperse one-dimensional assemblies in which the functional units communicate electronically through-space by way of π-orbital interactions. Reported herein is a series of oligorotaxanes containing one, two, three and four naphthalene diimide (NDI) redox-active units, which have been shown by cyclic voltammetry, and by EPR and ENDOR spectroscopies, to share electrons across the NDI stacks. Thermally driven motions between the neighboring NDI units in the oligorotaxanes influence the passage of electrons through the NDI stacks in a manner reminiscent of the conformationally gated charge transfer observed in DNA. PMID:24623608

  15. Correlated Single Quantum Dot Blinking and Interfacial Electron Transfer Dynamics.

    PubMed

    Jin, Shengye; Hsiang, Jung-Cheng; Zhu, Haiming; Song, Nianhui; Dickson, Robert M; Lian, Tianquan

    2010-08-31

    The electron transfer (ET) dynamics from core/multi-shell (CdSe/CdS(3ML)ZnCdS(2ML)ZnS(2ML)) quantum dots (QDs) to adsorbed Fluorescein (F27) molecules have been studied by single particle spectroscopy to probe the relationship between single QD interfacial electron transfer and blinking dynamics. Electron transfer from the QD to F27 and the subsequent recombination were directly observed by ensemble-averaged transient absorption spectroscopy. Single QD-F27 complexes show correlated fluctuation of fluorescence intensity and lifetime, similar to those observed in free QDs. With increasing ET rate (controlled by F27-to-QD ratio), the lifetime of on states decreases and relative contribution of off states increases. It was shown that ET is active for QDs in on states, the excited state lifetime of which reflects the ET rate, whereas in the off state QD excitons decay by Auger relaxation and ET is not a competitive quenching pathway. Thus, the blinking dynamics of single QDs modulate their interfacial ET activity. Furthermore, interfacial ET provides an additional pathway for generating off states, leading to correlated single QD interfacial ET and blinking dynamics in QD-acceptor complexes. Because blinking is a general phenomenon of single QDs, it appears that the correlated interfacial ET and blinking and the resulting intermittent ET activity are general phenomena for single QDs.

  16. Enhancement of charge ordering by dynamic electron-phonon interaction

    NASA Astrophysics Data System (ADS)

    Singer, Andrej; Fullerton, Eric; Shpyrko, Oleg

    Symmetry breaking and emergence of order is one of the most fascinating phenomena in condensed matter physics and leads to a plethora of intriguing ground states such as in antiferromagnets, Mott insulators, superconductors, and density-wave systems. Exploiting non-equilibrium dynamics of matter following ultrafast external excitation can provide even more striking routes to symmetry-lowered, ordered states, for instance, by accessing hidden equilibrium states in the free-energy landscape or dynamic stabilization of non-equilibrium states. This is remarkable because ultrafast excitation typically creates disorder, reduces the order parameter, and raises the symmetry. Here, we demonstrate for the case of antiferromagnetic chromium that moderate photo-excitation can transiently enhance the charge-density-wave (CDW) order by up to 30% above its equilibrium value, while strong excitation leads to an oscillating, large-amplitude CDW state that persists above the equilibrium transition temperature. Both effects result from dynamic electron-phonon interaction, which provides an efficient mechanism to selectively transform a broad excitation of the electronic order into a well defined, long-lived coherent lattice vibration. This mechanism may be exploited to transiently enhance the order parameter in other systems with coupled electronic and lattice orders. The data was collected at the x-ray free electron laser LCLS at SLAC.

  17. The quantum dynamics of electronically nonadiabatic chemical reactions

    NASA Astrophysics Data System (ADS)

    Truhlar, Donald G.

    1993-04-01

    Considerable progress was achieved on the quantum mechanical treatment of electronically nonadiabatic collisions involving energy transfer and chemical reaction in the collision of an electronically excited atom with a molecule. In the first step, a new diabatic representation for the coupled potential energy surfaces was created. A two-state diabatic representation was developed which was designed to realistically reproduce the two lowest adiabatic states of the valence bond model and also to have the following three desirable features: (1) it is more economical to evaluate; (2) it is more portable; and (3) all spline fits are replaced by analytic functions. The new representation consists of a set of two coupled diabatic potential energy surfaces plus a coupling surface. It is suitable for dynamics calculations on both the electronic quenching and reaction processes in collisions of Na(3p2p) with H2. The new two-state representation was obtained by a three-step process from a modified eight-state diatomics-in-molecules (DIM) representation of Blais. The second step required the development of new dynamical methods. A formalism was developed for treating reactions with very general basis functions including electronically excited states. Our formalism is based on the generalized Newton, scattered wave, and outgoing wave variational principles that were used previously for reactive collisions on a single potential energy surface, and it incorporates three new features: (1) the basis functions include electronic degrees of freedom, as required to treat reactions involving electronic excitation and two or more coupled potential energy surfaces; (2) the primitive electronic basis is assumed to be diabatic, and it is not assumed that it diagonalizes the electronic Hamiltonian even asymptotically; and (3) contracted basis functions for vibrational-rotational-orbital degrees of freedom are included in a very general way, similar to previous prescriptions for locally

  18. The quantum dynamics of electronically nonadiabatic chemical reactions

    NASA Technical Reports Server (NTRS)

    Truhlar, Donald G.

    1993-01-01

    Considerable progress was achieved on the quantum mechanical treatment of electronically nonadiabatic collisions involving energy transfer and chemical reaction in the collision of an electronically excited atom with a molecule. In the first step, a new diabatic representation for the coupled potential energy surfaces was created. A two-state diabatic representation was developed which was designed to realistically reproduce the two lowest adiabatic states of the valence bond model and also to have the following three desirable features: (1) it is more economical to evaluate; (2) it is more portable; and (3) all spline fits are replaced by analytic functions. The new representation consists of a set of two coupled diabatic potential energy surfaces plus a coupling surface. It is suitable for dynamics calculations on both the electronic quenching and reaction processes in collisions of Na(3p2p) with H2. The new two-state representation was obtained by a three-step process from a modified eight-state diatomics-in-molecules (DIM) representation of Blais. The second step required the development of new dynamical methods. A formalism was developed for treating reactions with very general basis functions including electronically excited states. Our formalism is based on the generalized Newton, scattered wave, and outgoing wave variational principles that were used previously for reactive collisions on a single potential energy surface, and it incorporates three new features: (1) the basis functions include electronic degrees of freedom, as required to treat reactions involving electronic excitation and two or more coupled potential energy surfaces; (2) the primitive electronic basis is assumed to be diabatic, and it is not assumed that it diagonalizes the electronic Hamiltonian even asymptotically; and (3) contracted basis functions for vibrational-rotational-orbital degrees of freedom are included in a very general way, similar to previous prescriptions for locally

  19. Electron theory of fast and ultrafast dissipative magnetization dynamics.

    PubMed

    Fähnle, M; Illg, C

    2011-12-14

    For metallic magnets we review the experimental and electron-theoretical investigations of fast magnetization dynamics (on a timescale of ns to 100 ps) and of laser-pulse-induced ultrafast dynamics (few hundred fs). It is argued that for both situations the dominant contributions to the dissipative part of the dynamics arise from the excitation of electron-hole pairs and from the subsequent relaxation of these pairs by spin-dependent scattering processes, which transfer angular momentum to the lattice. By effective field theories (generalized breathing and bubbling Fermi-surface models) it is shown that the Gilbert equation of motion, which is often used to describe the fast dissipative magnetization dynamics, must be extended in several aspects. The basic assumptions of the Elliott-Yafet theory, which is often used to describe the ultrafast spin relaxation after laser-pulse irradiation, are discussed very critically. However, it is shown that for Ni this theory probably yields a value for the spin-relaxation time T(1) in good agreement with the experimental value. A relation between the quantity α characterizing the damping of the fast dynamics in simple situations and the time T(1) is derived. PMID:22089491

  20. Dynamics of two-electron excitations in helium

    SciTech Connect

    Caldwell, C.D.; Menzel, A.; Frigo, S.P.

    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.

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

    SciTech Connect

    Ge, Nien-Hui

    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 dependence of

  2. Dynamic Pattern Formation in Electron-Beam-Induced Etching.

    PubMed

    Martin, Aiden A; Bahm, Alan; Bishop, James; Aharonovich, Igor; Toth, Milos

    2015-12-18

    We report highly ordered topographic patterns that form on the surface of diamond, span multiple length scales, and have a symmetry controlled by the precursor gas species used in electron-beam-induced etching (EBIE). The pattern formation dynamics reveals an etch rate anisotropy and an electron energy transfer pathway that is overlooked by existing EBIE models. We, therefore, modify established theory such that it explains our results and remains universally applicable to EBIE. The patterns can be exploited in controlled wetting, optical structuring, and other emerging applications that require nano- and microscale surface texturing of a wide band-gap material. PMID:26722926

  3. RIS probed dynamical effects in two-electron barium atom

    SciTech Connect

    Camus, Pierre; Cohen, Samuel

    1995-04-01

    We present for Ba Nsnl planetary states an energy level analysis in order to yield values for the Ba{sup +} Ns core polarizabilities. The parametrized effective dipole and quadrupole values extracted from our data for N=7-10 are compared to calculated ones using a static model. Dipole polarizabilities show very close similarities with static values and at the opposite quadrupole polarizabilities exhibit larger discrepancies. These give evidence of non-adiabatic effects between the two asymmetrically excited electrons which are attributed to the increasing strength of dynamical effects on the Ns electron caused by the motion of the outer nl one.

  4. Modeling Crabbing Dynamics in an Electron-Ion Collider

    SciTech Connect

    Castilla, Alejandro; Morozov, Vasiliy S.; Satogata, Todd J.; Delayen, Jean R.

    2015-09-01

    A local crabbing scheme requires π/2 (mod π) horizontal betatron phase advances from an interaction point (IP) to the crab cavities on each side of it. However, realistic phase advances generated by sets of quadrupoles, or Final Focusing Blocks (FFB), between the crab cavities located in the expanded beam regions and the IP differ slightly from π/2. To understand the effect of crabbing on the beam dynamics in this case, a simple model of the optics of the Medium Energy Electron-Ion Collider (MEIC) including local crabbing was developed using linear matrices and then studied numerically over multiple turns (1000 passes) of both electron and proton bunches. The same model was applied to both local and global crabbing schemes to determine the linear-order dynamical effects of the synchro-betatron coupling induced by crabbing.

  5. Electron Dynamics in Intense Laser Fields: A Bohmian Mechanics Study

    NASA Astrophysics Data System (ADS)

    Jooya, Hossein Z.; Telnov, Dmitry A.; Chu, Shih-I.

    2016-05-01

    We study the electron quantum dynamics of atomic hydrogen under intense near infrared laser fields by means of the De Broglie-Bohm's framework of Bohmian mechanics. This method is used to study the mechanism of the multiple plateau generation and the cut-off extension, as the main characteristic features of high order harmonic generation spectrum. Electron multiple recollision dynamics under intense mid-infrared laser fields is also investigated. In this case, the resulting patterns in the high-order harmonic generation and the above-threshold ionization spectra are analyzed by comprehensive picture provided by Bohmian mechanics. The time evolution of individual trajectories is closely studied to address some of the major structural features of the photoelectron angular distributions. This work is partially supported by DOE.

  6. Static and dynamic variational principles for strongly correlated electron systems

    NASA Astrophysics Data System (ADS)

    Potthoff, Michael

    2011-12-01

    The equilibrium state of a system consisting of a large number of strongly interacting electrons can be characterized by its density operator. This gives a direct access to the ground-state energy or, at finite temperatures, to the free energy of the system as well as to other static physical quantities. Elementary excitations of the system, on the other hand, are described within the language of Green's functions, i.e. time- or frequency-dependent dynamic quantities which give a direct access to the linear response of the system subjected to a weak time-dependent external perturbation. A typical example is angle-revolved photoemission spectroscopy which is linked to the single-electron Green's function. Since usually both, the static as well as the dynamic physical quantities, cannot be obtained exactly for lattice fermion models like the Hubbard model, one has to resort to approximations. Opposed to more ad hoc treatments, variational principles promise to provide consistent and controlled approximations. Here, the Ritz principle and a generalized version of the Ritz principle at finite temperatures for the static case on the one hand and a dynamical variational principle for the single-electron Green's function or the self-energy on the other hand are introduced, discussed in detail and compared to each other to show up conceptual similarities and differences. In particular, the construction recipe for non-perturbative dynamic approximations is taken over from the construction of static mean-field theory based on the generalized Ritz principle. Within the two different frameworks, it is shown which types of approximations are accessible, and their respective weaknesses and strengths are worked out. Static Hartree-Fock theory as well as dynamical mean-field theory are found as the prototypical approximations.

  7. Protein dynamics modulated electron transfer kinetics in early stage photosynthesis

    NASA Astrophysics Data System (ADS)

    Kundu, Prasanta; Dua, Arti

    2013-01-01

    A recent experiment has probed the electron transfer kinetics in the early stage of photosynthesis in Rhodobacter sphaeroides for the reaction center of wild type and different mutants [Science 316, 747 (2007)]. By monitoring the changes in the transient absorption of the donor-acceptor pair at 280 and 930 nm, both of which show non-exponential temporal decay, the experiment has provided a strong evidence that the initial electron transfer kinetics is modulated by the dynamics of protein backbone. In this work, we present a model where the electron transfer kinetics of the donor-acceptor pair is described along the reaction coordinate associated with the distance fluctuations in a protein backbone. The stochastic evolution of the reaction coordinate is described in terms of a non-Markovian generalized Langevin equation with a memory kernel and Gaussian colored noise, both of which are completely described in terms of the microscopics of the protein normal modes. This model provides excellent fits to the transient absorption signals at 280 and 930 nm associated with protein distance fluctuations and protein dynamics modulated electron transfer reaction, respectively. In contrast to previous models, the present work explains the microscopic origins of the non-exponential decay of the transient absorption curve at 280 nm in terms of multiple time scales of relaxation of the protein normal modes. Dynamic disorder in the reaction pathway due to protein conformational fluctuations which occur on time scales slower than or comparable to the electron transfer kinetics explains the microscopic origin of the non-exponential nature of the transient absorption decay at 930 nm. The theoretical estimates for the relative driving force for five different mutants are in close agreement with the experimental estimates obtained using electrochemical measurements.

  8. Dynamics of quantal heating in electron systems with discrete spectra

    NASA Astrophysics Data System (ADS)

    Dietrich, Scott; Mayer, William; Vitkalov, Sergey; Bykov, A. A.

    2015-05-01

    The temporal evolution of quantal Joule heating of two-dimensional (2D) electrons in a GaAs quantum well placed in quantizing magnetic fields is studied using a difference-frequency method. The method is based on measurements of the electron conductivity oscillating at the beat frequency f =f1-f2 between two microwaves applied to the 2D system at frequencies f1 and f2. The method provides direct access to the dynamical characteristics of the heating and yields the inelastic-scattering time τi n of 2D electrons. The obtained τi n is strongly temperature dependent, varying from 0.13 ns at 5.5 K to 1 ns at 2.4 K in magnetic field B =0.333 T . When the temperature T exceeds the Landau-level separation, the relaxation rate 1 /τi n is proportional to T2, indicating electron-electron interaction as the dominant mechanism limiting the quantal heating. At lower temperatures, the rate tends to be proportional to T3, indicating considerable contribution from electron-phonon scattering.

  9. Dynamics of Quantal Heating in Electron Systems with Discrete Spectra

    NASA Astrophysics Data System (ADS)

    Mayer, William; Dietrich, Scott; Vitkalov, Sergey; Bykov, Alexey

    2015-03-01

    The temporal evolution of quantal Joule heating of 2D electrons in GaAs quantum well placed in quantizing magnetic fields is studied using a difference frequency method. The method is based on measurements of the electron conductivity oscillating at the beat frequency f =f1 -f2 between two microwaves applied to 2D system at frequencies f1 and f2. The method provides direct access to the dynamical characteristics of the heating and yields the inelastic scattering time τin of 2D electrons. The obtained τin is strongly temperature dependent, varying from 0.13 ns at 5.5K to 1 ns at 2.4K in magnetic field B=0.333T. When temperature T exceeds the Landau level separation the relaxation rate 1 /τin is proportional to T2, indicating the electron-electron interaction as the dominant mechanism limiting the quantal heating. At lower temperatures the rate tends to be proportional to T3, indicating considerable contribution from electron-phonon scattering. This work was supported by the National Science Foundation (DMR 1104503), the Russian Foundation for Basic Research (project no.14-02-01158) and the Ministry of Education and Science of the Russian Federation.

  10. Probing ultrafast electronic and molecular dynamics with free-electron lasers

    NASA Astrophysics Data System (ADS)

    Fang, L.; Osipov, T.; Murphy, B. F.; Rudenko, A.; Rolles, D.; Petrovic, V. S.; Bostedt, C.; Bozek, J. D.; Bucksbaum, P. H.; Berrah, N.

    2014-06-01

    Molecular dynamics is an active area of research, focusing on revealing fundamental information on molecular structures and photon-molecule interaction and with broad impacts in chemical and biological sciences. Experimental investigation of molecular dynamics has been advanced by the development of new light sources and techniques, deepening our understanding of natural processes and enabling possible control and modification of chemical and biomolecular processes. Free-electron lasers (FELs) deliver unprecedented intense and short photon pulses in the vacuum ultraviolet and x-ray spectral ranges, opening a new era for the study of electronic and nuclear dynamics in molecules. This review focuses on recent molecular dynamics investigations using FELs. We present recent work concerning dynamics of molecular interaction with FELs using an intrinsic clock within a single x-ray pulse as well as using an external clock in a pump-probe scheme. We review the latest developments on correlated and coincident spectroscopy in FEL-based research and recent results revealing photo-induced interaction dynamics using these techniques. We also describe new instrumentations to conduct x-ray pump-x-ray probe experiments with spectroscopy and imaging detectors.

  11. Electron dynamics and valley relaxation in 2D semiconductors

    NASA Astrophysics Data System (ADS)

    Gundogdu, Kenan

    2015-03-01

    Single layer transition metal dichalcogenides are 2D semiconducting systems with unique electronic band structure. Two-valley energy bands along with strong spin-orbital coupling lead to valley dependent career spin polarization, which is the basis for recently proposed valleytronic applications. Since the durations of valley population provide the time window in which valley specific processes take place, it is an essential parameter for developing valleytronic devices. These systems also exhibit unusually strong many body affects, such as strong exciton and trion binding, due to reduced dielectric screening of Coulomb interactions. But there is not much known about the impact of strong many particle correlations on spin and valley polarization dynamics. Here we report direct measurements of ultrafast valley specific relaxation dynamics in single layer MoS2 and WS2. We found that excitonic many body interactions significantly contribute to the relaxation process. Biexciton formation reveals hole valley spin relaxation time. Our results also suggest initial fast intervalley electron scattering and electron spin relaxation leads to loss of electron valley polarization, which then facilitates hole valley relaxation via excitonic spin exchange interaction.

  12. Spectral dynamics of a collective free electron maser

    SciTech Connect

    Eecen, P.J.; Schep, T.J.; Tulupov, A.V.

    1995-12-31

    A theoretical and numerical study of the nonlinear spectral dynamics of a Free Electron Maser (FEM) is reported. The electron beam is modulated by a step-tapered undulator consisting of two sections with different strengths and lengths. The sections have equal periodicity and are separated by a field-free gap. The millimeter wave beam is guided through a rectangular corrugated waveguide. The electron energy is rather low and the current density is large, therefore, the FEM operates in the collective (Raman) regime. Results of a computational study on the spectral dynamics of the FEM are presented. The numerical code is based on a multifrequency model in the continuous beam limit with a 3D description of the electron beam. Space-charge forces are included by a Fourier expansion. These forces strongly influence the behaviour of the generated spectrum of the FEM. The linear gain of the FEM is high, therefore, the system quickly reaches the nonlinear regime. In saturation the gain is still relatively high and the spectral signal at the resonant frequency of the second undulator is suppressed. The behaviour of the sidebands is analysed and their dependence on mirror reflectivity and undulator parameters will be discussed.

  13. Dynamic magnetic island coalescence and associated electron acceleration

    SciTech Connect

    Tanaka, Kentaro G.; Fujimoto, Masaki; Badman, Sarah V.; Shinohara, Iku

    2011-02-15

    The system size dependence of electron acceleration during large-scale magnetic island coalescence is studied via a two-dimensional particle-in-cell simulation. Using a simulation box that is larger than those used in previous studies, injection by merging line acceleration and subsequent reacceleration inside a merged island are found to be the mechanisms for producing the most energetic electrons. This finding and knowledge of the reacceleration process enable us to predict that the high energy end of the electron energy spectrum continues to expand as the merged island size increases. Both the merging line acceleration and the reacceleration within a merged island require the island coalescence process to be so dynamic as to involve fast in-flow toward the center of a merged island. Once this condition is met in an early stage of the coalescence, it is likely to stay in the subsequent phase. In other words, if the thin elongated current sheet is initially able to host the dynamic magnetic island coalescence process, it will be a site where repeated upgrades in the maximum energy of electrons occur in a systematic manner.

  14. Time Resolved Phase Transitions via Dynamic Transmission Electron Microscopy

    SciTech Connect

    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.

  15. Dynamics of Azobenzene Dimer Photoisomerization: Electronic and Steric Effects.

    PubMed

    Titov, Evgenii; Granucci, Giovanni; Götze, Jan Philipp; Persico, Maurizio; Saalfrank, Peter

    2016-09-15

    While azobenzenes readily photoswitch in solution, their photoisomerization in densely packed self-assembled monolayers (SAMs) can be suppressed. Reasons for this can be steric hindrance and/or electronic quenching, e.g., by exciton coupling. We address these possibilities by means of nonadiabatic molecular dynamics with trajectory surface hopping calculations, investigating the trans → cis isomerization of azobenzene after excitation into the ππ* absorption band. We consider a free monomer, an isolated dimer and a dimer embedded in a SAM-like environment of additional azobenzene molecules, imitating in this way the gradual transition from an unconstrained over an electronically coupled to an electronically coupled and sterically hindered, molecular switch. Our simulations reveal that in comparison to the single molecule the quantum yield of the trans → cis photoisomerization is similar for the isolated dimer, but greatly reduced in the sterically constrained situation. Other implications of dimerization and steric constraints are also discussed. PMID:27542538

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

    PubMed

    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

  17. Pulsed Power for a Dynamic Transmission Electron Microscope

    SciTech Connect

    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.

  18. Dynamic Phase Shifts in Nanoscale Distance Measurements by Double Electron Electron Resonance (DEER)†

    SciTech Connect

    Bowman, Michael K.; Maryasov, Alexander G.

    2007-04-01

    The off-resonant pump pulse used in double electron electron resonance (DEER) measurements produces dynamic phase shifts that are explained here by simple analytic and vector descriptions of the full range of signal behaviors observed during DEER measurements, including: large phase shifts in the signal; changes in the position and shape of the detected echo; and changes in the signal intensity. The dynamic phase shifts depend on the width, amplitude and offset frequency of the pump pulse. Isolated radicals as well as pairs or clusters of dipolar-coupled radicals have the same dynamic phase shift that is independent of pump pulse delay in a typical measurement. A method of calibrating both the pump pulse offset frequency and the pump pulse field strength is outlined. A vector model is presented that explains the dynamic phase shifts in terms of precessing magnetization that is either spin locked or precessing about the effective pump field during the pump pulse. Implications of the dynamic phase shifts are discussed as they relate to setting up, calibrating and interpreting the results of DEER measurements.

  19. Dynamic electron arc radiotherapy (DEAR): a feasibility study.

    PubMed

    Rodrigues, Anna; Yin, Fang-Fang; Wu, Qiuwen

    2014-01-20

    Compared to other radiation therapy modalities, clinical electron beam therapy has remained practically unchanged for the past few decades even though electron beams with multiple energies are widely available on most linacs. In this paper, we present the concept of dynamic electron arc radiotherapy (DEAR), a new conformal electron therapy technique with synchronized couch motion. DEAR utilizes combination of gantry rotation, couch motion, and dose rate modulation to achieve desirable dose distributions in patient. The electron applicator is kept to minimize scatter and maintain narrow penumbra. The couch motion is synchronized with the gantry rotation to avoid collision between patient and the electron cone. In this study, we investigate the feasibility of DEAR delivery and demonstrate the potential of DEAR to improve dose distributions on simple cylindrical phantoms. DEAR was delivered on Varian's TrueBeam linac in Research Mode. In conjunction with the recorded trajectory log files, mechanical motion accuracies and dose rate modulation precision were analyzed. Experimental and calculated dose distributions were investigated for different energies (6 and 9 MeV) and cut-out sizes (1×10 cm(2) and 3×10 cm(2) for a 15×15 cm(2) applicator). Our findings show that DEAR delivery is feasible and has the potential to deliver radiation dose with high accuracy (root mean square error, or RMSE of <0.1 MU, <0.1° gantry, and <0.1 cm couch positions) and good dose rate precision (1.6 MU min(-1)). Dose homogeneity within ±2% in large and curved targets can be achieved while maintaining penumbra comparable to a standard electron beam on a flat surface. Further, DEAR does not require fabrication of patient-specific shields. These benefits make DEAR a promising technique for conformal radiotherapy of superficial tumors.

  20. Quantum dynamical phenomena of independent electrons in semiconductor superlattices subject to a uniform electric field

    SciTech Connect

    Bouchard, A.M.

    1994-07-27

    This report discusses the following topics: Bloch oscillations and other dynamical phenomena of electrons in semiconductor superlattices; solvable dynamical model of an electron in a one-dimensional aperiodic lattice subject to a uniform electric field; and quantum dynamical phenomena of electrons in aperiodic semiconductor superlattices.

  1. Local spin dynamics with the electron electric dipole moment

    NASA Astrophysics Data System (ADS)

    Fukuda, Masahiro; Soga, Kota; Senami, Masato; Tachibana, Akitomo

    2016-01-01

    The local spin dynamics of the electron is studied from the viewpoint of the electric dipole moment (EDM) of the electron in the framework of the quantum field theory. The improvements of the computational accuracy of the effective electric field (Eeff) for the EDM and the understanding of spin precession are important for the experimental determination of the upper bound of the EDM. Calculations of Eeff in YbF (2Σ1 /2 ), BaF (2Σ1 /2 ), ThO (3Δ1 ), and HF+ (2Π1 /2 ) are performed on the basis of the restricted active space configuration interaction approach by using the four-component relativistic electronic structure calculation. The spin precession is also discussed from the viewpoint of local spin torque dynamics. We show that a contribution to the torque density for the spin is brought into by the EDM. Distributions of the local spin angular momentum density and torque densities induced by external fields in the above molecules are calculated and a property related with large Eeff is discussed.

  2. Ultrafast electronic deactivation dynamics of the rare natural nucleobase hypoxanthine

    NASA Astrophysics Data System (ADS)

    Röttger, Katharina; Siewertsen, Ron; Temps, Friedrich

    2012-05-01

    The electronic deactivation of the 6-oxopurine derivative hypoxanthine, its nucleoside inosine and the nucleotide inosine monophosphate have been studied by femtosecond time-resolved spectroscopy after ππ∗ photoexcitation at λ = 260 nm. The development of a highly sensitive parallel broadband (near-UV/VIS) and single-color (deep-UV) transient absorption setup enabled us to monitor the excited-state decay and the ground-state recovery dynamics in one and the same experiment. The measurements revealed similar relaxation behavior, with time constants of τ1 ≲ 0.1 ps, τ2 ≈ 0.21 ± 0.08 ps and τ3 ≈ 1.8 ± 0.4 ps, for all three investigated molecules. The observed dynamics are assumed to take place through a conical intersection involving an out-of-plane puckering mode of the six-membered ring similar to guanine.

  3. Dynamic-scanning-electron-microscope study of friction and wear

    NASA Technical Reports Server (NTRS)

    Brainard, W. A.; Buckley, D. H.

    1974-01-01

    A friction and wear apparatus was built into a real time scanning electron microscope (SEM). The apparatus and SEM comprise a system which provides the capability of performing dynamic friction and wear experiments in situ. When the system is used in conjunction with dispersive X-ray analysis, a wide range of information on the wearing process can be obtained. The type of wear and variation with speed, load, and time can be investigated. The source, size, and distribution of wear particles can be determined and metallic transferal observed. Some typical results obtained with aluminum, copper, and iron specimens are given.

  4. Structural Preablation Dynamics of Graphite Observed by Ultrafast Electron Crystallography

    SciTech Connect

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

    2008-01-25

    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 carriers reach their equilibrium in less then one picosecond by transferring heat to a subset of strongly coupled optical phonons. The time-resolved diffraction data show that on such a time scale the crystal undergoes a contraction whose velocity depends on the excitation fluence. The contraction is followed by a large expansion which, at sufficiently high fluence, leads to the ablation of entire graphene layers, as recently predicted theoretically.

  5. Observation of Dislocation Dynamics in the Electron Microscope

    SciTech Connect

    Lagow, B W; Robertson, I M; Jouiad, M; Lassila, D H; Lee, T C; Birnbaum, H K

    2001-08-21

    Deformation experiments performed in-situ in the transmission electron microscope have led to an increased understanding of dislocation dynamics. To illustrate the capability of this technique two examples will be presented. In the first example, the processes of work hardening in Mo at room temperature will be presented. These studies have improved our understanding of dislocation mobility, dislocation generation, and dislocation-obstacle interactions. In the second example, the interaction of matrix dislocations with grain boundaries will be described. From such studies predictive criteria for slip transfer through grain boundaries have been developed.

  6. Observation of dislocation dynamics in the electron microscope

    SciTech Connect

    Lagow, B W; Robertson, I M; Jouiad, M; Lassila, D H; Lee, T C; Birnbaum, H K

    2001-01-17

    Deformation experiments performed in-situ in the transmission electron microscope have led to an increased understanding of dislocation dynamics. To illustrate the capability of this technique two examples will be presented. In the first example, the processes of work hardening in Mo at room temperature will be presented. These studies have improved our understanding of dislocation mobility, dislocation generation, and dislocation-obstacle interactions. In the second example, the interaction of matrix dislocations with grain boundaries will be described. From such studies predictive criteria for slip transfer through grain boundaries have been developed.

  7. Single and multiple electron dynamics in the strong field limit

    SciTech Connect

    Sheehy, B.; Walker, B.; Lafon, R.; Widmer, M.; Gambhir, A.; DiMauro, L.F.; Agostini, P.; Kulander, K.C.

    1996-12-31

    High precision photoelectron energy and angular distributions in helium and neon atoms for a broad intensity range reflect the change in the continuum dynamics that occurs as the ionization process evolves into the pure tunneling regime. Elastic rescattering of the laser-driven free electron from its parent ion core leaves a distinct signature on the spectra, providing a direct quantitative test of the various theories of strong field multiphoton ionization. They show that it takes a relatively complete semi-classical rescattering model to accurately reproduce the observed photoelectron distributions. However, the calculated inelastic rescattering rate fails to reproduce the measured nonsequential double ionization yields.

  8. Electron dynamics in the strong field limit of photoionization

    SciTech Connect

    Sheehy, B.; Walker, B.; Lafon, R.; Widmer, M.

    1998-12-31

    High precision photoelectron energy and angular distributions in helium and neon atoms for a broad intensity range reflect the change in the continuum dynamics that occurs as the ionization process evolves into the pure tunneling regime. Elastic rescattering of the laser-driven free electron from its parent ion core leaves a distinct signature on the spectra, providing a direct quantitative test of the various theories of strong field multiphoton ionization. We show that it takes a relatively complete semi-classical rescattering model to accurately reproduce the observed photoelectron distributions. However, the calculated inelastic rescattering rate fails to reproduce the measured nonsequential double ionization yields.

  9. Single and multiple electron dynamics in the strong field limit

    SciTech Connect

    Sheehy, B.; Walker, B.; Lafon, R.; Widmer, M.; Gambhir, A.; DiMauro, L.F.; Agostini, P.; Kulander, K.C.

    1996-10-01

    High precision photoelectron energy and angular distributions in helium and neon atoms for a broad intensity range reflect the change in the continuum dynamics that occurs as the ionization process evolves into the pure tunneling regime. Elastic rescattering of the laser-driven free electron from its parent ion core leaves a distinct signature on the spectra, providing a direct quantitative test of the various theories of strong field multiphoton ionization. We show that it takes a relatively complete semi-classical rescattering model to accurately reproduce the observed photoelectron distributions. However, the calculated inelastic rescattering rate fails to reproduce the measured nonsequential double ionization yields. 18 refs., 5 figs.

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

    NASA Astrophysics Data System (ADS)

    Wiechula, J.; Schönlein, A.; Iberler, M.; Hock, C.; Manegold, T.; Bohlender, B.; Jacoby, J.

    2016-07-01

    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 ArH2 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 ṡ 1015 cm-3 for a single accelerated plasma and a maximum value of ≈2.6 ṡ 1016 cm-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.

  11. Dissociation dynamics in the dissociative electron attachment to carbon dioxide

    NASA Astrophysics Data System (ADS)

    Nag, Pamir; Nandi, Dhananjay

    2015-05-01

    Dissociative electron attachment (DEA) to gas phase CO2 has been probed using a velocity slice imaging technique. DEA to CO2 produces only an O- ionic fragment and shows two major resonances located at 4.4 and 8.2 eV, respectively. The kinetic energy and angular distribution of the O- ions are measured around the second resonance with higher efficiency and sensitivity that provide details of the DEA dynamics. The kinetic energy distributions are in good agreement with the previous reports. However, the distinct angular distributions show substantial difference from the two recent studies within the limited electron energies. Our angular distribution results show two negative ion resonant states are involved in the underlying DEA process at the entire electron energies over the second resonance. We discussed the recent conflicting findings in the angular distribution results. The forward-backward asymmetry observed in the angular distributions is explained due to the interference effect of different partial waves associated with the attaching electron.

  12. Dynamic secondary electron contrast effects in liquid systems studied by environmental scanning electron microscopy.

    PubMed

    Stokes, D J; Thiel, B L; Donald, A M

    2000-01-01

    We report an investigation into a dynamic contrast phenomenon in water-oil emulsions imaged in the environmental scanning electron microscope. Secondary electron contrast between oil and water phases is shown to change with scan rate, even inverting in extreme cases. This effect is attributed to the fact that charge carriers in liquids have intermediate mobilities compared with those in metallic conductors and solid insulators. Thus, increasing the electron energy flux density (via slower scan rates) results in the temporary accumulation of excess charge, which in turn gives rise to increased secondary electron emission. Excess charge dissipates between frames, however, such that classical charging of the specimen is not observed. The oils used here have conductivities lower than that of water, making them more susceptible to the effect. However, the material within the primary electron interaction volume is a conductive medium. We demonstrate that charging effects are not seen in regions of the oil where the interaction volume is in contact with the more conductive continuous water phase. Secondary electron emission from these regions therefore approximates to the intrinsic yield.

  13. An accurate dynamical electron diffraction algorithm for reflection high-energy electron diffraction

    NASA Astrophysics Data System (ADS)

    Huang, J.; Cai, C. Y.; Lv, C. L.; Zhou, G. W.; Wang, Y. G.

    2015-12-01

    The conventional multislice method (CMS) method, one of the most popular dynamical electron diffraction calculation procedures in transmission electron microscopy, was introduced to calculate reflection high-energy electron diffraction (RHEED) as it is well adapted to deal with the deviations from the periodicity in the direction parallel to the surface. However, in the present work, we show that the CMS method is no longer sufficiently accurate for simulating RHEED with the accelerating voltage 3-100 kV because of the high-energy approximation. An accurate multislice (AMS) method can be an alternative for more accurate RHEED calculations with reasonable computing time. A detailed comparison of the numerical calculation of the AMS method and the CMS method is carried out with respect to different accelerating voltages, surface structure models, Debye-Waller factors and glancing angles.

  14. Protein electron transfer: is biology (thermo)dynamic?

    PubMed

    Matyushov, Dmitry V

    2015-12-01

    Simple physical mechanisms are behind the flow of energy in all forms of life. Energy comes to living systems through electrons occupying high-energy states, either from food (respiratory chains) or from light (photosynthesis). This energy is transformed into the cross-membrane proton-motive force that eventually drives all biochemistry of the cell. Life's ability to transfer electrons over large distances with nearly zero loss of free energy is puzzling and has not been accomplished in synthetic systems. The focus of this review is on how this energetic efficiency is realized. General physical mechanisms and interactions that allow proteins to fold into compact water-soluble structures are also responsible for a rugged landscape of energy states and a broad distribution of relaxation times. Specific to a protein as a fluctuating thermal bath is the protein-water interface, which is heterogeneous both dynamically and structurally. The spectrum of interfacial fluctuations is a consequence of protein's elastic flexibility combined with a high density of surface charges polarizing water dipoles into surface nanodomains. Electrostatics is critical to the protein function and the relevant questions are: (i) What is the spectrum of interfacial electrostatic fluctuations? (ii) Does the interfacial biological water produce electrostatic signatures specific to proteins? (iii) How is protein-mediated chemistry affected by electrostatics? These questions connect the fluctuation spectrum to the dynamical control of chemical reactivity, i.e. the dependence of the activation free energy of the reaction on the dynamics of the bath. Ergodicity is often broken in protein-driven reactions and thermodynamic free energies become irrelevant. Continuous ergodicity breaking in a dense spectrum of relaxation times requires using dynamically restricted ensembles to calculate statistical averages. When applied to the calculation of the rates, this formalism leads to the nonergodic activated

  15. Protein electron transfer: is biology (thermo)dynamic?

    PubMed

    Matyushov, Dmitry V

    2015-12-01

    Simple physical mechanisms are behind the flow of energy in all forms of life. Energy comes to living systems through electrons occupying high-energy states, either from food (respiratory chains) or from light (photosynthesis). This energy is transformed into the cross-membrane proton-motive force that eventually drives all biochemistry of the cell. Life's ability to transfer electrons over large distances with nearly zero loss of free energy is puzzling and has not been accomplished in synthetic systems. The focus of this review is on how this energetic efficiency is realized. General physical mechanisms and interactions that allow proteins to fold into compact water-soluble structures are also responsible for a rugged landscape of energy states and a broad distribution of relaxation times. Specific to a protein as a fluctuating thermal bath is the protein-water interface, which is heterogeneous both dynamically and structurally. The spectrum of interfacial fluctuations is a consequence of protein's elastic flexibility combined with a high density of surface charges polarizing water dipoles into surface nanodomains. Electrostatics is critical to the protein function and the relevant questions are: (i) What is the spectrum of interfacial electrostatic fluctuations? (ii) Does the interfacial biological water produce electrostatic signatures specific to proteins? (iii) How is protein-mediated chemistry affected by electrostatics? These questions connect the fluctuation spectrum to the dynamical control of chemical reactivity, i.e. the dependence of the activation free energy of the reaction on the dynamics of the bath. Ergodicity is often broken in protein-driven reactions and thermodynamic free energies become irrelevant. Continuous ergodicity breaking in a dense spectrum of relaxation times requires using dynamically restricted ensembles to calculate statistical averages. When applied to the calculation of the rates, this formalism leads to the nonergodic activated

  16. Protein electron transfer: is biology (thermo)dynamic?

    NASA Astrophysics Data System (ADS)

    Matyushov, Dmitry V.

    2015-12-01

    Simple physical mechanisms are behind the flow of energy in all forms of life. Energy comes to living systems through electrons occupying high-energy states, either from food (respiratory chains) or from light (photosynthesis). This energy is transformed into the cross-membrane proton-motive force that eventually drives all biochemistry of the cell. Life’s ability to transfer electrons over large distances with nearly zero loss of free energy is puzzling and has not been accomplished in synthetic systems. The focus of this review is on how this energetic efficiency is realized. General physical mechanisms and interactions that allow proteins to fold into compact water-soluble structures are also responsible for a rugged landscape of energy states and a broad distribution of relaxation times. Specific to a protein as a fluctuating thermal bath is the protein-water interface, which is heterogeneous both dynamically and structurally. The spectrum of interfacial fluctuations is a consequence of protein’s elastic flexibility combined with a high density of surface charges polarizing water dipoles into surface nanodomains. Electrostatics is critical to the protein function and the relevant questions are: (i) What is the spectrum of interfacial electrostatic fluctuations? (ii) Does the interfacial biological water produce electrostatic signatures specific to proteins? (iii) How is protein-mediated chemistry affected by electrostatics? These questions connect the fluctuation spectrum to the dynamical control of chemical reactivity, i.e. the dependence of the activation free energy of the reaction on the dynamics of the bath. Ergodicity is often broken in protein-driven reactions and thermodynamic free energies become irrelevant. Continuous ergodicity breaking in a dense spectrum of relaxation times requires using dynamically restricted ensembles to calculate statistical averages. When applied to the calculation of the rates, this formalism leads to the nonergodic

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

    NASA Astrophysics Data System (ADS)

    Haglund, Richard

    2015-03-01

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

  18. Investigations on interfacial dynamics with ultrafast electron diffraction

    NASA Astrophysics Data System (ADS)

    Murdick, Ryan A.

    An ultrafast electron diffractive voltammetry (UEDV) technique is introduced, extended from ultrafast electron diffraction, to investigate the ultrafast charge transport dynamics at interfaces and in nanostructures. Rooted in Coulomb-induced refraction, formalisms are presented to quantitatively deduce the transient surface voltages (TSVs), caused by photoinduced charge redistributions at interfaces, and are applied to examine a prototypical Si/SiO2 interface, known to be susceptible to photoinduced interfacial charging The ultrafast time resolution and high sensitivity to surface charges of this electron diffractive approach allows direct elucidation of the transient effects of photoinduced hot electron transport at nanometer (˜2 nm) interfaces. Two distinctive regimes are uncovered, characterized by the time scales associated with charge separation. At the low fluence regime, the charge transfer is described by a thermally-mediated process with linear dependence on the excitation fluence. Theoretical analysis of the transient thermal properties of the carriers show that it is well-described by a direct tunneling of the laser heated electrons through the dielectric oxide layer to surface states. At higher fluences, a coherent multiphoton absorption process is invoked to directly inject electrons into the conduction band of SiO2, leading to a more efficient surface charge accumulation. A quadratic fluence dependence on this coherent, 3-photon lead electron injection is characterized by the rapid dephasing of the intermediately generated hot electrons from 2-photon absorption, limiting the yield of the consecutive 1-photon absorption by free carriers. The TSV formalism is extended beyond the simple slab geometry associated with planar surfaces (Si/SiO2), to interfaces with arbitrary geometrical features, by imposing a corrective scheme to the slab model. The validity of this treatment is demonstrated in an investigation of the charge transfer dynamics at a metal

  19. Quantitative Carrier Density Wave Imaging in Silicon Solar Cells Using Photocarrier Radiometry and Lock-in Carrierography

    NASA Astrophysics Data System (ADS)

    Sun, Q. M.; Melnikov, A.; Mandelis, A.

    2016-04-01

    InGaAs camera-based low-frequency homodyne and high-frequency heterodyne lock-in carrierographies (LIC) are introduced for spatially resolved imaging of optoelectronic properties of Si solar cells. Based on the full theory of solar cell photocarrier radiometry (PCR), several simplification steps were performed aiming at the open circuit case, and a concise expression of the base minority carrier density depth profile was obtained. The model shows that solar cell PCR/LIC signals are mainly sensitive to the base minority carrier lifetime. Both homodyne and heterodyne frequency response data at selected locations on a mc-Si solar cell were used to extract the local base minority carrier lifetimes by best fitting local experimental data to theory.

  20. U31: Vehicle Stability and Dynamics: Electronic Stability Control

    SciTech Connect

    Petrolino, Joseph; Spezia, Tony; Arant, Michael; Delorenzis, Damon; LaClair, Tim J; Lim, Alvin; Pape, Doug

    2011-01-01

    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 stability control (ESC) products automatically slow a vehicle rounding a corner too quickly or apply individual brakes when necessary to improve the steering characteristics of a vehicle. Air brake systems in North America provide no electronic communication between a tractor and semitrailer, limiting the degree to which control systems can be optimized. Prior research has demonstrated stability improvements where dynamic measurements and control commands are communicated between units of a vehicle. Three related activities were undertaken: (1) Develop an algorithm for the optimum yaw and roll control of a combination vehicle. Vehicle state parameters needed to control the vehicle and the proper brake response were determined. An integrated stability control for the tractor and semitrailer requires communication between the two units. Dynamic models were used to assess the algorithm. (2) Implement the ESC algorithm in the laboratory. Hardware components suitable for the harsh environment for measurement, sensor-to-controller communication, and semitrailer-to-tractor communication and brake actuation were specified and assembled as a working system. The goal was to collect the needed vehicle state information, transmit the information to the ESC system, and then actuate the brakes in response to controller commands. (3) Develop a wireless network with the data rate and reliability necessary to communicate dynamic signals for a vehicle stability control system. Adaptive connectivity-aware, multi-hop routing was selected because it can perform in the harsh environment where packet collisions and fading often will exist. The protocol is to give high priority to urgent messages.

  1. Proton Dynamics on Goethite Nanoparticles and Coupling to Electron Transport.

    PubMed

    Zarzycki, Piotr; Smith, Dayle M; Rosso, Kevin M

    2015-04-14

    The surface chemistry of metal oxide particles is governed by the charge that develops at the interface with aqueous solution. Mineral transformation, biogeochemical reactions, remediation, and sorption dynamics are profoundly affected in response. Here we report implementation of replica-exchange constant-pH molecular dynamics simulations that use classical molecular dynamics for exploring configurational space and Metropolis Monte Carlo walking through protonation space with a simulated annealing escape route from metastable configurations. By examining the archetypal metal oxide, goethite (α-FeOOH), we find that electrostatic potential gradients spontaneously arise between intersecting low-index crystal faces and across explicitly treated oxide nanoparticles at a magnitude exceeding the Johnson-Nyquist voltage fluctuation. Fluctuations in adsorbed proton density continuously repolarize the surface potential bias between edge-sharing crystal faces, at a rate slower than the reported electron-polaron hopping rate in goethite interiors. This suggests that these spontaneous surface potential fluctuations will control the net movement of charge carriers in the lattice. PMID:26574382

  2. Electronic structure and dynamics of elements at high pressures

    NASA Astrophysics Data System (ADS)

    Mao, Ho-Kwang

    2011-03-01

    Electronic structure and dynamics information of materials under high pressure has been very scarce due to the experimental difficulties. The standard electronic probes using electron energy loss spectroscopy (EELS) is limited to vacuum pressures. The optical probes that can reach high-pressure samples through the diamond windows, on the other hand, are limited by the energy accessibility (5 eV) andnear - zeromomentumtransfer , q = (4 π /λ0) sinθ . Theseproblemscanbeovercomebythenewlyadvanced , two - photon , inelastic , xray , scattering (IXS) spectroscopywhichuseshighenergyxrays (~ 10 4 eV) toprovidetheatomic - levelmomentumtransferandtoenter (withenergy E) andexit (withenergy E0) thepressurevessel . Theelectronicspectraarerevealedbyanalyzingthexrayenergylossbetweenthetwophotons , ω = E -E0 . UsingIXSfacilitiesatthird - generationsynchrotronsource , westudiedelectronicstructureanddynamicsoftwoelementsathighpressuresinadiamond - anvilcell : i . e . , He , thewidest - gapinsulator , andNa , thearchetypalfree - electronmetal . At 11.9 - 17.9 GPainasinglecrystal 4 He , weobservedrichelectronexcitationspectra , includingacut - offedgeabove 23 eV , asharpexcitonpeakshowinglinearvolumedependence , andaseriesofexcitationsandcontinuumat 26 to 45 eV . Wedeterminedelectronicdispersionalongthe 100 directionovertwoBrillouinzones , andprovidedaquantitativepictureoftheheliumexcitonbeyondthesimplifiedWannier - Frenkeldescription . At 1.6 - 4.39 GPainapolycrystallineNasample , weobservedthesharpplasmonpeakatlow q anditsdispersionbeyondthecritical q c . Theplasmonshiftstohigherenergyundercompressionanddrasticreductionof rs . Ab-initio theoretical calculations are conducted for interpretation of the experimental results. The speaker would like to acknowledge collaborating researchers: R. Ahuja, Y. Cai, P. Chow, Y. Ding, P. Eng, R.J. Hemley, C.C. Kao, S. Lebegue, W.L. Mao, E.L. Shirley, J. Shu, & Y. Xiao.

  3. Dynamics of a high-current relativistic electron beam

    SciTech Connect

    Strelkov, P. S.; Tarakanov, V. P.; Ivanov, I. E. Shumeiko, D. V.

    2015-06-15

    The dynamics of a high-current relativistic electron beam is studied experimentally and by numerical simulation. The beam is formed in a magnetically insulated diode with a transverse-blade explosive-emission cathode. It is found experimentally that the radius of a 500-keV beam with a current of 2 kA and duration of 500 ns decreases with time during the beam current pulse. The same effect was observed in numerical simulations. This effect is explained by a change in the shape of the cathode plasma during the current pulse, which, according to calculations, leads to a change in the beam parameters, such as the electron pitch angle and the spread over the longitudinal electron momentum. These parameters are hard to measure experimentally; however, the time evolution of the radial profile of the beam current density, which can be measured reliably, coincides with the simulation results. This allows one to expect that the behavior of the other beam parameters also agrees with numerical simulations.

  4. Mechanisms of bridge-mediated electron transfer: a TDDFT electronic dynamics study.

    PubMed

    Ding, Feizhi; Chapman, Craig T; Liang, Wenkel; Li, Xiaosong

    2012-12-14

    We present a time-dependent density functional theory approach for probing the dynamics of electron transfer on a donor-bridge-acceptor polyene dye scaffold. Two kinds of mechanisms, namely, the superexchange mechanism and the sequential mechanism, may be involved in the electron transfer process. In this work, we have focused on the crossover between these two charge transfer mechanisms on a series of donor-bridge-acceptor polyene dye systems with varying lengths of conjugated bridges. A number of methods and quantities are used to assist in the analysis, including the phase relationship of charge evolution and frequency domain spectra of the time-dependent dipole. Our simulations show that the superexchange mechanism plays a dominant role in the electron transfer from donor to acceptor when the bridge length is small, and the sequential mechanism becomes more important as the polyene bridge is lengthened. Full Ehrenfest dynamics with nuclear motion show that molecular vibrations play a very small role in such ultrafast charge transfer processes.

  5. Time-resolved terahertz dynamics in thin films of the topological insulator Bi2Se3

    DOE PAGESBeta

    Valdés Aguilar, R.; Qi, J.; Brahlek, M.; Bansal, N.; Azad, A.; Bowlan, J.; Oh, S.; Taylor, A. J.; Prasankumar, R. P.; Yarotski, D. A.

    2015-01-07

    We use optical pump–THz probe spectroscopy at low temperatures to study the hot carrier response in thin Bi2Se3 films of several thicknesses, allowing us to separate the bulk from the surface transient response. We find that for thinner films the photoexcitation changes the transport scattering rate and reduces the THz conductivity, which relaxes within 10 picoseconds (ps). For thicker films, the conductivity increases upon photoexcitation and scales with increasing both the film thickness and the optical fluence, with a decay time of approximately 5 ps as well as a much higher scattering rate. Furthermore, these different dynamics are attributed tomore » the surface and bulk electrons, respectively, and demonstrate that long-lived mobile surface photo-carriers can be accessed independently below certain film thicknesses for possible optoelectronic applications.« less

  6. Imaging electron dynamics with time- and angle-resolved photoelectron spectroscopy

    NASA Astrophysics Data System (ADS)

    Popova-Gorelova, Daria; Küpper, Jochen; Santra, Robin

    2016-07-01

    We theoretically study how time- and angle-resolved photoemission spectroscopy can be applied for imaging coherent electron dynamics in molecules. We consider a process in which a pump pulse triggers coherent electronic dynamics in a molecule by creating a valence electron hole. An ultrashort extreme ultraviolet probe pulse creates a second electron hole in the molecule. Information about the electron dynamics is accessed by analyzing angular distributions of photoemission probabilities at a fixed photoelectron energy. We demonstrate that a rigorous theoretical analysis, which takes into account the indistinguishability of transitions induced by the ultrashort, broadband probe pulse and electron hole correlation effects, is necessary for the interpretation of time- and angle-resolved photoelectron spectra. We show how a Fourier analysis of time- and angle-resolved photoelectron spectra from a molecule can be applied to follow its electron dynamics by considering photoelectron distributions from an indole molecular cation with coherent electron dynamics.

  7. Surface electron density models for accurate ab initio molecular dynamics with electronic friction

    NASA Astrophysics Data System (ADS)

    Novko, D.; Blanco-Rey, M.; Alducin, M.; Juaristi, J. I.

    2016-06-01

    Ab initio molecular dynamics with electronic friction (AIMDEF) is a valuable methodology to study the interaction of atomic particles with metal surfaces. This method, in which the effect of low-energy electron-hole (e-h) pair excitations is treated within the local density friction approximation (LDFA) [Juaristi et al., Phys. Rev. Lett. 100, 116102 (2008), 10.1103/PhysRevLett.100.116102], can provide an accurate description of both e-h pair and phonon excitations. In practice, its applicability becomes a complicated task in those situations of substantial surface atoms displacements because the LDFA requires the knowledge at each integration step of the bare surface electron density. In this work, we propose three different methods of calculating on-the-fly the electron density of the distorted surface and we discuss their suitability under typical surface distortions. The investigated methods are used in AIMDEF simulations for three illustrative adsorption cases, namely, dissociated H2 on Pd(100), N on Ag(111), and N2 on Fe(110). Our AIMDEF calculations performed with the three approaches highlight the importance of going beyond the frozen surface density to accurately describe the energy released into e-h pair excitations in case of large surface atom displacements.

  8. Dynamics of a nanodroplet under a transmission electron microscope

    NASA Astrophysics Data System (ADS)

    Leong, Fong Yew; Mirsaidov, Utkur M.; Matsudaira, Paul; Mahadevan, L.

    2014-01-01

    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.

  9. Dynamics of a nanodroplet under a transmission electron microscope

    SciTech Connect

    Leong, Fong Yew; Mirsaidov, Utkur M.; Matsudaira, Paul; Mahadevan, L.

    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.

  10. Semiclassical Dynamics of Electron Wave Packet States with Phase Vortices

    SciTech Connect

    Bliokh, Konstantin Yu.; Bliokh, Yury P.; Savel'ev, Sergey; Nori, Franco

    2007-11-09

    We consider semiclassical higher-order wave packet solutions of the Schroedinger equation with phase vortices. The vortex line is aligned with the propagation direction, and the wave packet carries a well-defined orbital angular momentum (OAM) ({Dirac_h}/2{pi})l (l is the vortex strength) along its main linear momentum. The probability current coils around the momentum in such OAM states of electrons. In an electric field, these states evolve like massless particles with spin l. The magnetic-monopole Berry curvature appears in momentum space, which results in a spin-orbit-type interaction and a Berry/Magnus transverse force acting on the wave packet. This brings about the OAM Hall effect. In a magnetic field, there is a Zeeman interaction, which, can lead to more complicated dynamics.

  11. Effects of parallel electron dynamics on plasma blob transport

    SciTech Connect

    Angus, Justin R.; Krasheninnikov, Sergei I.; Umansky, Maxim V.

    2012-08-15

    The 3D effects on sheath connected plasma blobs that result from parallel electron dynamics are studied by allowing for the variation of blob density and potential along the magnetic field line and using collisional Ohm's law to model the parallel current density. The parallel current density from linear sheath theory, typically used in the 2D model, is implemented as parallel boundary conditions. This model includes electrostatic 3D effects, such as resistive drift waves and blob spinning, while retaining all of the fundamental 2D physics of sheath connected plasma blobs. If the growth time of unstable drift waves is comparable to the 2D advection time scale of the blob, then the blob's density gradient will be depleted resulting in a much more diffusive blob with little radial motion. Furthermore, blob profiles that are initially varying along the field line drive the potential to a Boltzmann relation that spins the blob and thereby acts as an addition sink of the 2D potential. Basic dimensionless parameters are presented to estimate the relative importance of these two 3D effects. The deviation of blob dynamics from that predicted by 2D theory in the appropriate limits of these parameters is demonstrated by a direct comparison of 2D and 3D seeded blob simulations.

  12. Femtosecond electron imaging of defect-modulated phonon dynamics

    NASA Astrophysics Data System (ADS)

    Cremons, Daniel R.; Plemmons, Dayne A.; Flannigan, David J.

    2016-04-01

    Precise manipulation and control of coherent lattice oscillations via nanostructuring and phonon-wave interference has the potential to significantly impact a broad array of technologies and research areas. Resolving the dynamics of individual phonons in defect-laden materials presents an enormous challenge, however, owing to the interdependent nanoscale and ultrafast spatiotemporal scales. Here we report direct, real-space imaging of the emergence and evolution of acoustic phonons at individual defects in crystalline WSe2 and Ge. Via bright-field imaging with an ultrafast electron microscope, we are able to image the sub-picosecond nucleation and the launch of wavefronts at step edges and resolve dispersion behaviours during propagation and scattering. We discover that the appearance of speed-of-sound (for example, 6 nm ps-1) wavefronts are influenced by spatially varying nanoscale strain fields, taking on the appearance of static bend contours during propagation. These observations provide unprecedented insight into the roles played by individual atomic and nanoscale features on acoustic-phonon dynamics.

  13. Femtosecond electron imaging of defect-modulated phonon dynamics.

    PubMed

    Cremons, Daniel R; Plemmons, Dayne A; Flannigan, David J

    2016-01-01

    Precise manipulation and control of coherent lattice oscillations via nanostructuring and phonon-wave interference has the potential to significantly impact a broad array of technologies and research areas. Resolving the dynamics of individual phonons in defect-laden materials presents an enormous challenge, however, owing to the interdependent nanoscale and ultrafast spatiotemporal scales. Here we report direct, real-space imaging of the emergence and evolution of acoustic phonons at individual defects in crystalline WSe2 and Ge. Via bright-field imaging with an ultrafast electron microscope, we are able to image the sub-picosecond nucleation and the launch of wavefronts at step edges and resolve dispersion behaviours during propagation and scattering. We discover that the appearance of speed-of-sound (for example, 6 nm ps(-1)) wavefronts are influenced by spatially varying nanoscale strain fields, taking on the appearance of static bend contours during propagation. These observations provide unprecedented insight into the roles played by individual atomic and nanoscale features on acoustic-phonon dynamics. PMID:27079790

  14. Femtosecond electron imaging of defect-modulated phonon dynamics

    PubMed Central

    Cremons, Daniel R.; Plemmons, Dayne A.; Flannigan, David J.

    2016-01-01

    Precise manipulation and control of coherent lattice oscillations via nanostructuring and phonon-wave interference has the potential to significantly impact a broad array of technologies and research areas. Resolving the dynamics of individual phonons in defect-laden materials presents an enormous challenge, however, owing to the interdependent nanoscale and ultrafast spatiotemporal scales. Here we report direct, real-space imaging of the emergence and evolution of acoustic phonons at individual defects in crystalline WSe2 and Ge. Via bright-field imaging with an ultrafast electron microscope, we are able to image the sub-picosecond nucleation and the launch of wavefronts at step edges and resolve dispersion behaviours during propagation and scattering. We discover that the appearance of speed-of-sound (for example, 6 nm ps−1) wavefronts are influenced by spatially varying nanoscale strain fields, taking on the appearance of static bend contours during propagation. These observations provide unprecedented insight into the roles played by individual atomic and nanoscale features on acoustic-phonon dynamics. PMID:27079790

  15. Nonequilibrium electron dynamics: Formation of the quasiparticle peak

    NASA Astrophysics Data System (ADS)

    Sayyad, Sharareh; Eckstein, Martin

    We characterize how the narrow quasiparticle band of the one-band Hubbard model forms out of a bad metallic state in a time-dependent metal-insulator transition, using nonequilibrium slave-rotor dynamical mean field theory. Our results exhibit a nontrivial electronic timescale which is much longer than the width of the quasiparticle peak itself. To study this timescale, we perform a fast ramp from the insulating phase into the metallic region of the phase diagram, resulting in a highly excited state, and study the equilibration of the system with a weakly coupled phononic bath. The slow relaxation behavior is explained by surveilling the interplay between spinon and rotor degrees of freedom. Since the system is initially prepared in an insulating phase, the quasi-particle peak emerges when spinons catch up the metal-insulator crossover region, which is reached earlier by the rotor. At this point, spinon and rotor become weakly coupled, and the resulting very slow equilibration of the spinon is a bottleneck for the dynamics. After the birth of the quasiparticle peak, its height enhances by the construction of the low-energy spectrum of the rotor, which then lacks behind the relaxation of the spinon.

  16. Dynamic Characterization and Modeling of Potting Materials for Electronics Assemblies

    NASA Astrophysics Data System (ADS)

    Joshi, Vasant; Lee, Gilbert; Santiago, Jaime

    2015-06-01

    Prediction of survivability of encapsulated electronic components subject to impact relies on accurate modeling. Both static and dynamic characterization of encapsulation material is needed to generate a robust material model. Current focus is on potting materials to mitigate high rate loading on impact. In this effort, encapsulation scheme consists of layers of polymeric material Sylgard 184 and Triggerbond Epoxy-20-3001. Experiments conducted for characterization of materials include conventional tension and compression tests, Hopkinson bar, dynamic material analyzer (DMA) and a non-conventional accelerometer based resonance tests for obtaining high frequency data. For an ideal material, data can be fitted to Williams-Landel-Ferry (WLF) model. A new temperature-time shift (TTS) macro was written to compare idealized temperature shift factor (WLF model) with experimental incremental shift factors. Deviations can be observed by comparison of experimental data with the model fit to determine the actual material behavior. Similarly, another macro written for obtaining Ogden model parameter from Hopkinson Bar tests indicates deviations from experimental high strain rate data. In this paper, experimental results for different materials used for mitigating impact, and ways to combine data from resonance, DMA and Hopkinson bar together with modeling refinements will be presented.

  17. Electronic structure and relaxation dynamics in a superconducting topological material.

    PubMed

    Neupane, Madhab; Ishida, Yukiaki; Sankar, Raman; Zhu, Jian-Xin; Sanchez, Daniel S; Belopolski, Ilya; Xu, Su-Yang; Alidoust, Nasser; Hosen, M Mofazzel; Shin, Shik; Chou, Fangcheng; Hasan, M Zahid; Durakiewicz, Tomasz

    2016-01-01

    Topological superconductors host new states of quantum matter which show a pairing gap in the bulk and gapless surface states providing a platform to realize Majorana fermions. Recently, alkaline-earth metal Sr intercalated Bi2Se3 has been reported to show superconductivity with a Tc ~ 3 K and a large shielding fraction. Here we report systematic normal state electronic structure studies of Sr0.06Bi2Se3 (Tc ~ 2.5 K) by performing photoemission spectroscopy. Using angle-resolved photoemission spectroscopy (ARPES), we observe a quantum well confined two-dimensional (2D) state coexisting with a topological surface state in Sr0.06Bi2Se3. Furthermore, our time-resolved ARPES reveals the relaxation dynamics showing different decay mechanism between the excited topological surface states and the two-dimensional states. Our experimental observation is understood by considering the intra-band scattering for topological surface states and an additional electron phonon scattering for the 2D states, which is responsible for the superconductivity. Our first-principles calculations agree with the more effective scattering and a shorter lifetime of the 2D states. Our results will be helpful in understanding low temperature superconducting states of these topological materials. PMID:26936229

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

    PubMed

    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. PMID:25763310

  19. Electronic Structure and Molecular Dynamics Calculations for KBH4

    NASA Astrophysics Data System (ADS)

    Papaconstantopoulos, Dimitrios; Shabaev, Andrew; Hoang, Khang; Mehl, Michael; Kioussis, Nicholas

    2012-02-01

    In the search for hydrogen storage materials, alkali borohydrides MBH4 (M=Li, Na, K) are especially interesting because of their light weight and the high number of hydrogen atoms per metal atom. Electronic structure calculations can give insights into the properties of these complex hydrides and provide understanding of the structural properties and of the bonding of hydrogen. We have performed first-principles density-functional theory (DFT) and tight-binding (TB) calculations for KBH4 in both the high temperature (HT) and low temperature (LT) phases to understand its electronic and structural properties. Our DFT calculations were carried out using the VASP code. The results were then used as a database to develop a tight-binding Hamiltonian using the NRL-TB method. This approach allowed for computationally efficient calculations of phonon frequencies and elastic constants using the static module of the NRL-TB, and also using the molecular dynamics module to calculate mean-square displacements and formation energies of hydrogen vacancies.

  20. Electron accommodation dynamics in the DNA base thymine

    SciTech Connect

    King, Sarah B.; Yandell, Margaret A.; Kunin, Alice; Stephansen, Anne B.; Yokoi, Yuki; Takayanagi, Toshiyuki; Neumark, Daniel M.

    2015-07-14

    The dynamics of electron attachment to the DNA base thymine are investigated using femtosecond time-resolved photoelectron imaging of the gas phase iodide-thymine (I{sup −}T) complex. An ultraviolet pump pulse ejects an electron from the iodide and prepares an iodine-thymine temporary negative ion that is photodetached with a near-IR probe pulse. The resulting photoelectrons are analyzed with velocity-map imaging. At excitation energies ranging from −120 meV to +90 meV with respect to the vertical detachment energy (VDE) of 4.05 eV for I{sup −}T, both the dipole-bound and valence-bound negative ions of thymine are observed. A slightly longer rise time for the valence-bound state than the dipole-bound state suggests that some of the dipole-bound anions convert to valence-bound species. No evidence is seen for a dipole-bound anion of thymine at higher excitation energies, in the range of 0.6 eV above the I{sup −}T VDE, which suggests that if the dipole-bound anion acts as a “doorway” to the valence-bound anion, it only does so at excitation energies near the VDE of the complex.

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

    PubMed

    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.

  2. Electronic structure and relaxation dynamics in a superconducting topological material

    DOE PAGESBeta

    Neupane, Madhab; Ishida, Yukiaki; Sankar, Raman; Zhu, Jian-Xin; Sanchez, Daniel S.; Belopolski, Ilya; Xu, Su-Yang; Alidoust, Nasser; Hosen, M. Mofazzel; Shin, Shik; et al

    2016-03-03

    Topological superconductors host new states of quantum matter which show a pairing gap in the bulk and gapless surface states providing a platform to realize Majorana fermions. Recently, alkaline-earth metal Sr intercalated Bi2Se3 has been reported to show superconductivity with a Tc~3K and a large shielding fraction. Here we report systematic normal state electronic structure studies of Sr0.06Bi2Se3 (Tc~2.5K) by performing photoemission spectroscopy. Using angle-resolved photoemission spectroscopy (ARPES), we observe a quantum well confined two-dimensional (2D) state coexisting with a topological surface state in Sr0.06Bi2Se3. Furthermore, our time-resolved ARPES reveals the relaxation dynamics showing different decay mechanism between the excitedmore » topological surface states and the two-dimensional states. Our experimental observation is understood by considering the intra-band scattering for topological surface states and an additional electron phonon scattering for the 2D states, which is responsible for the superconductivity. Our first-principles calculations agree with the more effective scattering and a shorter lifetime of the 2D states. In conclusion, our results will be helpful in understanding low temperature superconducting states of these topological materials.« less

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

    SciTech Connect

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

    2015-10-07

    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 2b{sub 1}, 6a{sub 1}, 4b{sub 2}, and 1a{sub 2} 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 A{sub 1}, B{sub 1}, and B{sub 2} 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.

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

    NASA Astrophysics Data System (ADS)

    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.

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

    PubMed

    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.

  6. Ultrafast excited state relaxation dynamics of electron deficient porphyrins: Conformational and electronic factors

    NASA Astrophysics Data System (ADS)

    Okhrimenko, Albert N.

    Metallo-tetrapyrroles (MTP) are highly stable macrocyclic pi-systems that display interesting properties that make them potential candidates for various applications. Among these applications are optoelectronics, magnetic materials, photoconductive materials, non-linear optical materials and photo tumor therapeutic drugs. These applications are generally related to their high stability and efficient light absorption ability in the visible and near-infrared region of the optical spectrum. Metallo porphyrins are well known and widely studied representatives of metallotetrapyrroles. Electron deficient substituents in the meso positions are well known to greatly influence the interaction between the metal d-orbitals and the nitrogen orbitals of the tetrapyrrole macrocycle. In this work, a series of electron deficient porphyrins has been studied to gain some knowledge about the change in the excited state dynamics with structural and electronic modifications. Among these porphyrins is nickel and iron modified species bearing perfluoro-, perprotio-, p-nitrophenyl- and perfluorophenyl-meso substituents. Ultrafast transient absorption spectrometry has been used as the main research instrument along with other spectroscopic and electrochemical methods. A new technique has been employed to study the photophysical properties of zinc (II) tetraphenylporphine cation radical. It employs a combination of controlled potential coulometry and femtosecond absorption spectrometry. The fast transient lifetime of 17 ps of the pi-cation species originates in very efficient mixing of the a2u HOMO cation orbital that places electronic density mainly on pyrrolic nitrogens and metal d-orbitals. That explains the lack of any emission of the cationic species. This non-radiative decay process might elucidate the processes taking place in photosynthetic systems when electron is removed from porphyrinic moiety and the hole is produced. In this work zinc(II) meso-tetraphenylporphine radial cation

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

    NASA Astrophysics Data System (ADS)

    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

  8. Ultrafast electronic dynamics in polyatomic molecules studied using femtosecond vacuum ultraviolet and x-ray pulses

    NASA Astrophysics Data System (ADS)

    Suzuki, Toshinori

    2014-06-01

    Time-resolved velocity map photoelectron imaging is performed using sub-20 fs deep ultraviolet and vacuum ultraviolet pulses to study electronic dynamics of isolated polyatomic molecules. The non-adiabatic dynamics of pyrazine, furan and carbon disulfide (CS2) are described as examples. Also described is sub-picosecond time-resolved x-ray direct absorption spectroscopy using a hard x-ray free electron laser (SACLA) and a synchronous near ultraviolet laser to study ultrafast electronic dynamics in solutions.

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

    NASA Astrophysics Data System (ADS)

    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

  10. Accaleration of Electrons of the Outer Electron Radiation Belt and Auroral Oval Dynamics

    NASA Astrophysics Data System (ADS)

    Antonova, Elizaveta; Ovchinnikov, Ilya; Riazantseva, Maria; Znatkova, Svetlana; Pulinets, Maria; Vorobjev, Viachislav; Yagodkina, Oksana; Stepanova, Marina

    2016-07-01

    We summarize the results of experimental observations demonstrating the role of auroral processes in the formation of the outer electron radiation belt and magnetic field distortion during magnetic storms. We show that the auroral oval does not mapped to the plasma sheet proper (region with magnetic field lines stretched in the tailward direction). It is mapped to the surrounding the Earth plasma ring in which transverse currents are closed inside the magnetosphere. Such currents constitute the high latitude continuation of the ordinary ring current. Mapping of the auroral oval to the region of high latitude continuation of the ordinary ring current explains the ring like shape of the auroral oval with finite thickness near noon and auroral oval dynamics during magnetic storms. The auroral oval shift to low latitudes during storms. The development of the ring current produce great distortion of the Earth's magnetic field and corresponding adiabatic variations of relativistic electron fluxes. Development of the asymmetric ring current produce the dawn-dusk asymmetry of such fluxes. We analyze main features of the observed processes including formation of sharp plasma pressure profiles during storms. The nature of observed pressure peak is analyzed. It is shown that the observed sharp pressure peak is directly connected with the creation of the seed population of relativistic electrons. The possibility to predict the position of new radiation belt during recovery phase of the magnetic storm using data of low orbiting and ground based observations is demonstrated.

  11. Nonadiabatic Evolution of Electronic States by Electron Nuclear Dynamics Theory: Application to Atom-Molecule Scattering Problems.

    NASA Astrophysics Data System (ADS)

    Hagelberg, Frank

    2004-03-01

    In this contribution, we address the problem how to determine accurately the nonadiabatic content of any given dynamic process involving molecular motion. More specifically, we generate a dynamic electronic wave function using Electron Nuclear Dynamics (END) theory^2 and cast this wave function into the language of electronic excitations. This is achieved by adiabatic transport of an electronic basis along the classical nuclear trajectories of the studied molecular system. This basis is chosen as the static UHF molecular ground state determinant of the system in conjunction with all determinants that arise from the ground state by single, double and triple substitutions. Projecting the dynamic wave function into this basis, we arrive at a natural distinction between adiabatic and nonadiabatic components of the motion considered. We will discuss this concept by the examples of various scattering problems, among them the interaction of proton projectiles with methylene targets. ^2E. Deumens et al., Rev. Mod. Phys. 1994, 66, 917.

  12. Time-resolved terahertz dynamics in thin films of the topological insulator Bi{sub 2}Se{sub 3}

    SciTech Connect

    Valdés Aguilar, R.; Qi, J.; Brahlek, M.; Bansal, N.; Oh, S.; Azad, A.; Bowlan, J.; Taylor, A. J.; Prasankumar, R. P.; Yarotski, D. A.

    2015-01-05

    We use optical pump–THz probe spectroscopy at low temperatures to study the hot carrier response in thin Bi{sub 2}Se{sub 3} films of several thicknesses, allowing us to separate the bulk from the surface transient response. We find that for thinner films the photoexcitation changes the transport scattering rate and reduces the THz conductivity, which relaxes within 10 picoseconds (ps). For thicker films, the conductivity increases upon photoexcitation and scales with increasing both the film thickness and the optical fluence, with a decay time of approximately 5 ps as well as a much higher scattering rate. These different dynamics are attributed to the surface and bulk electrons, respectively, and demonstrate that long-lived mobile surface photo-carriers can be accessed independently below certain film thicknesses for possible optoelectronic applications.

  13. Effect of electron spin dynamics on solid-state dynamic nuclear polarization performance.

    PubMed

    Siaw, Ting Ann; Fehr, Matthias; Lund, Alicia; Latimer, Allegra; Walker, Shamon A; Edwards, Devin T; Han, Song-I

    2014-09-21

    For the broadest dissemination of solid-state dynamic nuclear polarization (ssDNP) enhanced NMR as a material characterization tool, the ability to employ generic mono-nitroxide radicals as spin probes is critical. A better understanding of the factors contributing to ssDNP efficiency is needed to rationally optimize the experimental condition for the practically accessible spin probes at hand. This study seeks to advance the mechanistic understanding of ssDNP by examining the effect of electron spin dynamics on ssDNP performance at liquid helium temperatures (4-40 K). The key observation is that bi-radicals and mono-radicals can generate comparable nuclear spin polarization at 4 K and 7 T, which is in contrast to the observation for ssDNP at liquid nitrogen temperatures (80-150 K) that finds bi-radicals to clearly outperform mono-radicals. To rationalize this observation, we analyze the change in the DNP-induced nuclear spin polarization (Pn) and the characteristic ssDNP signal buildup time as a function of electron spin relaxation rates that are modulated by the mono- and bi-radical spin concentration. Changes in Pn are consistent with a systematic variation in the product of the electron spin-lattice relaxation time and the electron spin flip-flop rate that constitutes an integral saturation factor of an inhomogeneously broadened EPR spectrum. We show that the comparable Pn achieved with both radical species can be reconciled with a comparable integral EPR saturation factor. Surprisingly, the largest Pn is observed at an intermediate spin concentration for both mono- and bi-radicals. At the highest radical concentration, the stronger inter-electron spin dipolar coupling favors ssDNP, while oversaturation diminishes Pn, as experimentally verified by the observation of a maximum Pn at an intermediate, not the maximum, microwave (μw) power. At the maximum μw power, oversaturation reduces the electron spin population differential that must be upheld between

  14. Formation and nonlinear dynamics of the squeezed state of a helical electron beam with additional deceleration

    SciTech Connect

    Egorov, E. N. Koronovskii, A. A.; Kurkin, S. A.; Hramov, A. E.

    2013-11-15

    Results of numerical simulations and analysis of the formation and nonlinear dynamics of the squeezed state of a helical electron beam in a vircator with a magnetron injection gun as an electron source and with additional electron deceleration are presented. The ranges of control parameters where the squeezed state can form in such a system are revealed, and specific features of the system dynamics are analyzed. It is shown that the formation of a squeezed state of a nonrelativistic helical electron beam in a system with electron deceleration is accompanied by low-frequency longitudinal dynamics of the space charge.

  15. Development of an electron-temperature-dependent interatomic potential for molecular dynamics simulation of tungsten under electronic excitation

    NASA Astrophysics Data System (ADS)

    Khakshouri, S.; Alfè, D.; Duffy, D. M.

    2008-12-01

    Irradiation of a metal by lasers or swift heavy ions causes the electrons to become excited. In the vicinity of the excitation, an electronic temperature is established within a thermalization time of 10-100 fs, as a result of electron-electron collisions. For short times, corresponding to less than 1 ps after excitation, the resulting electronic temperature may be orders of magnitude higher than the lattice temperature. During this short time, atoms in the metal experience modified interatomic forces as a result of the excited electrons. These forces can lead to ultrafast nonthermal phenomena such as melting, ablation, laser-induced phase transitions, and modified vibrational properties. We develop an electron-temperature-dependent empirical interatomic potential for tungsten that can be used to model such phenomena using classical molecular dynamics simulations. Finite-temperature density functional theory calculations at high electronic temperatures are used to parametrize the model potential.

  16. 2003 Electronic Spectroscopy and Dynamics - July 6-11, 2003

    SciTech Connect

    Elliot Bernstein

    2004-09-10

    The Gordon Research Conference (GRC) on 2003 Electronic Spectroscopy and Dynamics - July 6-11, 2003 was held at Bates College, Lewiston, Maine, July 6-11, 2003. The Conference was well-attended with 103 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. In designing the formal speakers program, emphasis was placed on current unpublished research and discussion of the future target areas in this field. There was a conscious effort to stimulate lively discussion about the key issues in the field today. Time for formal presentations was limited in the interest of group discussions. In order that more scientists could communicate their most recent results, poster presentation time was scheduled. Attached is a copy of the formal schedule and speaker program and the poster program. In addition to these formal interactions, ''free time'' was scheduled to allow informal discussions. Such discussions are fostering new collaborations and joint efforts in the field.

  17. A diagnostic for electron dynamics in tokamaks. Final report

    SciTech Connect

    Skiff, F.; Boyd, D.

    1997-12-01

    The diagnostic was installed on TdeV and brought into operation. It was optimized to the extent that time and money permitted. A considerable quantity of data was accumulated and analyzed. Experiments ended in August 1995. The apparatus has been removed from TdeV and returned to the University of Maryland. Each of these activities is detailed here. The diagnostic worked very well. Although the distribution functions behaved in ways that were not anticipated and the refractive losses were sometimes higher than projected, the authors were able to adapt to the unexpected. In the authors` estimation, all of the effects listed above are significant, and warrant further study. The diagnostic is ready for use as a tool to study the physics of current drive and current profile modification. A mechanism for steering the launched beams is desirable to cope with the strong variations in refraction which are seen. Phased array launchers seem attractive for this purpose. Tuning of the length of the waveguide run is important to avoid troublesome reflections (return losses). It may be best to build in this capability in a future system. The perpendicular dynamics of the current driven electrons are invisible to us with the present form of the diagnostic. Simultaneous measurements at fundamental and harmonic frequencies would make perpendicular distribution function measurements possible.

  18. First principles based multiparadigm modeling of electronic structures and dynamics

    NASA Astrophysics Data System (ADS)

    Xiao, Hai

    Electronic structures and dynamics are the key to linking the material composition and structure to functionality and performance. An essential issue in developing semiconductor devices for photovoltaics is to design materials with optimal band gaps and relative positioning of band levels. Approximate DFT methods have been justified to predict band gaps from KS/GKS eigenvalues, but the accuracy is decisively dependent on the choice of XC functionals. We show here for CuInSe2 and CuGaSe2, the parent compounds of the promising CIGS solar cells, conventional LDA and GGA obtain gaps of 0.0-0.01 and 0.02-0.24 eV (versus experimental values of 1.04 and 1.67 eV), while the historically first global hybrid functional, B3PW91, is surprisingly the best, with band gaps of 1.07 and 1.58 eV. Furthermore, we show that for 27 related binary and ternary semiconductors, B3PW91 predicts gaps with a MAD of only 0.09 eV, which is substantially better than all modern hybrid functionals, including B3LYP (MAD of 0.19 eV) and screened hybrid functional HSE06 (MAD of 0.18 eV). The laboratory performance of CIGS solar cells (> 20% efficiency) makes them promising candidate photovoltaic devices. However, there remains little understanding of how defects at the CIGS/CdS interface affect the band offsets and interfacial energies, and hence the performance of manufactured devices. To determine these relationships, we use the B3PW91 hybrid functional of DFT with the AEP method that we validate to provide very accurate descriptions of both band gaps and band offsets. This confirms the weak dependence of band offsets on surface orientation observed experimentally. We predict that the CBO of perfect CuInSe2/CdS interface is large, 0.79 eV, which would dramatically degrade performance. Moreover we show that band gap widening induced by Ga adjusts only the VBO, and we find that Cd impurities do not significantly affect the CBO. Thus we show that Cu vacancies at the interface play the key role in

  19. Photocarrier Radiometry Investigation of Light-Induced Degradation of Boron-Doped Czochralski-Grown Silicon Without Surface Passivation

    NASA Astrophysics Data System (ADS)

    Wang, Qian; Li, Bincheng

    2016-04-01

    Light-induced degradation (LID) effects of boron-doped Cz silicon wafers without surface passivation are investigated in details by photocarrier radiometry (PCR). The resistivity of all samples is in the range of 0.006 Ω {\\cdot } {cm} to 38 Ω {\\cdot } {cm}. It is found that light-induced changes in surface state occupation have a great effect on LID under illumination. With the increasing contribution of light-induced changes in surface state occupation, the generation rate of the defect decreases. The light-induced changes in surface state occupation and light-induced degradation dominate the temporal behaviors of the excess carrier density of high- and low-resistivity Si wafers, respectively. Moreover, the temporal behaviors of PCR signals of these samples under laser illumination with different powers, energy of photons, and multiple illuminations were also analyzed to understand the light-induced change of material properties. Based on the nonlinear dependence of PCR signal on the excitation power, a theoretical model taking into account both light-induced changes in surface state occupation and LID processes was proposed to explain those temporal behaviors.

  20. Behavior of Photocarriers in the Light-Induced Metastable State in the p-n Heterojunction of a Cu(In,Ga)Se2 Solar Cell with CBD-ZnS Buffer Layer.

    PubMed

    Lee, Woo-Jung; Yu, Hye-Jung; Wi, Jae-Hyung; Cho, Dae-Hyung; Han, Won Seok; Yoo, Jisu; Yi, Yeonjin; Song, Jung-Hoon; Chung, Yong-Duck

    2016-08-31

    We fabricated Cu(In,Ga)Se2 (CIGS) solar cells with a chemical bath deposition (CBD)-ZnS buffer layer grown with varying ammonia concentrations in aqueous solution. The solar cell performance was degraded with increasing ammonia concentration, due to actively dissolved Zn atoms during CBD-ZnS precipitation. These formed interfacial defect states, such as hydroxide species in the CBD-ZnS film, and interstitial and antisite Zn defects at the p-n heterojunction. After light/UV soaking, the CIGS solar cell performance drastically improved, with a rise in fill factor. With the Zn-based buffer layer, the light soaking treatment containing blue photons induced a metastable state and enhanced the CIGS solar cell performance. To interpret this effect, we suggest a band structure model of the p-n heterojunction to explain the flow of photocarriers under white light at the initial state, and then after light/UV soaking. The determining factor is a p+ defect layer, containing an amount of deep acceptor traps, located near the CIGS surface. The p+ defect layer easily captures photoexcited electrons, and then when it becomes quasi-neutral, attracts photoexcited holes. This alters the barrier height and controls the photocurrent at the p-n junction, and fill factor values, determining the solar cell performance. PMID:27494649

  1. Behavior of Photocarriers in the Light-Induced Metastable State in the p-n Heterojunction of a Cu(In,Ga)Se2 Solar Cell with CBD-ZnS Buffer Layer.

    PubMed

    Lee, Woo-Jung; Yu, Hye-Jung; Wi, Jae-Hyung; Cho, Dae-Hyung; Han, Won Seok; Yoo, Jisu; Yi, Yeonjin; Song, Jung-Hoon; Chung, Yong-Duck

    2016-08-31

    We fabricated Cu(In,Ga)Se2 (CIGS) solar cells with a chemical bath deposition (CBD)-ZnS buffer layer grown with varying ammonia concentrations in aqueous solution. The solar cell performance was degraded with increasing ammonia concentration, due to actively dissolved Zn atoms during CBD-ZnS precipitation. These formed interfacial defect states, such as hydroxide species in the CBD-ZnS film, and interstitial and antisite Zn defects at the p-n heterojunction. After light/UV soaking, the CIGS solar cell performance drastically improved, with a rise in fill factor. With the Zn-based buffer layer, the light soaking treatment containing blue photons induced a metastable state and enhanced the CIGS solar cell performance. To interpret this effect, we suggest a band structure model of the p-n heterojunction to explain the flow of photocarriers under white light at the initial state, and then after light/UV soaking. The determining factor is a p+ defect layer, containing an amount of deep acceptor traps, located near the CIGS surface. The p+ defect layer easily captures photoexcited electrons, and then when it becomes quasi-neutral, attracts photoexcited holes. This alters the barrier height and controls the photocurrent at the p-n junction, and fill factor values, determining the solar cell performance.

  2. Time-resolved terahertz dynamics in thin films of the topological insulator Bi2Se3

    SciTech Connect

    Valdés Aguilar, R.; Qi, J.; Brahlek, M.; Bansal, N.; Azad, A.; Bowlan, J.; Oh, S.; Taylor, A. J.; Prasankumar, R. P.; Yarotski, D. A.

    2015-01-07

    We use optical pump–THz probe spectroscopy at low temperatures to study the hot carrier response in thin Bi2Se3 films of several thicknesses, allowing us to separate the bulk from the surface transient response. We find that for thinner films the photoexcitation changes the transport scattering rate and reduces the THz conductivity, which relaxes within 10 picoseconds (ps). For thicker films, the conductivity increases upon photoexcitation and scales with increasing both the film thickness and the optical fluence, with a decay time of approximately 5 ps as well as a much higher scattering rate. Furthermore, these different dynamics are attributed to the surface and bulk electrons, respectively, and demonstrate that long-lived mobile surface photo-carriers can be accessed independently below certain film thicknesses for possible optoelectronic applications.

  3. Probing Electron Dynamics with the Laplacian of the Momentum Density

    SciTech Connect

    Sukumar, N.; MacDougall, Preston J.; Levit, M. Creon

    2012-09-24

    This chapter in the above-titled monograph presents topological analysis of the Laplacian of the electron momentum density in organic molecules. It relates topological features in this distribution to chemical and physical properties, particularly aromaticity and electron transport.

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

    PubMed

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

    2015-08-01

    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.

  5. High Resolution Simulation of Beam Dynamics in Electron Linacs for Free Electron Lasers

    SciTech Connect

    Ryne, R.D.; Venturini, M.; Zholents, A.A.; Qiang, J.

    2009-01-05

    In this paper we report on large scale multi-physics simulation of beam dynamics in electron linacs for next generation free electron lasers (FELs). We describe key features of a parallel macroparticle simulation code including three-dimensional (3D) space-charge effects, short-range structure wake fields, longitudinal coherent synchrotron radiation (CSR) wake fields, and treatment of radiofrequency (RF) accelerating cavities using maps obtained from axial field profiles. A macroparticle up-sampling scheme is described that reduces the shot noise from an initial distribution with a smaller number of macroparticles while maintaining the global properties of the original distribution. We present a study of the microbunching instability which is a critical issue for future FELs due to its impact on beam quality at the end of the linac. Using parameters of a planned FEL linac at Lawrence Berkeley National Laboratory (LBNL), we show that a large number of macroparticles (beyond 100 million) is needed to control numerical shot noise that drives the microbunching instability. We also explore the effect of the longitudinal grid on simulation results. We show that acceptable results are obtained with around 2048 longitudinal grid points, and we discuss this in view of the spectral growth rate predicted from linear theory. As an application, we present results from simulations using one billion macroparticles of the FEL linac under design at LBNL. We show that the final uncorrelated energy spread of the beam depends not only on the initial uncorrelated energy spread but also depends strongly on the shape of the initial current profile. By using a parabolic initial current profile, 5 keV initial uncorrelated energy spread at 40 MeV injection energy, and improved linac design, those simulations demonstrate that a reasonable beam quality can be achieved at the end of the linac, with the final distribution having about 100 keV energy spread, 2.4 GeV energy, and 1.2 kA peak

  6. Electron quantum dynamics in atom-ion interaction.

    PubMed

    Sabzyan, H; Jenabi, M J

    2016-04-01

    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. PMID:27059569

  7. Electron quantum dynamics in atom-ion interaction.

    PubMed

    Sabzyan, H; Jenabi, M J

    2016-04-01

    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.

  8. Electron quantum dynamics in atom-ion interaction

    NASA Astrophysics Data System (ADS)

    Sabzyan, H.; Jenabi, M. J.

    2016-04-01

    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.

  9. Electron and nuclear dynamics in many-electron atoms, molecules and chlorophyll-protein complexes: a review.

    PubMed

    Shuvalov, Vladimir A

    2007-06-01

    It has been shown [V.A. Shuvalov, Quantum dynamics of electrons in many-electron atoms of biologically important compounds, Biochemistry (Mosc.) 68 (2003) 1333-1354; V.A. Shuvalov, Quantum dynamics of electrons in atoms of biologically important molecules, Uspekhi biologicheskoi khimii, (Pushchino) 44 (2004) 79-108] that the orbit angular momentum L of each electron in many-electron atoms is L=mVr=nPlanck's and similar to L for one-electron atom suggested by N. Bohr. It has been found that for an atom with N electrons the total electron energy equation E=-(Z(eff))(2)e(4)m/(2n(2)Planck's(2)N) is more appropriate for energy calculation than standard quantum mechanical expressions. It means that the value of L of each electron is independent of the presence of other electrons in an atom and correlates well to the properties of virtual photons emitted by the nucleus and creating a trap for electrons. The energies for elements of the 1st up to the 5th rows and their ions (total amount 240) of Mendeleev' Periodical table were calculated consistent with the experimental data (deviations in average were 5 x 10(-3)). The obtained equations can be used for electron dynamics calculations in molecules. For H(2) and H(2)(+) the interference of electron-photon orbits between the atoms determines the distances between the nuclei which are in agreement with the experimental values. The formation of resonance electron-photon orbit in molecules with the conjugated bonds, including chlorophyll-like molecules, appears to form a resonance trap for an electron with E values close to experimental data. Two mechanisms were suggested for non-barrier primary charge separation in reaction centers (RCs) of photosynthetic bacteria and green plants by using the idea of electron-photon orbit interference between the two molecules. Both mechanisms are connected to formation of the exciplexes of chlorophyll-like molecules. The first one includes some nuclear motion before exciplex formation, the

  10. Effects of inner electrons on atomic strong-field-ionization dynamics

    NASA Astrophysics Data System (ADS)

    Rapp, J.; Bauer, D.

    2014-03-01

    The influence of inner electrons on the ionization dynamics in strong laser fields is investigated in a wavelength regime where the inner electron dynamics is usually assumed to be negligible. The role of inner electrons is of particular interest for the application of frozen-core approximations and pseudopotentials in time-dependent density functional theory (TDDFT) and the single-active-electron (SAE) approximation in strong-field laser physics. Results of TDDFT and SAE calculations are compared with exact ones obtained by the numerical ab initio solution of the three-electron time-dependent Schrödinger equation for a lithium model atom. It is found that dynamical antiscreening, i.e., a particular form of dynamical core polarization, may substantially alter the ionization rate in the single-photon regime. Requirements for the validity of the approximations in the single and multiphoton ionization domain are identified.

  11. Electron nuclear dynamics of LiH and HF in an intense laser field

    NASA Astrophysics Data System (ADS)

    Broeckhove, J.; Coutinho-Neto, M. D.; Deumens, E.; Öhrn, Y.

    1997-12-01

    The electron nuclear dynamics theory (END) extended to include a time-dependent external field is briefly described. The dynamical equations, in addition to the full electron nuclear coupling terms, now also contain the interactions of both the nuclei and the electrons with the external field. This extended END theory is applied to the study of vibrational excitations of the simple diatomics HF and LiH. The END results using an intense infrared laser field are compared with those of molecular dynamics as well as those from quantum wave-packet calculations. While the effect of the nonadiabatic electron-nuclear coupling terms on the vibrational dynamics is negligible for the chosen application, the electron-field coupling has a significant impact.

  12. Electronic excited states and relaxation dynamics in polymer heterojunction systems

    NASA Astrophysics Data System (ADS)

    Ramon, John Glenn Santos

    The potential for using conducting polymers as the active material in optoelectronic devices has come to fruition in the past few years. Understanding the fundamental photophysics behind their operations points to the significant role played by the polymer interface in their performance. Current device architectures involve the use of bulk heterojunctions which intimately blend the donor and acceptor polymers to significantly increase not only their interfacial surface area but also the probability of exciton formation within the vicinity of the interface. In this dissertation, we detail the role played by the interface on the behavior and performance of bulk heterojunction systems. First, we explore the relation between the exciton binding energy to the band offset in determining device characteristics. As a general rule, when the exciton binding energy is greater than the band offset, the exciton remains the lowest energy excited state leading to efficient light-emitting properties. On the other hand, if the offset is greater than the binding energy, charge separation becomes favorable leading to better photovoltaic behavior. Here, we use a Wannier function, configuration interaction based approach to examine the essential excited states and predict the vibronic absorption and emission spectra of the PPV/BBL, TFB/F8BT and PFB/F8BT heterojunctions. Our results underscore the role of vibrational relaxation in the formation of charge-transfer states following photoexcitation. In addition, we look at the relaxation dynamics that occur upon photoexcitation. For this, we adopt the Marcus-Hush semiclassical method to account for lattice reorganization in the calculation of the interconversion rates in TFB/F8BT and PFB/F8BT. We find that, while a tightly bound charge-transfer state (exciplex) remains the lowest excited state, a regeneration pathway to the optically active lowest excitonic state in TFB/F8BT is possible via thermal repopulation from the exciplex. Finally

  13. Theoretical analysis of hot electron dynamics in nanorods

    PubMed Central

    Kumarasinghe, Chathurangi S.; Premaratne, Malin; Agrawal, Govind P.

    2015-01-01

    Localised surface plasmons create a non-equilibrium high-energy electron gas in nanostructures that can be injected into other media in energy harvesting applications. Here, we derive the rate of this localised-surface-plasmon mediated generation of hot electrons in nanorods and the rate of injecting them into other media by considering quantum mechanical motion of the electron gas. Specifically, we use the single-electron wave function of a particle in a cylindrical potential well and the electric field enhancement factor of an elongated ellipsoid to derive the energy distribution of electrons after plasmon excitation. We compare the performance of nanorods with equivolume nanoparticles of other shapes such as nanospheres and nanopallets and report that nanorods exhibit significantly better performance over a broad spectrum. We present a comprehensive theoretical analysis of how different parameters contribute to efficiency of hot-electron harvesting in nanorods and reveal that increasing the aspect ratio can increase the hot-electron generation and injection, but the volume shows an inverse dependency when efficiency per unit volume is considered. Further, the electron thermalisation time shows much less influence on the injection rate. Our derivations and results provide the much needed theoretical insight for optimization of hot-electron harvesting process in highly adaptable metallic nanorods. PMID:26202823

  14. Ultrafast Electronic Dynamics in Solid and Liquid Gallium Nanoparticles

    NASA Astrophysics Data System (ADS)

    Nisoli, M.; Stagira, S.; de Silvestri, S.; Stella, A.; Tognini, P.; Cheyssac, P.; Kofman, R.

    1997-05-01

    The electron thermalization process both in solid and liquid metallic gallium nanoparticles with radii in the range 50-90 Å is investigated by femtosecond pump-probe measurements. The results show that the temporal behavior of the electron energy relaxation is similar in both phases, with a time constant varying from ~0.6 to ~1.6 ps by increasing the nanoparticle size. We interpret the experimental data in terms of a size-dependent electron-surface interaction model and show the importance of the energy exchange with surface phonons in the electronic thermalization.

  15. Ultrafast electronic dynamics in laser-excited crystalline bismuth

    NASA Astrophysics Data System (ADS)

    Melnikov, Alexey A.; Misochko, Oleg V.; Chekalin, Sergey V.

    2013-07-01

    Femtosecond spectroscopy is applied to study transient electronic processes in bismuth. The components with relaxation times of 1 ps, 7 ps, and ˜1 ns are detected in the photoinduced reflectivity response of the crystal. To facilitate assignment of the observed relaxation to the decay of particular excited electronic states, we use pump pulses with central wavelengths ranging from 400 to 2300 nm. Additionally, we examine the variation of parameters of coherent A1g phonons upon the change of excitation and probing conditions. Data analysis reveals significant wavevector dependence of electron-hole and electron-phonon coupling strength along Γ-T direction of the Brillouin zone.

  16. Observation of strongly forbidden solid effect dynamic nuclear polarization transitions via electron-electron double resonance detected NMR

    SciTech Connect

    Smith, Albert A.; Corzilius, Björn; Haze, Olesya; Swager, Timothy M.; Griffin, Robert G.

    2013-12-07

    We present electron paramagnetic resonance experiments for which solid effect dynamic nuclear polarization transitions were observed indirectly via polarization loss on the electron. This use of indirect observation allows characterization of the dynamic nuclear polarization (DNP) process close to the electron. Frequency profiles of the electron-detected solid effect obtained using trityl radical showed intense saturation of the electron at the usual solid effect condition, which involves a single electron and nucleus. However, higher order solid effect transitions involving two, three, or four nuclei were also observed with surprising intensity, although these transitions did not lead to bulk nuclear polarization—suggesting that higher order transitions are important primarily in the transfer of polarization to nuclei nearby the electron. Similar results were obtained for the SA-BDPA radical where strong electron-nuclear couplings produced splittings in the spectrum of the indirectly observed solid effect conditions. Observation of high order solid effect transitions supports recent studies of the solid effect, and suggests that a multi-spin solid effect mechanism may play a major role in polarization transfer via DNP.

  17. Pulsars as cosmic ray particle accelerators: Dynamics of electrons

    NASA Technical Reports Server (NTRS)

    Thielheim, K. O.

    1985-01-01

    The Lorentz-Dirac-equation with Landau approximation has been solved numerically for electrons in the electromagnetic field of a magnetic dipole rotating with the angular velocity omega perpendicular to its magnetic moment mu. Results are discussed with respect to electron orbits and energy development.

  18. Radiolytic yields of solvated electrons in ionic liquid and its solvation dynamics at low temperature

    NASA Astrophysics Data System (ADS)

    Musat, Raluca M.; Kondoh, Takafumi; Gohdo, Masao; Yoshida, Yoichi; Takahashi, Kenji

    2016-07-01

    We present an investigation of the solvated electron in the ionic liquid 1-butyl-1-methylpyrrolidinium bis(trifluoromethylsulfonyl)imide (P14NTf2) using pulse radiolytic techniques. Temperature-dependent studies reveal that the yield of the solvated electron decreases with decreasing temperature. The lower initial yield measured indicates that we have a loss of some electrons before they become fully solvated. There may be a high probability that the excess dry electrons (pre-solvated electron) react before the electron solvation is completed because the solvation dynamics is slowing down with decreasing temperature.

  19. Coherently driven, ultrafast electron-phonon dynamics in transport junctions

    SciTech Connect

    Szekely, Joshua E.; Seideman, Tamar

    2014-07-28

    Although the vast majority of studies of transport via molecular-scale heterojunctions have been conducted in the (static) energy domain, experiments are currently beginning to apply time domain approaches to the nanoscale transport problem, combining spatial with temporal resolution. It is thus an opportune time for theory to develop models to explore both new phenomena in, and new potential applications of, time-domain, coherently driven molecular electronics. In this work, we study the interaction of a molecular phonon with an electronic wavepacket transmitted via a conductance junction within a time-domain model that treats the electron and phonon on equal footing and spans the weak to strong electron-phonon coupling strengths. We explore interference between two coherent energy pathways in the electronic subspace, thus complementing previous studies of coherent phenomena in conduction junctions, where the stationary framework was used to study interference between spatial pathways. Our model provides new insights into phase decoherence and population relaxation within the electronic subspace, which have been conventionally treated by density matrix approaches that often rely on phenomenological parameters. Although the specific case of a transport junction is explored, our results are general, applying also to other instances of coupled electron-phonon systems.

  20. Photoinduced homogeneous proton-coupled electron transfer: model study of isotope effects on reaction dynamics.

    PubMed

    Venkataraman, Charulatha; Soudackov, Alexander V; Hammes-Schiffer, Sharon

    2009-10-21

    A model Hamiltonian for photoinduced homogeneous proton-coupled electron transfer reactions is presented, and the equations of motion for the reduced density matrix elements in an electron-proton vibronic basis are derived. This formalism enables a detailed analysis of the proton vibrational dynamics, as well as the dynamics of the electronic state populations, following photoexcitation. The application of this theory to model systems provides insight into the fundamental physical principles underlying these types of processes. The initial nonequilibrium state is prepared by vertical photoexcitation from the ground electronic state to a coherent vibrational mixture in the donor electronic state. This nonstationary state relaxes to the equilibrium distributions in the donor and acceptor electronic states via dynamical processes arising from nonadiabatic transitions between the donor and acceptor vibronic states concurrent with energy dissipation to the bath. During the initial stage, when the proton vibrational population in the donor state is distributed among higher vibrational states and the donor proton wavepacket is oscillating with large amplitude, the electronic state population dynamics exhibits virtually no hydrogen/deuterium isotope effect. After vibrational relaxation, when the proton vibrational population in the donor state becomes concentrated in the lower vibrational states and the donor proton wavepacket becomes more localized near the minimum of the donor potential, a significant hydrogen/deuterium isotope effect on the electronic state population dynamics is exhibited. These model system calculations lead to experimentally testable predictions about the qualitative behavior of these isotope effects. PMID:20568867

  1. Electron dynamics upon ionization: Control of the timescale through chemical substitution and effect of nuclear motion

    SciTech Connect

    Vacher, Morgane; Bearpark, Michael J.; Robb, Michael A.; Mendive-Tapia, David

    2015-03-07

    Photoionization can generate a non-stationary electronic state, which leads to coupled electron-nuclear dynamics in molecules. In this article, we choose benzene cation as a prototype because vertical ionization of the neutral species leads to a Jahn-Teller degeneracy between ground and first excited states of the cation. Starting with equal populations of ground and first excited states, there is no electron dynamics in this case. However, if we add methyl substituents that break symmetry but do not radically alter the electronic structure, we see charge migration: oscillations in the spin density that we can correlate with particular localized electronic structures, with a period depending on the gap between the states initially populated. We have also investigated the effect of nuclear motion on electron dynamics using a complete active space self-consistent field (CASSCF) implementation of the Ehrenfest method, most previous theoretical studies of electron dynamics having been carried out with fixed nuclei. In toluene cation for instance, simulations where the nuclei are allowed to move show significant differences in the electron dynamics after 3 fs, compared to simulations with fixed nuclei.

  2. Final Report: Vibrational Dynamics in Photoinduced Electron Transfer

    SciTech Connect

    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

  3. Xenon Implantation in Nanodiamonds: In Situ Transmission Electron Microscopy Study and Molecular Dynamics Simulations

    NASA Astrophysics Data System (ADS)

    Shiryaev, A. A.; Hinks, J.; Marks, N.; Greaves, G.; Donnelly, S.; Fisenko, A. V.; Kiwi, M.

    2016-08-01

    We present results of the first investigation of the Xe implantation process into nanodiamonds of various sizes studied in situ in transmission electron microscope (TEM), complemented by advanced molecular dynamics simulations.

  4. Ultra-fast photo-carrier relaxation in Mott insulators with short-range spin correlations

    PubMed Central

    Eckstein, Martin; Werner, Philipp

    2016-01-01

    Ultra-fast spectroscopy can reveal the interplay of charges with low energy degrees of freedom, which underlies the rich physics of correlated materials. As a potential glue for superconductivity, spin fluctuations in Mott insulators are of particular interest. A theoretical description of the coupled spin and charge degrees of freedom is challenging, because magnetic order is often only short-lived and short-ranged. In this work we theoretically investigate how the spin-charge interactions influence the relaxation of a two-dimensional Mott-Hubbard insulator after photo-excitation. We use a nonequilibrium variant of the dynamical cluster approximation, which, in contrast to single-site dynamical mean-field theory, captures the effect of short-range correlations. The relaxation time is found to scale with the strength of the nearest-neighbor spin correlations, and can be 10–20 fs in the cuprates. Increasing the temperature or excitation density decreases the spin correlations and thus implies longer relaxation times. This may help to distinguish the effect of spin-fluctuations on the charge relaxation from the influence of other bosonic modes in the solid. PMID:26883536

  5. Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy

    NASA Astrophysics Data System (ADS)

    Ramasesha, Krupa; Leone, Stephen R.; Neumark, Daniel M.

    2016-05-01

    Attosecond science has paved the way for direct probing of electron dynamics in gases and solids. This review provides an overview of recent attosecond measurements, focusing on the wealth of knowledge obtained by the application of isolated attosecond pulses in studying dynamics in gases and solid-state systems. Attosecond photoelectron and photoion measurements in atoms reveal strong-field tunneling ionization and a delay in the photoemission from different electronic states. These measurements applied to molecules have shed light on ultrafast intramolecular charge migration. Similar approaches are used to understand photoemission processes from core and delocalized electronic states in metal surfaces. Attosecond transient absorption spectroscopy is used to follow the real-time motion of valence electrons and to measure the lifetimes of autoionizing channels in atoms. In solids, it provides the first measurements of bulk electron dynamics, revealing important phenomena such as the timescales governing the switching from an insulator to a metallic state and carrier-carrier interactions.

  6. Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy.

    PubMed

    Ramasesha, Krupa; Leone, Stephen R; Neumark, Daniel M

    2016-05-27

    Attosecond science has paved the way for direct probing of electron dynamics in gases and solids. This review provides an overview of recent attosecond measurements, focusing on the wealth of knowledge obtained by the application of isolated attosecond pulses in studying dynamics in gases and solid-state systems. Attosecond photoelectron and photoion measurements in atoms reveal strong-field tunneling ionization and a delay in the photoemission from different electronic states. These measurements applied to molecules have shed light on ultrafast intramolecular charge migration. Similar approaches are used to understand photoemission processes from core and delocalized electronic states in metal surfaces. Attosecond transient absorption spectroscopy is used to follow the real-time motion of valence electrons and to measure the lifetimes of autoionizing channels in atoms. In solids, it provides the first measurements of bulk electron dynamics, revealing important phenomena such as the timescales governing the switching from an insulator to a metallic state and carrier-carrier interactions. PMID:26980312

  7. Electron-Nuclear Dynamics of collision processes: Charge exchange and energy loss

    NASA Astrophysics Data System (ADS)

    Cabrera-Trujillo, Remigio; Sabin, John R.; Öhrn, Yngve; Deumens, Erik

    2004-03-01

    We present the Electron-Nuclear Dynamics (END) method for the study of time-dependent scattering processes. The END is a general approach for treating time-dependent problems which includes the dynamics of electrons and nuclei simultaneously by considering the full electron-nuclear coupling in the system and thus eliminates the necessity of constructing potential-energy surfaces. The theory approximates the time dependent Schrödinger equation starting from the time dependent variational principle by deriving a Hamiltonian dynamical system for time dependent nuclear and electronic wave function parameters. The wave function is described in a coherent state manifold, which leads to a system of Hamilton's equations of motion. Emphasis is put on electron exchange, differential cross section and energy loss (stopping cross section) of collision of ions, atoms and molecules involving H, He, C, N, O, and Ne atoms. We compare our results to available experimental data.

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

    SciTech Connect

    Iuchi, Satoru; Koga, Nobuaki

    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.

  9. High-temperature high-pressure phases of lithium from electron force field (eFF) quantum electron dynamics simulations

    PubMed Central

    Kim, Hyungjun; Su, Julius T.; Goddard, William A.

    2011-01-01

    We recently developed the electron force field (eFF) method for practical nonadiabatic electron dynamics simulations of materials under extreme conditions and showed that it gave an excellent description of the shock thermodynamics of hydrogen from molecules to atoms to plasma, as well as the electron dynamics of the Auger decay in diamondoids following core electron ionization. Here we apply eFF to the shock thermodynamics of lithium metal, where we find two distinct consecutive phase changes that manifest themselves as a kink in the shock Hugoniot, previously observed experimentally, but not explained. Analyzing the atomic distribution functions, we establish that the first phase transition corresponds to (i) an fcc-to-cI16 phase transition that was observed previously in diamond anvil cell experiments at low temperature and (ii) a second phase transition that corresponds to the formation of a new amorphous phase (amor) of lithium that is distinct from normal molten lithium. The amorphous phase has enhanced valence electron-nucleus interactions due to localization of electrons into interstitial locations, along with a random connectivity distribution function. This indicates that eFF can characterize and compute the relative stability of states of matter under extreme conditions (e.g., warm dense matter). PMID:21873210

  10. Fluctuations in Electronic Energy Affecting Singlet Fission Dynamics and Mixing with Charge-Transfer State: Quantum Dynamics Study.

    PubMed

    Fujihashi, Yuta; Ishizaki, Akihito

    2016-02-01

    Singlet fission is a spin-allowed process by which a singlet excited state is converted to two triplet states. To understand mechanisms of the ultrafast fission via a charge transfer (CT) state, one has investigated the dynamics through quantum-dynamical calculations with the uncorrelated fluctuation model; however, the electronic states are expected to experience the same fluctuations induced by the surrounding molecules because the electronic structure of the triplet pair state is similar to that of the singlet state except for the spin configuration. Therefore, the fluctuations in the electronic energies could be correlated, and the 1D reaction coordinate model may adequately describe the fission dynamics. In this work we develop a model for describing the fission dynamics to explain the experimentally observed behaviors. We also explore impacts of fluctuations in the energy of the CT state on the fission dynamics and the mixing with the CT state. The overall behavior of the dynamics is insensitive to values of the reorganization energy associated with the transition from the singlet state to the CT state, although the coherent oscillation is affected by the fluctuations. This result indicates that the mixing with the CT state is rather robust under the fluctuations in the energy of the CT state as well as the high-lying CT state. PMID:26732701

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

    PubMed

    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

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

    PubMed

    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

  13. Irving Langmuir Prize in Chemical Physics Talk: Attosecond Electron Dynamics

    NASA Astrophysics Data System (ADS)

    Leone, Stephen

    2011-03-01

    Isolated attosecond pulses are produced by the process of high order harmonics, and these pulses are used as a soft X-ray probe in wavelength-dispersed transient absorption. Inner shell core-level spectroscopic transitions are thus used to analyze the chemical and electronic environment of specific atomic states as a function of time following ionization and dissociation. High field ionization processes, using 800 nm pulses, result in spin-orbit electronic state populations, alignment, and electronic wave packet superpositions, all of which are investigated by the spectrally-resolved X-ray probe. By using isolated attosecond pulses as the probe, high field ionization events on a subfemtosecond timescale are investigated. The generality of the transient absorption method for attosecond dyamics is described, as well as the challenges during the pump-probe pulse overlap time period. The results are compared to theoretical calculations by collaborators. Supported by DOE, NSF and AFOSR.

  14. Beam dynamics studies and parametric characterization of a standing wave electron linac

    NASA Astrophysics Data System (ADS)

    Dash, R.; Mondal, J.; Sharma, A.; Mittal, K. C.

    2013-07-01

    This paper presents the results of electron beam tracking simulations for a 30 MeV standing wave electron linac at Electron Beam Centre Kharghar, Navi Mumbai, India. For the pulsed mode operation of the present linac preferential operation parameters have been determined from the results of beam dynamics studies. This electron accelerator is a general purpose facility for generation of Bremsstrahlung X-rays and neutron scattering experiments. This electron accelerator-based experimental neutron facility will be used for measurement of neutron cross-section (n,γ), (n, xn) and (n, f) reactions at different energies for various materials and material irradiation studies.

  15. Molecular dynamics study of electron-irradiation effects in single-walled carbon nanotubes

    SciTech Connect

    Yasuda, Masaaki; Kimoto, Yoshihisa; Tada, Kazuhiro; Mori, Hideki; Akita, Seiji; Hirai, Yoshihiko; Nakayama, Yoshikazu

    2007-05-15

    Molecular dynamics studies are carried out to investigate electron-irradiation effects in single-walled carbon nanotubes. We have proposed a simulation model which includes the interaction between a high-energy incident electron and a carbon atom, based on Monte Carlo method using the elastic-scattering cross section. The atomic level behavior of a single-walled carbon nanotube under electron irradiation is demonstrated in nanosecond time scale. The incident electron energy, tube diameter, and tube temperature dependences of electron-irradiation effects are studied with the simulation.

  16. Dynamical mechanism of charge separation by photoexcited generation of proton-electron pairs in organic molecular systems. A nonadiabatic electron wavepacket dynamics study

    NASA Astrophysics Data System (ADS)

    Yamamoto, Kentaro; Takatsuka, Kazuo

    2016-08-01

    In this perspective article, we review, along with presenting new results, a series of our theoretical analyses on the excited-state mechanism of charge separation (proton-electron pair creation) relevant to the photoinduced water-splitting reaction (2H2O → 4H+ + 4e- + O2) in organic and biological systems, which quite often includes Mn clusters in various molecular configurations. The present mechanism is conceived to be universal in the triggering process of the photoexcited water splitting dynamics. In other words, any Mn-based catalytic charge separation is quite likely to be initiated according to this mechanism. As computationally tractable yet realistic models, we examine a series of systems generally expressed as X-Mn-OH2⋯A, where X = (OH, Ca(OH)3) and A = (N-methylformamidine, guanidine, imidazole or ammonia cluster) in terms of the theory of nonadiabatic electron wavepacket dynamics. We first find both an electron and a proton are simultaneously transferred to the acceptors through conical intersections upon photoexcitation. In this mechanism, the electron takes different pathways from that of the proton and reaches the densely lying Rydberg-like states of the acceptors in the end, thereby inducing charge separation. Therefore the presence of the Rydberg-like diffused unoccupied states as an electron acceptor is critical for this reaction to proceed. We also have found another crucial nonadiabatic process that deteriorates the efficiency of charge separation by rendering the created pair of proton and electron back to the originally donor site through the states of d-d band originated from Mn atom. Repetition of this process gradually annihilates the created pair of proton and electron in a way different from the usual charge recombination process. We address this dynamics by means of our proposed path-branching representation. The dynamical roles of a doped Ca atom are also uncovered, which are relevant to controlling the pathways of electron

  17. Dynamic Testing with Tangible Electronics: Measuring Children's Change in Strategy Use with a Series Completion Task

    ERIC Educational Resources Information Center

    Resing, Wilma C. M.; Elliott, Julian G.

    2011-01-01

    Aims: This study sought to explore the use of a novel approach that incorporates dynamic testing and tangible electronics in the assessment of children's learning potential and strategy use. Sample: A total of 77 children with a mean age 8.9 years participated in the study; half of them were dynamically tested using graduate prompt techniques; the…

  18. Density matrix renormalization group with efficient dynamical electron correlation through range separation

    SciTech Connect

    Hedegård, Erik Donovan Knecht, Stefan; Reiher, Markus; Kielberg, Jesper Skau; Jensen, Hans Jørgen Aagaard

    2015-06-14

    We present a new hybrid multiconfigurational method based on the concept of range-separation that combines the density matrix renormalization group approach with density functional theory. This new method is designed for the simultaneous description of dynamical and static electron-correlation effects in multiconfigurational electronic structure problems.

  19. Dynamics of fast electron beams and bounded targets

    NASA Astrophysics Data System (ADS)

    Zabala, N.; Rivacoba, A.

    2015-07-01

    We analyze the full relativistic force experienced by swift electrons moving close to planar films for the experimental conditions commonly used in electron energy loss spectroscopy in STEM. In metals the main effects derive from the dispersion of the surface plasmons, which are clearly observed in the EEL spectra. In insulators we explore the role played by the Cherenkov radiation (CR) emitted in the energy gap window. The focus is placed on the transverse force and different factors which may turn this force into repulsive, as reported in recent experimental and theoretical works.

  20. Electron plasma dynamics during autoresonant excitation of the diocotron mode

    SciTech Connect

    Baker, C. J. Danielson, J. R. Hurst, N. C. Surko, C. M.

    2015-02-15

    Chirped-frequency autoresonant excitation of the diocotron mode is used to move electron plasmas confined in a Penning-Malmberg trap across the magnetic field for advanced plasma and antimatter applications. Plasmas of 10{sup 8} electrons, with radii small compared to that of the confining electrodes, can be moved from the magnetic axis to ≥90% of the electrode radius with near unit efficiency and reliable angular positioning. Translations of ≥70% of the wall radius are possible for a wider range of plasma parameters. Details of this process, including phase and displacement oscillations in the plasma response and plasma expansion, are discussed, as well as possible extensions of the technique.

  1. Femtosecond time-resolved electronic relaxation dynamics in tetrathiafulvalene

    SciTech Connect

    Staedter, D.; Polizzi, L.; Thiré, N.; Mairesse, Y.; Mayer, P.; Blanchet, V.

    2015-05-21

    In the present paper, the ultrafast electronic relaxation of tetrathiafulvalene (TTF) initiated around 4 eV is studied by femtosecond time-resolved velocity-map imaging. The goal is to investigate the broad double structure observed in the absorption spectrum at this energy. By monitoring the transients of the parent cation and its fragments and by varying the pump and the probe wavelengths, two internal conversions and intramolecular vibrational relaxation are detected both on the order of a few hundred of femtoseconds. Photoelectron images permit the assignment of a dark electronic state involved in the relaxation. In addition, the formation of the dimer of TTF has been observed.

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

    DOE PAGESBeta

    Caro, A.; Correa, A. A.; Tamm, A.; Samolyuk, G. D.; Stocks, G. M.

    2015-10-16

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

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

    SciTech Connect

    Caro, A.; Correa, A. A.; Tamm, A.; Samolyuk, G. D.; Stocks, G. M.

    2015-10-16

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

  4. Measuring Conformational Dynamics of Single Biomolecules Using Nanoscale Electronic Devices

    NASA Astrophysics Data System (ADS)

    Akhterov, Maxim V.; Choi, Yongki; Sims, Patrick C.; Olsen, Tivoli J.; Gul, O. Tolga; Corso, Brad L.; Weiss, Gregory A.; Collins, Philip G.

    2014-03-01

    Molecular motion can be a rate-limiting step of enzyme catalysis, but motions are typically too quick to resolve with fluorescent single molecule techniques. Recently, we demonstrated a label-free technique that replaced fluorophores with nano-electronic circuits to monitor protein motions. The solid-state electronic technique used single-walled carbon nanotube (SWNT) transistors to monitor conformational motions of a single molecule of T4 lysozyme while processing its substrate, peptidoglycan. As lysozyme catalyzes the hydrolysis of glycosidic bonds, two protein domains undergo 8 Å hinge bending motion that generates an electronic signal in the SWNT transistor. We describe improvements to the system that have extended our temporal resolution to 2 μs . Electronic recordings at this level of detail directly resolve not just transitions between open and closed conformations but also the durations for those transition events. Statistical analysis of many events determines transition timescales characteristic of enzyme activity and shows a high degree of variability within nominally identical chemical events. The high resolution technique can be readily applied to other complex biomolecules to gain insights into their kinetic parameters and catalytic function.

  5. Dynamics of Dissociative Electron Attachment to Uracil and Furane

    NASA Astrophysics Data System (ADS)

    Fonseca Dos Santos, Samantha; Douguet, Nicolas; Orel, Ann; Rescigno, Thomas

    2016-05-01

    We present the results of a theoretical study of dissociative electron attachment (DEA) to Uracil and Furan. In both cases we will present calculated angular distributions based on analysis of the entrance amplitudes obtained from the results of complex Kohn scattering calculations. For uracil, we will compare our results with available experimentally measured angular distributions obtained using the COLTRIMS method.

  6. Attosecond dynamics of electrons in molecules and liquids

    NASA Astrophysics Data System (ADS)

    Woerner, Hans Jakob

    2016-05-01

    The ultrafast motion of electrons and holes following light-matter interaction is fundamental to a broad range of chemical and biophysical processes. In this lecture, I will discuss two recent experiments carried out in our group that measure the atomic-scale motion of charge with attosecond temporal resolution (1 as = 10-18 s). The first experiment is carried out on isolated, spatially oriented molecules in the gas phase. We advance high-harmonic spectroscopy to resolve spatially and temporally the migration of an electron hole immediately following ionization of iodoacetylene, while simultaneously demonstrating extensive control over the process. A multidimensional approach, based on the measurement of both even and odd harmonic orders, enables us to reconstruct both quantum amplitudes and phases of the electronic states with a resolution of ~ 100 as. We separately reconstruct quasi-field-free and laser-controlled charge migration as a function of the spatial orientation of the molecule and determine the shape of the hole created by ionization. The second experiment is carried out on a free-flowing microjet of liquid water. We use an attosecond pulse train synchronized with a near-infrared laser pulse to temporally resolve the process of photoemission from liquid water using the RABBIT technique. We measure a delay on the order of 50 as between electrons emitted from the HOMO of liquid water compared to that of gas-phase water and a substantially reduced modulation contrast of the corresponding sidebands. Since our measurements on solvated water molecules are referenced to isolated ones, the measured delays reflect (i) the photoionization delays caused by electron transport through the aqueous environment and (ii) the effect of solvation on the parent molecule. The relative modulation contrast, in turn, contains information on (iii) the modification of transition amplitudes and (iv) dephasing processes. These experiments make the liquid phase and its fascinating

  7. Ab initio molecular dynamics study of the static, dynamic, and electronic properties of liquid mercury at room temperature.

    PubMed

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

    2009-05-21

    We report a study on several static, dynamic, and electronic properties of liquid Hg at room temperature. We have performed ab initio molecular dynamics simulations using Kohn-Sham density functional theory combined with a nonlocal ultrasoft pseudopotential. The calculated static structure shows good agreement with the available experimental data. We present results for the single-particle dynamics, and recent experimental data are analyzed. The calculated dynamic structure factors S(q,omega) fairly agree with their experimental counterparts as measured by inelastic x-ray (and neutron) scattering experiments. The dispersion relation exhibits a positive dispersion, which however is not so marked as suggested by the experiment; moreover, its slope at the long-wavelength limit provides a good estimate of the experimental sound velocity. We have also analyzed the dynamical processes behind the S(q,omega) in terms of a model including a relaxation mechanism with both fast and slow characteristic time scales. PMID:19466841

  8. Ring current electron dynamics during geomagnetic storms based on the Van Allen Probes measurements

    NASA Astrophysics Data System (ADS)

    Zhao, H.; Li, X.; Baker, D. N.; Claudepierre, S. G.; Fennell, J. F.; Blake, J. B.; Larsen, B. A.; Skoug, R. M.; Funsten, H. O.; Friedel, R. H. W.; Reeves, G. D.; Spence, H. E.; Mitchell, D. G.; Lanzerotti, L. J.

    2016-04-01

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

  9. Dynamics of Lopsided Energy Sharing between a Photoelectron and an Auger Electron in Solids

    NASA Astrophysics Data System (ADS)

    Iwano, Kaoru; Nasu, Keiichiro

    1995-09-01

    We study the dynamics of lopsided energy sharing between a photoelectron and an Auger electron in solids. The problem is formulated as an optical response theory, in which the energy distribution spectrum for these two propagating electrons is expressed in terms of T matrices. In order to perform numerical calculations, we use two different models, which are a partial-wave model and a cubic-lattice model. Firstly, we concentrate on the effect given by the change of the atomic valency following the Auger decay. As a result, in the former model we have reproduced the lopsidedness in the peak shifts and distortions of the main peaks. Such lopsidedness is realized even in the latter model in spite of the strong mixing among different partial waves. Furthermore, it should be emphasized that various types of dynamics can occur according to the local electronic structure around the atom of which core electron is excited. In particular, the energy spectrum of the two electrons receive modulations representing the local density of states around the initial atom. This is because the phenomenon is essentially local in the sense that both the electrons must be inside the Coulomb-potential region of the atom for the energy sharing to occur. Next, we study the effect of electron-electron scattering between the two propagating electrons, using a perturbation theory. It is concluded that, when the electron-electron scattering is weak enough, its effect is against the previous one and so reduces the lopsidedness in the energy sharing.

  10. Effects of surface trapped excess electrons on the dynamics of HCl adsorbed ice surfaces

    NASA Astrophysics Data System (ADS)

    Yoon, Yeohoon; Shin, Seokmin

    2007-05-01

    We report results of Car-Parrinello molecular dynamics simulations showing the effect of surface trapped electrons on the dynamics of HCl adsorbed ice surfaces. It is found that the existence of excess electrons can lead to extensive changes in structural and electronic properties of ice surfaces, which provide better environments for proton transfer. The results of simulations show rapid exchanging mechanism of the proton under such environment, suggesting the importance of interlayer proton transfer in the heterogeneous reaction of HCl adsorbed ice surfaces.

  11. Monitoring Nonadiabatic Electron-Nuclear Dynamics in Molecules by Attosecond Streaking of Photoelectrons

    NASA Astrophysics Data System (ADS)

    Kowalewski, Markus; Bennett, Kochise; Rouxel, Jérémy R.; Mukamel, Shaul

    2016-07-01

    Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry additional phase information, which can be retrieved by the streaking technique. In this contribution we extend the streaking formalism to include coupled electron and nuclear dynamics in molecules as well as initial coherences. We demonstrate how streaked photoelectrons offer a novel tool for monitoring nonadiabatic dynamics as it occurs in the vicinity of conical intersections and avoided crossings. Streaking can provide high time resolution direct signatures of electronic coherences, which affect many primary photochemical and biological events.

  12. Single-molecule interfacial electron transfer dynamics manipulated by an external electric current.

    PubMed

    Zhang, Guofeng; Xiao, Liantuan; Chen, Ruiyun; Gao, Yan; Wang, Xiaobo; Jia, Suotang

    2011-08-14

    Interfacial electron transfer (IET) dynamics in a 1,1'-dioctadecyl-3,3,3',3'-tetramethylindodicarbocyanine (DiD) dye molecule/indium tin oxide (ITO) film system have been probed at the ensemble and single-molecule levels. By comparing the difference in the external electric current (EEC) dependence of the fluorescence intensities and lifetimes of the ensembles and single molecules, it is shown that the single-molecule probe can effectively demonstrate IET dynamics. The backward electron transfer and electron transfer from the ground state induce single-molecule fluorescence quenching when an EEC is applied to the DiD/ITO film system.

  13. Monitoring Nonadiabatic Electron-Nuclear Dynamics in Molecules by Attosecond Streaking of Photoelectrons.

    PubMed

    Kowalewski, Markus; Bennett, Kochise; Rouxel, Jérémy R; Mukamel, Shaul

    2016-07-22

    Streaking of photoelectrons has long been used for the temporal characterization of attosecond extreme ultraviolet pulses. When the time-resolved photoelectrons originate from a coherent superposition of electronic states, they carry additional phase information, which can be retrieved by the streaking technique. In this contribution we extend the streaking formalism to include coupled electron and nuclear dynamics in molecules as well as initial coherences. We demonstrate how streaked photoelectrons offer a novel tool for monitoring nonadiabatic dynamics as it occurs in the vicinity of conical intersections and avoided crossings. Streaking can provide high time resolution direct signatures of electronic coherences, which affect many primary photochemical and biological events. PMID:27494470

  14. Dynamic modulation of electronic properties of graphene by localized carbon doping using focused electron beam induced deposition

    NASA Astrophysics Data System (ADS)

    Kim, S.; Russell, M.; Henry, M.; Kim, S. S.; Naik, R. R.; Voevodin, A. A.; Jang, S. S.; Tsukruk, V. V.; Fedorov, A. G.

    2015-09-01

    We report on the first demonstration of controllable carbon doping of graphene to engineer local electronic properties of a graphene conduction channel using focused electron beam induced deposition (FEBID). Electrical measurements indicate that an ``n-p-n'' junction on graphene conduction channel is formed by partial carbon deposition near the source and drain metal contacts by low energy (<50 eV) secondary electrons due to inelastic collisions of long range backscattered primary electrons generated from a low dose of high energy (25 keV) electron beam (1 × 1018 e- per cm2). Detailed AFM imaging provides direct evidence of the new mechanism responsible for dynamic evolution of the locally varying graphene doping. The FEBID carbon atoms, which are physisorbed and weakly bound to graphene, diffuse towards the middle of graphene conduction channel due to their surface chemical potential gradient, resulting in negative shift of Dirac voltage. Increasing a primary electron dose to 1 × 1019 e- per cm2 results in a significant increase of carbon deposition, such that it covers the entire graphene conduction channel at high surface density, leading to n-doping of graphene channel. Collectively, these findings establish a unique capability of FEBID technique to dynamically modulate the doping state of graphene, thus enabling a new route to resist-free, ``direct-write'' functional patterning of graphene-based electronic devices with potential for on-demand re-configurability.We report on the first demonstration of controllable carbon doping of graphene to engineer local electronic properties of a graphene conduction channel using focused electron beam induced deposition (FEBID). Electrical measurements indicate that an ``n-p-n'' junction on graphene conduction channel is formed by partial carbon deposition near the source and drain metal contacts by low energy (<50 eV) secondary electrons due to inelastic collisions of long range backscattered primary electrons generated

  15. Dynamic behavior of ion acoustic waves in electron-positron-ion magnetoplasmas with superthermal electrons and positrons

    SciTech Connect

    Saha, Asit E-mail: prasantachatterjee1@rediffmail.com; Pal, Nikhil; Chatterjee, Prasanta E-mail: prasantachatterjee1@rediffmail.com

    2014-10-15

    The dynamic behavior of ion acoustic waves in electron-positron-ion magnetoplasmas with superthermal electrons and positrons has been investigated in the framework of perturbed and non-perturbed Kadomtsev-Petviashili (KP) equations. Applying the reductive perturbation technique, we have derived the KP equation in electron-positron-ion magnetoplasma with kappa distributed electrons and positrons. Bifurcations of ion acoustic traveling waves of the KP equation are presented. Using the bifurcation theory of planar dynamical systems, the existence of the solitary wave solutions and the periodic traveling wave solutions has been established. Two exact solutions of these waves have been derived depending on the system parameters. Then, using the Hirota's direct method, we have obtained two-soliton and three-soliton solutions of the KP equation. The effect of the spectral index κ on propagations of the two-soliton and the three-soliton has been shown. Considering an external periodic perturbation, we have presented the quasi periodic behavior of ion acoustic waves in electron-positron-ion magnetoplasmas.

  16. Distribution and dynamics of electron transport complexes in cyanobacterial thylakoid membranes☆

    PubMed Central

    Liu, Lu-Ning

    2016-01-01

    The cyanobacterial thylakoid membrane represents a system that can carry out both oxygenic photosynthesis and respiration simultaneously. The organization, interactions and mobility of components of these two electron transport pathways are indispensable to the biosynthesis of thylakoid membrane modules and the optimization of bioenergetic electron flow in response to environmental changes. These are of fundamental importance to the metabolic robustness and plasticity of cyanobacteria. This review summarizes our current knowledge about the distribution and dynamics of electron transport components in cyanobacterial thylakoid membranes. Global understanding of the principles that govern the dynamic regulation of electron transport pathways in nature will provide a framework for the design and synthetic engineering of new bioenergetic machinery to improve photosynthesis and biofuel production. This article is part of a Special Issue entitled: Organization and dynamics of bioenergetic systems in bacteria, edited by Conrad Mullineaux. PMID:26619924

  17. Distribution and dynamics of electron transport complexes in cyanobacterial thylakoid membranes.

    PubMed

    Liu, Lu-Ning

    2016-03-01

    The cyanobacterial thylakoid membrane represents a system that can carry out both oxygenic photosynthesis and respiration simultaneously. The organization, interactions and mobility of components of these two electron transport pathways are indispensable to the biosynthesis of thylakoid membrane modules and the optimization of bioenergetic electron flow in response to environmental changes. These are of fundamental importance to the metabolic robustness and plasticity of cyanobacteria. This review summarizes our current knowledge about the distribution and dynamics of electron transport components in cyanobacterial thylakoid membranes. Global understanding of the principles that govern the dynamic regulation of electron transport pathways in nature will provide a framework for the design and synthetic engineering of new bioenergetic machinery to improve photosynthesis and biofuel production. This article is part of a Special Issue entitled: Organization and dynamics of bioenergetic systems in bacteria, edited by Conrad Mullineaux.

  18. Measuring correlated electronic and vibrational spectral dynamics using line shapes in two-dimensional electronic-vibrational spectroscopy

    NASA Astrophysics Data System (ADS)

    Lewis, Nicholas H. C.; Dong, Hui; Oliver, Thomas A. A.; Fleming, Graham R.

    2015-05-01

    Two-dimensional electronic-vibrational (2DEV) spectroscopy is an experimental technique that shows great promise in its ability to provide detailed information concerning the interactions between the electronic and vibrational degrees of freedom in molecular systems. The physical quantities 2DEV is particularly suited for measuring have not yet been fully determined, nor how these effects manifest in the spectra. In this work, we investigate the use of the center line slope of a peak in a 2DEV spectrum as a measure of both the dynamic and static correlations between the electronic and vibrational states of a dye molecule in solution. We show how this center line slope is directly related to the solvation correlation function for the vibrational degrees of freedom. We also demonstrate how the strength with which the vibration on the electronic excited state couples to its bath can be extracted from a set of 2DEV spectra. These analytical techniques are then applied to experimental data from the laser dye 3,3'-diethylthiatricarbocyanine iodide in deuterated chloroform, where we determine the lifetime of the correlation between the electronic transition frequency and the transition frequency for the backbone C = C stretch mode to be ˜1.7 ps. Furthermore, we find that on the electronic excited state, this mode couples to the bath ˜1.5 times more strongly than on the electronic ground state.

  19. Measuring correlated electronic and vibrational spectral dynamics using line shapes in two-dimensional electronic-vibrational spectroscopy

    SciTech Connect

    Lewis, Nicholas H. C.; Dong, Hui; Oliver, Thomas A. A.; Fleming, Graham R.

    2015-05-07

    Two-dimensional electronic-vibrational (2DEV) spectroscopy is an experimental technique that shows great promise in its ability to provide detailed information concerning the interactions between the electronic and vibrational degrees of freedom in molecular systems. The physical quantities 2DEV is particularly suited for measuring have not yet been fully determined, nor how these effects manifest in the spectra. In this work, we investigate the use of the center line slope of a peak in a 2DEV spectrum as a measure of both the dynamic and static correlations between the electronic and vibrational states of a dye molecule in solution. We show how this center line slope is directly related to the solvation correlation function for the vibrational degrees of freedom. We also demonstrate how the strength with which the vibration on the electronic excited state couples to its bath can be extracted from a set of 2DEV spectra. These analytical techniques are then applied to experimental data from the laser dye 3,3′-diethylthiatricarbocyanine iodide in deuterated chloroform, where we determine the lifetime of the correlation between the electronic transition frequency and the transition frequency for the backbone C = C stretch mode to be ∼1.7 ps. Furthermore, we find that on the electronic excited state, this mode couples to the bath ∼1.5 times more strongly than on the electronic ground state.

  20. Electron dynamics in a subproton-gyroscale magnetic hole

    NASA Astrophysics Data System (ADS)

    Gershman, Daniel J.; Dorelli, John C.; Viñas, Adolfo F.; Avanov, Levon A.; Gliese, Ulrik; Barrie, Alexander C.; Coffey, Victoria; Chandler, Michael; Dickson, Charles; MacDonald, Elizabeth A.; Salo, Chad; Holland, Matthew; Saito, Yoshifumi; Sauvaud, Jean-Andre; Lavraud, Benoit; Paterson, William R.; Torbert, Roy; Chen, Li-Jen; Goodrich, Katherine; Russell, Christopher T.; Strangeway, Robert J.; Giles, Barbara L.; Pollock, Craig J.; Moore, Thomas E.; Burch, James L.

    2016-05-01

    Magnetic holes are ubiquitous in space plasmas, occurring in the solar wind, downstream of planetary bow shocks, and inside the magnetosphere. Recently, kinetic-scale magnetic holes have been observed near Earth's central plasma sheet. The Fast Plasma Investigation on NASA's Magnetospheric Multiscale (MMS) mission enables measurement of both ions and electrons with 2 orders of magnitude increased temporal resolution over previous magnetospheric instruments. Here we present data from MMS taken in Earth's nightside plasma sheet and use high-resolution particle and magnetometer data to characterize the structure of a subproton-scale magnetic hole. Electrons with gyroradii above the thermal gyroradius but below the current layer thickness carry a current sufficient to account for a ~10-20% depression in magnetic field magnitude. These observations suggest that the size and magnetic depth of kinetic-scale magnetic holes is strongly dependent on the background plasma conditions.

  1. Probing Transient Electron Dynamics Using Ultrafast X Rays

    NASA Astrophysics Data System (ADS)

    Bucksbaum, Philip

    2016-05-01

    Linear x-ray absorption in atoms or molecules creates highly excited multi-electron quantum systems, which relax rapidly by fluorescence or Auger emission. These relaxation rates are usually less than a few femtoseconds in duration, and so they can reveal transient elecronic states in molecules as they undergo photo-induced transformations. I will show recent results from femtosecond x-ray experiments that display this phenomenon. There are efforts underway to push the temporal resolving power of ultrafast x-ray pulses into the attosecond regime, using stronger fields to initiate nonlinear absorption processes such as transient stimulated electronic Raman scattering. I will discuss current progress and future prospects for research in this area. This research is supported through Stanford PULSE Institute, SLAC National Accelerator Lab by the U.S. Department of Energy, Office of Basic Energy Sciences, Atomic, Molecular, and Optical Science Program.

  2. Melt pool dynamics during selective electron beam melting

    NASA Astrophysics Data System (ADS)

    Scharowsky, T.; Osmanlic, F.; Singer, R. F.; Körner, C.

    2014-03-01

    Electron beam melting is a promising additive manufacturing technique for metal parts. Nevertheless, the process is still poorly understood making further investigations indispensable to allow a prediction of the part's quality. To improve the understanding of the process especially the beam powder interaction, process observation at the relevant time scale is necessary. Due to the difficult accessibility of the building area, the high temperatures, radiation and the very high scanning speeds during the melting process the observation requires an augmented effort in the observation equipment. A high speed camera in combination with an illumination laser, band pass filter and mirror system is suitable for the observation of the electron beam melting process. The equipment allows to observe the melting process with a high spatial and temporal resolution. In this paper the adjustment of the equipment and results of the lifetime and the oscillation frequencies of the melt pool for a simple geometry are presented.

  3. Proton Dynamics on Goethite Nanoparticles and Coupling to Electron Transport

    SciTech Connect

    Zarzycki, Piotr P.; Smith, Dayle MA; Rosso, Kevin M.

    2015-04-14

    The surface chemistry of metal oxide particles is governed by the charge that develops at the interface with aqueous solution. Mineral transformation, biogeochemical reactions, remediation, and sorption dynamics are profoundly affected in response. Here we report implementation of replica-exchange constant-pH molecular dynamics simulations that use classical molecular dynamics for exploring configurational space and Metropolis Monte Carlo walking through protonation space with a simulated annealing escape route from metastable configurations. By examining the archetypal metal oxide, goethite (α-FeOOH), we find that electrostatic potential gradients spontaneously arise between intersecting low-index crystal faces and across explicitly treated oxide nanoparticles at a magnitude exceeding the Johnson–Nyquist voltage fluctuation. Fluctuations in adsorbed proton density continuously repolarize the surface potential bias between edge-sharing crystal faces, at a rate slower than the reported electron–polaron hopping rate in goethite interiors. This suggests that these spontaneous surface potential fluctuations will control the net movement of charge carriers in the lattice.

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

    NASA Technical Reports Server (NTRS)

    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.

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

    NASA Astrophysics Data System (ADS)

    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.

  6. "Watching" Polaron Pair Formation from First-Principles Electron-Nuclear Dynamics.

    PubMed

    Donati, Greta; Lingerfelt, David B; Petrone, Alessio; Rega, Nadia; Li, Xiaosong

    2016-09-22

    The formation of polaron pairs is one of the important photophysical processes that take place after the excitation in semiconducting organic polymers. First-principles Ehrenfest excited-state dynamics is a unique tool to investigate ultrafast photoinduced charge carrier dynamics and related nonequilibrium processes involving correlated electron-nuclear dynamics. In this work the formation of polaron pairs and their dynamical evolution in an oligomer of seven thiophene units is investigated with a combined approach of first-principles exciton-nuclear dynamics and wavelet analysis. The real-time formation of a polaron pair can be observed in the dipole evolution during the excited-state dynamics. The possible driving force of the polaron pair formation is investigated through qualitative correlation between the structural dynamics and the dipole evolution. The time-dependent characteristics and spectroscopic consequences of the polaron pair formation are probed using the wavelet analysis. PMID:27571540

  7. Communication: Adiabatic and non-adiabatic electron-nuclear motion: Quantum and classical dynamics

    NASA Astrophysics Data System (ADS)

    Albert, Julian; Kaiser, Dustin; Engel, Volker

    2016-05-01

    Using a model for coupled electronic-nuclear motion we investigate the range from negligible to strong non-adiabatic coupling. In the adiabatic case, the quantum dynamics proceeds in a single electronic state, whereas for strong coupling a complete transition between two adiabatic electronic states takes place. It is shown that in all coupling regimes the short-time wave-packet dynamics can be described using ensembles of classical trajectories in the phase space spanned by electronic and nuclear degrees of freedom. We thus provide an example which documents that the quantum concept of non-adiabatic transitions is not necessarily needed if electronic and nuclear motion is treated on the same footing.

  8. Communication: Adiabatic and non-adiabatic electron-nuclear motion: Quantum and classical dynamics.

    PubMed

    Albert, Julian; Kaiser, Dustin; Engel, Volker

    2016-05-01

    Using a model for coupled electronic-nuclear motion we investigate the range from negligible to strong non-adiabatic coupling. In the adiabatic case, the quantum dynamics proceeds in a single electronic state, whereas for strong coupling a complete transition between two adiabatic electronic states takes place. It is shown that in all coupling regimes the short-time wave-packet dynamics can be described using ensembles of classical trajectories in the phase space spanned by electronic and nuclear degrees of freedom. We thus provide an example which documents that the quantum concept of non-adiabatic transitions is not necessarily needed if electronic and nuclear motion is treated on the same footing.

  9. Time-dependent density-functional theory method in the electron nuclear dynamics framework

    NASA Astrophysics Data System (ADS)

    Ajith Perera, S.; McLaurin, Patrick M.; Grimes, Thomas V.; Morales, Jorge A.

    2010-08-01

    A time-dependent density-functional theory (DFT) dynamics method in the electron nuclear dynamics (END) framework is presented. This time-dependent variational method treats simultaneously the nuclei and electrons of a system without utilizing predetermined potential energy surfaces. Like the simplest-level END, this method adopts a classical-mechanics description for the nuclei and a Thouless single-determinantal representation for the electrons. However, the electronic description is now expressed in a Kohn-Sham DFT form that provides electron correlation effects absent in the simplest-level END. Current implementation of this method employs the adiabatic approximation in the exchange-correlation action and potential. Simulations of molecular vibrations and proton-molecule reactions attest to the accuracy of the present method.

  10. Electron nuclear dynamics for a zig-zag chain of nitrogen atoms

    NASA Astrophysics Data System (ADS)

    Pohl, Anna; Calais, Jean-Louis

    1995-02-01

    We study the nitrogen zig-zag chain with two atoms per unit cell within the electron nuclear dynamics (END) formalism. This amounts to an approximate solution of the time-dependent Schrödinger equation for all the particles in the system. In the present approximation the nuclei are treated classically. The time dependence of the electronic motion is brought in through time-dependent linear combinations of fixed Bloch sums. This implies that the immediate mutual interaction between electronic and nuclear motion is taken into account. We investigate in particular the long-range terms of the interaction so as to arrive at convergent lattice sums. Before going to the general case when electronic and nuclear motion is coupled, we investigate the special cases of END traditional lattice dynamics and the random phase approximation (RPA) for the electrons.

  11. Theory of spatiotemporally resolved spectroscopy for phase-separation dynamics in electron-hole systems

    NASA Astrophysics Data System (ADS)

    Ishikawa, Akira

    2013-02-01

    Phase separation such as the formation of electron-hole droplets has been observed in semiconductor electron-hole systems. In such conventional experiments, the information averaged in real space was obtained. However, in recent years, optical-near-field techniques have enabled us to acquire spatial information. In this study, I propose a theoretical formulation of spatiotemporal dynamics and spatiotemporally resolved optical response of the gas-liquid phase separation in electron-hole systems. In addition, the nature of the nonequilibrium open system is an essential point in electron-hole systems. Therefore, I investigate the effect of the finite lifetime of electron-hole pairs on phase-separation dynamics. Contribution to the Topical Issue "Excitonic Processes in Condensed Matter, Nanostructured and Molecular Materials", edited by Maria Antonietta Loi, Jasper Knoester and Paul H. M. van Loosdrecht.

  12. Single molecule electronics: increasing dynamic range and switching speed using cross-conjugated species.

    PubMed

    Andrews, David Q; Solomon, Gemma C; Van Duyne, Richard P; Ratner, Mark A

    2008-12-24

    Molecular electronics is partly driven by the goal of producing active electronic elements that rival the performance of their solid-state counterparts, but on a much smaller size scale. We investigate what constitutes an ideal switch or molecular device, and how it can be designed, by analyzing transmission plots. The interference features in cross-conjugated molecules provide a large dynamic range in electron transmission probability, opening a new area for addressing electronic functionality in molecules. This large dynamic range is accessible through changes in electron density alone, enabling fast and stable switching. Using cross-conjugated molecules, we show how the width, depth, and energetic location of the interference features can be controlled. In an example of a single molecule transistor, we calculate a change in conductance of 8 orders of magnitude with an applied gate voltage. Using multiple interference features, we propose and calculate the current/voltage behavior of a molecular rectifier with a rectification ratio of >150,000. We calculate a purely electronic negative differential resistance behavior, suggesting that the large dynamic range in electron transmission probability caused by quantum interference could be exploited in future electronic devices.

  13. Wavefunction dynamics in a quantum-dot electron pump under a high magnetic field

    NASA Astrophysics Data System (ADS)

    Ryu, Sungguen; Kataoka, Masaya; Sim, Heung-Sun

    2015-03-01

    A quantum-dot electron pump, formed and operated by applying time-dependent potential barriers to a two dimensional electron gas system, provides a promising redefinition of ampere. The pump operation consists of capturing an electron from a reservoir into a quantum dot and ejecting it to another reservoir. The capturing process has been theoretically understood by a semi-classical treatment of the tunneling between the dot and reservoir. But the dynamics of the wavefunction of the captured electron in the ejection process has not been theoretically addressed, although it is useful for enhancing pump accuracy and for utilizing the pump as a single-electron source for mesoscopic quantum electron devices. We study the dynamics under a strong magnetic field that leads to magnetic confinement of the captured electron, which dominates over the electrostatic confinement of the dot. We find that the wave packet of the captured electron has the Gaussian form with the width determined by the strength of the magnetic field, and that the time evolution of the packet follows the classical drift motion, with maintaining the Gaussian form. We discuss the possible signatures of the wave packet dynamics in experiments.

  14. Comment on 'electron holography on dynamic motion of secondary electrons around sciatic nerve tissues'.

    PubMed

    Beleggia, Marco; Pozzi, Giulio

    2008-10-01

    We present an alternative interpretation of the holographic phase dislocation loops revealed by Shindo et al. [J. Electron Microsc. 56(1): 1-5 (2007)] around a charged sample. Our interpretation does not involve the motion of secondary electrons around a charged object. It relates, instead, to fluctuating charges on the sample and to the resulting Moiré-type patterns in the hologram.

  15. Large dynamic range diagnostics for high current electron LINACs

    SciTech Connect

    Evtushenko, P.

    2013-11-07

    The Jefferson Lab FEL driver accelerator - Energy Recovery Linac has provided a beam with average current of up to 9 mA and beam energy of 135 MeV. The high power beam operations have allowed developing and testing methods and approaches required to set up and tune such a facility simultaneously for the high beam power and high beam quality required for high performance FEL operations. In this contribution we briefly review this experience and outline problems that are specific to high current - high power non-equilibrium linac beams. While the original strategy for beam diagnostics and tuning have proven to be quite successful, some shortcomings and unresolved issues were also observed. The most important issues are the non-equilibrium (non-Gaussian) nature of the linac beam and the presence of small intensity - large amplitude fraction of the beam a.k.a. beam halo. Thus we also present a list of the possible beam halo sources and discuss possible mitigations means. We argue that for proper understanding and management of the beam halo large dynamic range (>10{sup 6}) transverse and longitudinal beam diagnostics can be used. We also present results of transverse beam profile measurements with the dynamic range approaching 10{sup 5} and demonstrate the effect the increased dynamic range has on the beam characterization, i.e., emittance and Twiss parameters measurements. We also discuss near future work planned in this field and where the JLab FEL facility will be used for beam tests of the developed of new diagnostics.

  16. Large dynamic range diagnostics for high current electron LINACs

    SciTech Connect

    Evtushenko, Pavel

    2013-11-01

    The Jefferson Lab FEL driver accelerator - Energy Recovery Linac has provided a beam with average current of up to 9 mA and beam energy of 135 MeV. The high power beam operations have allowed developing and testing methods and approaches required to set up and tune such a facility simultaneously for the high beam power and high beam quality required for high performance FEL operations. In this contribution we briefly review this experience and outline problems that are specific to high current - high power non-equilibrium linac beams. While the original strategy for beam diagnostics and tuning have proven to be quite successful, some shortcomings and unresolved issues were also observed. The most important issues are the non-equilibrium (non-Gaussian) nature of the linac beam and the presence of small intensity - large amplitude fraction of the beam a.k.a. beam halo. Thus we also present a list of the possible beam halo sources and discuss possible mitigations means. We argue that for proper understanding and management of the beam halo large dynamic range (>10{sup 6}) transverse and longitudinal beam diagnostics can be used. We also present results of transverse beam profile measurements with the dynamic range approaching 10{sup 5} and demonstrate the effect the increased dynamic range has on the beam characterization, i.e., emittance and Twiss parameters measurements. We also discuss near future work planned in this field and where the JLab FEL facility will be used for beam tests of the developed of new diagnostics.

  17. Dynamic Pricing in Electronic Commerce Using Neural Network

    NASA Astrophysics Data System (ADS)

    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.

  18. Dynamic Void Growth and Shrinkage in Mg under Electron Irradiation

    SciTech Connect

    Xu, W. Z.; Zhang, Y. F.; Cheng, G. M.; Jian, W. W.; Millett, P. C.; Koch, C. C.; Mathaudhu, S. N.; Zhu, Y. T.

    2014-04-30

    We report in-situ atomic-scale investigation of void evolution, including growth, coalescence and shrinkage, under electron irradiation. With increasing irradiation dose, the total volume of voids increased linearly, while nucleation rate of new voids decreased slightly, and the total number of voids decreased. Some voids continued to grow while others shrank to disappear, depending on the nature of their interactions with nearby self-interstitial loops. For the first time, surface diffusion of adatoms was observed largely responsible for the void coalescence and thickening. These findings provide fundamental understanding to help with the design and modeling of irradiation-resistant materials.

  19. Ultrashort electron pulses as a four-dimensional diagnosis of plasma dynamics.

    PubMed

    Zhu, P F; Zhang, Z C; Chen, L; Li, R Z; Li, J J; Wang, X; Cao, J M; Sheng, Z M; Zhang, J

    2010-10-01

    We report an ultrafast electron imaging system for real-time examination of ultrafast plasma dynamics in four dimensions. It consists of a femtosecond pulsed electron gun and a two-dimensional single electron detector. The device has an unprecedented capability of acquiring a high-quality shadowgraph image with a single ultrashort electron pulse, thus permitting the measurement of irreversible processes using a single-shot scheme. In a prototype experiment of laser-induced plasma of a metal target under moderate pump intensity, we demonstrated its unique capability of acquiring high-quality shadowgraph images on a micron scale with a-few-picosecond time resolution.

  20. Non-equilibrium electron transport in degenerate nitride heterostructures-dynamic screening effects

    NASA Astrophysics Data System (ADS)

    Anderson, D. R.; Babiker, M.; Bennett, C. R.; Probert, M. I. J.

    2003-04-01

    We show how dynamic screening effects on non-equilibrium electron transport can be incorporated in the case of electronically dense GaN-based quantum wells. The theory is based on the Boltzmann equation, leading to evaluations of the momentum relaxation time and, hence, the electron mobility in these heterostructures. We find that both screening and anti-screening effects are manifest as the electron density varies. However, anti-screening dominates over a wide range of densities, with screening commencing at densities appropriate for phonon-plasmon coupling.

  1. Electronic dynamics under effect of a nonlinear Morse interaction and a static electric field

    NASA Astrophysics Data System (ADS)

    Ranciaro Neto, A.; de Moura, F. A. B. F.

    2016-11-01

    Considering non-interacting electrons in a one-dimension alloy in which atoms are coupled by a Morse potential, we study the system dynamics in the presence of a static electric field. Calculations are performed assuming a quantum mechanical treatment for the electronic transport and a classical Hamiltonian model for the lattice vibrations. We report numerical evidence of the existence of a soliton-electron pair, even when the electric field is turned on, and we offer a description of how the existence of such a phase depends on the magnitude of the electric field and the electron-phonon interaction.

  2. Dawn-dusk asymmetry and adiabatic dynamic of the radiation belt electrons during magnetic storm

    NASA Astrophysics Data System (ADS)

    Lazutin, Leonid L.

    2016-09-01

    The changes of the latitudinal profiles of outer belt energetic electrons during magnetic storms are mostly explained by the precipitation into the loss cone caused by VLF and EMIC waves or by the scattering into the magnetopause. In present work, energetic electron dynamics during magnetic storm of August 29-30, 2004 we attributed at most to the adiabatic transformation of the magnetic drift trajectories and Dst effect. This conclusion was based on the analysis of dawn-dusk asymmetry of the electron latitudinal profiles measured by low altitude polar orbiter SERVIS-1 and on the coincidence of pre-storm and after-storm profiles of radiation belt electrons and protons.

  3. Inhomogeneous dynamic nuclear polarization and suppression of electron polarization decay in a quantum dot

    NASA Astrophysics Data System (ADS)

    Wu, Na; Ding, Wenkui; Shi, Anqi; Zhang, Wenxian

    2016-08-01

    We investigate the dynamic nuclear polarization in a quantum dot. Due to the suppression of direct dipolar and indirect electron-mediated nuclear spin interactions by frequently injected electron spins, our analytical results under independent spin approximation agree well with quantum numerical simulations for a small number of nuclear spins. We find that the acquired nuclear polarization is highly inhomogeneous, proportional to the square of the local electron-nuclear hyperfine interaction constant. Starting from the inhomogeneously polarized nuclear spins, we further show that the electron polarization decay time can be extended 100 times even at a relatively low nuclear polarization.

  4. Hot and cold electron dynamics following high-intensity laser matter interaction.

    PubMed

    Antici, P; Fuchs, J; Borghesi, M; Gremillet, L; Grismayer, T; Sentoku, Y; d'Humières, E; Cecchetti, C A; Mancić, A; Pipahl, A C; Toncian, T; Willi, O; Mora, P; Audebert, P

    2008-09-01

    The characteristics of fast electrons laser accelerated from solids and expanding into a vacuum from the rear target surface have been measured via optical probe reflectometry. This allows access to the time- and space-resolved dynamics of the fast electron density and temperature and of the energy partition into bulk (cold) electrons. In particular, it is found that the density of the hot electrons on the target rear surface is bell shaped, and that their mean energy at the same location is radially homogeneous and decreases with the target thickness. PMID:18851222

  5. Nonequilibrium Dynamics in a Quasi-Two-Dimensional Electron Plasma after Ultrafast Intersubband Excitation

    SciTech Connect

    Lutgen, S.; Kaindl, R.A.; Woerner, M.; Elsaesser, T.; Hase, A.; Kuenzel, H.; Gulia, M.; Meglio, D.; Lugli, P.

    1996-10-01

    The dynamics of electrons in GaInAs/AlInAs quantum wells is studied after excitation from the {ital n}=1 to the {ital n}=2 conduction subband. Femtosecond pump-probe experiments demonstrate for the first time athermal distributions of {ital n}=1 electrons on a surprisingly long time scale of 2ps. Thermalization involves intersubband scattering of excited electrons via optical phonon emission with a time constant of 1ps and intrasubband Coulomb and phonon scattering. Ensemble Monte Carlo simulations show that the slow electron equilibration results from Pauli blocking and screening of carrier-carrier scattering. {copyright} {ital 1996 The American Physical Society.}

  6. Dynamical exchange-correlation potentials for the electron liquid

    NASA Astrophysics Data System (ADS)

    Qian, Zhixin; Vignale, Giovanni

    2002-03-01

    The imaginary parts of the exchange-correlation kernels f_xc^L,T(q=0, ω) in the linear density-density and transverse current-current response functions of a homogeneous electron liquid are calculated exactly at low frequency, to leading order in the Coulomb interaction. Combining these new results with the previously known high-frequency behaviors of Im f_xc^L,T(q=0, ω) and with the compressibility and the third frequency moment sum rules, we construct simple interpolation for Im f_xc^L,T(q=0, ω) in 3- and 2- dimensions. A novel feature of our interpolation formulas is that they explicitly take into account the two-plasmon component of the excitation spectrum: our longitudinal spectrum Im f_xc^L(q=0, ω) is thus intermediate between the Gross-Kohn interpolation, which ignores the two-plasmon contribution, and a recent approximate calculation by Nifosi, Conti, and Tosi, which probably overestimates it. Numerical results for both the real and imaginary parts of the exchange-correlation kernels at typical electron densities are presented, and compared with those obtained from previous approximations.

  7. A framework for stochastic simulations and visualization of biological electron-transfer dynamics

    NASA Astrophysics Data System (ADS)

    Nakano, C. Masato; Byun, Hye Suk; Ma, Heng; Wei, Tao; El-Naggar, Mohamed Y.

    2015-08-01

    Electron transfer (ET) dictates a wide variety of energy-conversion processes in biological systems. Visualizing ET dynamics could provide key insight into understanding and possibly controlling these processes. We present a computational framework named VizBET to visualize biological ET dynamics, using an outer-membrane Mtr-Omc cytochrome complex in Shewanella oneidensis MR-1 as an example. Starting from X-ray crystal structures of the constituent cytochromes, molecular dynamics simulations are combined with homology modeling, protein docking, and binding free energy computations to sample the configuration of the complex as well as the change of the free energy associated with ET. This information, along with quantum-mechanical calculations of the electronic coupling, provides inputs to kinetic Monte Carlo (KMC) simulations of ET dynamics in a network of heme groups within the complex. Visualization of the KMC simulation results has been implemented as a plugin to the Visual Molecular Dynamics (VMD) software. VizBET has been used to reveal the nature of ET dynamics associated with novel nonequilibrium phase transitions in a candidate configuration of the Mtr-Omc complex due to electron-electron interactions.

  8. Methodology for determining the electronic thermal conductivity of metals via direct nonequilibrium ab initio molecular dynamics

    NASA Astrophysics Data System (ADS)

    Yue, Sheng-Ying; Zhang, Xiaoliang; Stackhouse, Stephen; Qin, Guangzhao; Di Napoli, Edoardo; Hu, Ming

    2016-08-01

    Many physical properties of metals can be understood in terms of the free electron model, as proven by the Wiedemann-Franz law. According to this model, electronic thermal conductivity can be inferred from the Boltzmann transport equation (BTE). However, the BTE does not perform well for some complex metals, such as Cu. Moreover, the BTE cannot clearly describe the origin of the thermal energy carried by electrons or how this energy is transported in metals. The charge distribution of conduction electrons in metals is known to reflect the electrostatic potential of the ion cores. Based on this premise, we develop a methodology for evaluating electronic thermal conductivity of metals by combining the free electron model and nonequilibrium ab initio molecular dynamics simulations. We confirm that the kinetic energy of thermally excited electrons originates from the energy of the spatial electrostatic potential oscillation, which is induced by the thermal motion of ion cores. This method directly predicts the electronic thermal conductivity of pure metals with a high degree of accuracy, without explicitly addressing any complicated scattering processes of free electrons. Our methodology offers a route to understand the physics of heat transfer by electrons at the atomistic level. The methodology can be further extended to the study of similar electron-involved problems in materials, such as electron-phonon coupling, which is underway currently.

  9. Visible-Light Photoexcited Electron Dynamics of Scandium Endohedral Metallofullerenes: The Cage Symmetry and Substituent Effects.

    PubMed

    Wu, Bo; Hu, Jiahua; Cui, Peng; Jiang, Li; Chen, Zongwei; Zhang, Qun; Wang, Chunru; Luo, Yi

    2015-07-15

    Endohedral metallofullerenes (EMFs) have become an important class of molecular materials for optoelectronic applications. The performance of EMFs is known to be dependent on their symmetries and characters of the substituents, but the underlying electron dynamics remain unclear. Here we report a systematic study on several scandium EMFs and representative derivatives to examine the cage symmetry and substituent effects on their photoexcited electron dynamics using ultrafast transient absorption spectroscopy. Our attention is focused on the visible-light (530 nm as a demonstration) photoexcited electron dynamics, which is of broad interest to visible-light solar energy harvesting but is considered to be quite complicated as the visible-light photons would promote the system to a high-lying energy region where dense manifolds of electronic states locate. Our ultrafast spectroscopy study enables a full mapping of the photoinduced deactivation channels involved and reveals that the long-lived triplet exciton plays a decisive role in controlling the photoexcited electron dynamics under certain conditions. More importantly, it is found that the opening of the triplet channels is highly correlated to the fullerene cage symmetry as well as the electronic character of the substituents.

  10. Visible-Light Photoexcited Electron Dynamics of Scandium Endohedral Metallofullerenes: The Cage Symmetry and Substituent Effects.

    PubMed

    Wu, Bo; Hu, Jiahua; Cui, Peng; Jiang, Li; Chen, Zongwei; Zhang, Qun; Wang, Chunru; Luo, Yi

    2015-07-15

    Endohedral metallofullerenes (EMFs) have become an important class of molecular materials for optoelectronic applications. The performance of EMFs is known to be dependent on their symmetries and characters of the substituents, but the underlying electron dynamics remain unclear. Here we report a systematic study on several scandium EMFs and representative derivatives to examine the cage symmetry and substituent effects on their photoexcited electron dynamics using ultrafast transient absorption spectroscopy. Our attention is focused on the visible-light (530 nm as a demonstration) photoexcited electron dynamics, which is of broad interest to visible-light solar energy harvesting but is considered to be quite complicated as the visible-light photons would promote the system to a high-lying energy region where dense manifolds of electronic states locate. Our ultrafast spectroscopy study enables a full mapping of the photoinduced deactivation channels involved and reveals that the long-lived triplet exciton plays a decisive role in controlling the photoexcited electron dynamics under certain conditions. More importantly, it is found that the opening of the triplet channels is highly correlated to the fullerene cage symmetry as well as the electronic character of the substituents. PMID:26097975

  11. Disentangling electron tunneling and protein dynamics of cytochrome c through a rationally designed surface mutation.

    PubMed

    Alvarez-Paggi, Damián; Meister, Wiebke; Kuhlmann, Uwe; Weidinger, Inez; Tenger, Katalin; Zimányi, László; Rákhely, Gábor; Hildebrandt, Peter; Murgida, Daniel H

    2013-05-23

    Nonexponential distance dependence of the apparent electron-transfer (ET) rate has been reported for a variety of redox proteins immobilized on biocompatible electrodes, thus posing a physicochemical challenge of possible physiological relevance. We have recently proposed that this behavior may arise not only from the structural and dynamical complexity of the redox proteins but also from their interplay with strong electric fields present in the experimental setups and in vivo (J. Am Chem. Soc. 2010, 132, 5769-5778). Therefore, protein dynamics are finely controlled by the energetics of both specific contacts and the interaction between the protein's dipole moment and the interfacial electric fields. In turn, protein dynamics may govern electron-transfer kinetics through reorientation from low to high donor-acceptor electronic coupling orientations. Here we present a combined computational and experimental study of WT cytochrome c and the surface mutant K87C adsorbed on electrodes coated with self-assembled monolayers (SAMs) of varying thickness (i.e., variable strength of the interfacial electric field). Replacement of the positively charged K87 by a neutral amino acid allowed us to disentangle protein dynamics and electron tunneling from the reaction kinetics and to rationalize the anomalous distance dependence in terms of (at least) two populations of distinct average electronic couplings. Thus, it was possible to recover the exponential distance dependence expected from ET theory. These results pave the way for gaining further insight into the parameters that control protein electron transfer.

  12. Dynamical and anharmonic effects on the electron-phonon coupling and the zero-point renormalization of the electronic structure

    NASA Astrophysics Data System (ADS)

    Antonius, G.; Poncé, S.; Lantagne-Hurtubise, E.; Auclair, G.; Gonze, X.; Côté, M.

    2015-08-01

    The renormalization of the band structure at zero temperature due to electron-phonon coupling is explored in diamond, BN, LiF, and MgO crystals. We implement a dynamical scheme to compute the frequency-dependent self-energy and the resulting quasiparticle electronic structure. Our calculations reveal the presence of a satellite band below the Fermi level of LiF and MgO. We show that the renormalization factor (Z ), which is neglected in the adiabatic approximation, can reduce the zero-point renormalization (ZPR) by as much as 40 % . Anharmonic effects in the renormalized eigenvalues at finite atomic displacements are explored with the frozen-phonon method. We use a nonperturbative expression for the ZPR, going beyond the Allen-Heine-Cardona theory. Our results indicate that high-order electron-phonon coupling terms contribute significantly to the zero-point renormalization for certain materials.

  13. Understanding Dynamic Competitive Technology Diffusion in Electronic Markets

    NASA Astrophysics Data System (ADS)

    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.

  14. Versatile approach to spin dynamics in correlated electron systems

    NASA Astrophysics Data System (ADS)

    Behrmann, Malte; Lichtenstein, Alexander I.; Katsnelson, Mikhail I.; Lechermann, Frank

    2016-10-01

    Time-dependent spin phenomena in condensed matter are most often either described in the weakly correlated limit of metallic Stoner-Slater-like magnetism via band theory or in the strongly correlated limit of Heisenberg-like interacting spins in an insulator. However, many experimental studies, e.g., of (de)magnetization processes, focus on itinerant local-moment materials, such as transition metals and various of their compounds. We here present a general theoretical framework that is capable of addressing correlated spin dynamics, also in the presence of a vanishing charge gap. A real-space implementation of the time-dependent rotational-invariant slave boson methodology allows us to treat nonequilibrium spins numerically fast and efficiently beyond linear response as well as beyond the band-theoretical or Heisenberg limit.

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

    PubMed

    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.

  16. Ultrafast magnetization dynamics: Microscopic electronic configurations and ultrafast spectroscopy

    NASA Astrophysics Data System (ADS)

    Locht, I. L. M.; Di Marco, I.; Garnerone, S.; Delin, A.; Battiato, M.

    2015-08-01

    We provide an approach for the identification of the electronic and magnetic configurations of ferromagnetic Fe after an ultrafast decrease or increase of the magnetization. The model is based on the well-grounded assumption that, after an ultrafast variation of the magnetization, the system achieves a partial thermal equilibrium. With statistical arguments we show that the magnetic configurations are qualitatively different in the case of reduced or increased magnetization. The predicted magnetic configurations are then used to compute the dielectric response at the 3 p (M ) absorption edge, which is directly related to the changes observed in the experimental T-MOKE data. The good qualitative agreement between theory and experiment offers a substantial support for the validity of the model, and to the very existence of an ultrafast increase of the magnetization.

  17. Electron-Nuclear Dynamics of atomic and molecular collisions: Charge exchange and energy loss

    NASA Astrophysics Data System (ADS)

    Cabrera-Trujillo, Remigio; Sabin, John R.; Ohrn, Yngve; Deumens, Erik

    2004-05-01

    Processes like electron exchange (capture and loss), bond breaking, and chemical reactions are difficult to visualize and treat in a time-independent approach. In this work, we present the Electron-Nuclear Dynamics (END) method for the study of time-dependent scattering processes. The END is a general approach for treating time-dependent problems which includes the dynamics of electrons and nuclei simultaneously by considering the full electron-nuclear coupling in the system and thus eliminates the necessity of constructing potential-energy surfaces. The theory approximates the time dependent Schrödinger equation starting from the time dependent variational principle (TDVP) by deriving a Hamiltonian dynamical system for time dependent nuclear and electronic wave function parameters. The wave function is described in a coherent state manifold, which leads to a system of Hamilton's equations of motion. The resulting system of coupled, first order, ordinary differential equations approximates the Schrödinger equation. A detailed analysis of the END equations is given for the case of a single-determinantal state for the electrons and a classical treatment of the nuclei. Emphasis is put on electron exchange, differential cross section and energy loss (stopping cross section) of collision of ions, atoms and molecules involving H, He, C, N, O, and Ne atoms. We compare our results to available experimental data.

  18. Variations of energetic electrons associated with solar wind dynamic pressure enhancement in the outer radiation belt

    NASA Astrophysics Data System (ADS)

    Lee, J.; Lee, E.; Kim, K. H.; Lee, D. H.; Lee, J.; Spence, H. E.

    2015-12-01

    Earth's outer radiation belt varies dynamically under the variations of the solar wind. In this study, we investigated the variations of energetic electrons in the outer radiation belt caused by an enhancement of the solar wind dynamic pressure associated with an interplanetary shock using the measurements from the Van Allen Probes (VAP) satellites. The enhanced dynamic pressure lasted for about 24 hours, but magnetic storm was not occurred. The impact of the interplanetary shock on 13 April 2013 produced dipolarization of the magnetic field for a few minutes, which was simultaneously observed by VAP A and B moving in the nightside region. The enhancement of the electron fluxes with E < ~600 keV coincidentally occurred during the dipolarization. Later, drift echoes with energy dispersion and ULF-like modulations were observed. By comparing the measurements from VAP A and B we will discuss spatial and temporal characteristics of the enhancement of the energetic electron fluxes.

  19. Dynamics of chemical bonding mapped by energy-resolved 4D electron microscopy.

    PubMed

    Carbone, Fabrizio; Kwon, Oh-Hoon; Zewail, Ahmed H

    2009-07-10

    Chemical bonding dynamics are fundamental to the understanding of properties and behavior of materials and molecules. Here, we demonstrate the potential of time-resolved, femtosecond electron energy loss spectroscopy (EELS) for mapping electronic structural changes in the course of nuclear motions. For graphite, it is found that changes of milli-electron volts in the energy range of up to 50 electron volts reveal the compression and expansion of layers on the subpicometer scale (for surface and bulk atoms). These nonequilibrium structural features are correlated with the direction of change from sp2 [two-dimensional (2D) graphene] to sp3 (3D-diamond) electronic hybridization, and the results are compared with theoretical charge-density calculations. The reported femtosecond time resolution of four-dimensional (4D) electron microscopy represents an advance of 10 orders of magnitude over that of conventional EELS methods. PMID:19589997

  20. Optically controlled electron-nuclear spin dynamics in a quantum dot

    NASA Astrophysics Data System (ADS)

    Barnes, Edwin; Economou, Sophia

    2011-03-01

    In recent years, a large number of experiments involving coherent and incoherent control of electron spins in quantum dots have revealed the important role of the nuclear spins of the host material. Experiments with optical controls, both pulsed and continuous wave, have shown that the feedback of the nuclear spins on the electron spin strongly affects the electron spin response. However, a microscopic theory of this mechanism is not available at present. We introduce a formalism that allows us to investigate this system without invoking any phenomenological spin-flip rates for the nuclei. We derive the electron-nuclear dynamics under the influence of external periodic pulsed control to second order in the electron-nuclear hyperfine coupling. Our formalism should have wide applications in both coherently and incoherently driven electron spins interacting with a nuclear spin bath, including self-assembled and gated quantum dots. Work (EB) supported by LPS-CMTC and CNAM.

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

    NASA Astrophysics Data System (ADS)

    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.

  2. Ultrafast spectroscopy of prototypes of electronically nonadiabatic dynamics in solution chemistry

    NASA Astrophysics Data System (ADS)

    Silva, Carlos

    Femtosecond pump-probe spectroscopy of the equilibrated hydrated electron has been recorded with 35-femtosecond time resolution, revealing unprecedented transient features on the 30-80 fs time scales, which exhibit a solvent deuterium isotope effect (τ(D2O)/τ(H2O)~1.4). These previously unresolved dynamics have been assigned to inertial solvation dynamics of the photoexcited excess electron. The results support the importance of librational water motion in the relaxation dynamics of the hydrated electron. High excitation-pulse-intensity measurements reveal evidence of a two-photon channel involving ejection of the hydrated electron from its initial site to a different site in the solvent. Further pump-probe spectroscopy of the equilibrated solvated electron in alcohols has been studied with ~300 fs time resolution. At low pump power the observed dynamics are assigned to s→p excitation and subsequent relaxation of a localized solvated electron. In contrast, at high pump power, two-photon absorption apparently produces mobile 'conduction band' electrons, which are subsequently trapped and relax at a remote site from the initial equilibrated electron as observed for the hydrated electron. The two-photon excitation channel is also observed to induce an ultrafast proton-transfer reaction from the solvent to the excess electron. The metal-metal, charge-transfer (MMCT) absorption bands of the mixed-valence compounds (NH3)5RuIIINCRuII(CN)5/sp- (RuRu) and (NH3)5RuIIINCFeII(CN)5/sp- (RuFe) are studied with sufficient time resolution to measure the back-electron transfer (b-ET) time. In RuRu, the b-ET occurs in 85 ± 10 fs in H2O and increases to 122 ± 20 fs in D2O. Similar b-ET rates in these solvents are also observed for RuFe. The deuterium isotope effect is shown to originate from the solvent demonstrating that hydrogenic solvent motions are directly coupled to the electron transfer event. The pump-probe spectroscopy on the MMCT band also provides information on the

  3. Probing Molecular Organization and Electronic Dynamics at Buried Organic Interfaces

    NASA Astrophysics Data System (ADS)

    Roberts, Sean

    2015-03-01

    Organic semiconductors are a promising class of materials due to their ability to meld the charge transport capabilities of semiconductors with many of the processing advantages of plastics. In thin film organic devices, interfacial charge transfer often comprises a crucial step in device operation. As molecular materials, the density of states within organic semiconductors often reflect their intermolecular organization. Truncation of the bulk structure of an organic semiconductor at an interface with another material can lead to substantial changes in the density of states near the interface that can significantly impact rates for interfacial charge and energy transfer. Here, we will present the results of experiments that utilize electronic sum frequency generation (ESFG) to probe buried interfaces in these materials. Within the electric dipole approximation, ESFG is only sensitive to regions of a sample that experience a breakage of symmetry, which occurs naturally at material interfaces. Through modeling of signals measured for thin organic films using a transfer matrix-based formalism, signals from buried interfaces between two materials can be isolated and used to uncover the interfacial density of states.

  4. Nonadiabtic electron dynamics in densely quasidegenerate states in highly excited boron cluster.

    PubMed

    Yonehara, Takehiro; Takatsuka, Kazuo

    2016-04-28

    Following the previous study on nonadiabatic reaction dynamics including boron clusters [T. Yonehara and K. Takatsuka, J. Chem. Phys. 137, 22A520 (2012)], we explore deep into highly excited electronic states of the singlet boron cluster (B12) to find the characteristic features of the densely quasi-degenerate electronic state manifold, which undergo very frequent nonadiabatic transitions and thereby intensive electronic state mixing among very many of the relevant states. So much so, isolating the individual adiabatic states and tracking the expected potential energy surfaces both lose the physical sense. This domain of molecular situation is far beyond the realm of the Born-Oppenheimer approximation. To survey such a violent electronic state-mixing, we apply a method of nonadiabatic electron wavepacket dynamics, the semiclassical Ehrenfest method. We have tracked those electron wavepackets and found the electronic state mixing looks like an ultrafast diffusion in the Hilbert space, which results in huge fluctuation. Furthermore, due to such a violent mixing, the quantum phases associated with the electronic states are swiftly randomized, and consequently the coherence among the electronic states are lost quickly. Besides, these highly excited states are mostly of highly poly-radical nature, even in the spin singlet manifold and the number of radicals amounts up to 10 electrons in the sense of unpaired electrons. Thus the electronic states are summarized to be poly-radical and decoherent with huge fluctuation in shorter time scales of vibrational motions. The present numerical study sets a theoretical foundation for unknown molecular properties and chemical reactivity of such densely quasi-degenerate chemical species. PMID:27131547

  5. Nonadiabtic electron dynamics in densely quasidegenerate states in highly excited boron cluster

    NASA Astrophysics Data System (ADS)

    Yonehara, Takehiro; Takatsuka, Kazuo

    2016-04-01

    Following the previous study on nonadiabatic reaction dynamics including boron clusters [T. Yonehara and K. Takatsuka, J. Chem. Phys. 137, 22A520 (2012)], we explore deep into highly excited electronic states of the singlet boron cluster (B12) to find the characteristic features of the densely quasi-degenerate electronic state manifold, which undergo very frequent nonadiabatic transitions and thereby intensive electronic state mixing among very many of the relevant states. So much so, isolating the individual adiabatic states and tracking the expected potential energy surfaces both lose the physical sense. This domain of molecular situation is far beyond the realm of the Born-Oppenheimer approximation. To survey such a violent electronic state-mixing, we apply a method of nonadiabatic electron wavepacket dynamics, the semiclassical Ehrenfest method. We have tracked those electron wavepackets and found the electronic state mixing looks like an ultrafast diffusion in the Hilbert space, which results in huge fluctuation. Furthermore, due to such a violent mixing, the quantum phases associated with the electronic states are swiftly randomized, and consequently the coherence among the electronic states are lost quickly. Besides, these highly excited states are mostly of highly poly-radical nature, even in the spin singlet manifold and the number of radicals amounts up to 10 electrons in the sense of unpaired electrons. Thus the electronic states are summarized to be poly-radical and decoherent with huge fluctuation in shorter time scales of vibrational motions. The present numerical study sets a theoretical foundation for unknown molecular properties and chemical reactivity of such densely quasi-degenerate chemical species.

  6. Lattice dynamics and electronic structure of mixed halofluoride scintillators under high pressure

    SciTech Connect

    Kanchana, V.; Yedukondalu, N.; Vaitheeswaran, G.

    2015-06-24

    We report the structural, lattice dynamics and electronic structure of mixed halo-fluoride scintillators MClF (M = Ca, Sr) based on density functional theory within generalized gradient approximation. The pressure dependent structural parameters and zone centered phonon frequencies are in reasonable agreement with the available experimental data. Both the structures are dynamically stable up to 50 GPa. MClF compounds are found to have a direct band gap along Γ−Γ direction at ambient as well as under pressure. It is found that these materials can serve as good storage phosphors in the low pressure region from the calculated electronic structure and optical spectra.

  7. Imaging Ultra-fast Molecular Dynamics in Free Electron Laser Field

    NASA Astrophysics Data System (ADS)

    Zhang, Y. Z.; Jiang, Y. H.

    The free electron laser (FEL) provides the coherent, brilliant and ultrashort light pulse in short wavelength (extreme ultraviolet and X-ray) regimes, opening up possibilities to study ultra-fast molecular dynamics in photo-induced chemical reactions with new methodologies. In this chapter, we introduce the time-resolved pump-probe experiments on gas-phase targets with FEL facilities to image the nuclear and electronic motions in molecular reactions, which serve as a benchmark for further FEL applications like coherent diffraction imaging and coherent control of functional dynamics in complex molecular reactions.

  8. Some coherent-states aspects of the electron nuclear dynamics theory: past and present

    NASA Astrophysics Data System (ADS)

    Morales, Jorge A.

    2010-11-01

    Past and present coherent-states (CS) efforts with the electron nuclear dynamics (END) theory at its simplest level (SL-END) are reviewed. END is a time-dependent, variational, non-adiabatic, direct-dynamics method that describes simultaneously the nuclei and electrons of a molecular system. Within that characterization, SL-END adopts a classical-mechanics description for the nuclei and a quantum single-determinantal representation for the electrons. From its very inception, SL-END has been associated with the CS theory. CS sets are continuous and over-complete sets that satisfy the resolution of identity with a positive measure. Different CS sets can play an astonishing number of roles within SL-END that have several practical consequences. Originally, SL-END utilized the canonical and Thouless CS sets to correctly represent the nuclear and electronic parts of the SL-END wavefunction, respectively, thus defining a proper phase space for the SL-END dynamical equations. Later, canonical and rotational CS sets were used for reconstructing quantum vibrational and quantum rotational descriptions from the SL-END classical nuclear dynamics. That development proved essential to calculate state-resolved properties in ion-molecule and atom-molecule collisions with SL-END. Present CS efforts include a time-dependent Kohn-Sham density-functional-theory direct-dynamic method in the END framework and a CS approach to the charge-equilibration model inter alia.

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

    NASA Astrophysics Data System (ADS)

    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.

  10. Strong deviations from jellium behavior in the valence electron dynamics of potassium

    NASA Astrophysics Data System (ADS)

    Huotari, Simo; Sternemann, Christian; Troparevsky, M. Claudia; Eguiluz, Adolfo G.; Volmer, Martin; Sternemann, Henning; Müller, Harald; Monaco, Giulio; Schülke, Winfried

    2009-10-01

    We present experimental and ab initio theoretical determination of the dynamics of valence electrons in potassium by investigating the dynamical structure factor at nonvanishing momentum transfers. The spectra show large deviations from a jellium-type behavior due to the presence of d -type states above the Fermi level. In particular, we identify two well-defined interband excitations that have a direct correspondence with the density of states above the Fermi level.

  11. Electron nuclear dynamics of proton collisions with methane at 30 eV

    NASA Astrophysics Data System (ADS)

    Jacquemin, D.; Morales, J. A.; Deumens, E.; Öhrn, Y.

    1997-10-01

    The reactive collisions of protons with methane molecules at 30 eV in the laboratory frame are studied with the electron nuclear dynamics (END). The results from this theoretical approach, which does not invoke the Born-Oppenheimer approximation and does not impose any constraints on the nuclear dynamics, are compared to the results from time-of-flight measurements. Total differential cross sections and integral cross sections as well as fragmentation ratios and energy loss spectra are discussed.

  12. Entangled valence electron-hole dynamics revealed by stimulated attosecond x-ray Raman scattering

    SciTech Connect

    Healion, Daniel; Zhang, Yu; Biggs, Jason D.; Govind, Niranjan; Mukamel, Shaul

    2012-09-06

    We show that broadband x-ray pulses can create wavepackets of valence electrons and holes localized in the vicinity of a selected atom (nitrogen, oxygen or sulfur in cysteine) by resonant stimulated Raman scattering. The subsequent dynamics reveals highly correlated motions of entangled electrons and hole quasiparticles. This information goes beyond the time-dependent total charge density derived from x-ray diffraction.

  13. 2012 ELECTRONIC SPECTROSCOPY & DYNAMICS GORDON RESEARCH CONFERENCE, JULY 22-27, 2012

    SciTech Connect

    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.

  14. Two-photon photoemission and the dynamics of electrons at interfaces

    SciTech Connect

    Padowitz, D.F.; Harris, C.B.; Jordan, R.E.; Lingle, R.L. Jr.; McNeill, J.D.; Merry, W.R.

    1994-01-01

    A new instrument for angle-resolved two-photon photoemission with exceptional sensitivity and energy resolution has allowed a detailed examination of the interaction of image-state electrons with adsorbates. In addition to measuring the electrostatic properties of molecular-thickness films, the technique serves as a probe of adsorbate growth modes, and provides new opportunities to explore the dynamics of electrons in well-controlled two-dimensional systems.

  15. Ultrafast Electronic And Nuclear Dynamics In Dissociative Photoionization Of Molecular Hydrogen and Deuterium

    NASA Astrophysics Data System (ADS)

    Billaud, P.; Picard, Y. J.; Géléoc, M.; Hergott, J.-F.; Carré, B.; Breger, P.; Ruchon, T.; Veyrinas, K.; Roulliay, M.; Delmotte, F.; Böttcher, M.; Huetz, A.; Dowek, D.

    2012-11-01

    Single-photon dissociative photoionization of H2/D2 in the Q1, Q2 doubly excited states resonance regions, where ultrafast electronic and nuclear dynamics are coupled, is studied using the vector-correlation method with single selected femtosecond high-order harmonic and synchrotron radiation in the VUV. Results are compared at the level of electron-ion kinetic energy correlation diagrams, asymmetry parameters, and the molecular frame photoelectron angular distributions.

  16. Electron transfer and capture dynamics in ZnSe quantum wells grown on GaAs

    SciTech Connect

    Dongol, A.; Wagner, H. P.

    2013-12-04

    We investigate the transfer and capture dynamics of electrons in phase coherent photorefractive ZnSe quantum wells grown on GaAs using degenerate three-beam four-wave-mixing. The measurements reveal electron capture times by the quantum well in the order of several tens of picoseconds and a transit time of approximately 5 picoseconds from the GaAs substrate through the ZnMgSe barrier.

  17. Carrier-density-wave transport and local internal electric field measurements in biased metal-oxide-semiconductor n-Si devices using contactless laser photo-carrier radiometry

    NASA Astrophysics Data System (ADS)

    Mandelis, Andreas; Pawlak, Micha; Shaughnessy, Derrick

    2004-11-01

    Laser infrared photo-carrier radiometry was used with an n-type Si metal-oxide-semiconductor (MOS) diode and with a Si-SiO2 structure with a transparent electrode and under external bias. Application of three-dimensional PCR theory yielded values of the minority carrier (hole) transport properties in the presence of the thus created local internal electric field at fixed frequencies. Furthermore, the internal electric field at fixed applied voltage was calculated. Under the combination of increased temperature and voltage, the sub-interface position of the carrier-density-wave centroid was found to depend on a trade-off between increased recombination lifetime and decreased ambipolar (conductivity) mobility. The ability of PCR to measure local internal electric fields by combining applied bias sweeps and frequency scans appears to pave the way towards the contactless reconstruction of depth profiles of these fields in active devices.

  18. Towards disentangling coupled electronic-vibrational dynamics in ultrafast non-adiabatic processes

    PubMed

    Blanchet; Lochbrunner; Schmitt; Shaffer; Larsen; Zgierski; Seideman; Stolow

    2000-01-01

    Femtosecond time-resolved photoelectron spectroscopy is emerging as a new technique for investigating polyatomic excited state dynamics. Due to the sensitivity of photoelectron spectroscopy to both electronic configurations and vibrational dynamics, it is well suited to the study of non-adiabatic processes such as internal conversion, which often occur on sub-picosecond time scales. We discuss the technical requirements for such experiments, including lasers systems, energy- and angle-resolved photoelectron spectrometers and new detectors for coincidence experiments. We present a few examples of these methods applied to problems in diatomic wavepacket dynamics and ultrafast non-adiabatic processes in polyatomic molecules.

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

    NASA Astrophysics Data System (ADS)

    Kikuchi, Takashi; Horioka, Kazuhiko; Sasaki, Toru; Harada, Nob.

    2013-11-01

    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.

  20. Electron nuclear dynamics of H + +H2 collisions at Elab=30 eV

    NASA Astrophysics Data System (ADS)

    Morales, Jorge; Diz, Agustin; Deumens, E.; Öhrn, Yngve

    1995-12-01

    Proton collisions with hydrogen molecules at 30 eV in the laboratory frame is a simple ion-molecule system exhibiting a number of distinct processes such as inelastic scattering, charge transfer, rearrangement, and dissociation. The electron nuclear dynamics (END) theory which allows full electron nuclear coupling and which does not restrict the system from reaching any of the possible product channels, is applied to this sytem to produce transition probabilities, differential, and integral (vibrationally resolved) cross sections. Comparisons with experiment demonstrate that END, even in its simplest implementation, with a single determinantal state for the electrons and with classical nuclei, yields results that are competitive with other theoretical approaches.

  1. Charged nanoparticle dynamics in water induced by scanning transmission electron microscopy.

    PubMed

    White, E R; Mecklenburg, Matthew; Shevitski, Brian; Singer, S B; Regan, B C

    2012-02-28

    Using scanning transmission electron microscopy we image ~4 nm platinum nanoparticles deposited on an insulating membrane, where the membrane is one of two electron-transparent windows separating an aqueous environment from the microscope's high vacuum. Upon receiving a relatively moderate dose of ~10(4) e/nm(2), initially immobile nanoparticles begin to move along trajectories that are directed radially outward from the center of the field of view. With larger dose rates the particle motion becomes increasingly dramatic. These observations demonstrate that, even under mild imaging conditions, the in situ electron microscopy of aqueous environments can produce electrophoretic charging effects that dominate the dynamics of nanoparticles under observation.

  2. The electron-furfural scattering dynamics for 63 energetically open electronic states

    NASA Astrophysics Data System (ADS)

    da Costa, Romarly F.; do N. Varella, Márcio T.; Bettega, Márcio H. F.; Neves, Rafael F. C.; Lopes, Maria Cristina A.; Blanco, Francisco; García, Gustavo; Jones, Darryl B.; Brunger, Michael J.; Lima, Marco A. P.

    2016-03-01

    We report on integral-, momentum transfer- and differential cross sections for elastic and electronically inelastic electron collisions with furfural (C5H4O2). The calculations were performed with two different theoretical methodologies, the Schwinger multichannel method with pseudopotentials (SMCPP) and the independent atom method with screening corrected additivity rule (IAM-SCAR) that now incorporates a further interference (I) term. The SMCPP with N energetically open electronic states (Nopen) at either the static-exchange (Nopen ch-SE) or the static-exchange-plus-polarisation (Nopen ch-SEP) approximation was employed to calculate the scattering amplitudes at impact energies lying between 5 eV and 50 eV, using a channel coupling scheme that ranges from the 1ch-SEP up to the 63ch-SE level of approximation depending on the energy considered. For elastic scattering, we found very good overall agreement at higher energies among our SMCPP cross sections, our IAM-SCAR+I cross sections and the experimental data for furan (a molecule that differs from furfural only by the substitution of a hydrogen atom in furan with an aldehyde functional group). This is a good indication that our elastic cross sections are converged with respect to the multichannel coupling effect for most of the investigated intermediate energies. However, although the present application represents the most sophisticated calculation performed with the SMCPP method thus far, the inelastic cross sections, even for the low lying energy states, are still not completely converged for intermediate and higher energies. We discuss possible reasons leading to this discrepancy and point out what further steps need to be undertaken in order to improve the agreement between the calculated and measured cross sections.

  3. The electron-furfural scattering dynamics for 63 energetically open electronic states.

    PubMed

    da Costa, Romarly F; do N Varella, Márcio T; Bettega, Márcio H F; Neves, Rafael F C; Lopes, Maria Cristina A; Blanco, Francisco; García, Gustavo; Jones, Darryl B; Brunger, Michael J; Lima, Marco A P

    2016-03-28

    We report on integral-, momentum transfer- and differential cross sections for elastic and electronically inelastic electron collisions with furfural (C5H4O2). The calculations were performed with two different theoretical methodologies, the Schwinger multichannel method with pseudopotentials (SMCPP) and the independent atom method with screening corrected additivity rule (IAM-SCAR) that now incorporates a further interference (I) term. The SMCPP with N energetically open electronic states (N(open)) at either the static-exchange (N(open) ch-SE) or the static-exchange-plus-polarisation (N(open) ch-SEP) approximation was employed to calculate the scattering amplitudes at impact energies lying between 5 eV and 50 eV, using a channel coupling scheme that ranges from the 1ch-SEP up to the 63ch-SE level of approximation depending on the energy considered. For elastic scattering, we found very good overall agreement at higher energies among our SMCPP cross sections, our IAM-SCAR+I cross sections and the experimental data for furan (a molecule that differs from furfural only by the substitution of a hydrogen atom in furan with an aldehyde functional group). This is a good indication that our elastic cross sections are converged with respect to the multichannel coupling effect for most of the investigated intermediate energies. However, although the present application represents the most sophisticated calculation performed with the SMCPP method thus far, the inelastic cross sections, even for the low lying energy states, are still not completely converged for intermediate and higher energies. We discuss possible reasons leading to this discrepancy and point out what further steps need to be undertaken in order to improve the agreement between the calculated and measured cross sections. PMID:27036451

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

    PubMed

    Sun, Jingya; Adhikari, Aniruddha; Shaheen, Basamat S; Yang, Haoze; Mohammed, Omar F

    2016-03-17

    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 these techniques 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 subpicosecond 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 crystal and its powder film. We also discuss 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.

  5. Simulating electron spin resonance spectra of nitroxide spin labels from molecular dynamics and stochastic trajectories

    PubMed Central

    Sezer, Deniz; Freed, Jack H.; Roux, Benoît

    2008-01-01

    Simulating electron spin resonance spectra of nitroxide spin labels from motional models is necessary for the quantitative analysis of experimental spectra. We present a framework for modeling the spin label dynamics by using trajectories such as those from molecular dynamics (MD) simulations combined with stochastic treatment of the global protein tumbling. This is achieved in the time domain after two efficient numerical integrators are developed: One for the quantal dynamics of the spins and the other for the classical rotational diffusion. For the quantal dynamics, we propagate the relevant part of the spin density matrix in Hilbert space. For the diffusional tumbling, we work with quaternions, which enables the treatment of anisotropic diffusion in a potential expanded as a sum of spherical harmonics. Time-averaging arguments are invoked to bridge the gap between the smaller time step of the MD trajectories and the larger time steps appropriate for the rotational diffusion and∕or quantal spin dynamics. PMID:18447510

  6. Applications of time-domain spectroscopy to electron-phonon coupling dynamics at surfaces.

    PubMed

    Matsumoto, Yoshiyasu

    2014-10-01

    Photochemistry is one of the most important branches in chemistry to promote and control chemical reactions. In particular, there has been growing interest in photoinduced processes at solid surfaces and interfaces with liquids such as water for developing efficient solar energy conversion. For example, photoinduced charge transfer between adsorbates and semiconductor substrates at the surfaces of metal oxides induced by photogenerated holes and electrons is a core process in photovoltaics and photocatalysis. In these photoinduced processes, electron-phonon coupling plays a central role. This paper describes how time-domain spectroscopy is applied to elucidate electron-phonon coupling dynamics at metal and semiconductor surfaces. Because nuclear dynamics induced by electronic excitation through electron-phonon coupling take place in the femtosecond time domain, the pump-and-probe method with ultrashort pulses used in time-domain spectroscopy is a natural choice for elucidating the electron-phonon coupling at metal and semiconductor surfaces. Starting with a phenomenological theory of coherent phonons generated by impulsive electronic excitation, this paper describes a couple of illustrative examples of the applications of linear and nonlinear time-domain spectroscopy to a simple adsorption system, alkali metal on Cu(111), and more complex photocatalyst systems. PMID:25139240

  7. Analysis of electron dynamics and two mechanisms in a coaxial magnetic wiggler

    SciTech Connect

    Xie, Jialing; Teng, Yan; Chen, Changhua; Wang, Guangqiang; Li, Shuang; Song, Zhimin; Xiao, Renzhen; Chang, Chao

    2014-12-15

    The electron dynamics in a coaxial magnetic wiggler are analyzed numerically and studied in particle-in-cell (PIC) simulation. Electrons wiggle in angular direction to coherently generate a TE{sub 01} mode, and the results are consistent with each other. The trajectory of the electron in 3-D space and the effects on the trajectories of the initial phases of wiggler magnetic fields are researched, which helps to choose appropriate initial phases to control the trajectory of the electron. An oscillator of FEL with a coaxial magnetic wiggler based on a quasi cavity is designed for efficiently generating the TE{sub 01} mode with the high saturation power and high efficiency. The advantages of the quasi cavity structure are analyzed and the parameter-selection rules are investigated. Based on the electron dynamics, the process of electron bunching in the self amplified spontaneous emission (SASE) and the Seeded mechanisms are studied. The Seeded mechanism could accelerate electron bunching greatly and reduce the saturation time than the SASE by half.

  8. Investigation of collective electron dynamics in relativistically transparent laser-foil interactions

    NASA Astrophysics Data System (ADS)

    Gray, Ross; MacLellan, David; Gonzalez-Izquierdo, Bruno; Powell, Haydn; Carroll, David; Murphy, Christopher; Stockhausen, Luca; Rusby, Dean; Scott, Graeme; Wilson, Robbie; Booth, Nicola; Symes, Dan; Hawkes, Steve; Torres, Ricardo; Borghesi, Marco; Neely, David; McKenna, Paul

    2014-10-01

    The interaction of an intense laser pulse with a solid target produces high energy electrons at the target-vacuum boundary. For sufficiently high laser intensities and thin targets, the electrons become relativistic and rapidly expand into vacuum, lowering the peak electron density. The combined increase in the relativistically-corrected critical density and the reduction in the target electron density results in the onset of relativistic induced transparency (RIT) during the laser pulse, enabling the remainder of the pulse to propagate through the target and further interact with the accelerated electrons. We report on measurements of the collective dynamics of laser driven electrons in the RIT regime. The 2D profile of the beam of accelerated electrons is shown to change from an ellipse aligned along the laser polarization direction in the case of limited RIT, to a double-lobe structure aligned perpendicular to it, for a larger degree of RIT. The temporal dynamics of the interaction are investigated via PIC simulations. The implications of RIT for laser-driven ion acceleration is also explored.

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

    SciTech Connect

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

    2015-04-07

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

  10. Carrier dynamics of rubrene single-crystals revealed by transient broadband terahertz spectroscopy

    NASA Astrophysics Data System (ADS)

    Yada, H.; Uchida, R.; Sekine, H.; Terashige, T.; Tao, S.; Matsui, Y.; Kida, N.; Fratini, S.; Ciuchi, S.; Okada, Y.; Uemura, T.; Takeya, J.; Okamoto, H.

    2014-10-01

    Carrier dynamics of an organic molecular semiconductor, rubrene, was investigated by optical-pump terahertz-probe spectroscopy from 1 to 15 THz. At 294 K, a Drude-like response due to photogenerated hole carriers is observed below 8 THz. The real part σ 1 ( ω ) of the optical conductivity is suppressed below 2 THz, indicating the presence of a localization effect. Such a spectral feature was reproduced by a Drude-Anderson model including the effect of dynamical disorder due to intermolecular vibrations. At 50 K, the spectral weight of σ 1 ( ω ) due to photocarriers shifts to lower frequency below 4 THz and the suppression of σ 1 ( ω ) is hardly observed, which we associate with a reduction of thermal molecular motions. The overall photocarrier generation and recombination dynamics is also discussed.

  11. High-harmonic probing of electronic coherence in dynamically aligned molecules.

    PubMed

    Kraus, P M; Zhang, S B; Gijsbertsen, A; Lucchese, R R; Rohringer, N; Wörner, H J

    2013-12-13

    We introduce and demonstrate a new approach to measuring coherent electron wave packets using high-harmonic spectroscopy. By preparing a molecule in a coherent superposition of electronic states, we show that electronic coherence opens previously unobserved high-harmonic-generation channels that connect distinct but coherently related electronic states. Performing the measurements in dynamically aligned nitric oxide molecules we observe the complex temporal evolution of the electronic coherence under coupling to nuclear motion. Choosing a weakly allowed transition to prepare the wave packet, we demonstrate an unprecedented sensitivity that arises from optical interference between coherent and incoherent pathways. This mechanism converts a 0.1% excitation fraction into a ∼20% signal modulation.

  12. Crucial role of nuclear dynamics for electron injection in a dye–semiconductor complex

    SciTech Connect

    Monti, Adriano; Negre, Christian F. A.; Batista, Victor S.; Rego, Luis G. C.; de Groot, Huub J. M.; Buda, Francesco

    2015-06-05

    In this study, we investigate the electron injection from a terrylene-based chromophore to the TiO2 semiconductor bridged by a recently proposed phenyl-amide-phenyl molecular rectifier. The mechanism of electron transfer is studied by means of quantum dynamics simulations using an extended Hückel Hamiltonian. It is found that the inclusion of the nuclear motion is necessary to observe the photoinduced electron transfer. In particular, the fluctuations of the dihedral angle between the terrylene and the phenyl ring modulate the localization and thus the electronic coupling between the donor and acceptor states involved in the injection process. The electron propagation shows characteristic oscillatory features that correlate with interatomic distance fluctuations in the bridge, which are associated with the vibrational modes driving the process. The understanding of such effects is important for the design of functional dyes with optimal injection and rectification properties.

  13. Competition of static magnetic and dynamic photon forces in electronic transport through a quantum dot.

    PubMed

    Rauf Abdullah, Nzar; Tang, Chi-Shung; Manolescu, Andrei; Gudmundsson, Vidar

    2016-09-21

    We investigate theoretically the balance of the static magnetic and the dynamical photon forces in the electron transport through a quantum dot in a photon cavity with a single photon mode. The quantum dot system is connected to external leads and the total system is exposed to a static perpendicular magnetic field. We explore the transport characteristics through the system by tuning the ratio, [Formula: see text], between the photon energy, [Formula: see text], and the cyclotron energy, [Formula: see text]. Enhancement in the electron transport with increasing electron-photon coupling is observed when [Formula: see text]. In this case the photon field dominates and stretches the electron charge distribution in the quantum dot, extending it towards the contact area for the leads. Suppression in the electron transport is found when [Formula: see text], as the external magnetic field causes circular confinement of the charge density around the dot.

  14. Competition of static magnetic and dynamic photon forces in electronic transport through a quantum dot.

    PubMed

    Rauf Abdullah, Nzar; Tang, Chi-Shung; Manolescu, Andrei; Gudmundsson, Vidar

    2016-09-21

    We investigate theoretically the balance of the static magnetic and the dynamical photon forces in the electron transport through a quantum dot in a photon cavity with a single photon mode. The quantum dot system is connected to external leads and the total system is exposed to a static perpendicular magnetic field. We explore the transport characteristics through the system by tuning the ratio, [Formula: see text], between the photon energy, [Formula: see text], and the cyclotron energy, [Formula: see text]. Enhancement in the electron transport with increasing electron-photon coupling is observed when [Formula: see text]. In this case the photon field dominates and stretches the electron charge distribution in the quantum dot, extending it towards the contact area for the leads. Suppression in the electron transport is found when [Formula: see text], as the external magnetic field causes circular confinement of the charge density around the dot. PMID:27420809

  15. Wall-plug efficiency and beam dynamics in free-electron lasers using energy recovery linacs

    SciTech Connect

    Sprangle, P.; Ben-Zvi, I.; Penano, J.; Hafizi, B.

    2010-08-01

    In a high average power free-electron laser (FEL) the wall-plug efficiency is of critical importance in determining the size, complexity, and cost of the overall system. The wall-plug efficiency for the FEL oscillator and amplifier (uniform and tapered wiggler) is strongly dependent on the energy recovery process. A theoretical model for electron beam dynamics in the energy recovery linac is derived and applied to the acceleration and deceleration of nano-Coulomb electron bunches for a tapered FEL amplifier. For the tapered amplifier, the spent electron beam exiting the wiggler consists of trapped and untrapped electrons. Decelerating these two populations using different phases of the radio-frequency wave in the recovery process enhances wall-plug efficiency. For the parameters considered here, the wall-plug efficiency for the tapered amplifier can be {approx}10% using this approach.

  16. Crucial role of nuclear dynamics for electron injection in a dye–semiconductor complex

    DOE PAGESBeta

    Monti, Adriano; Negre, Christian F. A.; Batista, Victor S.; Rego, Luis G. C.; de Groot, Huub J. M.; Buda, Francesco

    2015-06-05

    In this study, we investigate the electron injection from a terrylene-based chromophore to the TiO2 semiconductor bridged by a recently proposed phenyl-amide-phenyl molecular rectifier. The mechanism of electron transfer is studied by means of quantum dynamics simulations using an extended Hückel Hamiltonian. It is found that the inclusion of the nuclear motion is necessary to observe the photoinduced electron transfer. In particular, the fluctuations of the dihedral angle between the terrylene and the phenyl ring modulate the localization and thus the electronic coupling between the donor and acceptor states involved in the injection process. The electron propagation shows characteristic oscillatorymore » features that correlate with interatomic distance fluctuations in the bridge, which are associated with the vibrational modes driving the process. The understanding of such effects is important for the design of functional dyes with optimal injection and rectification properties.« less

  17. Electron and hole self-energy contributions to the dynamic structure factor in interacting-electron systems

    NASA Astrophysics Data System (ADS)

    Green, F.; Neilson, D.; Szymański, J.

    1987-01-01

    A detailed investigation is made of the influence of particle self-energies on the dynamic response of the metallic electron gas. Two quite different approaches, the Green-Neilson-Szymański (GNS) theory and the quasiparticle-lifetime theory, are examined and contrasted. It is shown that the inclusion of off-shell effects in the quasiparticle-lifetime theory drastically alters its central conclusions. Moreover, that theory's neglect of cancellations between self-energy terms and other classes of terms seriously violates the major sum rules. These cancellations are closely connected with conservation principles. The GNS theory, being conserving, reproduces these cancellations in detail.

  18. Experimental Evidence for Dynamic Social Impact: The Emergence of Subcultures in Electronic Groups.

    ERIC Educational Resources Information Center

    Latane, Bibb; Bourgeois, Martin J.

    1996-01-01

    Presents results of experimental tests of Dynamic Social Impact Theory (DSIT) in which participants engaged in discussions over electronic mail. Finds support for the emergence of four group phenomena predicted by DSIT. Shows how, rewarded for being in the majority, individuals' choices resulted in the emergence of four forms of group level…

  19. Dynamics of electron fluxes in the near-rocket region in the ARAKS experiment

    NASA Astrophysics Data System (ADS)

    Izhovkina, N. I.

    2012-05-01

    In the ARAKS experiment, electron pulses were injected into the ionosphere from onboard a rocket. For different series of pulses, the initial energy of electrons was 27 and 15 keV and the current strength was ˜0.5 A. On board the rocket, the distributions of electron fluxes directed toward the rocket were measured using the retarding potential by the electron energy up to 3000 eV. In this work, it is shown that the appearance of extreme values of the intensity of electron fluxes higher than 200 eV at the tail of the electron energy distribution can be explained by the nonmonotonic acceleration of electrons in the fields of electrostatic turbulence. The dynamics of electron and ion fluxes can be influenced by the polarization drift. It should be noted that extreme values of the flux intensities were not observed at heights lower than 130 km. This can be connected with the suppression of electrostatic oscillations by collisions of electrons with ionospheric components.

  20. Excited state X-ray absorption spectroscopy: Probing both electronic and structural dynamics

    NASA Astrophysics Data System (ADS)

    Neville, Simon P.; Averbukh, Vitali; Ruberti, Marco; Yun, Renjie; Patchkovskii, Serguei; Chergui, Majed; Stolow, Albert; Schuurman, Michael S.

    2016-10-01

    We investigate the sensitivity of X-ray absorption spectra, simulated using a general method, to properties of molecular excited states. Recently, Averbukh and co-workers [M. Ruberti et al., J. Chem. Phys. 140, 184107 (2014)] introduced an efficient and accurate L 2 method for the calculation of excited state valence photoionization cross-sections based on the application of Stieltjes imaging to the Lanczos pseudo-spectrum of the algebraic diagrammatic construction (ADC) representation of the electronic Hamiltonian. In this paper, we report an extension of this method to the calculation of excited state core photoionization cross-sections. We demonstrate that, at the ADC(2)x level of theory, ground state X-ray absorption spectra may be accurately reproduced, validating the method. Significantly, the calculated X-ray absorption spectra of the excited states are found to be sensitive to both geometric distortions (structural dynamics) and the electronic character (electronic dynamics) of the initial state, suggesting that core excitation spectroscopies will be useful probes of excited state non-adiabatic dynamics. We anticipate that the method presented here can be combined with ab initio molecular dynamics calculations to simulate the time-resolved X-ray spectroscopy of excited state molecular wavepacket dynamics.

  1. Theoretical methods for attosecond electron and nuclear dynamics: applications to the H2 molecule

    NASA Astrophysics Data System (ADS)

    Palacios, Alicia; Sanz-Vicario, José Luis; Martín, Fernando

    2015-12-01

    Attosecond science, born at the beginning of this century with the generation of the first bursts of light with durations shorter than a femtosecond, has opened the way to look at electron dynamics in atoms and molecules at its natural timescale. Thus controlling chemical reactions at the electronic level or obtaining time-resolved images of the electronic motion has become a goal for many physics and chemistry laboratories all over the world. The new experimental capabilities have spurred the development of sophisticated theoretical methods that can accurately predict phenomena occurring in the sub-fs timescale. This review provides an overview of the capabilities of existing theoretical tools to describe electron and nuclear dynamics resulting from the interaction of femto- and attosecond UV/XUV radiation with simple molecular targets. We describe one of these methods in more detail, the time-dependent Feshbach close-coupling (TDFCC) formalism, which has been used successfully over the years to investigate various attosecond phenomena in the hydrogen molecule and can easily be extended to other diatomics. In addition to describing the details of the method and discussing its advantages and limitations, we also provide examples of the new physics that one can learn by applying it to different problems: from the study of the autoionization decay that follows attosecond UV excitation to the imaging of the coupled electron and nuclear dynamics in H2 using different UV-pump/IR-probe and UV-pump/UV-probe schemes.

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

    SciTech Connect

    Wang, R.; Williams, C. C.

    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.

  3. Restoring electronic coherence/decoherence for a trajectory-based nonadiabatic molecular dynamics

    PubMed Central

    Zhu, Chaoyuan

    2016-01-01

    By utilizing the time-independent semiclassical phase integral, we obtained modified coupled time-dependent Schrödinger equations that restore coherences and induce decoherences within original simple trajectory-based nonadiabatic molecular dynamic algorithms. Nonadiabatic transition probabilities simulated from both Tully’s fewest switches and semiclassical Ehrenfest algorithms follow exact quantum electronic oscillations and amplitudes for three out of the four well-known model systems. Within the present theory, nonadiabatic transitions estimated from statistical ensemble of trajectories accurately follow those of the modified electronic wave functions. The present theory can be immediately applied to the molecular dynamic simulations of photochemical and photophysical processes involving electronic excited states. PMID:27063337

  4. Azimuthal asymmetry in collective electron dynamics in relativistically transparent laser-foil interactions

    NASA Astrophysics Data System (ADS)

    Gray, R. J.; MacLellan, D. A.; Gonzalez-Izquierdo, B.; Powell, H. W.; Carroll, D. C.; Murphy, C. D.; Stockhausen, L. C.; Rusby, D. R.; Scott, G. G.; Wilson, R.; Booth, N.; Symes, D. R.; Hawkes, S. J.; Torres, R.; Borghesi, M.; Neely, D.; McKenna, P.

    2014-09-01

    Asymmetry in the collective dynamics of ponderomotively-driven electrons in the interaction of an ultraintense laser pulse with a relativistically transparent target is demonstrated experimentally. The 2D profile of the beam of accelerated electrons is shown to change from an ellipse aligned along the laser polarization direction in the case of limited transparency, to a double-lobe structure aligned perpendicular to it when a significant fraction of the laser pulse co-propagates with the electrons. The temporally-resolved dynamics of the interaction are investigated via particle-in-cell simulations. The results provide new insight into the collective response of charged particles to intense laser fields over an extended interaction volume, which is important for a wide range of applications, and in particular for the development of promising new ultraintense laser-driven ion acceleration mechanisms involving ultrathin target foils.

  5. Nonadiabatic Study of Dynamic Electronic Effects during Brittle Fracture of Silicon

    NASA Astrophysics Data System (ADS)

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

    2012-01-01

    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.

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

    PubMed

    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. PMID:22400860

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

    SciTech Connect

    Ortiz-Sanchez, Juan Manuel; Gelabert, Ricard; Moreno, Miquel; Lluch, Jose M.

    2008-12-07

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

  8. Momentum Imaging of the Dynamics of Dissociative Electron Attachment to Uracil

    NASA Astrophysics Data System (ADS)

    Slaughter, Dan; Kawarai, Yu; Weber, Thorsten; Azuma, Yoshiro; Winstead, Carl; McKoy, Vince; Belkacem, Ali

    2013-05-01

    Observation of the dynamics of dissociative electron attachment (DEA) in biomolecules has recently become possible by momentum imaging of the fragments resulting from the dissociating transient anion resonance. A momentum spectrometer featuring a 4 π solid angle of detection is combined with a pulsed electron beam and effusive molecular beam in a crossed geometry to measure the full 3D momentum distribution of dissociating negative ions. Guided by electronic structure calculations that indicate the most likely orientation of the molecule at the time of attachment, we present key aspects of the dynamics of ring-breaking dissociation of the transient anion formed upon DEA to the nucleobase uracil. Performed under the auspices of the US DOE by LBNL under Contract DE-AC02-05CH11231.

  9. Dissociative Electron Attachment Dynamics in the Nucleobase Uracil and Related Molecules

    NASA Astrophysics Data System (ADS)

    Slaughter, Daniel; Kuriyama, Yosuke; Kawarai, Yu; Azuma, Yoshiro; Winstead, Carl; McKoy, Vincent; Weber, Thorsten; Belkacem, Ali

    2015-05-01

    We report the dynamics of dissociative electron attachment (DEA) in the biologically-relevant molecule uracil and the diazines pyrazine and pyrimidine. Our DEA reaction microscope consists of a 3D momentum-imaging spectrometer, a pulsed low-energy electron gun and an effusive gas target. The experimental approach allows the measurement of kinetic energy and angular distributions of ionic fragments produced by DEA, in some cases elucidating the total kinetic energy release following two-body breakup. By comparison of calculations of the electron attachment probability in the molecular frame with measured ion angular distributions, we determine that one of the uracil anion resonances could be a Feshbach resonance and we compare the dynamics of the dissociation of the uracil anion with the diazines. Work supported by Chemical Sciences, Geosciences and Biosciences division of BES/DOE

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

    NASA Astrophysics Data System (ADS)

    Wang, R.; Williams, C. C.

    2015-09-01

    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.

  11. Time-dependent theoretical treatments of the dynamics of electrons and nuclei in molecular systems

    SciTech Connect

    Deumens, E.; Diz, A.; Longo, R.; Oehrn, Y. )

    1994-07-01

    An overview is presented of methods for time-dependent treatments of molecules as systems of electrons and nuclei. The theoretical details of these methods are reviewed and contrasted in the light of a recently developed time-dependent method called electron-nuclear dynamics. Electron-nuclear dynamics (END) is a formulation of the complete dynamics of electrons and nuclei of a molecular system that eliminates the necessity of constructing potential-energy surfaces. Because of its general formulation, it encompasses many aspects found in other formulations and can serve as a didactic device for clarifying many of the principles and approximations relevant in time-dependent treatments of molecular systems. The END equations are derived from the time-dependent variational principle applied to a chosen family of efficiently parametrized approximate state vectors. A detailed analysis of the END equations is given for the case of a single-determinantal state for the electrons and a classical treatment of the nuclei. The approach leads to a simple formulation of the fully nonlinear time-dependent Hartree-Fock theory including nuclear dynamics. The nonlinear END equations with the [ital ab] [ital initio] Coulomb Hamiltonian have been implemented at this level of theory in a computer program, ENDyne, and have been shown feasible for the study of small molecular systems. Implementation of the Austin Model 1 semiempirical Hamiltonian is discussed as a route to large molecular systems. The linearized END equations at this level of theory are shown to lead to the random-phase approximation for the coupled system of electrons and nuclei. The qualitative features of the general nonlinear solution are analyzed using the results of the linearized equations as a first approximation. Some specific applications of END are presented, and the comparison with experiment and other theoretical approaches is discussed.

  12. Time-dependent theoretical treatments of the dynamics of electrons and nuclei in molecular systems

    NASA Astrophysics Data System (ADS)

    Deumens, E.; Diz, A.; Longo, R.; Öhrn, Y.

    1994-07-01

    An overview is presented of methods for time-dependent treatments of molecules as systems of electrons and nuclei. The theoretical details of these methods are reviewed and contrasted in the light of a recently developed time-dependent method called electron-nuclear dynamics. Electron-nuclear dynamics (END) is a formulation of the complete dynamics of electrons and nuclei of a molecular system that eliminates the necessity of constructing potential-energy surfaces. Because of its general formulation, it encompasses many aspects found in other formulations and can serve as a didactic device for clarifying many of the principles and approximations relevant in time-dependent treatments of molecular systems. The END equations are derived from the time-dependent variational principle applied to a chosen family of efficiently parametrized approximate state vectors. A detailed analysis of the END equations is given for the case of a single-determinantal state for the electrons and a classical treatment of the nuclei. The approach leads to a simple formulation of the fully nonlinear time-dependent Hartree-Fock theory including nuclear dynamics. The nonlinear END equations with the ab initio Coulomb Hamiltonian have been implemented at this level of theory in a computer program, ENDyne, and have been shown feasible for the study of small molecular systems. Implementation of the Austin Model 1 semiempirical Hamiltonian is discussed as a route to large molecular systems. The linearized END equations at this level of theory are shown to lead to the random-phase approximation for the coupled system of electrons and nuclei. The qualitative features of the general nonlinear solution are analyzed using the results of the linearized equations as a first approximation. Some specific applications of END are presented, and the comparison with experiment and other theoretical approaches is discussed.

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

    NASA Astrophysics Data System (ADS)

    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

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

    NASA Astrophysics Data System (ADS)

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

    2014-12-01

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

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

    SciTech Connect

    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.

  16. Quantum dynamics with fermion coupled coherent states: Theory and application to electron dynamics in laser fields

    SciTech Connect

    Kirrander, Adam; Shalashilin, Dmitrii V.

    2011-09-15

    We present an alternate version of the coupled-coherent-state method, specifically adapted for solving the time-dependent Schroedinger equation for multielectron dynamics in atoms and molecules. This theory takes explicit account of the exchange symmetry of fermion particles, and it uses fermion molecular dynamics to propagate trajectories. As a demonstration, calculations in the He atom are performed using the full Hamiltonian and accurate experimental parameters. Single- and double-ionization yields by 160-fs and 780-nm laser pulses are calculated as a function of field intensity in the range 10{sup 14}-10{sup 16} W/cm{sup 2}, and good agreement with experiments by Walker et al. is obtained. Since this method is trajectory based, mechanistic analysis of the dynamics is straightforward. We also calculate semiclassical momentum distributions for double ionization following 25-fs and 795-nm pulses at 1.5x10{sup 15} W/cm{sup 2}, in order to compare them with the detailed experiments by Rudenko et al. For this more challenging task, full convergence is not achieved. However, major effects such as the fingerlike structures in the momentum distribution are reproduced.

  17. Electron dynamics and cross-shock potential at the quasi-perpendicular Earth's bow shock

    NASA Astrophysics Data System (ADS)

    Lefebvre, Bertrand; Schwartz, Steven J.; Fazakerley, Andrew F.; Décréau, Pierrette

    2007-09-01

    The evolution of the electron distribution function through quasi-perpendicular collisionless shocks is believed to be dominated by the electron dynamics in the large-scale coherent and quasi-stationary magnetic and electric fields. We investigate the electron distributions measured on board Cluster by the Plasma Electron and Current Experiment (PEACE) instrument during three quasi-perpendicular bow shock crossings. Observed distributions are compared with those predicted by electron dynamics resulting from conservation of the first adiabatic invariant and energy in the de Hoffmann-Teller frame, for all pitch angles and all types of trajectories (passing and, for the first time, reflected or trapped). The predicted downstream velocity distributions are mapped from upstream measurements using an improved Liouville mapping technique taking into account the overshoots. Furthermore, for one of these crossings we could take advantage of the configuration of the Cluster quartet to compare mapped upstream velocity distributions with those simultaneously measured at a relatively well magnetically connected downstream location. Consequences of energy and adiabatic invariant conservation are found to be compatible with the observed electron distributions, confirming the validity of electron ``heating'' theories based on DC fields as zeroth-order approximations, but some systematic deviations are found between the dynamics of low- and high-adiabatic invariant electrons. Our approach also provides a way to estimate the cross-shock electric potential profile making full use of the electron measurements, and the results are compared to other estimates relying on the steady state dissipationless electron fluid equations. At the temporal resolution of the instruments, the scales associated to the change of the potential generally appear to be comparable to those of the magnetic field, but some differences between the methods appear within the shock transition. It is argued that

  18. Combined treatment of relaxation and fluctuation dynamics in the calculation of two-dimensional electronic spectra

    SciTech Connect

    Seibt, Joachim; Pullerits, Tõnu

    2014-09-21

    While the theoretical description of population transfer subsequent to electronic excitation in combination with a line shape function description of vibrational dynamics in the context of 2D-spectroscopy is well-developed under the assumption of different timescales of population transfer and fluctuation dynamics, the treatment of the interplay between both kinds of processes lacks a comprehensive description. To bridge this gap, we use the cumulant expansion approach to derive response functions, which account for fluctuation dynamics and population transfer simultaneously. We compare 2D-spectra of a model system under different assumptions about correlations between fluctuations and point out under which conditions a simplified treatment is justified. Our study shows that population transfer and dissipative fluctuation dynamics cannot be described independent of each other in general. Advantages and limitations of the proposed calculation method and its compatibility with the modified Redfield description are discussed.

  19. Correlation between electron-irradiation defects and applied stress in graphene: A molecular dynamics study

    SciTech Connect

    Kida, Shogo; Yamamoto, Masaya; Kawata, Hiroaki; Hirai, Yoshihiko; Yasuda, Masaaki; Tada, Kazuhiro

    2015-09-15

    Molecular dynamics (MD) simulations are performed to study the correlation between electron irradiation defects and applied stress in graphene. The electron irradiation effect is introduced by the binary collision model in the MD simulation. By applying a tensile stress to graphene, the number of adatom-vacancy (AV) and Stone–Wales (SW) defects increase under electron irradiation, while the number of single-vacancy defects is not noticeably affected by the applied stress. Both the activation and formation energies of an AV defect and the activation energy of an SW defect decrease when a tensile stress is applied to graphene. Applying tensile stress also relaxes the compression stress associated with SW defect formation. These effects induced by the applied stress cause the increase in AV and SW defect formation under electron irradiation.

  20. Recombination dynamics of spatially confined electron-hole system in luminescent gold catalyzed silicon nanowires.

    PubMed

    Demichel, O; Calvo, V; Pauc, N; Besson, A; Noé, P; Oehler, F; Gentile, P; Magnea, N

    2009-07-01

    We study by time-resolved low temperature photoluminescence (PL) experiments of the electronic states of silicon nanowires (SiNWs) grown by gold catalyzed chemical vapor deposition and passivated by thermal SiO(2). The typical recombination line of free carriers in gold-catalyzed SiNWs (Au-SiNWs) is identified and studied by time-resolved experiments. We demonstrate that intrinsic Auger recombination governs the recombination dynamic of the dense e-h plasma generated inside the NW. In a few tens of nanoseconds after the pulsed excitation, the density of the initial electronic system rapidly decreases down to reach that of a stable electron-hole liquid phase. The comparison of the PL intensity decay time of Au-SiNWs with high crystalline quality and purity silicon layer allows us to conclude that the Au-SiNW electronic properties are highly comparable to those of bulk silicon crystal.

  1. Dynamical electron compressibility in the 3D topological insulator Bi2Se3

    NASA Astrophysics Data System (ADS)

    Inhofer, Andreas; Assaf, Badih; Wilmart, Quentin; Veyrat, Louis; Nowka, Christian; Dufouleur, Joseph; Giraud, Romain; Hampel, Silke; Buechner, Bernd; Fève, Gwendal; Berroir, Jean-Marc; Placais, Bernard

    Measurements of the quantum capacitance cq, related to the electron compressibility χ =cq /e2 is a sensitive tool to probe the density of states. In a topological insulator (TI) the situation is enriched by the coexistence and the interplay of topologically protected surface states and massive bulk carriers. We investigate top-gate metal-oxyde-TI capacitors using Bi2Se3 thin crystals at GHz frequencies. These measurements provide insight into the compressibillity of such a two electron-fluid system. Furthermore, the dynamical response yields information about electron scattering properties in TIs. More specifically, in our measurements we track simultaneously the conductivity σ and the compressibility as a function of a DC-gate voltage. Using the Einstein relation σ =cq D , we have access to the gate dependence of the electron diffusion constant D (Vg) , a signature of the peculiar scattering mechanisms in TIs.

  2. Correlated proton-electron hole dynamics in protonated water clusters upon extreme ultraviolet photoionization

    DOE PAGESBeta

    Li, Zheng; Vendrell, Oriol

    2016-01-13

    The ultrafast nuclear and electronic dynamics of protonated water clusters H+(H2O)n after extreme ultraviolet photoionization is investigated. In particular, we focus on cluster cations with n = 3, 6, and 21. Upon ionization, two positive charges are present in the cluster related to the excess proton and the missing electron, respectively. A correlation is found between the cluster's geometrical conformation and initial electronic energy with the size of the final fragments produced. As a result, for situations in which the electron hole and proton are initially spatially close, the two entities become correlated and separate in a time-scale of 20more » to 40 fs driven by strong non-adiabatic effects.« less

  3. Correlated proton-electron hole dynamics in protonated water clusters upon extreme ultraviolet photoionization

    PubMed Central

    Li, Zheng; Vendrell, Oriol

    2016-01-01

    The ultrafast nuclear and electronic dynamics of protonated water clusters H+(H2O)n after extreme ultraviolet photoionization is investigated. In particular, we focus on cluster cations with n = 3, 6, and 21. Upon ionization, two positive charges are present in the cluster related to the excess proton and the missing electron, respectively. A correlation is found between the cluster's geometrical conformation and initial electronic energy with the size of the final fragments produced. For situations in which the electron hole and proton are initially spatially close, the two entities become correlated and separate in a time-scale of 20 to 40 fs driven by strong non-adiabatic effects. PMID:26798842

  4. Electron Correlation Microscopy: A New Technique for Studying Local Atom Dynamics Applied to a Supercooled Liquid.

    PubMed

    He, Li; Zhang, Pei; Besser, Matthew F; Kramer, Matthew Joseph; Voyles, Paul M

    2015-08-01

    Electron correlation microscopy (ECM) is a new technique that utilizes time-resolved coherent electron nanodiffraction to study dynamic atomic rearrangements in materials. It is the electron scattering equivalent of photon correlation spectroscopy with the added advantage of nanometer-scale spatial resolution. We have applied ECM to a Pd40Ni40P20 metallic glass, heated inside a scanning transmission electron microscope into a supercooled liquid to measure the structural relaxation time τ between the glass transition temperature T g and the crystallization temperature, T x . τ determined from the mean diffraction intensity autocorrelation function g 2(t) decreases with temperature following an Arrhenius relationship between T g and T g +25 K, and then increases as temperature approaches T x . The distribution of τ determined from the g 2(t) of single speckles is broad and changes significantly with temperature.

  5. Dynamic defect correlations dominate activated electronic transport in SrTiO3

    PubMed Central

    Snijders, Paul C.; Şen, Cengiz; McConnell, Michael P.; Ma, Ying-Zhong; May, Andrew F.; Herklotz, Andreas; Wong, Anthony T.; Ward, T. Zac

    2016-01-01

    Strontium titanate (SrTiO3, STO) is a critically important material for the study of emergent electronic phases in complex oxides, as well as for the development of applications based on their heterostructures. Despite the large body of knowledge on STO, there are still many uncertainties regarding the role of defects in the properties of STO, including their influence on ferroelectricity in bulk STO and ferromagnetism in STO-based heterostructures. We present a detailed analysis of the decay of persistent photoconductivity in STO single crystals with defect concentrations that are relatively low but significantly affect their electronic properties. The results show that photo-activated electron transport cannot be described by a superposition of the properties due to independent point defects as current models suggest but is, instead, governed by defect complexes that interact through dynamic correlations. These results emphasize the importance of defect correlations for activated electronic transport properties of semiconducting and insulating perovskite oxides. PMID:27443503

  6. Electronic excitation induced amorphization in titanate pyrochlores: an ab initio molecular dynamics study

    DOE PAGESBeta

    Xiao, Haiyan Y.; Weber, William J.; Zhang, Yanwen; Zu, X. T.; Li, Sean

    2015-02-09

    In this study, the response of titanate pyrochlores (A2Ti2O7, A = Y, Gd and Sm) to electronic excitation is investigated utilizing an ab initio molecular dynamics method. All the titanate pyrochlores are found to undergo a crystalline-to-amorphous structural transition under a low concentration of electronic excitations. The transition temperature at which structural amorphization starts to occur depends on the concentration of electronic excitations. During the structural transition, O2-like molecules are formed, and this anion disorder further drives cation disorder that leads to an amorphous state. This study provides new insights into the mechanisms of amorphization in titanate pyrochlores under laser,more » electron and ion irradiations.« less

  7. Stability of graphene edges under electron beam: equilibrium energetics versus dynamic effects.

    PubMed

    Kotakoski, Jani; Santos-Cottin, David; Krasheninnikov, Arkady V

    2012-01-24

    Electron beam of a transmission electron microscope can be used to alter the morphology of graphene nanoribbons and create atomically sharp edges required for applications of graphene in nanoelectronics. Using density-functional-theory-based simulations, we study the radiation hardness of graphene edges and show that the response of the ribbons to irradiation is not determined by the equilibrium energetics as assumed in previous experiments, but by kinetic effects associated with the dynamics of the edge atoms after impacts of energetic electrons. We report an unexpectedly high stability of armchair edges, comparable to that of pristine graphene, and demonstrate that the electron energy should be below ~50 keV to minimize the knock-on damage.

  8. Dynamic defect correlations dominate activated electronic transport in SrTiO3.

    PubMed

    Snijders, Paul C; Şen, Cengiz; McConnell, Michael P; Ma, Ying-Zhong; May, Andrew F; Herklotz, Andreas; Wong, Anthony T; Ward, T Zac

    2016-01-01

    Strontium titanate (SrTiO3, STO) is a critically important material for the study of emergent electronic phases in complex oxides, as well as for the development of applications based on their heterostructures. Despite the large body of knowledge on STO, there are still many uncertainties regarding the role of defects in the properties of STO, including their influence on ferroelectricity in bulk STO and ferromagnetism in STO-based heterostructures. We present a detailed analysis of the decay of persistent photoconductivity in STO single crystals with defect concentrations that are relatively low but significantly affect their electronic properties. The results show that photo-activated electron transport cannot be described by a superposition of the properties due to independent point defects as current models suggest but is, instead, governed by defect complexes that interact through dynamic correlations. These results emphasize the importance of defect correlations for activated electronic transport properties of semiconducting and insulating perovskite oxides. PMID:27443503

  9. Dynamical Mean-Field Theory of Electronic Correlations in Models and Materials

    NASA Astrophysics Data System (ADS)

    Vollhardt, Dieter

    2010-11-01

    The concept of electronic correlations plays an important role in modern condensed matter physics. It refers to interaction effects which cannot be explained within a static mean-field picture as provided by Hartree-Fock theory. Electronic correlations can have a very strong influence on the properties of materials. For example, they may turn a metal into an insulator (Mott-Hubbard metal-insulator transition). In these lecture notes I (i) introduce basic notions of the physics of correlated electronic systems, (ii) discuss the construction of mean-field theories by taking the limit of high lattice dimensions, (iii) explain the simplifications of the many-body perturbation theory in this limit which provide the basis for the formulation of a comprehensive mean-field theory for correlated fermions, the dynamical mean-field theory (DMFT), (v) derive the DMFT self-consistency equations, and (vi) apply the DMFT to investigate electronic correlations in models and materials.

  10. Radiative damping and electron beam dynamics in plasma-based accelerators.

    PubMed

    Michel, P; Schroeder, C B; Shadwick, B A; Esarey, E; Leemans, W P

    2006-08-01

    The effects of radiation reaction on electron beam dynamics are studied in the context of plasma-based accelerators. Electrons accelerated in a plasma channel undergo transverse betatron oscillations due to strong focusing forces. These oscillations lead to emission by the electrons of synchrotron radiation, with a corresponding energy loss that affects the beam properties. An analytical model for the single particle orbits and beam moments including the classical radiation reaction force is derived and compared to the results of a particle transport code. Since the betatron amplitude depends on the initial transverse position of the electron, the resulting radiation can increase the relative energy spread of the beam to significant levels (e.g., several percent). This effect can be diminished by matching the beam into the channel, which could require micron sized beam radii for typical values of the beam emittance and plasma density.

  11. Radiative damping and electron beam dynamics in plasma-based accelerators

    NASA Astrophysics Data System (ADS)

    Michel, P.; Schroeder, C. B.; Shadwick, B. A.; Esarey, E.; Leemans, W. P.

    2006-08-01

    The effects of radiation reaction on electron beam dynamics are studied in the context of plasma-based accelerators. Electrons accelerated in a plasma channel undergo transverse betatron oscillations due to strong focusing forces. These oscillations lead to emission by the electrons of synchrotron radiation, with a corresponding energy loss that affects the beam properties. An analytical model for the single particle orbits and beam moments including the classical radiation reaction force is derived and compared to the results of a particle transport code. Since the betatron amplitude depends on the initial transverse position of the electron, the resulting radiation can increase the relative energy spread of the beam to significant levels (e.g., several percent). This effect can be diminished by matching the beam into the channel, which could require micron sized beam radii for typical values of the beam emittance and plasma density.

  12. Ultrafast Electronic Processes At Semiconductor Polymer Heterojunctions: A Molecular-Level, Quantum-Dynamical Analysis

    SciTech Connect

    Burghardt, I.; Tamura, H.; Bittner, E. R.

    2009-03-09

    This contribution gives an overview of our recent study of phonon-driven exciton dissociation at semiconductor polymer heterojunctions, using a quantum dynamical analysis based on a linear vibronic coupling model parametrized for three electronic states and 20-30 phonon modes. The decay of the photogenerated exciton towards an interfacial charge transfer state is an ultrafast (femtosecond to picosecond scale) process which initiates the photocurrent generation. We consider several representative interface configurations, which are shown to exhibit an efficient exciton dissociation. The process depends critically on the presence of intermediate states, and on the dynamical interplay between high-frequency (C=C stretch) and low-frequency (ring-torsional) modes. The dynamical mechanism is interpreted in terms of a hierarchical electron-phonon model which allows one to identify generalized reaction coordinates for the nonadiabatic process. This analysis highlights that the electron-phonon coupling is dominated by the high-frequency modes, but the low-frequency modes are crucial in mediating the transition to a charge-separated state. The ultra-fast, highly nonequilibrium dynamics is in accordance with spectroscopic observations.

  13. Dynamic Localization of Electronic Excitation in Photosynthetic Complexes Revealed with Chiral Two-Dimensional Spectroscopy

    PubMed Central

    Fidler, Andrew F.; Singh, Ved P.; Long, Phillip D.; Dahlberg, Peter D.; Engel, Gregory S.

    2014-01-01

    Time-resolved ultrafast optical probes of chiral dynamics provide a new window allowing us to explore how interactions with such structured environments drive electronic dynamics. Incorporating optical activity into time-resolved spectroscopies has proven challenging due to the small signal and large achiral background. Here, we demonstrate that two-dimensional electronic spectroscopy can be adapted to detect chiral signals and that these signals reveal how excitations delocalize and contract following excitation. We dynamically probe the evolution of chiral electronic structure in the light harvesting complex 2 of purple bacteria following photoexcitation by creating a chiral two-dimensional mapping. The dynamics of the chiral two-dimensional signal directly reports on changes in the degree of delocalization of the excitonic state following photoexcitation. The mechanism of energy transfer in this system may enhance transfer probability due to the coherent coupling among chromophores while suppressing fluorescence that arises from populating delocalized states. This generally applicable spectroscopy will provide an incisive tool to probe ultrafast transient molecular fluctuations that are obscured in non-chiral experiments. PMID:24504144

  14. Ultrafast Electronic Processes At Semiconductor Polymer Heterojunctions: A Molecular-Level, Quantum-Dynamical Analysis

    NASA Astrophysics Data System (ADS)

    Burghardt, I.; Bittner, E. R.; Tamura, H.

    2009-03-01

    This contribution gives an overview of our recent study of phonon-driven exciton dissociation at semiconductor polymer heterojunctions, using a quantum dynamical analysis based on a linear vibronic coupling model parametrized for three electronic states and 20-30 phonon modes. The decay of the photogenerated exciton towards an interfacial charge transfer state is an ultrafast (femtosecond to picosecond scale) process which initiates the photocurrent generation. We consider several representative interface configurations, which are shown to exhibit an efficient exciton dissociation. The process depends critically on the presence of intermediate states, and on the dynamical interplay between high-frequency (C=C stretch) and low-frequency (ring-torsional) modes. The dynamical mechanism is interpreted in terms of a hierarchical electron-phonon model which allows one to identify generalized reaction coordinates for the nonadiabatic process. This analysis highlights that the electron-phonon coupling is dominated by the high-frequency modes, but the low-frequency modes are crucial in mediating the transition to a charge-separated state. The ultra-fast, highly nonequilibrium dynamics is in accordance with spectroscopic observations.

  15. Charge-Transfer State Dynamics Following Hole and Electron Transfer in Organic Photovoltaic Devices.

    PubMed

    Bakulin, Artem A; Dimitrov, Stoichko D; Rao, Akshay; Chow, Philip C Y; Nielsen, Christian B; Schroeder, Bob C; McCulloch, Iain; Bakker, Huib J; Durrant, James R; Friend, Richard H

    2013-01-01

    The formation of bound electron-hole pairs, also called charge-transfer (CT) states, in organic-based photovoltaic devices is one of the dominant loss mechanisms hindering performance. Whereas CT state dynamics following electron transfer from donor to acceptor have been widely studied, there is not much known about the dynamics of bound CT states produced by hole transfer from the acceptor to the donor. In this letter, we compare the dynamics of CT states formed in the different charge-transfer pathways in a range of model systems. We show that the nature and dynamics of the generated CT states are similar in the case of electron and hole transfer. However the yield of bound and free charges is observed to be strongly dependent on the HOMOD-HOMOA and LUMOD-LUMOA energy differences of the material system. We propose a qualitative model in which the effects of static disorder and sampling of states during the relaxation determine the probability of accessing CT states favorable for charge separation.

  16. Dynamic localization of electronic excitation in photosynthetic complexes revealed with chiral two-dimensional spectroscopy.

    PubMed

    Fidler, Andrew F; Singh, Ved P; Long, Phillip D; Dahlberg, Peter D; Engel, Gregory S

    2014-01-01

    Time-resolved ultrafast optical probes of chiral dynamics provide a new window allowing us to explore how interactions with such structured environments drive electronic dynamics. Incorporating optical activity into time-resolved spectroscopies has proven challenging because of the small signal and large achiral background. Here we demonstrate that two-dimensional electronic spectroscopy can be adapted to detect chiral signals and that these signals reveal how excitations delocalize and contract following excitation. We dynamically probe the evolution of chiral electronic structure in the light-harvesting complex 2 of purple bacteria following photoexcitation by creating a chiral two-dimensional mapping. The dynamics of the chiral two-dimensional signal directly reports on changes in the degree of delocalization of the excitonic states following photoexcitation. The mechanism of energy transfer in this system may enhance transfer probability because of the coherent coupling among chromophores while suppressing fluorescence that arises from populating delocalized states. This generally applicable spectroscopy will provide an incisive tool to probe ultrafast transient molecular fluctuations that are obscured in non-chiral experiments. PMID:24504144

  17. Electron- and Photon-Induced Fragmentation Dynamics in Simple Atoms and Molecules

    NASA Astrophysics Data System (ADS)

    Rescigno, Thomas

    2008-10-01

    Advanced imaging techniques such as COLTRIMS, coupled with high-resolution electron- and new X-ray photon sources, have triggered a new class of kinematically complete experiments that probe the details of electron- and nuclear dynamics in simple atoms and small molecules. The interpretation of these experiments presents a formidable challenge for contemporary theory, often involving fully differential cross section and excited-state reaction dynamics calculations that require precise, non-perturbative quantum mechanical methodology. I will illustrate this topic with several examples in which state-of-the-art ab initio theory can shed light on experiments which probe electron and/or nuclear fragmentation dynamics in simple systems. The examples will include sequential and non-sequential two-photon double ionization of helium, diffraction effects in high-energy photo-double ionization of H2, core-hole localization in molecular nitrogen, inner-valence shell fragmentation of carbon monoxide and electron-induced three-body breakup of water.

  18. Imaging of the dissociation dynamics of polyatomic molecules following low-energy electron resonant attachment

    NASA Astrophysics Data System (ADS)

    Belkacem, Ali

    2014-05-01

    There is a very large body of experimental work on dissociative electron attachment to molecules but the majority of that work is focused on the measurement of absolute total cross sections or energetic positions of the resonances. There is scarce information on the dynamics of electron attachment and the subsequent dissociation that often involves highly non-Born-Oppenheimer dynamics, funneling through conical intersections or intricate nuclear motion during the dissociation process. Through COLTRIMS detection techniques we investigate the electron attachment in a fixed-in-frame manner that yields direct information on the symmetries of the neutral and negatively charged resonant states. We will present a study that combines experimental data along with theoretical analysis of dissociative electron attachment to carbon dioxide, methanol and uracil. In these studies we demonstrated that an understanding of anion dissociation dynamics beyond simple one-dimensional models is crucial in interpreting the measured angular distributions. This work is supported by the Chemical Sciences Biosciences and Geosciences Division, Basic Energy Sciences, DOE.

  19. Electronic and quantum dynamical insight into the ultrafast proton transfer of 1-hydroxy-2-acetonaphthone

    SciTech Connect

    Ortiz-Sanchez, Juan Manuel; Gelabert, Ricard; Moreno, Miquel; Lluch, Jose M.

    2007-08-28

    The ultrafast proton-transfer dynamics of 1-hydroxy-2-acetonaphthone has been theoretically analyzed in the ground and first singlet excited electronic states by density functional theory calculations and quantum dynamics. The potential energies obtained in the ground electronic state reveal that the proton-transfer process does not lead to a stable keto tautomer unless the transfer of the hydrogen from the enol form is accompanied by an internal rotation of the newly formed O-H bond. Calculations in the first singlet excited electronic state point to a very low barrier for the formation of the keto tautomer. The analysis of the calculated frequencies of the two tautomers in the excited state unveils a coupling of the skeletal motions (low frequency modes) with the proton-transfer process, as it has been stated from time-resolved experiments. The electronic energies obtained by the time-dependent density functional theory formalism have been fitted to a monodimensional potential energy surface in order to perform an exact quantum dynamics study of the process. Our results show that the proton-transfer process is completed within 25.5 fs, in remarkable good agreement with experiments.

  20. Simulation of Nitroxide Electron Paramagnetic Resonance Spectra from Brownian Trajectories and Molecular Dynamics Simulations

    PubMed Central

    DeSensi, Susan C.; Rangel, David P.; Beth, Albert H.; Lybrand, Terry P.; Hustedt, Eric J.

    2008-01-01

    A simulated continuous wave electron paramagnetic resonance spectrum of a nitroxide spin label can be obtained from the Fourier transform of a free induction decay. It has been previously shown that the free induction decay can be calculated by solving the time-dependent stochastic Liouville equation for a set of Brownian trajectories defining the rotational dynamics of the label. In this work, a quaternion-based Monte Carlo algorithm has been developed to generate Brownian trajectories describing the global rotational diffusion of a spin-labeled protein. Also, molecular dynamics simulations of two spin-labeled mutants of T4 lysozyme, T4L F153R1, and T4L K65R1 have been used to generate trajectories describing the internal dynamics of the protein and the local dynamics of the spin-label side chain. Trajectories from the molecular dynamics simulations combined with trajectories describing the global rotational diffusion of the protein are used to account for all of the dynamics of a spin-labeled protein. Spectra calculated from these combined trajectories correspond well to the experimental spectra for the buried site T4L F153R1 and the helix surface site T4L K65R1. This work provides a framework to further explore the modeling of the dynamics of the spin-label side chain in the wide variety of labeling environments encountered in site-directed spin labeling studies. PMID:18234808

  1. Accelerated electronic structure-based molecular dynamics simulations of shock-induced chemistry

    NASA Astrophysics Data System (ADS)

    Cawkwell, Marc

    2015-06-01

    The initiation and progression of shock-induced chemistry in organic materials at moderate temperatures and pressures are slow on the time scales available to regular molecular dynamics simulations. Accessing the requisite time scales is particularly challenging if the interatomic bonding is modeled using accurate yet expensive methods based explicitly on electronic structure. We have combined fast, energy conserving extended Lagrangian Born-Oppenheimer molecular dynamics with the parallel replica accelerated molecular dynamics formalism to study the relatively sluggish shock-induced chemistry of benzene around 13-20 GPa. We model interatomic bonding in hydrocarbons using self-consistent tight binding theory with an accurate and transferable parameterization. Shock compression and its associated transient, non-equilibrium effects are captured explicitly by combining the universal liquid Hugoniot with a simple shrinking-cell boundary condition. A number of novel methods for improving the performance of reactive electronic structure-based molecular dynamics by adapting the self-consistent field procedure on-the-fly will also be discussed. The use of accelerated molecular dynamics has enabled us to follow the initial stages of the nucleation and growth of carbon clusters in benzene under thermodynamic conditions pertinent to experiments.

  2. Femtosecond time-resolved photoemission electron microscopy for spatiotemporal imaging of photogenerated carrier dynamics in semiconductors

    SciTech Connect

    Fukumoto, Keiki Yamada, Yuki; Matsuki, Takashi; Koshihara, Shin-ya; Onda, Ken; Mukuta, Tatsuhiko; Tanaka, Sei-ichi

    2014-08-15

    We constructed an instrument for time-resolved photoemission electron microscopy (TR-PEEM) utilizing femtosecond (fs) laser pulses to visualize the dynamics of photogenerated electrons in semiconductors on ultrasmall and ultrafast scales. The spatial distribution of the excited electrons and their relaxation and/or recombination processes were imaged by the proposed TR-PEEM method with a spatial resolution about 100 nm and an ultrafast temporal resolution defined by the cross-correlation of the fs laser pulses (240 fs). A direct observation of the dynamical behavior of electrons on higher resistivity samples, such as semiconductors, by TR-PEEM has still been facing difficulties because of space and/or sample charging effects originating from the high photon flux of the ultrashort pulsed laser utilized for the photoemission process. Here, a regenerative amplified fs laser with a widely tunable repetition rate has been utilized, and with careful optimization of laser parameters, such as fluence and repetition rate, and consideration for carrier lifetimes, the electron dynamics in semiconductors were visualized. For demonstrating our newly developed TR-PEEM method, the photogenerated carrier lifetimes around a nanoscale defect on a GaAs surface were observed. The obtained lifetimes were on a sub-picosecond time scale, which is much shorter than the lifetimes of carriers observed in the non-defective surrounding regions. Our findings are consistent with the fact that structural defects induce mid-gap states in the forbidden band, and that the electrons captured in these states promptly relax into the ground state.

  3. Electronic structure dynamics in a low bandgap polymer studied by time-resolved photoelectron spectroscopy.

    PubMed

    Cappel, Ute B; Plogmaker, Stefan; Terschlüsen, Joachim A; Leitner, Torsten; Johansson, Erik M J; Edvinsson, Tomas; Sandell, Anders; Karis, Olof; Siegbahn, Hans; Svensson, Svante; Mårtensson, Nils; Rensmo, Håkan; Söderström, Johan

    2016-08-01

    Means to measure the temporal evolution following a photo-excitation in conjugated polymers are a key for the understanding and optimization of their function in applications such as organic solar cells. In this paper we study the electronic structure dynamics by direct pump-probe measurements of the excited electrons in such materials. Specifically, we carried out a time-resolved photoelectron spectroscopy (TRPES) study of the polymer PCPDTBT by combining an extreme ultraviolet (XUV) high harmonic generation source with a time-of-flight spectrometer. After excitation to either the 1st excited state or to a higher excited state, we follow how the electronic structure develops and relaxes on the electron binding energy scale. Specifically, we follow a less than 50 fs relaxation of the higher exited state and a 10 times slower relaxation of the 1st excited state. We corroborate the results using DFT calculations. Our study demonstrates the power of TRPES for studying photo-excited electron energetics and dynamics of solar cell materials. PMID:27440450

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

    PubMed Central

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

    2014-01-01

    Magnetization manipulation is essential for basic research and applications. A fundamental question is, how fast can the magnetization be reversed in nanoscale magnetic storage media. When subject to an ultrafast laser pulse, the speed of the magnetization dynamics depends on the nature of the energy transfer pathway. The order of the spin system can be effectively influenced through spin-flip processes mediated by hot electrons. It has been predicted that as electrons drive spins into the regime close to almost total demagnetization, characterized by a loss of ferromagnetic correlations near criticality, a second slower demagnetization process takes place after the initial fast drop of magnetization. By studying FePt, we unravel the fundamental role of the electronic structure. As the ferromagnet Fe becomes more noble in the FePt compound, the electronic structure is changed and the density of states around the Fermi level is reduced, thereby driving the spin correlations into the limit of critical fluctuations. We demonstrate the impact of the electrons and the ferromagnetic interactions, which allows a general insight into the mechanisms of spin dynamics when the ferromagnetic state is highly excited, and identifies possible recording speed limits in heat-assisted magnetization reversal. PMID:24496221

  5. The electron-ion dynamics in ionization of lithium carbide molecule under femtosecond laser pulses

    NASA Astrophysics Data System (ADS)

    Zhang, Xiaoqin; Wang, Feng; Hong, Xuhai; Su, Wenyong; Gou, Bingcong; Chen, Huimin

    2016-08-01

    The electron-ion dynamics of the linear lithium carbide molecule under femtosecond laser pulses have been investigated in the framework of Ehrenfest molecular dynamics, in which valence electrons are treated quantum mechanically by time-dependent density functional theory (TDDFT) and ions are described classically. The on- and off-resonant multiphoton ionization processes have been induced by regulating laser frequency and laser intensity. The laser pulse with on-resonant frequency induces pronounced enhancement in electron ionization, bond length vibration, and energy absorption. Moreover, the coulomb explosion is preferred to occur in the on-resonant case, which is in qualitative agreement with previous theoretical investigations. The subtle relations between escaped electron number and absorbed photon number are well discussed with the increasing of laser intensity. Finally, the effect of self-interaction error is analyzed by comparing escaped electron number calculated with LDA and LDA-ADSIC. And the revTPSS-meta-GGA, a currently more accurate nonempirical exchange-correlation energy functional from a point of static density functional theory, is introduced to display its capability for the description of ionization process within nonlinear and the nonperturbative regime of isolated systems.

  6. Atomic-scale dynamics of triangular hole growth in monolayer hexagonal boron nitride under electron irradiation

    NASA Astrophysics Data System (ADS)

    Ryu, Gyeong Hee; Park, Hyo Ju; Ryou, Junga; Park, Jinwoo; Lee, Jongyeong; Kim, Gwangwoo; Shin, Hyeon Suk; Bielawski, Christopher W.; Ruoff, Rodney S.; Hong, Suklyun; Lee, Zonghoon

    2015-06-01

    The production of holes by electron beam irradiation in hexagonal boron nitride (hBN), which has a lattice similar to that of graphene, is monitored over time using atomic resolution transmission electron microscopy. The holes appear to be initiated by the formation of a vacancy of boron and grow in a manner that retains an overall triangular shape. The hole growth process involves the formation of single chains of B and N atoms and is accompanied by the ejection of atoms and bundles of atoms along the hole edges, as well as atom migration. These observations are compared to density functional theory calculations and molecular dynamics simulations.The production of holes by electron beam irradiation in hexagonal boron nitride (hBN), which has a lattice similar to that of graphene, is monitored over time using atomic resolution transmission electron microscopy. The holes appear to be initiated by the formation of a vacancy of boron and grow in a manner that retains an overall triangular shape. The hole growth process involves the formation of single chains of B and N atoms and is accompanied by the ejection of atoms and bundles of atoms along the hole edges, as well as atom migration. These observations are compared to density functional theory calculations and molecular dynamics simulations. Electronic supplementary information (ESI) available. See DOI: 10.1039/c5nr01473e

  7. Effects of intense femtosecond pumping on ultrafast electronic-vibrational dynamics in molecular systems with relaxation

    NASA Astrophysics Data System (ADS)

    Egorova, Dassia; Gelin, Maxim F.; Thoss, Michael; Wang, Haobin; Domcke, Wolfgang

    2008-12-01

    We investigate the influence of strong femtosecond optical pulses on the ultrafast dynamics of molecular systems. The study is based on a series of generic molecular models of increasing complexity, which incorporate multiple and mutually coupled electronic states, electronic-vibrational interaction, and vibrational relaxation. The influence of vibrational relaxation is treated using multilevel Redfield theory. Comparisons to benchmark results of the multilayer multiconfiguration time-dependent Hartree (ML-MCTDH) method demonstrate the validity of the field-free implementation of Redfield theory employed in this work for weak system-bath interaction. The calculated electronic population and vibrational wave-packet dynamics demonstrate the intricate interplay of strong-field excitation, laser-induced Rabi oscillations, electronic interaction, vibronic coupling, and dissipation. In particular, we show that the interaction with a strong laser pulse may result in pronounced coherent vibrational motion in a dissipative system, even for laser pulses that are longer than the vibrational period. Furthermore, vibrational relaxation in combination with strong laser pulse excitation can lead to revivals of the electronic population after the excitation pulse is over.

  8. Dynamic secondary electron emission characteristics of polymers in negative charging process

    NASA Astrophysics Data System (ADS)

    Weng, Ming; Hu, Tian-Cun; Zhang, Na; Cao, Meng

    2016-04-01

    We studied the dynamic secondary electron emission (SEE) characteristics of a polyimide sample in negative charging process under electron bombardment. The time evolution of secondary electron yield (SEY) has been measured with a pulsed electron gun. The dynamic SEY, as well as the surface potential have been analyzed using a capacitance model. The shift in surface potential caused by the negative charge accumulation on the sample reduces the landing energy of the primary electrons (PEs), which in turn alters the SEY. The charging process tends to be stable when the landing energy of PEs reaches the secondary crossover energy where the corresponding SEY is 1. The surface potential has an approximately negative exponential relationship with the irradiation time. The total accumulated charge at the stable state is found to be proportional to the product of the sample capacitance and the difference between initial incident energy and the secondary crossover energy. The time constant of the exponential function is proportional to the ratio of final accumulated charge to the incident current.

  9. Nonadiabatic Dynamics May Be Probed through Electronic Coherence in Time-Resolved Photoelectron Spectroscopy.

    PubMed

    Bennett, Kochise; Kowalewski, Markus; Mukamel, Shaul

    2016-02-01

    We present a hierarchy of Fermi golden rules (FGRs) that incorporate strongly coupled electronic/nuclear dynamics in time-resolved photoelectron spectroscopy (TRPES) signals at different levels of theory. Expansion in the joint electronic and nuclear eigenbasis yields the numerically most challenging exact FGR (eFGR). The quasistatic Fermi Golden Rule (qsFGR) neglects nuclear motion during the photoionization process but takes into account electronic coherences as well as populations initially present in the pumped matter as well as those generated internally by coupling between electronic surfaces. The standard semiclassical Fermi Golden Rule (scFGR) neglects the electronic coherences and the nuclear kinetic energy during the ionizing pulse altogether, yielding the classical Condon approximation. The coherence contributions depend on the phase-profile of the ionizing field, allowing coherent control of TRPES signals. The photoelectron spectrum from model systems is simulated using these three levels of theory. The eFGR and the qsFGR show temporal oscillations originating from the electronic or vibrational coherences generated as the nuclear wave packet traverses a conical intersection. These oscillations, which are missed by the scFGR, directly reveal the time-evolving splitting between electronic states of the neutral molecule in the curve-crossing regime.

  10. Electron Transfer-Based Single Molecule Fluorescence as a Probe for Nano-Environment Dynamics

    PubMed Central

    Chen, Ruiyun; Wu, Ruixiang; Zhang, Guofeng; Gao, Yan; Xiao, Liantuan; Jia, Suotang

    2014-01-01

    Electron transfer (ET) is one of the most important elementary processes that takes place in fundamental aspects of biology, chemistry, and physics. In this review, we discuss recent research on single molecule probes based on ET. We review some applications, including the dynamics of glass-forming systems, surface binding events, interfacial ET on semiconductors, and the external field-induced dynamics of polymers. All these examples show that the ET-induced changes of fluorescence trajectory and lifetime of single molecules can be used to sensitively probe the surrounding nano-environments. PMID:24496314

  11. Dynamic polarizabilities of two-electron atoms, with rigorous upper and lower bounds

    NASA Technical Reports Server (NTRS)

    Glover, R. M.; Weinhold, F.

    1976-01-01

    Methods are described for calculating rigorous upper and lower bounds to dynamic dipole polarizabilities for frequencies up to and beyond the first excitation threshold, even when (as usual) the field-free problem cannot be solved exactly. These methods were employed to calculate rigorous bounds to the dynamic polarizabilities of the two-electron atoms H(-), He, and Li(+), using well correlated trial wavefunctions up to 135 terms in length. The majority of previous theoretical and experimental results for these atoms can thereby be ruled out, including the highly precise Starkschall-Gordon values, which had heretofore appeared to be the most accurate available.

  12. Phase space analysis for dynamics of three vortices of pure electron plasma trapped with Penning trap

    SciTech Connect

    Sanpei, Akio; Soga, Yukihiro; Ito, Kiyokazu; Himura, Haruhiko

    2015-06-29

    A trilinear phase space analysis is applied for dynamics of three electron clumps confined with a Penning-Malmberg trap. We show that the Aref’s concept of phase space describe the observed features of the dynamics of three point vortices qualitatively. In vacuum, phase point P moves to physical region boundary in phase space, i.e. triangular configuration cannot be kept. With the addition of a low level background vorticity distribution (BGVD), the excursion of the clumps is reduced and the distance between P and stable point does not extend in the phase space.

  13. Nano-electron beam induced current and hole charge dynamics through uncapped Ge nanocrystals

    NASA Astrophysics Data System (ADS)

    Marchand, A.; El Hdiy, A.; Troyon, M.; Amiard, G.; Ronda, A.; Berbezier, I.

    2012-04-01

    Dynamics of hole storage in spherical Ge nanocrystals (NCs) formed by a two step dewetting/nucleation process on an oxide layer grown on an n-doped <001> silicon substrate is studied using a nano-electron beam induced current technique. Carrier generation is produced by an electron beam irradiation. The generated current is collected by an atomic force microscope—tip in contact mode at a fixed position away from the beam spot of about 0.5 µm. This distance represents the effective diffusion length of holes. The time constants of holes charging are determined and the effect of the NC size is underlined.

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

    NASA Astrophysics Data System (ADS)

    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.

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

    PubMed

    Andresen, G B; Ashkezari, M D; Baquero-Ruiz, M; Bertsche, W; Bowe, P D; Butler, E; Cesar, C L; Chapman, S; Charlton, M; Deller, A; Eriksson, S; Fajans, J; Friesen, T; Fujiwara, M C; Gill, D R; Gutierrez, A; Hangst, J S; Hardy, W N; Hayden, M E; Humphries, A J; Hydomako, R; Jonsell, S; Madsen, N; Menary, S; Nolan, P; Olin, A; Povilus, A; Pusa, P; Robicheaux, F; Sarid, E; Silveira, D M; So, C; Storey, J W; Thompson, R I; van der Werf, D P; Wurtele, J S; Yamazaki, Y

    2011-04-01

    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.

  16. Centrifugal Separation and Equilibration Dynamics in an Electron-Antiproton Plasma

    SciTech Connect

    Andresen, G. B.; Bowe, P. D.; Hangst, J. S.; Ashkezari, M. D.; Hayden, M. E.; Baquero-Ruiz, M.; Chapman, S.; Fajans, J.; Povilus, A.; So, C.; Bertsche, W.; Butler, E.; Charlton, M.; Deller, A.; Eriksson, S.; Humphries, A. J.; Madsen, N.; Werf, D. P. van der; Cesar, C. L.; Friesen, T.

    2011-04-08

    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.

  17. Dynamical Characteristics of Rydberg Electrons Released by a Weak Electric Field.

    PubMed

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

    2016-04-01

    The dynamics of ultraslow 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 photoabsorption 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 1 meV. PMID:27104706

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

    DOE PAGESBeta

    Diesen, Elias; Saalmann, Ulf; Richter, Martin; Kunitski, Maksim; Dorner, Reinhard; Rost, Jan M.

    2016-04-08

    This paper discuss the dynamics of ultraslow electrons in the combined potential of an ionic core and a static electric field. With state-of-the-art detection it is possible to create such electrons through strong intense-field photoabsorption 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 1 meV.

  19. Dynamical Characteristics of Rydberg Electrons Released by a Weak Electric Field

    NASA Astrophysics Data System (ADS)

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

    2016-04-01

    The dynamics of ultraslow 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 photoabsorption 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 1 meV.

  20. Dynamics of nonequilibrium electrons on neutral center states of interstitial magnesium donors in silicon

    NASA Astrophysics Data System (ADS)

    Pavlov, S. G.; Deßmann, N.; Pohl, A.; Shuman, V. B.; Portsel, L. M.; Lodygin, A. N.; Astrov, Yu. A.; Winnerl, S.; Schneider, H.; Stavrias, N.; van der Meer, A. F. G.; Tsyplenkov, V. V.; Kovalevsky, K. A.; Zhukavin, R. Kh.; Shastin, V. N.; Abrosimov, N. V.; Hübers, H.-W.

    2016-08-01

    Subnanosecond dynamics of optically excited electrons bound to excited states of neutral magnesium donor centers in silicon has been investigated. Lifetimes of nonequilibrium electrons have been derived from the decay of the differential transmission at photon energies matching the intracenter and the impurity-to-conduction band transitions. In contrast to hydrogenlike shallow donors in silicon, significantly longer lifetimes have been observed. This indicates weaker two-phonon and off-resonant interactions dominate the relaxation processes in contrast to the single-intervalley-phonon-assisted impurity-phonon interactions in the case of shallow donors in silicon.

  1. Excited-state dynamics of oxazole: A combined electronic structure calculations and dynamic simulations study

    NASA Astrophysics Data System (ADS)

    Cao, Jun; Xie, Zhi-Zhong; Yu, Xiaodong

    2016-08-01

    In the present work, the combined electronic structure calculations and surface hopping simulations have been performed to investigate the excited-state decay of the parent oxazole in the gas phase. Our calculations show that the S2 state decay of oxazole is an ultrafast process characterized by the ring-opening and ring-closure of the five-membered oxazole ring, in which the triplet contribution is minor. The ring-opening involves the Osbnd C bond cleavage affording the nitrile ylide and airine intermediates, while the ring-closure gives rise to a bicyclic species through a 2sbnd 5 bond formation. The azirine and bicyclic intermediates in the S0 state are very likely involved in the phototranspositions of oxazoles. This is different from the previous mechanism in which these intermediates in the T1 state have been proposed for these phototranspositions.

  2. Quantum dynamics of electronic transitions with Gauss-Hermite wave packets

    NASA Astrophysics Data System (ADS)

    Borrelli, Raffaele; Peluso, Andrea

    2016-03-01

    A new methodology based on the superposition of time-dependent Gauss-Hermite wave packets is developed to describe 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 function parameters are obtained by employing the Dirac-Frenkel time-dependent variational principle. The methodology is applied to study the quantum dynamical behaviour of model systems with two interacting electronic states characterized by a relatively large reorganization energy and a range of energy biases. The favourable scaling properties make it a promising tool for the study of the dynamics of chemico-physical processes in molecular systems.

  3. Hole Surface Trapping Dynamics Directly Monitored by Electron Spin Manipulation in CdS Nanocrystals.

    PubMed

    Li, Xiao; Feng, Donghai; Tong, Haifang; Jia, Tianqing; Deng, Li; Sun, Zhenrong; Xu, Zhizhan

    2014-12-18

    A new detection technique, pump-spin orientation-probe ultrafast spectroscopy, is developed to study the hole trapping dynamics in colloidal CdS nanocrystals. The hole surface trapping process spatially separates the electron-hole pairs excited by the pump pulse, leaves the core negatively charged, and thus enhances the electron spin signal generated by the orientation pulse. The spin enhancement transients as a function of the pump-orientation delay reveal a fast and a slow hole trapping process with respective time constants of sub-10 ps and sub-100 ps, orders of magnitude faster than that of carrier recombination. The power dependence of hole trapping dynamics elucidates the saturation process and relative number of traps, and suggests that there are three subpopulations of nanoparticles related to hole surface trapping, one with the fast trapping pathway only, another with the slow trapping pathway only, and the third with both pathways together. PMID:26273979

  4. Carbon Nanotube Based Molecular Electronics and Motors: A View from Classical and Quantum Dynamics Simulations

    NASA Technical Reports Server (NTRS)

    Srivastava, Deepak; Saini, Subhash (Technical Monitor)

    1998-01-01

    The tubular forms of fullerenes popularly known as carbon nanotubes are experimentally produced as single-, multiwall, and rope configurations. The nanotubes and nanoropes have shown to exhibit unusual mechanical and electronic properties. The single wall nanotubes exhibit both semiconducting and metallic behavior. In short undefected lengths they are the known strongest fibers which are unbreakable even when bent in half. Grown in ropes their tensile strength is approximately 100 times greater than steel at only one sixth the weight. Employing large scale classical and quantum molecular dynamics simulations we will explore the use of carbon nanotubes and carbon nanotube junctions in 2-, 3-, and 4-point molecular electronic device components, dynamic strength characterization for compressive, bending and torsional strains, and chemical functionalization for possible use in a nanoscale molecular motor. The above is an unclassified material produced for non-competitive basic research in the nanotechnology area.

  5. Unified dynamics of electrons and photons via Zitterbewegung and spin-orbit interaction

    NASA Astrophysics Data System (ADS)

    Leary, C. C.; Smith, Karl H.

    2014-02-01

    We show that when an electron or photon propagates in a cylindrically symmetric waveguide, it experiences both a Zitterbewegung effect and a spin-orbit interaction leading to identical propagation dynamics for both particles. Applying a unified perturbative approach to both particles simultaneously, we find that to first order in perturbation theory, their Hamiltonians each contain identical Darwin (Zitterbewegung) and spin-orbit terms, resulting in the unification of their dynamics. The presence of the Zitterbewegung effect may be interpreted physically as the delocalization of the electron on the scale of its Compton wavelength, or the delocalization of the photon on the scale of its wavelength in the waveguide. The presence of the spin-orbit interaction leads to the prediction of several rotational effects: the spatial or time evolution of either particle's spin or polarization vector is controlled by the sign of its orbital angular momentum quantum number or, conversely, its spatial wave function is controlled by its spin angular momentum.

  6. Quantum dynamics of electronic transitions with Gauss-Hermite wave packets.

    PubMed

    Borrelli, Raffaele; Peluso, Andrea

    2016-03-21

    A new methodology based on the superposition of time-dependent Gauss-Hermite wave packets is developed to describe 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 function parameters are obtained by employing the Dirac-Frenkel time-dependent variational principle. The methodology is applied to study the quantum dynamical behaviour of model systems with two interacting electronic states characterized by a relatively large reorganization energy and a range of energy biases. The favourable scaling properties make it a promising tool for the study of the dynamics of chemico-physical processes in molecular systems. PMID:27004857

  7. Dynamical correlation effects on pair-correlation functions of spin polarized two-dimensional electron gas

    NASA Astrophysics Data System (ADS)

    Kumar, Krishan; Garg, Vinayak; Moudgil, R. K.

    2013-06-01

    We report a theoretical study on the spin-resolved pair-correlation functions gσσ'(r) of a two-dimensional electron gas having arbitrary spin polarization ζ by including the dynamics of exchange-correlations within the dynamical self-consistent mean-field theory of Hasegawa and Shimizu. The calculated g↑↑(r), g↓↓(r) and g↑↓(r) exhibit a nice agreement with the recent quantum Monte Carlo simulation data of Gori-Giorgi et al. However, the agreement for the minority spin correlation function g↓↓(r) decreases with increase in ζ and/or decrease in electron density. Nevertheless, the spin-summed correlation function remains close to the simulation data.

  8. Electron spin dynamics and spin-lattice relaxation of trityl radicals in frozen solutions.

    PubMed

    Chen, Hanjiao; Maryasov, Alexander G; Rogozhnikova, Olga Yu; Trukhin, Dmitry V; Tormyshev, Victor M; Bowman, Michael K

    2016-09-28

    Electron spin-lattice relaxation of two trityl radicals, d24-OX063 and Finland trityl, were studied under conditions relevant to their use in dissolution dynamic nuclear polarization (DNP). The dependence of relaxation kinetics on temperature up to 100 K and on concentration up to 60 mM was obtained at X- and W-bands (0.35 and 3.5 Tesla, respectively). The relaxation is quite similar at both bands and for both trityl radicals. At concentrations typical for DNP, relaxation is mediated by excitation transfer and spin-diffusion to fast-relaxing centers identified as triads of trityl radicals that spontaneously form in the frozen samples. These centers relax by an Orbach-Aminov mechanism and determine the relaxation, saturation and electron spin dynamics during DNP. PMID:27560644

  9. Electron ionization dynamics of N2 and O2 molecules: Velocity-map imaging

    NASA Astrophysics Data System (ADS)

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

    2015-02-01

    This paper reports a crossed-beam velocity-map imaging study into the electron ionization dynamics of jet-cooled N2 and O2 molecules at electron collision energies from 35 to 100 eV. The use of velocity-map imaging detection provides insight into the detailed ionization dynamics through the dimension of the product ion kinetic energy associated with impulsive dissociation. In particular, "mesoscopic" cross sections corresponding to ionization from manifolds of energetically close states converging to the same dissociation asymptote are reported for a number of single-ionization channels. In addition, a range of double-ionization cross sections have been characterized, including those yielding X2 2 + dications. These are found to be in excellent agreement with other cross sections determined in coincidence measurements. This agreement supports a meaningful and accurate determination of the single-ionization channels.

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

    PubMed

    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. PMID:27523194

  11. Strain dependent electron spin dynamics in bulk cubic GaN

    SciTech Connect

    Schaefer, A.; Buß, J. H.; Hägele, D.; Rudolph, J.; Schupp, T.; Zado, A.; As, D. J.

    2015-03-07

    The electron spin dynamics under variable uniaxial strain is investigated in bulk cubic GaN by time-resolved magneto-optical Kerr-rotation spectroscopy. Spin relaxation is found to be approximately independent of the applied strain, in complete agreement with estimates for Dyakonov-Perel spin relaxation. Our findings clearly exclude strain-induced relaxation as an effective mechanism for spin relaxation in cubic GaN.

  12. Strain dependent electron spin dynamics in bulk cubic GaN

    NASA Astrophysics Data System (ADS)

    Schaefer, A.; Buß, J. H.; Schupp, T.; Zado, A.; As, D. J.; Hägele, D.; Rudolph, J.

    2015-03-01

    The electron spin dynamics under variable uniaxial strain is investigated in bulk cubic GaN by time-resolved magneto-optical Kerr-rotation spectroscopy. Spin relaxation is found to be approximately independent of the applied strain, in complete agreement with estimates for Dyakonov-Perel spin relaxation. Our findings clearly exclude strain-induced relaxation as an effective mechanism for spin relaxation in cubic GaN.

  13. Dynamical resonant electron capture in atom surface collisions: H- formation in H-Al(111) collisions

    NASA Astrophysics Data System (ADS)

    Borisov, A. G.; Teillet-Billy, D.; Gauyacq, J. P.

    1992-05-01

    The formation of H- ion by grazing-angle collisions of hydrogen on an Al(111) surface is investigated with the newly developed coupled angular mode method. The capture process involves a dynamical resonant process induced by the collision velocity. All the resonance properties of the H- level in front of an Al(111) surface are determined: position, width, and angular distribution of ejected electrons. The results are shown to account for the recent observations on H- formation by Wyputta, Zimny, and Winter.

  14. Dissipative electron transfer dynamics in mixed valence dimers: Microscopic approach to the solid state problem

    NASA Astrophysics Data System (ADS)

    Palii, Andrew; Bosch-Serrano, Cristian; Clemente-Juan, Juan Modesto; Coronado, Eugenio; Tsukerblat, Boris

    2013-07-01

    We propose a microscopic analytical approach to the description of the low-temperature dissipative intracluster electron transfer dynamics in centrosymmetric one-electron mixed-valence (MV) dimers. The dissipative system (bath) is supposed to consist of the acoustic phonons of the crystal surrounding that are coupled to the delocalized electron(s) of a MV dimer. Although the concept of the bath is the spin-boson model is more generic, the present consideration is relevant, for example, to a MV bi-center impurity in an ionic crystal. The model allows us to develop an approximate microscopic approach within which the relaxation processes are explicitly taken into account without additional assumption regarding spectral function of the bath. It is assumed that initially the extra electron is localized on a certain center and then the time-dependent localization probability (averaged value of the electron dipole moment) is evaluated with the emphasis on the damping of the amplitude of the Rabi oscillations. The approach assumes the following conditions: (i) the vibrational spectrum of the crystal does not show the presence of local modes; (ii) the itinerant electron is weakly coupled to the long-waves acoustic phonons which is peculiar to fully delocalized Robin and Day class III MV systems; (iii) the Debye energy ℏωD exceeds the electronic resonance energy gap 2β (β is the electron transfer parameter). We have demonstrated that the dissipation in this case is super-ohmic with the low-frequency spectral function J(ω) ∝ ω5. The time dependences of the localization probabilities show nearly picosecond damped oscillations. The longitudinal relaxation time T1 has been shown to be two times shorter than the decoherence time T2 thus giving the upper bound for T2, T2 ≤ 2T1.

  15. Ultrafast electronic dynamics in Helium nanodroplets studied by femtosecond time-resolved EUV photoelectron imaging

    NASA Astrophysics Data System (ADS)

    Gessner, Oliver; Kornilov, Oleg; Wang, Chia; Leonard, Mathew; Healy, Andrew; Leone, Stephen; Neumark, Daniel

    2009-05-01

    Helium nanodroplets constitute a unique cryogenic matrix for the creation, isolation and spectroscopy of regular and exotic species, such as free radicals and molecules in high-spin states. The droplets readily pick up atoms and molecules but interact only very weakly with the respective dopants due to their superfluid nature. Despite the remarkable number of experimental and theoretical studies that have been performed on this new type of matter, neither the electronic structure nor the electron dynamics after EUV excitation are even remotely understood. We have performed the first femtosecond EUV-pump, IR-probe experiment to study the photoionization dynamics of pure Helium nanodroplets below the atomic Helium IP (24.6 eV) in real-time. Using Velocity-Map Imaging (VMI) photoelectron spectroscopy we were able to discern processes with associated timescales ranging from tens of femtoseconds to tens of picoseconds. The results will be discussed in the light of complementary energy-domain studies and theoretical models of the droplet's electronic and nuclear dynamics.

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

    NASA Astrophysics Data System (ADS)

    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.

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

    PubMed

    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. PMID:26750260

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

    PubMed

    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.

  19. Electron

    NASA Astrophysics Data System (ADS)

    Springford, Michael

    1997-03-01

    1. J. J. Thomson and the discovery of the electron A. B. P. Pippard; 2. The isolated electron W. N. Cottingham; 3. The relativistic electron D. I. Olive; 4. The electron glue B. L. Gyorffy; 5. The electron fluid P. Coleman; 6. The magnetic electron G. G. Lonzarich; 7. The paired electron A. J. Leggett; 8. The heavy electron M. Springford; 9. The coherent electron Y. Imry and M. Peskin; 10. The composite electron R. Nicholas; 11. The electron in the cosmos M. S. Longair.

  20. Electron

    NASA Astrophysics Data System (ADS)

    Springford, Michael

    2008-12-01

    1. J. J. Thomson and the discovery of the electron A. B. P. Pippard; 2. The isolated electron W. N. Cottingham; 3. The relativistic electron D. I. Olive; 4. The electron glue B. L. Gyorffy; 5. The electron fluid P. Coleman; 6. The magnetic electron G. G. Lonzarich; 7. The paired electron A. J. Leggett; 8. The heavy electron M. Springford; 9. The coherent electron Y. Imry and M. Peskin; 10. The composite electron R. Nicholas; 11. The electron in the cosmos M. S. Longair.

  1. Time-dependent mean field theory for quench dynamics in correlated electron systems.

    PubMed

    Schiró, Marco; Fabrizio, Michele

    2010-08-13

    A simple and very flexible variational approach to the out-of-equilibrium quantum dynamics in strongly correlated electron systems is introduced through a time-dependent Gutzwiller wave function. As an application, we study the simple case of a sudden change of the interaction in the fermionic Hubbard model and find at the mean-field level an extremely rich behavior. In particular, a dynamical transition between small and large quantum quench regimes is found to occur at half-filling, in accordance with the analysis of Eckstein, Phys. Rev. Lett. 103, 056403 (2009)10.1103/PhysRevLett.103.056403, obtained by dynamical mean-field theory, that turns into a crossover at any finite doping.

  2. Decoherence dynamics of coherent electronic excited states in the photosynthetic purple bacterium Rhodobacter sphaeroides.

    PubMed

    Liang, Xian-Ting; Zhang, Wei-Min; Zhuo, Yi-Zhong

    2010-01-01

    In this paper, we present a theoretical description to the quantum coherence and decoherence phenomena of energy transfer in photosynthesis observed in a recent experiment [Science 316, 1462 (2007)]. As a successive two-color laser pulses with selected frequencies cast on a sample of the photosynthetic purple bacterium Rb. sphaeroides two resonant excitations of electrons in chromophores can be generated. However, this effective two-level subsystem will interact with its protein environment and decoherence is inevitable. We describe this subsystem coupled with its environment as a dynamical spin-boson model. The non-Markovian decoherence dynamics is described using a quasiadiabatic propagator path integral (QUAPI) approach. With the photon-induced effective time-dependent level splitting energy and level flip coupling coefficient between the two excited states and the environment-induced non-Markovian decoherence dynamics, our theoretical result is in good agreement with the experimental data.

  3. Dynamics of the Rydberg electron in H*+D2-->D*+HD reactive collisions.

    PubMed

    Hayes, Michael Y; Skodje, Rex T

    2007-03-14

    Experimental crossed-beam studies carried out previously have indicated that the dynamics of the Rydberg-atom-molecule reaction H*+D2-->D*+HD are very similar to those of the corresponding ion-molecule reaction H++D2-->D++HD. The equivalence of the cross sections for these related systems would open up a new approach to the experimental study of ion-molecule reactions. However, a recent experimental and theoretical study has brought to light some important qualitative differences between the Rydberg-atom reaction and the ion-molecule reaction; in particular, the experimental cross section for the Rydberg-atom reaction exhibits a higher degree of forward-backward scattering asymmetry than predicted by a quasiclassical trajectory study of the ion-molecule reaction. In this paper, the authors consider the dynamics of the Rydberg-electron over the course of a reactive collision and the implications of these dynamics for the Rydberg-atom-molecule crossed-beam experiment. Using an approach based on perturbation theory, they estimate the attenuation of the experimental signal due to the Rydberg-electron dynamics as a function of the scattering angle. They show that at least part of the experimental asymmetry can be ascribed to this angle dependent attenuation. Their results offer general insight into the practical aspects of the experimental study of ion-molecule reactions by means of their Rydberg-atom counterparts. PMID:17362067

  4. Electron-phonon scattering dynamics in ferromagnetic metals and their influence on ultrafast demagnetization processes

    NASA Astrophysics Data System (ADS)

    Essert, Sven; Schneider, Hans Christian

    2011-12-01

    We theoretically investigate spin-dependent carrier dynamics due to the electron-phonon interaction after ultrafast optical excitation in ferromagnetic metals. We calculate the electron-phonon matrix elements including the spin-orbit interaction in the electronic wave functions and the interaction potential. Using the matrix elements in Boltzmann scattering integrals, the momentum-resolved carrier distributions are obtained by solving their equation of motion numerically. We find that the optical excitation with realistic laser intensities alone leads to a negligible magnetization change, and that the demagnetization due to electron-phonon interaction is mostly due to hole scattering. Importantly, the calculated demagnetization quenching due to this Elliot-Yafet-type depolarization mechanism is not large enough to explain the experimentally observed result. We argue that the ultrafast demagnetization of ferromagnets does not occur exclusively via an Elliott-Yafet type process, i.e., scattering in the presence of the spin-orbit interaction, but is influenced to a large degree by a dynamical change of the band structure, i.e., the exchange splitting.

  5. First-Principles Investigation of Electronic Excitation Dynamics in Water under Proton Irradiation

    NASA Astrophysics Data System (ADS)

    Reeves, Kyle; Kanai, Yosuke

    2015-03-01

    A predictive and quantitative understanding of electronic excitation dynamics in water under proton irradiation is of great importance in many technological areas ranging from utilizing proton beam therapy to preventing nuclear reactor damages. Despite its importance, an atomistic description of the excitation mechanism has yet to be fully understood. Identifying how a high-energy proton dissipates its kinetic energy into the electronic excitation is crucial for predicting atomistic damages, later resulting in the formation of different chemical species. In this work, we use our new, large-scale first-principles Ehrenfest dynamics method based on real-time time-dependent density functional theory to simulate the electronic response of bulk water to a fast-moving proton. In particular, we will discuss the topological nature of the electronic excitation as a function of the proton velocity. We will employ maximally-localized functions to bridge our quantitative findings from first-principles simulations to a conceptual understanding in the field of water radiolysis.

  6. Implementation of variable time step stochastic dynamics for electronically inelastic gas-surface collisions

    NASA Technical Reports Server (NTRS)

    Garrett, Bruce C.; Swaminathan, P. K.; Murthy, C. S.; Redmon, Michael J.

    1987-01-01

    A variable time step algorithm has been implemented for solving the stochastic equations of motion for gas-surface collisions. It has been tested for a simple model of electronically inelastic collisions with an insulator surface in which the phonon manifold acts as a heat bath and electronic states are localized. In addition to reproducing the accurate nuclear dynamics of the surface atoms, numerical calculations have shown the algorithm to yield accurate ensemble averages of physical observables such as electronic transition probabilities and total energy loss of the gas atom to the surface. This new algorithm offers a gain in efficieny of up to an order of magnitude compared to fixed time step integration.

  7. Probing Ultrafast Nuclear Dynamics in Halomethanes by Time-Resolved Electron and Ion Imaging

    NASA Astrophysics Data System (ADS)

    Ziaee, F.; Rudenko, A.; Rolles, D.; Savelyev, E.; Bomme, C.; Boll, R.; Manschwetus, B.; Erk, B.; Trippel, S.; Wiese, J.; Kuepper, J.; Amini, K.; Lee, J.; Brouard, M.; Brausse, F.; Rouzee, A.; Olshin, P.; Mereshchenko, A.; Lahl, J.; Johnsson, P.; Simon, M.; Marchenko, T.; Holland, D.; Underwood, J.

    2016-05-01

    Femtosecond pump-probe experiments provide opportunities to investigate photochemical reaction dynamics and the resulting changes in molecular structure in detail. Here, we present a study of the UV-induced photodissociation of gas-phase halomethane molecules (CH3 I, CH2 IBr, ...) in a pump-probe arrangement using two complementary probe schemes, either using a femtosecond near-infrared laser or the FLASH free-electron laser. We measured electrons and ions produced during the interaction using a double-sided velocity map imaging spectrometer equipped with a CCD camera for electron detection and with the Pixel Imaging Mass Spectrometry (PImMS) camera for ions, which can record the arrival time for up to four ions per pixel. This project is supported by the DOE, Office of Science, BES, Division of Chemical, Geological, and Biological Sciences.

  8. Wet cells and dry cells: In situ transmission electron microscopy of electrically-driven, dynamical processes

    NASA Astrophysics Data System (ADS)

    White, Edward Robert, IV

    Recent developments in nanofabrication techniques allow thin, wet systems to be imaged with high spatial and temporal resolution in the electron microscope. Coupling this ability with simultaneous, measured, electrical control, we cycle processes in liquid systems representing different electrochemical battery components. Dynamic processes imaged with these techniques, which represent a new state-of-the-art, include nanobubble collapse, dendrite growth, ion diffusion, and graphite intercalation. We also develop a sensitive system for measuring electron beam induced currents (EBIC) in the transmission electron microscope and apply it to graphene-MoS2 heterostructures. This new hybrid material has strong light-matter interactions, and the EBIC measurements map the minority carrier diffusion length, which we observe to decrease with increasing radiation damage. These results have direct implications for the function and service lifetime of solar cells based on molybdenum disulfide.

  9. Dynamics of electron bunches at the laser-plasma interaction in the bubble regime

    NASA Astrophysics Data System (ADS)

    Maslov, V. I.; Svystun, O. M.; Onishchenko, I. N.; Tkachenko, V. I.

    2016-09-01

    The multi-bunches self-injection, observed in laser-plasma accelerators in the bubble regime, affects the energy gain of electrons accelerated by laser wakefield. However, understanding of dynamics of the electron bunches formed at laser-plasma interaction may be challenging. We present here the results of fully relativistic electromagnetic particle-in-cell (PIC) simulation of laser wakefield acceleration driven by a short laser pulse in an underdense plasma. The trapping and acceleration of three witness electron bunches by the bubble-like structures were observed. It has been shown that with time the first two witness bunches turn into drivers and contribute to acceleration of the last witness bunch.

  10. Dynamical correlation effects on structure factor of spin-polarized two-dimensional electron gas

    SciTech Connect

    Singh, Gurvinder; Moudgil, R. K.; Kumar, Krishan; Garg, Vinayak

    2015-06-24

    We report a theoretical study on static density structure factor S(q) of a spin-polarized two-dimensional electron gas over a wide range of electron number density r{sub s}. The electron correlations are treated within the dynamical version of the self-consistent mean-field theory of Singwi, Tosi, Land, and Sjolander, the so-called qSTLS approach. The calculated S(q) exhibits almost perfect agreement with the quantum Monte Carlo simulation data at r{sub s}=1. However, the extent of agreement somewhat diminishes with increasing r{sub s}, particularly for q around 2k{sub F}. Seen in conjunction with the success of qSTLS theory in dealing with correlations in the unpolarized phase, our study suggests that the otherwise celebrated qSTLS theory is not that good in treating the like-spin correlations.

  11. Spin dynamics of hopping electrons in quantum wires: Algebraic decay and noise

    NASA Astrophysics Data System (ADS)

    Shumilin, A. V.; Sherman, E. Ya.; Glazov, M. M.

    2016-09-01

    We study theoretically the spin decoherence and intrinsic spin noise in semiconductor quantum wires caused by an interplay of electrons hopping between the localized states and the hyperfine interaction of electron and nuclear spins. At a sufficiently low density of localization sites the hopping rates have an exponentially broad distribution. It allows the description of the spin dynamics in terms of closely situated "pairs" of sites and single "reaching" states, from which the series of hops result in electrons localized inside a "pair." The developed analytical model and numerical simulations demonstrate disorder-dependent algebraic tails in the spin decay and power-law singularities features in the low-frequency part of the spin-noise spectrum.

  12. Self-Consistent 3D Modeling of Electron Cloud Dynamics and Beam Response

    SciTech Connect

    Furman, Miguel; Furman, M.A.; Celata, C.M.; Kireeff-Covo, M.; Sonnad, K.G.; Vay, J.-L.; Venturini, M.; Cohen, R.; Friedman, A.; Grote, D.; Molvik, A.; Stoltz, P.

    2007-04-02

    We present recent advances in the modeling of beam electron-cloud dynamics, including surface effects such as secondary electron emission, gas desorption, etc, and volumetric effects such as ionization of residual gas and charge-exchange reactions. Simulations for the HCX facility with the code WARP/POSINST will be described and their validity demonstrated by benchmarks against measurements. The code models a wide range of physical processes and uses a number of novel techniques, including a large-timestep electron mover that smoothly interpolates between direct orbit calculation and guiding-center drift equations, and a new computational technique, based on a Lorentz transformation to a moving frame, that allows the cost of a fully 3D simulation to be reduced to that of a quasi-static approximation.

  13. Semiclassical dynamics on multiple electronic surfaces - Three-dimensional treatment of reactive F + H2

    NASA Technical Reports Server (NTRS)

    Komornicki, A.; Morokuma, K.; George, T. F.

    1977-01-01

    The role of electron transitions in collisions is studied for the F + H2 reaction by combining quasi-classical Monte Carlo trajectories with a semiclassical decoupling approximation for the electron transitions. Attention is directed at the reaction of excited state F atoms reacting to form ground state products; the reactants are initiated in either of two spin-orbit states of the atom with the diatom in the ground vibrational state and the lowest four rotational states, at relative translational energies of 0.1, 0.2 and 0.3 eV. Even if the reactants are initiated on the excited state surface, the reactive cross sections (which are classically forbidden) are significant. The major dynamical effects of the excited state reaction are the flow of reactant electronic energy into product internal energy.

  14. Beam dynamics simulations in laser electron storage rings and optical stochastic cooling

    NASA Astrophysics Data System (ADS)

    Duru, Alper

    Laser-electron storage rings are potential compact X-ray sources. Longitudinal dynamics in laser-electron storage rings is studied including the effects of both laser interaction and synchrotron radiation. It is shown that the steady state energy spread can reach as high as a few percent. The main reason is the wide spread in the energy loss by electrons to laser photons. Optical stochastic cooling has been studied numerically. The effects of the finite bandwidth of the amplifier are mixing and signal distortion. Both are included in the simulations and the results are compared to theoretical results. It is shown that the beam can be cooled both in transverse and longitudinal phase phase spaces simultaneously.

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

    PubMed

    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. PMID:25860253

  16. Forecasting and Remote Sensing Relativistic Electron Dynamics from Low-Earth-Orbits

    NASA Astrophysics Data System (ADS)

    Chen, Yue; Reeves, Geoffrey; Tu, Weichao; Cunningham, Gregory; Henderson, Michael; Keltzing, Craig; Redmon, Rob

    2015-04-01

    Relativistic electrons trapped in the Earth’s outer radiation belt present a highly hazardous radiation environment for electronic hardware on board satellites and spacecraft. Thus developing a forecasting capability for MeV electron levels as well as understanding the physics have been deemed critical for both space research and industry communities. In this work, we first demonstrate that a high cross-energy, cross-pitch-angle and time-delayed coherence (with correlation values up to ~0.85) exists between the trapped MeV electrons and precipitating >~100s KeV electrons—observed respectively by Van Allen Probes and NOAA POES satellites in very different orbits—by conducting a survey on measurements from both high- and low-altitudes. Then, based upon the coherence, we further test the feasibility of using linear prediction filter models, driven by POES observations from low-Earth-orbits (LEOs), to predict the energization of MeV electrons during geomagnetic storms, as well as the evolving distributions of MeV electrons afterwards. These models predict MeV electron levels with high fidelity and have performance efficiency of ~0.74 (0.66) for 5-hour (1-day) forecasts. Last, after further investigating the high coherence by using pitch-angle resolved electron data from Van Allen Probes, we provide our explanations based upon case calculations from an analytic wave-particle resonance model. Results from this study unveil new knowledge of radiation belt dynamics, add new science significance to a long existing space infrastructure, and provide practical and powerful tools to the whole space community.

  17. ULTRAFAST ELECTRON SPIN DYNAMICS OF AS-GROWN Ga1-xMnxAs WITH APPROPRIATE Mn DOPING

    NASA Astrophysics Data System (ADS)

    Yue, Han

    2013-06-01

    The electron spin dynamics in the as-grown Ga1-xMnxAs films with appropriate Mn doping of x 2-5% is studied using time-resolved magneto-optical Kerr effect measurements. Due to the existence of Mn interstitials, the s-d exchange scattering is found to play an important role for the as-grown Ga1-xMnxAs, and compete with p-d exchange coupling to dominate the electron spin relaxation process. The contribution of electron-electron Coulomb scattering to the electron spin dynamics for the as-grown Ga1-x MnxAs appears to be as important as that of the annealed ones. Our findings are fundamentally important for better understanding the electron spin dynamics in Ga1-xMnxAs for its future spintronic applications.

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

    NASA Astrophysics Data System (ADS)

    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

  19. Dynamical electron diffraction simulation for non-orthogonal crystal system by a revised real space method.

    PubMed

    Lv, C L; Liu, Q B; Cai, C Y; Huang, J; Zhou, G W; Wang, Y G

    2015-01-01

    In the transmission electron microscopy, a revised real space (RRS) method has been confirmed to be a more accurate dynamical electron diffraction simulation method for low-energy electron diffraction than the conventional multislice method (CMS). However, the RRS method can be only used to calculate the dynamical electron diffraction of orthogonal crystal system. In this work, the expression of the RRS method for non-orthogonal crystal system is derived. By taking Na2 Ti3 O7 and Si as examples, the correctness of the derived RRS formula for non-orthogonal crystal system is confirmed by testing the coincidence of numerical results of both sides of Schrödinger equation; moreover, the difference between the RRS method and the CMS for non-orthogonal crystal system is compared at the accelerating voltage range from 40 to 10 kV. Our results show that the CMS method is almost the same as the RRS method for the accelerating voltage above 40 kV. However, when the accelerating voltage is further lowered to 20 kV or below, the CMS method introduces significant errors, not only for the higher-order Laue zone diffractions, but also for zero-order Laue zone. These indicate that the RRS method for non-orthogonal crystal system is necessary to be used for more accurate dynamical simulation when the accelerating voltage is low. Furthermore, the reason for the increase of differences between those diffraction patterns calculated by the RRS method and the CMS method with the decrease of the accelerating voltage is discussed. PMID:26461207

  20. Dynamical effects on vibrational and electronic spectra of hydroperoxyl radical water clusters

    NASA Astrophysics Data System (ADS)

    Iyengar, Srinivasan S.

    2005-08-01

    We have carried out ab initio molecular-dynamics studies on hydroperoxyl water clusters. Our studies are complemented by optimization, frequency, and excited-state calculations. The three main results we obtained are (a) the dynamically averaged energy gap between the highest-occupied molecular orbital and the lowest-unoccupied molecular orbital monotonically decreases as the number of water molecules is increased in a hydroperoxyl water cluster system, (b) the dynamical averaging of the potential-energy surface at finite temperature broadens the electronic excitation spectrum and changes the infrared spectrum in nontrivial ways, and (c) the structural analysis of our dynamics simulation indicates that the oxygen-oxygen distance in a solvated hydroperoxyl-water cluster is very similar to that found in protonated water clusters (Zundel: H5O2+) inspite of the fact that the latter possesses a positive charge and the hydroperoxyl-water cluster does not. Dynamical charge analysis and the weak acidity of HO2 are used to justify this result.

  1. Competition of static magnetic and dynamic photon forces in electronic transport through a quantum dot

    NASA Astrophysics Data System (ADS)

    Abdullah, Nzar Rauf; Tang, Chi-Shung; Manolescu, Andrei; Gudmundsson, Vidar

    2016-09-01

    We investigate theoretically the balance of the static magnetic and the dynamical photon forces in the electron transport through a quantum dot in a photon cavity with a single photon mode. The quantum dot system is connected to external leads and the total system is exposed to a static perpendicular magnetic field. We explore the transport characteristics through the system by tuning the ratio, \\hslash {ωγ}/\\hslash {ωc} , between the photon energy, \\hslash {ωγ} , and the cyclotron energy, \\hslash {ωc} . Enhancement in the electron transport with increasing electron-photon coupling is observed when \\hslash {ωγ}/\\hslash {ωc}>1 . In this case the photon field dominates and stretches the electron charge distribution in the quantum dot, extending it towards the contact area for the leads. Suppression in the electron transport is found when \\hslash {ωγ}/\\hslash {ωc}<1 , as the external magnetic field causes circular confinement of the charge density around the dot.

  2. Time-resolved energy dynamics after single electron injection into an interacting helical liquid

    NASA Astrophysics Data System (ADS)

    Calzona, Alessio; Acciai, Matteo; Carrega, Matteo; Cavaliere, Fabio; Sassetti, Maura

    2016-07-01

    The possibility of injecting a single electron into ballistic conductors is at the basis of the new field of electron quantum optics. Here, we consider a single electron injection into the helical edge channels of a topological insulator. Their counterpropagating nature and the unavoidable presence of electron-electron interactions dramatically affect the time evolution of the single wave packet. Modeling the injection process from a mesoscopic capacitor in the presence of nonlocal tunneling, we focus on the time-resolved charge and energy packet dynamics. Both quantities split up into counterpropagating contributions whose profiles are strongly affected by the interaction strength. In addition, stronger signatures are found for the injected energy, which is also affected by the finite width of the tunneling region, in contrast to what happens for the charge. Indeed, the energy flow can be controlled by tuning the injection parameters, and we demonstrate that, in the presence of nonlocal tunneling, it is possible to achieve a situation in which charge and energy flow in opposite directions.

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

    PubMed

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

    2012-02-01

    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.

  4. Watching the dynamics of electrons and atoms at work in solar energy conversion.

    PubMed

    Canton, S E; Zhang, X; Liu, Y; Zhang, J; Pápai, M; Corani, A; Smeigh, A L; Smolentsev, G; Attenkofer, K; Jennings, G; Kurtz, C A; Li, F; Harlang, T; Vithanage, D; Chabera, P; Bordage, A; Sun, L; Ott, S; Wärnmark, K; Sundström, V

    2015-01-01

    The photochemical reactions performed by transition metal complexes have been proposed as viable routes towards solar energy conversion and storage into other forms that can be conveniently used in our everyday applications. In order to develop efficient materials, it is necessary to identify, characterize and optimize the elementary steps of the entire process on the atomic scale. To this end, we have studied the photoinduced electronic and structural dynamics in two heterobimetallic ruthenium-cobalt dyads, which belong to the large family of donor-bridge-acceptor systems. Using a combination of ultrafast optical and X-ray absorption spectroscopies, we can clock the light-driven electron transfer processes with element and spin sensitivity. In addition, the changes in local structure around the two metal centers are monitored. These experiments show that the nature of the connecting bridge is decisive for controlling the forward and the backward electron transfer rates, a result supported by quantum chemistry calculations. More generally, this work illustrates how ultrafast optical and X-ray techniques can disentangle the influence of spin, electronic and nuclear factors on the intramolecular electron transfer process. Finally, some implications for further improving the design of bridged sensitizer-catalysts utilizing the presented methodology are outlined.

  5. Lattice dynamics and elastic properties of the 4f electron system: CeN

    NASA Astrophysics Data System (ADS)

    Kanchana, V.; Vaitheeswaran, G.; Zhang, Xinxin; Ma, Yanming; Svane, A.; Eriksson, O.

    2011-11-01

    The electronic structure, structural stability, and lattice dynamics of cerium mononitride are investigated using ab initio density-functional methods involving an effective potential derived from the generalized gradient approximation and without special treatment for the 4f states. The 4f states are hence allowed to hop from site to site, without an on-site Hubbard U, and contribute to the bonding, in a picture often referred to as itinerant. It is argued that this picture is appropriate for CeN at low temperatures, while the anomalous thermal expansion observed at elevated temperatures indicates entropy-driven localization of the Ce f electrons, similar to the behavior of elemental cerium. The elastic constants are predicted from the total energy variation of strained crystals and are found to be large, typical for nitrides. The phonon dispersions are calculated showing no soft modes, and the Grüneisen parameter behaves smoothly. The electronic structure is also calculated using the quasiparticle self-consistent GW approximation (where G denotes the Green's function and W denotes the screened interaction). The Fermi surface of CeN is dominated by large egg-shaped electron sheets centered on the X points, which stem from the p-f mixing around the X point. In contrast, assuming localized f electrons leads to a semimetallic picture with small band overlaps around X.

  6. Development of Multi-GeV Electron Radiography for Measurements of Fast, Dynamic Systems

    NASA Astrophysics Data System (ADS)

    Merrill, Frank; Danly, Christopher; Fabritius, Joseph; Mariam, Fesseha; Poulson, Daniel; Simpson, Raspberry; Walstrom, Peter; Wilde, Carl

    2015-06-01

    Charged particle radiography has been developed in the past decade to provide high-resolution, muti-frame flash radiography of dynamic systems. This development has focused on proton radiography utilizing 11 MeV to 50 GeV protons for a wide range of measurements. Recently, these techniques are being applied to the use of high energy electrons for applications at a future LANL MaRIE facility. At MaRIE Multi-GeV electrons will be used to diagnose small, quickly evolving systems, requiring resolution and frame rates beyond the capability of the existing 800 MeV proton radiography. The electron accelerator proposed for MaRIE will be capable of meeting the fast frame rate and resolution requirements for MaRIE. Because of the light mass of the electrons, bremsstrahlung processes become dominant in the electron interactions within the material being studied. Simulations have been performed to study these interactions, but measurements are required to fully understand the capabilities of this new measurement technique. A radiography system to make these measurements is being designed for measurements at the SLAC accelerator facility. We will present the plans for these measurements along with an estimate from simulations of the performance characteristics of a future capability.

  7. Modification of Defect Structures in Graphene by Electron Irradiation: Ab Initio Molecular Dynamics Simulations

    SciTech Connect

    Wang, Zhiguo; Zhou, Yungang; Bang, Junhyeok; Prange, Micah P.; Zhang, Shengbai; Gao, Fei

    2012-08-02

    Defects play an important role on the unique properties of the sp2-bonded materials, such as graphene. The creation and evolution of mono-vacancy, di-vacancy, Stone-Wales (SW) and grain boundaries (GBs) under irradiation in graphene are investigated using density functional theory and time-dependent density functional theory molecular dynamics simulations. It is of great interest to note that the patterns of these defects can be controlled through electron irradiation. The SW defects can be created by electron irradiation with energy of above the displacement threshold energy (Td, {approx}19 eV) and can be healed with an energy (14-18 eV) lower than Td. The transformation between four types of divacancies, V2(5-8-5), V2(555-777), V2(5555-6-7777), and V2(55-77) can be realized through bond rotation induced by electron irradiation. The migrations of divancancies, SW defects, and GBs can also be controlled by electron irradiation. Thus, electron irradiation can serve as an important tool to modify morphology in a controllable manner, and to tailor the physical properties of graphene.

  8. Dynamic nuclear polarization from current-induced electron spin polarization in n-InGaAs

    NASA Astrophysics Data System (ADS)

    Trowbridge, Christopher; Norman, Benjamin; Kato, Yuichiro; Awschalom, David; Sih, Vanessa

    2014-03-01

    Control of the nuclear spin system could prove useful for applications in spintronics or spin-based quantum computation for intermediate term data storage and for the suppression of electron spin dephasing resulting from hyperfine coupling. We investigate the role of nuclear spins in materials with electrically generated spin polarization. The electron spin polarization generated by electrical current in a non-magnetic semiconductor is transferred via dynamic nuclear polarization to the nuclei. The resulting nuclear field is interrogated using Larmor magnetometry. We measure the nuclear field as a function of applied magnetic field, current magnitude and direction, and temperature. An unexpected spatial asymmetry in saturated nuclear field is found. The direction of the nuclear polarization is determined by the directions of the electron spin alignment and external magnetic field, allowing electronic control over the sign of the nuclear alignment direction. Careful study of the nuclear field also enables characterization of the current-induced electron spin polarization in situations that are otherwise experimentally inaccessible. Work supported by AFOSR, NSF and ONR.

  9. Watching the dynamics of electrons and atoms at work in solar energy conversion

    SciTech Connect

    Canton, S. E.; Zhang, X.; Liu, Y.; Zhang, J.; Pápai, M.; Corani, A.; Smeigh, A. L.; Smolentsev, G.; Attenkofer, K.; Jennings, G.; Kurtz, C. A.; Li, F.; Harlang, T.; Vithanage, D.; Chabera, P.; Bordage, A.; Sun, L.; Ott, S.; Wärnmark, K.; Sundström, V.

    2015-07-06

    The photochemical reactions performed by transition metal complexes have been proposed as viable routes towards solar energy conversion and storage into other forms that can be conveniently used in our everyday applications. In order to develop efficient materials, it is necessary to identify, characterize and optimize the elementary steps of the entire process on the atomic scale. To this end, we have studied the photoinduced electronic and structural dynamics in two heterobimetallic ruthenium–cobalt dyads, which belong to the large family of donor–bridge–acceptor systems. Using a combination of ultrafast optical and X-ray absorption spectroscopies, we can clock the light-driven electron transfer processes with element and spin sensitivity. In addition, the changes in local structure around the two metal centers are monitored. These experiments show that the nature of the connecting bridge is decisive for controlling the forward and the backward electron transfer rates, a result supported by quantum chemistry calculations. More generally, this work illustrates how ultrafast optical and X-ray techniques can disentangle the influence of spin, electronic and nuclear factors on the intramolecular electron transfer process. Finally, some implications for further improving the design of bridged sensitizer-catalysts utilizing the presented methodology are outlined.

  10. Analysis of the H(2)(+) with H(2) reaction using electron nuclear dynamics

    NASA Astrophysics Data System (ADS)

    Oreiro, Juan J. G.

    The END formalism addresses the solution of the time- dependent Schrodinger equation, treating both electrons and nuclei simultaneously. It differs from the other traditional fully quantum mechanical time-dependent methods in that it does not require a potential energy surface (PES) to carry the nuclear motion. The interaction between electronic and nuclear motion is, therefore, obtained in a transparent way, not relying on PES gradients to obtain the coupling between electrons and nuclei. We analyze the H2+ + H2 reaction at energies below 4 eV using different approximations and basis sets. Other than the choice of initial conditions, form of wave function, and basis set, no constraints are imposed on the system evolution. The nuclei are treated in the classical limit, and the electronic part is described by a single determinantal, unrestricted wave function. We obtain properties, such as Mulliken populations, transition probabilities, and cross-sections, from the resulting trajectories. These results are compared with other current theoretical approaches, and with experimental values. The relevance of the electron- nuclear coupling is estimated by comparing the END trajectories with molecular dynamics calculations for selected initial conditions in different basis sets.

  11. Dynamics of neutralized electrons and the focusability of intenseion beams in HIF accelerating structures

    SciTech Connect

    Lifschitz, A.F.; Maynard, G.; Vay, J.-V.

    2005-01-18

    In most of the proposals for HIF reactors, beams propagate ballistically through the containment chamber. To get the required final radius ({approx} 3 mm), the charge of the beam must be neutralized to some extent. Several neutralization schemes are possible, as co-injection of negative-ions beams, inclusion of external sources of electrons, or it can be provided by electrons coming from ionization of the background gas. In this work, we study the role of the electron dynamic on the neutralization and final radius of the beam. This is done by performing fully-electromagnetic PIC simulations of the beam ballistic transport using the BPIC code[1]. In agreement with previous works we found that the evolution of an isolated beam is well described as a bidimensional adiabatic compression, and the beam neutralization degree and final radius can be estimated from the initial electron transversal temperature. When a background gas is present the evolution differs significantly from an adiabatic compression. Even for low gas densities, the continuous electrons flow coming from gas ionization limits efficiently the compressional heating, thus reducing the final radius. Aspects of beam neutralization by background gas ionization are discussed.

  12. Optoelectronic transport properties in amorphous/crystalline silicon solar cell heterojunctions measured by frequency-domain photocarrier radiometry: Multi-parameter measurement reliability and precision studies

    SciTech Connect

    Zhang, Y.; Melnikov, A.; Mandelis, A.; Halliop, B.; Kherani, N. P.; Zhu, R.

    2015-03-15

    A theoretical one-dimensional two-layer linear photocarrier radiometry (PCR) model including the presence of effective interface carrier traps was used to evaluate the transport parameters of p-type hydrogenated amorphous silicon (a-Si:H) and n-type crystalline silicon (c-Si) passivated by an intrinsic hydrogenated amorphous silicon (i-layer) nanolayer. Several crystalline Si heterojunction structures were examined to investigate the influence of the i-layer thickness and the doping concentration of the a-Si:H layer. The experimental data of a series of heterojunction structures with intrinsic thin layers were fitted to PCR theory to gain insight into the transport properties of these devices. The quantitative multi-parameter results were studied with regard to measurement reliability (uniqueness) and precision using two independent computational best-fit programs. The considerable influence on the transport properties of the entire structure of two key parameters that can limit the performance of amorphous thin film solar cells, namely, the doping concentration of the a-Si:H layer and the i-layer thickness was demonstrated. It was shown that PCR can be applied to the non-destructive characterization of a-Si:H/c-Si heterojunction solar cells yielding reliable measurements of the key parameters.

  13. Photocarrier radiometry for predicting the degradation of electrical parameters of monocrystalline silicon (c-Si) solar cell irradiated by 100 KeV proton beams

    NASA Astrophysics Data System (ADS)

    Song, P.; Liu, J. Y.; Yuan, H. M.; Oliullah, Md.; Wang, F.; Wang, Y.

    2016-09-01

    In this study, the monocrystalline silicon (c-Si) solar cell irradiated by 100 KeV proton beams at various fluences is investigated. A one-dimensional two-layer carrier density wave model has been developed to estimate the minority carrier lifetime of n-region and p-region of the non-irradiated c-Si solar cell by best fitting with the experimental photocarrier radiometry (PCR) signal (the amplitude and the phase). Furthermore, the lifetime is used to determine the initial defect density of the quasi-neutral region (QNR) of the solar cell to predict its I-V characteristics. The theoretically predicted short-circuit current density (Jsc), and open-circuit voltage (Voc) of the non-irradiated samples are in good agreement with experiment. Then a three-region defect distribution model for the c-Si solar cell irradiated by proton beams is carried out to describe the defect density distribution according to Monte Carlo simulation results and the initial defect density of the non-irradiated sample. Finally, we find that the electrical measurements of Jsc and Voc of the solar cells irradiated at different fluences using 100 KeV proton beams are consistent with the PCR predicting results.

  14. Real-Time Determination of Absolute Frequency in Continuous-Wave Terahertz Radiation with a Photocarrier Terahertz Frequency Comb Induced by an Unstabilized Femtosecond Laser

    NASA Astrophysics Data System (ADS)

    Minamikawa, Takeo; Hayashi, Kenta; Mizuguchi, Tatsuya; Hsieh, Yi-Da; Abdelsalam, Dahi Ghareab; Mizutani, Yasuhiro; Yamamoto, Hirotsugu; Iwata, Tetsuo; Yasui, Takeshi

    2016-05-01

    A practical method for the absolute frequency measurement of continuous-wave terahertz (CW-THz) radiation uses a photocarrier terahertz frequency comb (PC-THz comb) because of its ability to realize real-time, precise measurement without the need for cryogenic cooling. However, the requirement for precise stabilization of the repetition frequency ( f rep) and/or use of dual femtosecond lasers hinders its practical use. In this article, based on the fact that an equal interval between PC-THz comb modes is always maintained regardless of the fluctuation in f rep, the PC-THz comb induced by an unstabilized laser was used to determine the absolute frequency f THz of CW-THz radiation. Using an f rep-free-running PC-THz comb, the f THz of the frequency-fixed or frequency-fluctuated active frequency multiplier chain CW-THz source was determined at a measurement rate of 10 Hz with a relative accuracy of 8.2 × 10-13 and a relative precision of 8.8 × 10-12 to a rubidium frequency standard. Furthermore, f THz was correctly determined even when fluctuating over a range of 20 GHz. The proposed method enables the use of any commercial femtosecond laser for the absolute frequency measurement of CW-THz radiation.

  15. Optoelectronic transport properties in amorphous/crystalline silicon solar cell heterojunctions measured by frequency-domain photocarrier radiometry: multi-parameter measurement reliability and precision studies.

    PubMed

    Zhang, Y; Melnikov, A; Mandelis, A; Halliop, B; Kherani, N P; Zhu, R

    2015-03-01

    A theoretical one-dimensional two-layer linear photocarrier radiometry (PCR) model including the presence of effective interface carrier traps was used to evaluate the transport parameters of p-type hydrogenated amorphous silicon (a-Si:H) and n-type crystalline silicon (c-Si) passivated by an intrinsic hydrogenated amorphous silicon (i-layer) nanolayer. Several crystalline Si heterojunction structures were examined to investigate the influence of the i-layer thickness and the doping concentration of the a-Si:H layer. The experimental data of a series of heterojunction structures with intrinsic thin layers were fitted to PCR theory to gain insight into the transport properties of these devices. The quantitative multi-parameter results were studied with regard to measurement reliability (uniqueness) and precision using two independent computational best-fit programs. The considerable influence on the transport properties of the entire structure of two key parameters that can limit the performance of amorphous thin film solar cells, namely, the doping concentration of the a-Si:H layer and the i-layer thickness was demonstrated. It was shown that PCR can be applied to the non-destructive characterization of a-Si:H/c-Si heterojunction solar cells yielding reliable measurements of the key parameters. PMID:25832239

  16. Dynamic Photorefractive Memory and its Application for Opto-Electronic Neural Networks.

    NASA Astrophysics Data System (ADS)

    Sasaki, Hironori

    This dissertation describes the analysis of the photorefractive crystal dynamics and its application for opto-electronic neural network systems. The realization of the dynamic photorefractive memory is investigated in terms of the following aspects: fast memory update, uniform grating multiplexing schedules and the prevention of the partial erasure of existing gratings. The fast memory update is realized by the selective erasure process that superimposes a new grating on the original one with an appropriate phase shift. The dynamics of the selective erasure process is analyzed using the first-order photorefractive material equations and experimentally confirmed. The effects of beam coupling and fringe bending on the selective erasure dynamics are also analyzed by numerically solving a combination of coupled wave equations and the photorefractive material equation. Incremental recording technique is proposed as a uniform grating multiplexing schedule and compared with the conventional scheduled recording technique in terms of phase distribution in the presence of an external dc electric field, as well as the image gray scale dependence. The theoretical analysis and experimental results proved the superiority of the incremental recording technique over the scheduled recording. Novel recirculating information memory architecture is proposed and experimentally demonstrated to prevent partial degradation of the existing gratings by accessing the memory. Gratings are circulated through a memory feed back loop based on the incremental recording dynamics and demonstrate robust read/write/erase capabilities. The dynamic photorefractive memory is applied to opto-electronic neural network systems. Module architecture based on the page-oriented dynamic photorefractive memory is proposed. This module architecture can implement two complementary interconnection organizations, fan-in and fan-out. The module system scalability and the learning capabilities are theoretically

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

    PubMed Central

    Bainbridge, A. R.; Barlow Myers, C. W.; Bryan, W. A.

    2016-01-01

    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. PMID:27158637

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

    PubMed

    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. PMID:26322659

  19. Ultrafast dynamics in photo-induced correlated electronic states in ladder cuprates

    NASA Astrophysics Data System (ADS)

    Ishihara, Sumio; Hashimoto, Hiroshi

    2014-03-01

    Ultrafast photo-induced dynamics in correlated electron systems, in particular, photon irradiation effects in half filled Mott insulators have been studied intensively from theoretical and experimental sides, and photo-induced Mott insulator to metal transition has been observed. On the other side, in recent ultrafast pump-probe experiments in ladder cuprates away from half filling, photo-irradiation weakens initial metallic state. We study ultrafast dynamics in photo-induced states in a ladder system. Real time dynamics in a ladder-type Hubbard model are analyzed by the numerical exact diagonalization method. Optical conductivity spectra and density of states show that the initial metallic state is changed into a bad metallic state by photo irradiation, in contrast to the photo-doped effect in half-filled Mott insulators. Through the calculation of the carrier pair correlation functions, we find that coherent motion of carrier pairs in initial states are reduced by pump photon irradiation. We further simulate a double pulse irradiation. Our simulations as well as the experimental results suggest an optical control of pair coherence in correlated electron system.

  20. Dynamic Precision for Electron Repulsion Integral Evaluation on Graphical Processing Units (GPUs).

    PubMed

    Luehr, Nathan; Ufimtsev, Ivan S; Martínez, Todd J

    2011-04-12

    It has recently been demonstrated that novel streaming architectures found in consumer video gaming hardware such as graphical processing units (GPUs) are well-suited to a broad range of computations including electronic structure theory (quantum chemistry). Although recent GPUs have developed robust support for double precision arithmetic, they continue to provide 2-8× more hardware units for single precision. In order to maximize performance on GPU architectures, we present a technique of dynamically selecting double or single precision evaluation for electron repulsion integrals (ERIs) in Hartree-Fock and density functional self-consistent field (SCF) calculations. We show that precision error can be effectively controlled by evaluating only the largest integrals in double precision. By dynamically scaling the precision cutoff over the course of the SCF procedure, we arrive at a scheme that minimizes the number of double precision integral evaluations for any desired accuracy. This dynamic precision scheme is shown to be effective for an array of molecules ranging in size from 20 to nearly 2000 atoms. PMID:26606344

  1. Ultrafast Electron and Ion Dynamics in Strong-Field-Ionized Liquid Water

    NASA Astrophysics Data System (ADS)

    Loh, Zhi-Heng; Li, Jialin; Nie, Zhaogang; Zheng, Yi Ying; Dong, Shuo; Low, Pei Jiang

    2016-05-01

    The ionization of liquid water functions as the principal trigger for a myriad of phenomena that are relevant to radiation chemistry and biology. The earliest events that follow the ionization of water, however, remain relatively unknown. Here, femtosecond coherence spectroscopy is combined with polarization anisotropy measurements to elucidate the ultrafast electron and ion dynamics in ionized water. The results show that strong-field ionization of liquid water produces an aligned p electron distribution. Furthermore oscillations observed in the polarization anisotropy are suggestive of valence electron motion in the highly reactive H2 O+ radical cation, whose lifetime with respect to proton transfer is found to be 196 +/- 5 fs. Coherent intermolecular motions that signal initial solvent reorganization and subsequent long-lived ballistic proton transport that involves the H3 O+ end-product are also detected in the time domain. These results offer new insight into the elementary dynamics of ionized liquid water. This work is supported by the Ministry of Education (MOE2014-T2-2-052), A*Star (122-PSF-0011), and the Nanyang Assistant Professorship.

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

    SciTech Connect

    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 Ru{sup 2+}-Ru{sup 3+} 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.

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

    NASA Astrophysics Data System (ADS)

    Oberhofer, Harald; Blumberger, Jochen

    2009-08-01

    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.

  4. Dynamics of a laser-induced relativistic electron beam inside a solid dielectric

    NASA Astrophysics Data System (ADS)

    Sarkisov, G. S.; Ivanov, V. V.; Sentoku, Y.; Yates, K.; Leblanc, P.; Wiewior, P.; Kindel, J.; Bychenkov, V. Yu.; Jobe, D.; Spielman, R.

    2010-11-01

    Two-frame interferometry and shadowgraphy were used to investigate the dynamics of interaction of a powerful laser (UNR Leopard 2x10^18 W/cm^2, 0.5ps, 1057nm) with a glass target. The two-frame laser diagnostic reveals an ionization wave propagating inside the glass with half the speed of light. The interferometry delineates regions of ionization and excitation inside the glass target. A ``fountain effect'' of fast electrons inside the solid dielectric has been observed for the first time: a radially compact electron beam with sub-light speed fans out from the axis of the original beam, heading back to the target surface. Comparison with French (˜10^19W/cm^2) and UK (˜10^17W/cm^2) experiments implies a logarithmic dependence of the ionization depth with the laser intensity. Relativistic electron beam dynamics stemming from intense laser-glass interaction is a critical concern for the NIF ``fast ignition'' concept.

  5. Ultrafast Heme Dynamics of Ferric Cytochrome c in Different Environments: Electronic, Vibrational, and Conformational Relaxation.

    PubMed

    Karunakaran, Venugopal

    2015-12-21

    The excited-state dynamics of ferric cytochrome c (Cyt c), an important electron-transfer heme protein, in acidic to alkaline medium and in its unfolded form are investigated by using femtosecond pump-probe spectroscopy, exciting the heme and Tryptophan (Trp) to understand the electronic, vibrational, and conformational relaxation of the heme. At 390 nm excitation, the electronic relaxation of heme is found to be ≈150 fs at different pH values, increasing to 480 fs in the unfolded form. Multistep vibrational relaxation dynamics of the heme, including fast and slow processes, are observed at pH 7. However, in the unfolded form and at pH 2 and 11, fast phases of vibrational relaxation dominate, revealing the energy dissipation occurring through the covalent bond interaction between the heme and the nearest amino acids. A significant shortening of the excited-state lifetime of Trp is observed at various pH values at 280 nm excitation due to resonance energy transfer to the heme. The longer time constant (25 ps) observed in the unfolded form is attributed to a complete global conformational relaxation of Cyt c.

  6. Spin dynamics simulation of electron spin relaxation in Ni{sup 2+}(aq)

    SciTech Connect

    Rantaharju, Jyrki Mareš, Jiří Vaara, Juha

    2014-07-07

    The ability to quantitatively predict and analyze the rate of electron spin relaxation of open-shell systems is important for electron paramagnetic resonance and paramagnetic nuclear magnetic resonance spectroscopies. We present a combined molecular dynamics (MD), quantum chemistry (QC), and spin dynamics simulation method for calculating such spin relaxation rates. The method is based on the sampling of a MD trajectory by QC calculations, to produce instantaneous parameters of the spin Hamiltonian used, in turn, to numerically solve the Liouville-von Neumann equation for the time evolution of the spin density matrix. We demonstrate the approach by simulating the relaxation of electron spin in an aqueous solution of Ni{sup 2+} ion. The spin-lattice (T{sub 1}) and spin-spin (T{sub 2}) relaxation rates are extracted directly from the simulations of the time dependence of the longitudinal and transverse magnetization, respectively. Good agreement with the available, indirectly obtained experimental data is obtained by our method.

  7. Ultrafast electronic and vibrational dynamics in brominated aluminum corroles: Energy relaxation and triplet formation.

    PubMed

    Stensitzki, T; Yang, Y; Berg, A; Mahammed, A; Gross, Z; Heyne, K

    2016-07-01

    We combined femtosecond (fs) VIS pump-IR probe spectroscopy with fs VIS pump-supercontinuum probe spectroscopy to characterize the photoreaction of the hexacoordinated Al(tpfc-Br8)(py)2 in a comprehensive way. Upon fs excitation at ∼400 nm in the Soret band, the excitation energy relaxes with a time constant of (250 ± 80) fs to the S2 and S1 electronic excited states. This is evident from the rise time of the stimulated emission signal in the visible spectral range. On the same time scale, narrowing of broad infrared signals in the C=C stretching region around 1500 cm(-1) is observed. Energy redistribution processes are visible in the vibrational and electronic dynamics with time constants between ∼2 ps and ∼20 ps. Triplet formation is detected with a time constant of (95 ± 3) ps. This is tracked by the complete loss of stimulated emission. Electronic transition of the emerging triplet absorption band overlaps considerably with the singlet excited state absorption. In contrast, two well separated vibrational marker bands for triplet formation were identified at 1477 cm(-1) and at 1508 cm(-1). These marker bands allow a precise identification of triplet dynamics in corrole systems. PMID:27226980

  8. Ultrafast electronic and vibrational dynamics in brominated aluminum corroles: Energy relaxation and triplet formation

    PubMed Central

    Stensitzki, T.; Yang, Y.; Berg, A.; Mahammed, A.; Gross, Z.; Heyne, K.

    2016-01-01

    We combined femtosecond (fs) VIS pump–IR probe spectroscopy with fs VIS pump–supercontinuum probe spectroscopy to characterize the photoreaction of the hexacoordinated Al(tpfc-Br8)(py)2 in a comprehensive way. Upon fs excitation at ∼400 nm in the Soret band, the excitation energy relaxes with a time constant of (250 ± 80) fs to the S2 and S1 electronic excited states. This is evident from the rise time of the stimulated emission signal in the visible spectral range. On the same time scale, narrowing of broad infrared signals in the C=C stretching region around 1500 cm−1 is observed. Energy redistribution processes are visible in the vibrational and electronic dynamics with time constants between ∼2 ps and ∼20 ps. Triplet formation is detected with a time constant of (95 ± 3) ps. This is tracked by the complete loss of stimulated emission. Electronic transition of the emerging triplet absorption band overlaps considerably with the singlet excited state absorption. In contrast, two well separated vibrational marker bands for triplet formation were identified at 1477 cm−1 and at 1508 cm−1. These marker bands allow a precise identification of triplet dynamics in corrole systems. PMID:27226980

  9. Visualising many-body electron dynamics using one-body densities and orbitals

    NASA Astrophysics Data System (ADS)

    Dutoi, Anthony D.

    2014-01-01

    As experimental techniques begin to probe electronic motions in increasing detail, the need is arising for compact and informative visualisations of simulations of such processes. The inherent challenge is that a full many-electron wavefunction is a high-dimensional object, representing the complicated correlations of strongly repulsive bodies in a small molecular volume. A general procedure is needed to distill this to a smaller amount of information that does not rely on any specific level of approximation. The result should allow for easy and intuitive interpretation while drawing out nontrivial aspects of the underlying many-body dynamics, such as the complex phase information inherent of a nonstationary state. Current visualisation schemes based on physical observables or the qualitative information contained in simple wavefunctions, such as time-dependent configuration-interaction-singles (TD-CIS) and time-dependent self-consistent-field (TD-SCF), are discussed. This information is compared to an analysis based on the one-body reduced density operator (1-RDO), which is well-defined for general wavefunctions. It is seen that the distinction between two paradigms of many-body dynamics, electron transport and energy transport, is reflected in the coherences of a difference-1-RDO, or lack thereof.

  10. Simulative research on the anode plasma dynamics in the high-power electron beam diode

    SciTech Connect

    Cai, Dan; Liu, Lie; Ju, Jin-Chuan; Zhang, Tian-Yang; Zhao, Xue-Long; Zhou, Hong-Yu

    2015-07-15

    Anode plasma generated by electron beams could limit the electrical pulse-length, modify the impedance and stability of diode, and affect the generator to diode power coupling. In this paper, a particle-in-cell code is used to study the dynamics of anode plasma in the high-power electron beam diode. The effect of gas type, dynamic characteristic of ions on the diode operation with bipolar flow model are presented. With anode plasma appearing, the amplitude of diode current is increased due to charge neutralizations of electron flow. The lever of neutralization can be expressed using saturation factor. At same pressure of the anode gas layer, the saturation factor of CO{sub 2} is bigger than the H{sub 2}O vapor, namely, the generation rate of C{sup +} ions is larger than the H{sup +} ions at the same pressure. The transition time of ions in the anode-cathode gap could be used to estimate the time of diode current maximum.

  11. Dynamic Electron Correlation Effects on the Ground State Potential Energy Surface of a Retinal Chromophore Model.

    PubMed

    Gozem, Samer; Huntress, Mark; Schapiro, Igor; Lindh, Roland; Granovsky, Alexander A; Angeli, Celestino; Olivucci, Massimo

    2012-11-13

    The ground state potential energy surface of the retinal chromophore of visual pigments (e.g., bovine rhodopsin) features a low-lying conical intersection surrounded by regions with variable charge-transfer and diradical electronic structures. This implies that dynamic electron correlation may have a large effect on the shape of the force fields driving its reactivity. To investigate this effect, we focus on mapping the potential energy for three paths located along the ground state CASSCF potential energy surface of the penta-2,4-dieniminium cation taken as a minimal model of the retinal chromophore. The first path spans the bond length alternation coordinate and intercepts a conical intersection point. The other two are minimum energy paths along two distinct but kinetically competitive thermal isomerization coordinates. We show that the effect of introducing the missing dynamic electron correlation variationally (with MRCISD) and perturbatively (with the CASPT2, NEVPT2, and XMCQDPT2 methods) leads, invariably, to a stabilization of the regions with charge transfer character and to a significant reshaping of the reference CASSCF potential energy surface and suggesting a change in the dominating isomerization mechanism. The possible impact of such a correction on the photoisomerization of the retinal chromophore is discussed. PMID:26605574

  12. Simulation of radiation belt electron dynamics using in-situ global model of chorus waves inferred from the low-altitude electron precipitation

    NASA Astrophysics Data System (ADS)

    Li, W.; Thorne, R. M.; Ni, B.; Bortnik, J.; Ma, Q.; Chen, L.; Kletzing, C.; Kurth, W. S.; Hospodarsky, G. B.; Green, J. C.; Baker, D. N.; Kanekal, S. G.; Reeves, G. D.; Henderson, M. G.; Spence, H.; Blake, J. B.; Fennell, J. F.; Claudepierre, S. G.

    2013-12-01

    The global evolution of chorus wave intensity is crucial to evaluate the electron local acceleration by chorus waves, which is fundamentally important for radiation belt electron dynamics. Based on the fact that chorus waves play a dominant role in scattering 30-100 keV electrons, we adopt a physics-based technique of inferring chorus wave amplitudes from the low-altitude electron population (30-100 keV) measured by multiple POES/MetOp satellites, which provide extensive coverage over a broad L-MLT region. This technique is validated through analyzing conjunction events with the Van Allen Probes measuring chorus wave amplitudes near the equator and POES/MetOp satellites measuring the 30-100 keV electron population at the conjugate low altitudes. We adopt this technique to construct chorus wave intensity distributions, which are then used to simulate the radiation belt electron dynamics during the 09 October 2012 storm. The simulation results show that the pronounced electron acceleration to relativistic energies with a peak in phase space density observed by the Van Allen probes was primarily caused by chorus-driven local acceleration. Our numerical simulation of local stochastic acceleration not only accounts for the timescale and energy dependence of the rapid increase in electron flux in the heart of the outer radiation belt, but also reproduces the evolution of the observed electron pitch angle distribution.

  13. The sensitivities of high-harmonic generation and strong-field ionization to coupled electronic and nuclear dynamics.

    PubMed

    Baykusheva, Denitsa; Kraus, Peter M; Zhang, Song Bin; Rohringer, Nina; Wörner, Hans Jakob

    2014-01-01

    The sensitivities of high-harmonic generation (HHG) and strong-field ionization (SFI) to coupled electronic and nuclear dynamics are studied, using the nitric oxide (NO) molecule as an example. A coherent superposition of electronic and rotational states of NO is prepared by impulsive stimulated Raman scattering and probed by simultaneous detection of HHG and SFI yields. We observe a fourfold higher sensitivity of high-harmonic generation to electronic dynamics and attribute it to the presence of inelastic quantum paths connecting coherently related electronic states [Kraus et al., Phys. Rev. Lett.111, 243005 (2013)]. Whereas different harmonic orders display very different sensitivities to rotational or electronic dynamics, strong-field ionization is found to be most sensitive to electronic motion. We introduce a general theoretical formalism for high-harmonic generation from coupled nuclear-electronic wave packets. We show that the unequal sensitivities of different harmonic orders to electronic or rotational dynamics result from the angle dependence of the photorecombination matrix elements which encode several autoionizing and shape resonances in the photoionization continuum of NO. We further study the dependence of rotational and electronic coherences on the intensity of the excitation pulse and support the observations with calculations.

  14. Coupled quantum-classical method for long range charge transfer: relevance of the nuclear motion to the quantum electron dynamics

    NASA Astrophysics Data System (ADS)

    da Silva, Robson; Hoff, Diego A.; Rego, Luis G. C.

    2015-04-01

    Charge and excitonic-energy transfer phenomena are fundamental for energy conversion in solar cells as well as artificial photosynthesis. Currently, much interest is being paid to light-harvesting and energy transduction processes in supramolecular structures, where nuclear dynamics has a major influence on electronic quantum dynamics. For this reason, the simulation of long range electron transfer in supramolecular structures, under environmental conditions described within an atomistic framework, has been a difficult problem to study. This work describes a coupled quantum mechanics/molecular mechanics method that aims at describing long range charge transfer processes in supramolecular systems, taking into account the atomistic details of large molecular structures, the underlying nuclear motion, and environmental effects. The method is applied to investigate the relevance of electron-nuclei interaction on the mechanisms for photo-induced electron-hole pair separation in dye-sensitized interfaces as well as electronic dynamics in molecular structures.

  15. Ultrafast spectroscopy of electron transfer dynamics in liquids; excitation transfer studies of phase transitions

    NASA Astrophysics Data System (ADS)

    Goun, Alexei A.

    The transfer of an electron from a donor to an acceptor is the fundamental step in a wide range of chemical and biological processes. As a result, electron-transfer reactions have been the focus of numerous theoretical and experimental efforts aimed at understanding the kinetics and mechanism of the transfer event. Liquid solvents are an important medium for electron-transfer processes. The influences of the distance dependence, diffusion, the radial distribution function, and the hydrodynamic effect have been incorporated into the theory of electron transfer in solution, as well as into the theory of electron transfer between donors and acceptors in the head group regions of micelles. The development of new laser system with a pulse duration of tens of femtoseconds, with tunable wavelength allowed us to study these processes on a considerably shorter time scale than previous studies. This allowed us to observe not only the diffusion controlled but also the kinetics of electron transfer for donor/acceptor pairs that are in close proximity. In one set of experiments we have studied the kinetics of electron transfer in electron accepting molecule (rhodamine 3B) dissolved in electron donating solvent (N,N-dimethylaniline). The data for the forward electron transfer and geminate recombination are approximated by the statistical theory of the electron transfer. Optical anisotropy observed in the experiment demonstrates the orientation dependence of the electron transfer rate. In further experiments we investigated the electron transfer in non-hydrogen bonding liquids of increasing viscosity. The effective value of the donor/acceptor electronic coupling was found to decrease with viscosity. Electron transfer experiments were also carried out on the surface of micelles. The systems studied are the hole donor octadecyl-rhodamine B (ODRB) and the hole acceptor N,N-dimethyl-aniline (DMA) in micelles made of dodecyltrimethylammonium bromide (DTAB) and

  16. Ad-hoc Solutions for Capturing Electronic Structure Details in Classical Dynamics Simulations

    NASA Astrophysics Data System (ADS)

    Crill, John Wesley

    Traditional empirical potentials used in molecular dynamics (MD) simulations replace an explicit treatment of the electronic structure with an appropriate interatomic potential energy expression. This enables MD simulations to model atomistic processes, such as dislocation dynamics and plastic deformation, which typically require size and time domains exceeding what is currently feasible with computationally-demanding first principles techniques. However, discarding the electronic degrees of freedom prevents MD simulations from properly resolving certain phenomena which are dominated by electronic interactions. One example is thermal transport in metals, which is often underestimated by orders of magnitude in MD simulations. A recently-developed multi-scale simulation approach, allowing ad-hoc feedback from continuum heat flow solutions to thermostat atoms in an MD simulation, is used to model Joule-heating in nano-scale metallic contacts under electromagnetic stress. The simulations are carried out under conditions representative of contact surfaces in Radio Frequency Electromechanical Switches (RF MEMS) and rail/armature components of Electromagnetic Launchers (EMLs) and are used to speculate on the mechanisms for experimentally-observed material transfer. Another phenomenon that is typically neglected in MD simulations is charge transfer between atoms of dissimilar electronegativity. A common approach to incorporating a dynamic treatment of charge in a classical potential simulation is to solve atomic charges using an equalization of electronegativity in the charge equilibration (QEq) method. The current work studies the effectiveness of the QEq to mimic the charge distribution properties of f-center defects in a sodium chloride crystal. The results indicate that the QEq is able to replicate some of the electrostatic energy features of an f-center, which include an extremely localized potential well in the vicinity of the defect.

  17. Photoisomerization mechanism of 4-methylpyridine explored by electronic structure calculations and nonadiabatic dynamics simulations

    SciTech Connect

    Cao Jun; Fang Weihai; Fang Qiu

    2011-01-28

    In the present paper, different electronic structure methods have been used to determine stationary and intersection structures on the ground (S{sub 0}) and {sup 1}{pi}{pi}* (S{sub 2}) states of 4-methylpyridine, which is followed by adiabatic and nonadiabatic dynamics simulations to explore the mechanistic photoisomerization of 4-methylpyridine. Photoisomerization starts from the S{sub 2}({sup 1}{pi}{pi}*) state and overcomes a small barrier, leading to formation of the prefulvene isomer in the S{sub 0} state via a S{sub 2}/S{sub 0} conical intersection. The ultrafast S{sub 2}{yields} S{sub 0} nonradiative decay and low quantum yield for the photoisomerization reaction were well reproduced by the combined electronic structure calculation and dynamics simulation. The prefulvene isomer was assigned as a long-lived intermediate and suggested to isomerize to 4-methylpyridine directly in the previous study, which is not supported by the present calculation. The nonadiabatic dynamics simulation and electronic structure calculation reveal that the prefulvene isomer is a short-lived intermediate and isomerizes to benzvalene form very easily. The benzvalene form was predicted as the stable isomer in the present study and is probably the long-lived intermediate observed experimentally. A consecutive light and thermal isomerization cycle via Dewar isomer was determined and this cycle mechanism is different from that reported in the previous study. It should be pointed out that formation of Dewar isomer from the S{sub 2}({sup 1}{pi}{pi}*) state is not in competition with the isomerization to the prefulvene form. The Dewar structure observed experimentally may originate from other excited states.

  18. Observation of the dynamics leading to a conical intersection in dissociative electron attachment to water

    SciTech Connect

    Haxton, Dan; Adaniya, Hidihito; Slaughter, Dan; Rudek, B.; Osipov, Timur; Weber, Thorsten; Rescigno, Tom; McCurdy, Bill; Belkacem, Ali

    2011-06-08

    Following prior work on the lower-energy resonances, we apply techniques of momentum imaging and ab initio scattering calculations to the process of dissociative electron attachment to water via the highest-energy {sup 2}B{sub 2} resonance. We focus on the H{sup -} anion fragment, which is produced via dynamics passing through and avoiding the conical intersection with the lower A{sub 1} state, leading to OH ((sup 2}{Pi} ) and OH ({sup 2}{Sigma} ), respectively. The momentum imaging technique, when combined with theoretical calculations on the attachment amplitude and dissociation dynamics, demonstrates that the angular distributions provide a signature of the location of the conical intersection in the space of nuclear con gurations.

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

    NASA Astrophysics Data System (ADS)

    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.

  20. Ultrafast time dynamics studies of periodic lattices with free electron laser radiation

    SciTech Connect

    Quevedo, W.; Busse, G.; Hallmann, J.; More, R.; Petri, M.; Rajkovic, I.; Krasniqi, F.; Rudenko, A.; Tschentscher, T.; Stojanovic, N.; Duesterer, S.; Treusch, R.; Tolkiehn, M.; Techert, S.

    2012-11-01

    It has been proposed that radiation from free electron laser (FEL) at Hamburg (FLASH) can be used for ultrafast time-resolved x-ray diffraction experiments based on the near-infrared (NIR) pump/FEL probe scheme. Here, investigation probing the ultrafast structural dynamics of periodic nano-crystalline organic matter (silver behenate) with such a scheme is reported. Excitation with a femtosecond NIR laser leads to an ultrafast lattice modification which time evolution has been studied through the scattering of vacuum ultraviolet FEL pulses. The found effect last for 6 ps and underpins the possibility for studying nanoperiodic dynamics down to the FEL source time resolution. Furthermore, the possibility of extending the use of silver behenate (AgBh) as a wavelength and temporal calibration tool for experiments with soft x-ray/FEL sources is suggested.