Photocarrier dynamics in anatase TiO{sub 2} investigated by pump-probe absorption spectroscopy
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.
Time-Resolved Measurements of Photocarrier Dynamics in TiS3 Nanoribbons.
Cui, Qiannan; Lipatov, Alexey; Wilt, Jamie Samantha; Bellus, Matthew Z; Zeng, Xiao Cheng; Wu, Judy; Sinitskii, Alexander; Zhao, Hui
2016-07-20
We report synthesis and time-resolved transient absorption measurements of TiS3 nanoribbons. TiS3 nanoribbons were fabricated by direct reaction of titanium and sulfur. Dynamics of the photocarriers in these samples were studied by transient absorption measurements. It was found that following ultrafast injection of nonequilibrium and hot photocarriers, the thermalization, energy relaxation, and exciton formation all occur on a subpicosecond time scale. Several key parameters describing the dynamical properties of photocarriers, including their recombination lifetime, diffusion coefficient, mobility, and diffusion length, were deduced. PMID:27362332
Photocarrier dynamics in transition metal dichalcogenide alloy Mo0.5W0.5S2.
He, Jiaqi; He, Dawei; Wang, Yongsheng; Zhao, Hui
2015-12-28
We report a transient absorption study of photocarrier dynamics in transition metal dichalcogenide alloy, Mo0.5W0.5S2. Photocarriers were injected by a 400-nm pump pulse and detected by a 660-nm probe pulse. We observed a fast energy relaxation process of about 0.7 ps. The photocarrier lifetime is in the range of 50 - 100 ps, which weakly depends on the injected photocarrier density and is a few times shorter than MoS2 and WS2, reflecting the relatively lower crystalline quality of the alloy. Saturable absorption was also observed in Mo0.5W0.5S2, with a saturation energy fluence of 32 μJ cm(-2). These results provide important parameters on photocarrier properties of transition metal dichalcogenide alloys. PMID:26832001
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.
NASA Astrophysics Data System (ADS)
Lane, Paul A.; Cunningham, Paul D.; Melinger, Joseph S.; Heilweil, Edwin J.
2014-10-01
We present a study of charge transfer and carrier dynamics in films of zinc phthalocyanine (ZnPc) and buckmisnsterfullerene (C60) by investigated by time-resolved terahertz spectroscopy (TRTS). We compare terahertz photoconductivity dynamics in composite and multi-layered films of C60 and ZnPc. The few picosecond terahertz photoconductivity dynamics arise from autoionization and recombination between C60 molecules and cooling of hot photocarriers following from charge transfer between C60 and ZnPc.
Photocarrier recombination dynamics in ternary chalcogenide CuInS2 quantum dots.
Sun, Jianhui; Ikezawa, Michio; Wang, Xiuying; Jing, Pengtao; Li, Haibo; Zhao, Jialong; Masumoto, Yasuaki
2015-05-14
Photocarrier recombination dynamics in ternary chalcogenide CuInS2 quantum dots (CIS QDs) was studied by means of femtosecond transient-absorption (TA) and nanosecond time-resolved photoluminescence (PL) spectroscopy. Under strong excitation, the TA dynamics in CIS QDs is well described by a simple rate equation including single-carrier trapping, free-to-bound recombination, and trap-assisted Auger recombination. Under weak excitation, on the other hand, the PL decays of the QDs are composed of a short-lived component caused by surface trapping and a long-lived one caused by free-to-bound recombination. It is found that the surface trapping accelerates markedly with decreasing QD size while the free-to-bound radiative recombination hardly depends on the QD size. Besides this, we observed both a decrease in the PL lifetimes and a dynamic spectral redshift, which are attributed to the surface trapping and the coexistent inhomogeneous broadening in CIS QDs. The spectral redshift becomes less pronounced in CIS/ZnS core/shell QDs because of the suppression of the fast nonradiative recombination caused by the passivation of the surface traps. These results give clear evidence that the free-to-bound model is appropriate for interpreting the optical properties of CIS QDs. PMID:25728207
Temperature-dependent photocarrier recombination dynamics in Cu{sub 2}ZnSnS{sub 4} single crystals
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.
Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells
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
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.
Ultrafast decoherence dynamics govern photocarrier generation efficiencies in polymer solar cells.
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
NASA Astrophysics Data System (ADS)
Quang Phuong, Le; Okano, Makoto; Yamashita, Genki; Nagai, Masaya; Ashida, Masaaki; Nagaoka, Akira; Yoshino, Kenji; Kanemitsu, Yoshihiko
2015-06-01
We investigated the effects of sodium doping on the photocarrier dynamics in Cu2ZnSnS4 (CZTS) single crystals using optical pump-THz probe transient reflectivity (THz-TR) and time-resolved photoluminescence (PL) spectroscopy. The THz-TR and PL decay dynamics are influenced by sodium doping, and their sodium-induced changes are consistent with each other. These time-resolved measurements revealed that the lifetime of photocarriers increases with sodium doping. This result indicates that a part of defects is suppressed by doping sodium into CZTS and implies that sodium doping improves the charge transport properties of CZTS, leading to an improvement in the performance of CZTS-based solar cells.
NASA Astrophysics Data System (ADS)
Wang, Qian; Li, Bincheng
2015-12-01
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.
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.
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.
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.
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.
Photocarrier drift distance in organic solar cells and photodetectors
Stolterfoht, Martin; Armin, Ardalan; Philippa, Bronson; White, Ronald D.; Burn, Paul L.; Meredith, Paul; Juška, Gytis; Pivrikas, Almantas
2015-01-01
Light harvesting systems based upon disordered materials are not only widespread in nature, but are also increasingly prevalent in solar cells and photodetectors. Examples include organic semiconductors, which typically possess low charge carrier mobilities and Langevin-type recombination dynamics – both of which negatively impact the device performance. It is accepted wisdom that the “drift distance” (i.e., the distance a photocarrier drifts before recombination) is defined by the mobility-lifetime product in solar cells. We demonstrate that this traditional figure of merit is inadequate for describing the charge transport physics of organic light harvesting systems. It is experimentally shown that the onset of the photocarrier recombination is determined by the electrode charge and we propose the mobility-recombination coefficient product as an alternative figure of merit. The implications of these findings are relevant to a wide range of light harvesting systems and will necessitate a rethink of the critical parameters of charge transport. PMID:25919439
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.
Electric-field dependence of photocarrier generation efficiency of organic photoconductors
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.
Exceptional and Anisotropic Transport Properties of Photocarriers in Black Phosphorus.
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. PMID:25961945
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.
Electronic Spectroscopy & Dynamics
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.
Dynamic Transmission Electron Microscopy
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.
Electron Cyclotron Resonances in Electron Cloud Dynamics
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.
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.
LETTER TO THE EDITOR: Efficient photocarrier injection in a transition metal oxide heterostructure
NASA Astrophysics Data System (ADS)
Muraoka, Y.; Yamauchi, T.; Ueda, Y.; Hiroi, Z.
2002-12-01
An efficient method for doping a transition metal oxide (TMO) with hole carriers is presented: photocarrier injection (PCI) in an oxide heterostructure. It is shown that an insulating vanadium dioxide (VO2) film is rendered metallic under light irradiation by PCI from an n-type titanium dioxide (TiO2) substrate doped with Nb. Consequently, a large photoconductivity, which is exceptional for TMOs, is found in the VO2/TiO2:Nb heterostructure. We propose an electronic band structure where photoinduced holes created in TiO2:Nb can be transferred into the filled V 3d band via the low-lying O 2p band of VO2.
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.
Dynamic imaging with electron microscopy
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.
Dynamic imaging with electron microscopy
Campbell, Geoffrey; McKeown, Joe; Santala, Melissa
2014-05-30
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.
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.
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.
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.
NASA Astrophysics Data System (ADS)
Zhou, Zhongxiang; Li, Yang; Tian, Hao; Li, Jun; Liu, Yuqiang; Yang, Yanqiang
2009-07-01
The photocarrier mobility of Fe 0.03 wt%-doped potassium lithium tantalate niobate (K 0.95Li 0.05Ta 0.61Nb 0.39O 3) was investigated by time-of-flight (TOF) measurement. The longitudinal photocarrier response due to pulsed excitation leads to values of the drift mobility of μh = 1.45 × 10 -2 cm 2/V s for holes, μe = 0.325 × 10 -2 cm 2/V s for electrons, and a value for the range of holes ( μτ) h = 4.38 × 10 -5 cm 2/V at room temperature and at low field 3 KV/cm. The response time of holes and electrons (or the relaxation time) is determined to be 3.02 × 10 -3 s and 3.74 × 10 -3 s, respectively. The mobility of holes strongly depends on the field strength, and is observed to decrease with increasing bias field.
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.
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
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
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.
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.
Dynamical effects in electron spectroscopy
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.
Dynamical effects in electron spectroscopy.
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
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 (1.5
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.
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.
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. PMID:24830733
Electron magnetohydrodynamics: dynamics and turbulence.
Lyutikov, Maxim
2013-11-01
We consider dynamics and turbulent interaction of whistler modes within the framework of inertialess electron magnetohydrodynamics (EMHD). We argue that there is no energy principle in EMHD: any stationary closed configuration is neutrally stable. On the other hand, the relaxation principle, the long term evolution of a weakly dissipative system towards Taylor-Beltrami state, remains valid in EMHD. We consider the turbulent cascade of whistler modes. We show that (i) harmonic whistlers are exact nonlinear solutions; (ii) collinear whistlers do not interact (including counterpropagating); (iii) waves with the same value of the wave vector k(1)=k(2) do not interact; (iv) whistler modes have a dispersion that allows a three-wave decay, including into a zero frequency mode; (v) the three-wave interaction effectively couples modes with highly different wave numbers and propagation angles. In addition, linear interaction of a whistler with a single zero mode can lead to spatially divergent structures via parametric instability. All these properties are drastically different from MHD, so that the qualitative properties of the Alfvén turbulence can not be transferred to the EMHD turbulence. We derive the Hamiltonian formulation of EMHD, and using Bogoliubov transformation reduce it to the canonical form; we calculate the matrix elements for the three-wave interaction of whistlers. We solve numerically the kinetic equation and show that, generally, the EMHD cascade develops within a broad range of angles, while transiently it may show anisotropic, nearly two-dimensional structures. Development of a cascade depends on the forcing (nonuniversal) and often fails to reach a steady state. Analytical estimates predict the spectrum of magnetic fluctuations for the quasi-isotropic cascade [proportionality]k(-2). The cascade remains weak (not critically balanced). The cascade is UV local, while the infrared locality is weakly (logarithmically) violated. PMID:24329368
Electron magnetohydrodynamics: Dynamics and turbulence
NASA Astrophysics Data System (ADS)
Lyutikov, Maxim
2013-11-01
We consider dynamics and turbulent interaction of whistler modes within the framework of inertialess electron magnetohydrodynamics (EMHD). We argue that there is no energy principle in EMHD: any stationary closed configuration is neutrally stable. On the other hand, the relaxation principle, the long term evolution of a weakly dissipative system towards Taylor-Beltrami state, remains valid in EMHD. We consider the turbulent cascade of whistler modes. We show that (i) harmonic whistlers are exact nonlinear solutions; (ii) collinear whistlers do not interact (including counterpropagating); (iii) waves with the same value of the wave vector k1=k2 do not interact; (iv) whistler modes have a dispersion that allows a three-wave decay, including into a zero frequency mode; (v) the three-wave interaction effectively couples modes with highly different wave numbers and propagation angles. In addition, linear interaction of a whistler with a single zero mode can lead to spatially divergent structures via parametric instability. All these properties are drastically different from MHD, so that the qualitative properties of the Alfvén turbulence can not be transferred to the EMHD turbulence. We derive the Hamiltonian formulation of EMHD, and using Bogoliubov transformation reduce it to the canonical form; we calculate the matrix elements for the three-wave interaction of whistlers. We solve numerically the kinetic equation and show that, generally, the EMHD cascade develops within a broad range of angles, while transiently it may show anisotropic, nearly two-dimensional structures. Development of a cascade depends on the forcing (nonuniversal) and often fails to reach a steady state. Analytical estimates predict the spectrum of magnetic fluctuations for the quasi-isotropic cascade ∝k-2. The cascade remains weak (not critically balanced). The cascade is UV local, while the infrared locality is weakly (logarithmically) violated.
Dynamics of energetic plasma sheet electrons
NASA Astrophysics Data System (ADS)
Burin Des Roziers, Edward
2009-06-01
The dynamics of energetic plasma sheet electrons plays an important role in many geomagnetic processes. The intent of this thesis is to extend the current understanding of the relationship between the solar wind and energetic plasma sheet electrons (~> 40 keV ), as well as the variability of these electrons within the plasma sheet. The statistical relationship between tens of keV plasma sheet electrons and the solar wind, as well as > 2 MeV geosynchronous electrons, is investigated, using plasma sheet measurements from Cluster (2001 - 2005) and Geotail (1998 - 2005), and concurrent solar wind measurements from ACE. Statistically, plasma sheet electron flux variations are compared to solar wind velocity, density, dynamic pressure, IMF B z , and solar wind energetic electrons, as well as > 2 MeV electrons at geosynchronous orbit. Several new results are revealed: (1) there is a strong positive correlation between energetic plasma sheet electrons and solar wind velocity; (2) this correlation is valid throughout the plasma sheet and extends to distances of X GSM =-30 R E ; (3) there is evidence of a weak negative correlation between energetic plasma sheet electrons and solar wind density; (4) energetic plasma sheet electrons are enhanced during times of southward interplanetary magnetic field (IMF); (5) there is no clear correlation between energetic plasma sheet electrons and solar wind electrons of comparable energies; and (6) there is a strong correlation between energetic electrons in the plasma sheet and > 2 MeV electrons at geosynchronous orbit measured 2 days later. In addition, the variability of energetic electron fluxes within the plasma sheet is explored. Interesting events were found using a combination of automated methods and visual inspection. Events are classified into 4 main types: (1) plasma sheet empty of energetic electrons; (2) decreasing plasma sheet energetic electron fluxes; (3) increasing plasma sheet energetic electron fluxes; and (4) sharp
Electron dynamics controlled via self-interaction.
Tamburini, Matteo; Keitel, Christoph H; Di Piazza, Antonino
2014-02-01
The dynamics of an electron in a strong laser field can be significantly altered by radiation reaction. This usually results in a strongly damped motion, with the electron losing a large fraction of its initial energy. Here we show that the electron dynamics in a bichromatic laser pulse can be indirectly controlled by a comparatively small radiation reaction force through its interplay with the Lorentz force. By changing the relative phase between the two frequency components of the bichromatic laser field, an ultrarelativistic electron bunch colliding head-on with the laser pulse can be deflected in a controlled way, with the deflection angle being independent of the initial electron energy. The effect is predicted to be observable with laser powers and intensities close to those of current state-of-the-art petawatt laser systems. PMID:25353414
Hot electron dynamics in graphene
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
Dynamic electron control using light and nanostructure
NASA Astrophysics Data System (ADS)
Huang, Cheng-Wei
The advent of nano-technology has made possible the manipulation of electron or light through nanostructures. For example, a nano-tip in near-field optical microscopy allows imaging beyond the diffraction limit, and a nano-fabricated hologram is used to produce electron vortex beam. While most schemes of electron control utilize only static components, dynamic electron beam control using both light and nanostructures has not yet been realized. In this dissertation, we explore this possibility and study the interplay between electron, light, and nanostructures. A understanding of such a system may facilitate dynamic electron beam control or even bring new insights to fundamental quantum mechanics. The direct interaction between light and free electrons is weak, but the presence of nanostructures may modify the electron-light interaction in different ways. First, nanostructures may change a free electron's behavior by deforming the local vacuum field. When the electron's behavior is modified, its interaction with light could change too. Second, the illumination of light on nanostructures may give rise to induced surface charges or surface plasmon polaritons. The near-field of these charge structures could couple strongly with free electrons. To learn about electron dynamics in the vacuum field, we start with a classical harmonic oscillator. When the oscillator is immersed in the vacuum field, its interaction with light could be modified. Our study shows that the harmonic oscillator exhibits an integer-spaced spectrum instead of a single resonance. On the other hand, to study how induced surface charges could mediate interaction between light and free electrons, we illuminated different surfaces with a low-intensity laser. As an electron beam is brought close to a surface that is illuminated with light, electron deflection was observed. This is considered to be a preliminary study to the effect of light on the electrons in the presence of nanostructures. The
Electronic continuum model for molecular dynamics simulations.
Leontyev, I V; Stuchebrukhov, A A
2009-02-28
A simple model for accounting for electronic polarization in molecular dynamics (MD) simulations is discussed. In this model, called molecular dynamics electronic continuum (MDEC), the electronic polarization is treated explicitly in terms of the electronic continuum (EC) approximation, while the nuclear dynamics is described with a fixed-charge force field. In such a force-field all atomic charges are scaled to reflect the screening effect by the electronic continuum. The MDEC model is rather similar but not equivalent to the standard nonpolarizable force-fields; the differences are discussed. Of our particular interest is the calculation of the electrostatic part of solvation energy using standard nonpolarizable MD simulations. In a low-dielectric environment, such as protein, the standard MD approach produces qualitatively wrong results. The difficulty is in mistreatment of the electronic polarizability. We show how the results can be much improved using the MDEC approach. We also show how the dielectric constant of the medium obtained in a MD simulation with nonpolarizable force-field is related to the static (total) dielectric constant, which includes both the nuclear and electronic relaxation effects. Using the MDEC model, we discuss recent calculations of dielectric constants of alcohols and alkanes, and show that the MDEC results are comparable with those obtained with the polarizable Drude oscillator model. The applicability of the method to calculations of dielectric properties of proteins is discussed. PMID:19256627
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.
Dynamics of dissociative electron attachment to ammonia
NASA Astrophysics Data System (ADS)
Rescigno, T. N.; Trevisan, C. S.; Orel, A. E.; Slaughter, D. S.; Adaniya, H.; Belkacem, A.; Weyland, Marvin; Dorn, Alexander; McCurdy, C. W.
2016-05-01
Ab initio theoretical studies and momentum-imaging experiments are combined to provide a consistent picture of the dynamics of dissociative electron attachment to ammonia through its 5.5- and 10.5-eV resonance channels. The present study clarifies the character and symmetry of the anion states involved and the dynamics that leads to the observed fragment-ion channels, their branching ratios, and angular distributions.
Cyclotron Resonances in Electron Cloud Dynamics
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.
Chaotic electron dynamics in gyrotron resonators
Kominis, Y.; Dumbrajs, O.; Avramides, K.A.; Hizanidis, K.; Vomvoridis, J.L.
2005-04-15
Phase space analysis of electron dynamics is used in combination with the canonical perturbation method and the KAM (Kolmogorov-Arnold-Moser) theory in order to study the dependence of the efficient gyrotron operation on the rf field profile and frequency mismatch. Knowledge of the boundaries of the electron motion provided through robust (slightly distorted) KAM surfaces is useful for optimizing depressed collectors and thereby for enhancement of overall efficiency of gyrotron operation.
Electron Dynamics Near a Charged Radiator
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.
Protein electron transfer: Dynamics and statistics.
Matyushov, Dmitry V
2013-07-14
Electron transfer between redox proteins participating in energy chains of biology is required to proceed with high energetic efficiency, minimizing losses of redox energy to heat. Within the standard models of electron transfer, this requirement, combined with the need for unidirectional (preferably activationless) transitions, is translated into the need to minimize the reorganization energy of electron transfer. This design program is, however, unrealistic for proteins whose active sites are typically positioned close to the polar and flexible protein-water interface to allow inter-protein electron tunneling. The high flexibility of the interfacial region makes both the hydration water and the surface protein layer act as highly polar solvents. The reorganization energy, as measured by fluctuations, is not minimized, but rather maximized in this region. Natural systems in fact utilize the broad breadth of interfacial electrostatic fluctuations, but in the ways not anticipated by the standard models based on equilibrium thermodynamics. The combination of the broad spectrum of static fluctuations with their dispersive dynamics offers the mechanism of dynamical freezing (ergodicity breaking) of subsets of nuclear modes on the time of reaction/residence of the electron at a redox cofactor. The separation of time-scales of nuclear modes coupled to electron transfer allows dynamical freezing. In particular, the separation between the relaxation time of electro-elastic fluctuations of the interface and the time of conformational transitions of the protein caused by changing redox state results in dynamical freezing of the latter for sufficiently fast electron transfer. The observable consequence of this dynamical freezing is significantly different reorganization energies describing the curvature at the bottom of electron-transfer free energy surfaces (large) and the distance between their minima (Stokes shift, small). The ratio of the two reorganization energies
Ultrafast Dynamics of Electrons in Ammonia
NASA Astrophysics Data System (ADS)
Vöhringer, Peter
2015-04-01
Solvated electrons were first discovered in solutions of metals in liquid ammonia. The physical and chemical properties of these species have been studied extensively for many decades using an arsenal of electrochemical, spectroscopic, and theoretical techniques. Yet, in contrast to their hydrated counterpart, the ultrafast dynamics of ammoniated electrons remained completely unexplored until quite recently. Femtosecond pump-probe spectroscopy on metal-ammonia solutions and femtosecond multiphoton ionization spectroscopy on the neat ammonia solvent have provided new insights into the optical properties and the reactivities of this fascinating species. This article reviews the nature of the optical transition, which gives the metal-ammonia solutions their characteristic blue appearance, in terms of ultrafast relaxation processes involving bound and continuum excited states. The recombination processes following the injection of an electron via photoionization of the solvent are discussed in the context of the electronic structure of the liquid and the anionic defect associated with the solvated electron.
Ultrafast dynamics of electrons in ammonia.
Vöhringer, Peter
2015-04-01
Solvated electrons were first discovered in solutions of metals in liquid ammonia. The physical and chemical properties of these species have been studied extensively for many decades using an arsenal of electrochemical, spectroscopic, and theoretical techniques. Yet, in contrast to their hydrated counterpart, the ultrafast dynamics of ammoniated electrons remained completely unexplored until quite recently. Femtosecond pump-probe spectroscopy on metal-ammonia solutions and femtosecond multiphoton ionization spectroscopy on the neat ammonia solvent have provided new insights into the optical properties and the reactivities of this fascinating species. This article reviews the nature of the optical transition, which gives the metal-ammonia solutions their characteristic blue appearance, in terms of ultrafast relaxation processes involving bound and continuum excited states. The recombination processes following the injection of an electron via photoionization of the solvent are discussed in the context of the electronic structure of the liquid and the anionic defect associated with the solvated electron. PMID:25493716
Cyclotron Resonances in Electron Cloud Dynamics
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.
Ultrafast electron optics: Propagation dynamics of femtosecond electron packets
NASA Astrophysics Data System (ADS)
Siwick, Bradley J.; Dwyer, Jason R.; Jordan, Robert E.; Miller, R. J. Dwayne
2002-08-01
Time-resolved electron diffraction harbors great promise for resolving the fastest chemical processes with atomic level detail. The main obstacles to achieving this real-time view of a chemical reaction are associated with delivering short electron pulses with sufficient electron density to the sample. In this article, the propagation dynamics of femtosecond electron packets in the drift region of a photoelectron gun are investigated with an N-body numerical simulation and mean-field model. It is found that space-charge effects can broaden the electron pulse to many times its original length and generate many eV of kinetic energy bandwidth in only a few nanoseconds. There is excellent agreement between the N-body simulation and the mean-field model for both space-charge induced temporal and kinetic energy distribution broadening. The numerical simulation also shows that the redistribution of electrons inside the packet results in changes to the pulse envelope and the development of a spatially linear axial velocity distribution. These results are important for (or have the potential to impact on) the interpretation of time-resolved electron diffraction experiments and can be used in the design of photoelectron guns and streak tubes with temporal resolution of several hundred femtoseconds.
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.
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.
Dynamics of electron transfer in amine photooxidation
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.
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.
Probing Structural and Electronic Dynamics with Ultrafast Electron Microscopy
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
Structure and Dynamics with Ultrafast Electron Microscopes
NASA Astrophysics Data System (ADS)
Siwick, Bradley
In this talk I will describe how combining ultrafast lasers and electron microscopes in novel ways makes it possible to directly `watch' the time-evolving structure of condensed matter, both at the level of atomic-scale structural rearrangements in the unit cell and at the level of a material's nano- microstructure. First, I will briefly describe my group's efforts to develop ultrafast electron diffraction using radio- frequency compressed electron pulses in the 100keV range, a system that rivals the capabilities of xray free electron lasers for diffraction experiments. I will give several examples of the new kinds of information that can be gleaned from such experiments. In vanadium dioxide we have mapped the detailed reorganization of the unit cell during the much debated insulator-metal transition. In particular, we have been able to identify and separate lattice structural changes from valence charge density redistribution in the material on the ultrafast timescale. In doing so we uncovered a previously unreported optically accessible phase/state of vanadium dioxide that has monoclinic crystallography like the insulator, but electronic structure and properties that are more like the rutile metal. We have also combined these dynamic structural measurements with broadband ultrafast spectroscopy to make detailed connections between structure and properties for the photoinduced insulator to metal transition. Second, I will show how dynamic transmission electron microscopy (DTEM) can be used to make direct, real space images of nano-microstructural evolution during laser-induced crystallization of amorphous semiconductors at unprecedented spatio-temporal resolution. This is a remarkably complex process that involves several distinct modes of crystal growth and the development of intricate microstructural patterns on the nanosecond to ten microsecond timescales all of which can be imaged directly with DTEM.
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.
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.
Dynamical electronic nematicity from Mott physics
Okamoto, Satoshi; Senechal, D.; Civelli, M.; Tremblay, A.-M.
2010-01-01
Very large anisotropies in transport quantities have been observed in the presence of very small in-plane structural anisotropy in many strongly correlated electron materials. By studying the two-dimensional Hubbard model with dynamical-mean-field theory for clusters, we show that such large anisotropies can be induced without static stripe order if the interaction is large enough to yield a Mott transition. Anisotropy decreases at large frequency. The maximum effect on conductivity anisotropy occurs in the underdoped regime, as observed in high temperature superconductors.
Origin of Photocarrier Losses in Iron Pyrite (FeS2) Nanocubes.
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
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.
Dynamically programmable electronic pill dispenser system.
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
Electron trapping in amorphous silicon: A quantum molecular dynamics study
Yang, Lin H.; Kalia, R.K.; Vashishta, P.
1990-12-01
Quantum molecular dynamics (QMD) simulations provide the real-time dynamics of electrons and ions through numerical solutions of the time-dependent Schrodinger and Newton equations, respectively. Using the QMD approach we have investigated the localization behavior of an excess electron in amorphous silicon at finite temperatures. For time scales on the order of a few picoseconds, we find the excess electron is localized inside a void of radius {approximately}3 {Angstrom} at finite temperatures. 12 refs.
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.
Electronic and Ionic Transport Dynamics in Organolead Halide Perovskites.
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. PMID:27315525
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…
ELECTRON COUD DYNAMICS IN HIGH-INTENSITY RINGS.
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.
Relativistic dynamics of the Compton diffusion on a bound electron
NASA Astrophysics Data System (ADS)
Al Saleh, Salwa
2016-05-01
A covariant relativistic formalism for the electron-photon and nuclear dynamics is summarised making more accurate predictions in agreement with experiments for Compton scattering in shells with large electron binding energy. An exact solution for the Dirac equation for an electron in the nuclear Coulomb field is obtained, in order to write the relativistic dynamics for this QED process. This is a preparation for the calculation of the relativistic cross-section for Compton scattering on bound electrons, as a precision test for QED.
Runaway electron dynamics in tokamak plasmas with high impurity content
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.
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.
Electron Spin Dynamics in Semiconductor Quantum Dots
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.
Imaging the molecular dynamics of dissociative electron attachment to water
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.
Electron spin decoherence in nuclear spin baths and dynamical decoupling
Zhao, N.; Yang, W.; Ho, S. W.; Hu, J. L.; Wan, J. T. K.; Liu, R. B.
2011-12-23
We introduce the quantum theory of the electron spin decoherence in a nuclear spin bath and the dynamical decoupling approach for protecting the electron spin coherence. These theories are applied to various solid-state systems, such as radical spins in molecular crystals and NV centers in diamond.
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.
Role of Many-Electron Dynamics in High Harmonic Generation
Gordon, Ariel; Kaertner, Franz X.; Rohringer, Nina; Santra, Robin
2006-06-09
High harmonic generation (HHG) in many-electron atoms is studied theoretically. The breakdown of the frozen-core single active electron approximation is demonstrated, as it predicts roughly the same radiation amplitude in all noble gases. This is in contradiction with experiments, where heavier noble gases are known to emit much stronger HHG radiation than lighter ones. This experimental behavior of the noble gases can be qualitatively reproduced when many-electron dynamics, within a simple approximation, is taken into account.
Radiation Belt Electron Dynamics: Modeling Atmospheric Losses
NASA Technical Reports Server (NTRS)
Selesnick, R. S.
2003-01-01
The first year of work on this project has been completed. This report provides a summary of the progress made and the plan for the coming year. Also included with this report is a preprint of an article that was accepted for publication in Journal of Geophysical Research and describes in detail most of the results from the first year of effort. The goal for the first year was to develop a radiation belt electron model for fitting to data from the SAMPEX and Polar satellites that would provide an empirical description of the electron losses into the upper atmosphere. This was largely accomplished according to the original plan (with one exception being that, for reasons described below, the inclusion of the loss cone electrons in the model was deferred). The main concerns at the start were to accurately represent the balance between pitch angle diffusion and eastward drift that determines the dominant features of the low altitude data, and then to accurately convert the model into simulated data based on the characteristics of the particular electron detectors. Considerable effort was devoted to achieving these ends. Once the model was providing accurate results it was applied to data sets selected from appropriate periods in 1997, 1998, and 1999. For each interval of -30 to 60 days, the model parameters were calculated daily, thus providing good short and long term temporal resolution, and for a range of radial locations from L = 2.7 to 3.9. .
Electron transfer dynamics: Zusman equation versus exact theory.
Shi, Qiang; Chen, Liping; Nan, Guangjun; Xu, Ruixue; Yan, YiJing
2009-04-28
The Zusman equation has been widely used to study the effect of solvent dynamics on electron transfer reactions. However, application of this equation is limited by the classical treatment of the nuclear degrees of freedom. In this paper, we revisit the Zusman equation in the framework of the exact hierarchical equations of motion formalism, and show that a high temperature approximation of the hierarchical theory is equivalent to the Zusman equation in describing electron transfer dynamics. Thus the exact hierarchical formalism naturally extends the Zusman equation to include quantum nuclear dynamics at low temperatures. This new finding has also inspired us to rescale the original hierarchical equations and incorporate a filtering algorithm to efficiently propagate the hierarchical equations. Numerical exact results are also presented for the electron transfer reaction dynamics and rate constant calculations. PMID:19405605
Atomically resolved real-space imaging of hot electron dynamics
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
Atomically resolved real-space imaging of hot electron dynamics.
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
Atomically resolved real-space imaging of hot electron dynamics
NASA Astrophysics Data System (ADS)
Lock, D.; Rusimova, K. R.; Pan, T. L.; Palmer, R. E.; Sloan, P. A.
2015-09-01
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.
Ultrafast dynamics of electrons at interfaces
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
Electron dynamics with radiation and nonlinear wigglers
Jowett, J.M.
1986-06-01
The physics of electron motion in storage rings is described by supplementing the Hamiltonian equations of motion with fluctuating radiation reaction forces to describe the effects of synchrotron radiation. This leads to a description of radiation damping and quantum diffusion in single-particle phase-space by means of Fokker-Planck equations. For practical purposes, most storage rings remain in the regime of linear damping and diffusion; this is discussed in some detail with examples, concentrating on longitudinal phase space. However special devices such as nonlinear wigglers may permit the new generation of very large rings to go beyond this into regimes of nonlinear damping. It is shown how a special combined-function wiggler can be used to modify the energy distribution and current profile of electron bunches.
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.
Dynamical backaction cooling with free electrons
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
Loiudice, Anna; Cooper, Jason K; Hess, Lucas H; Mattox, Tracy M; Sharp, Ian D; Buonsanti, R
2015-11-11
Multicomponent oxides and their heterostructures are rapidly emerging as promising light absorbers to drive oxidative chemistry. To fully exploit their functionality, precise tuning of their composition and structure is crucial. Here, we report a novel solution-based route to nanostructured bismuth vanadate (BiVO4) that facilitates the assembly of BiVO4/metal oxide (TiO2, WO3, and Al2O3) nanocomposites in which the morphology of the metal oxide building blocks is finely tailored. The combination of transient absorption spectroscopy-spanning from picoseconds to second time scales-and photoelectrochemical measurements reveals that the achieved structural tunability is key to understanding and directing charge separation, transport, and efficiency in these complex oxide heterostructured films. PMID:26457457
Dynamics of runaway electrons in magnetized plasmas
Moghaddam-Taaheri, E.
1986-01-01
The evolution of a runaway electron tail driven by a subcritical dc electric field in a magnetized plasma is studied numerically using a quasi-linear numerical code (2-D in v- and k-space) based on the Ritz-Galerkin method and finite elements. Three different regimes in the evolution of the runaway tail depending on the strength of the dc electric field and the ratio of plasma to gyrofrequency, were found. The tail can be (a) stable and the electrons are accelerated to large parallel velocities, (b) unstable to the Cerenkov resonance due to the formation of a positive slope on the runaway tail, (c) unstable to the anomalous Doppler resonance instability driven by the large velocity anisotropy in the tail. Once an instability is triggered (Cerenkov or anomalous Doppler resonance) the tail relaxes into an isotropic distribution resulting in less acceleration. The synchrotron emission of the runaway electrons shows large enhancement in the radiation level at the high-frequency end of the spectrum during the pitch-angle scattering of the fast particles. The results are relevant to recent experimental data from the Princeton Large Torus (PLT) during current-drive experiments and to the microwave bursts observed during solar flares.
Understanding electronically non-adiabatic relaxation dynamics in singlet fission.
Tao, Guohua
2015-01-13
Nonadiabatic relaxation of one singlet state into two triplet states is the key step in singlet fission dynamics, the understandings of which may help design next generation solar cells. In this work we perform the symmetrical quasi-classical (SQC) nonadiabatic molecular dynamics (MD) simulation [Cotton and Miller, J. Phys. Chem. A, 2013, 117, 7190; Meyer and Miller, J. Chem. Phys. 1979, 70, 3214] for a model system to study the real-time fission dynamics. The dependence of the nonadiabatic relaxation dynamics on energy levels, electronic couplings, and electronic-phonon couplings has been examined, in comparison with other analytical approximations, such as Förster theory and Marcus theory. Unlike many other methods, the SQC nondiabatic MD simulation approach is able to describe fission dynamics efficiently and accurately enough to provide microscopic insights into singlet fission. PMID:26574200
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.
Dynamics of Hybrid Electronic-Neuronal Systems
NASA Astrophysics Data System (ADS)
Breen, Barbara; Garcia, Paul; Furman, Michael D.; Lindner, John; Ditto, William
2001-03-01
Hybrid systems of neurons and nonlinear electrical components may make possible a new breed of computer optimized for such applications as pattern recognition and the combinatorially explosive problems that are the bane of traditional computers. Because the dynamics of arrays of neurons are high dimensional, and as they are difficult to measure and control, we have focused our initial efforts on more manageable hybrid silicon-neuron systems. Here we present results from our numerical simulations and biological experiments involving a neuron coupled to Chua’s famous chaotic circuit. The results of our simulations reinforce the possibility of using the dynamics of hybrid systems for encoding numbers and performing computation [1]. For example, bi-directionally coupling the FitzHugh-Nagumo model neuron to the Chua model circuit resulted in co-existing stable limit cycles, which can be used to store information. The coupling was also able to convert periodic neuronal spiking to chaotic bursting. We observed similar results with the more physiologically relevant Pinsky-Rinzel [2] model neuron, which facilitated our transition to a living neuron, the rodent hippocampal CA3 pyramidal cell, which we coupled to an analog Chua circuit. [1] Sinha, S., Ditto, W.L., Phys. Rev. Lett., 81, 2156-2159 (1998); Sinha, S., Ditto, W.L., Phys. Rev. E, 60, 363-377 (1999) [2] Pinsky, P., Rinzel, J., Journ. Comp. Neuroscience, 1, 39-60 (1994)
Coherent electron hole dynamics near a conical intersection.
Timmers, Henry; Li, Zheng; Shivaram, Niranjan; Santra, Robin; Vendrell, Oriol; Sandhu, Arvinder
2014-09-12
The coherent evolution of an electron hole in a photoionized molecule represents an unexplored facet of charge transfer phenomena occurring in complex systems. Using ultrafast extreme ultraviolet spectroscopy, we investigate the real-time dynamics of an electron hole wave packet created near a conical intersection in CO_{2}. We resolve the oscillation of the electron hole density between σ and π character, driven by the coupled bending and asymmetric stretch vibrations of the molecule. We also quantify the mixing between electron hole configurations and find that the wave packet coherence diminishes with time due to thermal dephasing. PMID:25259975
Electron Dynamics in Nanostructures in Strong Laser Fields
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.
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.
NASA Astrophysics Data System (ADS)
Sha, Wei E. I.; Choy, Wallace C. H.; Cho Chew, Weng
2012-11-01
A multiphysics study carries out on organic solar cells (OSCs) by solving Maxwell's and semiconductor equations simultaneously. By introducing a metallic rectangular-grating as the anode, surface plasmons are excited resulting in nonuniform exciton generation. Meanwhile, the internal E-field of plasmonic OSCs is modified with the modulated anode boundary. The plasmonic OSC improves 13% of short-circuit current but reduces 7% of fill factor (FF) compared to the standard one with a planar anode. The uneven photocarrier generation and transport by the grating anode are physical origins of the dropped FF. This work provides fundamental multiphysics modeling and understanding for plasmonic OSCs.
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.
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.
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.
Direct observation of electron dynamics in the attosecond domain.
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
Identifying the Stern-Gerlach force of classical electron dynamics.
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
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.
Modeling of explosive electron emission and electron beam dynamics in high-current devices
NASA Astrophysics Data System (ADS)
Anishchenko, S. V.; Gurinovich, A. A.
2014-03-01
Based on a detailed analysis of explosive electron emission in high-current electronic devices, we formulate a system of equations that describes the expansion of the cathode plasma and the generation of high-current electron beams. The system underlies the numerical algorithm for the hybrid code which enables simulating the charged particles' dynamics in high-current vircators with open resonators. Using the Gabor-Morlet transform, we perform the time-frequency analysis of vircator radiation.
Dynamics and reactivity of trapped electrons on supported ice crystallites.
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
Local dynamic range compensation for scanning electron microscope imaging system.
Sim, K S; Huang, Y H
2015-01-01
This is the extended project by introducing the modified dynamic range histogram modification (MDRHM) and is presented in this paper. This technique is used to enhance the scanning electron microscope (SEM) imaging system. By comparing with the conventional histogram modification compensators, this technique utilizes histogram profiling by extending the dynamic range of each tile of an image to the limit of 0-255 range while retains its histogram shape. The proposed technique yields better image compensation compared to conventional methods. PMID:25969945
Electron-hole dynamics in CdTe tetrapods.
Malkmus, Stephan; Kudera, Stefan; Manna, Liberato; Parak, Wolfgang J; Braun, Markus
2006-09-01
We present transient absorption studies with femtosecond time resolution on the electron-hole dynamics in CdTe tetrapod nanostructures. Electron-hole pairs are generated by optical excitation in the visible spectral range, and an immediate bleach and induced absorption signal are observed. The relaxation dynamics to the lowest excitonic state is completed in about 6 ps. Experiments with polarized excitation pulses give information about the localization of the excited-state wave functions. The influence of the nanocrystal shape on the optical properties of CdTe nanoparticles is discussed. PMID:16942067
Molecular interferometer to decode attosecond electron-nuclear dynamics.
Palacios, Alicia; González-Castrillo, Alberto; Martín, Fernando
2014-03-18
Understanding the coupled electronic and nuclear dynamics in molecules by using pump-probe schemes requires not only the use of short enough laser pulses but also wavelengths and intensities that do not modify the intrinsic behavior of the system. In this respect, extreme UV pulses of few-femtosecond and attosecond durations have been recognized as the ideal tool because their short wavelengths ensure a negligible distortion of the molecular potential. In this work, we propose the use of two twin extreme UV pulses to create a molecular interferometer from direct and sequential two-photon ionization processes that leave the molecule in the same final state. We theoretically demonstrate that such a scheme allows for a complete identification of both electronic and nuclear phases in the wave packet generated by the pump pulse. We also show that although total ionization yields reveal entangled electronic and nuclear dynamics in the bound states, doubly differential yields (differential in both electronic and nuclear energies) exhibit in addition the dynamics of autoionization, i.e., of electron correlation in the ionization continuum. Visualization of such dynamics is possible by varying the time delay between the pump and the probe pulses. PMID:24591647
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.
Electronically Nonadiabatic Dynamics via Semiclassical Initial Value Methods
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.
Special issue on ultrafast electron and molecular dynamics
NASA Astrophysics Data System (ADS)
Martin, Fernando; Hishikawa, Akiyoshi; Vrakking, Marc
2014-06-01
In the last few years, the advent of novel experimental and theoretical approaches has made possible the investigation of (time-resolved) molecular dynamics in ways not anticipated before. Experimentally, the introduction of novel light sources such as high-harmonic generation (HHG) and XUV/x-ray free electron lasers, and the emergence of novel detection strategies, such as time-resolved electron/x-ray diffraction and the fully coincident detection of electrons and fragment ions in reaction microscopes, has significantly expanded the arsenal of available techniques, and has taken studies of molecular dynamics into new domains of spectroscopic, spatial and temporal resolution, the latter including first explorations into the attosecond domain, thus opening completely new avenues for imaging electronic and nuclear dynamics in molecules. Along the way, particular types of molecular dynamics, e.g., dynamics around conical intersections, have gained an increased prominence, sparked by the realization of the essential role that this dynamics plays in relaxation pathways in important bio-molecular systems. In the short term, this will allow one to uncover and control the dynamics of elementary chemical processes such as, e.g., ultrafast charge migration, proton transfer, isomerization or multiple ionization, and to address new key questions about the role of attosecond coherent electron dynamics in chemical reactivity. The progress on the theoretical side has been no less impressive. Novel generations of supercomputers and a series of novel computational strategies have allowed nearly exact calculations in small molecules, as well as highly successful approximate calculations in large, polyatomic molecules, including biomolecules. Frequent and intensive collaborations involving both theory and experiment have been essential for the progress that has been accomplished. The special issue 'Ultrafast electron and molecular dynamics' seeks to provide an overview of the current
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.
Phase-space Dynamics of Runaway Electrons In Tokamaks
Xiaoyin Guan, Hong Qin, and Nathaniel J. Fisch
2010-08-31
The phase-space dynamics of runaway electrons is studied, including the influence of loop voltage, radiation damping, and collisions. A theoretical model and a numerical algorithm for the runaway dynamics in phase space are developed. Instead of standard integrators, such as the Runge-Kutta method, a variational symplectic integrator is applied to simulate the long-term dynamics of a runaway electron. The variational symplectic integrator is able to globally bound the numerical error for arbitrary number of time-steps, and thus accurately track the runaway trajectory in phase space. Simulation results show that the circulating orbits of runaway electrons drift outward toward the wall, which is consistent with experimental observations. The physics of the outward drift is analyzed. It is found that the outward drift is caused by the imbalance between the increase of mechanical angular momentum and the input of toroidal angular momentum due to the parallel acceleration. An analytical expression of the outward drift velocity is derived. The knowledge of trajectory of runaway electrons in configuration space sheds light on how the electrons hit the first wall, and thus provides clues for possible remedies.
Dynamics Of Electronic Excitation Of Solids With Ultrashort Laser Pulse
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.
Identifying the Stern-Gerlach force of classical electron dynamics
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
Emulating Molecular Orbitals and Electronic Dynamics with Ultracold Atoms
NASA Astrophysics Data System (ADS)
Lühmann, Dirk-Sören; Weitenberg, Christof; Sengstock, Klaus
2015-07-01
In recent years, ultracold atoms in optical lattices have proven their great value as quantum simulators for studying strongly correlated phases and complex phenomena in solid-state systems. Here, we reveal their potential as quantum simulators for molecular physics and propose a technique to image the three-dimensional molecular orbitals with high resolution. The outstanding tunability of ultracold atoms in terms of potential and interaction offer fully adjustable model systems for gaining deep insight into the electronic structure of molecules. We study the orbitals of an artificial benzene molecule and discuss the effect of tunable interactions in its conjugated π electron system with special regard to localization and spin order. The dynamical time scales of ultracold atom simulators are on the order of milliseconds, which allows for the time-resolved monitoring of a broad range of dynamical processes. As an example, we compute the hole dynamics in the conjugated π system of the artificial benzene molecule.
Diagnostic techniques for measuring suprathermal electron dynamics in plasmas (invited)
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.
Photocathode Optimization for a Dynamic Transmission Electron Microscope: Final Report
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.
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.
Electron-phonon interaction within classical molecular dynamics
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
The dynamical correlation in spacer-mediated electron transfer couplings
Yang, C.-H.; Hsu, C.-P.
2006-06-28
The dynamical correlation effect in electron transfer (ET) coupling was studied in this work, for cases where electrons tunnel through a many-electron environment. The ET couplings for three different bridge-mediated model systems were calculated: (I) trans-alkyl chains [H{sub 2}C-(CH{sub 2}){sub n}-CH{sub 2}, n=2-10], (II) two isomers of trans-1,4-dimethylenecyclohexane, and (III) two ethylenes spaced by a saturated ethane molecule. The couplings were calculated as half energy gaps of the two lowest adiabatic states. The dynamical correlation was included with spin-flip (SF) and ionization potential or electron affinity coupled-cluster singles and doubles (SF-CCSD and IP/EA-CCSD) and a {delta}CCSD scheme. The direct coupling (DC) scheme is also used as a way to obtain a solution with nondynamical correlation, since DC uses approximated eigenstates that are symmetry-restoring linear combinations of two symmetry-broken unrestricted Hartree-Fock configurations. For all cases tested except for one, results from the DC scheme closely follow the CCSD data, indicating that the dual-configuration solutions can be a good approximation of wave functions with nondynamical correlation included, but there exist exceptions. Comparing the DC results with SF-CCSD and IP or EA-CCSD data, we concluded that the dynamical correlation effect is small for most of the cases we tested.
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.
New attosecond spectroscopies for correlation-induced electron hole dynamics
NASA Astrophysics Data System (ADS)
Averbukh, Vitali
2014-05-01
In this talk I will present two of our recent ideas for new attosecond time-resolved measurements of electron hole dynamics: 1. Single-photon laser enabled Auger decay (spLEAD) spectroscopy and 2. High-harmonic generation (HHG) spectroscopy of Auger-type transitions. Unlike the well-known attosecond streaking, the proposed spectroscopies do not rely on photo- or secondary electron emission and are applicable to ultrafast electronic processes involving bound-bound transitions, such as electron correlation-driven charge migration. We simulate the new attosecond spectroscopies using both model and ab initio methods. Specific applications include hole migration in glycine, atomic Auger and Coster-Kronig decays as well as quasi-exponential dynamics of molecular orbital breakdown in trans-butadiene and propanal. The author acknowledges the financial support of the Engineering and Physical Sciences Research Council (EPSRC, UK) through the Career Acceleration Fellowship (Award No. EP/H003657/1) and the Programme Grant on Attosecond Dynamics (Award No. EP/I032517).
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.
Gated electron sharing within dynamic naphthalene diimide-based oligorotaxanes.
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
Electron-Wavepacket Reaction Dynamics in Proton Transfer of Formamide
NASA Astrophysics Data System (ADS)
Nagashima, Kengo; Takatsuka, Kazuo
2009-10-01
We apply the semiclassical Ehrenfest theory, which provides electron wavepacket dynamics coupled to nuclear motion, to a study of water-assisted proton relay in formamide compared with a forced proton transfer in gas phase, both of which are associated with the tautomerization. We start with the enol (imidic acid) form HO-CH═NH and track its proton transfer process to the keto (amide) form O═CH-NH2. Identifying the fact that this is indeed a "proton transfer process" rather than hydrogen-atom migration in terms of radical character on the proton, we show a collective quantum flux of electrons, which flows backward against the proton motion. This backward flux compensates the electrons tightly covering the proton, as represented in the Mulliken charge. The enol form formamide is one of the simplest species in the group O═CR1-NHR2, which is a unit of polypeptide. In the gas phase, the nitrogen atom may have a pyramidal structure as in the ammonium molecule; therefore, the C-N bond may allow low barrier rotation along it. This rotation is strongly prohibited by the formation of the double bond C═N induced by the proton transfer. Not only the dynamical process of proton transfer itself but also the electronic structures left behind are greatly affected by the presence of water molecule(s) and polar solvents. In discussing the relative stability of the formamide after the proton transfer, the following resonance structures are frequently mentioned, O--CH═N+H2 ↔ O═CH-NH2. Here we address the dynamical manifestation of the resonance structures in terms of our dynamical electron theory.
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
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
Electron transfer, decoherence, and protein dynamics: insights from atomistic simulations.
Narth, Christophe; Gillet, Natacha; Cailliez, Fabien; Lévy, Bernard; de la Lande, Aurélien
2015-04-21
Electron transfer in biological systems drives the processes of life. From cellular respiration to photosynthesis and enzymatic catalysis, electron transfers (ET) are chemical processes on which essential biological functions rely. Over the last 40 years, scientists have sought understanding of how these essential processes function in biology. One important breakthrough was the discovery that Marcus theory (MT) of electron transfer is applicable to biological systems. Chemists have experimentally collected both the reorganization energies (λ) and the driving forces (ΔG°), two parameters of Marcus theory, for a large variety of ET processes in proteins. At the same time, theoretical chemists have developed computational approaches that rely on molecular dynamics and quantum chemistry calculations to access numerical estimates of λ and ΔG°. Yet another crucial piece in determining the rate of an electron transfer is the electronic coupling between the initial and final electronic wave functions. This is an important prefactor in the nonadiabatic rate expression, since it reflects the probability that an electron tunnels from the electron donor to the acceptor through the intervening medium. The fact that a protein matrix supports electron tunneling much more efficiently than vacuum is now well documented, both experimentally and theoretically. Meanwhile, many chemists have provided examples of the rich physical chemistry that can be induced by protein dynamics. This Account describes our studies of the dynamical effects on electron tunneling. We present our analysis of two examples of natural biological systems through MD simulations and tunneling pathway analyses. Through these examples, we show that protein dynamics sustain efficient tunneling. Second, we introduce two time scales: τcoh and τFC. The former characterizes how fast the electronic coupling varies with nuclear vibrations (which cause dephasing). The latter reflects the time taken by the system
Quantum dynamics and electronic spectroscopy within the framework of wavelets
NASA Astrophysics Data System (ADS)
Toutounji, Mohamad
2013-03-01
This paper serves as a first-time report on formulating important aspects of electronic spectroscopy and quantum dynamics in condensed harmonic systems using the framework of wavelets, and a stepping stone to our future work on developing anharmonic wavelets. The Morlet wavelet is taken to be the mother wavelet for the initial state of the system of interest. This work reports daughter wavelets that may be used to study spectroscopy and dynamics of harmonic systems. These wavelets are shown to arise naturally upon optical electronic transition of the system of interest. Natural birth of basis (daughter) wavelets emerging on exciting an electronic two-level system coupled, both linearly and quadratically, to harmonic phonons is discussed. It is shown that this takes place through using the unitary dilation and translation operators, which happen to be part of the time evolution operator of the final electronic state. The corresponding optical autocorrelation function and linear absorption spectra are calculated to test the applicability and correctness of the herein results. The link between basis wavelets and the Liouville space generating function is established. An anharmonic mother wavelet is also proposed in the case of anharmonic electron-phonon coupling. A brief description of deriving anharmonic wavelets and the corresponding anharmonic Liouville space generating function is explored. In conclusion, a mother wavelet (be it harmonic or anharmonic) which accounts for Duschinsky mixing is suggested.
Electron-spin dynamics induced by photon spins
NASA Astrophysics Data System (ADS)
Bauke, Heiko; Ahrens, Sven; Keitel, Christoph H.; Grobe, Rainer
2014-10-01
Strong rotating magnetic fields may cause a precession of the electron's spin around the rotation axis of the magnetic field. The superposition of two counterpropagating laser beams with circular polarization and opposite helicity features such a rotating magnetic field component but also carries spin. The laser's spin density, which can be expressed in terms of the laser's electromagnetic fields and potentials, couples to the electron's spin via a relativistic correction to the Pauli equation. We show that the quantum mechanical interaction of the electron's spin with the laser's rotating magnetic field and with the laser's spin density counteract each other in such a way that a net spin rotation remains with a precession frequency that is much smaller than the frequency one would expect from the rotating magnetic field alone. In particular, the frequency scales differently with the laser's electric field strength depending on whether relativistic corrections are taken into account or not. Thus, the relativistic coupling of the electron's spin to the laser's spin density changes the dynamics not only quantitatively but also qualitatively as compared to the nonrelativistic theory. The electron's spin dynamics are a genuine quantum mechanical relativistic effect.
Dynamics of two-electron excitations in helium
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.
Dynamical conductivity of strongly correlated electron systems at oxide interfaces
NASA Astrophysics Data System (ADS)
Ouellette, Daniel Gerald
The Mott metal-insulator transition (MIT) in transition-metal complex oxides results from strong electron-electron interactions and is accompanied by a rich spectrum of phenomena, including magnetic, charge, and orbital ordering, superconductivity, structural distortions, polarons, and very high-density 2-dimensional interface electron liquids. Recent advances in oxide heteroepitaxy allow interface control as a promising new approach to tuning the exotic properties of materials near the quantum critical point, with potential application to technologies including phase-change electronics, high power transistors, and sensors. The dynamical conductivity of oxide heterostructures is measured using a combination of terahertz time-domain spectroscopy, Fourier transform infrared spectroscopy, and dc magnetotransport. The rare-earth nickelates RNiO3 (R = La, Nd...) exhibit a temperature and bandwidth controlled MIT in bulk. Measurements of the Drude response in epitaxial thin films provide quantification of the strain-dependent mass enhancement in the metallic phase due to strong correlations. Reduction of LaNiO 3 film thickness leads to additional mass renormalization attributed to structural distortions at the heteroepitaxial interface, and an MIT is observed depending on the interfacing materials in coherent perovskite heterostructures. The rare-earth titanates RTiO3 exhibit a bandwidth and band filling controlled Mott MIT. Furthermore, the heterointerface between Mott insulating GdTiO3 and band insulating SrTiO3 exhibits a 2-dimensional itinerant electron liquid, with extremely high sheet densities of 3 x 1014 cm-2. The dynamical conductivity of the interface electrons is analyzed in terms of subband-dependent electron mobility and the established large polaron dynamics in bulk SrTiO3. Additional confinement of the electron liquids is achieved by decreasing the SrTiO3 layer thickness, with attendant increase in the dynamical mass. Taking the confinement to its extreme
Ultrafast electron relaxation dynamics in coupled metal nanoparticles in aggregates.
Jain, Prashant K; Qian, Wei; El-Sayed, Mostafa A
2006-01-12
We report the effect of aggregation in gold nanoparticles on their ultrafast electron-phonon relaxation dynamics measured by femtosecond transient absorption pump-probe spectroscopy. UV-visible extinction and transient absorption of the solution-stable aggregates of gold nanoparticles show a broad absorption in the 550-700-nm region in addition to the isolated gold nanoparticle plasmon resonance. This broad red-shifted absorption can be attributed to contributions from gold nanoparticle aggregates with different sizes and/or different fractal structures. The electron-phonon relaxation, reflected as a fast decay component of the transient bleach, is found to depend on the probe wavelength, suggesting that each wavelength interrogates one particular subset of the aggregates. As the probe wavelength is changed from 520 to 635 nm across the broad aggregate absorption, the rate of electron-phonon relaxation increases. The observed trend in the hot electron lifetimes can be explained on the basis of an increased overlap of the electron oscillation frequency with the phonon spectrum and enhanced interfacial electron scattering, with increasing extent of aggregation. The experimental results strongly suggest the presence of intercolloid electronic coupling within the nanoparticle aggregates, besides the well-known dipolar plasmon coupling. PMID:16471511
Ultrafast studies of electron dynamics at metal-dielectric interfaces
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
Modeling Crabbing Dynamics in an Electron-Ion Collider
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.
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.
SO(5, 1) dynamical symmetry for electron Zitterbewegung
NASA Astrophysics Data System (ADS)
Bruce, S. A.; Minning, P. C.
1985-10-01
Electron rest-frame internal canonical coordinates are reobtained by the free-particle Foldy-Wouthuysen transformation: Schrödinger “microscopic momentum”, Barut-Bracken “microscopic coordinate”, and the rest Hamiltonian, which describe Zitterbewegung in this frame. SO(4, 1) Snyder space-time invariant quantization is considered in order to construct a dynamical group for Zitterbewegung. The electron's internal structure appears associated with its secondorder self-energy process and governed by the 15-parameter dynamical group SO(5, 1). This is a generalization of Barut-Bracken symmetry which describes Zitterbewegung as generated by an algebra of the rotation group SO(5). This noncompact symmetry SO(5, 1) permits a natural interpretation for the operators of its algebra and introduces a generalization to higher-dimensional fermionic representations.
Attosecond Dynamics of Electron Wave Packets in Intense Laser Fields
NASA Astrophysics Data System (ADS)
Varjú, K.; Johnsson, P.; Mauritsson, J.; López-Martens, R.; Gustafsson, E.; Remetter, T.; L'huillier, A.
The continuous progress in the performances of light sources as well as detection techniques allows us to investigate and control the states of matter in even finer details. Light sources, ranging from the infrared (IR) to the extreme ultraviolet (XUV), are becoming increasingly coherent, intense, well characterized, and controlled. The shortest available light pulses are now significantly shorter than 1 fs [1]-[4], thus offering unique promise for studies of ultrafast electron dynamics.
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.
Control of electron spin decoherence caused by electron nuclear spin dynamics in a quantum dot
NASA Astrophysics Data System (ADS)
Liu, Ren-Bao; Yao, Wang; Sham, L. J.
2007-07-01
Control of electron spin decoherence in contact with a mesoscopic bath of many interacting nuclear spins in an InAs quantum dot is studied by solving the coupled quantum dynamics. The nuclear spin bath, because of its bifurcated evolution predicated on the electron spin up or down state, measures the which-state information of the electron spin and hence diminishes its coherence. The many-body dynamics of the nuclear spin bath is solved with a pair-correlation approximation. In the relevant timescale, nuclear pair-wise flip flops, as elementary excitations in the mesoscopic bath, can be mapped into the precession of non-interacting pseudo-spins. Such mapping provides a geometrical picture for understanding the decoherence and for devising control schemes. A close examination of nuclear bath dynamics reveals a wealth of phenomena and new possibilities of controlling the electron spin decoherence. For example, when the electron spin is flipped by a π-pulse at τ, its coherence will partially recover at \\sqrt{2}\\tau as a consequence of quantum disentanglement from the mesoscopic bath. In contrast to the re-focusing of inhomogeneously broadened phases by conventional spin-echoes, the disentanglement is realized through shepherding quantum evolution of the bath state via control of the quantum object. A concatenated construction of pulse sequences can eliminate the decoherence with arbitrary accuracy, with the nuclear nuclear spin interaction strength acting as the controlling small parameter.
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.
Protein dynamics modulated electron transfer kinetics in early stage photosynthesis.
Kundu, Prasanta; Dua, Arti
2013-01-28
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. PMID:23387626
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.
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.
Spectral dynamics of a collective free electron maser
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.
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.
Imaging the dynamics of free-electron Landau states
Schattschneider, P.; Schachinger, Th.; Stöger-Pollach, M.; Löffler, S.; Steiger-Thirsfeld, A.; Bliokh, K. Y.; Nori, Franco
2014-01-01
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. PMID:25105563
The Delicate Balance of Static and Dynamic Electron Correlation.
Stein, Christopher J; von Burg, Vera; Reiher, Markus
2016-08-01
Multi-configurational approaches yield universal wave function parametrizations that can qualitatively well describe electronic structures along reaction pathways. For quantitative results, multi-reference perturbation theory is required to capture dynamic electron correlation from the otherwise neglected virtual orbitals. Still, the overall accuracy suffers from the finite size and choice of the active orbital space and peculiarities of the perturbation theory. Fortunately, the electronic wave functions at equilibrium structures of reactants and products can often be well described by single-reference methods and hence are accessible to accurate coupled cluster calculations. Here, we calculate the heterolytic double dissociation energy of four 3d-metallocenes with the complete active space self-consistent field method and compare to highly accurate coupled cluster data. Our coupled cluster data are well within the experimental error bars. This accuracy can also be approached by complete active space calculations with an orbital selection based on information entropy measures. The entropy based active space selection is discussed in detail. We find a very subtle balance between static and dynamic electron correlation effects that emphasizes the need for algorithmic active space selection and that differs significantly from restricted active space results for identical active spaces reported in the literature. PMID:27409981
Imaging the dynamics of free-electron Landau states.
Schattschneider, P; Schachinger, Th; Stöger-Pollach, M; Löffler, S; Steiger-Thirsfeld, A; Bliokh, K Y; Nori, Franco
2014-01-01
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. PMID:25105563
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.
Time Resolved Phase Transitions via Dynamic Transmission Electron Microscopy
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.
Dynamics of photoinduced electron transfer from adsorbed molecules into solids
NASA Astrophysics Data System (ADS)
Gundlach, L.; Ernstorfer, R.; Willig, F.
2007-08-01
Ultrafast interfacial electron transfer from the donor orbital of organic chromophores into empty electronic acceptor states of a semiconductor and of a metal was investigated by two-photon photoemission spectroscopy (2PPE). Experimental tools and procedures have been developed for carrying out wet-chemistry preparation of the molecule/solid interface. The organic chromophore perylene was investigated with several different bridge/anchor groups on TiO2(110). One perylene compound was investigated for comparison on Ag(110). Angle and polarization dependent 2PPE measurements revealed the orientation of the perylene chromophore on the surface as controlled by the adsorption geometry of the respective anchor group on TiO2. UPS measurements gave the position of the HOMO level of the chromophore with respect to the Fermi level of the solid. The donor level of each molecule was found high enough to fulfill the “wide band limit” of heterogeneous electron transfer dynamics. Time constants for heterogeneous electron transfer were extracted from 2PPE transients. A difference by a factor of four was found, 13 fs against 47 fs, when a conjugated bond was exchanged for a saturated bond in the otherwise identical bridge group. The two different contributions to the 2PPE transients arising firstly from the excited state of the chromophore and secondly from the injected electrons were separated by measuring the latter contribution separately in the case of instantaneous interfacial electron transfer realized with catechol as adsorbate. The time scales measured for the electron transfer step and for the subsequent electron escape process from the surface into the bulk of TiO2 showed both good agreement with recent theoretical predictions of other groups for these systems.
NASA Astrophysics Data System (ADS)
Nishitani, Junichi; Nagashima, Takeshi; Lippmaa, Mikk; Suemoto, Tohru
2016-04-01
The dynamics of photoexcited electrons in various excited d-states was investigated in a transition metal oxide MnO by tunable optical pump-terahertz probe measurements. Photoexcited electrons in the lowest excited d-state showed the longest relaxation time among the three excited d-states that are accessible in MnO at room temperature. The relaxation rate in the lowest excited d-state showed a drastic increase below the Neel temperature TN = 120 K in MnO. We conclude that this increase is caused by the appearance of a decay channel related to magnetic-excitation-assisted photoluminescence from self-trapped exciton (STE) states. The opening of relaxation channels to the STE states in an antiferromagnetic phase suggests that it may be possible to control photocarrier lifetime by magnetic order in transition metal oxides.
Pulsed Power for a Dynamic Transmission Electron Microscope
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.
Electron dynamics and ion acceleration in expanding-plasma thrusters
NASA Astrophysics Data System (ADS)
Lafleur, T.; Cannat, F.; Jarrige, J.; Elias, P. Q.; Packan, D.
2015-12-01
In most expanding-plasma thrusters, ion acceleration occurs due to the formation of ambipolar-type electric fields; a process that depends strongly on the electron dynamics of the discharge. The electron properties also determine the heat flux leaving the thruster as well as the maximum ion energy, which are important parameters for the evaluation of thruster performance. Here we perform an experimental and theoretical investigation with both magnetized, and unmagnetized, low-pressure thrusters to explicitly determine the relationship between the ion energy, E i , and the electron temperature, T e0. With no magnetic field a relatively constant value of {{E}i}/{{T}e0}≈ 6 is found for xenon, while when a magnetic nozzle is present, {{E}i}/{{T}e0} is between about 4-5. These values are shown to be a function of both the magnetic field strength, as well as the electron energy distribution function, which changes significantly depending on the mass flow rate (and hence neutral gas pressure) used in the thruster. The relationship between the ion energy and electron temperature allows estimates to be made for polytropic indices of use in a number of fluid models, as well as estimates of the upper limits to the performance of these types of systems, which for xenon and argon result in maximum specific impulses of about 2500 s and 4500 s respectively.
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.
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.
Dynamic electron arc radiotherapy (DEAR): a feasibility study
NASA Astrophysics Data System (ADS)
Rodrigues, Anna; Yin, Fang-Fang; Wu, Qiuwen
2014-01-01
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 cm2 and 3×10 cm2 for a 15×15 cm2 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.
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.
Tracing molecular electronic excitation dynamics in real time and space.
Dutoi, Anthony D; Cederbaum, Lorenz S; Wormit, Michael; Starcke, Jan Hendrik; Dreuw, Andreas
2010-04-14
We present a method for studying the movement of electrons and energy within and between electronically excited molecules. The dynamically changing state is a many-electron wavepacket, for which we numerically integrate the Schrodinger equation using the ADC(2) effective Hamiltonian for the particle-hole propagator. We develop the tools necessary for following the separate motions of the particles and holes. Total particle and hole densities can be used to give an overview of the dynamics, which can be atomically decomposed in a Mulliken fashion, or individual particle and hole states give a more detailed look at the structure of an excitation. We apply our model to a neon chain, as an illustrative example, projecting an excited eigenstate of an isolated atom onto the coupled system as the initial state. In addition to demonstrating our propagation and analysis machinery, the results show a dramatic difference in excitation-energy transfer rates as a consequence of initial polarization. Furthermore, already in a system with three constituents, an important aspect of multiple coupled systems appears, in that one absorbing system essentially shields another, changing the effective sitewise coupling parameters. PMID:20405991
Time-resolved terahertz dynamics in thin films of the topological insulator Bi2Se3
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
Atomic-Resolution 3D Electron Microscopy with Dynamic Diffraction
O'Keefe, Michael A.; Downing, Kenneth H.; Wenk, Hans-Rudolf; Meisheng, Hu
2005-02-15
Achievement of atomic-resolution electron-beam tomography will allow determination of the three-dimensional structure of nanoparticles (and other suitable specimens) at atomic resolution. Three-dimensional reconstructions will yield ''section'' images that resolve atoms overlapped in normal electron microscope images (projections), resolving lighter atoms such as oxygen in the presence of heavier atoms, and atoms that lie on non-lattice sites such as those in non-periodic defect structures. Lower-resolution electron microscope tomography has been used to produce reconstructed 3D images of nanoparticles [1] but extension to atomic resolution is considered not to be straightforward. Accurate three-dimensional reconstruction from two-dimensional projections generally requires that intensity in the series of 2-D images be a monotonic function of the specimen structure (often specimen density, but in our case atomic potential). This condition is not satisfied in electron microscopy when specimens with strong periodicity are tilted close to zone-axis orientation and produce ''anomalous'' image contrast because of strong dynamic diffraction components. Atomic-resolution reconstructions from tilt series containing zone-axis images (with their contrast enhanced by strong dynamical scattering) can be distorted when the stronger zone-axis images overwhelm images obtained in other ''random'' orientations in which atoms do not line up in neat columns. The first demonstrations of 3-D reconstruction to atomic resolution used five zone-axis images from test specimens of staurolite consisting of a mix of light and heavy atoms [2,3]. Initial resolution was to the 1.6{angstrom} Scherzer limit of a JEOL-ARM1000. Later experiments used focal-series reconstruction from 5 to 10 images to produce staurolite images from the ARM1000 with resolution extended beyond the Scherzer limit to 1.38{angstrom} [4,5]. To obtain a representation of the three-dimensional structure, images were obtained
Temporal dynamics of storage ring free electron lasers
NASA Astrophysics Data System (ADS)
Couprie, M. E.; Hara, T.; Gontier, D.; Troussel, P.; Garzella, D.; Delboulbé, A.; Billardon, M.
1996-02-01
The growth and saturation of a storage ring free electron laser (SRFEL) is driven by the beam behavior, including bunch lengthening or coherent modes of longitudinal motion (the bunch length being related to the energy spread), detuning effects, and a modification of the bunch distribution by the FEL interaction; all of these phenomena are accumulated for various passes, leading to complex dynamical processes. The knowledge and understanding of the dynamics, together with the stability over time are essential for efficient use of SRFEL sources. This is illustrated with the Super-ACO FEL experiment, analyzed from growth from the positron bunch to laser saturation and induced positron beam modification. Stability analysis (jitter, shape, intensity) is then performed carefully. A longitudinal feedback system can significantly improve it. Information provided with a streak camera reveals the distribution of a single FEL micropulse or synchrotron radiation pulse without any averaging or sampling.
Electron-spin dynamics in elliptically polarized light waves
NASA Astrophysics Data System (ADS)
Bauke, Heiko; Ahrens, Sven; Grobe, Rainer
2014-11-01
We investigate the coupling of the spin angular momentum of light beams with elliptical polarization to the spin degree of freedom of free electrons. It is shown that this coupling, which is of similar origin as the well-known spin-orbit coupling, can lead to spin precession. The spin-precession frequency is proportional to the product of the laser field's intensity and its spin density. The electron-spin dynamics is analyzed by employing exact numerical methods as well as time-dependent perturbation theory based on the fully relativistic Dirac equation and on the nonrelativistic Pauli equation that is amended by a relativistic correction that accounts for the light's spin density.
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.
Protein electron transfer: is biology (thermo)dynamic?
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
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
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.
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
U31: Vehicle Stability and Dynamics: Electronic Stability Control
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.
Proton Dynamics on Goethite Nanoparticles and Coupling to Electron Transport.
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
Dissipative many-electron dynamics of ionizing systems.
Tremblay, Jean Christophe; Klinkusch, Stefan; Klamroth, Tillmann; Saalfrank, Peter
2011-01-28
In this paper, we perform many-electron dynamics using the time-dependent configuration-interaction method in its reduced density matrix formulation (ρ-TDCI). Dissipation is treated implicitly using the Lindblad formalism. To include the effect of ionization on the state-resolved dynamics, we extend a recently introduced heuristic model for ionizing states to the ρ-TDCI method, which leads to a reduced density matrix evolution that is not norm-preserving. We apply the new method to the laser-driven excitation of H(2) in a strongly dissipative environment, for which the state-resolve lifetimes are tuned to a few femtoseconds, typical for dynamics of adsorbate at metallic surfaces. Further testing is made on the laser-induced intramolecular charge transfer in a quinone derivative as a model for a molecular switch. A modified scheme to treat ionizing states is proposed to reduce the computational burden associated with the density matrix propagation, and it is thoroughly tested and compared to the results obtained with the former model. The new approach scales favorably (∼N(2)) with the number of configurations N used to represent the reduced density matrix in the ρ-TDCI method, as compared to a N(3) scaling for the model in its original form. PMID:21280729
Nanoscale Dynamics of Radiosensitivity: Role of Low Energy Electrons
NASA Astrophysics Data System (ADS)
Sanche, Léon
This chapter addresses the nanoscale dynamics involved in the sensitization of biological cells to ionizing radiation. More specifically, it describes the role of low energy electrons (LEE) in radiosensitization by gold nanoparticles and chemotherapeutic agents, as well as potential applications to radiotherapy. The basic mechanisms of action of the LEE generated within nanoscopic volumes by ionizing radiation are described in solid water ice and various forms of DNA. These latter include the subunits (i.e., a base, a sugar or the phosphate group), short single strands (i.e., oligonucleotides) and plasmid and linear DNA. By comparing the results from experiments with the different forms of the DNA molecule and theory, it is possible to determine fundamental mechanisms that are involved in the dissociation of the subunits, base release and the production of single, double-strand breaks and cross-links. Below 15 eV, LEE localize on DNA subunits to form transient negative ions. Such states can damage DNA by dissociating into a stable anion and radical fragment(s), via dissociative electron attachment, or by decaying into dissociative electronically excited states. LEE can also transfer from one DNA subunit to another, particularly from a base to the phosphate group, where they can induce cleavage of the C-O bond (i.e., break a strand). DNA damage and the corresponding nanoscale dynamics are found to be modified in the presence of other cellular constituents. For example, condensing on DNA the most abundant cellular molecule, H2O, induces the formation of a new type of transient anion whose parent is a H2O-DNA complex.
Dynamics of a high-current relativistic electron beam
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.
Time-resolved terahertz dynamics in thin films of the topological insulator Bi{sub 2}Se{sub 3}
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.
Nonadiabatic electron dynamics of single-electron transport in a perpendicular magnetic field
He, JianHong; Guo, HuaZhong; Gao, Jie
2014-04-28
We present results of our investigation into the nonadiabatic electron dynamics of a moving quantum dot assisted by surface acoustic waves (SAWs) in a perpendicular magnetic field. The measurements show the evolution of a quantized acoustoelectric current in a modulated external field, which provides direct information of the energy spectrum and the occupation of the SAW-induced elliptical dynamical quantum dot. By comparing the magnetic field dependence of the spectrum with that of a somewhat symmetric circular dot, we find the appearance of nonadiabatic excitations at low magnetic fields resulting from the anisotropy of the dot. We also detect the transitions between different quantum states of the elliptical dot, achieved by exploiting the interference of two phase-tuned SAWs. Our results demonstrate that the quantum states in an asymmetric dot are fragile and extremely sensitive to their environment.
Entanglement dynamics of electron-electron scattering in low-dimensional semiconductor systems
Buscemi, F.; Bordone, P.; Bertoni, A.
2006-05-15
We perform the quantitative evaluation of the entanglement dynamics in scattering events between two indistinguishable electrons interacting via the Coulomb potential in one- and two-dimensional semiconductor nanostructures. We apply a criterion based on the von Neumann entropy and the Schmidt decomposition of the global state vector suitable for systems of identical particles. From the time-dependent numerical solution of the two-particle wave function of the scattering carriers we compute their entanglement evolution for different spin configurations: two electrons with the same spin, with different spin, and singlet and triplet spin states. The procedure allows us to evaluate the mechanisms that govern entanglement creation and their connection with the characteristic physical parameters and initial conditions of the system. The cases in which the evolution of entanglement is similar to the one obtained for distinguishable particles are discussed.
Dynamics and spectroscopy of CH₂OO excited electronic states.
Kalinowski, Jaroslaw; Foreman, Elizabeth S; Kapnas, Kara M; Murray, Craig; Räsänen, Markku; Gerber, R Benny
2016-04-28
The excited states of the Criegee intermediate CH2OO are studied in molecular dynamics simulations using directly potentials from multi-reference perturbation theory (MR-PT2). The photoexcitation of the species is simulated, and trajectories are propagated in time on the excited state. Some of the photoexcitation events lead to direct fragmentation of the molecule, but other trajectories describe at least several vibrations in the excited state, that may terminate by relaxation to the ground electronic state. Limits on the role of non-adiabatic contributions to the process are estimated by two different simulations, one that forces surface-hopping at potential crossings, and another that ignores surface hopping altogether. The effect of non-adiabatic transitions is found to be small. Spectroscopic implications and consequences for the interpretation of experimental results are discussed. PMID:27040614
Semiclassical Dynamics of Electron Wave Packet States with Phase Vortices
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.
Dynamics of a nanodroplet under a transmission electron microscope
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.
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.
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.
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.
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.
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.
Femtosecond electron imaging of defect-modulated phonon dynamics
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
Femtosecond electron imaging of defect-modulated phonon dynamics.
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
Invisible Electronic States and Their Dynamics Revealed by Perturbations
NASA Astrophysics Data System (ADS)
Merer, Anthony J.
2011-06-01
Sooner or later everyone working in the field of spectroscopy encounters perturbations. These can range in size from a small shift of a single rotational level to total destruction of the vibrational and rotational patterns of an electronic state. To some workers perturbations are a source of terror, but to others they are the most fascinating features of molecular spectra, because they give information about molecular dynamics, and about states that would otherwise be invisible as a result of unfavorable selection rules. An example of the latter is the essentially complete characterization of the tilde{b}^3A_2 state of SO_2 from the vibronic perturbations it causes in the tilde{a}^3B_1 state. The S_1-trans state of acetylene is a beautiful example of dynamics in action. The level patterns of the three bending vibrations change dramatically with increasing vibrational excitation as a result of the vibrational angular momentum and the approach to the isomerization barrier. Several vibrational levels of the S_1-cis isomer, previously thought to be unobservable, can now be assigned. They obtain their intensity through interactions with nearby levels of the trans isomer.
Effects of parallel electron dynamics on plasma blob transport
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.
Electron accommodation dynamics in the DNA base thymine
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.
Dynamic electronic institutions in agent oriented cloud robotic systems.
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
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.
Electronic structure and relaxation dynamics in a superconducting topological material
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
Electronic structure and relaxation dynamics in a superconducting topological material
NASA Astrophysics Data System (ADS)
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
2016-03-01
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.
Electronic structure and relaxation dynamics in a superconducting topological material
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
Electronic structure and relaxation dynamics in a superconducting topological material.
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
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
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.
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. PMID:26450316
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.
Ungar, L W; Scherer, N F; Voth, G A
1997-01-01
Classical molecular dynamics simulations are used to investigate the nuclear motions associated with photoinduced electron transfer in plastocyanin. The blue copper protein is modeled using a molecular mechanics potential; potential parameters for the copper-protein interactions are determined using an x-ray crystallographic structure and absorption and resonance Raman spectra. Molecular dynamics simulations yield a variety of information about the ground (oxidized) and optically excited (charge-transfer) states: 1) The probability distribution of the potential difference between the states, which is used to determine the coordinate and energy displacements, places the states well within the Marcus inverted region. 2) The two-time autocorrelation function of the difference potential in the ground state and the average of the difference potential after instantaneous excitation to the excited state are very similar (confirming linear response in this system); their decay indicates that vibrational relaxation occurs in about 1 ps in both states. 3) The spectral densities of various internal coordinates begin to identify the vibrations that affect the optical transition; the spectral density of the difference potential correlation function should also prove useful in quantum simulations of the back electron transfer. 4) Correlation functions of the protein atomic motions with the difference potential show that the nuclear motions are correlated over a distance of more than 20 A, especially along proposed electron transport paths. Images FIGURE 1 FIGURE 7 PMID:8994588
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
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
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
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.
High resolution simulation of beam dynamics in electron linacs for x-ray free electron lasers
NASA Astrophysics Data System (ADS)
Qiang, J.; Ryne, R. D.; Venturini, M.; Zholents, A. A.; Pogorelov, I. V.
2009-10-01
In this paper we report on large-scale high resolution simulations of beam dynamics in electron linacs for the next-generation x-ray free electron lasers (FELs). We describe key features of a parallel macroparticle simulation code including three-dimensional (3D) space-charge effects, short-range structure wakefields, coherent synchrotron radiation (CSR) wakefields, and treatment of radio-frequency (rf) accelerating cavities using maps obtained from axial field profiles. We present a study of the microbunching instability causing severe electron beam fragmentation in the longitudinal phase space which is a critical issue for future FELs. Using parameters for a proposed FEL linac at Lawrence Berkeley National Laboratory (LBNL), we show that a large number of macroparticles (beyond 100 million) is generally needed to control the numerical macroparticle shot noise and avoid overestimating the microbunching instability. We explore the effect of the longitudinal grid on simulation results. We also study the effect of initial uncorrelated energy spread on the final uncorrelated energy spread of the beam for the FEL linac.
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.
Time-resolved terahertz dynamics in thin films of the topological insulator Bi_{2}Se_{3}
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 Bi_{2}Se_{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. 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.
NASA Astrophysics Data System (ADS)
Egorov, E. N.; Koronovskii, A. A.; Kurkin, S. A.; Hramov, A. E.
2013-11-01
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.
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.
Dynamic Corneal Surface Mapping with Electronic Speckle Pattern Interferometry
NASA Astrophysics Data System (ADS)
Iqbal, S.; Gualini, M. M. S.
2013-06-01
In view of the fast advancement in ophthalmic technology and corneal surgery, there is a strong need for the comprehensive mapping and characterization techniques for corneal surface. Optical methods with precision non-contact approaches have been found to be very useful for such bio measurements. Along with the normal mapping approaches, elasticity of corneal surface has an important role in its characterization and needs to be appropriately measured or estimated for broader diagnostics and better prospective surgical results, as it has important role in the post-op corneal surface reconstruction process. Use of normal corneal topographic devices is insufficient for any intricate analysis since these devices operate at relatively moderate resolution. In the given experiment, Pulsed Electronic Speckle Pattern Interferometry has been utilized along with an excitation mechanism to measure the dynamic response of the sample cornea. A Pulsed ESPI device has been chosen for the study because of its micron-level resolution and other advantages in real-time deformation analysis. A bovine cornea has been used as a sample in the subject experiment. The dynamic response has been taken on a chart recorder and it is observed that it does show a marked deformation at a specific excitation frequency, which may be taken as a characteristic elasticity parameter for the surface of that corneal sample. It was seen that outside resonance conditions the bovine cornea was not that much deformed. Through this study, the resonance frequency and the corresponding corneal deformations are mapped and plotted in real time. In these experiments, data was acquired and processed by FRAMES plus computer analysis system. With some analysis of the results, this technique can help us to refine a more detailed corneal surface mathematical model and some preliminary work was done on this. Such modelling enhancements may be useful for finer ablative surgery planning. After further experimentation
A diagnostic for electron dynamics in tokamaks. Final report
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.
2003 Electronic Spectroscopy and Dynamics - July 6-11, 2003
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.
Modeling Charge Transfer in Fullerene Collisions via Real-Time Electron Dynamics.
Jakowski, Jacek; Irle, Stephan; Sumpter, Bobby G; Morokuma, Keiji
2012-06-01
An approach for performing real-time dynamics of electron transfer in a prototype redox reaction that occurs in reactive collisions between neutral and ionic fullerenes is discussed. The quantum dynamical simulations show that the electron transfer occurs within 60 fs directly preceding the collision of the fullerenes, followed by structural changes and relaxation of electron charge. The consequences of real-time electron dynamics are fully elucidated for the far from equilibrium processes of collisions between neutral and multiply charged fullerenes. PMID:26285634
Nonequilibrium electron dynamics in a solid with a changing nodal excitation gap
NASA Astrophysics Data System (ADS)
Smallwood, Christopher L.; Miller, Tristan L.; Zhang, Wentao; Kaindl, Robert A.; Lanzara, Alessandra
2016-06-01
We develop a computationally inexpensive model to examine the dynamics of boson-assisted electron relaxation in solids, studying nonequilibrium dynamics in a metal, in a nodal superconductor with a stationary density of states, and in a nodal superconductor where the gap dynamically opens. In the metallic system, the electron population resembles a thermal population at all times, but the presence of even a fixed nodal gap both invalidates a purely thermal treatment and sharply curtails relaxation rates. For a gap that is allowed to open as electron relaxation proceeds, effects are even more pronounced, and gap dynamics become coupled to the dynamics of the electron population. Comparisons to experiments reveal that phase-space restrictions in the presence of a gap are likely to play a significant role in the widespread observation of coexisting femtosecond and picosecond dynamics in the cuprate high-temperature superconductors.
Ion-induced electron emission from surfaces: Dynamical screening effects
Kouzakov, Konstantin A.; Berakdar, Jamal
2003-08-01
A theoretical model is developed for the description of the single-electron emission from surfaces following the impact of fast ions. The theory describes quantum mechanically the ion reflection at the surface and the excitation of the valence band electrons via an ion-electron interaction renormalized by the dielectric response of the target. Numerical calculations are presented and analyzed for the electron emission from the conduction band of an aluminum surface upon proton impact. Particular attention is devoted to the influence of the dielectric screening on the energy distributions and the angular distributions of the ejected electrons. In addition, the role of the surface electronic structure is studied.
Ultra-fast photo-carrier relaxation in Mott insulators with short-range spin correlations.
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
Ultra-fast photo-carrier relaxation in Mott insulators with short-range spin correlations
NASA Astrophysics Data System (ADS)
Eckstein, Martin; Werner, Philipp
2016-02-01
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.
Ultra-fast photo-carrier relaxation in Mott insulators with short-range spin correlations
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
Electron dynamics in strong laser pulse illumination of large rare gas clusters
NASA Astrophysics Data System (ADS)
Saalmann, U.; Rost, J. M.
2005-11-01
We analyze the dynamics of up to 105 electrons resulting from illuminating a xenon cluster with 9093 atoms with intense laser pulses of different length and peak intensity. Interesting details of electron motion are identified which can be probed with a time resolution of 100 attoseconds. Corresponding experiments would shed light on unexplored territory in complex electronic systems such as clusters and they would also permit to critically access the present theoretical description of this dynamics.
Probing Electron Dynamics with the Laplacian of the Momentum Density
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.
NASA Astrophysics Data System (ADS)
Peltola, J.; Nordlund, K.; Keinonen, J.
2006-09-01
Molecular dynamics simulations have proven to be accurate in predicting depth distributions of low-energy ions implanted in materials. Free parameters adjusted for every ion-target combination are conventionally used to obtain depth profiles in accordance with the experimental ones. We have previously developed a model for predicting depth profiles in crystalline Si without free parameters. The electronic stopping power was calculated using local total electron density. The model underestimated the stopping in the < 1 1 0 > channeling direction. We have now taken a new approach to calculate the electronic stopping power. We use the local valence (3p(2)) electron density to account for the electronic energy loss between collisions and the Firsov model to account for the electronic energy loss during collision. The lowest electron densities are adjusted with a parametrization that is same for all ions in all implanting directions to correct the problems in the < 1 1 0 > channeling direction.
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
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.
Electron quantum dynamics in atom-ion interaction.
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
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
Theoretical analysis of hot electron dynamics in nanorods.
Kumarasinghe, Chathurangi S; Premaratne, Malin; Bao, Qiaoliang; 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
Theoretical analysis of hot electron dynamics in nanorods
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
Monte Carlo simulation of electron dynamics in liquid water
NASA Astrophysics Data System (ADS)
Huthmacher, Klaus; Herzwurm, André; Gnewuch, Michael; Ritter, Klaus; Rethfeld, Baerbel
2015-07-01
We present a stochastic model for the energy loss of low-energy electrons (<100 eV) in water in the liquid phase. More precisely, we treat the electrons as independent particles and are thus able to model the time evolution of the kinetic energy of a single electron as a so-called pure jump process. Free electrons are created due to irradiation of an extreme ultraviolet femtosecond laser pulse. In our model, free electrons may interact with water molecules via elastic scattering and impact ionization. Moreover, we present numerical results for the kinetic energy of electrons during and after laser irradiation. Furthermore, we distinguish between primary and secondary electrons, where the latter are created by impact ionization. The numerical results show that creation of secondary electrons due to impact ionization occurs almost entirely during laser irradiation. After irradiation, only a small amount of the laser pulse energy remains in the electron system, while the majority is stored in holes of water molecules.
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.
NASA Astrophysics Data System (ADS)
Smith, Albert A.; Corzilius, Björn; Haze, Olesya; Swager, Timothy M.; Griffin, Robert G.
2013-12-01
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.
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.
Hao, Yajiang; Inhester, Ludger; Hanasaki, Kota; Son, Sang-Kil; Santra, Robin
2015-07-01
We present the implementation of an electronic-structure approach dedicated to ionization dynamics of molecules interacting with x-ray free-electron laser (XFEL) pulses. In our scheme, molecular orbitals for molecular core-hole states are represented by linear combination of numerical atomic orbitals that are solutions of corresponding atomic core-hole states. We demonstrate that our scheme efficiently calculates all possible multiple-hole configurations of molecules formed during XFEL pulses. The present method is suitable to investigate x-ray multiphoton multiple ionization dynamics and accompanying nuclear dynamics, providing essential information on the chemical dynamics relevant for high-intensity x-ray imaging. PMID:26798806
Efficient electronic structure calculation for molecular ionization dynamics at high x-ray intensity
Hao, Yajiang; Inhester, Ludger; Hanasaki, Kota; Son, Sang-Kil; Santra, Robin
2015-01-01
We present the implementation of an electronic-structure approach dedicated to ionization dynamics of molecules interacting with x-ray free-electron laser (XFEL) pulses. In our scheme, molecular orbitals for molecular core-hole states are represented by linear combination of numerical atomic orbitals that are solutions of corresponding atomic core-hole states. We demonstrate that our scheme efficiently calculates all possible multiple-hole configurations of molecules formed during XFEL pulses. The present method is suitable to investigate x-ray multiphoton multiple ionization dynamics and accompanying nuclear dynamics, providing essential information on the chemical dynamics relevant for high-intensity x-ray imaging. PMID:26798806
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.
Coherently driven, ultrafast electron-phonon dynamics in transport junctions
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.
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.
Kim, S; Russell, M; Henry, M; Kim, S S; Naik, R R; Voevodin, A A; Jang, S S; Tsukruk, V V; Fedorov, A G
2015-09-28
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 × 10(18) e(-) per cm(2)). 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 × 10(19) e(-) per cm(2) 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. PMID:26302897
Dynamics of electron injection from the excited state of anchored molecules into semiconductors
NASA Astrophysics Data System (ADS)
Gundlach, L.; Ernstorfer, R.; Willig, F.
A complete picture of different interfacial electron transfer dynamics has been obtained from transient absorption and two-photon photoemission data when inserting different anchor/bridge groups between the excited organic donor and the electrode surface.
Electronically non-adiabatic influences in surface chemistry and dynamics.
Wodtke, Alec M
2016-07-01
Electronically nonadiabatic interactions between molecules and metal surfaces are now well known. Evidence is particularly clear from studies of diatomic molecules that molecular vibration can be strongly coupled to electrons of the metal leading to efficient energy transfer between these two kinds of motion. Since molecular vibration is the same motion needed for bond breaking, it is logical to postulate that electronically nonadiabatic influences on surface chemical reaction probabilities would be strong. Still there are few if any examples where such influences have been clearly investigated. This review recounts the evidence for and against the aforementioned postulate emphasizing reacting systems that have yet to receive full attention and where electronically nonadiabatic influence of reaction probabilities might be clearly demonstrated. PMID:27152489
Final Report: Vibrational Dynamics in Photoinduced Electron Transfer
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
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.
Real-Time Probing of Electron Dynamics Using Attosecond Time-Resolved Spectroscopy.
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
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.
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
Observations of Nanobubble Dynamics with Transmission Electron Microscopy
NASA Astrophysics Data System (ADS)
Mohan, Meera Kanakamma; Arora, Manish; Mirsaidov, Utkur; Ohl, Claus-Dieter
2013-11-01
Recent developments in transmission electron microscopy (TEM) allow the imaging of liquids with high spatial resolution. Here we report on novel studies of water trapped between two monolayers of graphene sheets. The geometry prevents evaporation of the liquid into the low pressure environment of the TEM while providing excellent electron-optical properties for investigations. The graphene sheets are supported by a conventional TEM grid. We report on the nucleation of bubbles, the coalescence between neighbouring bubbles, rupture of thin liquid filaments, and their slow shrinkage. At a dose rate of 100-155 e-Å-2s-1 these events are observed conveniently at video frame rate. The correlation with the local electron beam dose rate suggests that the radiolysis induced by the electron beam is the main driving force for most events. In general, we observed bubbles with lateral sizes between 20 nm and 100 nm and estimated heights between 6 nm and 30 nm. Likely, the bubbles connect both graphene sheets. In the absence of the electron beam the nanobubbles do not dissolve completely but surprisingly remain stable for even up to one hour. This resembles the stability of surface attached nanobubbles.
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…
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
Many-beam dynamical simulation of electron backscatter diffraction patterns.
Winkelmann, Aimo; Trager-Cowan, Carol; Sweeney, Francis; Day, Austin P; Parbrook, Peter
2007-01-01
We present an approach for the simulation of complete electron backscatter diffraction (EBSD) patterns where the relative intensity distributions in the patterns are accurately reproduced. The Bloch wave theory is applied to describe the electron diffraction process. For the simulation of experimental patterns with a large field of view, a large number of reflecting planes has to be taken into account. This is made possible by the Bethe perturbation of weak reflections. Very good agreement is obtained for simulated and experimental patterns of gallium nitride GaN{0001} at 20kV electron energy. Experimental features like zone-axis fine structure and higher-order Laue zone rings are accurately reproduced. We discuss the influence of the diffraction of the incident beam in our experiment. PMID:17126489
Attosecond Electron Wave Packet Dynamics in Strong Laser Fields
Johnsson, P.; Remetter, T.; Varju, K.; L'Huillier, A.; Lopez-Martens, R.; Valentin, C.; Balcou, Ph.; Kazamias, S.; Mauritsson, J.; Gaarde, M. B.; Schafer, K. J.; Mairesse, Y.; Wabnitz, H.; Salieres, P.
2005-07-01
We use a train of sub-200 attosecond extreme ultraviolet (XUV) pulses with energies just above the ionization threshold in argon to create a train of temporally localized electron wave packets. We study the energy transfer from a strong infrared (IR) laser field to the ionized electrons as a function of the delay between the XUV and IR fields. When the wave packets are born at the zero crossings of the IR field, a significant amount of energy ({approx}20 eV) is transferred from the field to the electrons. This results in dramatically enhanced above-threshold ionization in conditions where the IR field alone does not induce any significant ionization. Because both the energy and duration of the wave packets can be varied independently of the IR laser, they are valuable tools for studying and controlling strong-field processes.
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.
Electron injection dynamics in high-potential porphyrin photoanodes.
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
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
NASA Astrophysics Data System (ADS)
Ma, Haibo; Schollwöck, Ulrich
2008-12-01
We present numerical studies of the transport dynamics of a charged soliton in conjugated polymers under the influence of an external time-dependent electric field. All relevant electron-phonon and electron-electron interactions are nearly fully taken into account by simulating the monomer displacements with classical molecular dynamics and evolving the wave function for the π electrons by virtue of the adaptive time-dependent density matrix renormalization group simultaneously and nonadiabatically. It is found that after a smooth turn on of the external electric field the charged soliton is accelerated at first up to a stationary constant velocity as one entity consisting of both the charge and the lattice deformation. An Ohmic region (6 mV/A˚<=E0<=12 mV/A˚) where the stationary velocity increases linearly with the electric field strength is observed. The relationship between electron-electron interactions and charged soliton transport is also investigated in detail. We find that the dependence of the stationary velocity of a charged soliton on the on-site Coulomb interactions U and the nearest-neighbor interactions V is due to the extent of delocalization of the charged soliton defect.
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.
Molecular dynamics study of electron-irradiation effects in single-walled carbon nanotubes
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.
Target surface area effects on hot electron dynamics from high intensity laser–plasma interactions
NASA Astrophysics Data System (ADS)
Zulick, C.; Raymond, A.; McKelvey, A.; Chvykov, V.; Maksimchuk, A.; Thomas, A. G. R.; Willingale, L.; Yanovsky, V.; Krushelnick, K.
2016-06-01
Reduced surface area targets were studied using an ultra-high intensity femtosecond laser in order to determine the effect of electron sheath field confinement on electron dynamics. X-ray emission due to energetic electrons was imaged using a {K}α imaging crystal. Electrons were observed to travel along the surface of wire targets, and were slowed mainly by the induced fields. Targets with reduced surface areas were correlated with increased hot electron densities and proton energies. Hybrid Vlasov–Fokker–Planck simulations demonstrated increased electric sheath field strength in reduced surface area targets.
Electron plasma dynamics during autoresonant excitation of the diocotron mode
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.
Femtosecond time-resolved electronic relaxation dynamics in tetrathiafulvalene
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.
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.
Structure and dynamics in two-electron atoms
NASA Astrophysics Data System (ADS)
Shuman, Edward Somerville
In this dissertation, I present experimental studies of two-electron atoms. I have been primarily concerned with the effects of external perturbations on dielectronic recombination (DR). Specifically I have examined dielectronic recombination in the presence of electric, microwave, and combined electric and magnetic fields. These measurements illustrate that any external perturbation must have a coupling in excess of the autoionization rate to affect the DR rate. I have also studied the structure of two-electron atoms using microwave resonance techniques. In particular I present experiments which provide new insight into the core polarization model and which provide techniques for measuring both bound and autoionizing energy levels with microwaves.
Adequacy of damped dynamics to represent the electron-phonon interaction in solids
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
Adequacy of damped dynamics to represent the electron-phonon interaction in solids
NASA Astrophysics Data System (ADS)
Caro, A.; Correa, A. A.; Tamm, A.; Samolyuk, G. D.; Stocks, G. M.
2015-10-01
Time-dependent density functional theory and Ehrenfest dynamics are used to calculate the electronic excitations produced by a moving Ni ion in a Ni crystal in the case of energetic MeV range (electronic stopping power regime), as well as thermal energy meV range (electron-phonon interaction regime). Results at high energy compare well to experimental databases of stopping power, and at low energy the electron-phonon interaction strength determined in this way is very similar to the linear response calculation and experimental measurements. This approach to electron-phonon interaction as an electronic stopping process provides the basis for a unified framework to perform classical molecular dynamics of ion-solid interaction with ab initio type nonadiabatic terms in a wide range of energies.
Adequacy of damped dynamics to represent the electron-phonon interaction in solids
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.
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
Dynamic filling factor in the Super-ACO free electron laser
NASA Astrophysics Data System (ADS)
Nutarelli, D.; Garzella, D.; Couprie, M.-E.; Billardon, M.
1997-02-01
Here, the Free Electron Laser evolution before the start-up from the spontaneous radiation of an undulator, is considered. This analysis is carried on through the dynamical behaviour of the Filling-factor, representing the transverse overlap between the light pulse and the electron bunch. In such a framework, the gain optimization before the laser start-up is presented and more generally applied to low-gain storage-ring free electron lasers, such as on Super-ACO.
An Electron Emission Effect on Dynamics of Laser Ablation
Nastoyashchii, A. F.
2004-03-30
The paper deals with the effect of electron emission on a heat transfer in the area of a plasma critical density (near plasma-solid surface boundary). As is known, experimental data show the limitation of electron thermal conductivity in the mentioned area. In the laser fusion research just the limitation of the heat transfer at target irradiation with long-wave lasers has made application of CO2-lasers unreasonable in spite of their high efficiency. On other hand, as to the applied tasks of laser ablation (e.g. in launching small-scale satellites) the aspect of the CO2-lasers application is being widely discussed. In the paper the mentioned limitation is explained on the basis of classical representations. It is marked, that the heat transfer limitations arise from the conditions of preserving plasma quasi-neutrality at the absorption area boundary where the electron density is close to critical one for the given laser wavelength. Possible mechanisms of the electron emission in the mode of the laser ablation are discussed.
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
Kurayev, Alexander A.; Rak, Alexey O.; Sinitsyn, Anatoly K.
2011-07-01
On the basis of the exact nonlinear theory relativistic TWT and BWO on irregular hollow waveguides with cathode filters-modulators with the account as propagating, and beyond cut-off waves, with the account of losses in walls of a waveguide and inhomogeneity directing an electronic beam magnetostatic fields finds out influence of dynamic stratification influence on efficiency of the generator. Possibility of almost fill compensation the electronic beam dynamic stratification influence on efficiency by optimization of an electronic beam arrangement in inhomogeneous high frequency and magnetic fields and characteristics of the irregular corrugated waveguide is shown. (author)
Restoring electronic coherence/decoherence for a trajectory-based nonadiabatic molecular dynamics
NASA Astrophysics Data System (ADS)
Zhu, Chaoyuan
2016-04-01
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.
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
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.
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.
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.
Distribution and dynamics of electron transport complexes in cyanobacterial thylakoid membranes.
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. PMID:26619924
Distribution and dynamics of electron transport complexes in cyanobacterial thylakoid membranes☆
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
Imaging Excited State Dynamics with 2d Electronic Spectroscopy
NASA Astrophysics Data System (ADS)
Engel, Gregory S.
2012-06-01
Excited states in the condensed phase have extremely high chemical potentials making them highly reactive and difficult to control. Yet in biology, excited state dynamics operate with exquisite precision driving solar light harvesting in photosynthetic complexes though excitonic transport and photochemistry through non-radiative relaxation to photochemical products. Optimized by evolution, these biological systems display manifestly quantum mechanical behaviors including coherent energy transfer, steering wavepacket trajectories through conical intersections and protection of long-lived quantum coherence. To image the underlying excited state dynamics, we have developed a new spectroscopic method allowing us to capture excitonic structure in real time. Through this method and other ultrafast multidimensional spectroscopies, we have captured coherent dynamics within photosynthetic antenna complexes. The data not only reveal how biological systems operate, but these same spectral signatures can be exploited to create new spectroscopic tools to elucidate the underlying Hamiltonian. New data on the role of the protein in photosynthetic systems indicates that the chromophores mix strongly with some bath modes within the system. The implications of this mixing for excitonic transport will be discussed along with prospects for transferring underlying design principles to synthetic systems.
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.
Dynamics of R.F. Captured Electron Cooled Proton Beams
Kells, W.; Mills, F.;
1983-01-01
In the course of electron cooling experiments at the Electron Cooling Ring (ECR) at Fermilab, several peculiar features of the longitudinal phase space of cold protons (200 MeV) captured in R.F. buckets were observed. Here we present the experimental facts, present a simple theory, and summarize computer simulation results which support the theory and facts. The experimental apparatus and measurement techniques have been described elsewhere. R.F. bunching was achieved with a single PPA, loaded cavity gap driven at harmonic number 6({approx} 7.56 MHz) of the revolution frequency. R.F. voltage could be developed across this gap sufficient to entirely capture even the uncooled circulating proton beam ({delta}p/p FWHM = 0.17%).
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.
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.
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
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.
Electron dynamics in the process of mode switching in gyrotrons
Dumbrajs, O.; Kominis, Y.; Nusinovich, G. S.
2009-01-15
The present paper is devoted to the analysis of electron interaction process in the course of gyrotron switching from one mode to another. This analysis is based on the use of the Hamiltonian formalism that allows one to construct Poincare plots for different instants of switching time. The study is carried out for a 170 GHz, MW-class gyrotron for the International Thermonuclear Experimental Reactor (ITER) [ITER web site: http://www.iter.org].
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.
Ultrafast Structural Dynamics of Tertiary Amines upon Electronic Excitation
NASA Astrophysics Data System (ADS)
Cheng, Xinxin; Minitti, Michael P.; Deb, Sanghamitra; Zhang, Yao; Budarz, James; Weber, Peter M.
2011-06-01
The structural response of several tertiary amines to electronic excitation has been investigated using Rydberg Fingerprint Spectroscopy. The 3p Rydberg states are reached by excitation with a 5.93 eV photon while 3s states are populated by electronic relaxation from 3p state. We observe binding energy shifts on ultrafast time scales in all peaks that reflect the structural change of the molecular ion cores. The shifts are in the range of 15 meV to 30 meV, within time scales of less than 500 fs, depending on the specific molecular systems and the nature of the electronic state. In cases where the p states are spectrally separate, the trends of the energy shifts are different for the p_z and p_x_y Rydberg states whereas the p_z and s states are similar. This suggests that the response of the Rydberg states to structural displacements depends on the symmetry. Very fast binding energy shifts, observed on sub-picosecond time scales, are attributed to the structural adjustment from a pyramidal to a planar structure upon Rydberg excitation. The quantitative values of the binding energy shifts can also be affected by laser chirp, which we model using simulations.
Dashdorj, Naranbaatar; Xu, Wu; Cohen, Rachel O; Golbeck, John H; Savikhin, Sergei
2005-02-01
Point mutations were introduced near the primary electron acceptor sites assigned to A0 in both the PsaA and PsaB branches of Photosystem I in the cyanobacterium Synechocystis sp. PCC 6803. The residues Met688PsaA and Met668PsaB, which provide the axial ligands to the Mg2+ of the eC-A3 and eC-B3 chlorophylls, were changed to leucine and asparagine (chlorophyll notation follows Jordan et al., 2001). The removal of the ligand is expected to alter the midpoint potential of the A0/A0- redox pair and result in a change in the intrinsic charge separation rate and secondary electron transfer kinetics from A0- to A1. The dynamics of primary charge separation and secondary electron transfer were studied at 690 nm and 390 nm in these mutants by ultrafast optical pump-probe spectroscopy. The data reveal that mutations in the PsaB branch do not alter electron transfer dynamics, whereas mutations in the PsaA branch have a distinct effect on electron transfer, slowing down both the primary charge separation and the secondary electron transfer step (the latter by a factor of 3-10). These results suggest that electron transfer in cyanobacterial Photosystem I is asymmetric and occurs primarily along the PsaA branch of cofactors. PMID:15542554
Subotnik, Joseph E; Alguire, Ethan C; Ou, Qi; Landry, Brian R; Fatehi, Shervin
2015-05-19
Electronically photoexcited dynamics are complicated because there are so many different relaxation pathways: fluorescence, phosphorescence, radiationless decay, electon transfer, etc. In practice, to model photoexcited systems is a very difficult enterprise, requiring accurate and very efficient tools in both electronic structure theory and nonadiabatic chemical dynamics. Moreover, these theoretical tools are not traditional tools. On the one hand, the electronic structure tools involve couplings between electonic states (rather than typical single state energies and gradients). On the other hand, the dynamics tools involve propagating nuclei on multiple potential energy surfaces (rather than the usual ground state dynamics). In this Account, we review recent developments in electronic structure theory as directly applicable for modeling photoexcited systems. In particular, we focus on how one may evaluate the couplings between two different electronic states. These couplings come in two flavors. If we order states energetically, the resulting adiabatic states are coupled via derivative couplings. Derivative couplings capture how electronic wave functions change as a function of nuclear geometry and can usually be calculated with straightforward tools from analytic gradient theory. One nuance arises, however, in the context of time-dependent density functional theory (TD-DFT): how do we evaluate derivative couplings between TD-DFT excited states (which are tricky, because no wave function is available)? This conundrum was recently solved, and we review the solution below. We also discuss the solution to a second, pesky problem of origin dependence, whereby the derivative couplings do not (strictly) satisfy translation variance, which can lead to a lack of momentum conservation. Apart from adiabatic states, if we order states according to their electronic character, the resulting diabatic states are coupled via electronic or diabatic couplings. The couplings
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.
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.
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. PMID:25956093
Large dynamic range diagnostics for high current electron LINACs
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.
Large dynamic range diagnostics for high current electron LINACs
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.
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.
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.
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.
Exploration of ultra-fast electron dynamics using time-dependent R-matrix theory
NASA Astrophysics Data System (ADS)
van der Hart, Hugo; Rey, Hector; Hassouneh, Ola; Brown, Andrew
2014-05-01
When an atom is subjected to an intense laser field, the full atomic response can involve a collective response involving several electrons. This collective response will be affected by electron-electron repulsion, coupling the overall electron dynamics. In order to investigate this dynamics for a multi-electron system from first principles, we have developed time-dependent R-matrix theory. The theory applies the basic principles of R-matrix theory, in which all interactions between all electrons are taken into account close to the nucleus, but exchange interactions are neglected when one electron has become distanced from the parent atom. In this contribution, we will explain the basic principles of this theory and demonstrate its application to ultra-fast dynamics in C+, and harmonic generation in singly ionised noble-gas atoms. Both studies demonstrate that it is important to go beyond the single-active-electron approximation. This research has been supported by EPSRC UK, and by the EU Initial Training Network CORINF.
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.
Zhang Fengkui; Wu Xiande; Ding Yongjie; Li Hong; Yu Daren
2011-10-15
In Hall thrusters, the electron velocity distribution function is not only depleted at high energies, but also strongly anisotropic. With these electrons interacting with the channel wall, the sheath will be changed in its dynamic characteristics. In the present letter, a two dimensional particle-in-cell code is used to simulate these effects in a collisionless plasma slab. The simulated results indicate that the sheath changes from steady regime to temporal oscillation regime when the electron velocity distribution function alters from isotropy to anisotropy. Moreover, the temporal oscillation sheath formed by the anisotropic electrons has a much greater oscillating amplitude and a much smaller average potential drop than that formed by the isotropic electrons has. The anisotropic electrons are also found to lower the critical value of electron temperature needed for the appearance of the spatial oscillation sheath.
Ultrafast Carrier Dynamics and Hot Electron Extraction in Tetrapod-Shaped CdSe Nanocrystals.
Jing, Pengtao; Ji, Wenyu; Yuan, Xi; Qu, Songnan; Xie, Renguo; Ikezawa, Michio; Zhao, Jialong; Li, Haibo; Masumoto, Yasuaki
2015-04-22
The ultrafast carrier dynamics and hot electron extraction in tetrapod-shaped CdSe nanocrystals was studied by femtosecond transient absorption (TA) spectroscopy. The carriers relaxation process from the higher electronic states (CB2, CB3(2), and CB4) to the lowest electronic state (CB1) was demonstrated to have a time constant of 1.04 ps, resulting from the spatial electron transfer from arms to a core. The lowest electronic state in the central core exhibited a long decay time of 5.07 ns in agreement with the reported theoretical calculation. The state filling mechanism and Coulomb blockade effect in the CdSe tetrapod were clearly observed in the pump-fluence-dependent transient absorption spectra. Hot electrons were transferred from arm states into the electron acceptor molecules before relaxation into core states. PMID:25838148
Dynamic-pressure measurements using an electronically scanned pressure module
NASA Technical Reports Server (NTRS)
Chapin, W. G.
1983-01-01
Frequency response was measured for different lengths and diameters of tubing between a sinusoidal pressure source and a pressure sensing module from an electronically scanned pressure measuring system. Measurements were made for straight runs of both steel and vinyl tubing. For steel tubing, measured results are compared with results calculated by using equations developed by Tijdeman and Bergh. Measurements were also made with a bend in the vinyl tubing at the module. In addition, measurements were made with two coils placed in the tubing near the middle of the run.
Dynamical localization of electrons in an aperiodic superlattice
Luban, M.; Luscombe, J.H.
1998-04-01
We derive the analytical form of the time-dependent wave function for a single-band tight-binding model of independent conduction electrons within an aperiodic semiconductor superlattice, created by modifications in the composition of a single layer of an otherwise periodic superlattice. While the wave function for long times is known to feature both diffusive and localized behavior, the latter originating in the superlattice aperiodicity, we provide quantitative results for these features for all values of the time. {copyright} {ital 1998} {ital The American Physical Society}
Dynamic Void Growth and Shrinkage in Mg under Electron Irradiation
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.
Ultrashort electron pulses as a four-dimensional diagnosis of plasma dynamics.
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. PMID:21034089
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.
NASA Astrophysics Data System (ADS)
Töben, L.; Gundlach, L.; Ernstorfer, R.; Eichberger, R.; Hannappel, T.; Willig, F.; Zeiser, A.; Förstner, J.; Knorr, A.; Hahn, P. H.; Schmidt, W. G.
2005-02-01
Time-dependent two-photon photoemission spectra are used to resolve the femtosecond dynamics of hot electrons at the energetically lowest surface resonance of reconstructed InP(100). Two different cases are studied, where electrons either are lifted into the surface resonance via a direct optical transition or are captured from bulk states. These data are the first of this kind recorded with a time resolution below 70 fs. The microscopic analysis shows that electron-phonon scattering is a major mechanism for electron transfer between surface and bulk states.
NASA Astrophysics Data System (ADS)
Gundlach, Lars; Burfeindt, Bernd; Mahrt, Jürgen; Willig, Frank
2012-08-01
The general case of a heterogeneous electron transfer reaction is realized by ultrafast electron transfer from a photo-excited molecule to a wide continuum of electronic acceptor states. Two different theoretical model calculations addressing the injection dynamics have recently been presented. The first scenario predicts a wide energy distribution for the injected electron via excitations of high-energy vibrational modes in the ionized molecule, whereas the second scenario ascribes the width to thermal fluctuations. We present experimental data at different temperatures and identify the valid injection scenario for perylene/TiO2 systems. The results are discussed in view of recent solar energy conversion scenarios.
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.
Hot and Cold Electron Dynamics Following High-Intensity Laser Matter Interaction
Antici, P.; Fuchs, J.; Mancic, A.; Audebert, P.; Borghesi, M.; Cecchetti, C. A.; Gremillet, L.; Grismayer, T.; Mora, P.; Sentoku, Y.; D'Humieres, E.; Pipahl, A. C.; Toncian, T.; Willi, O.
2008-09-05
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.
NASA Astrophysics Data System (ADS)
Serebryannikov, E. E.; Verhoef, A. J.; Mitrofanov, A.; Baltuška, A.; Zheltikov, A. M.
2009-11-01
The sensitivity of electron tunneling to the phase of an ionizing light field is shown to manifest itself in detectable features in the spectral and temporal evolution of intense few-cycle light pulses in an ionizing medium. An ultrafast buildup of electron density in the regime of tunneling ionization gives rise to a modulation of a few-cycle field wave form and enhances the short-wavelength part of its spectrum. In a low-pressure gas, the signatures of electron tunneling in the evolution of few-cycle pulses can be isolated from the effects related to atomic nonlinear susceptibilities, giving an access to attosecond electron tunneling dynamics.
Hot and cold electron dynamics following high-intensity laser matter interaction.
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
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.
Dynamics of electronically inelastic collisions from 3D Doppler measurements
Suits, A.G.; de Pujo, P.; Sublemontier, O.; Visticot, J.; Berlande, J.; Cuvellier, J.; Gustavsson, T.; Mestdagh, J.; Meynadier, P. ); Lee, Y.T. )
1991-11-25
Flux-velocity contour maps were obtained for the inelastic collision process Ba({sup 1}{ital P}{sub 1})+O{sub 2}N{sub 2}{r arrow}Ba({sup 3}{ital P}{sub 2})+O{sub 2}N{sub 2} from Doppler scans of scattered Ba({sup 3}{ital P}{sub 2}) taken over a range of probe laser directions in a crossed-beam experiment. Collision with O{sub 2} resulted in sharply forward scattered Ba({sup 3}{ital P}{sub 2}), with efficient conversion of inital electronic energy into O{sub 2} internal energy and little momentum transfer. Collision with N{sub 2} was dominated by wide-angle scattering with most of the available electronic energy appearing in product translation. The results suggest the importance of large-impact-parameter collisions and a near-resonant energy transfer in the case of O{sub 2}, while for N{sub 2} close collisions dominate despite the presence of an analogous near-resonant channel. The results represent the first direct experimental demonstration of a near-resonant quenching process.
NASA Astrophysics Data System (ADS)
Li, Run-Ze; Zhu, Pengfei; Chen, Long; Chen, Jie; Cao, Jianming; Sheng, Zheng-Ming; Zhang, Jie
2014-03-01
Ultrafast electron diffraction and microscopy are very promising methods to study transient structural dynamics with atomic spatial-temporal resolution. However, in these laser-pump electron-probe studies of structural dynamics, a transient electric field induced by laser excitation of the sample could deflect probing electrons, which may eventually leads to a misinterpretation of the diffraction data. Here, picosecond structural dynamics and transient surface electric field evolution, excited by femtosecond laser interaction with a metallic thin film, have been observed simultaneously in real time by ultrashort electron pulses in a transmission configuration. By tracing time dependent changes of electron diffraction and deflection angles, these two processes are found to be significantly different and distinguishable in their temporal behavior. This observation provides an effective approach to extract the otherwise obscured ultrafast structural dynamics and may help to improve the spatiotemporal resolution in ultrafast electron diffraction and microscopy studies. This work was supported by the National Basic Research Program of China and the National Natural Science Foundation of China.
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. PMID:23611698
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.
Electron dynamics and harmonic generation in the free-electron laser
Al-Abawi, H.Y.
1982-01-01
A classical theory of the FEL is discussed. This theory uses the Boltzmann distribution to describe the electrons and Maxwell equation to describe the evolution of the laser field. The harmonic expansion of the Boltzmann equation leads to a set of quasi-Bloch equations describing the electron distribution. The behavior of the momentum distribution is discussed theoretically in the small-signal regime of the FEL. The distribution function changes in nontrivial ways. The electron distribution does not only experience a recoil, but is also subject to spread through the amplification process. The recoil plays a relatively minor role compared to the spread. This behavior of the electron distribution may play an important role in the efficiency of the FEL. Free-electron lasers, except for those using helical wigglers, are predicted in most cases to generate higher harmonics, of the fundamental optical frequency, in the forward direction. The basic equations describing this process are derived by using the multiple-scaling perturbation theory, which leads to the slowly-varying Maxwell and Boltzmann equations. Harmonic generation in the FEL offers a possible means to extend the wavelength range of the device towards high frequency. Numerical calculations are shown for CW operation using a linearly polarized wiggler. Higher harmonic emission becomes enhanced as the magnetic field is increased and as the energy spread in the electron beam is reduced. Coherent pulse propagation in the picosecond pulse regime of the FEL is treated. Coherent transient effects such as laser lethargy are discussed. Numerical calculations of the harmonics in the pulsed FEL are presented.
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.
Dynamics of chemical bonding mapped by energy-resolved 4D electron microscopy.
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
Electron-ion dynamics of H(2)(+) in intense laser fields
NASA Astrophysics Data System (ADS)
Khosravi, Shahram
1997-12-01
The interaction of the molecular hydrogen ion H2+ with intense laser fields is currently an area of active investigation. Since this interaction is highly nonlinear, nonperturbative techniques are required, which go beyond Fermi's golden rule and perturbation theory. In previous work, the Born-Oppenheimer approximation has been used to separate the molecular Schrodinger equation into two equations, one for the electron and one for the ions. This approximation has the following important shortcomings: First, it ignores the coupling between the electron dynamics and the ion dynamics, which is an important aspect of the system. Second, in the analysis of the electron dynamics, the ions are assumed to be fixed in space. Our simulations will show that the ions move significantly during the interaction. and that their motion has an important effect on the final outcome of the reaction. The first stage of the present work was the construction of a realistic and quantitatively accurate model for the relevant electronic states, as functions of the internuclear separation R. Then simulations were performed, with the dynamics of the electron and the ions treated through numerical solution of the time-dependent Schrodinger equation and Newton's equation of motion. Various initial conditions for the molecule were assumed, together with different intensities and durations for the laser pulse. Some of the more interesting runs are shown and discussed in this dissertation. We find a rich variety of phenomena, including ion trapping (on a subpicosecond time scale), sudden electronic transitions (as the system follows an adiabatic potential curve), above-threshold dissociation (ATD), bond softening, and harmonic generation (up to order 11 in the present simulations). Many of these phenomena can be understood using a dressed-state picture, or Floquet analysis. However, detailed understanding must be based on the intricate interplay between the dynamics of the electron and the ions, a
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
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.
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.
Lattice dynamics and electronic structure of mixed halofluoride scintillators under high pressure
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.
Electron dynamics and γ and e-e+ production by colliding laser pulses
NASA Astrophysics Data System (ADS)
Jirka, M.; Klimo, O.; Bulanov, S. V.; Esirkepov, T. Zh.; Gelfer, E.; Bulanov, S. S.; Weber, S.; Korn, G.
2016-02-01
The dynamics of an electron bunch irradiated by two focused colliding super-intense laser pulses and the resulting γ and e-e+ production are studied. Due to attractors of electron dynamics in a standing wave created by colliding pulses the photon emission and pair production, in general, are more efficient with linearly polarized pulses than with circularly polarized ones. The dependence of the key parameters on the laser intensity and wavelength allows us to identify the conditions for the cascade development and γ e-e+ plasma creation.
Electron dynamics and γ and e^{-}e^{+} production by colliding laser pulses.
Jirka, M; Klimo, O; Bulanov, S V; Esirkepov, T Zh; Gelfer, E; Bulanov, S S; Weber, S; Korn, G
2016-02-01
The dynamics of an electron bunch irradiated by two focused colliding super-intense laser pulses and the resulting γ and e^{-}e^{+} production are studied. Due to attractors of electron dynamics in a standing wave created by colliding pulses the photon emission and pair production, in general, are more efficient with linearly polarized pulses than with circularly polarized ones. The dependence of the key parameters on the laser intensity and wavelength allows us to identify the conditions for the cascade development and γe^{-}e^{+} plasma creation. PMID:26986432
Domain motions and electron transfer dynamics in 2Fe-superoxide reductase.
Horch, Marius; Utesch, Tillmann; Hildebrandt, Peter; Mroginski, Maria Andrea; Zebger, Ingo
2016-08-17
Superoxide reductases are non-heme iron enzymes that represent valuable model systems for the reductive detoxification of reactive oxygen species. In the present study, we applied different theoretical methods to study the structural dynamics of a prototypical 2Fe-superoxide reductase and its influence on electron transfer towards the active site. Using normal mode and essential dynamics analyses, we could show that enzymes of this type are capable of well-defined, electrostatically triggered domain movements, which may allow conformational proofreading for cellular redox partners involved in intermolecular electron transfer. Moreover, these global modes of motion were found to enable access to molecular configurations with decreased tunnelling distances between the active site and the enzyme's second iron centre. Using all-atom classical molecular dynamics simulations and the tunnelling pathway model, however, we found that electron transfer between the two metal sites is not accelerated under these conditions. This unexpected finding suggests that the unperturbed enzymatic structure is optimized for intramolecular electron transfer, which provides an indirect indication of the biological relevance of such a mechanism. Consistently, efficient electron transfer was found to depend on a distinct route, which is accessible via the equilibrium geometry and characterized by a quasi conserved tyrosine that could enable multistep-tunnelling (hopping). Besides these explicit findings, the present study demonstrates the importance of considering both global and local protein dynamics, and a generalized approach for the functional analysis of these aspects is provided. PMID:27491757
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.
A dynamical approach to non-adiabatic electron transfers at the bio-inorganic interface.
Zanetti-Polzi, Laura; Corni, Stefano
2016-04-21
A methodology is proposed to investigate electron transfer reactions between redox-active biomolecular systems (e.g. a protein) and inorganic surfaces. The whole system is modelled at the atomistic level using classical molecular dynamics - making an extensive sampling of the system's configurations possible - and the energies associated with the redox-active complex reduction are calculated using a hybrid quantum/classical approach along the molecular dynamics trajectory. The non-adiabaticity is introduced a posteriori using a Monte Carlo approach based on the Landau-Zener theory extended to treat a metal surface. This approach thus allows us to investigate the role of the energy fluctuations, determined by the dynamical evolution of the system, as well as the role of non-adiabaticity in affecting the kinetic rate of the electron transfer reaction. Most notably, it allows us to investigate the two contributions separately, hence achieving a detailed picture of the mechanisms that determine the rate. The analysis of the system configurations also allows us to relate the estimated electronic coupling to the structural and dynamic properties of the system. As a test case, the methodology is here applied to study the electron transfer reaction between cytochrome c and a gold surface. The results obtained explain the different electron transfer rates experimentally measured for two different concentrations of proteins on the electrode surface. PMID:27031179
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.
Nonadiabtic electron dynamics in densely quasidegenerate states in highly excited boron cluster.
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
Femtosecond studies of electron dynamics and structure at metal-molecular interfaces
Miller, Andre D.
2002-07-15
Femtosecond angle resolved two photon photoemission spectroscopy is used to study the electronic structure and electron dynamics at interfaces. At interfaces of thiolates chemisorbed on Ag(111), the adsorbate molecular electronic orbitals are observed to be nondispersive at low coverages and become dispersive at higher coverages. This is attributed to a phase transition of the layer. The molecules initially adsorb with their chains parallel to the surface. As the coverage is increased, the molecules order into a layer with the chains standing up from the surface. This closer packing results in a larger overlap between neighboring molecular orbitals and a dispersive electronic state. The lack of a change in the n=1 image potential state electron lifetimes as a function of chain length indicate that the electrons reside in the layer. The n=2 and 3 image potential state electron lifetimes decrease as the chain length is increased. This is attributed to the repulsive potential of the alkyl chains pushing the electron density into the sulfur portion of the layer. At a layer of acetonitrile molecules adsorbed on Ag(111), the image potential state electrons interact strongly with the adsorbate molecular dipoles. The dipoles rotate to solvate the electron, resulting in a decrease of the observed photoemitted electron kinetic energy as a function of time delay between population and photoemission. This is attributed to a change in the local work function resulting from the reorganization of the adsorbate layer molecules. For two layers of acetonitrile adsorbed on the Ag(111) substrate, dynamic electron localization is also observed.
Electronic Spectroscopy and Dynamics of the Acetylene - Complex
NASA Astrophysics Data System (ADS)
Ju, Shan-Shan
The structures, intermolecular forces and excited state dynamics of acetylene(A) cdot Ar complex are investigated by combination of laser induced fluorescence spectroscopy pairwise potential model calculations. Acetylene is linear in the X state while trans-bent in the (A) state. Although only one structure has been known to exist for the acetylene(X) cdot Ar complex, two isomeric structures are determined for the acetylene(A) cdot Ar complex from the rotational band shape analysis of the fluorescence excitation spectra. One of the isomers has the argon sitting in the molecular plane of C _2H_2 (A), 3.77 A away from the center-of-mass of acetylene, the other has the argon 3.71 A above the plane on the C_2 axis. Formulas useful for calculating axis switching angles in non-planar molecules have been derived and applied to the two isomeric structures. It was found that despite the acetylene geometry change from the (X) to the (A) state, the axis switching effect is negligible for the complex spectral calculation. A pair potential model with parameters directly extracted from the ones calculated for ethene (X) cdot Ar is able to produce the two structures. Based on the structures and the calculated potential surface, three of the vdW frequencies are assigned to be: upsilon_{rm stretch } = 28 cm^{-1} for the out-of-plane isomer, upsilon_ {rm bend1} = 11 cm^ {-1} (the in-plane bend) and upsilon_{rm bend2} = 8.5 cm^{-1} (the out -of-plane bend) for the in-plane isomer. The existence of the two isomers allowed the study of the orientation dependence in intersystem crossing (ISC) of acetylene(S _1) induced by interaction with argon. Similar ISC lifetimes (~100 ns) were observed for the two isomers, suggesting that the pi and pi^* orbitals are equally susceptible to spin-changing interactions with Ar.
2012 ELECTRONIC SPECTROSCOPY & DYNAMICS GORDON RESEARCH CONFERENCE, JULY 22-27, 2012
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.
Electron transfer and capture dynamics in ZnSe quantum wells grown on GaAs
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.
Two-photon photoemission and the dynamics of electrons at interfaces
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.
NASA Astrophysics Data System (ADS)
Souto, J.; Alemany, M. M. G.; Gallego, L. J.; Gonzalez, L. E.; Gonzalez, D. J.
2013-03-01
We perform an ab initio molecular dynamics study of the static, dynamic and electronic properties of the liquid Bi-Pb alloy at three concentrations, including the eutectic one. This alloy is of particular technological interest for its possible use as coolant in fast reactors. Our predictions are in good agreement with the available experimental data. In particular, the computed total static structure factors reproduce accurately the neutron diffraction results, and the predicted adiabatic sound velocity and shear viscosity compare well with the experimental values. The partial dynamic structure factors exhibit clear side peaks indicative of propagating density fluctuations, and the longitudinal and transverse dispersion relations show several branches.The electronic density of states show that the liquid Bi-Pb alloy is a good metal, but with strong deviations from the free-electron parabolic curve. Supported by FIS2008-02490/FIS, FIS2008-04894/FIS, VA068A06, GR120, INCITE09E2R206033ES and INCITE08PXIB206107PR
Alemany, Manuel M. G.; Longo, Roberto; Gallego, Luis; Gonzales, D. J.; Gonzales, L. E.; Tiago, Murilo L; Chelikowsky, James
2007-01-01
We performed a comprehensive study of the static, dynamic and electronic properties of liquid Pb at T = 650 kelvins, density 0.0309 angstroms^{-3} by means of 216-particle ab initio molecular dynamics simulations based on a real-space implementation of pseudopotentials constructed within density-functional theory. The predicted results and available experimental data are very in good agreement, which confirms the adequacy of this technique to achieve a reliable description of the behavior of liquid metals, including their dynamic properties. Although some of the computed properties of liquid Pb are similar to those of simple liquid metals, others differ markedly. Our results show that an appropriate description of liquid Pb requires the inclusion of relativistic effects in the determination of the pseudopotentials of Pb.
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. PMID:26911313
Analysis of electron dynamics and two mechanisms in a coaxial magnetic wiggler
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.
How electronic dynamics with Pauli exclusion produces Fermi-Dirac statistics.
Nguyen, Triet S; Nanguneri, Ravindra; Parkhill, John
2015-04-01
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. PMID:25854234
Applications of time-domain spectroscopy to electron-phonon coupling dynamics at surfaces.
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
How electronic dynamics with Pauli exclusion produces Fermi-Dirac statistics
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.
How electronic dynamics with Pauli exclusion produces Fermi-Dirac statistics
NASA Astrophysics Data System (ADS)
Nguyen, Triet S.; Nanguneri, Ravindra; Parkhill, John
2015-04-01
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.
Auer, Benjamin; Soudackov, Alexander V; Hammes-Schiffer, Sharon
2012-07-01
Theoretical approaches for simulating the ultrafast dynamics of photoinduced proton-coupled electron transfer (PCET) reactions in solution are developed and applied to a series of model systems. These processes are simulated by propagating nonadiabatic surface hopping trajectories on electron-proton vibronic surfaces that depend on the solute and solvent nuclear coordinates. The PCET system is represented by a four-state empirical valence bond model, and the solvent is treated either as explicit solvent molecules or as a dielectric continuum, in which case the solvent dynamics is described in terms of two collective solvent coordinates corresponding to the energy gaps associated with electron and proton transfer. The explicit solvent simulations reveal two distinct solvent relaxation time scales, where the faster time scale relaxation corresponds to librational motions of solvent molecules in the first solvation shell, and the slower time scale relaxation corresponds to the bulk solvent dielectric response. The charge transfer dynamics is strongly coupled to both the fast and slow time scale solvent dynamics. The dynamical multistate continuum theory is extended to include the effects of two solvent relaxation time scales, and the resulting coupled generalized Langevin equations depend on parameters that can be extracted from equilibrium molecular dynamics simulations. The implicit and explicit solvent approaches lead to qualitatively similar charge transfer and solvent dynamics for model PCET systems, suggesting that the implicit solvent treatment captures the essential elements of the nonequilibrium solvent dynamics for many systems. A combination of implicit and explicit solvent approaches will enable the investigation of photoinduced PCET processes in a variety of condensed phase systems. PMID:22651684
The electron-furfural scattering dynamics for 63 energetically open electronic states.
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
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.
NASA Astrophysics Data System (ADS)
Elkins, Madeline H.; Williams, Holly L.; Neumark, Daniel M.
2016-05-01
The excited state relaxation dynamics of the solvated electron in H2O and D2O are investigated using time-resolved photoelectron spectroscopy in a liquid microjet. The data show that the initial excited state decays on a time scale of 75 ± 12 fs in H2O and 102 ± 8 fs in D2O, followed by slower relaxation on time scales of 400 ± 70 fs and 390 ± 70 fs that are isotopically invariant within the precision of our measurements. Based on the time evolution of the transient signals, the faster and slower time constants are assigned to p → s internal conversion (IC) of the hydrated electron and relaxation on the ground electronic state, respectively. This assignment is consistent with the non-adiabatic mechanism for relaxation of the hydrated electron and yields an isotope effect of 1.4 ± 0.2 for IC of the hydrated electron.
Crucial role of nuclear dynamics for electron injection in a dye–semiconductor complex
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
Crucial role of nuclear dynamics for electron injection in a dye–semiconductor complex
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 TiO_{2} 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.
NASA Astrophysics Data System (ADS)
Cousineau, S.; Holmes, J. A.; Plum, M. A.; Lu, W.
2011-06-01
The Spallation Neutron Source accelerator utilizes H- charge exchange injection to merge a 1 GeV, 1 MW beam from a linac into an accumulator ring. The design calls for the 545 keV foil-stripped electrons to be absorbed by an electron catcher located below the foil. However, multiple observations of hardware damage caused by stripped electrons indicate that at least a fraction of the electrons are reflected back into the vacuum chamber. This paper presents the results of a 3D computational model employed to simulate the dynamics of foil-stripped electrons, including a surface interaction model for the catcher. Simulation results are compared with experimental observations, and the implications for high power beam operations are discussed.
Wall-plug efficiency and beam dynamics in free-electron lasers using energy recovery linacs
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.
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
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…
NASA Astrophysics Data System (ADS)
Syed, A. Samad; Trontl, V. Mikšić; Ligges, M.; Sakong, S.; Kratzer, P.; Lükermann, D.; Zhou, P.; Avigo, I.; Pfnür, H.; Tegenkamp, C.; Bovensiepen, U.
2015-10-01
The unoccupied electronic structure of quasi-one-dimensional reconstructions of Pb atoms on a Si(557) surface is investigated by means of femtosecond time- and angle-resolved two-photon photoemission. Two distinct unoccupied electronic states are observed at E -EF=3.55 and 3.30 eV, respectively. Density functional theory calculations reveal that these states are spatially located predominantly on the lead wires and that they are energetically degenerated with an energy window of reduced electronic density of states in Si. We further find momentum-averaged lifetimes of 24 and 35 fs of these two states, respectively. The photoemission yield and the population dynamics depend on the electron momentum component perpendicular to the steps of the Si substrate, and the momentum-dependent dynamics cannot be described by means of rate equations. We conclude that momentum- and direction-dependent dephasing of the electronic excitations, likely caused by elastic scattering at the step edges on the vicinal surface, modifies the excited-state population dynamics in this system.
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.
Non-Markov dissipative dynamics of electron transfer in a photosynthetic reaction center
NASA Astrophysics Data System (ADS)
Poddubnyy, V. V.; Glebov, I. O.; Eremin, V. V.
2014-02-01
We consider the dissipative dynamics of electron transfer in the photosynthetic reaction center of purple bacteria and propose a model where the transition between electron states arises only due to the interaction between a chromophore system and the protein environment and is not accompanied by the motion of nuclei of the reaction subsystem. We establish applicability conditions for the Markov approximation in the framework of this model and show that these conditions are not necessarily satisfied in the protein medium. We represent the spectral function of the "system+heat bath" interaction in the form of one or several Gaussian functions to study specific characteristics of non-Markov dynamics of the final state population, the presence of an induction period and vibrations. The consistency of the computational results obtained for non-Markov dynamics with experimental data confirms the correctness of the proposed approach.
Solving non-centrosymmetric two-dimensional crystal structures by dynamic electron diffraction.
Koch, Christoph T
2005-03-01
Despite the fast increase in expertise developed in the field of electron crystallography, dynamic scattering effects still remain a severe obstacle in this field, a hurdle that is being circumvented rather than fully tackled. In this paper, a new way of straightforward interpretation of conventional many-beam zone-axis dynamical electron diffraction patterns is presented that helps to solve the phase problem for non-centrosymmetric two-dimensional crystal structures, in particular if these contain only a few heavier atoms. While the implementation of this method is easiest for fairly weak multiple scattering, its extension to arbitrarily strong dynamical effects is mentioned. A method to obtain high-resolution diffraction data in the presence of specimen bending is proposed. PMID:15724073
Restoring electronic coherence/decoherence for a trajectory-based nonadiabatic molecular dynamics
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
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.
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.
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.
Judith C. Yang; Ralph G. Nuzzo, Duane Johnson, Anatoly Frenkel
2008-07-01
The distinguishing feature of our collaborative program of study is the focus it brings to emergent phenomena originating from the unique structural/electronic environments found in nanoscale materials. We exploit and develop frontier methods of atomic-scale materials characterization based on electron microscopy (Yang) and synchrotron X-ray absorption spectroscopy (Frenkel) that are in turn coupled innately with advanced first principles theory and methods of computational modeling (Johnson). In the past year we have made significant experimental advances that have led to important new understandings of the structural dynamics of what are unquestionably the most important classes of heterogeneous catalysts—the materials used to both produce and mitigate the consequences of the use of liquid hydrocarbon fuels.
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.
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
Teuscher, Joël; Décoppet, Jean-David; Punzi, Angela; Zakeeruddin, Shaik M; Moser, Jacques-E; Grätzel, Michael
2012-12-20
We report a pump-probe spectroscopy study of electron injection rates in dye-sensitized solar cell (DSSC) devices. We examine the case of working devices employing an N719 ruthenium sensitizer and an iodide electrolyte. Electron injection is found to occur mainly on a sub-100 fs time scale, followed by a slower component with a lifetime of 26.9 ps, in accordance with previous reports on model samples. The amplitude of this latter component varies with electrolyte composition from 25 to 9%. The appearance of slower components in the electron injection dynamics may be attributed to an aggregated or weakly bound state of the surface-adsorbed N719 sensitizer. Further measurements are reported varying the cell light bias and load conditions, revealing no influence on electron injection dynamics. No other electron injection event is found to occur up to 1 ns. These results show no evidence for a slowdown of electron injection under working conditions compared to model systems for the electrolytes examined in this study. PMID:26291112
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.
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.
The effect of ULF compressional modes and field line resonances on relativistic electron dynamics
NASA Astrophysics Data System (ADS)
Degeling, A. W.; Rankin, R.; Kabin, K.; Marchand, R.; Mann, I. R.
2007-04-01
The adiabatic, drift-resonant interaction between relativistic, equatorially mirroring electrons and a ULF compressional wave that couples to a field line resonance (FLR) is modelled. Investigations are focussed on the effect of azimuthal localisation in wave amplitude on the electron dynamics. The ULF wave fields on the equatorial plane (r, φ) are modelled using a box model [Zhu, X., Kivelson, M.G., 1988. Analytic formulation and quantitative solutions of the coupled ULF wave problem. J. Geophys. Res. 93(A8), 8602-8612], and azimuthal variations are introduced by adding a discrete spectrum of azimuthal modes. Electron trajectories are calculated using drift equations assuming constant magnetic moment M, and the evolution of the distribution function f(r,φ,M,t) from an assumed initial condition is calculated by assuming f remains constant along electron trajectories. The azimuthal variation in ULF wave structure is shown to have a profound effect on the electron dynamics once a threshold in azimuthal variation is exceeded. Electron energy changes occur that are significantly larger than the trapping width corresponding to the maximum wave amplitude. We show how this can be explained in terms of the overlap of multiple resonance islands, produced by the introduction of azimuthal amplitude variation. This anomalous energisation is characterised by performing parameter scans in the modulation amplitude ɛ and the wave electric field. A simple parametric model for the threshold is shown to give reasonable agreement with the threshold observed in the electron dynamics model. Above the threshold, the radial transport averaged over φ is shown to become diffusive in nature over a timescale of about 25 wave periods. The anomalous energisation described in this paper occurs over the first 15 wave periods, indicating the importance of convective transport in this process.
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.
NASA Astrophysics Data System (ADS)
Fidler, Andrew F.; Singh, Ved P.; Long, Phillip D.; Dahlberg, Peter D.; Engel, Gregory S.
2014-02-01
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.
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.
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.
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.
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.
Dynamic defect correlations dominate activated electronic transport in SrTiO3
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
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
Li, Zheng; Vendrell, Oriol
2016-07-01
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
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.
Direct observation of space charge dynamics by picosecond low-energy electron scattering
NASA Astrophysics Data System (ADS)
Cirelli, C.; Hengsberger, M.; Dolocan, A.; Over, H.; Osterwalder, J.; Greber, T.
2009-01-01
The transient electric field governing the dynamics of space charge is investigated by time- and energy-resolved low-energy electron scattering. The space charge above a copper target is produced by high-intensity femtosecond laser pulses. The pump-probe experiment has a measured temporal resolution of better than 35 ps at 55 eV probe electron energy. The probe electron acceleration due to space charge is reproduced within a 3-dimensional non-relativistic model, which determines an effective number of electrons in the space charge cloud and its initial diameter. Comparison of the simulations with the experiments indicates a Coulomb explosion, which is consistent with transients in the order of 1 ns, the terminal kinetic energy of the cloud and the thermoemission currents predicted by the Richardson-Dushman formula.
Stability of graphene edges under electron beam: equilibrium energetics versus dynamic effects.
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. PMID:22188561
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
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.
Dynamic defect correlations dominate activated electronic transport in SrTiO3.
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
Ultrafast Electron Dynamics in Gold in the Presence of Laser Excited Surface Plasma Waves
Raynaud, M.
2010-02-02
Surface plasmon excitation with ultrashort intense laser pulses enhances efficiently laser absorption in metals and creates local high fields and non-equilibrium hot electrons population that have attractivity for numerous applications such as the development of intense sources of high-energy particles or photons and in the fast ignitor scheme in the framework of inertial fusion. In this context, the knowledge of the dynamics of relaxation of the collective electrons behavior is of importance. Using gold grating, we have investigated electrons relaxation in the presence of laser excited surface plasmon waves using a multiple-wavelengh femtosecond pump-probe technique. The results yield evidence of longer relaxation time in the presence of the collective excitation than that of individual electronic states.
Dynamics of Excess-Electron Transfer through Alternating Adenine:Thymine Sequences in DNA.
Lin, Shih-Hsun; Fujitsuka, Mamoru; Majima, Tetsuro
2015-11-01
This paper presents the results of an investigation into the sequence-dependent excess-electron transfer (EET) dynamics in DNA, which plays an important role in DNA damage/repair. There are many published studies on EET in consecutive adenine:thymine (A:T) sequences (Tn), but those in alternating A:T sequences (ATn) remain limited. Here, two series of functionalized DNA oligomers, Tn and ATn, were synthesized with a strongly electron-donating photosensitizer, a trimer of ethylenedioxythiophene (3 E), and an electron acceptor, diphenylacetylene (DPA). Laser flash photolysis experiments showed that the EET rate constant of AT3 is two times lower than that of T3 due to the lack of π-stacking of Ts in AT3. Thus, it was indicated that excess-electron hopping is affected by the interaction between LUMOs of nucleotides. PMID:26398266
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
Dynamic defect correlated dominate activated electronic transport in SrTiO3
Snijders, Paul C; Sen, Cengiz; McConnell, Michael; Ma, Yingzhong; May, Andrew F; Herklotz, Andreas; Wong, Anthony T; Ward, Thomas 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.
Radiative damping and electron beam dynamics in plasma-based accelerators.
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. PMID:17025550
Structural and dynamical control of the reaction rate in protein electron transfer
NASA Astrophysics Data System (ADS)
Balabin, Ilya A.
Electron transfer (ET) reactions in proteins are key steps in many vital bioenergetic processes, and the reaction rate is known to be highly sensitive to the protein structure in some cases. For most bioenergetic reactions, as described by the Fermi Golden rule, the rate is proportional to a product of the average square of the effective electronic donor to acceptor coupling and a Franck-Condon factor, which accounts for the nuclear control of the energy gap. The nuclear factor is reasonably well described in Marcus theory and its modifications, and this work is focused on the mechanisms that control the effective coupling. About ten years ago, the Pathways model described for the first time how protein environment may control the effective coupling. In this work, a novel theoretical approach is developed to explore the mechanisms of structural and dynamical control beyond the qualitative level of the Pathways model. In Chapter 1, the assumptions of the Pathways model, its limitations and effects of the structure and the electronic Hamiltonian are investigated for model chain-like bridges using the Dyson's equations. In Chapter II, the framework to explore the sensitivity of the effective coupling to quality of the electronic Hamiltonian, the interference among the dominant pathways and the bridge dynamics is presented. This analysis employs the Green's function technique and includes combined molecular dynamics and electronic structure calculations. Finally, in Chapter III, this framework is tested on the bacterial photosynthetic reaction center, and the mechanisms of the structural and dynamical control for different ET steps are discussed.
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.
Time-domain ab initio studies of photoinduced electron dynamics in nanoscale semiconductors
NASA Astrophysics Data System (ADS)
Prezhdo, Oleg
2010-03-01
Design of novel materials for energy harvesting and storage requires an understanding of the dynamical response on the nanometer scale. We have developed state-of-the-art non-adiabatic molecular dynamics techniques and implemented them within time-dependent density functional theory in order to model the ultrafast processes in these materials at the atomistic level and in real time. Quantum dots (QD) are quasi-zero dimensional structures with a unique combination of molecular and bulk properties. As a result, QDs exhibit new physical phenomena such as the electron-phonon relaxation bottleneck and carrier multiplication, which have the potential to greatly increase solar cell efficiencies. Photoinduced charge separation across molecular/bulk interfaces drives the dye-sensitized semiconductor solar cell. A subject of active research, it creates many challenges due to the stark differences between the quantum states of molecular and periodic systems, as well as the different sets of theories and experimental tools used by physicists and chemists. Our time-domain atomistic simulations create a detailed picture of these materials. By comparing and contrasting their properties, we provide a unifying description of quantum dynamics on the nanometer scale, resolve several highly debated issues, and generate theoretical guidelines for development of novel systems for energy harvesting and storage. [4pt] [1] O. V. Prezhdo ``Photoinduced dynamics in semiconductor quantum-dots: insights from time-domain ab initio studies'', Acc. Chem. Res., available online.[0pt] [2] O. V. Prezhdo, W. R. Duncan, V. V. Prezhdo, ``Photoinduced electron dynamics at semiconductor interfaces: a time-domain ab initio prospective'', Prog. Surf. Science, 84, 39 (2009).[0pt] [3] O. V. Prezhdo, et al., ``Dynamics of the photoexcited electron at the chromophore-semiconductor interface'', Acc. Chem. Res., 41, 339 (2008).[0pt] [4] W. R. Duncan, O. V. Prezhdo, ``Theoretical studies of photoinduced electron
Fukumoto, Keiki; Onda, Ken; Yamada, Yuki; Matsuki, Takashi; Mukuta, Tatsuhiko; Tanaka, Sei-ichi; Koshihara, Shin-ya
2014-08-01
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. PMID:25173274
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.
Influence of the nonlinear dynamic plasma screening on the electron-dust collision in dusty plasmas
Ki, Dae-Han; Jung, Young-Dae
2012-05-07
The nonlinear dynamic plasma screening effects on the elastic electron-dust grain collision are investigated in dusty plasmas. The results show that the nonlinear dynamic screening effect significantly increases the magnitude of the eikonal phase shift. It is also found that the magnitude of the phase shift decreases with an increase of the thermal energy. In addition, it is found that the differential eikonal cross section shows the oscillatory behavior, and the oscillating peaks approach to the collision center with increasing thermal energy. It is also found that the total eikonal cross section decreases with an increase of the thermal energy.
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.
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.
NASA Astrophysics Data System (ADS)
Gans, Timo
2015-09-01
Radio-frequency atmospheric pressure plasmas are versatile and efficient sources for reactive species at ambient room temperature. The non-equilibrium chemical kinetics is initiated and determined by the electron dynamics. Due to the strongly collisional environment and associated short electron energy relaxation times the electron dynamics can be tailored using multi-frequency power coupling techniques, enabling separate control of key parameters like electron density and electron mean energy. Details of the chemical kinetics depend on the feedgas composition and desired application. Measurements and predictive simulations of key reactive species are equally challenging due to the strongly collisional environment and their multi-scale nature in space and time. The most promising approach is the exploitation of complementary advantages in direct measurements combined with specifically designed numerical simulations. The employed diagnostic techniques include picosecond laser spectroscopy, synchrotron VUV spectroscopy, IR absorption spectroscopy and nanosecond optical imaging spectroscopy. The presentation will focus on examples of He-O2-N2 mixtures for bio-medical applications and He/Ar-CO2 mixtures for CO2 conversion into value-added chemicals. This work has been supported by the UK EPSRC (EP/K018388/1 & EP/H003797/1).
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
NASA Astrophysics Data System (ADS)
Tomadin, Andrea; Brida, Daniele; Cerullo, Giulio; Ferrari, Andrea C.; Polini, Marco
2013-07-01
We present a combined analytical and numerical study of the early stages (sub-100-fs) of the nonequilibrium dynamics of photoexcited electrons in graphene. We employ the semiclassical Boltzmann equation with a collision integral that includes contributions from electron-electron (e-e) and electron-optical phonon interactions. Taking advantage of circular symmetry and employing the massless Dirac fermion (MDF) Hamiltonian, we are able to perform an essentially analytical study of the e-e contribution to the collision integral. This allows us to take particular care of subtle collinear scattering processes—processes in which incoming and outgoing momenta of the scattering particles lie on the same line—including carrier multiplication (CM) and Auger recombination (AR). These processes have a vanishing phase space for two-dimensional MDF bare bands. However, we argue that electron-lifetime effects, seen in experiments based on angle-resolved photoemission spectroscopy, provide a natural pathway to regularize this pathology, yielding a finite contribution due to CM and AR to the Coulomb collision integral. Finally, we discuss in detail the role of physics beyond the Fermi golden rule by including screening in the matrix element of the Coulomb interaction at the level of the random phase approximation (RPA), focusing in particular on the consequences of various approximations including static RPA screening, which maximizes the impact of CM and AR processes, and dynamical RPA screening, which completely suppresses them.
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.
Resolving the role of femtosecond heated electrons in ultrafast spin dynamics
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
Dynamics of Soft Nanomaterials Captured by Transmission Electron Microscopy in Liquid Water
Proetto, Maria T.; Rush, Anthony M.; Chien, Miao-Ping; Baeza, Patricia Abellan; Patterson, Joseph P.; Thompson, Matthew P.; Olson, Norman H.; Moore, Curtis E.; Rheingold, Arnold L.; Andolina, Christopher; Millstone, Jill; Howell, Stephen B.; Browning, Nigel D.; Evans, James E.; Gianneschi, Nathan C.
2014-01-01
In this paper we present in situ transmission electron microscopy (TEM) of synthetic polymeric nanoparticles with emphasis on capturing motion in a solvated, aqueous state. The nanoparticles studied were obtained from the direct polymerization of a Pt(II)-containing monomer. The resulting structures provided sufficient contrast for facile imaging in situ. We contend that this technique will quickly become essential in the characterization of analogous systems, especially where dynamics are of interest in the solvated state. We describe the preparation of the synthetic micellar nanoparticles together with their characterization and motion in liquid water with comparison to conventional electron microscopy analyses. PMID:24422495
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.
Dynamical Characteristics of Rydberg Electrons Released by a Weak Electric Field.
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
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.
Dynamical characteristics of Rydberg electrons released by a weak electric field
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.
NASA Astrophysics Data System (ADS)
Singh, Raj; Bhatt, Pragya; Yadav, Namita; Shanker, R.
2011-05-01
We describe a new experimental setup for studying the fragmentation dynamics of molecules induced by the impact of keV electrons using the well-known technique of recoil ion momentum spectroscopy. The apparatus consists of mainly a time- and position-sensitive multi-hit particle detector for ion analysis and a channel electron multiplier detector for detecting the ejected electrons. Different components of the setup and the relevant electronics for data acquisition are described in detail with their working principles. In order to verify the reliable performance of the setup, we have recorded the collision-induced ionic spectra of the CO2 molecule by the impact of keV electrons. Information about the ion pairs of CO+:O+, C+:O+ and O+:O+ resulting from dissociative ionizing collisions of 20 and 26 keV electrons with a dilute gaseous target of CO2 molecules has been obtained. Under conditions of the present experiment, the momentum resolutions of the spectrometer for the combined momenta of CO+ and O+ ions in the direction of the time-of-flight axis and perpendicular to the direction of an electron beam are found to be 10.0 ± 0.2 and 15.0 ± 0.3 au, respectively.
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. PMID:26691822
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.
Li Hong; Liu Hui; Yu Daren; Zhang Fengkui
2010-07-15
It is demonstrated that the features of measured electron current profile in the near-wall region of a Hall effect thruster are mainly due to the substantive breakdown of electron Hall drifts caused by the azimuthal field of the two-dimensional dynamic sheath. This kind of cross-field diffusion shows its close connection with the anomalous electron transport.
Hole Surface Trapping Dynamics Directly Monitored by Electron Spin Manipulation in CdS Nanocrystals.
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
NASA Astrophysics Data System (ADS)
Jooya, Hossein Z.; Telnov, Dmitry A.; Chu, Shih-I.
2016-06-01
Electron multiple recollision dynamics under intense midinfrared laser fields is studied by means of the de Broglie-Bohm framework of Bohmian mechanics. Bohmian trajectories contain all the information embedded in the time-dependent wave function. This makes the method suitable to investigate the coherent dynamic processes for which the phase information is crucial. In this study, the appearance of the subpeaks in the high-harmonic-generation time-frequency profiles and the asymmetric fine structures in the above-threshold ionization spectrum are analyzed by the comprehensive and intuitive picture provided by Bohmian mechanics. The time evolution of the individual electron trajectories is closely studied to address some of the major structural features of the photoelectron angular distributions.
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.
Quantum dynamics of electronic transitions with Gauss-Hermite wave packets.
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
Decay dynamics of N2O under the impact of fast electrons
NASA Astrophysics Data System (ADS)
Khan, Arnab; Misra, Deepankar
2016-03-01
We experimentally investigate the two- and three-body breakup dynamics of N2O{}q+ (q=2,3) under the impact of fast (5 keV) electrons using a coincidence momentum spectroscopy technique. The kinetic energy release (KER) distributions have been derived from the measured momenta for various breakup channels. The present values are found to be quite different from a previously reported high energy electron impact study. From the measured momentum vectors, the geometry of the precursor molecular ion prior to the fragmentation has been reconstructed. The three-body decay dynamics of N2O3+ has been studied using Dalitz plots and Newton diagrams with a view of concerted and sequential decay mechanisms. It is found that the sequential process is present along with the concerted process for the N2O3+ \\to N+ + NO2+ \\quad \\to N+ + N+ + O+ channel.
Electron beam dynamics in the DARHT-II linear induction accelerator
Ekdahl, Carl A; Abeyta, Epifanio O; Aragon, Paul; Archuleta, Rita; Cook, Gerald; Dalmas, Dale; Esquibel, Kevin; Gallegos, Robert A; Garnett, Robert; Harrison, James F; Johnson, Jeffrey B; Jacquez, Edward B; Mccuistian, Brian T; Montoya, Nicholas A; Nath, Subrata; Nielsen, Kurt; Oro, David; Prichard, Benjamin; Rowton, Lawrence; Sanchez, Manolito; Scarpetti, Raymond; Schauer, Martin M; Seitz, Gerald; Schulze, Martin; Bender, Howard A; Broste, William B; Carlson, Carl A; Frayer, Daniel K; Johnson, Douglas E; Tom, C Y; Trainham, C; Genoni, Thomas; Hughes, Thomas; Toma, Carsten
2008-01-01
The DARHT-II linear induction accelerator (LIA) accelerates a 2-kA electron beam to more than 17 MeV. The beam pulse has a greater than 1.5-microsecond flattop region over which the electron kinetic energy is constant to within 1%. The beam dynamics are diagnosed with 21 beam-position monitors located throughout the injector, accelerator, and after the accelerator exit, where we also have beam imaging diagnostics. We discuss the tuning of the injector and accelerator, and present data for the resulting beam dynamics. We discuss the tuning procedures and other methods used to minimize beam motion, which is undesirable for its application as a bremsstrahlung source for multi-pulse radiography of exlosively driven hydrodynamic experiments. We also present beam stability measurements, which we relate to previous stability experiments at lower current and energy.
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.
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.
Nonradiative Relaxation in Real-Time Electronic Dynamics OSCF2: Organolead Triiodide Perovskite.
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
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.
Electron-Nuclear Spin Dynamics in a Mesoscopic Solid-State Quantum Computer
Berman, G.P.; Campbell, D.K.; Doolen, G.D.; Nagaev, K.E.
1998-12-07
We numerically simulate the process of nuclear spin measurement in Kane's quantum computer. For this purpose, we model the quantum dynamics of two coupled nuclear spins located on {sup 31}P donors implanted in Si. We estimate the minimum time of measurement necessary for the reliable transfer of quantum information from the nuclear spin subsystem to the electronic one and the probability of error for typical values of external noise.
NASA Astrophysics Data System (ADS)
Sebastianelli, F.; Gianturco, F. A.
2012-02-01
The quantum dynamics of low-energy free electrons colliding with linear carbonaceous species like HC3N and HC5N is examined to identify the locations and structural features of their metastable negative ions (resonant compound states of the colliding partners) with the aim of suggesting, at the molecular level, the possible mechanisms of anionic stabilization which lead to the several stable species observed in the interstellar and circumstellar media in connection with polyyne structures.
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.
Strain dependent electron spin dynamics in bulk cubic GaN
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.
Dynamic Motions of Ion Acoustic Waves in Plasmas with Superthermal Electrons
NASA Astrophysics Data System (ADS)
Saha, Asit; Chatterjee, Prasanta; Wong, C. S.
2015-12-01
The dynamic motions of ion acoustic waves an unmagnetized plasma with superthermal ( q-nonextensive) electrons are investigated employing the bifurcation theory of planar dynamical systems through direct approach. Using traveling wave transformation and initial conditions, basic equations are transformed to a planar dynamical system. Using numerical computations, all possible phase portraits of the dynamical system are presented. Corresponding to homoclinic and periodic orbits of the phase portraits, two new analytical forms of solitary and periodic wave solutions are derived depending on the nonextensive parameter q and speed v of the traveling wave. Considering an external periodic perturbation, the quasiperiodic and chaotic motions of ion acoustic waves are presented. Depending upon different ranges of nonextensive parameter q, the effect of q is shown on quasiperiodic and chaotic motions of ion acoustic waves with fixed value of v. It is seen that the unperturbed dynamical system has the solitary and periodic wave solutions, but the perturbed dynamical system has the quasiperiodic and chaotic motions with same values of parameters q and v.
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.
NASA Astrophysics Data System (ADS)
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.
Sezer, Deniz; Freed, Jack H; Roux, Benoit
2008-09-01
Simulating electron spin resonance (ESR) spectra directly from molecular dynamics simulations of a spin-labeled protein necessitates a large number (hundreds or thousands) of relatively long (hundreds of nanoseconds) trajectories. To meet this challenge, we explore the possibility of constructing accurate stochastic models of the spin label dynamics from atomistic trajectories. A systematic, two-step procedure, based on the probabilistic framework of hidden Markov models, is developed to build a discrete-time Markov chain process that faithfully captures the internal spin label dynamics on time scales longer than about 150 ps. The constructed Markov model is used both to gain insight into the long-lived conformations of the spin label and to generate the stochastic trajectories required for the simulation of ESR spectra. The methodology is illustrated with an application to the case of a spin-labeled poly alanine alpha helix in explicit solvent. PMID:18698714
NASA Astrophysics Data System (ADS)
Garashchuk, Sophya
2014-03-01
A massively parallel, direct quantum molecular dynamics method is described. The method combines a quantum trajectory (QT) representation of the nuclear wavefunction discretized into an ensemble of trajectories with an electronic structure (ES) description of electrons, namely using the Density Functional Tight Binding (DFTB) theory. Quantum nuclear effects are included into the dynamics of the nuclei via quantum corrections to the classical forces. To reduce computational cost and increase numerical accuracy, the quantum corrections to dynamics resulting from localization of the nuclear wavefunction are computed approximately and included into selected degrees of freedom representing light particles where the quantum effects are expected to be the most pronounced. A massively parallel implementation, based on the Message Passing Interface allows for efficient simulations of ensembles of thousands of trajectories at once. The QTES-DFTB dynamics approach is employed to study the role of quantum nuclear effects on the interaction of hydrogen with a model graphene sheet, revealing that neglect of nuclear effects can lead to an overestimation of adsorption. Supported by the National Science Foundation and the Petroleum Research Fund of the American Chemical Society.
Zhang, Yuyuan; Dood, Jordan; Beckstead, Ashley A; Li, Xi-Bo; Nguyen, Khiem V; Burrows, Cynthia J; Improta, Roberto; Kohler, Bern
2015-06-18
Femtosecond time-resolved IR spectroscopy is used to investigate the excited-state dynamics of a dinucleotide containing an 8-oxoguanine anion at the 5'-end and neutral adenine at the 3'-end. UV excitation of the dinucleotide transfers an electron from deprotonated 8-oxoguanine to its π-stacked neighbor adenine in less than 1 ps, generating a neutral 8-oxoguanine radical and an adenine radical anion. These species are identified by the excellent agreement between the experimental and calculated IR difference spectra. The quantum efficiency of this ultrafast charge shift reaction approaches unity. Back electron transfer from the adenine radical anion to the 8-oxguanine neutral radical occurs in 9 ps, or approximately 6 times faster than between the adenine radical anion and the 8-oxoguanine radical cation (Zhang, Y. et al. Proc. Natl. Acad. Sci. U.S.A. 2014, 111, 11612-11617). The large asymmetry in forward and back electron transfer rates is fully rationalized by semiclassical nonadiabatic electron transfer theory. Forward electron transfer is ultrafast because the driving force is nearly equal to the reorganization energy, which is estimated to lie between 1 and 2 eV. Back electron transfer is highly exergonic and takes place much more slowly in the Marcus inverted region. PMID:25660103
High Dynamic Range Pixel Array Detector for Scanning Transmission Electron Microscopy.
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
Dynamics of the OH group and the electronic structure of liquid alcohols
Schreck, Simon; Pietzsch, Annette; Kunnus, Kristjan; Kennedy, Brian; Quevedo, Wilson; Miedema, Piter S.; Wernet, Philippe; Föhlisch, Alexander
2014-01-01
In resonant inelastic soft x-ray scattering (RIXS) from molecular and liquid systems, the interplay of ground state structural and core-excited state dynamical contributions leads to complex spectral shapes that partially allow for ambiguous interpretations. In this work, we dissect these contributions in oxygen K-edge RIXS from liquid alcohols. We use the scattering into the electronic ground state as an accurate measure of nuclear dynamics in the intermediate core-excited state of the RIXS process. We determine the characteristic time in the core-excited state until nuclear dynamics give a measurable contribution to the RIXS spectral profiles to τdyn = 1.2 ± 0.8 fs. By detuning the excitation energy below the absorption resonance we reduce the effective scattering time below τdyn, and hence suppress these dynamical contributions to a minimum. From the corresponding RIXS spectra of liquid methanol, we retrieve the “dynamic-free” density of states and find that it is described solely by the electronic states of the free methanol molecule. From this and from the comparison of normal and deuterated methanol, we conclude that the split peak structure found in the lone-pair emission region at non-resonant excitation originates from dynamics in the O–H bond in the core-excited state. We find no evidence that this split peak feature is a signature of distinct ground state structural complexes in liquid methanol. However, we demonstrate how changes in the hydrogen bond coordination within the series of linear alcohols from methanol to hexanol affect the split peak structure in the liquid alcohols. PMID:26798783
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.
Surface residues dynamically organize water bridges to enhance electron transfer between proteins
de la Lande, Aurélien; Babcock, Nathan S.; Řezáč, Jan; Sanders, Barry C.; Salahub, Dennis R.
2010-01-01
Cellular energy production depends on electron transfer (ET) between proteins. In this theoretical study, we investigate the impact of structural and conformational variations on the electronic coupling between the redox proteins methylamine dehydrogenase and amicyanin from Paracoccus denitrificans. We used molecular dynamics simulations to generate configurations over a duration of 40 ns (sampled at 100-fs intervals) in conjunction with an ET pathway analysis to estimate the ET coupling strength of each configuration. In the wild-type complex, we find that the most frequently occurring molecular configurations afford superior electronic coupling due to the consistent presence of a water molecule hydrogen-bonded between the donor and acceptor sites. We attribute the persistence of this water bridge to a “molecular breakwater” composed of several hydrophobic residues surrounding the acceptor site. The breakwater supports the function of nearby solvent-organizing residues by limiting the exchange of water molecules between the sterically constrained ET region and the more turbulent surrounding bulk. When the breakwater is affected by a mutation, bulk solvent molecules disrupt the water bridge, resulting in reduced electronic coupling that is consistent with recent experimental findings. Our analysis suggests that, in addition to enabling the association and docking of the proteins, surface residues stabilize and control interprotein solvent dynamics in a concerted way. PMID:20547871
NASA Astrophysics Data System (ADS)
Fromhold, Mark; Greenaway, Mark; Alexeeva, Natalia; Balanov, Alexander; Makarovsky, Oleg; Patane, Amalia; Gaifullin, Marat; Kusmartsev, Feo
We show in both measurements and calculations that a tilted magnetic field can transform the structure and THz dynamics of charge domains in a biased semiconductor superlattice (SL). In SLs, at critical field values, when the Bloch frequency equals the cyclotron frequency corresponding to the magnetic field component along the SL axis, the semiclassical electron motion changes abruptly from localized stable trajectories to unbounded chaotic paths, which propagate rapidly through the SL. This delocalisation of the electron creates a series of sharp resonant peaks in drift velocity-field characteristics, which were detected in previous DC current-voltage measurements. We show that these additional peaks can create multiple propagating charge domains, shaped by both the strength and tilt angle of the magnetic field. As a result, the tilted magnetic field generates AC currents whose magnitude and frequencies are far higher than with no magnetic field applied. Chaos-assisted single-electron transport induced by the interplay between cyclotron and Bloch motion therefore provides a mechanism for controlling the collective dynamics of miniband electrons, and thus enhancing the high frequency response of SLs.
Hot electron dynamics at semiconductor surfaces: Implications for quantum dot photovoltaics
NASA Astrophysics Data System (ADS)
Tisdale, William A., III
Finding a viable supply of clean, renewable energy is one of the most daunting challenges facing the world today. Solar cells have had limited impact in meeting this challenge because of their high cost and low power conversion efficiencies. Semiconductor nanocrystals, or quantum dots, are promising materials for use in novel solar cells because they can be processed with potentially inexpensive solution-based techniques and because they are predicted to have novel optoelectronic properties that could enable the realization of ultra-efficient solar power converters. However, there is a lack of fundamental understanding regarding the behavior of highly-excited, or "hot," charge carriers near quantum-dot and semiconductor interfaces, which is of paramount importance to the rational design of high-efficiency devices. The elucidation of these ultrafast hot electron dynamics is the central aim of this Dissertation. I present a theoretical framework for treating the electronic interactions between quantum dots and bulk semiconductor surfaces and propose a novel experimental technique, time-resolved surface second harmonic generation (TR-SHG), for probing these interactions. I then describe a series of experimental investigations into hot electron dynamics in specific quantum-dot/semiconductor systems. A two-photon photoelectron spectroscopy (2PPE) study of the technologically-relevant ZnO(1010) surface reveals ultrafast (sub-30fs) cooling of hot electrons in the bulk conduction band, which is due to strong electron-phonon coupling in this highly polar material. The presence of a continuum of defect states near the conduction band edge results in Fermi-level pinning and upward (n-type) band-bending at the (1010) surface and provides an alternate route for electronic relaxation. In monolayer films of colloidal PbSe quantum dots, chemical treatment with either hydrazine or 1,2-ethanedithiol results in strong and tunable electronic coupling between neighboring quantum dots
Dynamical correlation effects on structure factor of spin-polarized two-dimensional electron gas
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.
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.
Exact Potential Driving the Electron Dynamics in Enhanced Ionization of H2+
NASA Astrophysics Data System (ADS)
Khosravi, Elham; Abedi, Ali; Maitra, Neepa T.
2015-12-01
It was recently shown that the exact factorization of the electron-nuclear wave function allows the construction of a Schrödinger equation for the electronic system, in which the potential contains exactly the effect of coupling to the nuclear degrees of freedom and any external fields. Here we study the exact potential acting on the electron in charge-resonance enhanced ionization in a model one-dimensional H2+ molecule. We show there can be significant differences between the exact potential and that used in the traditional quasistatic analyses, arising from nonadiabatic coupling to the nuclear system, and that these are crucial to include for accurate simulations of time-resolved ionization dynamics and predictions of the ionization yield.
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.
Self-Consistent 3D Modeling of Electron Cloud Dynamics and Beam Response
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.
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.
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.
Reeves, Kyle G; Schleife, André; Correa, Alfredo A; Kanai, Yosuke
2015-10-14
The role of surface termination on phonon-mediated relaxation of an excited electron in quantum dots was investigated using first-principles simulations. The surface terminations of a silicon quantum dot with hydrogen and fluorine atoms lead to distinctively different relaxation behaviors, and the fluorine termination shows a nontrivial relaxation process. The quantum confined electronic states are significantly affected by the surface of the quantum dot, and we find that a particular electronic state dictates the relaxation behavior through its infrequent coupling to neighboring electronic states. Dynamical fluctuation of this electronic state results in a slow shuttling behavior within the manifold of unoccupied electronic states, controlling the overall dynamics of the excited electron with its characteristic frequency of this shuttling behavior. The present work revealed a unique role of surface termination, dictating the hot electron relaxation process in quantum-confined systems in the way that has not been considered previously. PMID:26331672
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
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.
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
Nanoscale heat transport via electrons and phonons by molecular dynamics simulations
NASA Astrophysics Data System (ADS)
Lin, Keng-Hua
Nanoscale heat transport has become a crucial research topic due to the growing importance of nanotechnology for manufacturing, energy conversion, medicine and electronics. Thermal transport properties at the nanoscale are distinct from the macroscopic ones since the sizes of nanoscale features, such as free surfaces and interfaces, are comparable to the wavelengths and mean free paths of the heat carriers (electrons and phonons), and lead to changes in thermal transport properties. Therefore, understanding how the nanoscale features and energy exchange between the heat carriers affect thermal transport characteristics are the goals of this research. Molecular dynamics (MD) is applied in this research to understand the details of nanoscale heat transport. The advantage of MD is that the size effect, anharmonicity, atomistic structure, and non-equilibrium behavior of the system can all be captured since the dynamics of atoms are described explicitly in MD. However, MD neglects the thermal role of electrons and therefore it is unable to describe heat transport in metal or metal-semiconductor systems accurately. To address this limitation of MD, we develop a method to simulate electronic heat transport by implementing electronic degrees of freedom to MD. In this research, nanoscale heat transport in semiconductor, metal, and metal-semiconductor systems is studied. Size effects on phonon thermal transport in SiGe superlattice thin films and nanowires are studied by MD. We find that, opposite to the macroscopic trend, superlattice thin films can achieve lower thermal conductivity than nanowires at small scales due to the change of phonon nature caused by adjusting the superlattice periodic length and specimen length. Effects of size and electron-phonon coupling rate on thermal conductivity and thermal interface resistivity in Al and model metal-semiconductor systems are studied by MD with electronic degrees of freedom. The results show that increasing the specimen
Vibrationally resolved optical spectra and ultrafast electronic relaxation dynamics of diamantane.
Röhr, Merle I S; Mitrić, Roland; Petersen, Jens
2016-03-28
We present theoretical simulations of the vibrationally resolved photoabsorption and photoemission spectra of diamantane combined with nonadiabatic dynamics simulations in order to identify the state responsible for the measured photoluminescence of diamantane and to determine the mechanism and the time-scales of the electronic state relaxation. Diamantane is a prototype representative of the diamondoid class of hydrocarbons which have recently gained significant interest due to their unique electronic properties. This molecule is characterised by an almost dark first excited state, which therefore cannot be directly excited. Moreover, the calculated vertical transition from the geometrically relaxed first excited state to the ground state also bears no intensity. However, recent experiments suggest that the observed photoluminescence originates from the lowest excited state. We have performed spectral simulations in the frame of the Herzberg-Teller approximation for vibronic transitions, which goes beyond the Franck-Condon approximation of constant transition dipole moments and takes into account their linear dependence on the geometrical deformations. In this way, the available experimental spectrum could be fully reproduced, resolving the issue about the origin of the photoluminescence. Moreover, the photoemission from the first excited state also implies that ultrafast nonradiative processes have to take place after the initial excitation of the bright electronic states. We have determined the mechanism and time-scales of these relaxation processes by performing nonadiabatic dynamics simulations in the manifold of s- and p-type Rydberg excited states. The simulations demonstrate that the lowest excited electronic state of diamantane gains significant population from higher-lying states already after several hundreds of femtoseconds. Thus, our dynamics simulations combined with spectra calculated using the Herzberg-Teller approximation allow us to fully explain
Gilmore, Joel; McKenzie, Ross H
2008-03-20
A biomolecular chromophore can be viewed as a quantum system with a small number of degrees of freedom interacting with an environment (the surrounding protein and solvent) which has many degrees of freedom, the majority of which can be described classically. The system-environment interaction can be described by a spectral density for a spin-boson model. The quantum dynamics of electronic excitations in the chromophore are completely determined by this spectral density, which is of great interest for describing quantum decoherence and quantum measurements. Specifically, the spectral density determines the time scale for the "collapse" of the wave function of the chromophore due to continuous measurement of its quantum state by the environment. Although of fundamental interest, there very few physical systems for which the spectral density has been determined experimentally and characterized. In contrast, here, we give the parameters for the spectral densities for a wide range of chromophores, proteins, and solvents. Expressions for the spectral density are derived for continuum dielectric models of the chromophore environment. There are contributions to the spectral density from each component of the environment: the protein, the water bound to the protein, and the bulk solvent. Each component affects the quantum dynamics of the chromophore on distinctly different time scales. Our results provide a natural description of the different time scales observed in ultrafast laser spectroscopy, including three pulse photon echo decay and dynamic Stokes shift measurements. We show that even if the chromophore is well separated from the solvent by the surrounding protein, ultrafast solvation can be still be dominated by the solvent. Consequently, we suggest that the subpicosecond solvation observed in some biomolecular chromophores should not necessarily be assigned to ultrafast protein dynamics. The magnitude of the chromophore-environment coupling is sufficiently strong
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
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.
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.
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.
Suga, Mitsuo; Nishiyama, Hidetoshi; Konyuba, Yuji; Iwamatsu, Shinnosuke; Watanabe, Yoshiyuki; Yoshiura, Chie; Ueda, Takumi; Sato, Chikara
2011-12-01
Although conventional electron microscopy (EM) requires samples to be in vacuum, most chemical and physical reactions occur in liquid or gas. The Atmospheric Scanning Electron Microscope (ASEM) can observe dynamic phenomena in liquid or gas under atmospheric pressure in real time. An electron-permeable window made of pressure-resistant 100 nm-thick silicon nitride (SiN) film, set into the bottom of the open ASEM sample dish, allows an electron beam to be projected from underneath the sample. A detector positioned below captures backscattered electrons. Using the ASEM, we observed the radiation-induced self-organization process of particles, as well as phenomena accompanying volume change, including evaporation-induced crystallization. Using the electrochemical ASEM dish, we observed tree-like electrochemical depositions on the cathode. In silver nitrate solution, we observed silver depositions near the cathode forming incidental internal voids. The heated ASEM dish allowed observation of patterns of contrast in melting and solidifying solder. Finally, to demonstrate its applicability for monitoring and control of industrial processes, silver paste and solder paste were examined at high throughput. High resolution, imaging speed, flexibility, adaptability, and ease of use facilitate the observation of previously difficult-to-image phenomena, and make the ASEM applicable to various fields. PMID:22088441
Pandey, Kavita; Yadav, Pankaj; Singh, Deobrat; Gupta, Sanjeev K; Sonvane, Yogesh; Lukačević, Igor; Kim, Joondong; Kumar, Manoj
2016-01-01
In the present paper, the nature of electronic states and transport properties of nanostructured flower-like molybdenum disulphide grown by hydrothermal route has been studied. The band structure, electronic nature of charge, thermodynamics and the limit of phonon scattering through density functional theory (DFT) has also been studied. The band tail states, dynamics of trap states and transport of carriers was investigated through intensive impedance spectroscopy analysis. The direct fingerprint of density and band tail state is analyzed from the capacitance plot as capacitance reflects the capability of a semiconductor to accept or release the charge carriers with a corresponding change in its Fermi potential levels. A recently introduced infrared photo-carrier radiometry and density functional perturbation theory (DFPT) techniques have been used to determine the temperature dependence of carrier mobility in flower type-MoS2. The present study illustrates that a large amount of trapped charges leads to an underestimation of the measured effective mobility and the potential of the material. Thus, a continuous engineering effort is required to improve the quality of fabricated nanostructures for its potential applications. PMID:27615369
Parks, Joel H; Semrouni, David; Clavaguéra, Carine; Ohanessian, Gilles
2013-02-14
Recent time-resolved lifetime measurements studied the quenching of the fluorescence emitted by a dye covalently bound to the desolvated peptide Dye-Pro(4)-Arg(+)-Trp. This peptide sequence was chosen for study since intramolecular interactions constrain all large-scale fluctuations except for those of the interacting dye and Trp side chain. It was shown that quenching occurred as a result of interaction between the excited dye and tryptophan side chain. These measurements exhibited a temperature dependence that suggested the quenching mechanism was related to electron transfer. This paper presents a comparison of the experimental quenching rate with the Marcus electron transfer model performed with molecular dynamics (MD) calculations. Taking advantage of the AMOEBA force field that explicitly includes polarizability ensures that the intramolecular electrostatic and polarization interactions in this desolvated peptide ion are treated realistically. MD calculations identify both large-scale fluctuations between conformations as well as small-scale fluctuations within a conformation that are shown to be correlated with torsional dynamics of the Trp side chain. Trajectories of the Dye-Trp distance identify the occurrence of close separations required for efficient electron transfer. The temperature dependence of the quenching rate closely follows the rate predicted by the Marcus electron transfer model within uncertainties resulting from statistical averages. Estimates of the energy parameters characterizing the Marcus model indicate the electronic coupling matrix element and the reaction free energy derived from the fits are consistent with published values for transfer in polyproline bridged peptides. These calculations help to provide a molecular basis for investigating conformational changes in desolvated biomolecular ions by fluorescence quenching measurements. PMID:23297809
Femtosecond few- to single-electron point-projection microscopy for nanoscale dynamic imaging.
Bainbridge, A R; Barlow Myers, C W; Bryan, W A
2016-03-01
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
Femtosecond few- to single-electron point-projection microscopy for nanoscale dynamic imaging
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
Intra-protein hydrogen bonding is dynamically stabilized by electronic polarization
NASA Astrophysics Data System (ADS)
Duan, Li L.; Mei, Ye; Zhang, Qing G.; Zhang, John Z. H.
2009-03-01
Molecular dynamics (MD) simulation has been carried out to study dynamical stability of intra-protein hydrogen bonds based on two set of atomic charges, the standard AMBER charge and the polarized protein-specific charge (PPC). The latter is derived from quantum mechanical calculation for protein in solution using a recently developed molecular fractionation with conjugate caps-Poisson-Boltzmann (MFCC-PB) approach and therefore includes electronic polarization effect of the protein at native structure. MD simulations are performed for a number of benchmark proteins containing helix and/or beta sheet secondary structures. The computational result shows that occupancy percentage of hydrogen bonds averaged over simulation time, as well as the number of hydrogen bonds as a function of simulation time, is consistently higher under PPC than AMBER charge. In particular, some intra-protein hydrogen bonds are found broken during MD simulation using AMBER charge but they are stable using PPC. The breaking of some intra-protein hydrogen bonds in AMBER simulation is responsible for deformation or denaturing of some local structures of proteins during MD simulation. The current study provides strong evidence that hydrogen bonding is dynamically more stable using PPC than AMBER charge, highlighting the stabilizing effect of electronic polarization on protein structure.
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. PMID:26416435
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.
Dynamics of a mesoscopic nuclear spin ensemble interacting with an optically driven electron spin
NASA Astrophysics Data System (ADS)
Stanley, M. J.; Matthiesen, C.; Hansom, J.; Le Gall, C.; Schulte, C. H. H.; Clarke, E.; Atatüre, M.
2014-11-01
The ability to discriminate between simultaneously occurring noise sources in the local environment of semiconductor InGaAs quantum dots, such as electric and magnetic field fluctuations, is key to understanding their respective dynamics and their effect on quantum dot coherence properties. We present a discriminatory approach to all-optical sensing based on two-color resonance fluorescence of a quantum dot charged with a single electron. Our measurements show that local magnetic field fluctuations due to nuclear spins in the absence of an external magnetic field are described by two correlation times, both in the microsecond regime. The nuclear spin bath dynamics show a strong dependence on the strength of resonant probing, with correlation times increasing by a factor of 4 as the optical transition is saturated. We interpret the behavior as motional averaging of both the Knight field of the resident electron spin and the hyperfine-mediated nuclear spin-spin interaction due to optically induced electron spin flips.
Simulative research on the anode plasma dynamics in the high-power electron beam diode
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.
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.
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.
Bogner, Lea; Yang, Zechao; Corso, Martina; Fitzner, Roland; Bäuerle, Peter; Franke, Katharina J; Pascual, José Ignacio; Tegeder, Petra
2015-10-28
Dicyanovinyl (DCV)-substituted oligothiophenes are promising donor materials in vacuum-processed small-molecule organic solar cells. Here, we studied the structural and the electronic properties of DCV-dimethyl-pentathiophene (DCV5T-Me2) adsorbed on Au(111) from submonolayer to multilayer coverages. Using a multi-technique experimental approach (low-temperature scanning tunneling microscopy/spectroscopy (STM/STS), atomic force microscopy (AFM), and two-photon photoemission (2PPE) spectroscopy), we determined the energetic position of several affinity levels as well as ionization potentials originating from the lowest unoccupied molecular orbitals (LUMO) and the highest occupied molecular orbitals (HOMO), evidencing a transport gap of 1.4 eV. Proof of an excitonic state was found to be a spectroscopic feature located at 0.6 eV below the LUMO affinity level. With increasing coverage photoemission from excitonic states gains importance. We were able to track the dynamics of several electronically excited states of multilayers by means of femtosecond time-resolved 2PPE. We resolved an intriguing relaxation dynamics involving four processes, ranging from sub-picosecond (ps) to several hundred ps time spans. These show a tendency to increase with increasing coverage. The present study provides important parameters such as energetic positions of transport levels as well as lifetimes of electronically excited states, which are essential for designing organic-molecule-based optoelectronic devices. PMID:26414934
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
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
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
RELEC Experiment on board Vernov Satellite: Relativistic Electron Flux Dynamics in Near-Earth Space
NASA Astrophysics Data System (ADS)
Svertilov, Sergiey
2015-04-01
The main goal of RELEC mission is study of magnetosphere relativistic electron precipitation with it possible acting on the upper atmosphere and ionosphere as well as the monitor observation of radiation and electromagnetic environment in the near-Earth Space. The RELEC set of instruments includes two identical detectors of X- and gamma-rays of high temporal resolution and sensitivity (DRGE-1 & DRGE-2), three axe directed detectors of energetic electrons and protons DRGE-3, UV TLE imager MTEL, UV detector DUV, low-frequency analyser LFA, radio-frequency analyser RFA, module of electronics intended for commands and data collection BE. The small satellite now named Vernov with RELEC instruments was successfully launched July, 8 2014. The mission orbit is solar-synchronous with apogee 830 km, perigee 640 km, inclination 98.4o and orbital period about 100 min. The total data output is about 1.2 Gbyte per day. The fluxes and spectra of electrons in the wide energy range from 0.2 to 15 MeV are measured with the use of three detectors with axe normally directed to each other: to the local zenith, opposite to the satellite velocity vector and along the direction added two previous to the Cartesian system. Due to such detector system it is possible to estimate the electron flux anisotropy. The wide dynamical range from ~1 up to 104 part/cm2s and fine time resolution (~10 mcs) allows observations of trapped, quasi-trapped and precipitated electron flux and spectral variations in different areas in the near-Earth space including low L-shells. Comparative analysis of electron fluxes measured by RELEC with experimental data on electron detection in the experiments on board the spacecraft Electro-L with geostationary orbit, and Meteor-M2 with 800 km altitude circular polar orbit similar to Vernov allows to reconstruct the energetic electron spatial distribution in the near-Earth space. A comparison will be held for periods of moderate geomagnetic disturbances of August 26
Modeling Earth's Outer Radiation Belt Electron Dynamics---Radial Diffusion, Heating, and Loss
NASA Astrophysics Data System (ADS)
Tu, Weichao
belt electrons at low altitudes demonstrate that the adiabatic flux drop of electrons during the storm main phase is both altitude and storm dependent. During the main phase of a moderate geomagnetic storm, due solely to adiabatic effects a satellite at low altitude sees either zero electron flux or a fractional flux drop depending on its altitude. To physically quantify the radial diffusion rate, we use power spectral density and global mode structure of the Ultra-Low-Frequency (ULF) waves, which are derived from the Lyon-Fedder-Mobarry (LFM) MHD simulation and validated by field data from real satellites. The calculated total diffusion rate is shown to be dominated by the contribution from magnetic field perturbations, and much less from the electric field. Fast diffusion generally occurs when solar wind dynamic pressure is high or nightside geomagnetic activity is strong and with higher diffusion rates at higher L regions. Work performed in this thesis provides realistic loss rate and radial diffusion rate of radiation belt electrons, as well as a comprehensive Fokker-Planck model that can take the loss and radial diffusion rates as inputs and then determine the internal heating rate with less uncertainty. By this approach, we will be able to quantitatively understand the relative contribution of radial diffusion, wave heating, and loss to the variations of radiation belt electrons.
NASA Astrophysics Data System (ADS)
Kondoh, Takafumi; Kashima, Hiroaki; Yang, Jinfeng; Yoshida, Yoichi; Tagawa, Seiichi
2008-10-01
In intensity-modulated radiation therapy (IMRT), the aim is to deliver reduced doses of radiation to normal tissue. As a step toward IMRT, we examined dynamic optical modulation of an electron beam produced by a photocathode RF gun. Images on photomasks were transferred onto a photocathode by relay imaging. The resulting beam was controlled by a remote mirror. The modulated electron beam maintained its shape on acceleration, had a fine spatial resolution, and could be moved dynamically by optical methods.
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.
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.
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.
Modeling dynamical electron scattering with Bethe potentials and the scattering matrix.
Wang, A; De Graef, M
2016-01-01
Bethe potentials were introduced by Bethe in 1928 as a first order perturbation approach to reducing the number of diffracted beams in dynamical electron scattering problems. The approach starts from the Bloch wave representation, and uses a threshold criterion to split the diffracted beams into two subsets, namely strong and weak beams. Since the use of Bloch wave based Bethe potentials for defect simulations is somewhat tedious, this paper applies the perturbation approach to the scattering matrix formalism, which is more readily adaptable for defect image simulations. The size of the dynamical matrix, and hence the computation time, can be reduced significantly. A threshold criterion for the separation of scattered beams into strong and weak sets is introduced. A general guideline in setting the threshold for strong or weak beam selection is discussed along with several parameters that may influence the threshold values, such as atomic number, accelerating voltage, structure complexity, incident beam tilt and temperature. PMID:26433091
Caballero, Karla; Akella, Ram
2015-01-01
In this paper, we propose a framework to dynamically estimate the probability that a patient is readmitted after he is discharged from the ICU and transferred to a lower level care. We model this probability as a latent state which evolves over time using Dynamical Linear Models (DLM). We use as an input a combination of numerical and text features obtained from the patient Electronic Medical Records (EMRs). We process the text from the EMRs to capture different diseases, symptoms and treatments by means of noun phrases and ontologies. We also capture the global context of each text entry using Statistical Topic Models. We fill out the missing values using a Expectation Maximization based method (EM). Experimental results show that our method outperforms other methods in the literature terms of AUC, sensitivity and specificity. In addition, we show that the combination of different features (numerical and text) increases the prediction performance of the proposed approach. PMID:26958282
Ultrafast time dynamics studies of periodic lattices with free electron laser radiation
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.
Numerical bound state electron dynamics of carbon dioxide in the strong-field regime.
Smith, Stanley M; Romanov, Dmitri A; Li, Xiaosong; Sonk, Jason A; Schlegel, H Bernhard; Levis, Robert J
2010-02-25
Time-dependent Hartree-Fock simulations for a linear triatomic molecule (CO(2)) interacting with a short IR (1.63 eV) three-cycle pulse reveal that the carrier-envelope shape and phase are the essential field parameters determining the bound state electron dynamics during and after the laser-molecule interaction. Analysis of the induced dipole oscillation reveals that the envelope shape (Gaussian or trapezoidal) controls the excited state population distribution. Varying the carrier envelope phase for each of the two pulse envelope shapes considerably changes the excited state populations. Increasing the electric field amplitude alters the relative populations of the excited states, generally exciting higher states. A windowed Fourier transform analysis of the dipole evolution during the laser pulse reveals the dynamics of state excitation and in particular state coupling as the laser intensity increases. PMID:20113001
Reconstruction of correlation-driven electron-hole dynamics by high-harmonic-generation spectroscopy
NASA Astrophysics Data System (ADS)
Leeuwenburgh, Jonathan; Cooper, Bridgette; Averbukh, Vitali; Marangos, Jonathan P.; Ivanov, Misha
2014-09-01
We present detailed analysis of the recently proposed technique of high-order-harmonic generation spectroscopy of correlation-driven electron hole dynamics in atoms and molecules. This novel technique resolves Auger-type processes with attosecond-scale resolution by clocking the decay process with high-harmonic generation. The harmonic generation is driven by an attosecond, XUV pump pulse and a long-duration, infrared pulse. We present the strong-field-approximation-based theory of such an XUV-initiated high-order-harmonic generation process. We detail different ways of recovering the hole survival probability by altering experimental parameters to change the time-energy mapping of the harmonics. The various reconstruction methods are then simulated for M4,5NN Auger decay in krypton and molecular-orbital breakdown dynamics in trans-butadiene and propanal.
Control of spin dynamics in a two-dimensional electron gas by electromagnetic dressing
NASA Astrophysics Data System (ADS)
Pervishko, A. A.; Kibis, O. V.; Morina, S.; Shelykh, I. A.
2015-11-01
We solved the Schrödinger problem for a two-dimensional electron gas (2DEG) with the Rashba spin-orbit interaction in the presence of a strong high-frequency electromagnetic field (dressing field). The found eigenfunctions and eigenenergies of the problem are used to describe the spin dynamics of the dressed 2DEG within the formalism of the density matrix response function. Solving the equations of spin dynamics, we show that the dressing field can switch the spin relaxation in the 2DEG between the cases corresponding to the known Elliott-Yafet and D'yakonov-Perel' regimes. As a result, the spin properties of the 2DEG can be tuned by a high-frequency electromagnetic field. The present effect opens an unexplored way for controlling the spin with light and, therefore, forms the physical prerequisites for creating light-tuned spintronics devices.
Haxton, D.; Adaniya, H.; Slaughter, D. S.; Rudek, B.; Osipov, T.; Weber, T.; Rescigno, T. N.; McCurdy, C. W.; Belkacem, A.
2011-08-11
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 configurations.
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}#5;) and OH ({sup 2}{Sigma}#6;), 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#12;gurations.
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.
Wang, Zhu-Jun; Weinberg, Gisela; Zhang, Qiang; Lunkenbein, Thomas; Klein-Hoffmann, Achim; Kurnatowska, Michalina; Plodinec, Milivoj; Li, Qing; Chi, Lifeng; Schloegl, R; Willinger, Marc-Georg
2015-02-24
This work highlights the importance of in situ experiments for an improved understanding of graphene growth on copper via metal-catalyzed chemical vapor deposition (CVD). Graphene growth inside the chamber of a modified environmental scanning electron microscope under relevant low-pressure CVD conditions allows visualizing structural dynamics of the active catalyst simultaneously with graphene nucleation and growth in an unparalleled way. It enables the observation of a complete CVD process from substrate annealing through graphene nucleation and growth and, finally, substrate cooling in real time and nanometer-scale resolution without the need of sample transfer. A strong dependence of surface dynamics such as sublimation and surface premelting on grain orientation is demonstrated, and the influence of substrate dynamics on graphene nucleation and growth is presented. Insights on the growth mechanism are provided by a simultaneous observation of the growth front propagation and nucleation rate. Furthermore, the role of trace amounts of oxygen during growth is discussed and related to graphene-induced surface reconstructions during cooling. Above all, this work demonstrates the potential of the method for in situ studies of surface dynamics on active metal catalysts. PMID:25584770
Linear and nonlinear dynamics of electron temperature gradient mode in non-Maxwellian plasmas
Zakir, U.; Qamar, A.; Haque, Q.
2013-05-15
The effect of non-Maxwellian distributed ions on electron temperature gradient mode is investigated. The linear dispersion relation of η{sub e}−mode is obtained which shows that the behavior of this mode changes in the presence of superthermal ions. The growth rate of η{sub e}−mode driven linear instability is found and is observed to modify due to nonthermal ions. However, it is found that this leaves the electron energy transport coefficient unchanged. In the nonlinear regime, a dipolar vortex solution is derived which indicates that the dynamic behavior of the vortices changes with the inclusion of kappa distributed ions. The importance of present study with respect to space and laboratory plasmas is also pointed out.
Douguet, N; Slaughter, D S; Adaniya, H; Belkacem, A; Orel, A E; Rescigno, T N
2015-10-14
We present a combined experimental and theoretical investigation of the dynamics and angular dependence of dissociative electron attachment to methane. We show that a triply degenerate (T2) Feshbach resonance is responsible for the broad 10 eV dissociation peak in methane. This resonance alone is shown to correlate asymptotically to the various dissociation channels observed experimentally. The molecular-frame entrance amplitude for electron attachment is calculated for each component of the threefold degenerate resonance. By investigating the topology of the anion potential energy surfaces, we deduce the main pathways to two- and three-body breakup channels involving both bond scission and bond formation. The computed fragment angular distributions reproduce the main trends of the experimental measurements. PMID:26371546
Coherent spin dynamics of donor bound electrons in GaAs
NASA Astrophysics Data System (ADS)
Phelps, Carey; O'Leary, Shannon; Prineas, John; Wang, Hailin
2011-08-01
We report experimental studies of coherent spin dynamics of donor-bound electrons in high-purity GaAs by using transient differential transmission. The donor-bound exciton transitions, which are not visible in the linear absorption spectrum, are spectrally resolved in the nonlinear differential transmission spectra. The spin beats in the transient differential transmission response, arising from electron spin precession in an external magnetic field, are investigated with the pump and probe coupling to various donor-bound exciton transitions. The spectral dependence of the spin beats provides important information on the polarization selection rule for the underlying donor-bound exciton transitions. The polarization selection rules deduced from these experiments indicate that contributions from higher-energy donor-bound exciton transitions can severely limit the effectiveness of optical spin control using mechanisms such as polarization-dependent optical Stark shifts.
NASA Astrophysics Data System (ADS)
Kawahara, Kazuaki; Shirasawa, Tetsuroh; Lin, Chun-Liang; Nagao, Ryo; Tsukahara, Noriyuki; Takahashi, Toshio; Arafune, Ryuichi; Kawai, Maki; Takagi, Noriaki
2016-09-01
We have investigated the atomic structure of the "multilayer silicene" grown on the Ag(111) single crystal surface by using low energy electron diffraction (LEED) and scanning tunneling microscopy (STM). We measured the intensity of the LEED spot as a function of the incident electron energy (I-V curve) and analyzed the I-V curve using a dynamical LEED theory. We have found that the Si(111)(√{ 3} ×√{ 3})-Ag model well reproduces the I-V curve whereas the models consisting of the honeycomb structure of Si do not. The bias dependence of the STM image of multilayer silicene agrees with that of the Si(111)(√{ 3} ×√{ 3})-Ag reconstructed surface. Consequently, we have concluded that the multilayer silicene grown on Ag(111) is identical to the Si(111)(√{ 3} ×√{ 3})-Ag reconstructed structure.
Nonlinear electron dynamics of gold ultrathin films induced by intense terahertz waves
Minami, Yasuo Takeda, Jun; Katayama, Ikufumi; Dao, Thang Duy; Nagao, Tadaaki; Kitajima, Masahiro
2014-12-15
Linear and nonlinear electron dynamics of polycrystalline gold (Au) ultrathin films with thicknesses ranging from 1.4 to 5.8 nm were investigated via transmittance terahertz (THz) spectroscopy with intense electric field transients. We prepared ultrathin films with low surface roughness formed on a Si–(7 × 7) reconstructed surface, leading to the observation of monotonic decrease in THz transmittance with respect to film thickness. Furthermore, at all tested thicknesses, the transmittance decreased nonlinearly by 10%–30% with the application if high-intensity THz electric fields. Based on a Drude-model analysis, we found a significant decrease in the damping constant induced by the THz electric field, indicating that electrons are driven beyond the polycrystalline grain boundaries in Au thin films, and consequently leading to the suppression of the electron–boundary scattering rate.