Imaging and spectromicroscopy of photocarrier electron dynamics in C60 fullerene thin films
NASA Astrophysics Data System (ADS)
Shibuta, Masahiro; Yamagiwa, Kana; Eguchi, Toyoaki; Nakajima, Atsushi
2016-11-01
We have employed a two-photon photoelectron emission microscopy (2P-PEEM) to observe the photocarrier electron dynamics in an organic thin film of fullerene (C60) formed on a highly oriented pyrolytic graphite with a spatial resolution of ca. 135 nm. In this approach, photocarrier electrons in C60 single-layer islands generated by the first pump photon are detected by the second probe photon. These spectromicroscopic observations conducted over a 100 × 100 nm2 region of C60 islands consistently reproduced the macroscopic two-photon photoemission spectrum of fully covered C60 monolayer film, where the energy of photocarrier electron in the islands was +0.9 eV relative to the Fermi level. Time-resolved 2P-PEEM revealed that the photocarrier electron decayed from the monolayered C60 islands into the substrate with a time constant of 470 ± 30 fs.
NASA Astrophysics Data System (ADS)
Shibuta, Masahiro; Yamamoto, Kazuo; Ohta, Tsutomu; Nakaya, Masato; Eguchi, Toyoaki; Nakajima, Atsushi
2016-10-01
Time-resolved two-photon photoemission (TR-2PPE) spectroscopy is employed to probe the electronic states of a C60 fullerene film formed on highly oriented pyrolytic graphite (HOPG), acting as a model two-dimensional (2D) material for multi-layered graphene. Owing to the in-plane sp2-hybridized nature of the HOPG, the TR-2PPE spectra reveal the energetics and dynamics of photocarriers in the C60 film: after hot excitons are nascently formed in C60 via intramolecular excitation by a pump photon, they dissociate into photocarriers of free electrons and the corresponding holes, and the electrons are subsequently detected by a probe photon as photoelectrons. The decay rate of photocarriers from the C60 film into the HOPG is evaluated to be 1.31 × 1012 s‑1, suggesting a weak van der Waals interaction at the interface, where the photocarriers tentatively occupy the lowest unoccupied molecular orbital (LUMO) of C60. The photocarrier electron dynamics following the hot exciton dissociation in the organic thin films has not been realized for any metallic substrates exhibiting strong interactions with the overlayer. Furthermore, the thickness dependence of the electron lifetime in the LUMO reveals that the electron hopping rate in C60 layers is 3.3 ± 1.2 × 1013 s‑1.
Shibuta, Masahiro; Yamamoto, Kazuo; Ohta, Tsutomu; Nakaya, Masato; Eguchi, Toyoaki; Nakajima, Atsushi
2016-01-01
Time-resolved two-photon photoemission (TR-2PPE) spectroscopy is employed to probe the electronic states of a C60 fullerene film formed on highly oriented pyrolytic graphite (HOPG), acting as a model two-dimensional (2D) material for multi-layered graphene. Owing to the in-plane sp2-hybridized nature of the HOPG, the TR-2PPE spectra reveal the energetics and dynamics of photocarriers in the C60 film: after hot excitons are nascently formed in C60 via intramolecular excitation by a pump photon, they dissociate into photocarriers of free electrons and the corresponding holes, and the electrons are subsequently detected by a probe photon as photoelectrons. The decay rate of photocarriers from the C60 film into the HOPG is evaluated to be 1.31 × 1012 s−1, suggesting a weak van der Waals interaction at the interface, where the photocarriers tentatively occupy the lowest unoccupied molecular orbital (LUMO) of C60. The photocarrier electron dynamics following the hot exciton dissociation in the organic thin films has not been realized for any metallic substrates exhibiting strong interactions with the overlayer. Furthermore, the thickness dependence of the electron lifetime in the LUMO reveals that the electron hopping rate in C60 layers is 3.3 ± 1.2 × 1013 s−1. PMID:27775005
Hot photocarrier dynamics in organic solar cells.
Lane, P A; Cunningham, P D; Melinger, J S; Esenturk, O; Heilweil, E J
2015-07-16
Photocurrent in an organic solar cell is generated by a charge transfer reaction between electron donors and acceptors. Charge transfer is expected to proceed from thermalized states, but this picture has been challenged by recent studies that have investigated the role of hot excitons. Here we show a direct link between excess excitation energy and photocarrier mobility. Charge transfer from excited donor molecules generates hot photocarriers with excess energy coming from the offset between the lowest unoccupied molecular orbital of the donor and that of the acceptor. Hot photocarriers manifest themselves through a short-lived spike in terahertz photoconductivity that decays on a picosecond timescale as carriers thermalize. Different dynamics are observed when exciting the acceptor at its absorption edge to a thermalized state. Charge transfer in this case generates thermalized carriers described by terahertz photoconductivity dynamics consisting of an instrument-limited rise to a long-lived signal.
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.
Photocarrier recombination dynamics in perovskite CH3NH3PbI3 for solar cell applications.
Yamada, Yasuhiro; Nakamura, Toru; Endo, Masaru; Wakamiya, Atsushi; Kanemitsu, Yoshihiko
2014-08-20
Using time-resolved photoluminescence and transient absorption measurements at room temperature, we report excitation-intensity-dependent photocarrier recombination processes in thin films made from the organo-metal halide perovskite semiconductor CH3NH3PbI3 for solar-cell applications. The photocarrier dynamics are well described by a simple rate equation including single-carrier trapping and electron-hole radiative recombination. This result provides clear evidence that the free-carrier model is better than the exciton model for interpreting the optical properties of CH3NH3PbI3. The observed large two-carrier recombination rate suggests the promising potential of perovskite semiconductors for optoelectronic device applications. Our findings provide the information about the dynamical behaviors of photoexcited carriers that is needed for developing high-efficiency perovskite solar cells.
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)
Tanibuchi, T.; Kada, T.; Asahi, S.; Watanabe, D.; Kaizu, T.; Harada, Y.; Kita, T.
2016-11-01
We studied time-resolved photocarrier transport through InAs/GaAs quantum dot superlattice (QDSL) solar cells (SCs) using time-of-flight spectroscopy with an optical probe QD structure beneath the QDSL. Carriers optically pumped in the top p -GaAs layer were transported through the intrinsic layer, including the QDSLs, before arriving at the probe QDs. The photoexcited carrier density significantly influenced the time-resolved photoluminescence (PL) of the QDSLs and probe QDs. The time-resolved PL profile of the probe QDs indicated that excitation densities in excess of 25 nJ /c m2 drastically decreased the rise time, suggesting rapid carrier transport through the QDSLs. This was also confirmed by QDSL carrier transport dynamics, for which the PL intensity of the excited states decayed rapidly above this excitation power density, 25 nJ /c m2 , while the ground state remained constant. These results demonstrate that filling the ground states of QDSLs and starting to populate the excited state miniband accelerates carrier transport in QDSL SCs. Furthermore, according to two-step photon absorption measurements taken with a 1.3-μm infrared laser light source, electrons play a key role in the generation of extra photocurrent by sub-band-gap photon irradiation.
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
Photo-Carrier Multi-Dynamical Imaging at the Nanometer Scale in Organic and Inorganic Solar Cells.
Fernández Garrillo, Pablo A; Borowik, Łukasz; Caffy, Florent; Demadrille, Renaud; Grévin, Benjamin
2016-11-16
Investigating the photocarrier dynamics in nanostructured and heterogeneous energy materials is of crucial importance from both fundamental and technological points of view. Here, we demonstrate how noncontact atomic force microscopy combined with Kelvin probe force microscopy under frequency-modulated illumination can be used to simultaneously image the surface photopotential dynamics at different time scales with a sub-10 nm lateral resolution. The basic principle of the method consists in the acquisition of spectroscopic curves of the surface potential as a function of the illumination frequency modulation on a two-dimensional grid. We show how this frequency-spectroscopy can be used to probe simultaneously the charging rate and several decay processes involving short-lived and long-lived carriers. With this approach, dynamical images of the trap-filling, trap-delayed recombination and nongeminate recombination processes have been acquired in nanophase segregated organic donor-acceptor bulk heterojunction thin films. Furthermore, the spatial variation of the minority carrier lifetime has been imaged in polycrystalline silicon thin films. These results establish two-dimensional multidynamical photovoltage imaging as a universal tool for local investigations of the photocarrier dynamics in photoactive materials and devices.
NASA Astrophysics Data System (ADS)
Quang Phuong, Le; Braly, Ian L.; Katahara, John K.; Hillhouse, Hugh W.; Kanemitsu, Yoshihiko
2017-10-01
Mixed-halide perovskites, whose bandgap energies can be widely controlled through choice of composition, are promising for various optoelectronic applications. Herein, we report the photocarrier recombination dynamics in mixed-halide CH3NH3Pb(I1‑ x Br x )3 perovskite films with different Br contents. We observed small changes in the single-carrier trapping rate with respect to the Br content. In contrast, the two-carrier radiative and three-carrier Auger recombination rates increased significantly with the Br content. These increases in the multicarrier recombination rates likely originated from the enhancement of the Coulomb interactions between electrons and holes caused by incorporating Br. Our findings are useful for designing mixed-halide perovskite-based optoelectronic devices.
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.
Spatial-Temporal Imaging of Anisotropic Photocarrier Dynamics in Black Phosphorus
NASA Astrophysics Data System (ADS)
Liao, Bolin; Zhao, Huan; Najafi, Ebrahim; Yan, Xiaodong; Tian, He; Tice, Jesse; Minnich, Austin J.; Wang, Han; Zewail, Ahmed H.
2017-06-01
As an emerging single elemental layered material with a low symmetry in-plane crystal lattice, black phosphorus (BP) has attracted significant research interest owing to its unique electronic and optoelectronic properties, including its widely tunable bandgap, polarization dependent photoresponse and highly anisotropic in-plane charge transport. Despite extensive study of the steady-state charge transport in BP, there has not been direct characterization and visualization of the hot carriers dynamics in BP immediately after photoexcitation, which is crucial to understanding the performance of BP-based optoelectronic devices. Here we use the newly developed scanning ultrafast electron microscopy (SUEM) to directly visualize the motion of photo-excited hot carriers on the surface of BP in both space and time. We observe highly anisotropic in-plane diffusion of hot holes, with a 15-times higher diffusivity along the armchair (x-) direction than that along the zigzag (y-) direction. Our results provide direct evidence of anisotropic hot carrier transport in BP and demonstrate the capability of SUEM to resolve ultrafast hot carrier dynamics in layered two-dimensional materials.
Photo-carrier and Electronic Studies of Silicon-Doped GaAs Grown by MBE Using PCR
NASA Astrophysics Data System (ADS)
Villada, J. A.; Jiménez-Sandoval, S.; López-López, M.; Mendoza, J.; Espinosa-Arbeláez, D. G.; Rodríguez-García, M. E.
2010-05-01
Photo-carrier radiometry (PCR) has been used to study the distribution of impurities and the lattice damage in silicon-doped gallium arsenide in a noncontact way. The results from the PCR study are correlated with Hall effect measurements. Samples for this study were grown by molecular beam epitaxy. Of all possible parameters that can be manipulated, the silicon effusion cell temperature was the only one that was varied, in order to obtain samples with different silicon concentrations. The distribution of impurities was obtained by scanning the surface of each sample. The PCR amplitude and phase images were obtained as a function of the x- y position. According to the PCR images, it is evident that the impurities are not uniformly distributed across the sample. From these images, the average value of the amplitude and phase data across the surface was obtained for each sample in order to study the PCR signal behavior as a function of the silicon effusion cell temperature.
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.
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.
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
Pawlak, M.; Chirtoc, M.; Horny, N.; Pelzl, J.
2016-03-28
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 f{sub tc} 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 β{sub eff}, and the bulk carrier lifetime τ{sub c}. 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 n{sub 0}. 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.
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.
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.
Photocarrier Lifetime and Transport in Silicon Supersaturated with Sulfur
2012-01-01
gradients. Photocarriers generated in and near the impurity gradient can separate into different coplanar transport layers, leading to enhanced...carrier mobility-lifetime product of 10-8 cm2/V for heavily sulfur doped silicon. We conclude that the 1. REPORT DATE ( DD -MM-YYYY) 4. TITLE AND...can result in large concentration gradients. Photocarriers generated in and near the impurity gradient can separate into different coplanar transport
Photocarrier transport in 2D macroporous silicon structures
NASA Astrophysics Data System (ADS)
Karachevtseva, L.; Onyshchenko, V.; Sachenko, A.
2010-12-01
The mechanisms of photocarrier transport through a barrier in the surface space-charge region (SCR) of 2D macroporous silicon structures have been studied at photon energies comparable to that of the silicon indirect band-to-band transition. It was found that the photoconductivity relaxation time was determined by the light modulation of barrier on the macropore surface; as a result, the relaxation itself obeyed the logarithmic law. The temperature dependence of the photoconductivity relaxation time was determined by the thermionic emission mechanism of the current transport in the SCR at temperatures T > 180 K, and by the tunnel current flow at T < 100 K, with temperature-independent tunnelling probability. The photo-emf was found to become saturated or reverse its sign to negative at temperatures below 130 K because of light absorption due to optical transitions via surface electronic states close to the silicon conduction band. In this case, the surface band bending increases due to the growth of a negative charge of the semiconductor surface. The equilibrium electrons in the bulk and photoexcited holes on the macropore surface recombine through the channel of multistage tunnel recombination between the conduction and valence bands.
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.
Semi-infinite photocarrier radiometric model for the characterization of semiconductor wafer
NASA Astrophysics Data System (ADS)
Liu, Xianming; Li, Bincheng; Huang, Qiuping
2010-03-01
The analytical expression is derived to describe the photocarrier radiometric (PCR) signal for a semi-infinite semiconductor wafer excited by a square-wave modulated laser. For comparative study, the PCR signals are calculated by the semi-infinite model and the finite thickness model with several thicknesses. The fitted errors of the electronic transport properties by semi-infinite model are analyzed. From these results it is evident that for thick samples or at high modulation frequency, the semiconductor can be considered as semi-infinite.
NASA Astrophysics Data System (ADS)
Yamashita, Genki; Matsubara, Eiichi; Nagai, Masaya; Kim, Changsu; Akiyama, Hidefumi; Kanemitsu, Yoshihiko; Ashida, Masaaki
2017-02-01
We demonstrate the sensitive measurement of photocarriers in an active layer of a GaAs-based photovoltaic device using time-resolved terahertz reflection spectroscopy. We found that the reflection dip caused by Fabry-Pérot interference is strongly affected by the carrier profile in the active layer of the p-i-n structure. The experimental results show that this method is suitable for quantitative evaluation of carrier dynamics in active layers of solar cells under operating conditions.
Dynamics of Electronically Nonadiabatic Processes
NASA Astrophysics Data System (ADS)
Truhlar, Donald G.; Hack, Michael D.; Volobuev, Yuri L.; Jasper, Ahren W.; Topaler, Maria S.
2000-03-01
We are developing new semiclassical methods and testing existing semiclassical methods for modeling electronically nonadiabatic chemical processes in the gas phase. The semiclassical methods under consideration include trajectory surface hopping in the adiabatic and diabatic representations, time-dependent self-consistent-field theory (Ehrenfest method), and continuous surface switching. To test the methods, we are carrying out converged quantum dynamics calculations for three-body electronically nonadiabatic chemical reactions of the form M* + AB -> MA + B (M, A, and B are atoms, and an asterisk denotes electronic excitation) and quenching processes of the form M* + AB -> M + AB. The quantum dynamics calculations are carried out by a time-independent linear algebraic variational method using multi-arrangement dynamically adapted basis functions. Quantities tested include reaction probabilities, quenching probabilities, and vibrational and rotational distributions of the products. The talk will summarize the current status of these investigations.
Dynamic imaging with electron microscopy
Campbell, Geoffrey; McKeown, Joe; Santala, Melissa
2016-07-12
Livermore researchers have perfected an electron microscope to study fast-evolving material processes and chemical reactions. By applying engineering, microscopy, and laser expertise to the decades-old technology of electron microscopy, the dynamic transmission electron microscope (DTEM) team has developed a technique that can capture images of phenomena that are both very small and very fast. DTEM uses a precisely timed laser pulse to achieve a short but intense electron beam for imaging. When synchronized with a dynamic event in the microscope's field of view, DTEM allows scientists to record and measure material changes in action. A new movie-mode capability, which earned a 2013 R&D 100 Award from R&D Magazine, uses up to nine laser pulses to sequentially capture fast, irreversible, even one-of-a-kind material changes at the nanometer scale. DTEM projects are advancing basic and applied materials research, including such areas as nanostructure growth, phase transformations, and chemical reactions.
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.
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.
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.
Imaging the motion of electrons across semiconductor heterojunctions
NASA Astrophysics Data System (ADS)
Man, Michael K. L.; Margiolakis, Athanasios; Deckoff-Jones, Skylar; Harada, Takaaki; Wong, E. Laine; Krishna, M. Bala Murali; Madéo, Julien; Winchester, Andrew; Lei, Sidong; Vajtai, Robert; Ajayan, Pulickel M.; Dani, Keshav M.
2017-01-01
Technological progress since the late twentieth century has centred on semiconductor devices, such as transistors, diodes and solar cells. At the heart of these devices is the internal motion of electrons through semiconductor materials due to applied electric fields or by the excitation of photocarriers. Imaging the motion of these electrons would provide unprecedented insight into this important phenomenon, but requires high spatial and temporal resolution. Current studies of electron dynamics in semiconductors are generally limited by the spatial resolution of optical probes, or by the temporal resolution of electronic probes. Here, by combining femtosecond pump-probe techniques with spectroscopic photoemission electron microscopy, we imaged the motion of photoexcited electrons from high-energy to low-energy states in a type-II 2D InSe/GaAs heterostructure. At the instant of photoexcitation, energy-resolved photoelectron images revealed a highly non-equilibrium distribution of photocarriers in space and energy. Thereafter, in response to the out-of-equilibrium photocarriers, we observed the spatial redistribution of charges, thus forming internal electric fields, bending the semiconductor bands, and finally impeding further charge transfer. By assembling images taken at different time-delays, we produced a movie lasting a few trillionths of a second of the electron-transfer process in the photoexcited type-II heterostructure—a fundamental phenomenon in semiconductor devices such as solar cells. Quantitative analysis and theoretical modelling of spatial variations in the movie provide insight into future solar cells, 2D materials and other semiconductor devices.
Imaging the motion of electrons across semiconductor heterojunctions.
Man, Michael K L; Margiolakis, Athanasios; Deckoff-Jones, Skylar; Harada, Takaaki; Wong, E Laine; Krishna, M Bala Murali; Madéo, Julien; Winchester, Andrew; Lei, Sidong; Vajtai, Robert; Ajayan, Pulickel M; Dani, Keshav M
2017-01-01
Technological progress since the late twentieth century has centred on semiconductor devices, such as transistors, diodes and solar cells. At the heart of these devices is the internal motion of electrons through semiconductor materials due to applied electric fields or by the excitation of photocarriers. Imaging the motion of these electrons would provide unprecedented insight into this important phenomenon, but requires high spatial and temporal resolution. Current studies of electron dynamics in semiconductors are generally limited by the spatial resolution of optical probes, or by the temporal resolution of electronic probes. Here, by combining femtosecond pump-probe techniques with spectroscopic photoemission electron microscopy, we imaged the motion of photoexcited electrons from high-energy to low-energy states in a type-II 2D InSe/GaAs heterostructure. At the instant of photoexcitation, energy-resolved photoelectron images revealed a highly non-equilibrium distribution of photocarriers in space and energy. Thereafter, in response to the out-of-equilibrium photocarriers, we observed the spatial redistribution of charges, thus forming internal electric fields, bending the semiconductor bands, and finally impeding further charge transfer. By assembling images taken at different time-delays, we produced a movie lasting a few trillionths of a second of the electron-transfer process in the photoexcited type-II heterostructure-a fundamental phenomenon in semiconductor devices such as solar cells. Quantitative analysis and theoretical modelling of spatial variations in the movie provide insight into future solar cells, 2D materials and other semiconductor devices.
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.
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.
Dynamics of electrons and nuclei
NASA Astrophysics Data System (ADS)
Deumens, Erik; Öhrn, Yngve
2010-11-01
This paper presents the theory of Electron Nuclear Dynamics (END), which was developed and applied over the past 20 years or so in collaboration with a group of talented graduate students and postdoctoral associates. The Introduction presents the gist of this theoretical and computational approach to the study of molecular transformations. The next section outlines the major achievements of this time-dependent, direct, and non-adiabatic theory to the study of chemical change.
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.
Tayagaki, Takeshi; Hoshi, Yusuke; Kishimoto, Yuko; Usami, Noritaka
2014-03-10
We demonstrate enhanced photocarrier generation using photonic nanostructures fabricated by a wet etching technique with vertically aligned quantum dots (QDs). Using photoluminescence excitation spectroscopy, we found that the photocarrier generation in Ge/Si QDs placed close to the surface is enhanced below the band gap energy of crystalline silicon. The enhancement is explained by light trapping owing to the photonic nanostructures. Electromagnetic wave simulations indicate that the photonic nanostructure with a subwavelength size will be available to light trapping for efficient photocarrier generation by increasing their dip depth.
Enhanced photocarrier extraction mechanisms in ultra-thin photovoltaic GaAs n/p junctions
NASA Astrophysics Data System (ADS)
York, Mark C. A.; Proulx, Francine; Masson, Denis P.; Jaouad, Abdelatif; Bouzazi, Boussairi; Arès, Richard; Aimez, Vincent; Fafard, Simon
2016-03-01
PV devices with active areas of ~3:4 mm2 were fabricated and tested with top electrodes having different emitter gridline spacings with active area shadowing values between 0% and 1.8%. As expected, the thicker n/p junctions exhibit hindered photocarrier extraction, with low fill factor (FF) values, for devices prepared with sparse gridline designs. However, this study clearly demonstrates that for thin n/p junctions photocarrier extraction can still be efficient (FF > 80%) even for devices with no gridlines, which we explain using a TCAD model. The electric field profiles of devices with and without hindered photocarrier extraction are also discussed.
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
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.
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
2015-02-17
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.
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.
Attosecond Electron Dynamics in Molecules.
Nisoli, Mauro; Decleva, Piero; Calegari, Francesca; Palacios, Alicia; Martín, Fernando
2017-08-23
Advances in attosecond science have led to a wealth of important discoveries in atomic, molecular, and solid-state physics and are progressively directing their footsteps toward problems of chemical interest. Relevant technical achievements in the generation and application of extreme-ultraviolet subfemtosecond pulses, the introduction of experimental techniques able to follow in time the electron dynamics in quantum systems, and the development of sophisticated theoretical methods for the interpretation of the outcomes of such experiments have raised a continuous growing interest in attosecond phenomena, as demonstrated by the vast literature on the subject. In this review, after introducing the physical mechanisms at the basis of attosecond pulse generation and attosecond technology and describing the theoretical tools that complement experimental research in this field, we will concentrate on the application of attosecond methods to the investigation of ultrafast processes in molecules, with emphasis in molecules of chemical and biological interest. The measurement and control of electronic motion in complex molecular structures is a formidable challenge, for both theory and experiment, but will indubitably have a tremendous impact on chemistry in the years to come.
NASA Astrophysics Data System (ADS)
Kumazaki, Yusuke; Uemura, Keisuke; Sato, Taketomo; Hashizume, Tamotsu
2017-05-01
The photocarrier-regulated electrochemical (PREC) process was developed for fabricating recessed-gate AlGaN/GaN high-electron-mobility transistors (HEMTs) for normally off operation. The PREC process is based on photo-assisted electrochemical etching using low-energy chemical reactions. The fundamental photo-electrochemical measurements on AlGaN/GaN heterostructures revealed that the photo-carriers generated in the top AlGaN layer caused homogeneous etching of AlGaN with a smooth surface, but those generated in the GaN layer underneath caused inhomogeneous etching that roughens the surface. The concept of the PREC process is to supply the photo-carriers generated only in the AlGaN layer by selecting proper conditions on light wavelength and voltage. The phenomenon of self-termination etching has been observed during the PREC process, where the etching depth was controlled by light intensity. The recessed-gate AlGaN/GaN HEMT fabricated with the PREC process showed positive threshold voltage and improvement in transconductance compared to planar-gate AlGaN/GaN HEMTs.
Nonadiabatic evolution of electronic states by electron nuclear dynamics theory
NASA Astrophysics Data System (ADS)
Hagelberg, Frank
The problem of how to determine the nonadiabatic content of any given dynamic process involving molecular motion is addressed in the context of Electron Nuclear Dynamics (END) theory. Specifically, it is proposed to cast the dynamic END wave function into the language of static electronic configurations with time dependent complex-valued amplitudes. This is achieved by adiabatic transport of an electronic basis along the classical nuclear trajectories of the studied molecular system, as yielded by END simulation. Projecting the dynamic wave function on this basis yields a natural distinction between adiabatic and nonadiabatic components of the motion considered. Tracing the evolution of the leading configurations is shown to be a helpful device for clarifying the physical nature of electronic excitation processes. For illustration of these concepts, dynamic configuration analysis is applied to the scattering of a proton by a lithium atom.
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.
NASA Astrophysics Data System (ADS)
Schmitt, S. W.; Brönstrup, G.; Shalev, G.; Srivastava, S. K.; Bashouti, M. Y.; Döhler, G. H.; Christiansen, S. H.
2014-06-01
Vertically aligned silicon nanowire (SiNW) diodes are promising candidates for the integration into various opto-electronic device concepts for e.g. sensing or solar energy conversion. Individual SiNW p-n diodes have intensively been studied, but to date an assessment of their device performance once integrated on a silicon substrate has not been made. We show that using a scanning electron microscope (SEM) equipped with a nano-manipulator and an optical fiber feed-through for tunable (wavelength, power using a tunable laser source) sample illumination, the dark and illuminated current-voltage (I-V) curve of individual SiNW diodes on the substrate wafer can be measured. Surprisingly, the I-V-curve of the serially coupled system composed of SiNW/wafers is accurately described by an equivalent circuit model of a single diode and diode parameters like series and shunting resistivity, diode ideality factor and photocurrent can be retrieved from a fit. We show that the photo-carrier collection efficiency (PCE) of the integrated diode illuminated with variable wavelength and intensity light directly gives insight into the quality of the device design at the nanoscale. We find that the PCE decreases for high light intensities and photocurrent densities, due to the fact that considerable amounts of photo-excited carriers generated within the substrate lead to a decrease in shunting resistivity of the SiNW diode and deteriorate its rectification. The PCE decreases systematically for smaller wavelengths of visible light, showing the possibility of monitoring the effectiveness of the SiNW device surface passivation using the shown measurement technique. The integrated device was pre-characterized using secondary ion mass spectrometry (SIMS), TCAD simulations and electron beam induced current (EBIC) measurements to validate the properties of the characterized material at the single SiNW diode level.Vertically aligned silicon nanowire (SiNW) diodes are promising candidates for
Nonequilibrium electron dynamics in noble metals
NASA Astrophysics Data System (ADS)
del Fatti, N.; Voisin, C.; Achermann, M.; Tzortzakis, S.; Christofilos, D.; Vallée, F.
2000-06-01
Electron-electron and electron-lattice interactions in noble metals are discussed in the light of two-color femtosecond pump-probe measurements in silver films. The internal thermalization of a nonequilibrium electron distribution created by intraband absorption of a pump pulse is followed by probing the induced optical property changes in the vicinity of the frequency threshold for the d band to Fermi surface transitions. This is shown to take place with a characteristic time constant of 350 fs, significantly shorter than previously reported in gold. This difference is ascribed to a weaker screening of the electron-electron interaction by the d-band electrons in silver than in gold. These results are in quantitative agreement with numerical simulations of the electron relaxation dynamics using a reduced static screening of the electron-electron Coulomb interaction, and including bound electron screening. Electron-lattice thermalization has been studied using a probe frequency out of resonance with the interband transitions. In both materials, the transient nonthermal nature of the electron distribution leads to the observation of a short-time delay reduction of the energy-loss rate of the electron gas to the lattice, in very good agreement with our theoretical model.
On electronic representations in molecular reaction dynamics
NASA Astrophysics Data System (ADS)
Killian, Benjamin J.
For many decades, the field of chemical reaction dynamics has utilized computational methods that rely on potential energy surfaces that are constructed using stationary-state calculations. These methods are typically devoid of dynamical couplings between the electronic and nuclear degrees of freedom, a fact that can result in incorrect descriptions of dynamical processes. Often, non-adiabatic coupling expressions are included in these methodologies. The Electron-Nuclear Dynamics (END) formalism, in contrast, circumvents these deficiencies by calculating all intermolecular forces directly at each time step in the dynamics and by explicitly maintaining all electronic-nuclear couplings. The purpose of this work is to offer two new frameworks for implementing electronic representations in dynamical calculations. Firstly, a new schema is proposed for developing atomic basis sets that are consistent with dynamical calculations. Traditionally, basis sets have been designed for use in stationary-state calculations of the structures and properties of molecules in their ground states. As a consequence of common construction techniques that utilize energy optimization methods, the unoccupied orbitals bear little resemblance to physical virtual atomic orbitals. We develop and implement a method for basis set construction that relies upon physical properties of atomic orbitals and that results in meaningful virtual orbitals. These basis sets are shown to provide a significant improvement in the accuracy of calculated dynamical properties such as charge transfer probabilities. Secondly, the theoretical framework of END is expanded to incorporate a multi-configurational representation for electrons. This formalism, named Vector Hartree-Fock, is based in the theory of vector coherent states and utilizes a complete active space electronic representation. The Vector Hartree-Fock method is fully disclosed, with derivation of the equations of motion. The expressions for the equation
Dynamics of electron solvation in molecular clusters.
Ehrler, Oli T; Neumark, Daniel M
2009-06-16
Solvated electrons, and hydrated electrons in particular, are important species in condensed phase chemistry, physics, and biology. Many studies have examined the formation mechanism, reactivity, spectroscopy, and dynamics of electrons in aqueous solution and other solvents, leading to a fundamental understanding of the electron-solvent interaction. However, key aspects of solvated electrons remain controversial, and the interaction between hydrated electrons and water is of central interest. For example, although researchers generally accept that hydrated electrons, eaq-, occupy solvent cavities, another picture suggests that the electron resides in a diffuse orbital localized on a H3O radical. In addition, researchers have proposed two physically distinct models for the relaxation mechanism when the electron is excited. These models, formulated to interpret condensed phase experiments, have markedly different timescales for the internal conversion from the excited p state to the ground s state.Studies of negatively charged clusters, such as (H2O)n- and I-(H2O)n, offer a complementary perspective for studying aqueous electron solvation. In this Account, we use time-resolved photoelectron spectroscopy (TRPES), a femtosecond pump-probe technique in which mass-selected anions are electronically excited and then photodetached at a series of delay times, to focus on time-resolved dynamics in these and similar species. In (H2O)n-,TRPES gives evidence for ultrafast internal conversion in clusters up to n=100. Extrapolation of these results yields a p-state lifetime of 50 fs in the bulk limit. This is in good agreement with the nonadiabatic solvation model, one of the models proposed for relaxation of eaq-. Similarly, experiments on (MeOH)n- up to n=450 give an extrapolated p-state lifetime of 150fs. TRPES investigations of I-(H2O)n and I-(CH3CN)n probe a different aspect of electron solvation dynamics. In these experiments,an ultraviolet pump pulse excites the cluster
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
Ultrafast electron dynamics in gold nanoshells
NASA Astrophysics Data System (ADS)
Westcott, Sarah Linda
2001-10-01
In metallic nanostructures, the interaction of excited electrons with the nanostructure surface may result in electron relaxation dynamics that are significantly different than those predicted by electron-lattice coupling. These ultrafast electron dynamics were monitored by pump-probe measurements of the time-resolved change in transmission. Using femtosecond pulses from a cavity-dumped titanium-doped sapphire laser, two types of nanoparticles with a core-shell geometry were studied. Nanoshells are nanoparticles with a dielectric core surrounded by a continuous thin metal shell. For nanoshells, the plasmon resonance wavelength is tunable by changing the core and shell dimensions. For nanoshells with a gold sulfide core and a gold shell, two conditions were observed under which electron relaxation was different than predicted by electron-phonon coupling. First, electron relaxation occurred more rapidly for gold-gold sulfide nanoshells embedded in polymer films than for nanoshells dispersed in water, with lifetimes of 1.6 ps and 3 to 5 ps, respectively. Second, for nanoshells dispersed in water, the electron relaxation lifetime decreased with adsorption of p-aminobenzoic acid (to 1.7 ps) or aniline (to 1.9 ps) on the nanoshells. With adsorbed n-propylamine or p-mercaptobenzoic acid, electron relaxation transpired in 2.8 ps or 2.4 ps, respectively. Density functional theory calculations indicated that the molecules leading to the fastest electron relaxation possessed the largest induced dipole moments near a metal surface. Semicontinuous gold films grown around a silica nanoparticle core exhibited spectral and dynamical optical signatures of the percolation threshold. Compared to continuous shells, the electron dynamics in the semicontinuous shell layer were dramatically different as additional induced bleaching was observed in the first 500 fs. The observed dynamics are consistent with a rate equation model in which the electrons are initially excited in localized
Kada, T; Asahi, S; Kaizu, T; Harada, Y; Tamaki, R; Okada, Y; Kita, T
2017-07-19
We studied the effects of the internal electric field on two-step photocarrier generation in InAs/GaAs quantum dot superlattice (QDSL) intermediate-band solar cells (IBSCs). The external quantum efficiency of QDSL-IBSCs was measured as a function of the internal electric field intensity, and compared with theoretical calculations accounting for interband and intersubband photoexcitations. The extra photocurrent caused by the two-step photoexcitation was maximal for a reversely biased electric field, while the current generated by the interband photoexcitation increased monotonically with increasing electric field intensity. The internal electric field in solar cells separated photogenerated electrons and holes in the superlattice (SL) miniband that played the role of an intermediate band, and the electron lifetime was extended to the microsecond scale, which improved the intersubband transition strength, therefore increasing the two-step photocurrent. There was a trade-off relation between the carrier separation enhancing the two-step photoexcitation and the electric-field-induced carrier escape from QDSLs. These results validate that long-lifetime electrons are key to maximising the two-step photocarrier generation in QDSL-IBSCs.
Electron correlation dynamics in atoms and molecules.
Nest, M; Ludwig, M; Ulusoy, I; Klamroth, T; Saalfrank, P
2013-04-28
In this paper, we present quantum dynamical calculations on electron correlation dynamics in atoms and molecules using explicitly time-dependent ab initio configuration interaction theory. The goals are (i) to show that in which cases it is possible to switch off the electronic correlation by ultrashort laser pulses, and (ii) to understand the temporal evolution and the time scale on which it reappears. We characterize the appearance of correlation through electron-electron scattering when starting from an uncorrelated state, and we identify pathways for the preparation of a Hartree-Fock state from the correlated, true ground state. Exemplary results for noble gases, alkaline earth elements, and selected molecules are provided. For Mg we show that the uncorrelated state can be prepared using a shaped ultrashort laser pulse.
Electron correlation dynamics in atoms and molecules
Nest, M.; Ludwig, M.; Ulusoy, I.; Klamroth, T.; Saalfrank, P.
2013-04-28
In this paper, we present quantum dynamical calculations on electron correlation dynamics in atoms and molecules using explicitly time-dependent ab initio configuration interaction theory. The goals are (i) to show that in which cases it is possible to switch off the electronic correlation by ultrashort laser pulses, and (ii) to understand the temporal evolution and the time scale on which it reappears. We characterize the appearance of correlation through electron-electron scattering when starting from an uncorrelated state, and we identify pathways for the preparation of a Hartree-Fock state from the correlated, true ground state. Exemplary results for noble gases, alkaline earth elements, and selected molecules are provided. For Mg we show that the uncorrelated state can be prepared using a shaped ultrashort laser pulse.
Electron correlation dynamics in atoms and molecules
NASA Astrophysics Data System (ADS)
Nest, M.; Ludwig, M.; Ulusoy, I.; Klamroth, T.; Saalfrank, P.
2013-04-01
In this paper, we present quantum dynamical calculations on electron correlation dynamics in atoms and molecules using explicitly time-dependent ab initio configuration interaction theory. The goals are (i) to show that in which cases it is possible to switch off the electronic correlation by ultrashort laser pulses, and (ii) to understand the temporal evolution and the time scale on which it reappears. We characterize the appearance of correlation through electron-electron scattering when starting from an uncorrelated state, and we identify pathways for the preparation of a Hartree-Fock state from the correlated, true ground state. Exemplary results for noble gases, alkaline earth elements, and selected molecules are provided. For Mg we show that the uncorrelated state can be prepared using a shaped ultrashort laser pulse.
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.
Electron dynamics in an elliptical bubble regime
NASA Astrophysics Data System (ADS)
Hemmati, Atefeh; Sedaghatizadeh, Mahmoud; Kordbacheh, Amir Hossein Ahmadkhan
2017-09-01
In this paper, the dynamics of the electron in an elliptical bubble regime is investigated. In this regime, a high intensity laser pulse in a plasma creates an electron cavity called the blow-out (bubble or cavitation) regime which is usually considered to be in a spherical shape at rest. Through balancing the ponderomotive potential of a non-plane laser pulse and bubble electrostatic potential, the shape of the bubble is analyzed to be elliptical in contrast to most available theories which indicate the spherical bubble. Thus, the present model introduces a different dynamics for the electron compared with the spherical one. The longitudinal electric field experienced by the electron and also the electron energy gain in the elliptical model is investigated to be more than that in the spherical model. Moreover, it is found that the shape of the bubble will influence the electron trapping range so that the electron is bounded more in the spherical bubble. As a result, it is crucially important to take the shape of the bubble influence on the electron acceleration process into account. The results indicate that the distribution of the electromagnetic fields inside the bubble in the ellipse model is more close to particle-in-cell simulation compared to the spherical one [Kostyukov et al., Phys. Plasmas 11(11), 5256 (2004)].
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.
Dynamics of dissociative electron attachment to ammonia
Rescigno, T. N.; Trevisan, C. S.; Orel, A. E.; Slaughter, D. S.; Adaniya, H.; Belkacem, A.; Weyland, Marvin; Dorn, Alexander; McCurdy, C. W.
2016-05-12
We present that 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.
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.
Dynamics of dissociative electron attachment to ammonia
Rescigno, T. N.; Trevisan, C. S.; Orel, A. E.; ...
2016-05-12
We present that 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.
Free electron laser mode dynamics
NASA Astrophysics Data System (ADS)
Kan, Shidong
The University of Hawai'i at Manoa (UHM) Fox-Smith project opens a door for great research opportunities to the fields of high resolution infrared laser spectroscopy, quantum optics, coherent x-ray production and new and fundamental applications of phase-locked pulse trains and coherent frequency combs. An understanding of FEL mode dynamics is essential for facilitating this multimirror laser cavity design and improving laser performance for applications. Of particular interest is the nonlinear mode competition and mode evolution in the time domain which can give insight understanding of FELs' mode spectrum evolution. In this dissertation, I report the first thorough investigation and analysis of the nonlinear mode competition and mode evolution from the small signal regime through deep saturation using a time domain full particle simulation code based on the fundamental FEL equations of motion. It is found that the passive eigenmode theory of multimirror resonator FEL is not fully applicable in the large signal saturated regime. Extreme mode competition at the midpoint-phase offset versus beamsplitter reflectance indicating enhanced single mode operation is also discovered. In addition, matrix analysis including the proper form of the FEL gain saturation and the phase of the complex gain is also performed. This dissertation, for the first time known to the author, proposes a Michelson configuration which couples every third pulse. The feasibility and performance of the proposed configuration is elaborately investigated. An experimental design for evaluating the extreme mode competition effect discovered during the course of this dissertation research is described, based on the Mark V FEL in the current Michelson and the proposed new Michelson configurations. Finally, I report the construction and calibration of a Fox-Smith beamsplitter using a rotatable birefringent sapphire plate. High assembly precision is achieved. The angular beam wander caused by the rotation
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.
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.
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.
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.
Dynamics of electron transfer in photosystem II.
Burda, Kvetoslava
2007-01-01
Photosystem II, being a constituent of light driven photosynthetic apparatus, is a highly organized pigment-protein-lipid complex. The arrangement of PSII active redox cofactors insures efficiency of electron transfer within it. Donation of electrons extracted from water by the oxygen evolving complex to plastoquinones requires an additional activation energy. In this paper we present theoretical discussion of the anharmonic fluctuations of the protein-lipid matrix of PSII and an experimental evidence showing that the fluctuations are responsible for coupling of its donor and acceptor side. We argue that the fast collective motions liberated at temperatures higher that 200 K are crucial for the two final steps of the water splitting cycle and that one can distinguish three different dynamic regimes of PSII action which are controlled by the timescales of forward electron transfer, which vary with temperature. The three regimes of the dynamical behavior are related to different spatial domains of PSII.
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.
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.
Ultrafast Electron Dynamics in Solar Energy Conversion.
Ponseca, Carlito S; Chábera, Pavel; Uhlig, Jens; Persson, Petter; Sundström, Villy
2017-08-23
Electrons are the workhorses of solar energy conversion. Conversion of the energy of light to electricity in photovoltaics, or to energy-rich molecules (solar fuel) through photocatalytic processes, invariably starts with photoinduced generation of energy-rich electrons. The harvesting of these electrons in practical devices rests on a series of electron transfer processes whose dynamics and efficiencies determine the function of materials and devices. To capture the energy of a photogenerated electron-hole pair in a solar cell material, charges of opposite sign have to be separated against electrostatic attractions, prevented from recombining and being transported through the active material to electrodes where they can be extracted. In photocatalytic solar fuel production, these electron processes are coupled to chemical reactions leading to storage of the energy of light in chemical bonds. With the focus on the ultrafast time scale, we here discuss the light-induced electron processes underlying the function of several molecular and hybrid materials currently under development for solar energy applications in dye or quantum dot-sensitized solar cells, polymer-fullerene polymer solar cells, organometal halide perovskite solar cells, and finally some photocatalytic systems.
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
Electron Dynamics in Finite Quantum Systems
NASA Astrophysics Data System (ADS)
McDonald, Christopher R.
The multiconfiguration time-dependent Hartree-Fock (MCTDHF) and multiconfiguration time-dependent Hartree (MCTDH) methods are employed to investigate nonperturbative multielectron dynamics in finite quantum systems. MCTDHF is a powerful tool that allows for the investigation of multielectron dynamics in strongly perturbed quantum systems. We have developed an MCTDHF code that is capable of treating problems involving three dimensional (3D) atoms and molecules exposed to strong laser fields. This code will allow for the theoretical treatment of multielectron phenomena in attosecond science that were previously inaccessible. These problems include complex ionization processes in pump-probe experiments on noble gas atoms, the nonlinear effects that have been observed in Ne atoms in the presence of an x-ray free-electron laser (XFEL) and the molecular rearrangement of cations after ionization. An implementation of MCTDH that is optimized for two electrons, each moving in two dimensions (2D), is also presented. This implementation of MCTDH allows for the efficient treatment of 2D spin-free systems involving two electrons; however, it does not scale well to 3D or to systems containing more that two electrons. Both MCTDHF and MCTDH were used to treat 2D problems in nanophysics and attosecond science. MCTDHF is used to investigate plasmon dynamics and the quantum breathing mode for several electrons in finite lateral quantum dots. MCTDHF is also used to study the effects of manipulating the potential of a double lateral quantum dot containing two electrons; applications to quantum computing are discussed. MCTDH is used to examine a diatomic model molecular system exposed to a strong laser field; nonsequential double ionization and high harmonic generation are studied and new processes identified and explained. An implementation of MCTDHF is developed for nonuniform tensor product grids; this will allow for the full 3D implementation of MCTDHF and will provide a means to
Optical power-driven electron spin relaxation regime crossover in Mn-doped bulk GaAs
NASA Astrophysics Data System (ADS)
Münzhuber, F.; Kiessling, T.; Ossau, W.; Molenkamp, L. W.; Astakhov, G. V.
2015-09-01
We demonstrate tunability of the electron spin lifetime in Mn-doped GaAs by purely optical means. The observed behavior stems from a crossover of the electron spin relaxation rate with increasing excitation density, first decreasing due to the exchange interaction of Mn bound holes with Mn ions, and then increasing again as the valence band is populated and Bir-Aranov-Pikus relaxation sets in. On this account, we explain the complex spatial spin polarization profiles emerging from inhomogeneous optical excitation, which are the result of the combined action of this nonmonotonic spin relaxation characteristics and the intricate photocarrier decay dynamics.
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.
NASA Astrophysics Data System (ADS)
Kanemoto, Katsuichi; Nakatani, Hitomi; Domoto, Shinya
2014-10-01
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/cm2 is determined to be 3.5 × 1016 cm-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.
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.
Electronic-structural dynamics in graphene.
Gierz, Isabella; Cavalleri, Andrea
2016-09-01
We review our recent time- and angle-resolved photoemission spectroscopy experiments, which measure the transient electronic structure of optically driven graphene. For pump photon energies in the near infrared ([Formula: see text]), we have discovered the formation of a population-inverted state near the Dirac point, which may be of interest for the design of THz lasing devices and optical amplifiers. At lower pump photon energies ([Formula: see text]), for which interband absorption is not possible in doped samples, we find evidence for free carrier absorption. In addition, when mid-infrared pulses are made resonant with an infrared-active in-plane phonon of bilayer graphene ([Formula: see text]), a transient enhancement of the electron-phonon coupling constant is observed, providing interesting perspective for experiments that report light-enhanced superconductivity in doped fullerites in which a similar lattice mode was excited. All the studies reviewed here have important implications for applications of graphene in optoelectronic devices and for the dynamical engineering of electronic properties with light.
Electronic-structural dynamics in graphene
Gierz, Isabella; Cavalleri, Andrea
2016-01-01
We review our recent time- and angle-resolved photoemission spectroscopy experiments, which measure the transient electronic structure of optically driven graphene. For pump photon energies in the near infrared (ℏωpump=950 meV), we have discovered the formation of a population-inverted state near the Dirac point, which may be of interest for the design of THz lasing devices and optical amplifiers. At lower pump photon energies (ℏωpump<400 meV), for which interband absorption is not possible in doped samples, we find evidence for free carrier absorption. In addition, when mid-infrared pulses are made resonant with an infrared-active in-plane phonon of bilayer graphene (ℏωpump=200 meV), a transient enhancement of the electron-phonon coupling constant is observed, providing interesting perspective for experiments that report light-enhanced superconductivity in doped fullerites in which a similar lattice mode was excited. All the studies reviewed here have important implications for applications of graphene in optoelectronic devices and for the dynamical engineering of electronic properties with light. PMID:27822486
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.
Radiowave Imaging of Ionospheric Electron Dynamics
NASA Astrophysics Data System (ADS)
van Bavel, Gregory Hugh
1998-12-01
This dissertation is a study of disturbances in the polar ionosphere. A relative ionospheric opacity meter (riometer) is a radio frequency instrument that enables the remote sensing of ionospheric disturbances by recording variations in the cosmic radio noise power received at a terrestrial antenna. The Imaging Riometer for Ionospheric Studies (IRIS) produces images of relative ionospheric opacity. In the ionosphere, the attenuation of a radio signal's amplitude is proportional to the electron number density n and the effective collision frequency ν. Therefore, a riometer is sensitive to variations of the product n/nu, but their effects are not separated. The theory of HF radiowave attenuation in a cold magetoplasma and electron continuity yield a pair of uni-directional wave equations that couple the dynamics of cosmic radio noise absorption to the vertical mean value of ν. These equations, and some simplifying assumptions, are the basis of a data analysis that transforms IRIS images into physical quantities related to the absorbing ionospheric electrons: mean velocity, mean effective collision frequency, net production rate and column density. A critical test case and coincident auroral observations support the reliability of the general results of the data analysis. Variations in the mean flow velocity indicate that the ionosphere is not in equilibrium. The mean effective collision frequency shows significant structural variations over 100 km and 1 minute intervals. Column density depletions lead enhancements in a geomagnetic poleward drift, while a net production region moves with the column density enhancement and intensifies as the pole-ward motion ceases. Regions of persistent electron production or loss are found where the collision frequency is relatively low, and specific locations can oscillate between net production and loss with periods of about 1 to 2 minutes. It is found that the spatial structure of a riometer image is chiefly determined by the
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.
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.
Electronic Structure and Dynamics of Nitrosyl Porphyrins
Scheidt, W. Robert; Barabanschikov, Alexander; Pavlik, Jeffrey W.; Silvernail, Nathan J.; Sage, J. Timothy
2010-01-01
fully successful at capturing the interaction between the axial NO and imidazole ligands. This supports previous conclusions that hemeNO complexes exhibit an unusual degree of variability with respect to computational method, and we speculate that this variability hints at a genuine electronic instability that a protein can exploit to tune reactivity. We anticipate that ongoing characterization of heme-NO complexes will deepen our understanding of their structure, dynamics, and reactivity. PMID:20666384
Electronic structure and dynamics of nitrosyl porphyrins.
Scheidt, W Robert; Barabanschikov, Alexander; Pavlik, Jeffrey W; Silvernail, Nathan J; Sage, J Timothy
2010-07-19
functionals are not fully successful at capturing the trans interaction between the axial NO and imidazole ligands. This supports previous conclusions that heme-NO complexes exhibit an unusual degree of variability with respect to the computational method, and we speculate that this variability hints at a genuine electronic instability that a protein can exploit to tune its reactivity. We anticipate that ongoing characterization of heme-NO complexes will deepen our understanding of their structure, dynamics, and reactivity.
Electronic Delocalization, Vibrational Dynamics, and Energy Transfer in Organic Chromophores.
Nelson, Tammie; Fernandez-Alberti, Sebastian; Roitberg, Adrian E; Tretiak, Sergei
2017-07-06
The efficiency of materials developed for solar energy and technological applications depends on the interplay between molecular architecture and light-induced electronic energy redistribution. The spatial localization of electronic excitations is very sensitive to molecular distortions. Vibrational nuclear motions can couple to electronic dynamics driving changes in localization. The electronic energy transfer among multiple chromophores arises from several distinct mechanisms that can give rise to experimentally measured signals. Atomistic simulations of coupled electron-vibrational dynamics can help uncover the nuclear motions directing energy flow. Through careful analysis of excited state wave function evolution and a useful fragmenting of multichromophore systems, through-bond transport and exciton hopping (through-space) mechanisms can be distinguished. Such insights are crucial in the interpretation of fluorescence anisotropy measurements and can aid materials design. This Perspective highlights the interconnected vibrational and electronic motions at the foundation of nonadiabatic dynamics where nuclear motions, including torsional rotations and bond vibrations, drive electronic transitions.
Ultrafast pseudospin dynamics in graphene
NASA Astrophysics Data System (ADS)
Trushin, M.; Grupp, A.; Soavi, G.; Budweg, A.; De Fazio, D.; Sassi, U.; Lombardo, A.; Ferrari, A. C.; Belzig, W.; Leitenstorfer, A.; Brida, D.
2015-10-01
Interband optical transitions in graphene are subject to pseudospin selection rules. Impulsive excitation with linearly polarized light generates an anisotropic photocarrier occupation in momentum space that evolves at time scales shorter than 100 fs. Here, we investigate the evolution of nonequilibrium charges towards an isotropic distribution by means of fluence-dependent ultrafast spectroscopy and develop an analytical model able to quantify the isotropization process. In contrast to conventional semiconductors, the isotropization is governed by optical phonon emission, rather than electron-electron scattering, which nevertheless contributes in shaping the anisotropic photocarrier occupation within the first few femtoseconds.
Vibrational- and Laser-Driven Electronic Dynamics in the Molecules
NASA Astrophysics Data System (ADS)
Stolow, Albert
2014-05-01
Electronic dynamics within molecules can be driven by both motions of the atoms, via non-Born-Oppenheimer coupling, and by applied laser fields, driving electron motions on sub-cycle time scales. The challenging but most general case of Molecular Dynamics is where electronic and vibrational motions are fully coupled, the making and breaking of chemical bonds being the most prominent example. Time-Resolved Coincidence Imaging Spectroscopy (TRCIS) is a ultrafast photoelectron probe of Molecular Frame dynamics in polyatomic molecules. It makes use of full 3D recoil momentum vector determination of coincident photoions and photoelectrons as a function of time, permitting observations of coupled electronic-vibrational dynamics from the Molecular Frame rather than the Lab Frame point of view. Methods in non-resonant quantum control, based on the dynamic Stark effect, have also emerged as important tools for enhancing molecular dynamics studies. In particular, molecular alignment can fix the Molecular Frame within the Lab Frame, avoiding loss of information due to orientational averaging. Provided that the molecular dynamics are fast compared to rotational dephasing, this method also permits time-resolved Molecular Frame observations. As laser fields get stronger, a sub-cycle (attosecond) physics emerges, leading to new probes of driven multi-electron dynamics in polyatomic molecules. Understanding driven multi-electron responses will be central to advancing attosecond science towards polyatomic molecules and complex systems.
Efficiency of Photocarrier Injection in a VO2/TiO2:Nb Heterostructure
NASA Astrophysics Data System (ADS)
Hiroi, Zenji; Yamauchi, Tohru; Muraoka, Yuji; Muramatsu, Takaki; Yamaura, Jun-Ichi
2003-12-01
The efficiency of photocarrier injection in a VO2/TiO2:Nb heterostructure is studied by measuring I-V characteristics at room temperature under ultraviolet light irradiation. It is revealed that photogenerated hole carriers in the TiO2:Nb substrate are injected and accumulated in the VO2 film by the photovoltaic effect. The surface charge density is controlled successfully in a wide range of 109-1013 cm-2 as a function of light irradiance. The maximum hole density of 9× 1018 cm-3 is attained at a light irradiance of 133 mW/cm2, which is estimated by assuming the uniform distribution of holes in the film. It is suggested that high efficiency can be achieved by utilizing the large dielectric constant of titanium oxide substrates.
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.
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.
Living Books and Dynamic Electronic Libraries.
ERIC Educational Resources Information Center
Barker, Philip
1996-01-01
Discusses changes that have taken place within library systems as a consequence of the emergence of new computer-based technologies. Highlights include using electronic documents; electronic libraries; digital projects; educational applications; and a case study of OASIS (Open Access Student Information Service), a document handling system in the…
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…
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…
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.
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.
Real-time electron dynamics simulation of two-electron transfer reactions induced by nuclear motion
NASA Astrophysics Data System (ADS)
Suzuki, Yasumitsu; Yamashita, Koichi
2012-04-01
Real-time electron dynamics of two-electron transfer reactions induced by nuclear motion is calculated by three methods: the numerically exact propagation method, the time-dependent Hartree (TDH) method and the Ehrenfest method. We find that, as long as the nuclei move as localized wave packets, the TDH and Ehrenfest methods can reproduce the exact electron dynamics of a simple charge transfer reaction model containing two electrons qualitatively well, even when nonadiabatic transitions between adiabatic states occur. In particular, both methods can reproduce the cases where a complete two-electron transfer reaction occurs and those where it does not occur.
Dynamic screening and electron electron scattering in low-dimensional metallic systems
NASA Astrophysics Data System (ADS)
Silkin, V. M.; Quijada, M.; Muiño, R. Díez; Chulkov, E. V.; Echenique, P. M.
2007-09-01
The modification of dynamic screening in the electron-electron interaction in systems with reduced dimensionality and tunable one-particle electronic structure is studied. Two examples of such systems are considered, namely, the adsorbate-induced quantum well states at the Na adlayer covered Cu(1 1 1) surface, and metal clusters of sizes up to few nanometers. The dependence of the electron-electron decay rates on the Na coverage in the former case and on the cluster size in the latter is investigated. The role played by the dynamical screened interaction in such processes is addressed as well.
Some aspects of electron dynamics in electron cyclotron resonance ion sources
NASA Astrophysics Data System (ADS)
Mironov, V.; Bogomolov, S.; Bondarchenko, A.; Efremov, A.; Loginov, V.
2017-07-01
Electron dynamics in an electron cyclotron resonance ion source is numerically simulated by using a particle-in-cell code combined with simulations of the ion dynamics. Mean electron energies are found to be around 70 keV, close to values that are derived from spectra of x-ray emission out of the source. The electron lifetime is defined by losses of low-energy electrons created in ionizing collisions; the losses are regulated by electron heating rate, which depends on the magnitude of the microwave electric field. Changes in the ion confinement with variations in the microwave electric field and gas flow are simulated. The influence of electron dynamics on the afterglow and two-frequency heating effects is discussed.
High-temporal-resolution electron microscopy for imaging ultrafast electron dynamics
NASA Astrophysics Data System (ADS)
Hassan, M. Th.; Baskin, J. S.; Liao, B.; Zewail, A. H.
2017-07-01
Ultrafast electron microscopy (UEM) has been demonstrated as an effective table-top technique for imaging the temporally evolving dynamics of matter with a subparticle spatial resolution on the timescale of atomic motion. However, imaging the faster motion of electron dynamics in real time has remained beyond reach. Here we demonstrate more than an order of magnitude (16 times) enhancement in the typical temporal resolution of UEM by generating isolated ∼30 fs electron pulses, accelerated at 200 keV, via the optical-gating approach, with sufficient intensity to probe efficiently the electronic dynamics of matter. Moreover, we investigate the feasibility of attosecond optical gating to generate isolated subfemtosecond electron pulses and attain the desired temporal resolution in electron microscopy to establish 'attomicroscopy' to allow the imaging of electron motion in the act.
Functional Electronic Amplifiers with Broad Dynamic Band,
1983-09-27
dynamic properties of amplifiers, assembled on this type of amplifier instruments, it is expedient to introduce the concept of the dynamic quality...qjvL> ql. 3. Amplifier has data: K" =K’/m; , vus,, q -q4cujvv.4 in Fig. 1). Functional amplifier is assembled on the block diagram Fig. 2b. It has...following data: K-mr’ vv;m-v-mvv’-" qpYmq j° ey" As can be seen from the given examples, dynamic quality of FU, assembled on the identical amplifier
On the electron wavepacket dynamics of photoionizing states
NASA Astrophysics Data System (ADS)
Takatsuka, Kazuo
2014-06-01
To study electron wavepacket dynamics of photoionizing states in polyatomic molecules, we discuss two crucial issues to be overcome in the theory of molecular electronic wavepacket dynamics in an intense laser field (Takatsuka and Yonehara 2011 Phys. Chem. Chem. Phys. 13 4987). One is about the description of the ionization process from electronically excited states composed of many multiply excited configuration-state functions. The other is how to reconstruct the electronic states remaining in the molecular site while electrons are flowing out of the molecular bounds. These are both critical to extend the realm of the theories of electron dynamics based on the so-called expansion (algebraic) method in terms of basis functions. To calculate the photoionization amplitude and thereby to estimate the time-dependent amount of electron loss from a molecule, we extract the electron flux (probability current density) from the electron wavepackets without use of scattering theory. This is justified by the success of the recent works by Bandrauk’s group for attosecond photoionization dynamics from the hydrogen molecule ion, who performed numerical integration of the relevant Schrödinger equation (Yuan et al 2013 J. Chem. Phys. 138 134316). A key feature in the present study, on the other hand, is to calculate the electron flux in terms of complex-valued NOs, which arise from the complex electronic wavepackets. Through the change of these NOs, we reconstruct the involved electronic configurations during the flow of electrons out of molecular regions. These repopulated electronic wavefunctions are (non-adiabatically) evolved in time under laser fields.
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.
Entanglement Dynamics of Electrons and Photons
NASA Astrophysics Data System (ADS)
Wu, Xiang-Yao; Liu, Xiao-Jing; Lu, Jing-Bin; Li, Tian-Shun; Zhang, Si-Qi; Liang, Yu; Ma, Ji; Li, Hong
2016-12-01
Entanglement is a fundamental feature of quantum theory as well as a key resource for quantum computing and quantum communication, but the entanglement mechanism has not been found at present. We think when the two subsystems exist interaction directly or indirectly, they can be in entanglement state. such as, in the Jaynes-Cummings model, the entanglement between the atom and the light field comes from their interaction. In this paper, we have studied the entanglement mechanism of electron-electron and photon-photon, which are from the spin-spin interaction. We found their total entanglement states are relevant both space state and spin state. When two electrons or two photons are far away, their entanglement states should be disappeared even if their spin state is entangled.
2012-01-01
The heterojunction effects of TiO2 nanotubes on photoconductive characteristics were investigated. For ITO/TiO2/Si diodes, the photocurrent is controlled either by the TiO2/Si heterojunction (p-n junction) or the ITO-TiO2 heterojunction (Schottky contact). In the short circuit (approximately 0 V) condition, the TiO2-Si heterojunction dominates the photocarrier transportation direction due to its larger space-charge region and potential gradient. The detailed transition process of the photocarrier direction was investigated with a time-dependent photoresponse study. The results showed that the diode transitioned from TiO2-Si heterojunction-controlled to ITO-TiO2 heterojunction-controlled as we applied biases from approximately 0 to -1 V on the ITO electrode. PMID:22525197
A model for electron nuclear dynamics of a monatomic chain
NASA Astrophysics Data System (ADS)
Calais, Jean-Louis; Deumens, Erik; Ohrn, Yngve
1994-05-01
The Electron Nuclear Dynamics (END) approach is developed for a linear chain in a parametrized model inspired by the PPP (Pariser-Parr-Pople) model. Particular attention is given to the model parameters, and the choice of basis functions in this time-dependent theory. The resulting equations of motion include electronic-vibrational couplings. Explicit analysis of the simplest model leads to coupling between the highest frequency longitudinal vibrational mode and the electrons.
A model for electron nuclear dynamics of a monatomic chain
NASA Astrophysics Data System (ADS)
Calais, Jean-Louis; Deumens, Erik; Öhrn, Yngve
1994-09-01
The electron nuclear dynamics (END) approach is developed for a linear chain in a parametrized model inspired by the PPP (Pariser-Parr-Pople) model. Particular attention is given to the model parameters, and the choice of basis functions in this time-dependent theory. The resulting equations of motion include electronic-vibrational couplings. Explicit analysis of the simplest model leads to coupling between the highest frequency longitudinal vibrational mode and the electrons.
Electron-Nuclear Dynamics of Molecular Systems
1994-04-18
approach with a completely general form of trial function yields the time - dependent Schr ~ dinger equation . Restricting the...dynamical equations approximating the time - dependent SchrOdinger equation . These equations govern the time evolution of the relevant state vector parameters... equations that apprximate the Apuit 18, 1994 time - dependent Schradinger equation and govern the time evolution of
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. .
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
NASA Astrophysics Data System (ADS)
Ishibashi, Akira; Kobayashi, H.; Taniguchi, T.; Kondo, K.; Kasai, T.
2016-12-01
We have calculated optical fields for waveguide-coupled orthogonal photon-photocarrier propagation solar cell (MOP3SC)in which the photons propagate in the direction orthogonal to that of the photocarriers'. By exploiting the degree of freedom along the photon propagation and using multi-semiconductor stripes in which the incoming photons first encounter the widest gap semiconductor, and the narrowest at last, we can convert virtually the whole spectrum of solar spectrum into electricity resulting in high conversion efficiency. The waveguide-coupled MOP3SC can not only optimize the absorption of light and the photocarrier collection independently converting virtually the whole spectrum of sunlight into electricity, but also can serve as a highly efficient concentration solar-cell system with low temperature rise thanks to its minimal thermal dissipation and the diffusive-light-convertibility when used with the parabola cross-section structure on top of the waveguide. The waveguide-coupled MOP3SC is also of potential interest as a high reliability system, because the high energy photons that can damage bonding of the materials, being converted into electricity already at upstream, never go into the medium or narrow gap semiconductors, resulting in low degradation of materials used in the MOP3SC.
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.
Niguès, A; Siria, A; Verlot, P
2015-09-18
The ability to cool single ions, atomic ensembles, and more recently macroscopic degrees of freedom down to the quantum ground state has generated considerable progress and perspectives in fundamental and technological science. These major advances have been essentially obtained by coupling mechanical motion to a resonant electromagnetic degree of freedom in what is generally known as laser cooling. Here, we experimentally demonstrate the first self-induced coherent cooling mechanism that is not mediated by an electromagnetic resonance. Using a focused electron beam, we report a 50-fold reduction of the motional temperature of a nanowire. Our result primarily relies on the sub-nanometre confinement of the electron beam and generalizes to any delayed and spatially confined interaction, with important consequences for near-field microscopy and fundamental nanoscale dissipation mechanisms.
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
Ultrafast dynamics of electrons at interfaces
McNeill, Jason Douglas
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
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.
Effect of Partially Screened Nuclei on Fast-Electron Dynamics
NASA Astrophysics Data System (ADS)
Hesslow, L.; Embréus, O.; Stahl, A.; DuBois, T. C.; Papp, G.; Newton, S. L.; Fülöp, T.
2017-06-01
We analyze the dynamics of fast electrons in plasmas containing partially ionized impurity atoms, where the screening effect of bound electrons must be included. We derive analytical expressions for the deflection and slowing-down frequencies, and show that they are increased significantly compared to the results obtained with complete screening, already at subrelativistic electron energies. Furthermore, we show that the modifications to the deflection and slowing down frequencies are of equal importance in describing the runaway current evolution. Our results greatly affect fast-electron dynamics and have important implications, e.g., for the efficacy of mitigation strategies for runaway electrons in tokamak devices, and energy loss during relativistic breakdown in atmospheric discharges.
Capturing atomic-scale carrier dynamics with electrons
NASA Astrophysics Data System (ADS)
Baum, Peter; Krausz, Ferenc
2017-09-01
Light-driven electronic motion unfolds on times as short as the cycle period of light and on length scales as small as the distance between two neighboring atoms in a molecule. Visualizing fundamental light-matter interactions therefore requires access to attosecond and picometer dimensions. Here we report on a potential unification of electron diffraction and microscopy with attosecond technology, which could provide a full space-time access to elementary electronic processes in matter and materials. We review recent progress in ultrafast diffraction and microscopy towards temporal resolutions approaching 10 fs by use of state-of-the-art microwave technology and discuss our latest findings on all-optical compression approaches for reaching sub-femtosecond, sub-optical-cycle resolution. Four-dimensional electron diffraction with attosecond-picometer resolution will access all dynamics outside the atomic core, offering an all-embracing insight into fundamental electron-nuclear dynamics of complex materials.
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.
Ryabinkin, Ilya G; Izmaylov, Artur F
2017-01-19
An accurate description of nonadiabatic dynamics of molecular species on metallic surfaces poses a serious computational challenge associated with a multitude of closely spaced electronic states. We propose a mixed quantum-classical scheme that addresses this challenge by introducing collective electronic variables. These variables are defined through analytic block-diagonalization applied to the time-dependent Hamiltonian matrix governing the electronic dynamics. We compare our scheme with a simplified Ehrenfest approach and with a full-memory electronic friction model on a 1D "adatom + atomic chain" model. Our simulations demonstrate that collective-mode dynamics with only a few (two to three) electronic variables is robust and can describe a variety of situations: from a chemisorbed atom on an insulator to an atom on a metallic surface. Our molecular model also reveals that the friction approach is prone to unpredictable and catastrophic failures.
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.
Electronic coherence dynamics in trans-polyacetylene oligomers.
Franco, Ignacio; Brumer, Paul
2012-04-14
Electronic coherence dynamics in trans-polyacetylene oligomers are considered by explicitly computing the time dependent molecular polarization from the coupled dynamics of electronic and vibrational degrees of freedom in a mean-field mixed quantum-classical approximation. The oligomers are described by the Su-Schrieffer-Heeger Hamiltonian and the effect of decoherence is incorporated by propagating an ensemble of quantum-classical trajectories with initial conditions obtained by sampling the Wigner distribution of the nuclear degrees of freedom. The electronic coherence of superpositions between the ground and excited and between pairs of excited states is examined for chains of different length, and the dynamics is discussed in terms of the nuclear overlap function that appears in the off-diagonal elements of the electronic reduced density matrix. For long oligomers the loss of coherence occurs in tens of femtoseconds. This time scale is determined by the decay of population into other electronic states through vibronic interactions, and is relatively insensitive to the type and class of superposition considered. By contrast, for smaller oligomers the decoherence time scale depends strongly on the initially selected superposition, with superpositions that can decay as fast as 50 fs and as slow as 250 fs. The long-lived superpositions are such that little population is transferred to other electronic states and for which the vibronic dynamics is relatively harmonic.
Special issue on ultrafast electron and molecular dynamics
NASA Astrophysics Data System (ADS)
Hishikawa, Akiyoshi; Martin, Fernando; Vrakking, Marc
2013-07-01
Your invitation to submit. Journal of Physics. B: Atomic Molecular and Optical Physics (JPhysB) is delighted to announce a forthcoming special issue on ultrafast electron and molecular dynamics to appear in 2014, and invites you to submit a paper. Within the last decade, a number of novel approaches have emerged, both experimental and theoretical, that allow the investigation of (time-resolved) molecular dynamics in novel ways not anticipated before. Experimentally, the introduction of novel light sources such as high-harmonic generation and XUV/x-ray free electron lasers, and the emergence of novel detection strategies, such as time-resolved electron/x-ray diffraction and the fully coincident detection of electrons and fragment ions in reaction microscopes, has significantly expanded the arsenal of available techniques, and has taken studies of molecular dynamics into new domains of spectroscopic, spatial and temporal resolution, the latter including first explorations into the attosecond domain. Along the way, particular types of molecular dynamics, such as dynamics around conical intersections, have gained an increased prominence, sparked by an emerging realization about the essential role that this dynamics plays in relaxation pathways in important bio-molecular systems. The progress on the theoretical side has been no less impressive. Novel generations of supercomputers and a series of novel computational strategies have allowed nearly exact calculations in small molecules, as well as highly successful approximate calculations in large, polyatomic molecules. Frequent and intensive collaborations involving both theory and experiment have been essential for the progress that has been accomplished. The special issue 'Ultrafast electron and molecular dynamics' seeks to provide an overview of some of the most important developments in the field, while at the same time indicating how studies of (time-resolved) molecular dynamics are likely to evolve in the coming
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.
Identifying the Stern-Gerlach force of classical electron dynamics.
Wen, Meng; Bauke, Heiko; Keitel, Christoph H
2016-08-22
Different classical theories are commonly applied in various branches of physics to describe the relativistic dynamics of electrons by coupled equations for the orbital motion and spin precession. Exemplarily, we benchmark the Frenkel model and the classical Foldy-Wouthuysen model with spin-dependent forces (Stern-Gerlach forces) to the quantum dynamics as predicted by the Dirac equation. Both classical theories can lead to different or even contradicting predictions how the Stern-Gerlach forces modify the electron's orbital motion, when the electron moves in strong electromagnetic field configurations of emerging high-intensity laser facilities. In this way, one may evaluate the validity and identify the limits of these classical theories via a comparison with possible experiments to provide a proper description of spin-induced dynamics. Our results indicate that the Foldy-Wouthuysen model is qualitatively in better agreement with the Dirac theory than the widely used Frenkel model.
Spin Dynamics of Electrons Confined in Silicon Heterostructures
NASA Astrophysics Data System (ADS)
Jock, Ryan Michael
The spin states of electrons confined in silicon heterostructures have shown promise as qubits for quantum information processing. Recently, a host of single and few electron silicon quantum dot device architectures have arisen as implementations for quantum computation. These devices often combine regions of low density two-dimensional (2D) electrons, localized electrons, and interfaces depleted of electrons. Electron spin resonance (ESR) is a unique tool for probing the spin dynamics of both mobile and localized electrons at silicon heterointerfaces and investigating the effects limiting the ability to control electrons and their spin states in these structures. We use a continuous wave ESR method to examine localized 2D electron band-tail states at Si/SiO 2 interfaces in large area metal-oxide-semiconductor transistors. We compare two devices, fabricated in different laboratories, which display similar low temperature (4.2 K) peak mobilities. We find that one of the devices displays a smaller band-tail density of confined states and a shallower characteristic confinement. Thus, ESR reveals a difference in device quality, which is not apparent from mobility measurements, and is a valuable tool for evaluating the interface quality in Si/SiO2 heterostructures. Additionally, we use pulsed ESR techniques to study the spin dynamics of electrons confined in Si/SiGe heterostructures. For mobile 2D electrons, the density-dependent Dyakonov-Perel mechanism dominates spin relaxation. At low 2D densities, stronger electron-electron interactions cause an increase in the electron effective mass, leading to an increase in spin susceptibility. For very low densities, natural disorder localizes electrons at the silicon heterointerface. Naturally localized electrons in these structures display short spin relaxation times (< 0.1 ms). By electrostatically confining electrons to quantum dots, the spin relaxation time may be extended. We fabricate large-area dual-gated devices which
Yamada, Yasuhiro; Sato, Hiroki K; Hikita, Yasuyuki; Hwang, Harold Y; Kanemitsu, Yoshihiko
2013-07-26
The photocarrier relaxation dynamics of an n-type LaAlO3/SrTiO3 heterointerface is investigated using femtosecond transient absorption (TA) spectroscopy at low temperatures. In both LaAlO3/SrTiO3 heterostructures and electron-doped SrTiO3 bulk crystals, the TA spectrum shows a Drude-like free carrier absorption immediately after excitation. In addition, a broad absorption band gradually appears within 40 ps, which corresponds to the energy relaxation of photoexcited free electrons into self-trapped polaron states. We reveal that the polaron formation time is enhanced considerably at the LaAlO3/SrTiO3 heterointerface as compared to bulk crystals. Further, we discuss the interface effects on the electron relaxation dynamics in conjunction with the splitting of the t2g subbands due to the interface potential.
Relaxation and possible dynamical transition in electron glass
NASA Astrophysics Data System (ADS)
Bhandari, Preeti; Malik, Vikas; Kumar, Deepak
2017-05-01
We have considered here the relaxation properties of three dimensional lattice model of an electron glass. We have modeled the kinetics of site-occupation numbers as Ising spins by Kawasaki Dynamics. The master equation governing the dynamics is approximated by making mean field approximation. We have calculated the eigenvalues and localization characteristics of the linear dynamical matrix. The behavior of the eigenvalues at different temperatures is used to detect the presence of a possible dynamical transition. We have also calculated eigenvalues of inverse susceptibility matrix and its behavior with temperature is used as additional input to analyze the slow dynamics and aging. Due to localized states having long lifetime the dynamics of the system slows down with decreasing temperature. We found the gap exponent of density of states of Hartree energy to be close to δ≈d-1 as predicted by Efros and Shklovskii.
Dynamics of boundary layer electrons around a laser wakefield bubble
NASA Astrophysics Data System (ADS)
Luo, J.; Chen, M.; Zhang, G.-B.; Yuan, T.; Yu, J.-Y.; Shen, Z.-C.; Yu, L.-L.; Weng, S.-M.; Schroeder, C. B.; Esarey, E.
2016-10-01
The dynamics of electrons forming the boundary layer of a highly nonlinear laser wakefield driven in the so called bubble or blowout regime is investigated using particle-in-cell simulations. It is shown that when the driver pulse intensity increases or the focal spot size decreases, a significant amount of electrons initially pushed by the laser pulse can detach from the bubble structure at its tail, middle, or front and form particular classes of waves locally with high densities, referred to as the tail wave, lateral wave, and bow wave. The tail wave and bow wave correspond to real electron trajectories, while the lateral wave does not. The detached electrons can be ejected transversely, containing considerable energy, and reducing the efficiency of the laser wakefield accelerator. Some of the transversely emitted electrons may obtain MeV level energy. These electrons can be used for wake evolution diagnosis and producing high frequency radiation.
Controlling Electron Dynamics of Oriented Molecules Using Attosecond Pulses
NASA Astrophysics Data System (ADS)
Miyabe, S.; Lucchese, R.; Rescigno, T.; Midorikawa, K.; McCurdy, C. W.
2016-05-01
Attosecond pulses offer routes to study and potentially manipulate ultrafast electron dynamics of atoms and molecules on their intrinsic time scale, and therefore attracted attention from various disciplines. In this report we show that for a molecule, oriented in space and excited by an attosecond pulse, the amount of electronic coherence left in the ion depends not only on the orientation of the electric field polarization vector in the molecular-frame, but also on the angular distribution in molecular-frame of electrons ejected in different ionization channels. In our numerical simulation we use one-photon single ionization amplitudes calculated using the complex-Kohn variational method, and we express the amount of coherence in the ion in terms of the (N+1)-electron reduced density matrix of the full N-electron system of the ion plus ionized electron.
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
Modeling electron cloud dynamics in high-frequency accelerators
NASA Astrophysics Data System (ADS)
Veitzer, Seth A.; Stoltz, Peter H.
2017-03-01
The dynamics of electron cloud buildup, saturation, and dissipation represent a complex interaction between accelerator and beam parameters. In many accelerators bunch charges are large and beam frequencies are small. In this case electrons have a good probability of being accelerated to the opposite side of the beam pipe before the next bunch crossing. If the time for electrons to drift across the beam pipe is less than the time to the next bunch crossing the cloud density can build up rapidly under this scenario. However, in accelerators where buch charges are small and beam frequencies are large, electrons created by secondary electron emission will not be accelerated to the opposite wall before the next bunch crossing. In this case the time for a cloud to build up is larger, but the amount of electron cloud that exists close to the beam may be increased. In this paper, we report simulation results for modeling of electron cloud buildup and dynamics in high-frequency accelerators. We model parameters relevant to the JLab Electron-Ion Collider (JLEIC) that is currently being designed. We consider beam frequencies up to 476 MHz for a variety of different ions, from protons up to Pb (82+), and with bunch charges ranging from 4.2 × 109 (p) to 0.05 × 109 (Pb) ions per bunch, and ion energies from 100 (p) - 40 (Pb) GeV/u. We compare simulations of electron cloud buildup and dynamics for these different cases, and contrast with similar simulations of proton-driven electron cloud buildup in the Fermilab recycler under the PIP-II upgrade scenario, with a frequency of 52.8 MHz, bunch charge of 80 × 109 p/bunch, and energies ranging from 8 - 20 GeV.
Electron temperature dynamics of TEXTOR plasmas
NASA Astrophysics Data System (ADS)
Udintsev, Victor Sergeevich
2003-11-01
To study plasma properties in the presence of large and small MHD modes, new high-resolution ECE diagnostics have been installed at TEXTOR tokamak, and some of the already existing systems have been upgraded. Two models for the plasma transport properties inside large m/n = 2/1 MHD islands have been found to give estimations for the heat diffusivities, which are much lower than the global plasma heat diffusivity, which is in agreement with previous measurements in different tokamaks. The 3D-reconstruction of large m/n = 2/1 modes in TEXTOR with the help of all available ECE diagnostics allows modelling the island as a structure with closed flux surfaces. The main plasma heat flux flows through the X-point area probably along stochastic magnetic field lines. The confinement is improved within the magnetic island, compared to the background plasma. This is confirmed by a temperature profile flattening and sometimes even a secondary peaking inside the island, compared to the X-point. Making use of the mode rotation, assumed to be a rigid rotor, it has been possible to obtain information on the topology of the m = 1 precursor mode leading to sawtooth collapses. It becomes clear that this precursor cannot be described by an m = 1 cold tearing mode island but by a hot crescent wrapped around a cold high-density bubble. In the future multi-chord ECE-imaging will allow this mode reconstruction without the assumption of the rotation to be rigid. From the measurements of the broadband temperature and density fluctuations one can conclude that the turbulent structures inside the q = 1 surface are separated from the turbulence outside the q = 1 surface. This fits nicely with the observation that q = 1 surface acts as a barrier for the thermal transport. Correlation length and time measured inside q = 1 are in agreement with the observed turbulent heat diffusivity. Qualitative studies of non-thermal electrons at different heating regimes (ECRH and Ohmic) at TEXTOR were done
Solvent as electron donor: Donor/acceptor electronic coupling is a dynamical variable
Castner, E.W. Jr.; Kennedy, D.; Cave, R.J.
2000-04-06
The authors combine analysis of measurements by femtosecond optical spectroscopy, computer simulations, and the generalized Mulliken-Hush (GMH) theory in the study of electron-transfer reactions and electron donor-acceptor interactions. The study focus is on ultrafast photoinduced electron-transfer reactions from aromatic amine solvent donors to excited-state acceptors. The experimental results from femtosecond dynamical measurements fall into three categories: six coumarin acceptors reductively quenched by N,N-dimethylaniline (DMA), eight electron-donating amine solvents reductively quenching coumarin 152 (7-(dimethylamino)-4-(trifluoromethyl)-coumarin), and reductive quenching dynamics of two coumarins by DMA as a function of dilution in the nonreactive solvents toluene and chlorobenzene. Applying a combination of molecular dynamics trajectories, semiempirical quantum mechanical calculations (of the relevant adiabatic electronic states), and GMH theory to the C152/DMA photoreaction, the authors calculate the electron donor/acceptor interaction parameter H{sub DA} at various time frames, H{sub DA} is strongly modulated by both inner-sphere and outer-sphere nuclear dynamics, leading us to conclude that H{sub DA} must be considered as a dynamical variable.
Electron spin dynamics in cubic GaN
NASA Astrophysics Data System (ADS)
Buß, J. H.; Schupp, T.; As, D. J.; Brandt, O.; Hägele, D.; Rudolph, J.
2016-12-01
The electron spin dynamics in cubic GaN is comprehensively investigated by time-resolved magneto-optical Kerr-rotation spectroscopy over a wide range of temperatures, magnetic fields, and doping densities. The spin dynamics is found to be governed by the interplay of spin relaxation of localized electrons and Dyakonov-Perel relaxation of delocalized electrons. Localized electrons significantly contribute to spin relaxation up to room temperature at moderate doping levels, while Dyakonov-Perel relaxation dominates for high temperatures or degenerate doping levels. Quantitative agreement to Dyakonov-Perel theory requires a larger value of the spin-splitting constant than theoretically predicted. Possible reasons for this discrepancy are discussed, including the role of charged dislocations.
Imaging the dynamics of free-electron Landau states
NASA Astrophysics Data System (ADS)
Schattschneider, P.; Schachinger, Th.; Stöger-Pollach, M.; Löffler, S.; Steiger-Thirsfeld, A.; Bliokh, K. Y.; Nori, Franco
2014-08-01
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.
Phase-space dynamics of runaway electrons in magnetic fields
Guo, Zehua; McDevitt, Christopher Joseph; Tang, Xian-Zhu
2017-02-16
Dynamics of runaway electrons in magnetic fields are governed by the competition of three dominant physics: parallel electric field acceleration, Coulomb collision, and synchrotron radiation. Examination of the energy and pitch-angle flows reveals that the presence of local vortex structure and global circulation is crucial to the saturation of primary runaway electrons. Models for the vortex structure, which has an O-point to X-point connection, and the bump of runaway electron distribution in energy space have been developed and compared against the simulation data. Lastly, identification of these velocity-space structures opens a new venue to re-examine the conventional understanding of runawaymore » electron dynamics in magnetic fields.« less
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
2014-08-08
Landau levels and states of electrons in a magnetic field are fundamental quantum entities underlying the quantum Hall and related effects in condensed matter physics. However, the real-space properties and observation of Landau wave functions remain elusive. Here we report the real-space observation of Landau states and the internal rotational dynamics of free electrons. States with different quantum numbers are produced using nanometre-sized electron vortex beams, with a radius chosen to match the waist of the Landau states, in a quasi-uniform magnetic field. Scanning the beams along the propagation direction, we reconstruct the rotational dynamics of the Landau wave functions with angular frequency ~100 GHz. We observe that Landau modes with different azimuthal quantum numbers belong to three classes, which are characterized by rotations with zero, Larmor and cyclotron frequencies, respectively. This is in sharp contrast to the uniform cyclotron rotation of classical electrons, and in perfect agreement with recent theoretical predictions.
Phase-space dynamics of runaway electrons in magnetic fields
NASA Astrophysics Data System (ADS)
Guo, Zehua; McDevitt, Christopher J.; Tang, Xian-Zhu
2017-04-01
Dynamics of runaway electrons in magnetic fields are governed by the competition of three dominant physics: parallel electric field acceleration, Coulomb collision, and synchrotron radiation. Examination of the energy and pitch-angle flows reveals that the presence of local vortex structure and global circulation is crucial to the saturation of primary runaway electrons. Models for the vortex structure, which has an O-point to X-point connection, and the bump of runaway electron distribution in energy space have been developed and compared against the simulation data. Identification of these velocity-space structures opens a new venue to re-examine the conventional understanding of runaway electron dynamics in magnetic fields.
NASA Astrophysics Data System (ADS)
Wang, Jing; Mandelis, Andreas; Melnikov, Alexander
2015-06-01
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 radiative recombination photon emissions and exclusion of thermal infrared photons, has been applied to a coupled PbS CQD thin film with inter-dot spacing of 0.5 nm to 1 nm for the analysis of charge transport properties. As the nanoparticle bandgap depends on the size of the quantum dots, polydispersity of the CQD thin film causes bandgap variability leading to photoexcited carrier (exciton) decay lifetime broadening and temperature dependence. The carrier transport mechanisms of QDs are quite different from bulk semiconductors, so the conventional carrier-diffusion wave-based PCR theory was modified into a non-diffusive limit model. A developed variational discrete lifetime reconstruction approach was used to analyze PCR frequency scans under two optical excitation modes: a modulated laser source without, and with, an additional continuous laser source. Using this model, the CQD mean lifetime values were found and variational discrete lifetime spectra were reconstructed.
Electronic neural network for dynamic resource allocation
NASA Technical Reports Server (NTRS)
Thakoor, A. P.; Eberhardt, S. P.; Daud, T.
1991-01-01
A VLSI implementable neural network architecture for dynamic assignment is presented. The resource allocation problems involve assigning members of one set (e.g. resources) to those of another (e.g. consumers) such that the global 'cost' of the associations is minimized. The network consists of a matrix of sigmoidal processing elements (neurons), where the rows of the matrix represent resources and columns represent consumers. Unlike previous neural implementations, however, association costs are applied directly to the neurons, reducing connectivity of the network to VLSI-compatible 0 (number of neurons). Each row (and column) has an additional neuron associated with it to independently oversee activations of all the neurons in each row (and each column), providing a programmable 'k-winner-take-all' function. This function simultaneously enforces blocking (excitatory/inhibitory) constraints during convergence to control the number of active elements in each row and column within desired boundary conditions. Simulations show that the network, when implemented in fully parallel VLSI hardware, offers optimal (or near-optimal) solutions within only a fraction of a millisecond, for problems up to 128 resources and 128 consumers, orders of magnitude faster than conventional computing or heuristic search methods.
Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses
NASA Astrophysics Data System (ADS)
Calegari, F.; Ayuso, D.; Trabattoni, A.; Belshaw, L.; De Camillis, S.; Anumula, S.; Frassetto, F.; Poletto, L.; Palacios, A.; Decleva, P.; Greenwood, J. B.; Martín, F.; Nisoli, M.
2014-10-01
In the past decade, attosecond technology has opened up the investigation of ultrafast electronic processes in atoms, simple molecules, and solids. Here, we report the application of isolated attosecond pulses to prompt ionization of the amino acid phenylalanine and the subsequent detection of ultrafast dynamics on a sub-4.5-femtosecond temporal scale, which is shorter than the vibrational response of the molecule. The ability to initiate and observe such electronic dynamics in polyatomic molecules represents a crucial step forward in attosecond science, which is progressively moving toward the investigation of more and more complex systems.
Ultrafast electron dynamics in phenylalanine initiated by attosecond pulses.
Calegari, F; Ayuso, D; Trabattoni, A; Belshaw, L; De Camillis, S; Anumula, S; Frassetto, F; Poletto, L; Palacios, A; Decleva, P; Greenwood, J B; Martín, F; Nisoli, M
2014-10-17
In the past decade, attosecond technology has opened up the investigation of ultrafast electronic processes in atoms, simple molecules, and solids. Here, we report the application of isolated attosecond pulses to prompt ionization of the amino acid phenylalanine and the subsequent detection of ultrafast dynamics on a sub-4.5-femtosecond temporal scale, which is shorter than the vibrational response of the molecule. The ability to initiate and observe such electronic dynamics in polyatomic molecules represents a crucial step forward in attosecond science, which is progressively moving toward the investigation of more and more complex systems.
Kinetic modelling of runaway electrons in dynamic scenarios
NASA Astrophysics Data System (ADS)
Stahl, A.; Embréus, O.; Papp, G.; Landreman, M.; Fülöp, T.
2016-11-01
Improved understanding of runaway-electron formation and decay processes are of prime interest for the safe operation of large tokamaks, and the dynamics of the runaway electrons during dynamical scenarios such as disruptions are of particular concern. In this paper, we present kinetic modelling of scenarios with time-dependent plasma parameters; in particular, we investigate hot-tail runaway generation during a rapid drop in plasma temperature. With the goal of studying runaway-electron generation with a self-consistent electric-field evolution, we also discuss the implementation of a collision operator that conserves momentum and energy and demonstrate its properties. An operator for avalanche runaway-electron generation, which takes the energy dependence of the scattering cross section and the runaway distribution into account, is investigated. We show that the simplified avalanche model of Rosenbluth and Putvinskii (1997 Nucl. Fusion 37 1355) can give inaccurate results for the avalanche growth rate (either lower or higher) for many parameters, especially when the average runaway energy is modest, such as during the initial phase of the avalanche multiplication. The developments presented pave the way for improved modelling of runaway-electron dynamics during disruptions or other dynamic events.
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.
Dynamics of electron transfer and exciton formation at interfaces
NASA Astrophysics Data System (ADS)
Wolf, Martin
2014-03-01
The combination of inorganic semiconductors with organic molecules to hybrid systems promises superior functionality of the interface compared to optoelectronic properties of the single materials. We have investigated the electron dynamics of the ZnO(10-10) surface and the influence of hydrogen and several organic molecules on the electronic structure using time-resolved two-photon-photoemission (2PPE) spectroscopy. Hydrogen termination leads to the formation a metallic ZnO surface, whereas e.g. by pyridine adsorption a substantial work function reduction up to 2.9 eV is achieved, which can be useful controlling the energy level alignment at inorganic/organic interfaces. Furthermore, we directly monitor the hot electron relaxation in the ZnO conduction band and the formation of an excitonic state at the surface within a few ps, which decays mediated a thermal activated process on a 100 ps timescale. In a second set of experiments we have studied the dynamics of photoinduced electron transfer and solvation processes at the water ice-metal interface and the effect of co-adsorbed alkali ions (Na, K, Cs). Time-resolved 2PPE provides direct access to elementary processes like electron injection and the subsequent solvation dynamics which competes with the electron transfer back to the Cu(111) substrate. In particular, we study the electronic structure changes and ultrafast dynamics for the bulid-up of a solvation shell (up to about 6 water molecules) around individual alkali atoms at the metal surface. For ice mulitlayers doped with alkali ions we observe the formation of longlived electron alkali-water complexes.
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
2009-02-26
In the late 1970s Meyer and Miller (MM) [J. Chem. Phys. 1979, 70, 3214.] 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 by treating the nuclear and electronic degrees of freedom (DOF) in an equivalent dynamical framework (i.e., by classical mechanics), thereby describing nonadiabatic dynamics in a more unified manner. Much later Stock and Thoss (ST) [Phys. Rev. Lett. 1997, 78, 578.] 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 Schrodinger 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 nonadiabatic 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 nonadiabaticity 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.
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.
Instantaneous band gap collapse in photoexcited monoclinic VO2 due to photocarrier doping.
Wegkamp, Daniel; Herzog, Marc; Xian, Lede; Gatti, Matteo; Cudazzo, Pierluigi; McGahan, Christina L; Marvel, Robert E; Haglund, Richard F; Rubio, Angel; Wolf, Martin; Stähler, Julia
2014-11-21
Using femtosecond time-resolved photoelectron spectroscopy we demonstrate that photoexcitation transforms monoclinic VO2 quasi-instantaneously into a metal. Thereby, we exclude an 80 fs structural bottleneck for the photoinduced electronic phase transition of VO2. First-principles many-body perturbation theory calculations reveal a high sensitivity of the VO2 band gap to variations of the dynamically screened Coulomb interaction, supporting a fully electronically driven isostructural insulator-to-metal transition. We thus conclude that the ultrafast band structure renormalization is caused by photoexcitation of carriers from localized V 3d valence states, strongly changing the screening before significant hot-carrier relaxation or ionic motion has occurred.
NASA Astrophysics Data System (ADS)
Tang, Xin; Wu, Guang Fu; Lai, King Wai Chiu
2017-06-01
We report a strategy to realize and facilitate the photocarrier transport from mercury selenium colloidal quantum dots (HgSe CQDs) into silicon with the assistance of twisted graphene. A nanocomposite material consisting of HgSe CQDs and twisted graphene has been synthesized. By bringing the nanocomposites into contact with silicon, a HgSe CQD-twisted graphene nanocomposite/silicon junction was fabricated and demonstrated photoresponses in the long-wave infrared range. In the nanocomposites, the surface of twisted graphene was decorated with HgSe CQDs. Benefiting from the twisted structure in the nanocomposites, the active sensing area and light-matter interaction length are greatly increased. Driven by the interfacial built-in potential, photocarriers directly transfer from HgSe CQDs into the twist graphene, which serves as a fast carrier transport pathway to silicon, leading to high photocarrier collection efficiency. Compared with vertically stacked HgSe CQD film/flat graphene, the application of HgSe CQD-twisted graphene nanocomposites avoids photocarriers transporting via the hopping mechanism and over 2700% enhancement ratio of spectral responsivity was achieved, reaching 31.5 mA/W@9 μm. The interfacial energy band diagram was deduced for a better understanding of the photocarrier transfer process occurring at the interface between HgSe colloidal quantum dots, twist graphene, and silicon.
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
Electron nuclear dynamics of H + + H 2O collisions
NASA Astrophysics Data System (ADS)
Hedström, M.; Morales, J. A.; Deumens, E.; Öhrn, Y.
1997-11-01
Proton water collisions at 46 eV in the center of mass frame are studied within the electron nuclear dynamics theory (END). The electronic degrees of freedom are described with a coherent state formulation of determinantal wavefunctions. The nuclei are treated as classical particles but full nonadiabatic couplings are retained. The equations of motion are formulated in a generalized phase space and bypass the use of preconstructed potential energy surfaces. Differential cross sections for inelastic and electron transfer reactions as well as energy transfer are compared with experiment.
Carrier dynamics in type-II quantum dots for wide-bandgap intermediate-band solar cells
NASA Astrophysics Data System (ADS)
Tayagaki, Takeshi; Sugaya, Takeyoshi
2016-03-01
Type-II quantum dots (QDs) have attracted attention for the formation of multiband solar cells based on the intermediate-band (IB) concept. The type-II confinement potential causes a spatial separation between electrons and holes, which strongly suppresses the carrier recombination in the QDs. As a result, the carrier lifetime in the QDs increases, which results in an increase in the number of photocarriers in the QDs under continuous light irradiation. This enhanced carrier number in the IB has an advantage for efficient two-step photon absorption because the probability of the second optical excitation to extract carriers from the QDs depends on the number of photocarriers in the QDs. Thus far, type-II QDs, such as GaSb/GaAs and Ge/Si QDs, have been introduced to demonstrate the operation principle of IB solar cells. In narrow-bandgap semiconductors, however, the photocarriers are extracted from the QDs by thermal excitation, which causes reduced carrier lifetime even in type-II QDs, and inefficient two-step photon absorption. In this paper, the carrier dynamics in type-II InP QDs in the wide-bandgap InGaP host are investigated by using time-resolved optical spectroscopy. The photoluminescence spectra of the InP QDs exhibit a high-energy shift with increasing excitation power density, which is a typical behavior of type-II QDs. Time-resolved photoluminescence measurements show a longer carrier lifetime in type-II InP QDs compared to that in the well-known type-I InAs QDs. Temperature dependent photoluminescence of the photoluminescence indicates that type-II InP QDs in the InGaP host are a promising candidate for realizing IB solar cells.
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.
High-Harmonic Generation Enhanced by Dynamical Electron Correlation
NASA Astrophysics Data System (ADS)
Tikhomirov, Iliya; Sato, Takeshi; Ishikawa, Kenichi L.
2017-05-01
We theoretically study multielectron effects in high-harmonic generation (HHG), using all-electron first-principles simulations for a one-dimensional model atom. In addition to the usual plateau and cutoff (from a cation in the present case, since the neutral is immediately ionized), we find a prominent resonance peak far above the plateau and a second plateau extended beyond the first cutoff. These features originate from the dication response enhanced by orders of magnitude due to the action of the Coulomb force from the rescattering electron, and, hence, are a clear manifestation of electron correlation. Although the present simulations are done in 1D, the physical mechanism underlying the dramatic enhancement is expected to hold also for three-dimensional real systems. This will provide new possibilities to explore dynamical electron correlation in intense laser fields using HHG, which is usually considered to be of single-electron nature in most cases.
Nonadiabatic dynamics at metal surfaces: Independent-electron surface hopping
NASA Astrophysics Data System (ADS)
Shenvi, Neil; Roy, Sharani; Tully, John C.
2009-05-01
Recent experiments have shown convincing evidence for nonadiabatic energy transfer from adsorbate degrees of freedom to surface electrons during the interaction of molecules with metal surfaces. In this paper, we propose an independent-electron surface hopping algorithm for the simulation of nonadiabatic gas-surface dynamics. The transfer of energy to electron-hole pair excitations of the metal is successfully captured by hops between electronic adiabats. The algorithm is able to account for the creation of multiple electron-hole pairs in the metal due to nonadiabatic transitions. Detailed simulations of the vibrational relaxation of nitric oxide on a gold surface, employing a multistate potential energy surface fit to density functional theory calculations, confirm that our algorithm can capture the underlying physics of the inelastic scattering process.
Dynamics of Photocarriers in Crystalline α-Al_2O3 and MgO
NASA Astrophysics Data System (ADS)
Shan, Jie; Wang, Feng; Bonn, Mishca; Heinz, Tony F.
2003-03-01
The lifetime of mobile carriers in crystalline insulators is often very short because of the presence of traps, as well as exciton localization effects. Consequently direct measurement of the lifetime are challenging. Here we report application of terahertz time-domain spectroscopy together with ultrafast optical excitation [1] to probe photo-generated carriers in crystalline α-Al_2O3 (sapphire) and MgO. In high purity samples, carrier lifetimes ˜ 100 ps are observed. Sapphire shows a single exponential behavior, while bi-exponential decay is seen in MgO. We analyze these results, and their temperature dependence, in terms of a model based on trap states. 1. E Knoesel, M. Bonn, J. Shan, and T.F. Heinz, Phys. Rev. Lett. 86, 340 (2001)
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.
Photocarrier transport and dynamics in mixed-phase BiFeO_{3} films.
Li, Pan; Dong, Xianglei; Gao, Yuqiang; Ren, Lixia; Jin, Kexin
2016-04-18
We report a remarkable photoinduced relaxation process and its dependence of thickness and temperature in mixed-phase BiFeO_{3} films grown on (001) LaAlO_{3} substrates. When the films are illuminated by the light above the bandgap, their resistances are reduced with the increase of temperature. The photoinduced change of resistance reaches to the maximum of about 2.17 × 10^{5%} at 300 K. It is noted that the relaxation processes of the resistance are significantly different between T-like phase and T-R mixed phase due to structural strain, symmetry breaking and built-in electric field at the phase boundaries. These results provide more insights into intrinsic mechanisms of mixed-phase multiferroic materials and potential applications in all-oxide photoelectric devices.
Hot electron dynamics and impurity scattering on gold nanoshell surfaces
NASA Astrophysics Data System (ADS)
Wolfgang, John Adam
2000-10-01
Recent ultrafast pump-probe experiments studying the relaxation rate of an optically excited hot electron distribution on Au/Au2S gold nanoshells indicate that this relaxation rate can be modified by the chemical environment surrounding the shell. This work will begin a theoretical investigation of the effect of chemical adsorbates---solvents and impurities---upon nanoshell hot electron dynamics. The effects of water, polyvinyl alcohol (PVA), sulfur, p-aminobenzoic acid, p-mercaptobenzoic acid and propylamine adsorbates are examined for their electronic interaction with a noble metal surface. p-Aminobenzoic acid is found to have a very large dipole moment when adsorbed to the metal surface, in contrast to p-mercaptobenzoic acid, propylamine and water. This correlates well to the experimentally observed results where nanoshells dispersed in an aqueous soulution with p-aminobenzoic acid display a faster relaxation rate compared to nanoshells dispersed in a pure water, aqueous propylamine or aqueous p-mercaptobenzoic acid environments. This thesis will also introduce a non-equilibrium Green's function approach, based on the formalism developed by Baym and Kadanoff, to model the dynamics of a hot electron distribution. The model will be discussed in terms of a simple potential scattering mechanism, which may in later work be expanded to include more complex electron-electron and electron-phonon interactions. Lastly acoustic oscillation modes are calculated for solid gold spheres and gold-silicon nanoshells. These modes describe an effect of electron-phonon coupling between the hot electron distribution and the nanoshell lattice, whereby the electronic energy is converted into mechanical energy.
Calculation of Cross Sections in Electron-Nuclear Dynamics
NASA Astrophysics Data System (ADS)
Cabrera-Trujillo, R.; Sabin, John R.; Deumens, E.; Öhrn, Y.
In this work, we present an overview of the study of total and differential cross section calculations within the electron-nuclear dynamics (END). END is a method to solve the time-dependent Schrödinger equation in a non-adiabatic approach to direct dynamics. The method takes advantage of a coherent state representation of the molecular wave function. A quantum-mechanical Lagrangian formulation is employed to approximate the Schrödinger equation, via the time-dependent variational principle, to a set of coupled first-order differential equations in time for the END. We obtain the final wave function for the system allowing the determination of collisional properties of interest, as for example, deflection functions, charge exchange probabilities and amplitudes, and differential cross sections. We discuss the use and selection of basis sets for both the electronic description of the colliding systems as well as for their importance in the description of electron capture. As quantum effects are important in many cases and lacking for classical nuclei, we discuss the Schiff methodology and its advantages over other traditional methods for including semiclassical corrections. Time-lapse rendering of the dynamics of the participating electrons and atomic nuclei provides for a detailed view of dynamical and reactive processes. Comparison to experimental and other theoretical results is provided where appropriate data are available.
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.
Classical molecular dynamics simulation of electronically non-adiabatic processes.
Miller, William H; Cotton, Stephen J
2016-12-22
Both classical and quantum mechanics (as well as hybrids thereof, i.e., semiclassical approaches) find widespread use in simulating dynamical processes in molecular systems. For large chemical systems, however, which involve potential energy surfaces (PES) of general/arbitrary form, it is usually the case that only classical molecular dynamics (MD) approaches are feasible, and their use is thus ubiquitous nowadays, at least for chemical processes involving dynamics on a single PES (i.e., within a single Born-Oppenheimer electronic state). This paper reviews recent developments in an approach which extends standard classical MD methods to the treatment of electronically non-adiabatic processes, i.e., those that involve transitions between different electronic states. The approach treats nuclear and electronic degrees of freedom (DOF) equivalently (i.e., by classical mechanics, thereby retaining the simplicity of standard MD), and provides "quantization" of the electronic states through a symmetrical quasi-classical (SQC) windowing model. The approach is seen to be capable of treating extreme regimes of strong and weak coupling between the electronic states, as well as accurately describing coherence effects in the electronic DOF (including the de-coherence of such effects caused by coupling to the nuclear DOF). A survey of recent applications is presented to illustrate the performance of the approach. Also described is a newly developed variation on the original SQC model (found universally superior to the original) and a general extension of the SQC model to obtain the full electronic density matrix (at no additional cost/complexity).
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.
Phase-space dynamics of runaway electrons in tokamaks
Guan Xiaoyin; Qin Hong; Fisch, Nathaniel J.
2010-09-15
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.
Ab initio calculations of correlated electron dynamics in ultrashort pulses
NASA Astrophysics Data System (ADS)
Feist, Johannes
2010-03-01
The availability of ultrashort and intense light pulses on the femtosecond and attosecond timescale promises to allow to directly probe and control electron dynamics on their natural timescale. A crucial ingredient to understanding the dynamics in many-electron systems is the influence of electron correlation, induced by the interelectronic repulsion. In order to study electron correlation in ultrafast processes, we have implemented an ab initio simulation of the two-electron dynamics in helium atoms. We solve the time-dependent Schr"odinger equation in its full dimensionality, with one temporal and five spatial degrees of freedom in linearly polarized laser fields. In our computational approach, the wave function is represented through a combination of time-dependent close coupling with the finite element discrete variable representation, while time propagation is performed using an Arnoldi-Lanczos approximation with adaptive step size. This approach is optimized to allow for efficient parallelization of the program and has been shown to scale linearly using up to 1800 processor cores for typical problem sizes. This has allowed us to perform highly accurate and well- converged computations for the interaction of ultrashort laser pulses with He. I will present some recent results on using attosecond and femtosecond pulses to probe and control the temporal structure of the ionization process. This work was performed in collaboration with Stefan Nagele, Renate Pazourek, Andreas Kaltenb"ack, Emil Persson, Barry I. Schneider, Lee A. Collins, and Joachim Burgd"orfer.
Born-Oppenheimer Dynamics, Electronic Friction, and the Inclusion of Electron-Electron Interactions
NASA Astrophysics Data System (ADS)
Dou, Wenjie; Miao, Gaohan; Subotnik, Joseph E.
2017-07-01
We present a universal expression for the electronic friction as felt by a set of classical nuclear degrees of freedom (DOFs) coupled to a manifold of quantum electronic DOFs; no assumptions are made regarding the nature of the electronic Hamiltonian and electron-electron repulsions are allowed. Our derivation is based on a quantum-classical Liouville equation for the coupled electronic-nuclear motion, followed by an adiabatic approximation whereby electronic transitions are assumed to equilibrate faster than nuclear movement. The resulting form of friction is completely general, but does reduce to previously published expressions for the quadratic Hamiltonian (i.e., Hamiltonians without electronic correlation). At equilibrium, the second fluctuation-dissipation theorem is satisfied and the frictional matrix is symmetric. To demonstrate the importance of electron-electron correlation, we study electronic friction within the Anderson-Holstein model, where a proper treatment of electron-electron interactions shows signatures of a Kondo resonance and a mean-field treatment is completely inadequate.
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
Ab initio electronic and lattice dynamical properties of cerium dihydride
NASA Astrophysics Data System (ADS)
Gurel, Tanju; Eryigit, Resul
2007-03-01
The rare-earth metal hydrides are interesting systems because of the dramatic structural and electronic changes due to the hydrogen absorption and desorption. Among them, cerium dihydride (CeH2) is one of the less studied rare-earth metal-hydride. To have a better understanding, we have performed an ab initio study of electronic and lattice dynamical properties of CeH2 by using pseudopotential density functional theory within local density approximation (LDA) and a plane-wave basis. Electronic band structure of CeH2 have been obtained within LDA and as well as GW approximation. Lattice dynamical properties are calculated using density functional perturbation theory. The phonon spectrum is found to contain a set of high-frequency (˜ 850-1000 cm-1) optical bands, mostly hydrogen related, and low frequency cerium related acoustic modes climbing to 160 cm^ -1 at the zone boundary.
Study of non-equilibrium electron dynamics in metals
NASA Astrophysics Data System (ADS)
Ibrahim, Wael Mohamed Gomaa
Thermal phenomena, such as heat propagation, lattice melting, and ablation, are the result of energy deposition in metals. A fundamental understanding of the electron dynamics leading to these thermal phenomena would benefit many laser applications, such as laser deposition of thin films and laser processing. In this work, thin metal films were prepared using the resistive heating evaporation technique. High dynamic range autocorrelators were constructed to characterize the different laser systems used in this study. The nonequilibrium electron dynamics in single layer gold films, multi-layer gold-vanadium, and gold-titanium films were studied. The time evolution of the electron temperature was monitored using femtosecond time-resolved thermoreflectivity (DeltaR/R) measurements. The validity of the Two-Temperature Model (TTM) in describing ultrafast laser heating processes was checked. The effect of the padding layer on the surface damage threshold was investigated. The experimental results revealed a reduction of the thermoreflectivity signal, DeltaRmax, for the multi-layer film that signifies a reduction in the surface electron temperature. Multi-shot damage experiments, in contrast to the thermoreflectivity measurements and the results of Qiu et al., showed no evidence of surface damage in the case of the gold sample, whereas the multi-layer sample experienced an onset of surface damage at the same experimental conditions. The suitability of the Two-Temperature Model (TTM) in describing the transport and relaxation dynamics of hot electrons accurately was verified. A new methodology for the correction of the TTM to account for the internal thermalization of the electron gas and convolution effects was achieved.
Femtosecond electron diffraction: heralding the era of atomically resolved dynamics
NASA Astrophysics Data System (ADS)
Sciaini, Germán; Miller, R. J. Dwayne
2011-09-01
One of the great dream experiments in Science is to directly observe atomic motions as they occur. Femtosecond electron diffraction provided the first 'light' of sufficient intensity to achieve this goal by attaining atomic resolution to structural changes on the relevant timescales. This review covers the technical progress that made this new level of acuity possible and gives a survey of the new insights gained from an atomic level perspective of structural dynamics. Atomic level views of the simplest possible structural transition, melting, are discussed for a number of systems in which both thermal and purely electronically driven atomic displacements can be correlated with the degree of directional bonding. Optical manipulation of charge distributions and effects on interatomic forces/bonding can be directly observed through the ensuing atomic motions. New phenomena involving strongly correlated electron-lattice systems are also discussed in which optically induced changes in the potential energy landscape lead to ballistic structural changes. Concepts such as the structural order parameters are now directly observable at the atomic level of inspection to give a remarkable view of the extraordinary degree of cooperativity involved in strongly correlated electron-lattice systems. These recent examples, in combination with time-resolved real space imaging now possible with electron probes, are truly defining an emerging field that holds great promise to make a significant impact in how we understand structural dynamics. This article is dedicated to the memory of Professor David John Hugh Cockayne, a world leader in electron microscopy, who sadly passed away in December.
Electronic currents and Born-Oppenheimer molecular dynamics
NASA Astrophysics Data System (ADS)
Patchkovskii, Serguei
2012-08-01
Born-Oppenheimer variable separation is the mainstay of studies of chemical reactivity and dynamics. A long-standing problem of this ansatz is the absence of electronic currents in a system undergoing dynamics. I analyze the physical origin of the "missing" electronic currents in Born-Oppenheimer wavefunctions. By examining the problem within the multi-state Born-Huang ansatz, I demonstrate that electronic currents arise from the first-order non-adiabatic coupling to electronically excited states. I derive two expressions for the electronic currents induced by nuclear motion. The sum-over-the-states formula, identical to the result of "complete adiabatic" treatment of Nafie [J. Chem. Phys. 79, 4950 (1983)], 10.1063/1.445588 leads to a transparent and intuitive physical picture of the induced currents, but is unsuitable for practical implementation in all but the simplest systems. The equivalent expression in terms of the electronic energy derivatives is straightforward to implement numerically. I present first applications of this approach to small systems of potential chemical interest.
Correlated electron-nuclear dissociation dynamics: classical versus quantum motion
NASA Astrophysics Data System (ADS)
Schaupp, Thomas; Albert, Julian; Engel, Volker
2017-01-01
We investigate the coupled electron-nuclear dynamics in a model system which undergoes dissociation. In choosing different initial conditions, the cases of adiabatic and non-adiabatic dissociation are realized. We treat the coupled electronic and nuclear motion in the complete configuration space so that classically, no surface hopping procedures have to be incorporated in the case that more than a single adiabatic electronic state is populated during the fragmentation. Due to the anharmonic interaction potential, it is expected that classical mechanics substantially deviate from quantum mechanics. However, we provide examples where the densities and fragmentation yields obtained from the two treatments are in astonishingly strong agreement in the case that one starts in the electronic ground state initially. As expected, larger deviations are found if one starts in electronically excited states where trajectories are sampled from the more spatially extended electronic wave function. In that case, higher initial energies are accessed, and the motion proceeds in regions with increasing degree of anharmonicity. Contribution to the Topical Issue "Dynamics of Molecular Systems (MOLEC 2016)", edited by Alberto Garcia-Vela, Luis Banares and Maria Luisa Senent.
NASA Astrophysics Data System (ADS)
Ma, Qian; Dai, Jiayu; Zhao, Zengxiu
2016-10-01
The electron-ion temperature relaxation is an important non-equilibrium process in the generation of dense plasmas, particularly in Inertial Confinement Fusion. Classical molecular dynamics considers electrons as point charges, ignoring important quantum processes. We use an Electron Force Field (EFF) method to study the temperature relaxation processes, considering the nuclei as semi-classical point charges and assume electrons as Gaussian wave packets which includes the influences of the size and the radial motion of electrons. At the same time, a Pauli potential is used to describe the electronic exchange effect. At this stage, quantum effects such as exchange, tunneling can be included in this model. We compare the results from EFF and classical molecular dynamics, and find that the relaxation time is much longer with including quantum effects, which can be explained directly by the deference of collision cross sections between quantum particles and classical particles. Further, the final thermal temperature of electron and ion is different compared with classical results that the electron quantum effects cannot be neglected.
Electron dynamics in the minimagnetosphere above a lunar magnetic anomaly
NASA Astrophysics Data System (ADS)
Usui, Hideyuki; Miyake, Yohei; Nishino, Masaki N.; Matsubara, Takuma; Wang, Joseph
2017-02-01
We consider a three-dimensional electromagnetic particle-in-cell simulation of the boundary layer current in a minimagnetosphere created by the interaction between a magnetized plasma flow, which models the typical solar wind, and a small-scale magnetic dipole, which represents the Reiner Gamma magnetic anomaly on the lunar surface. The size of this magnetic anomaly (measured as the distance from the dipole center to the position where the pressure of the local magnetic field equals the dynamic pressure of the solar wind) is one quarter that of the Larmor radius of the solar wind ions. In spite of the weak magnetization of the ions, a minimagnetosphere is formed above the magnetic anomaly. In the boundary layer of the minimagnetosphere, the electron current is dominant. Due to the intense electric field induced by charge separation, electrons entering the boundary layer undergo E × B drift. In each hemisphere, the electron boundary current due to the drift shows a structure where the convection reverses; these structures are symmetric with respect to the magnetic equator. Detailed analysis of the electron cyclotron motion shows that electrons at the edge of the inner boundary layer obtain maximum velocity by the electric field acceleration due to the charge separation, not due to the drift of the electron's guiding center. The maximum electron velocity is approximately 8 times that of the upstream plasma. The width of the boundary layer current becomes approximately equal to the radius of the local electron cyclotron.
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.
Test ion acceleration in a dynamic planar electron sheath
NASA Astrophysics Data System (ADS)
Basko, M. M.
2007-03-01
New exact results are obtained for relativistic acceleration of test positive ions in the laminar zone of a planar electron sheath evolving from an initially mono-energetic electron distribution. The electron dynamics is calculated against the background of motionless foil ions. The limiting gamma-factor γp∞ of accelerated ions is shown to be determined primarily by the values of the ion-electron charge-over-mass ratio μ=meZp/mp and the initial gamma-factor γ0 of the accelerated electrons. For μ> 1/8 a test ion always overtakes the electron front and attains γp∞> γ0. For μ< 1/8 a test ion can catch up with the electron front only when γ0 is above a certain critical value γcr, which for μ≪1 can most often be evaluated as γ_{cr} = ({1}/{4}) μexpleft(μ^{-1}-1right). In this model the protons and heavier test ions, for which γcr> 10398 is enormous, always lag behind the front edge of the electron sheath and have γp∞< γ0; for their maximum energy an appropriate intermediate asymptotic formula is derived. The domain of applicability of the laminar-zone results is analyzed in detail.
Shaheen, Basamat S; Sun, Jingya; Yang, Ding-Shyue; Mohammed, Omar F
2017-06-01
Understanding light-triggered charge carrier dynamics near photovoltaic-material surfaces and at interfaces has been a key element and one of the major challenges for the development of real-world energy devices. Visualization of such dynamics information can be obtained using the one-of-a-kind methodology of scanning ultrafast electron microscopy (S-UEM). Here, we address the fundamental issue of how the thickness of the absorber layer may significantly affect the charge carrier dynamics on material surfaces. Time-resolved snapshots indicate that the dynamics of charge carriers generated by electron impact in the electron-photon dynamical probing regime is highly sensitive to the thickness of the absorber layer, as demonstrated using CdSe films of different thicknesses as a model system. This finding not only provides the foundation for potential applications of S-UEM to a wide range of devices in the fields of chemical and materials research, but also has impact on the use and interpretation of electron beam-induced current for optimization of photoactive materials in these devices.
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.
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 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.; ...
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
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 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.
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.
Singularities and internal rotational dynamics of electron beams
NASA Astrophysics Data System (ADS)
Velasco-Martínez, D.; Ibarra-Sierra, V. G.; Sandoval-Santana, J. C.; Cardoso, J. L.; Kunold, A.
2016-12-01
We study the internal rotational dynamics of electronic beams in relation to the phase singularities of their wave functions. Given their complex singularity structure, Hermite-Gaussian beams and other superpositions of Laguerre-Gaussian modes are studied here. We show that by inspecting the lowest nonvanishing terms of the wave function near the singularity, it is possible to infer the structure of the Bohmian streamlines. Conversely, starting from a map of the electron's Bohmian velocities, we demonstrate that it is possible to derive the form of the electron's wave function near the singularity. We outline a procedure that could yield an experimental method to determine the main parameters of the electron's wave function close to a singularity.
Molecular dynamics simulations of electron irradiated PVDF nanofibers
NASA Astrophysics Data System (ADS)
Miao, Jiayuan; Bhatta, Ram; Kisielowski, Christian; Lolla, Dinesh; Reneker, Darrell; Tsige, Mesfin; Taylor, Philip
2014-03-01
High-resolution, aberration corrected transmission electron microscopy was used to observe morphological changes and segmental motion of electrospun poly(vinylidene fluoride) nanofibers in an 80 kilovolt electron beam. Atomic and molecular scale high-resolution images of fibers were made with an aberration corrected electron microscope. Chemical and morphological changes, which include the breaking of the fiber, loss of fluorine atoms and cross-linking of chains, caused by the high-energy electron beam were observed. We present the results of molecular dynamics (MD) simulations of such atomic and molecular level observations. The calculational models include the influence of chain scission, chain recoiling, and torsional defects on the morphology of a nanofiber. The effects of the loss of fluorine atoms and the applied tension on the morphology of the fibers were also investigated. Work supported by the Petroleum Research Fund of the American Chemical Society.
Extraction dynamics of electrons from magneto-optically trapped atoms
NASA Astrophysics Data System (ADS)
Fedchenko, Olena; Chernov, Sergii; McCulloch, Andrew; Vielle-Grosjean, Mélissa; Comparat, Daniel; Schönhense, Gerd
2017-07-01
Pulsed photoionization of laser-cooled atoms in a magneto-optical trap (MOT) has the potential to create cold electron beams of few meV bandwidths and few ps pulse lengths. Such a source would be highly attractive for the study of fast low-energy processes like coherent phonon excitation. To study the suitability of MOT-based sources for the production of simultaneously cold and fast electrons, we study the photoionization dynamics of trapped Cs atoms. A momentum-microscope-like setup with a delay-line detector allows for the simultaneous measurement of spatial and temporal electron distributions. The measured patterns are complex, due to the Lorentz force inducing spiral trajectories. Ray-tracing simulations reproduce the main features. We find that the production of electron bunches with bandwidths of a few meV is straightforward; however, pulses in the ps-range are more demanding and require beam blanking or partial blocking.
Dissipation and energy balance in electronic dynamics of Na clusters
NASA Astrophysics Data System (ADS)
Vincendon, Marc; Suraud, Eric; Reinhard, Paul-Gerhard
2017-06-01
We investigate the impact of dissipation on the energy balance in the electron dynamics of metal clusters excited by strong electro-magnetic pulses. The dynamics is described theoretically by Time-Dependent Density-Functional Theory (TDDFT) at the level of Local Density Approximation (LDA) augmented by a self interaction correction term and a quantum collision term in Relaxation-Time Approximation (RTA). We evaluate the separate contributions to the total excitation energy, namely energy exported by electron emission, potential energy due to changing charge state, intrinsic kinetic and potential energy, and collective flow energy. The balance of these energies is studied as function of the laser parameters (frequency, intensity, pulse length) and as function of system size and charge. We also look at collisions with a highly charged ion and here at the dependence on the impact parameter (close versus distant collisions). Dissipation turns out to be small where direct electron emission prevails namely for laser frequencies above any ionization threshold and for slow electron extraction in distant collisions. Dissipation is large for fast collisions and at low laser frequencies, particularly at resonances. Contribution to the Topical Issue "Dynamics of Systems at the Nanoscale", edited by Andrey Solov'yov and Andrei Korol.
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
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
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.
Perpendicular dynamics of runaway electrons in tokamak plasmas
Fernandez-Gomez, I.; Martin-Solis, J. R.; Sanchez, R.
2012-10-15
In this paper, it will be shown that the runaway phenomenon in tokamak plasmas cannot be reduced to a one-dimensional problem, based on the competence between electric field acceleration and collisional friction losses in the parallel direction. A Langevin approach, including collisional diffusion in velocity space, will be used to analyze the two-dimensional runaway electron dynamics. An investigation of the runaway probability in velocity space will yield a criterion for runaway, which will be shown to be consistent with the results provided by the more simple test particle description of the runaway dynamics [Fuchs et al., Phys. Fluids 29, 2931 (1986)]. Electron perpendicular collisional scattering will be found to play an important role, relaxing the conditions for runaway. Moreover, electron pitch angle scattering perpendicularly broadens the runaway distribution function, increasing the electron population in the runaway plateau region in comparison with what it should be expected from electron acceleration in the parallel direction only. The perpendicular broadening of the runaway distribution function, its dependence on the plasma parameters, and the resulting enhancement of the runaway production rate will be discussed.
Explicit inclusion of electronic correlation effects in molecular dynamics
NASA Astrophysics Data System (ADS)
Julien, Jean-Pierre; Kress, Joel D.; Zhu, Jian-Xin
2017-07-01
We design a quantum molecular dynamics method for strongly correlated electron metals. The strong electronic correlation effects are treated within a real-space version of the Gutzwiller variational approximation (GA), which is suitable for the inhomogeneity inherent in the process of quantum molecular dynamics (MD) simulations. We also propose an efficient algorithm based on the second-moment approximation to the electronic density of states for the search of the optimal variation parameters, from which the renormalized interatomic MD potentials are fully determined. By considering a minimal one-correlated-orbital Anderson model with parameterized spatial dependence of tight-binding hopping integrals, this fast GA-MD method is benchmarked with that using exact diagonalization to solve the GA variational parameters. The efficiency and accuracy are illustrated. We have demonstrated the effect of temperature coupled with electronic correlation on structural properties simulated with MD. This method will open up an unprecedented opportunity enabling large-scale quantum MD simulations of strongly correlated electronic materials.
Femtosecond Dynamics of Electrons in 2-D Dissipative Systems
NASA Astrophysics Data System (ADS)
Harris, Charles
2000-03-01
Transitions between weakly coupled initial and final states can be treated with a lowest order perturbation theory in the electronic coupling which yields the well-known golden rule in this non-adiabatic limit. In strongly interacting systems, one often resorts to semiclassical treatments, such as the Landau-Zener formula for the transition probability in the adiabatic limit. Recent electron transfer theory by Stuchebrukhov and Song treats the two limit on equal footing by summing over all perturbation orders in electronic coupling[1]. Here we present the application of this theory to model the dynamics of electron self-trapping in 2-D at the n-heptane/Ag(111) and anthracene/Ag(111) interface. Our results revealed an intermediate electronic coupling for the self-trapping process at the n-heptane/Ag(111) interface which can mainly be described by a non-adiabatic process. Results for electron self-trapping at the anthracene/Ag(111) interface revealed a stronger electronic coupling which requires the summing of higher perturbation orders. [1] A.A. Stuchebrukhov and X. song, J. Chem. Phys. 101, 9354, 1994. [2] N.-H. Ge,C.M. Wong, R.L. Lingle, Jr., J.D. McNeill, K.J. Gaffney, and C.B. Harris, Science 279, 202, 1998.
Quantum electron-vibrational dynamics at finite temperature: Thermo field dynamics approach.
Borrelli, Raffaele; Gelin, Maxim F
2016-12-14
Quantum electron-vibrational dynamics in molecular systems at finite temperature is described using an approach based on the thermo field dynamics theory. This formulation treats temperature effects in the Hilbert space without introducing the Liouville space. A comparison with the theoretically equivalent density matrix formulation shows the key numerical advantages of the present approach. The solution of thermo field dynamics equations with a novel technique for the propagation of tensor trains (matrix product states) is discussed. Numerical applications to model spin-boson systems show that the present approach is a promising tool for the description of quantum dynamics of complex molecular systems at finite temperature.
Spectral signals from electronic dynamics in sodium clusters
Calvayrac, F.; Reinhard, P.G.; Suraud, E.
1997-03-01
We study the dynamics of the electron cloud in sodium clusters for small and large amplitude excitations in the time-dependent local-density approximation (TDLDA), without referring to linear approximations. In particular, we discuss the interpretation of strength function and power spectrum as obtained from dynamical calculations. We demonstrate the constructive and destructive interference contained in the various spectral states. We search for a special signature of nonlinear couplings in the large amplitude regime, but do not find pronounced effects. {copyright} 1997 Academic Press, Inc.
Dynamical nonlocal coherent-potential approximation for itinerant electron magnetism.
Rowlands, D A; Zhang, Yu-Zhong
2014-11-26
A dynamical generalisation of the nonlocal coherent-potential approximation is derived based upon the functional integral approach to the interacting electron problem. The free energy is proven to be variational with respect to the self-energy provided a self-consistency condition on a cluster of sites is satisfied. In the present work, calculations are performed within the static approximation and the effect of the nonlocal physics on the formation of the local moment state in a simple model is investigated. The results reveal the importance of the dynamical correlations.
Dynamics of Low Energy Electron Attachment to Formic Acid
Rescigno, Thomas N.; Trevisan, Cynthia S.; Orel, Ann E.
2006-04-03
Low-energy electrons (<2 eV) can fragment gas phaseformic acid (HCOOH) molecules through resonant dissociative attachmentprocesses. Recent experiments have shown that the principal reactionproducts of such collisions are formate ions (HCOO-) and hydrogen atoms.Using first-principles electron scattering calculations, we haveidentified the responsible negative ion state as a transient \\pi* anion.Symmetry considerations dictate that the associated dissociation dynamicsare intrinsically polyatomic: a second anion surface, connected to thefirst by a conical intersection, is involved in the dynamics and thetransient anion must necessarily deform to non-planar geometries beforeit can dissociate to the observed stable products.
NASA Astrophysics Data System (ADS)
Ivanov, Dmitriy S.; Zhigilei, Leonid V.; Bringa, Eduardo M.; De Koning, Maurice; Remington, Bruce A.; Caturla, Maria Jose; Pollaine, Stephen M.
2004-07-01
Shocks are often simulated using the classical molecular dynamics (MD) method in which the electrons are not included explicitly and the interatomic interaction is described by an effective potential. As a result, the fast electronic heat conduction in metals and the coupling between the lattice vibrations and the electronic degrees of freedom can not be represented. Under conditions of steep temperature gradients that can form near the shock front, however, the electronic heat conduction can play an important part in redistribution of the thermal energy in the shocked target. We present the first atomistic simulation of a shock propagation including the electronic heat conduction and electron-phonon coupling. The computational model is based on the two-temperature model (TTM) that describes the time evolution of the lattice and electron temperatures by two coupled non-linear differential equations. In the combined TTM-MD method, MD substitutes the TTM equation for the lattice temperature. Simulations are performed with both MD and TTM-MD models for an EAM Al target shocked at 300 kbar. The target includes a tilt grain boundary, which provides a region where shock heating is more pronounced and, therefore, the effect of the electronic heat conduction is expected to be more important. We find that the differences between the predictions of the MD and TTM-MD simulations are significantly smaller as compared to the hydrodynamics calculations performed at similar conditions with and without electronic heat conduction.
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.
Evolving complex dynamics in electronic models of genetic networks
NASA Astrophysics Data System (ADS)
Mason, Jonathan; Linsay, Paul S.; Collins, J. J.; Glass, Leon
2004-09-01
Ordinary differential equations are often used to model the dynamics and interactions in genetic networks. In one particularly simple class of models, the model genes control the production rates of products of other genes by a logical function, resulting in piecewise linear differential equations. In this article, we construct and analyze an electronic circuit that models this class of piecewise linear equations. This circuit combines CMOS logic and RC circuits to model the logical control of the increase and decay of protein concentrations in genetic networks. We use these electronic networks to study the evolution of limit cycle dynamics. By mutating the truth tables giving the logical functions for these networks, we evolve the networks to obtain limit cycle oscillations of desired period. We also investigate the fitness landscapes of our networks to determine the optimal mutation rate for evolution.
Exciton Relaxation and Electron Transfer Dynamics of Semiconductor Quantum Dots
NASA Astrophysics Data System (ADS)
Liu, Cunming
Quantum dots (QDs), also referred to as colloidal semiconductor nanocrystals, exhibit unique electronic and optical properties arising from their three-dimensional confinement and strongly enhanced coulomb interactions. Developing a detailed understanding of the exciton relaxation dynamics within QDs is important not only for sake of exploring the fundamental physics of quantum confinement processes, but also for their applications. Ultrafast transient absorption (TA) spectroscopy, as a powerful tool to explore the relaxation dynamics of excitons, was employed to characterize the hot single/multiexciton relaxation dynamics at the first four exciton states of CdSe/CdZnS QDs. We observed for the first time that the hot hole can relax through two possible pathways: Intraband multiple phonon coupling and intrinsic defect trapping, with a lifetime of ˜7 ps. Additionally, an ultra-short component of ˜ 8 ps, directly associated with the Auger recombination of highly energetic exciton states, was discovered. After exploring the exciton relaxation inside QDs, ultrafast TA spectroscopy was further applied to study the electron transferring outside from QDs. By using a brand-new photocatalytic system consisting of CdSe QDs and Ni-dihydrolipoic acid (Ni-DHLA) catalyst, which has represented a robust photocatalysis of H2 from water, the photoinduced electron transfer (ET) dynamics between QD and the catalyst, one of most important steps during H2 generation, was studied. We found smaller bare CdSe QDs exhibit a better ET performance and CdS shelling on the bare QDs leads to worsen the ET. The calculations of effective mass approximation (EMA) and Marcus theory show the ET process is mainly dominated by driving force, electronic coupling strength and reorganization energy between QD and the catalyst.
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.
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.
Surface and bulk hot electron dynamics in silicon
NASA Astrophysics Data System (ADS)
Jeong, Seongtae; Bokor, Jeffrey
1997-03-01
The direct time domain study of hot electron dynamics on the silicon surface has been an active area of research. Dynamics in Si(100) surface states was observed(M.W. Rowe, H. Liu, G. P. Williams, Jr., and R. T. Williams, Phys. Rev. B 47, 2048 (1993)) as well as cooling of a hot but thermal distribution of carriers in bulk silicon(J. R. Goldman, and J. A. Prybyla, Phys. Rev. Lett. 72, 1364 (1994)). In this work, a time-resolved photoemission study on the Si(100)2x1 surface with 1.55 eV pump and 4.66 eV probe with 0.2 psec time resolution is reported. It is observed that two-photon absorption is responsible for high kinetic energy electrons above the conduction band minimum (CBM) but direct single-photon excitation into surface states and conduction band states followed by the surface recombination dominates the dynamics. Also observed are an early nonthermal electronic distribution in silicon and its transition into a thermal one followed by a rapid cooling.
Dynamics of Quantal Heating in Electron Systems with Discrete Spectra
NASA Astrophysics Data System (ADS)
Mayer, William; Dietrich, Scott; Vitkalov, Sergey; Bykov, Alexey
2015-03-01
The temporal evolution of quantal Joule heating of 2D electrons in GaAs quantum well placed in quantizing magnetic fields is studied using a difference frequency method. The method is based on measurements of the electron conductivity oscillating at the beat frequency f =f1 -f2 between two microwaves applied to 2D system at frequencies f1 and f2. The method provides direct access to the dynamical characteristics of the heating and yields the inelastic scattering time τin of 2D electrons. The obtained τin is strongly temperature dependent, varying from 0.13 ns at 5.5K to 1 ns at 2.4K in magnetic field B=0.333T. When temperature T exceeds the Landau level separation the relaxation rate 1 /τin is proportional to T2, indicating the electron-electron interaction as the dominant mechanism limiting the quantal heating. At lower temperatures the rate tends to be proportional to T3, indicating considerable contribution from electron-phonon scattering. This work was supported by the National Science Foundation (DMR 1104503), the Russian Foundation for Basic Research (project no.14-02-01158) and the Ministry of Education and Science of the Russian Federation.
Martin, Aiden A.; Bahm, Alan; Bishop, James; ...
2015-12-15
Here, we report highly ordered topographic patterns that form on the surface of diamond, span multiple length scales, and have a symmetry controlled by the precursor gas species used in electron-beam-induced etching (EBIE). The pattern formation dynamics reveals an etch rate anisotropy and an electron energy transfer pathway that is overlooked by existing EBIE models. Therefore, we, modify established theory such that it explains our results and remains universally applicable to EBIE. Furthermore, the patterns can be exploited in controlled wetting, optical structuring, and other emerging applications that require nano- and microscale surface texturing of a wide band-gap material.
Optical properties and electron dynamics in carbon nanodots
NASA Astrophysics Data System (ADS)
Wen, Xiaoming; Huang, Shujuan; Conibeer, Gavin; Shrestha, Santosh; Yu, Pyng; Toh, Yon-Rui; Tang, Jau
2013-12-01
Carbon nanodots (CNDs) have emerged as fascinating materials with exceptional electronic and optical properties, and thus they offer promising applications in photonics, photovoltaics and photocatalysis. Herein we study the optical properties and electron dynamics in CNDs using steady state and time-resolved spectroscopy. The photoluminescence (PL) is determined to originate from both core and surface. The massive surface fluorophores result in a broad spectral fluorescence. In addition to various synthesis techniques, it is demonstrated that the PL of CNDs can be extended from the blue to the near infrared by thermal assisted growth. Directional electron transfer was observed as fast as femtosecond in CND-graphene oxide nanocomposites from CND into graphene oxide. These results suggest CNDs can be promising in many applications.
Probing Electron Dynamics in Simple Molecules with Attosecond Pulses
NASA Astrophysics Data System (ADS)
Rivière, Paula; Palacios, Alicia; Pérez-Torres, Jhon Fredy; Martín, Fernando
Attosecond pulses are an ideal tool to explore electron and nuclear dynamics in atoms and molecules. Either as single attosecond pulses (SAP), in attosecond pulse trains (APT), or in combination with infrared (IR) pulses, these pulses, with frequencies in the VUV-XUV regime, have been widely used to probe ionization, electron tunneling, or autoionization in atoms. More recently, similar processes have been studied in molecules. A correct theoretical description of such processes in molecules often requires a fully dimensional treatment due to the important role of nuclear motion and electron correlation. This restricts ab initio calculations to the simplest molecules. In this chapter, we discuss single ionization of hydrogen molecules (H2 and D2) induced by time-delayed SAP+IR and APT+IR schemes. Ab initio time-dependent theoretical calculations are compared with existing experiments.
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 Azobenzene Dimer Photoisomerization: Electronic and Steric Effects.
Titov, Evgenii; Granucci, Giovanni; Götze, Jan Philipp; Persico, Maurizio; Saalfrank, Peter
2016-09-15
While azobenzenes readily photoswitch in solution, their photoisomerization in densely packed self-assembled monolayers (SAMs) can be suppressed. Reasons for this can be steric hindrance and/or electronic quenching, e.g., by exciton coupling. We address these possibilities by means of nonadiabatic molecular dynamics with trajectory surface hopping calculations, investigating the trans → cis isomerization of azobenzene after excitation into the ππ* absorption band. We consider a free monomer, an isolated dimer and a dimer embedded in a SAM-like environment of additional azobenzene molecules, imitating in this way the gradual transition from an unconstrained over an electronically coupled to an electronically coupled and sterically hindered, molecular switch. Our simulations reveal that in comparison to the single molecule the quantum yield of the trans → cis photoisomerization is similar for the isolated dimer, but greatly reduced in the sterically constrained situation. Other implications of dimerization and steric constraints are also discussed.
Electronic Excitation Dynamics in Liquid Water under Proton Irradiation
Reeves, Kyle G.; Kanai, Yosuke
2017-01-01
Molecular behaviour of liquid water under proton irradiation is of great importance to a number of technological and medical applications. The highly energetic proton generates a time-varying field that is highly localized and heterogeneous at the molecular scale, and massive electronic excitations are produced as a result of the field-matter interaction. Using first-principles quantum dynamics simulations, we reveal details of how electrons are dynamically excited through non-equilibrium energy transfer from highly energetic protons in liquid water on the atto/femto-second time scale. Water molecules along the path of the energetic proton undergo ionization at individual molecular level, and the excitation primarily derives from lone pair electrons on the oxygen atom of water molecules. A reduced charge state on the energetic proton in the condensed phase of water results in the strongly suppressed electronic response when compared to water molecules in the gas phase. These molecular-level findings provide important insights into understanding the water radiolysis process under proton irradiation. PMID:28084420
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
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.
Delocalization of Electrons in Strong Insulators at High Dynamic Pressures
Nellis, William J.
2011-01-01
Systematics of material responses to shock flows at high dynamic pressures are discussed. Dissipation in shock flows drives structural and electronic transitions or crossovers, such as used to synthesize metallic liquid hydrogen and most probably Al2O3 metallic glass. The term “metal” here means electrical conduction in a degenerate system, which occurs by band overlap in degenerate condensed matter, rather than by thermal ionization in a non-degenerate plasma. Since H2 and probably disordered Al2O3 become poor metals with minimum metallic conductivity (MMC) virtually all insulators with intermediate strengths do so as well under dynamic compression. That is, the magnitude of strength determines the split between thermal energy and disorder, which determines material response. These crossovers occur via a transition from insulators with electrons localized in chemical bonds to poor metals with electron energy bands. For example, radial extents of outermost electrons of Al and O atoms are 7 a0 and 4 a0, respectively, much greater than 1.7 a0 needed for onset of hybridization at 300 GPa. All such insulators are Mott insulators, provided the term “correlated electrons” includes chemical bonds.
Electronic Excitation Dynamics in Liquid Water under Proton Irradiation
NASA Astrophysics Data System (ADS)
Reeves, Kyle G.; Kanai, Yosuke
2017-01-01
Molecular behaviour of liquid water under proton irradiation is of great importance to a number of technological and medical applications. The highly energetic proton generates a time-varying field that is highly localized and heterogeneous at the molecular scale, and massive electronic excitations are produced as a result of the field-matter interaction. Using first-principles quantum dynamics simulations, we reveal details of how electrons are dynamically excited through non-equilibrium energy transfer from highly energetic protons in liquid water on the atto/femto-second time scale. Water molecules along the path of the energetic proton undergo ionization at individual molecular level, and the excitation primarily derives from lone pair electrons on the oxygen atom of water molecules. A reduced charge state on the energetic proton in the condensed phase of water results in the strongly suppressed electronic response when compared to water molecules in the gas phase. These molecular-level findings provide important insights into understanding the water radiolysis process under proton irradiation.
Electron-electron collision dynamics of the four-electron escape in Be close to threshold
NASA Astrophysics Data System (ADS)
Emmanouilidou, A.; Price, H.
2013-04-01
We explore the escape geometry of four electrons a few eV above threshold following single-photon absorption from the ground state of Be. We find that the four electrons leave the atom on the vertices of a triangular pyramid instead of a previously predicted regular tetrahedron. To illustrate the physical mechanisms of quadruple ionization we use a momentum transferring attosecond collision scheme which we show to be in accord with the triangular pyramid breakup pattern.
Electron beam dynamics in an ultrafast transmission electron microscope with Wehnelt electrode.
Bücker, K; Picher, M; Crégut, O; LaGrange, T; Reed, B W; Park, S T; Masiel, D J; Banhart, F
2016-12-01
High temporal resolution transmission electron microscopy techniques have shown significant progress in recent years. Using photoelectron pulses induced by ultrashort laser pulses on the cathode, these methods can probe ultrafast materials processes and have revealed numerous dynamic phenomena at the nanoscale. Most recently, the technique has been implemented in standard thermionic electron microscopes that provide a flexible platform for studying material's dynamics over a wide range of spatial and temporal scales. In this study, the electron pulses in such an ultrafast transmission electron microscope are characterized in detail. The microscope is based on a thermionic gun with a Wehnelt electrode and is operated in a stroboscopic photoelectron mode. It is shown that the Wehnelt bias has a decisive influence on the temporal and energy spread of the picosecond electron pulses. Depending on the shape of the cathode and the cathode-Wehnelt distance, different emission patterns with different pulse parameters are obtained. The energy spread of the pulses is determined by space charge and Boersch effects, given by the number of electrons in a pulse. However, filtering effects due to the chromatic aberrations of the Wehnelt electrode allow the extraction of pulses with narrow energy spreads. The temporal spread is governed by electron trajectories of different length and in different electrostatic potentials. High temporal resolution is obtained by excluding shank emission from the cathode and aberration-induced halos in the emission pattern. By varying the cathode-Wehnelt gap, the Wehnelt bias, and the number of photoelectrons in a pulse, tradeoffs between energy and temporal resolution as well as beam intensity can be made as needed for experiments. Based on the characterization of the electron pulses, the optimal conditions for the operation of ultrafast TEMs with thermionic gun assembly are elaborated. Copyright © 2016 Elsevier B.V. All rights reserved.
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.
Dynamic phase shifts in nanoscale distance measurements by double electron electron resonance (DEER)
NASA Astrophysics Data System (ADS)
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.
NASA Astrophysics Data System (ADS)
Parkhill, John A.; Markovich, Thomas; Tempel, David G.; Aspuru-Guzik, Alan
2012-12-01
In this work, we develop an approach to treat correlated many-electron dynamics, dressed by the presence of a finite-temperature harmonic bath. Our theory combines a small polaron transformation with the second-order time-convolutionless master equation and includes both electronic and system-bath correlations on equal footing. Our theory is based on the ab initio Hamiltonian, and is thus well-defined apart from any phenomenological choice of basis states or electronic system-bath coupling model. The equation-of-motion for the density matrix we derive includes non-Markovian and non-perturbative bath effects and can be used to simulate environmentally broadened electronic spectra and dissipative dynamics, which are subjects of recent interest. The theory also goes beyond the adiabatic Born-Oppenheimer approximation, but with computational cost scaling such as the Born-Oppenheimer approach. Example propagations with a developmental code are performed, demonstrating the treatment of electron-correlation in absorption spectra, vibronic structure, and decay in an open system. An untransformed version of the theory is also presented to treat more general baths and larger systems.
Parkhill, John A; Markovich, Thomas; Tempel, David G; Aspuru-Guzik, Alan
2012-12-14
In this work, we develop an approach to treat correlated many-electron dynamics, dressed by the presence of a finite-temperature harmonic bath. Our theory combines a small polaron transformation with the second-order time-convolutionless master equation and includes both electronic and system-bath correlations on equal footing. Our theory is based on the ab initio Hamiltonian, and is thus well-defined apart from any phenomenological choice of basis states or electronic system-bath coupling model. The equation-of-motion for the density matrix we derive includes non-markovian and non-perturbative bath effects and can be used to simulate environmentally broadened electronic spectra and dissipative dynamics, which are subjects of recent interest. The theory also goes beyond the adiabatic Born-Oppenheimer approximation, but with computational cost scaling such as the Born-Oppenheimer approach. Example propagations with a developmental code are performed, demonstrating the treatment of electron-correlation in absorption spectra, vibronic structure, and decay in an open system. An untransformed version of the theory is also presented to treat more general baths and larger systems.
Plasmon Response and Electron Dynamics in Charged Metallic Nanoparticles.
Zapata Herrera, Mario; Aizpurua, Javier; Kazansky, Andrey K; Borisov, Andrei G
2016-03-22
Using the time-dependent density functional theory, we perform quantum calculations of the electron dynamics in small charged metallic nanoparticles (clusters) of spherical geometry. We show that the excess charge is accumulated at the surface of the nanoparticle within a narrow layer given by the typical screening distance of the electronic system. As a consequence, for nanoparticles in vacuum, the dipolar plasmon mode displays only a small frequency shift upon charging. We obtain a blue shift for positively charged clusters and a red shift for negatively charged clusters, consistent with the change of the electron spill-out from the nanoparticle boundaries. For negatively charged clusters, the Fermi level is eventually promoted above the vacuum level leading to the decay of the excess charge via resonant electron transfer into the continuum. We show that, depending on the charge, the process of electron loss can be very fast, on the femtosecond time scale. Our results are of great relevance to correctly interpret the optical response of the nanoparticles obtained in electrochemistry, and demonstrate that the measured shift of the plasmon resonances upon charging of nanoparticles cannot be explained without account for the surface chemistry and the dielectric environment.
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.
Role of Core Electrons in Quantum Dynamics Using TDDFT.
Foglia, Nicolás O; Morzan, Uriel N; Estrin, Dario A; Scherlis, Damian A; Gonzalez Lebrero, Mariano C
2017-01-10
The explicit simulation of time dependent electronic processes requires computationally onerous routes involving the temporal integration of motion equations for the charge density. Efficiency optimization of these methods typically relies on increasing the integration time-step and on the reduction of the computational cost per step. The implicit representation of inner electrons by effective core potentials-or pseudopotentials-is a standard practice in localized-basis quantum-chemistry implementations to improve the efficiency of ground-state calculations, still preserving the quality of the output. This article presents an investigation on the impact that effective core potentials have on the overall efficiency of real time electron dynamics with TDDFT. Interestingly, the speedups achieved with the use of pseudopotentials in this kind of simulation are on average much more significant than in ground-state calculations, reaching in some cases a factor as large as 600×. This boost in performance originates from two contributions: on the one hand, the size of the density matrix, which is considerably reduced, and, on the other, the elimination of high-frequency electronic modes, responsible for limiting the maximum time-step, which vanish when the core electrons are not propagated explicitly. The latter circumstance allows for significant increases in time-step, that in certain cases may reach up to 3 orders of magnitude, without losing any relevant chemical or spectroscopic information.
Collective Dynamics in Spin-Textured Electronic Systems
NASA Astrophysics Data System (ADS)
Wong, Clement H.
2010-06-01
In chapter I and II, we develop the hydrodynamic theory of collinear spin currents coupled to magnetization dynamics in metallic ferromagnets. The collective spin density couples to the spin current through a U(1) Berry-phase gauge field determined by the local texture and dynamics of the magnetization. We determine phenomenologically the dissipative corrections to the equation of motion for the electronic current, which consist of a dissipative spin-motive force generated by magnetization dynamics and a magnetic texture-dependent resistivity tensor. The reciprocal dissipative, adiabatic spin torque on the magnetic texture follows from the Onsager principle. By applying general thermodynamic relations, we determine a lower bound on the magnetic-texture resistivity. We investigate the effects of thermal fluctuations and find that electronic dynamics contribute to a nonlocal Gilbert damping tensor in the Landau-Lifshitz-Gilbert equation for the magnetization. In chapter III, we apply our general theory to soliton dynamics in spin-textured metals. We find it necessary to modify the Landau-Lifshitz-Gilbert equation and the corresponding solitonic equations of motion to include higher-order texture effects stemming hydrodynamic backaction. As an example, we consider the gyration of a vortex in a point-contact spin valve, and discuss modifications of orbit radius, frequency, and dissipation power. In chapter IV, we generalize our hydrodynamic theory to a kinetic equation, which we derive in a semiclassical expansion of the density-matrix equation of motion up to the first order in quantum mechanical corrections for a general two-band Hamiltonian. We find, in addition to corrections to the single-particle equation of motion due to Berry curvatures, a modification to the phase-space density of states, and interband terms associated with transport through a general curved phase space. We apply our kinetic equation to the case of inhomogeneities stemming from gauge
Dynamic electron arc radiotherapy (DEAR): a feasibility study.
Rodrigues, Anna; Yin, Fang-Fang; Wu, Qiuwen
2014-01-20
Compared to other radiation therapy modalities, clinical electron beam therapy has remained practically unchanged for the past few decades even though electron beams with multiple energies are widely available on most linacs. In this paper, we present the concept of dynamic electron arc radiotherapy (DEAR), a new conformal electron therapy technique with synchronized couch motion. DEAR utilizes combination of gantry rotation, couch motion, and dose rate modulation to achieve desirable dose distributions in patient. The electron applicator is kept to minimize scatter and maintain narrow penumbra. The couch motion is synchronized with the gantry rotation to avoid collision between patient and the electron cone. In this study, we investigate the feasibility of DEAR delivery and demonstrate the potential of DEAR to improve dose distributions on simple cylindrical phantoms. DEAR was delivered on Varian's TrueBeam linac in Research Mode. In conjunction with the recorded trajectory log files, mechanical motion accuracies and dose rate modulation precision were analyzed. Experimental and calculated dose distributions were investigated for different energies (6 and 9 MeV) and cut-out sizes (1×10 cm(2) and 3×10 cm(2) for a 15×15 cm(2) applicator). Our findings show that DEAR delivery is feasible and has the potential to deliver radiation dose with high accuracy (root mean square error, or RMSE of <0.1 MU, <0.1° gantry, and <0.1 cm couch positions) and good dose rate precision (1.6 MU min(-1)). Dose homogeneity within ±2% in large and curved targets can be achieved while maintaining penumbra comparable to a standard electron beam on a flat surface. Further, DEAR does not require fabrication of patient-specific shields. These benefits make DEAR a promising technique for conformal radiotherapy of superficial tumors.
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.
NASA Astrophysics Data System (ADS)
Hu, Lilei; Mandelis, Andreas; Melnikov, Alexander; Lan, Xinzheng; Hoogland, Sjoerd; Sargent, Edward H.
2017-01-01
Solution-processed colloidal quantum dots (CQDs) are promising materials for realizing low-cost, large-area, and flexible photovoltaic devices. The study of charge carrier transport in quantum dot solids is essential for understanding energy conversion mechanisms. Recently, solution-processed two-layer oleic-acid-capped PbS CQD solar cells with one layer treated with tetrabutylammonium iodide (TBAI) serving as the main light-absorbing layer and the other treated with 1,2-ethanedithiol (EDT) acting as an electron-blocking/hole-extraction layer were reported. These solar cells demonstrated a significant improvement in power conversion efficiency of 8.55% and long-term air stability. Coupled with photocarrier radiometry measurements, this work used a new trap-state mediated exciton hopping transport model, specifically for CQD thin films, to unveil and quantify exciton transport mechanisms through the extraction of hopping transport parameters including exciton lifetimes, hopping diffusivity, exciton detrapping time, and trap-state density. It is shown that PbS-TBAI has higher trap-state density than PbS-EDT that results in higher PbS-EDT exciton lifetimes. Hopping diffusivities of both CQD thin film types show similar temperature dependence, particularly higher temperatures yield higher hopping diffusivity. The higher diffusivity of PbS-TBAI compared with PbS-EDT indicates that PbS-TBAI is a much better photovoltaic material than PbS-EDT. Furthermore, PCR temperature spectra and deep-level photothermal spectroscopy provided additional insights to CQD surface trap states: PbS-TBAI thin films exhibit a single dominant trap level, while PbS-EDT films with lower trap-state densities show multiple trap levels.
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.
Complex formation dynamics in a single-molecule electronic device
Wen, Huimin; Li, Wengang; Chen, Jiewei; He, Gen; Li, Longhua; Olson, Mark A.; Sue, Andrew C.-H.; Stoddart, J. Fraser; Guo, Xuefeng
2016-01-01
Single-molecule electronic devices offer unique opportunities to investigate the properties of individual molecules that are not accessible in conventional ensemble experiments. However, these investigations remain challenging because they require (i) highly precise device fabrication to incorporate single molecules and (ii) sufficient time resolution to be able to make fast molecular dynamic measurements. We demonstrate a graphene-molecule single-molecule junction that is capable of probing the thermodynamic and kinetic parameters of a host-guest complex. By covalently integrating a conjugated molecular wire with a pendent crown ether into graphene point contacts, we can transduce the physical [2]pseudorotaxane (de)formation processes between the electron-rich crown ether and a dicationic guest into real-time electrical signals. The conductance of the single-molecule junction reveals two-level fluctuations that are highly dependent on temperature and solvent environments, affording a nondestructive means of quantitatively determining the binding and rate constants, as well as the activation energies, for host-guest complexes. The thermodynamic processes reveal the host-guest binding to be enthalpy-driven and are consistent with conventional 1H nuclear magnetic resonance titration experiments. This electronic device opens up a new route to developing single-molecule dynamics investigations with microsecond resolution for a broad range of chemical and biochemical applications. PMID:28138528
Muchová, Eva; Slavícek, Petr; Sobolewski, Andrzej L; Hobza, Pavel
2007-06-21
The goal of this study is to explore the photochemical processes following optical excitation of the glycine molecule into its two low-lying excited states. We employed electronic structure methods at various levels to map the PES of the ground state and the two low-lying excited states of glycine. It follows from our calculations that the photochemistry of glycine can be regarded as a combination of photochemical behavior of amines and carboxylic acid. The first channel (connected to the presence of amino group) results in ultrafast decay, while the channels characteristic for the carboxylic group occur on a longer time scale. Dynamical calculations provided the branching ratio for these channels. We also addressed the question whether conformationally dependent photochemistry can be observed for glycine. While electronic structure calculations favor this possibility, the ab initio multiple spawning (AIMS) calculations showed only minor relevance of the reaction path resulting in conformationally dependent dynamics.
NASA Astrophysics Data System (ADS)
Brand, Joachim; Cederbaum, Lorenz S.; Meyer, Hans-Dieter
1999-10-01
We derive a rigorous optical potential for electron-molecule scattering including the effects of nuclear dynamics by extending the common many-body Green's function approach to optical potentials beyond the fixed-nuclei limit for molecular targets. Our formalism treats the projectile electron and the nuclear motion of the target molecule on the same footing whereby the dynamical optical potential rigorously accounts for the complex many-body nature of the scattering target. One central result of the present work is that the common fixed-nuclei optical potential is a valid adiabatic approximation to the dynamical optical potential even when projectile and nuclear motion are (nonadiabatically) coupled as long as the scattering energy is well below the electronic excitation thresholds of the target. For extremely low projectile velocities, however, when the cross sections are most sensitive to the scattering potential, we expect the influences of the nuclear dynamics on the optical potential to become relevant. For these cases, a systematic way to improve the adiabatic approximation to the dynamical optical potential is presented that yields nonlocal operators with respect to the nuclear coordinates.
Electronic and structural dynamics of alkali-halide cluster anions
NASA Astrophysics Data System (ADS)
Dally, Andrew James
We have used photoelectron spectroscopy to study alkali-halide cluster anions that contain excess electrons. We have used ultrafast lasers to probe the dynamics of isomerization and photon stimulated desorption in these clusters. Our motivations are to gain information about these tiny systems in order to bring about a better understanding of similar processes in the bulk and to observe interesting phenomena that are found exclusively in clusters. We have observed in real-time the dynamics of isomerization occurring in Cs4I3- and (CsCl)7 - by depleting certain isomers from an ensemble that has established equilibrium populations for the isomers and watching as the ensemble reestablishes equilibrium. We have observed that the rates at which the re-equilibration occurs increase with the temperature of the nozzle in which the clusters are created. The lifetimes of the isomers all decrease with increasing temperature and are on the order of tens to hundreds of picoseconds. At the highest temperatures, the lifetimes are approaching the timescale for interconversion so that the clusters are effectively becoming molten. In effect, we have observed an approach to the analog of melting in the bulk, with a phase equilibrium between solid-like and liquid-like behavior across the temperature range studied. We have also observed photon stimulated desorption of an alkali anion from two-excess-electron clusters. By using an ultrashort laser pulse to excite one of the excess electrons and then using a second pulse to probe the resulting dynamics, we have observed the decay of this excited state and the subsequent desorption of an alkali anion. The timescale for producing alkali anions after the initial photon absorption is on the order of picoseconds. Increasing the temperature of these clusters increases the rate at which the desorption occurs. These studies should help to elucidate similar processes occurring in the bulk.
How Does the Electron Dynamics Affect the Global Reconnection Rate
NASA Technical Reports Server (NTRS)
Hesse, Michael
2012-01-01
The question of whether the microscale controls the macroscale or vice-versa remains one of the most challenging problems in plasmas. A particular topic of interest within this context is collisionless magnetic reconnection, where both points of views are espoused by different groups of researchers. This presentation will focus on this topic. We will begin by analyzing the properties of electron diffusion region dynamics both for guide field and anti-parallel reconnection, and how they can be scaled to different inflow conditions. As a next step, we will study typical temporal variations of the microscopic dynamics with the objective of understanding the potential for secular changes to the macroscopic system. The research will be based on a combination of analytical theory and numerical modeling.
Dynamics of adsorbate rotation in electron-induced reaction
NASA Astrophysics Data System (ADS)
Hu, Zhixin; Anggara, Kelvin; Polanyi, John C.
2017-09-01
Molecular rotors at surfaces are of current interest. Here we employ molecular dynamics to examine rotation in the chemisorbed product, meta-iodophenyl, from electron-induced reaction of meta-diiodobenzene at a noble metal (M(1 1 0)). Electron attachment gives iodophenyl that rotates unidirectionally ('clockwise') around a carbon-metal (C-M) 'pivot bond', due to I-M attractions. Mobility is enhanced by tilting the phenyl. During rotation the I-atom of iodophenyl bounces off successive M-atoms. As M changes from Cu to Ag to Au, the surface increasingly damps the bounce, diminishing rotation. Reconstruction of the gold can cause the atomic pivot-point to shift substantially, thereby giving opposite 'anticlockwise' rotation.
Analysis of electron dynamics in non-ideal Penning traps
Coppa, G.; Mulas, R.; D'Angola, A.
2012-06-15
Penning traps that are used for particular applications, such as in ion pump technology, Larmor, bouncing, and diocotron frequencies, can be of the same order of magnitude. The paper deals with the dynamics of electrons confined in such devices starting from the study of the properties of the trajectories. In cases of interest, in which electron-neutral collision frequency is much smaller with respect to the characteristic frequencies of the motion, suitable time averages of the trajectories are introduced in order to simplify the analysis of the problem. In the work, time averages have been calculated in a simple way by using an approximate r-z decoupling of the effective potential. Results obtained with the method are presented and discussed in both linear and nonlinear regimes.
TOPICAL REVIEW: Electron dynamics in inhomogeneous magnetic fields
NASA Astrophysics Data System (ADS)
Nogaret, Alain
2010-06-01
This review explores the dynamics of two-dimensional electrons in magnetic potentials that vary on scales smaller than the mean free path. The physics of microscopically inhomogeneous magnetic fields relates to important fundamental problems in the fractional quantum Hall effect, superconductivity, spintronics and graphene physics and spins out promising applications which will be described here. After introducing the initial work done on electron localization in random magnetic fields, the experimental methods for fabricating magnetic potentials are presented. Drift-diffusion phenomena are then described, which include commensurability oscillations, magnetic channelling, resistance resonance effects and magnetic dots. We then review quantum phenomena in magnetic potentials including magnetic quantum wires, magnetic minibands in superlattices, rectification by snake states, quantum tunnelling and Klein tunnelling. The third part is devoted to spintronics in inhomogeneous magnetic fields. This covers spin filtering by magnetic field gradients and circular magnetic fields, electrically induced spin resonance, spin resonance fluorescence and coherent spin manipulation.
Jacob's ladder of approximations to paraxial dynamic electron scattering
NASA Astrophysics Data System (ADS)
Lubk, A.; Rusz, J.
2015-12-01
Dynamical scattering theory describes the dominant scattering process of beam electrons at targets in the transmission electron microscope (TEM). Hence, practically every quantitative TEM study has to consider its ramifications, typically by some approximate modeling. Here, we elaborate on a hierarchy within the various approximations focusing on the two principal approaches used in practice, Bloch wave and multislice. We reveal characteristic differences in the capability of these methods to reproduce the correct local propagation of the wave function, while convergent results are obtained over larger propagation distances. We investigate the dependency of local variations of the wave function on the atomic number of the atomic scatterers and discuss their significance for, e.g., inelastic scattering.
Dynamics of electron-plasma vortex in background vorticity distribution.
Kiwamoto, Y; Ito, K; Sanpei, A; Mohri, A
2000-10-09
Dynamics of a point vortex in interaction with a broad profile of background vorticity is studied experimentally by using an electron plasma. The observed motion of the vortex compares favorably with a recently proposed theoretical model [D. A. Schecter and D. H. E. Dubin, Phys. Rev. Lett. 83, 2191 (1999)]. Perturbations in the background distribution in the wake of the spiral orbit of the vortex amount to several tens of percent and are considered to be a major reason for deviations of the observation from the linear theoretical model.
Dynamic-scanning-electron-microscope study of friction and wear
NASA Technical Reports Server (NTRS)
Brainard, W. A.; Buckley, D. H.
1974-01-01
A friction and wear apparatus was built into a real time scanning electron microscope (SEM). The apparatus and SEM comprise a system which provides the capability of performing dynamic friction and wear experiments in situ. When the system is used in conjunction with dispersive X-ray analysis, a wide range of information on the wearing process can be obtained. The type of wear and variation with speed, load, and time can be investigated. The source, size, and distribution of wear particles can be determined and metallic transferal observed. Some typical results obtained with aluminum, copper, and iron specimens are given.
Dynamics of Electron-Plasma Vortex in Background Vorticity Distribution
NASA Astrophysics Data System (ADS)
Kiwamoto, Y.; Ito, K.; Sanpei, A.; Mohri, A.
2000-10-01
Dynamics of a point vortex in interaction with a broad profile of background vorticity is studied experimentally by using an electron plasma. The observed motion of the vortex compares favorably with a recently proposed theoretical model [D. A. Schecter and D. H. E. Dubin, Phys. Rev. Lett. 83, 2191 (1999)]. Perturbations in the background distribution in the wake of the spiral orbit of the vortex amount to several tens of percent and are considered to be a major reason for deviations of the observation from the linear theoretical model.
Electron density and plasma dynamics of a colliding plasma experiment
Wiechula, J. Schönlein, A.; Iberler, M.; Hock, C.; Manegold, T.; Bohlender, B.; Jacoby, J.
2016-07-15
We present experimental results of two head-on colliding plasma sheaths accelerated by pulsed-power-driven coaxial plasma accelerators. The measurements have been performed in a small vacuum chamber with a neutral-gas prefill of ArH{sub 2} at gas pressures between 17 Pa and 400 Pa and load voltages between 4 kV and 9 kV. As the plasma sheaths collide, the electron density is significantly increased. The electron density reaches maximum values of ≈8 ⋅ 10{sup 15} cm{sup −3} for a single accelerated plasma and a maximum value of ≈2.6 ⋅ 10{sup 16} cm{sup −3} for the plasma collision. Overall a raise of the plasma density by a factor of 1.3 to 3.8 has been achieved. A scaling behavior has been derived from the values of the electron density which shows a disproportionately high increase of the electron density of the collisional case for higher applied voltages in comparison to a single accelerated plasma. Sequences of the plasma collision have been taken, using a fast framing camera to study the plasma dynamics. These sequences indicate a maximum collision velocity of 34 km/s.
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. © 2014 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim.
Optical electronic computer systems design in stationary and dynamic modes
NASA Astrophysics Data System (ADS)
Perju, Veacheslav L.
2001-03-01
The theory of designing the optical-electronic image processing computer systems has been presented. A model of parallel image processing system has been considered, that is based on the principle of function decomposition. The implementation possibilities of different image processing operations with the help of optical and electronic computer means have been analyzed. A structure model of computer system has been examined, that is a conveyor of parallel computer devices. The evaluation of time outlay in the system, while processing an image or a series of them has been made. The differences of time outlay from conveyor length change and the correlation of optical and electronic devices and processing time in them have been exposed. The designing method of image processing systems in static made has been elaborated. There are presented the results of investigations of the influence of the median square deviation, the influence of time of the processing in the modules on the throughput capacity of the system under the different electronic and optical modules quantity. According to the results of investigations the recommendations of increasing the system's throughput the capacity are formulated. On the basis of these recommendations, the system design method of image processing in the dynamic mode is elaborated.
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
Ki, Dae-Han; Jung, Young-Dae
2013-03-15
The influence of the dynamic shielding on the Wannier ridge electron escapes into the continuum states by the electron-impact is investigated in weakly coupled plasmas. The dynamically shielded renormalized electron charge and screened Wannier exponent are obtained by considering the equation of motion in the Wannier configuration mode with the effective interaction potential as functions of the charge of the residual ion, Debye length, projectile energy, and thermal energy. The result shows that the dynamic renormalized effective electron charge decreases with an increase of the thermal energy, especially for large distances. It is found that the dynamic shielding effect enhances the Wannier exponent for the double-electron escape. The variation of the dynamic shielding effect on the screened Wannier exponent is also discussed.
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.
NASA Astrophysics Data System (ADS)
Sigmund, Jochen; Lampin, Jean-François; Ivannikov, Valentin; Sydlo, Cezary; Feiginov, Michail; Pavlidis, Dimitris; Meissner, Peter; Hartnagel, Hans L.
We report on continuous-wave optoelectronic terahertz (THz) measurements using low-temperature grown (LTG) GaAsSb as photomixer material. A broadband log-periodic antenna and a six interdigital finger photomixer with 1μm gap is fabricated on LTG-GaAsSb for THz generation and detection. At 0.37THz, the resonance frequency of the inner most antenna tooth, we obtained a power of 6.3nW. A Golay cell was used as detector. The photocarrier lifetime of the material was determined to be 700fs by pump-probe experiments with an optical wavelength close to the band gap of LTG-GaAsSb. The band gap was 1.0eV, measured by wavelength dependent pump-probe measurements.
Electronically coarse-grained molecular dynamics using quantum Drude oscillators
NASA Astrophysics Data System (ADS)
Jones, A. P.; Crain, J.; Cipcigan, F. S.; Sokhan, V. P.; Modani, M.; Martyna, G. J.
2013-12-01
Standard molecular dynamics (MD) simulations generally make use of a basic description of intermolecular forces which consists of fixed, pairwise, atom-centred Coulomb, van der Waals and short-range repulsive terms. Important interactions such as many-body polarisation and many-body dispersion which are sensitive to changes in the environment are usually neglected, and their effects treated effectively within mean-field approximations to reproduce a single thermodynamic state point or physical environment. This leads to difficulties in modelling the complex interfaces of interest today where the behaviour may be quite different from the regime of parameterisation. Here, we describe the construction and properties of a Gaussian coarse-grained electronic structure, which naturally generates many-body polarisation and dispersion interactions. The electronic structure arises from a fully quantum mechanical treatment of a set of distributed quantum Drude oscillators (QDOs), harmonic atoms which interact with each other and other moieties via electrostatic (Coulomb) interactions; this coarse-grained approach is capable of describing many-body polarisation and dispersion but not short-range interactions which must be parametrised. We describe how on-the-fly forces due to this exchange-free Gaussian model may be generated with linear scale in the number of atoms in the system using an adiabatic path integral molecular dynamics for quantum Drude oscillators technique (APIMD-QDO). We demonstrate the applicability of the QDO approach to realistic systems via a study of the liquid-vapour interface of water.
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.
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.
Dynamic characterization and modeling of potting materials for electronics assemblies
NASA Astrophysics Data System (ADS)
Joshi, Vasant S.; Lee, Gilbert F.; Santiago, Jaime R.
2017-01-01
Prediction of survivability of encapsulated electronic components subject to impact relies on accurate modeling, which in turn needs both static and dynamic characterization of individual electronic components and encapsulation material to generate reliable material parameters for a robust material model. Current focus is on potting materials to mitigate high rate loading on impact. In this effort, difficulty arises in capturing one of the critical features characteristic of the loading environment in a high velocity impact: multiple loading events coupled with multi-axial stress states. Hence, potting materials need to be characterized well to understand its damping capacity at different frequencies and strain rates. An encapsulation scheme to protect electronic boards consists of multiple layers of filled as well as unfilled polymeric materials like Sylgard 184 and Trigger bond Epoxy # 20-3001. A combination of experiments conducted for characterization of materials used Split Hopkinson Pressure Bar (SHPB), and dynamic material analyzer (DMA). For material which behaves in an ideal manner, a master curve can be fitted to Williams-Landel-Ferry (WLF) model. To verify the applicability of WLF model, a new temperature-time shift (TTS) macro was written to compare idealized temperature shift factor with experimental incremental shift factor. Deviations can be readily observed by comparison of experimental data with the model fit to determine if model parameters reflect the actual material behavior. Similarly, another macro written for obtaining Ogden model parameter from Hopkinson Bar tests can readily indicate deviations from experimental high strain rate data. Experimental results for different materials used for mitigating impact, and ways to combine data from DMA and Hopkinson bar together with modeling refinements are presented.
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.
Dissipative many-electron dynamics of ionizing systems
NASA Astrophysics Data System (ADS)
Tremblay, Jean Christophe; Klinkusch, Stefan; Klamroth, Tillmann; Saalfrank, Peter
2011-01-01
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.
Smooth landscape solvent dynamics in electron transfer reactions
NASA Astrophysics Data System (ADS)
Leite, Vitor B. P.
1999-05-01
Solvent effects play a major role in controlling electron-transfer reactions. The solvent dynamics happens on a very high-dimensional surface, and this complex landscape is populated by a large number of minima. A critical problem is to understand the conditions under which the solvent dynamics can be represented by a single collective reaction coordinate. When this unidimensional representation is valid, one recovers the successful Marcus theory. In this study the approach used in a previous work [V. B. P. Leite and J. N. Onuchic; J. Phys. Chem. 100, 7680 (1996)] is extended to treat a more realistic solvent model, which includes energy correlation. The dynamics takes place in a smooth and well behaved landscape. The single shell of solvent molecules around a cavity is described by a two-dimensional system with periodic boundary conditions with nearest neighbor interaction. It is shown how the polarization-dependent effects can be inferred. The existence of phase transitions depends on a factor γ proportional to the contribution from the two parameters of the model. For the present model, γ suggests the existence of "weak kinetic phase transitions," which are used in the analysis of solvent effects in charge-transfer reactions.
Slow dynamics of electron glasses: The role of disorder
NASA Astrophysics Data System (ADS)
Ovadyahu, Z.
2017-04-01
We examine in this work the role of disorder in contributing to the sluggish relaxation observed in intrinsic electron glasses. Our approach is guided by several empirical observations: First and foremost, Anderson localization is a pre-requisite for observing these nonequilibrium phenomena. Secondly, sluggish relaxation appears to favor Anderson insulators with relatively large Fermi energies (hence proportionally large disorder). These observations motivated us to consider a way to measure the underlying disorder in a realistic Anderson insulator. Optical studies using a series of amorphous indium oxide (InxO ) establish a simple connection between carrier concentration and the disorder necessary to approach the metal-insulator transition from the insulating side. This is used to estimate the typical magnitude of the quenched potential fluctuation in the electron-glass phase of this system. The implications of our findings on the slow dynamics of Anderson insulators are discussed. In particular, the reason for the absence of a memory dip and the accompanying electron-glass effects in lightly-doped semiconductors emerges as a natural consequence of their weak disorder.
Organic (opto)electronic materials: understanding charge carrier dynamics
NASA Astrophysics Data System (ADS)
Ostroverkhova, Oksana
2008-05-01
There is growing interest in using organic (opto)electronic materials for applications in electronics and photonics. In particular, organic semiconductor thin films offer several advantages over traditional silicon technology, including low-cost processing, the potential for large-area flexible devices, high-efficiency light emission, and widely tunable properties through functionalization of the molecules. Over the past decade, remarkable progress in materials design and purification has been made, which led to applications of organic semiconductors in light-emitting diodes, polymer lasers, photovoltaic cells, high-speed photodetectors, organic thin-film transistors, and many others. Most of the applications envisioned for organic semiconductors rely on their conductive or photoconductive properties. However, despite remarkable progress in organic electronics and photonics, the nature of charge carrier photogeneration and transport in organic semiconductors is not completely understood and remains controversial, partly due to difficulties in assessing intrinsic properties that are often masked by impurities, grain boundaries, etc. Measurements of charge carrier dynamics at picosecond time scales after excitation reveal the intrinsic nature of mobile charge carriers before they are trapped at defect sites. In this presentation, I will review the current state of the field and summarize our recent results on photoconductivity of novel high-performance organic semiconductors (such as functionalized pentacene and anthradithiophene thin films) from picoseconds to seconds after photoexcitation. Photoluminescent properties of these novel materials will also be discussed.
Dynamic Control of Electron Transfers in Diflavin Reductases
Aigrain, Louise; Fatemi, Fataneh; Frances, Oriane; Lescop, Ewen; Truan, Gilles
2012-01-01
Diflavin reductases are essential proteins capable of splitting the two-electron flux from reduced pyridine nucleotides to a variety of one electron acceptors. The primary sequence of diflavin reductases shows a conserved domain organization harboring two catalytic domains bound to the FAD and FMN flavins sandwiched by one or several non-catalytic domains. The catalytic domains are analogous to existing globular proteins: the FMN domain is analogous to flavodoxins while the FAD domain resembles ferredoxin reductases. The first structural determination of one member of the diflavin reductases family raised some questions about the architecture of the enzyme during catalysis: both FMN and FAD were in perfect position for interflavin transfers but the steric hindrance of the FAD domain rapidly prompted more complex hypotheses on the possible mechanisms for the electron transfer from FMN to external acceptors. Hypotheses of domain reorganization during catalysis in the context of the different members of this family were given by many groups during the past twenty years. This review will address the recent advances in various structural approaches that have highlighted specific dynamic features of diflavin reductases. PMID:23203109
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 Bi2Se3
Valdés Aguilar, R.; Qi, J.; Brahlek, M.; ...
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
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.
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.
Pacheco, Alexander B; Iyengar, Srinivasan S
2011-02-21
We recently proposed a multistage ab initio wavepacket dynamics (MS-AIWD) treatment for the study of delocalized electronic systems as well as electron transport through donor-bridge-acceptor systems such as those found in molecular-wire/electrode networks. In this method, the full donor-bridge-acceptor open system is treated through a rigorous partitioning scheme that utilizes judiciously placed offsetting absorbing and emitting boundary conditions. In this manner, the electronic coupling between the bridge molecule and surrounding electrodes is accounted. Here, we extend MS-AIWD to include the dynamics of open-electronic systems in conjunction with (a) simultaneous treatment of nuclear dynamics and (b) external electromagnetic fields. This generalization is benchmarked through an analysis of wavepackets propagated on a potential modeled on an Al(27) - C(7) - Al(27) nanowire. The wavepacket results are inspected in the momentum representation and the dependence of momentum of the wavepacket as well as its transmission probabilities on the magnitude of external bias are analyzed.
NASA Astrophysics Data System (ADS)
Pacheco, Alexander B.; Iyengar, Srinivasan S.
2011-02-01
We recently proposed a multistage ab initio wavepacket dynamics (MS-AIWD) treatment for the study of delocalized electronic systems as well as electron transport through donor-bridge-acceptor systems such as those found in molecular-wire/electrode networks. In this method, the full donor-bridge-acceptor open system is treated through a rigorous partitioning scheme that utilizes judiciously placed offsetting absorbing and emitting boundary conditions. In this manner, the electronic coupling between the bridge molecule and surrounding electrodes is accounted. Here, we extend MS-AIWD to include the dynamics of open-electronic systems in conjunction with (a) simultaneous treatment of nuclear dynamics and (b) external electromagnetic fields. This generalization is benchmarked through an analysis of wavepackets propagated on a potential modeled on an Al27 - C7 - Al27 nanowire. The wavepacket results are inspected in the momentum representation and the dependence of momentum of the wavepacket as well as its transmission probabilities on the magnitude of external bias are analyzed.
NASA Astrophysics Data System (ADS)
Pacheco, Alexander B.; Iyengar, Srinivasan S.
2010-07-01
We propose a multistage quantum wavepacket dynamical treatment for the study of delocalized electronic systems as well as electron transport through donor-bridge-acceptor systems such as those found in molecular-wire/electrode networks. The full donor-bridge-acceptor system is treated through a rigorous partitioning scheme that utilizes judiciously placed offsetting absorbing and emitting boundary conditions. These facilitate a computationally efficient and potentially accurate treatment of the long-range coupling interactions between the bridge and donor/acceptor systems and the associated open system boundary conditions. Time-independent forms of the associated, partitioned equations are also derived. In the time-independent form corresponding to the bridge system, coupling to donor and acceptor, that is long-range interactions, is completely accounted. For the time-dependent study, the quantum dynamics of the electronic flux through the bridge-donor/acceptor interface is constructed using an accurate and efficient representation of the discretized quantum-mechanical free-propagator. A model for an electrode-molecular wire-electrode system is used to test the accuracy of the scheme proposed. Transmission probability is obtained directly from the probability density of the electronic flux in the acceptor region. Conductivity through the molecular wire is computed using a wavepacket flux correlation function.
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 Schrödinger 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) variant Planck's over 2pil (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.
Single Molecule Lysozyme Dynamics Monitored by an Electronic Circuit
Choi, Yongki; Moody, Issa S.; Sims, Patrick C.; Hunt, Steven R.; Corso, Brad L.; Perez, Israel; Weiss, Gregory A.; Collins, Philip G.
2014-01-01
Tethering a single lysozyme molecule to a carbon nanotube field effect transistor (FET) produced a stable, high-bandwidth transducer for protein motion. Electronic monitoring during 10-minute periods extended well beyond the limitations of fluorescence techniques to uncover dynamic disorder within a single molecule and establish lysozyme as a processive enzyme. On average, 100 chemical bonds are processively hydrolyzed, at 15-Hertz rates, before lysozyme returns to its nonproductive, 330-Hertz hinge motion. Statistical analysis differentiated single-step hinge closure from enzyme opening, which requires two steps. Seven independent time scales governing lysozyme’s activity we re observed. The pH dependence of lysozyme activity arises not from changes to its processive kinetics but rather from increasing time spent in either nonproductive rapid motions or an inactive, closed conformation. PMID:22267809
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.
Dynamic local field factor of an uniform electron liquid
NASA Astrophysics Data System (ADS)
Mukhopadhyay, G.
1988-08-01
We present an expression for the dynamic local field factor of a uniform interacting electron liquid, as G(q, ω) = G1(q) + G2(q, ω), where G1 is the static local field factor of the STLS-theory, and G2 has a structure similar to that obtainable from the mode-coupling theory of the Memory-function approach. The q → 0 limit of the imaginary part of G, which is of interest in the time-dependent Local-density-functional theory, has the correct ω-3/2 dependence, and yields the long-wavelength plasmon damping coefficient in good agreement with diagramatic calculations as well as the mode-coupling approach; detailed numerical results are also presented.
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.
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
Two dimensional electron spin resonance: Structure and dynamics of biomolecules
NASA Astrophysics Data System (ADS)
Saxena, Sunil; Freed, Jack H.
1998-03-01
The potential of two dimensional (2D) electron spin resonance (ESR) for measuring the structural properties and slow dynamics of labeled biomolecules will be presented. Specifically, it will be shown how the recently developed method of double quantum (DQ) 2D ESR (S. Saxena and J. H. Freed, J. Chem. Phys. 107), 1317, (1997) can be used to measure large interelectron distances in bilabeled peptides. The need for DQ ESR spectroscopy, as well as the challenges and advantages of this method will be discussed. The elucidation of the slow reorientational dynamics of this peptide (S. Saxena and J. H. Freed, J. Phys. Chem. A, 101) 7998 (1997) in a glassy medium using COSY and 2D ELDOR ESR spectroscopy will be demonstrated. The contributions to the homogeneous relaxation time, T_2, from the overall and/or internal rotations of the nitroxide can be distinguished from the COSY spectrum. The growth of spectral diffusion cross-peaks^2 with mixing time in the 2D ELDOR spectra can be used to directly determine a correlation time from the experiment which can be related to the rotational correlation time.
Photolyase: Dynamics and electron-transfer mechanisms of DNA repair.
Zhang, Meng; Wang, Lijuan; Zhong, Dongping
2017-08-09
Photolyase, a flavoenzyme containing flavin adenine dinucleotide (FAD) molecule as a catalytic cofactor, repairs UV-induced DNA damage of cyclobutane pyrimidine dimer (CPD) and pyrimidine-pyrimidone (6-4) photoproduct using blue light. The FAD cofactor, conserved in the whole protein superfamily of photolyase/cryptochromes, adopts a unique folded configuration at the active site that plays a critical functional role in DNA repair. Here, we review our comprehensive characterization of the dynamics of flavin cofactor and its repair photocycles by different classes of photolyases on the most fundamental level. Using femtosecond spectroscopy and molecular biology, significant advances have recently been made to map out the entire dynamical evolution and determine actual timescales of all the catalytic processes in photolyases. The repair of CPD reveals seven electron-transfer (ET) reactions among ten elementary steps by a cyclic ET radical mechanism through bifurcating ET pathways, a direct tunneling route mediated by the intervening adenine and a two-step hopping path bridged by the intermediate adenine from the cofactor to damaged DNA, through the conserved folded flavin at the active site. The unified, bifurcated ET mechanism elucidates the molecular origin of various repair quantum yields of different photolyases from three life kingdoms. For 6-4 photoproduct repair, a similar cyclic ET mechanism operates and a new cyclic proton transfer with a conserved histidine residue at the active site of (6-4) photolyases is revealed. Copyright © 2017 Elsevier Inc. All rights reserved.
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.
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.
Coupled electron-nuclear wavepacket dynamics in potassium dimers
NASA Astrophysics Data System (ADS)
Braun, Hendrike; Bayer, Tim; Sarpe, Cristian; Siemering, Robert; de Vivie-Riedle, Regina; Baumert, Thomas; Wollenhaupt, Matthias
2014-06-01
Recently we have demonstrated control of valence-bond excitation of a molecule due to the interplay of the induced charge oscillation with the precisely tailored phase of the driving laser field (Bayer et al 2013 Phys. Rev. Lett. 110 123003). In this contribution we describe in more detail the two-colour experiment—a control pulse sequence followed by an ionizing probe pulse of a different wavelength. We provide details on the quantum dynamics simulations carried out to reproduce and to analyse the experimental results. The procedure for averaging over the focal intensity distribution in the interaction region and the method for orientation averaging, which are both crucial for the reproduction of our strong-field measurements, are also described in detail. The analysis of the temporal evolution of the expectation values of the wavepackets on the relevant potentials, the induced energetic shifts in the molecule and the modulation in the charge oscillation provides further insights into the interplay of the coupled nuclear-electron dynamics. Because the measured photoelectron spectra reveal the population of the target states we describe the quantum mechanical approach to calculate the photoelectron spectra and rationalize the results using Mulliken's difference potential method.
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.
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.
Morini, Filippo; Watanabe, Noboru; Kojima, Masataka; Deleuze, Michael Simon; 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 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.
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.
Electron accommodation dynamics in the DNA base thymine
NASA Astrophysics Data System (ADS)
King, Sarah B.; Stephansen, Anne B.; Yokoi, Yuki; Yandell, Margaret A.; Kunin, Alice; Takayanagi, Toshiyuki; Neumark, Daniel M.
2015-07-01
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-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-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-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.
Electronic structure and relaxation dynamics in a superconducting topological material
Neupane, Madhab; Ishida, Yukiaki; Sankar, Raman; ...
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
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
2016-03-03
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 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. In conclusion, our results will be helpful in understanding low temperature superconducting states of these topological materials.
Steady-state and transient electronic dynamics in granular metals
NASA Astrophysics Data System (ADS)
Chen, Wei
In this thesis two very different approaches, steady state and transient, are taken to help understand the electronic dynamics in the nanogranular Cux(SiO2)1-x composite thin films. The electrical conductivity and thermopower are measured from 2 K to room temperature with the Cu volume fraction x varying from 1 down to 0.43. At low temperatures, a T dependence of the electrical conductivity is observed well above the percolation threshold due to the disorder-enhanced electron-electron interaction and as the metal-insulator transition is approached, the electrical conductivity assumes a T1/3 dependence. The thermopower is found to be small and rather insensitive to the degree of disorder in the system. It varies linearly with temperatures at both low and high temperatures. Annealing has considerable influence to the behavior of the electrical conductivity while introducing little changes to the thermopower. Femtosecond pump-probe experiments were performed on a series of Cu x(SiO2)1-x composite films with volume fraction x varying from 0.7 to 1.0 to study the reflectivity change DeltaR/R as a function of composition and temperature. It is discovered that DeltaR/R undergoes drastic changes as the metal content is lowered. Very small amount of SiO 2 inclusions can start to result in qualitatively different Delta R/R behavior from pure Cu. Changes in the dielectric constant of Cu are investigated and possible explanations for the DeltaR/R behaviors in the composite films are discussed.
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
Nakamura, A.; Shimojima, T.; Nakano, M.; Iwasa, Y.; Ishizaka, K.
2016-01-01
We report the ultrafast dynamics of electrons and lattice in transition metal thin films (Au, Cu, and Mo) investigated by a combination of ultrafast electron diffraction (UED) and pump-probe optical methods. For a single-crystalline Au thin film, we observe the suppression of the diffraction intensity occuring in 10 ps, which direcly reflects the lattice thermalization via the electron-phonon interaction. By using the two-temperature model, the electron-phonon coupling constant (g) and the electron and lattice temperatures (Te, Tl) are evaluated from UED, with which we simulate the transient optical transmittance. The simulation well agrees with the experimentally obtained transmittance data, except for the slight deviations at the initial photoexcitation and the relaxed quasi-equilibrium state. We also present the results similarly obtained for polycrystalline Au, Cu, and Mo thin films and demonstrate the electron and lattice dynamics occurring in metals with different electron-phonon coupling strengths. PMID:28004010
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.
NASA Astrophysics Data System (ADS)
Hagelberg, Frank
2004-03-01
In this contribution, we address the problem how to determine accurately the nonadiabatic content of any given dynamic process involving molecular motion. More specifically, we generate a dynamic electronic wave function using Electron Nuclear Dynamics (END) theory^2 and cast this wave function into the language of electronic excitations. This is achieved by adiabatic transport of an electronic basis along the classical nuclear trajectories of the studied molecular system. This basis is chosen as the static UHF molecular ground state determinant of the system in conjunction with all determinants that arise from the ground state by single, double and triple substitutions. Projecting the dynamic wave function into this basis, we arrive at a natural distinction between adiabatic and nonadiabatic components of the motion considered. We will discuss this concept by the examples of various scattering problems, among them the interaction of proton projectiles with methylene targets. ^2E. Deumens et al., Rev. Mod. Phys. 1994, 66, 917.
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
Precession dynamics of the relativistic electron spin in laser-plasma acceleration
Pugacheva, D V; Andreev, N E
2016-01-31
A model is developed to study the precession dynamics of the relativistic electron spin in a laser-plasma accelerator versus the initial energy of the electron and its injection phase. Optimal parameters providing minimum depolarisation of the electron in the acceleration process are determined. (laser -plasma acceleration of electrons)
Dynamics of valence-shell electrons and nuclei probed by strong-field holography and rescattering
NASA Astrophysics Data System (ADS)
Walt, Samuel G.; Bhargava Ram, Niraghatam; Atala, Marcos; Shvetsov-Shilovski, Nikolay I.; von Conta, Aaron; Baykusheva, Denitsa; Lein, Manfred; Wörner, Hans Jakob
2017-06-01
Strong-field photoelectron holography and laser-induced electron diffraction (LIED) are two powerful emerging methods for probing the ultrafast dynamics of molecules. However, both of them have remained restricted to static systems and to nuclear dynamics induced by strong-field ionization. Here we extend these promising methods to image purely electronic valence-shell dynamics in molecules using photoelectron holography. In the same experiment, we use LIED and photoelectron holography simultaneously, to observe coupled electronic-rotational dynamics taking place on similar timescales. These results offer perspectives for imaging ultrafast dynamics of molecules on femtosecond to attosecond timescales.
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.
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.
Effect of electron spin dynamics on solid-state dynamic nuclear polarization performance.
Siaw, Ting Ann; Fehr, Matthias; Lund, Alicia; Latimer, Allegra; Walker, Shamon A; Edwards, Devin T; Han, Song-I
2014-09-21
For the broadest dissemination of solid-state dynamic nuclear polarization (ssDNP) enhanced NMR as a material characterization tool, the ability to employ generic mono-nitroxide radicals as spin probes is critical. A better understanding of the factors contributing to ssDNP efficiency is needed to rationally optimize the experimental condition for the practically accessible spin probes at hand. This study seeks to advance the mechanistic understanding of ssDNP by examining the effect of electron spin dynamics on ssDNP performance at liquid helium temperatures (4-40 K). The key observation is that bi-radicals and mono-radicals can generate comparable nuclear spin polarization at 4 K and 7 T, which is in contrast to the observation for ssDNP at liquid nitrogen temperatures (80-150 K) that finds bi-radicals to clearly outperform mono-radicals. To rationalize this observation, we analyze the change in the DNP-induced nuclear spin polarization (Pn) and the characteristic ssDNP signal buildup time as a function of electron spin relaxation rates that are modulated by the mono- and bi-radical spin concentration. Changes in Pn are consistent with a systematic variation in the product of the electron spin-lattice relaxation time and the electron spin flip-flop rate that constitutes an integral saturation factor of an inhomogeneously broadened EPR spectrum. We show that the comparable Pn achieved with both radical species can be reconciled with a comparable integral EPR saturation factor. Surprisingly, the largest Pn is observed at an intermediate spin concentration for both mono- and bi-radicals. At the highest radical concentration, the stronger inter-electron spin dipolar coupling favors ssDNP, while oversaturation diminishes Pn, as experimentally verified by the observation of a maximum Pn at an intermediate, not the maximum, microwave (μw) power. At the maximum μw power, oversaturation reduces the electron spin population differential that must be upheld between
Terahertz Dynamics of Quantum-Confined Electrons in Carbon Nanomaterials
NASA Astrophysics Data System (ADS)
Ren, Lei
The terahertz (THz) frequency range. 0.1 - 20 THz, exists between the microwave and infrared ranges and contains abundant information on the dynamics of charge and spin carriers in condensed matter systems. Since its advent two decades ago, THz spectroscopy has been extensively used to study a wide range of solid state materials, including typical semiconductors, conducting polymers, insulators, superconductors, and artificially grown structures such as quantum wells. In these systems, electronic and photonic events tend to occur on the time scale of tens to hundreds of femtoseconds, which results in many important excitations, resonances and dynamical phenomena in the THz frequency range. In this dissertation work, we have developed a typical THz time-domain spectroscopy (TDS) system to investigate the THz dynamics of quantum-confined electrons in two important types of carbon nanomaterial: single-walled carbon nanotubes (SWNTs) and graphene. Polarization dependent THz transmission measurements were conducted on a highly-aligned SWNT film on a sapphire substrate, revealing extremely high anisotropy: virtually no attenuation was observed when the polarization of the THz beam was perpendicular to the nanotube axis, while the THz beam was strongly absorbed when its polarization was parallel to the tube axis. From the measured absorption anisotropy, we calculated the reduced linear dichrosim to be 3, corresponding to a nematic order parameter of 1. These observations are a direct result of the one-dimensional nature of conduction electrons in the nanotubes and at the same time, demonstrate that any misalignment of nanotubes in the film mast have characteristic length scales much smaller than the wavelengths used in these experiments (1.5 mm -- 150 mum). Based on this work, an ideal THz linear polarizer built with parallel stacks of such aligned SWNT films was synthesized, exhibiting a degree of polarization of 99.9% throughout the frequency range 0.2 -- 2.2 THz and a
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
Li, Lesheng; Kanai, Yosuke
2016-04-21
Excited electron dynamics at semiconductor-molecule interfaces is ubiquitous in various energy conversion technologies. However, a quantitative understanding of how molecular details influence the quantum dynamics of excited electrons remains a great scientific challenge because of the complex interplay of different processes with various time scales. Here, we employ first-principles electron dynamics simulations to investigate how molecular features govern the dynamics in a representative interface between the hydrogen-terminated Si(111) surface and a cyanidin molecule. Hot electron transfer to the chemisorbed molecule was observed but was short-lived on the molecule. Interfacial electron transfer to the chemisorbed molecule was found to be largely decoupled from hot electron relaxation within the semiconductor surface. While the hot electron relaxation was found to take place on a time scale of several hundred femtoseconds, the subsequent interfacial electron transfer was slower by an order of magnitude. At the same time, this secondary process of picosecond electron transfer is comparable in time scale to typical electron trapping into defect states in the energy gap.
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.
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
NASA Astrophysics Data System (ADS)
Gorcester, Jeff; Rananavare, Shankar B.; Freed, Jack H.
1989-05-01
Electron spin-echo (ESE) and two-dimensional electron-electron double resonance (2D ELDOR) experiments have been performed as a function of director orientation and temperature in the smectic A phase of the liquid crystal S2 for the spin-probe PD-tempone(2×10-3 M). Over the entire temperature range studied (288-323 K) we observe significant 2D ELDOR cross peaks only for ΔMI =±1 indicative of 14N spin-relaxation and negligible Heisenberg exchange. From the angular dependent 14N spin-relaxation rates we obtain the dipolar spectral densities at the hyperfine (hf) frequency, whereas from a combination of ESE and 2D ELDOR we obtain the dipolar and Zeeman-dipolar spectral densities at zero frequency. The angular dependent spectral densities were successfully decomposed into their basic components in accordance with theory. The angular dependent spectral densities at the hf frequency are not predicted by a model of anisotropic rotational diffusion in a nematic orienting potential, but are consistent with predictions of a model due to Moro and Nordio of solute rototranslational diffusion in a McMillan-type potential. The angular dependence also indicates that order director fluctuations in the smectic phase are suppressed at frequencies on the order of 10 MHz. An additional contribution to solute reorientation due to cooperative hydrocarbon chain fluctuations is suggested to account for the behavior of the observed spectral densities at zero frequency. An evaluation of the relevance of several other dynamical models to this experimental work is also presented.
Vlasov simulations of electron hole dynamics in inhomogeneous magnetic field
NASA Astrophysics Data System (ADS)
Kuzichev, Ilya; Vasko, Ivan; Agapitov, Oleksiy; Mozer, Forrest; Artemyev, Anton
2017-04-01
Electron holes (EHs) or phase space vortices are solitary electrostatic waves existing due to electrons trapped within EH electrostatic potential. Since the first direct observation [1], EHs have been widely observed in the Earth's magnetosphere: in reconnecting current sheets [2], injection fronts [3], auroral region [4], and many other space plasma systems. EHs have typical spatial scales up to tens of Debye lengths, electric field amplitudes up to hundreds of mV/m and propagate along magnetic field lines with velocities of about electron thermal velocity [5]. The role of EHs in energy dissipation and supporting of large-scale potential drops is under active investigation. The accurate interpretation of spacecraft observations requires understanding of EH evolution in inhomogeneous plasma. The critical role of plasma density gradients in EH evolution was demonstrated in [6] using PIC simulations. Interestingly, up to date no studies have addressed a role of magnetic field gradients in EH evolution. In this report, we use 1.5D gyrokinetic Vlasov code to demonstrate the critical role of magnetic field gradients in EH dynamics. We show that EHs propagating into stronger (weaker) magnetic field are decelerated (accelerated) with deceleration (acceleration) rate dependent on the magnetic field gradient. Remarkably, the reflection points of decelerating EHs are independent of the average magnetic field gradient in the system and depend only on the EH parameters. EHs are decelerated (accelerated) faster than would follow from the "quasi-particle" concept assuming that EH is decelerated (accelerated) entirely due to the mirror force acting on electrons trapped within EH. We demonstrate that EH propagation in inhomogeneous magnetic fields results in development of a net potential drop along an EH, which depends on the magnetic field gradient. The revealed features will be helpful for interpreting spacecraft observations and results of advanced particle simulations. In
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.
Electron density dynamics in the electronic ground state: motion along the Kekulé mode of benzene.
Schild, Axel; Choudhary, Deepanshu; Sambre, Vaibhav D; Paulus, Beate
2012-11-26
If the Born-Oppenheimer approximation is invoked for the description of chemical reactions, the electron density rearranges following the motion of the nuclei. Even though this approach is central to theoretical chemistry, the explicit time dependence of the electron density is rarely studied, especially if the nuclei are treated quantum mechanically. In this article, we model the motion of benzene along the Kekulé vibrational coordinate to simulate the nuclear dynamics and electron density dynamics in the electronic ground state. Details of the change of core, valence, and π electrons are determined and analyzed. We show how the pictures anticipated by drawing Lewis structures of the rearrangement correlate with the time-dependent quantum description of the process.
NASA Astrophysics Data System (ADS)
Matsuoka, Takahide; Takatsuka, Kazuo
2017-04-01
A theory for dynamics of molecular photoionization from nonadiabatic electron wavepackets driven by intense pulse lasers is proposed. Time evolution of photoelectron distribution is evaluated in terms of out-going electron flux (current of the probability density of electrons) that has kinetic energy high enough to recede from the molecular system. The relevant electron flux is in turn evaluated with the complex-valued electronic wavefunctions that are time evolved in nonadiabatic electron wavepacket dynamics in laser fields. To uniquely rebuild such wavefunctions with its electronic population being lost by ionization, we adopt the complex-valued natural orbitals emerging from the electron density as building blocks of the total wavefunction. The method has been implemented into a quantum chemistry code, which is based on configuration state mixing for polyatomic molecules. Some of the practical aspects needed for its application will be presented. As a first illustrative example, we show the results of hydrogen molecule and its isotope substitutes (HD and DD), which are photoionized by a two-cycle pulse laser. Photon emission spectrum associated with above threshold ionization is also shown. Another example is taken from photoionization dynamics from an excited state of a water molecule. Qualitatively significant effects of nonadiabatic interaction on the photoelectron spectrum are demonstrated.
Electron-phonon thermalization in a scalable method for real-time quantum dynamics
Rizzi, Valerio; Todorov, Tchavdar N.; Kohanoff, Jorge J.; Correa, Alfredo A.
2016-01-27
Here, we present a quantum simulation method that follows the dynamics of out-of-equilibrium many-body systems of electrons and oscillators in real time. Its cost is linear in the number of oscillators and it can probe time scales from attoseconds to hundreds of picoseconds. Contrary to Ehrenfest dynamics, it can thermalize starting from a variety of initial conditions, including electronic population inversion. While an electronic temperature can be defined in terms of a nonequilibrium entropy, a Fermi-Dirac distribution in general emerges only after thermalization. These results can be used to construct a kinetic model of electron-phonon equilibration based on the explicit quantum dynamics.
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.
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.
Self-consistent Bohmian description of strong field-driven electron dynamics
Botheron, P.; Pons, B.
2010-08-15
Drawing from the Bohmian formulation of the time-dependent Schroedinger equation, we present a self-consistent hydrodynamical method to describe electron dynamics in strong field light-matter interactions. Prototypical implementation is made for one-dimensional H atom embedded in short and intense laser pulses. The method provides very accurate electron densities and yields quantum trajectories that shed light on the electron dynamics, beyond the strong-field approximation.
Gas dynamic theory of flight of fast electron flux in plasma
NASA Astrophysics Data System (ADS)
Melnik, V. N.
The one-dimensional flight of a fast electron flux in plasma is investigated taking into account generation and absorption of plasma waves. The transition from the kinetic description to the gas dynamics is made. The closed set of gas dynamic equations for electrons and plasmons is derived and an automodel solution is obtained in the case of instantaneous injection. This solution represents the beam-plasma formation on natural oscillations in the system electrons+plasmons is considered.
A method of dynamic chromatic aberration correction in low-voltage scanning electron microscopes.
Khursheed, Anjam
2005-07-01
A time-of-flight concept that dynamically corrects for chromatic aberration effects in scanning electron microscopes (SEMs) is presented. The method is predicted to reduce the microscope's chromatic aberration by an order of magnitude. The scheme should significantly improve the spatial resolution of low-voltage scanning electron microscopes (LVSEMs). The dynamic means of correcting for chromatic aberration also allows for the possibility of obtaining high image resolution from electron guns that have relatively large energy spreads.
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.
Khruschev, S S; Abaturova, A M; Diakonova, A N; Fedorov, V A; Ustinin, D M; Kovalenko, I B; Riznichenko, G Yu; Rubin, A B
2015-01-01
The application of Brownian dynamics for simulation of transient protein-protein interactions is reviewed. The review focuses on theoretical basics of Brownian dynamics method, its particular implementations, advantages and drawbacks of the method. The outlook for future development of Brownian dynamics-based simulation techniques is discussed. Special attention is given to analysis of Brownian dynamics trajectories. The second part of the review is dedicated to the role of Brownian dynamics simulations in studying photosynthetic electron transport. Interactions of mobile electron carriers (plastocyanin, cytochrome c6, and ferredoxin) with their reaction partners (cytochrome b6f complex, photosystem I, ferredoxin:NADP-reductase, and hydrogenase) are considered.
Wang, Cong; Jiang, Lan; Wang, Feng; Li, Xin; Yuan, Yanping; Xiao, Hai; Tsai, Hai-Lung; Lu, Yongfeng
2012-07-11
A real-time and real-space time-dependent density functional is applied to simulate the nonlinear electron-photon interactions during shaped femtosecond laser pulse train ablation of diamond. Effects of the key pulse train parameters such as the pulse separation, spatial/temporal pulse energy distribution and pulse number per train on the electron excitation and energy absorption are discussed. The calculations show that photon-electron interactions and transient localized electron dynamics can be controlled including photon absorption, electron excitation, electron density, and free electron distribution by the ultrafast laser pulse train.
Zhao, Jing; Wang, Mei; Fu, Aiyun; Yang, Hongfang; Bu, Yuxiang
2015-08-03
We present an ab initio molecular dynamics (AIMD) simulation study into the transfer dynamics of an excess electron from its cavity-shaped hydrated electron state to a hydrated nucleobase (NB)-bound state. In contrast to the traditional view that electron localization at NBs (G/A/C/T), which is the first step for electron-induced DNA damage, is related only to dry or prehydrated electrons, and a fully hydrated electron no longer transfers to NBs, our AIMD simulations indicate that a fully hydrated electron can still transfer to NBs. We monitored the transfer dynamics of fully hydrated electrons towards hydrated NBs in aqueous solutions by using AIMD simulations and found that due to solution-structure fluctuation and attraction of NBs, a fully hydrated electron can transfer to a NB gradually over time. Concurrently, the hydrated electron cavity gradually reorganizes, distorts, and even breaks. The transfer could be completed in about 120-200 fs in four aqueous NB solutions, depending on the electron-binding ability of hydrated NBs and the structural fluctuation of the solution. The transferring electron resides in the π*-type lowest unoccupied molecular orbital of the NB, which leads to a hydrated NB anion. Clearly, the observed transfer of hydrated electrons can be attributed to the strong electron-binding ability of hydrated NBs over the hydrated electron cavity, which is the driving force, and the transfer dynamics is structure-fluctuation controlled. This work provides new insights into the evolution dynamics of hydrated electrons and provides some helpful information for understanding the DNA-damage mechanism in solution.
High Resolution Simulation of Beam Dynamics in Electron Linacs for Free Electron Lasers
Ryne, R.D.; Venturini, M.; Zholents, A.A.; Qiang, J.
2009-01-05
In this paper we report on large scale multi-physics simulation of beam dynamics in electron linacs for next generation free electron lasers (FELs). We describe key features of a parallel macroparticle simulation code including three-dimensional (3D) space-charge effects, short-range structure wake fields, longitudinal coherent synchrotron radiation (CSR) wake fields, and treatment of radiofrequency (RF) accelerating cavities using maps obtained from axial field profiles. A macroparticle up-sampling scheme is described that reduces the shot noise from an initial distribution with a smaller number of macroparticles while maintaining the global properties of the original distribution. We present a study of the microbunching instability which is a critical issue for future FELs due to its impact on beam quality at the end of the linac. Using parameters of a planned FEL linac at Lawrence Berkeley National Laboratory (LBNL), we show that a large number of macroparticles (beyond 100 million) is needed to control numerical shot noise that drives the microbunching instability. We also explore the effect of the longitudinal grid on simulation results. We show that acceptable results are obtained with around 2048 longitudinal grid points, and we discuss this in view of the spectral growth rate predicted from linear theory. As an application, we present results from simulations using one billion macroparticles of the FEL linac under design at LBNL. We show that the final uncorrelated energy spread of the beam depends not only on the initial uncorrelated energy spread but also depends strongly on the shape of the initial current profile. By using a parabolic initial current profile, 5 keV initial uncorrelated energy spread at 40 MeV injection energy, and improved linac design, those simulations demonstrate that a reasonable beam quality can be achieved at the end of the linac, with the final distribution having about 100 keV energy spread, 2.4 GeV energy, and 1.2 kA peak
Dynamics of emitting electrons in strong laser fields
Sokolov, Igor V.; Naumova, Natalia M.; Nees, John A.; Yanovsky, Victor P.; Mourou, Gerard A.
2009-09-15
A new derivation of the motion of a radiating electron is given, leading to a formulation that differs from the Lorentz-Abraham-Dirac equation and its published modifications. It satisfies the proper conservation laws. Particularly, it conserves the generalized momentum, eliminating the symmetry-breaking runaway solution. The equation allows a consistent calculation of the electron current, the radiation effect on the electron momentum, and the radiation itself, for a single electron or plasma electrons in strong electromagnetic fields. The equation is then applied to a simulation of a strong laser pulse interaction with a plasma target. Some analytical solutions are also provided.
Dynamics of interacting electrons under effect of a Morse potential.
Dos Santos, J L L; Sales, M O; Neto, A Ranciaro; de Moura, F A B F
2017-05-01
We consider interacting electrons moving in a nonlinear Morse lattice. We set the initial conditions as follows: electrons were initially localized at the center of the chain and a solitonic deformation was produced by an impulse excitation on the center of the chain. By solving quantum and classical equations for this system numerically, we found that a fraction of electronic wave function was trapped by the solitonic excitation, and trapping specificities depend on the degree of interaction among electrons. Also, there is evidence that the effective electron velocity depends on Coulomb interaction and electron-phonon coupling in a nontrivial way. This association is explained in detail along this work. In addition, we briefly discuss the dependence of our results with the type of initial condition we choose for the electrons and lattice.
Breaking of dynamical adiabaticity in direct laser acceleration of electrons
NASA Astrophysics Data System (ADS)
Robinson, A. P. L.; Arefiev, A. V.
2017-02-01
The interaction of an electron oscillating in an ion channel and irradiated by a plane electromagnetic wave is considered. It is shown that the interaction qualitatively changes with the increase of electron energy, as the oscillations across the channel become relativistic. The "square-wave-like" profile of the transverse velocity in the relativistic case enables breaking of the adiabaticity that precludes electron energy retention in the non-relativistic case. For an electron with a relativistic factor γ0, the adiabaticity breaks if ωL/ωp0≪√{γ0 } . Under these conditions, the kinetic energy acquired by the electron is retained once the interaction with the laser field ceases. This mechanism notably enables electron heating in regimes that do not require a resonant interaction between the initially oscillating electron and the laser electric field.
Shuvalov, Vladimir A
2007-06-01
It has been shown [V.A. Shuvalov, Quantum dynamics of electrons in many-electron atoms of biologically important compounds, Biochemistry (Mosc.) 68 (2003) 1333-1354; V.A. Shuvalov, Quantum dynamics of electrons in atoms of biologically important molecules, Uspekhi biologicheskoi khimii, (Pushchino) 44 (2004) 79-108] that the orbit angular momentum L of each electron in many-electron atoms is L=mVr=nPlanck's and similar to L for one-electron atom suggested by N. Bohr. It has been found that for an atom with N electrons the total electron energy equation E=-(Z(eff))(2)e(4)m/(2n(2)Planck's(2)N) is more appropriate for energy calculation than standard quantum mechanical expressions. It means that the value of L of each electron is independent of the presence of other electrons in an atom and correlates well to the properties of virtual photons emitted by the nucleus and creating a trap for electrons. The energies for elements of the 1st up to the 5th rows and their ions (total amount 240) of Mendeleev' Periodical table were calculated consistent with the experimental data (deviations in average were 5 x 10(-3)). The obtained equations can be used for electron dynamics calculations in molecules. For H(2) and H(2)(+) the interference of electron-photon orbits between the atoms determines the distances between the nuclei which are in agreement with the experimental values. The formation of resonance electron-photon orbit in molecules with the conjugated bonds, including chlorophyll-like molecules, appears to form a resonance trap for an electron with E values close to experimental data. Two mechanisms were suggested for non-barrier primary charge separation in reaction centers (RCs) of photosynthetic bacteria and green plants by using the idea of electron-photon orbit interference between the two molecules. Both mechanisms are connected to formation of the exciplexes of chlorophyll-like molecules. The first one includes some nuclear motion before exciplex formation, the
NASA Astrophysics Data System (ADS)
Winter, Bernd
2009-03-01
X-ray photoelectron spectroscopy measurements from a vacuum liquid microjet are performed to investigate the electronic structure of aqueous solutions. Here, focus is on the excited-state dynamics of chloride and hydroxide anions in water, following core-level excitation. A series of Cl^-(aq) charge-transfer-to-solvent (CTTS) states, and their ultrafast relaxation, on the time scale of the core hole, is identified from the occurrence of spectator Auger decay. Resonant oxygen 1s excitation of aqueous hydroxide, in contrast, leads to non-local decay, involving energy transfer into a neighboring water molecule. This channel is argued to arise from the weak hydrogen donor bond of OH^-(aq), and thus identifies a special transient hydration configuration, which can explain hydroxide's unusual and fast transport in water. Analogous measurements from pure water point to a similar relaxation channel, which is concluded from a strong isotope effect. The characteristic resonance spectral features are considerably stronger for H2O(aq) than for D2O(aq). As for OH^-(aq) the results can be understood in terms of energy transfer from the excited water molecule to a neighbor water molecule.
Dynamics of energetic electrons in nonstationary quasi-perpendicular shocks
NASA Astrophysics Data System (ADS)
Matsukiyo, Shuichi; Scholer, Manfred
2012-11-01
A one-dimensional full particle-in-cell (PIC) code is utilized to investigate energetic electron bursts produced at a nonstationary quasi-perpendicular shock. A number of electrons are intermittently energized by interacting with nonstationary electromagnetic fields in the shock front. Some of the energetic electrons are reflected at the shock and form an upstream non-thermal population. The reflection process is strongly affected by the non-coplanar magnetic field component which is temporarily rather strong in the transition region of a highly nonstationary shock. Oblique whistler waves in the transition region influence the distribution function of the reflected electrons. Waves excited by the modified two-stream instability may pitch angle scatter the electrons and thus blur the loss cone feature of the reflected electrons. Dispersive standing whistler waves are also emitted locally in the foot even when a Mach number exceeds a critical value. These whistler waves may also scatter the electrons to blur the loss cone. Furthermore, the whistler waves produce clumps of the reflected electrons in a phase space. Some electrons are trapped by the ion holes produced downstream as a remnant of a self-reformation process of the shock front and accelerated through a drift mechanism. It is also discussed how physical quantities associated with the reflected electrons observed upstream of the shock can give information about the shock front nonstationarity as well as about local small scale wave activities in the transition region.
NASA Astrophysics Data System (ADS)
Vacher, Morgane; Bearpark, Michael J.; Robb, Michael A.; Malhado, João Pedro
2017-02-01
Knowledge about the electronic motion in molecules is essential for our understanding of chemical reactions and biological processes. The advent of attosecond techniques opens up the possibility to induce electronic motion, observe it in real time, and potentially steer it. A fundamental question remains the factors influencing electronic decoherence and the role played by nuclear motion in this process. Here, we simulate the dynamics upon ionization of the polyatomic molecules paraxylene and modified bismethylene-adamantane, with a quantum mechanical treatment of both electron and nuclear dynamics using the direct dynamics variational multiconfigurational Gaussian method. Our simulations give new important physical insights about the expected decoherence process. We have shown that the decoherence of electron dynamics happens on the time scale of a few femtoseconds, with the interplay of different mechanisms: the dephasing is responsible for the fast decoherence while the nuclear overlap decay may actually help maintain it and is responsible for small revivals.
Electron nuclear dynamics of LiH and HF in an intense laser field
NASA Astrophysics Data System (ADS)
Broeckhove, J.; Coutinho-Neto, M. D.; Deumens, E.; Öhrn, Y.
1997-12-01
The electron nuclear dynamics theory (END) extended to include a time-dependent external field is briefly described. The dynamical equations, in addition to the full electron nuclear coupling terms, now also contain the interactions of both the nuclei and the electrons with the external field. This extended END theory is applied to the study of vibrational excitations of the simple diatomics HF and LiH. The END results using an intense infrared laser field are compared with those of molecular dynamics as well as those from quantum wave-packet calculations. While the effect of the nonadiabatic electron-nuclear coupling terms on the vibrational dynamics is negligible for the chosen application, the electron-field coupling has a significant impact.
Effects of inner electrons on atomic strong-field-ionization dynamics
NASA Astrophysics Data System (ADS)
Rapp, J.; Bauer, D.
2014-03-01
The influence of inner electrons on the ionization dynamics in strong laser fields is investigated in a wavelength regime where the inner electron dynamics is usually assumed to be negligible. The role of inner electrons is of particular interest for the application of frozen-core approximations and pseudopotentials in time-dependent density functional theory (TDDFT) and the single-active-electron (SAE) approximation in strong-field laser physics. Results of TDDFT and SAE calculations are compared with exact ones obtained by the numerical ab initio solution of the three-electron time-dependent Schrödinger equation for a lithium model atom. It is found that dynamical antiscreening, i.e., a particular form of dynamical core polarization, may substantially alter the ionization rate in the single-photon regime. Requirements for the validity of the approximations in the single and multiphoton ionization domain are identified.
Khalilpour, H.; Moslehi-Fard, M.; Foroutan, G.; Li, B.; Robinson, P. A.
2009-07-15
The dynamics of a beam of hot electrons traveling through a cold plasma and the generation of Langmuir waves are investigated in the presence of a nonthermal tail of electrons in the background distribution function. Using quasilinear simulations, it is shown that in the presence of the nonthermal electrons, the relaxation of the beam distribution function in velocity space is retarded and the Langmuir waves are strongly damped at low velocities. The average velocity of beam propagation is almost constant but its magnitude is larger in the presence of nonthermal electrons than their absence. It is found that the self-similarity of the system is preserved in the presence of nonthermal electrons. The effects of nonthermal electrons on the evolution of gas-dynamical parameters of the beam, including the height of plateau in the beam distribution function, its upper and lower velocity boundaries, and beam velocity width, are also studied. It is found that initially the values of the upper and lower velocity boundaries are almost unaltered, but at large times the lower (upper) boundary velocity is larger (smaller) in the presence of nonthermal electrons than without the nonthermal electrons.
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.
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.
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
Dynamics of electron injection in a laser-wakefield accelerator
NASA Astrophysics Data System (ADS)
Xu, J.; Buck, A.; Chou, S.-W.; Schmid, K.; Shen, B.; Tajima, T.; Kaluza, M. C.; Veisz, L.
2017-08-01
The detailed temporal evolution of the laser-wakefield acceleration process with controlled injection, producing reproducible high-quality electron bunches, has been investigated. The localized injection of electrons into the wakefield has been realized in a simple way—called shock-front injection—utilizing a sharp drop in plasma density. Both experimental and numerical results reveal the electron injection and acceleration process as well as the electron bunch's temporal properties. The possibility to visualize the plasma wave gives invaluable spatially resolved information about the local background electron density, which in turn allows for an efficient suppression of electron self-injection before the controlled process of injection at the sharp density jump. Upper limits for the electron bunch duration of 6.6 fs FWHM, or 2.8 fs (r.m.s.) were found. These results indicate that shock-front injection not only provides stable and tunable, but also few-femtosecond short electron pulses for applications such as ultrashort radiation sources, time-resolved electron diffraction or for the seeding of further acceleration stages.
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
Electron and Ion Dynamics of the Solar Wind Interaction with a Weakly Outgassing Comet.
Deca, Jan; Divin, Andrey; Henri, Pierre; Eriksson, Anders; Markidis, Stefano; Olshevsky, Vyacheslav; Horányi, Mihály
2017-05-19
Using a 3D fully kinetic approach, we disentangle and explain the ion and electron dynamics of the solar wind interaction with a weakly outgassing comet. We show that, to first order, the dynamical interaction is representative of a four-fluid coupled system. We self-consistently simulate and identify the origin of the warm and suprathermal electron distributions observed by ESA's Rosetta mission to comet 67P/Churyumov-Gerasimenko and conclude that a detailed kinetic treatment of the electron dynamics is critical to fully capture the complex physics of mass-loading plasmas.
The multi-configuration electron-nuclear dynamics method applied to LiH.
Ulusoy, Inga S; Nest, Mathias
2012-02-07
The multi-configuration electron-nuclear dynamics (MCEND) method is a nonadiabatic quantum dynamics approach to the description of molecular processes. MCEND is a combination of the multi-configuration time-dependent Hartree (MCTDH) method for atoms and its antisymmetrized equivalent MCTDHF for electrons. The purpose of this method is to simultaneously describe nuclear and electronic wave packets in a quantum dynamical way, without the need to calculate potential energy surfaces and diabatic coupling functions. In this paper we present first exemplary calculations of MCEND applied to the LiH molecule, and discuss computational and numerical details of our implementation.
Plasma ion dynamics and beam formation in electron cyclotron resonance ion sources
Mascali, D.; Neri, L.; Miracoli, R.; Gammino, S.; Celona, L.; Ciavola, G.; Gambino, N.; Chikin, S.
2010-02-15
In electron cyclotron resonance ion sources it has been demonstrated that plasma heating may be improved by means of different microwave to plasma coupling mechanisms, including the ''frequency tuning'' and the ''two frequency heating''. These techniques affect evidently the electron dynamics, but the relationship with the ion dynamics has not been investigated in details up to now. Here we will try to outline these relations: through the study of ion dynamics we may try to understand how to optimize the electron cyclotron resonance ion sources brightness. A simple model of the ion confinement and beam formation will be presented, based on particle-in-cell and single particle simulations.
NASA Astrophysics Data System (ADS)
Winney, Alexander H.; Lee, Suk Kyoung; Lin, Yun Fei; Liao, Qing; Adhikari, Pradip; Basnayake, Gihan; Schlegel, H. Bernhard; Li, Wen
2017-09-01
With a novel three-dimensional electron-electron coincidence imaging technique and two-electron angular streaking method, we show that the emission time delay between two electrons can be measured from tens of attoseconds to more than 1 fs. Surprisingly, in benzene, the double ionization rate decays as the time delay between the first and second electron emission increases during the first 500 as. This is further supported by the decay of the Coulomb repulsion in the direction perpendicular to the laser polarization. This result reveals that laser-induced electron correlation plays a major role in strong field double ionization of benzene driven by a nearly circularly polarized field.
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.
Graphically Mapping Electronic Discussions: Understanding Online Conversational Dynamics
ERIC Educational Resources Information Center
Duncan-Howell, Jennifer
2008-01-01
Transcripts of electronic discussions have traditionally been examined via the use of conversational analysis techniques. Coding such transcripts provides rich data regarding the content and nature of the discussions that take place. However, understanding the content of a message is not limited to the actual message itself. An electronic message…
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
Simulation of nonlinear electron dynamics in tetramer metal-carbon nanoclusters
NASA Astrophysics Data System (ADS)
Yaltychenko, O. V.; Kanarovskii, E. Yu.; Baranov, S. A.; Gorinchoy, N. N.
2016-12-01
In this paper the simulation of nonlinear electron dynamics in the metal-carbon tetramer nanocluster was carried out using the modified approach in a framework of jellium model. The model Hamiltonian includes the terms accounting the action of external electric field and the interaction between the tunneling electron with the vibrational modes of carbon shell. As a result, the system of differential equations for the amplitudes of the electron localization probability at the MCN centers was obtained and then at the various sets of model parameters it was solved numerically. The different regimes in the electron localization dynamics were revealed and the control role of the electric field was shown.
Li, Run-Ze; Zhu, Pengfei; Chen, Long; Chen, Jie E-mail: jzhang1@sjtu.edu.cn; Sheng, Zheng-Ming; Zhang, Jie E-mail: jzhang1@sjtu.edu.cn; Cao, Jianming
2014-05-14
The ultrafast structure dynamics and surface transient electric field, which are concurrently induced by laser excited electrons of an aluminum nanofilm, have been investigated simultaneously by the same transmission electron diffraction patterns. These two processes are found to be significantly different and distinguishable by tracing the time dependent changes of electron diffraction and deflection angles, respectively. This study also provides a practical means to evaluate simultaneously the effect of transient electric field during the study of structural dynamics under low pump fluence by transmission ultrafast electron diffraction.
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.
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.
Determining the locus for photocarrier recombination in dye-sensitized solar cells
NASA Astrophysics Data System (ADS)
Zhu, Kai; Schiff, E. A.; Park, N.-G.; van de Lagemaat, J.; Frank, A. J.
2002-01-01
We present intensity-modulated photocurrent and infrared transmittance measurements on dye-sensitized solar cells based on a mesoporous titania (TiO2) matrix immersed in an iodine-based electrolyte. Under short-circuit conditions, we show that an elementary analysis accurately relates the two measurements. Under open-circuit conditions, infrared transmittance, and photovoltage measurements yield information on the characteristic depth at which electrons recombine with ions (the "locus of recombination"). For one particular series of samples recombination occurred near the substrate supporting the titania film, as opposed to homogeneously throughout the film.
NASA Astrophysics Data System (ADS)
Shiryaev, A. A.; Hinks, J.; Marks, N.; Greaves, G.; Donnelly, S.; Fisenko, A. V.; Kiwi, M.
2016-08-01
We present results of the first investigation of the Xe implantation process into nanodiamonds of various sizes studied in situ in transmission electron microscope (TEM), complemented by advanced molecular dynamics simulations.
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.
NASA Astrophysics Data System (ADS)
Swartz, C. H.; Zaunbrecher, K. N.; Sohal, S.; LeBlanc, E. G.; Edirisooriya, M.; Ogedengbe, O. S.; Petersen, J. E.; Jayathilaka, P. A. R. D.; Myers, T. H.; Holtz, M. W.; Barnes, T. M.
2016-10-01
CdSeTe/CdMgTe double heterostructures were produced with both n-type and unintentionally doped absorber layers. Measurements of the dependence of photoluminescence intensity on excitation intensity were carried out, as well as measurements of time-resolved photoluminescence decay after an excitation pulse. It was found that decay times under very low photon injection conditions are dominated by a non-radiative Shockley-Read-Hall process described using a recombination center with an asymmetric capture cross section, where the cross section for holes is larger than that for electrons. As a result of the asymmetry, the center effectively extends photoluminescence decay by a hole trapping phenomenon. A reduction in electron capture cross section appeared at doping densities over 1016cm-3. An analysis of the excitation intensity dependence of room temperature photoluminescence revealed a strong relationship with doping concentration. This allows estimates of the carrier concentration to be made through a non-destructive optical method. Iodine was found to be an effective n-type dopant for CdTe, allowing controllable carrier concentrations without an increased rate of non-radiative recombination.
Swartz, C. H.; Zaunbrecher, Katherine N.; Sohal, S.; LeBlanc, E. G.; Edirisooriya, M.; Ogedengbe, O. S.; Petersen, J. E.; Jayathilaka, P. A. R. D.; Myers, T. H.; Holtz, M. W.; Barnes, Teresa M.
2016-10-28
CdSeTe/CdMgTe double heterostructures were produced with both n-type and unintentionally doped absorber layers. Measurements of the dependence of photoluminescence intensity on excitation intensity were carried out, as well as measurements of time-resolved photoluminescence decay after an excitation pulse. It was found that decay times under very low photon injection conditions are dominated by a non-radiative Shockley-Read-Hall process described using a recombination center with an asymmetric capture cross section, where the cross section for holes is larger than that for electrons. As a result of the asymmetry, the center effectively extends photoluminescence decay by a hole trapping phenomenon. A reduction in electron capture cross section appeared at doping densities over 10^16cm-3. An analysis of the excitation intensity dependence of room temperature photoluminescence revealed a strong relationship with doping concentration. This allows estimates of the carrier concentration to be made through a non-destructive optical method. Iodine was found to be an effective n-type dopant for CdTe, allowing controllable carrier concentrations without an increased rate of non-radiative recombination.
Swartz, Craig H.; Zaunbrecher, K. N.; Sohal, S.; ...
2016-10-28
CdSeTe/CdMgTe double heterostructures were produced with both n-type and unintentionally doped absorber layers. Measurements of the dependence of photoluminescence intensity on excitation intensity were carried out, as well as measurements of time-resolved photoluminescence decay after an excitation pulse. It was found that decay times under very low photon injection conditions are dominated by a non-radiative Shockley-Read-Hall process described using a recombination center with an asymmetric capture cross section, where the cross section for holes is larger than that for electrons. As a result of the asymmetry, the center effectively extends photoluminescence decay by a hole trapping phenomenon. A reduction inmore » electron capture cross section appeared at doping densities over 1016cm-3. An analysis of the excitation intensity dependence of room temperature photoluminescence revealed a strong relationship with doping concentration. Here, this allows estimates of the carrier concentration to be made through a non-destructive optical method. Iodine was found to be an effective n-type dopant for CdTe, allowing controllable carrier concentrations without an increased rate of non-radiative recombination.« less
Amorphous two-dimensional black phosphorus with exceptional photocarrier transport properties
NASA Astrophysics Data System (ADS)
Bellus, Matthew Z.; Yang, Zhibin; Hao, Jianhua; Lau, Shu Ping; Zhao, Hui
2017-06-01
Recently, two-dimensional materials have been extensively studied. Due to the reduced dielectric screening and confinement of electrons in two dimensions, these materials show dramatically different electronic and optical properties from their bulk counterparts. So far, studies on two-dimensional materials have mainly focused on crystalline materials. Here we report studies of atomically thin amorphous black phosphorus, as the first two-dimensional amorphous material. Spatially and temporally resolved pump-probe measurements show that large-area and uniform atomic layers of amorphous black phosphorus, synthesized at low temperature, possess a long exciton lifetime of about 400 ps, a room-temperature exciton diffusion coefficient of 5 cm2 s-1, which is at least two orders of magnitude larger than amorphous silicon, and an exciton mobility of about 200 cm2 V-1 s-1. We also deduce from these values an exciton mean free time of 50 fs, a mean free path of 5 nm, and a diffusion length of 450 nm. These results suggest that amorphous black phosphorus can be potentially used in low-cost optoelectronic devices.
Nonlinear dynamics study of the SIBERIA-2 electron storage ring
Levichev, E.; Sajaev, V.
1995-09-01
Dedicated {ital SR} sources with minimized beam emittance possess a great deal of chromaticity. For the latter to be compensated, strong sextupole lenses producing a nonlinear influence on the beam dynamics and giving rise to the limitation of the motion stability area are employed. The paper presents the results concerning the single-particle nonlinear dynamics of SIBERIA-2. We have applied a perturbation theory based on canonical Lie transforms. It enables us to study high order perturbation effects.
Dynamical enhanced electron emission and discharges at contaminated surfaces
NASA Astrophysics Data System (ADS)
Halbritter, J.
1986-01-01
Broad-area electrodes show electron emission already at electric field strengths F≈107 V/m. This enhanced field emission (EFE) occurs only for contaminated surfaces. EFE is accompanied by photon emission and gas desorption yielding finally discharges. EFE is caused by dust and contaminants initiating the following effects: an electron is stochastically emitted in a trigger zone the electron gains energy ΔE≃eΔxF * which excites electronic states which relax by the emission of electrons, photons, and atoms where the positive charges left behind enhance F *= βF (β≫1) initiating so an electron avalanche, i.e., a high conductivity channel. Because of charge migration and neutralization, this avalanche has a life time. This pulsating EFE is accompanied by light emission and gas desorption yielding finally a gas cloud and a discharge. The pulsating, self-sustained EFE has the same root as: the enhanced secondary emission found first by Malter the conductivity switching exhibited by thin (≈ 1 μm) layers of semiconductors or insulators the normal cathode fall and the firing-wave instability in neurodynamics.
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.
Electron-Nuclear Dynamics of collision processes: Charge exchange and energy loss
NASA Astrophysics Data System (ADS)
Cabrera-Trujillo, Remigio; Sabin, John R.; Öhrn, Yngve; Deumens, Erik
2004-03-01
We present the Electron-Nuclear Dynamics (END) method for the study of time-dependent scattering processes. The END is a general approach for treating time-dependent problems which includes the dynamics of electrons and nuclei simultaneously by considering the full electron-nuclear coupling in the system and thus eliminates the necessity of constructing potential-energy surfaces. The theory approximates the time dependent Schrödinger equation starting from the time dependent variational principle by deriving a Hamiltonian dynamical system for time dependent nuclear and electronic wave function parameters. The wave function is described in a coherent state manifold, which leads to a system of Hamilton's equations of motion. Emphasis is put on electron exchange, differential cross section and energy loss (stopping cross section) of collision of ions, atoms and molecules involving H, He, C, N, O, and Ne atoms. We compare our results to available experimental data.
He, Z-H; Beaurepaire, B; Nees, J A; Gallé, G; Scott, S A; Pérez, J R Sánchez; Lagally, M G; Krushelnick, K; Thomas, A G R; Faure, J
2016-11-08
Recent progress in laser wakefield acceleration has led to the emergence of a new generation of electron and X-ray sources that may have enormous benefits for ultrafast science. These novel sources promise to become indispensable tools for the investigation of structural dynamics on the femtosecond time scale, with spatial resolution on the atomic scale. Here, we demonstrate the use of laser-wakefield-accelerated electron bunches for time-resolved electron diffraction measurements of the structural dynamics of single-crystal silicon nano-membranes pumped by an ultrafast laser pulse. In our proof-of-concept study, we resolve the silicon lattice dynamics on a picosecond time scale by deflecting the momentum-time correlated electrons in the diffraction peaks with a static magnetic field to obtain the time-dependent diffraction efficiency. Further improvements may lead to femtosecond temporal resolution, with negligible pump-probe jitter being possible with future laser-wakefield-accelerator ultrafast-electron-diffraction schemes.
NASA Astrophysics Data System (ADS)
He, Z.-H.; Beaurepaire, B.; Nees, J. A.; Gallé, G.; Scott, S. A.; Pérez, J. R. Sánchez; Lagally, M. G.; Krushelnick, K.; Thomas, A. G. R.; Faure, J.
2016-11-01
Recent progress in laser wakefield acceleration has led to the emergence of a new generation of electron and X-ray sources that may have enormous benefits for ultrafast science. These novel sources promise to become indispensable tools for the investigation of structural dynamics on the femtosecond time scale, with spatial resolution on the atomic scale. Here, we demonstrate the use of laser-wakefield-accelerated electron bunches for time-resolved electron diffraction measurements of the structural dynamics of single-crystal silicon nano-membranes pumped by an ultrafast laser pulse. In our proof-of-concept study, we resolve the silicon lattice dynamics on a picosecond time scale by deflecting the momentum-time correlated electrons in the diffraction peaks with a static magnetic field to obtain the time-dependent diffraction efficiency. Further improvements may lead to femtosecond temporal resolution, with negligible pump-probe jitter being possible with future laser-wakefield-accelerator ultrafast-electron-diffraction schemes.
Vibrational Modes and the Dynamic Solvent Effect in Electron and Proton Transfer
1992-05-18
Vibrational Modes and the Dynamic Solvent Effect in Electron and Proton Transfer Paul F. Barbara, Gilbert C. Walker and Terrance P. Smith Science, 256, 975...Copies of the form are available from cognizant grant of contract administrator 92-13720i|i|Hfl|fl MARTICLES Vibrational Modes and the Dynamic Solvent...photosynthetic systems. (X + AGO)’ The kinetic impact of high-frequency In order to set the stage for a discussion A = (1) vibrational modes in electron
Littarru, Paolo
2007-01-01
After an overview about the criteria of odour nuisance in different technical laws, about electronic noses analysers and about dynamic olfactometry, in the present paper the authors describe an application of dynamic olfactometry in combination with the determinations of electronic noses. The coordination of the two approaches permits optimisation of the advantages offered by both methods to the measurable and objective evaluation of the odour nuisance from waste treatment plants and chemical plants.
Dynamics of the Chemistry of Electronically Excited Atoms in Defined Quantum States.
1978-05-01
laser development . In essence, this research concerns itself with the elucidation of the role of electronic energy in affecting the chemistry or photochemistry of excited halogen atoms and molecules. While much is known about the dynamics of chemical and physical processes which are carried out on the lowest potential energy hypersurface correlating with reactants and products in their electronic ground state, relatively little is known about the dynamics of such phenomena as energy transfer and chemical reactivity on higher-lying potential
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.
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
Target surface area effects on hot electron dynamics from high intensity laser–plasma interactions
Zulick, C.; Raymond, A.; McKelvey, A.; ...
2016-06-15
Reduced surface area targets were studied using an ultra-high intensity femtosecond laser in order to determine the effect of electron sheath field confinement on electron dynamics. X-ray emission due to energetic electrons was imaged using a Kα imaging crystal. Electrons were observed to travel along the surface of wire targets, and were slowed mainly by the induced fields. Targets with reduced surface areas were correlated with increased hot electron densities and proton energies. Furthermore, Hybrid Vlasov–Fokker–Planck simulations demonstrated increased electric sheath field strength in reduced surface area targets.
Comparison of electron and hole charge-discharge dynamics in germanium nanocrystal flash memories
NASA Astrophysics Data System (ADS)
Akca, Imran B.; Dâna, Aykutlu; Aydinli, Atilla; Turan, Rasit
2008-02-01
Electron and hole charge and discharge dynamics are studied on plasma enhanced chemical vapor deposition grown metal-oxide-silicon germanium nanocrystal flash memory devices. Electron and hole charge and discharge currents are observed to differ significantly and depend on annealing conditions chosen for the formation of nanocrystals. At low annealing temperatures, holes are seen to charge slower but to escape faster than electrons. They discharge slower than electrons when annealing temperatures are raised. The results suggest that discharge currents are dominated by the interface layer acting as a quantum well for holes and by direct tunneling for elec-trons.
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
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
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.
Adequacy of damped dynamics to represent the electron-phonon interaction in solids
Caro, A.; Correa, A. A.; Tamm, A.; ...
2015-10-16
Time-dependent density functional theory and Ehrenfest dynamics are used to calculate the electronic excitations produced by a moving Ni ion in a Ni crystal in the case of energetic MeV range (electronic stopping power regime), as well as thermal energy meV range (electron-phonon interaction regime). Results at high energy compare well to experimental databases of stopping power, and at low energy the electron-phonon interaction strength determined in this way is very similar to the linear response calculation and experimental measurements. This approach to electron-phonon interaction as an electronic stopping process provides the basis for a unified framework to perform classicalmore » molecular dynamics of ion-solid interaction with ab initio type nonadiabatic terms in a wide range of energies.« less
Adequacy of damped dynamics to represent the electron-phonon interaction in solids
Caro, A.; Correa, A. A.; Tamm, A.; ...
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
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…
Relaxation dynamics of the electronically excited vanadium Met-Car cluster
NASA Astrophysics Data System (ADS)
Leskiw, B. D.; Knappenberger, K. L.; Castleman, A. W., Jr.
2002-11-01
The relaxation dynamics of the vanadium Met-Car cluster, V8C12, excited electronically using femtosecond laser pulses of various wavelengths, is reported. Particular attention is focused on time-resolved measurements in the vicinity of 2 eV where experimental evidence of an electronic state is acquired.
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.
Adjoint Fokker-Planck equation and runaway electron dynamics
NASA Astrophysics Data System (ADS)
Liu, Chang; Brennan, Dylan P.; Bhattacharjee, Amitava; Boozer, Allen H.
2016-01-01
The adjoint Fokker-Planck equation method is applied to study the runaway probability function and the expected slowing-down time for highly relativistic runaway electrons, including the loss of energy due to synchrotron radiation. In direct correspondence to Monte Carlo simulation methods, the runaway probability function has a smooth transition across the runaway separatrix, which can be attributed to effect of the pitch angle scattering term in the kinetic equation. However, for the same numerical accuracy, the adjoint method is more efficient than the Monte Carlo method. The expected slowing-down time gives a novel method to estimate the runaway current decay time in experiments. A new result from this work is that the decay rate of high energy electrons is very slow when E is close to the critical electric field. This effect contributes further to a hysteresis previously found in the runaway electron population.
Adjoint Fokker-Planck equation and runaway electron dynamics
Liu, Chang; Brennan, Dylan P.; Bhattacharjee, Amitava; Boozer, Allen H.
2016-01-15
The adjoint Fokker-Planck equation method is applied to study the runaway probability function and the expected slowing-down time for highly relativistic runaway electrons, including the loss of energy due to synchrotron radiation. In direct correspondence to Monte Carlo simulation methods, the runaway probability function has a smooth transition across the runaway separatrix, which can be attributed to effect of the pitch angle scattering term in the kinetic equation. However, for the same numerical accuracy, the adjoint method is more efficient than the Monte Carlo method. The expected slowing-down time gives a novel method to estimate the runaway current decay time in experiments. A new result from this work is that the decay rate of high energy electrons is very slow when E is close to the critical electric field. This effect contributes further to a hysteresis previously found in the runaway electron population.
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.
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.
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
Fujihashi, Yuta; Ishizaki, Akihito
2016-02-04
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.
Attosecond x-ray pulses for molecular electronic dynamics
NASA Astrophysics Data System (ADS)
Abel, Mark Joseph
Attosecond pulses are opening a wide new field on the border of chemistry and physics. They offer the opportunity to initiate and probe electronic rearrangement of atoms, molecules, solids and clusters on the natural timescale of the electron motion. This thesis is about making and measuring attosecond pulses, with the ultimate goal of applying attosecond spectroscopy to molecules. In chapter 1, attosecond spectroscopy is reviewed in general. The applications of attosecond pulses to atoms and molecules, including successful experiments and theoretical predictions, are discussed. In chapter 2, techniques for making and measuring attosecond radiation are presented. This chapter focuses on high harmonic generation from tabletop laser sources, since synchrotron- and free-electron laser-based techniques are not yet experimentally demonstrated. Chapters 3 and 4 discuss in detail the laboratory setup for attosecond pulse generation, including the laser source, optical diagnostics, and attosecond delay line. The attosecond control of free electron motion with few-cycle laser pulses is presented in chapter 5. There, the carrier-envelope phase (CEP), and thus the attosecond temporal evolution of the laser field, leads to quantum interferences between free electron wavefunctions and lends control over the direction of electron emission. Attosecond pulse production is achieved in chapter 6 by gating harmonic generation on the leading edge of the driving laser pulse. The gate mechanism is shown to rely on the macroscopic ionization of the harmonic generation medium. This final chapter also demonstrates a new technique for assessing attosecond pulse temporal structure based on the inversion of the driving laser field in the laboratory frame of reference, called CEP-scanning.
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.
Dynamical Cooper pairing in nonequilibrium electron-phonon systems
NASA Astrophysics Data System (ADS)
Knap, Michael; Babadi, Mehrtash; Refael, Gil; Martin, Ivar; Demler, Eugene
2016-12-01
We analyze Cooper pairing instabilities in strongly driven electron-phonon systems. The light-induced nonequilibrium state of phonons results in a simultaneous increase of the superconducting coupling constant and the electron scattering. We demonstrate that the competition between these effects leads to an enhanced superconducting transition temperature in a broad range of parameters. Our results may explain the observed transient enhancement of superconductivity in several classes of materials upon irradiation with high intensity pulses of terahertz light, and may pave new ways for engineering high-temperature light-induced superconducting states.
Electron-Spin Dynamics in Strongly Correlated Metals
NASA Astrophysics Data System (ADS)
Dóra, Balázs; Simon, Ferenc
2009-04-01
The temperature dependence of the electron-spin lifetime T1 and the g factor are anomalous in alkali fullerides (K,Rb)3C60, which cannot be explained by the canonical Elliott-Yafet theory. These materials are archetypes of strongly correlated and narrow band metals. We introduce the concept of a “complex electron-spin resonance frequency shift” to treat these measurables in a unified manner within the Kubo formalism. The theory is applicable for metals with nearly degenerate conduction bands and large momentum scattering even with an anomalous temperature dependence and sizable residual value.
Dynamical Cooper pairing in nonequilibrium electron-phonon systems
Knap, Michael; Babadi, Mehrtash; Refael, Gil; Martin, Ivar; Demler, Eugene
2016-12-08
In this paper, we analyze Cooper pairing instabilities in strongly driven electron-phonon systems. The light-induced nonequilibrium state of phonons results in a simultaneous increase of the superconducting coupling constant and the electron scattering. We demonstrate that the competition between these effects leads to an enhanced superconducting transition temperature in a broad range of parameters. Finally, our results may explain the observed transient enhancement of superconductivity in several classes of materials upon irradiation with high intensity pulses of terahertz light, and may pave new ways for engineering high-temperature light-induced superconducting states.
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.
Buffat, Philippe André
2003-02-15
High-resolution transmission electron microscopy shows that metal nanoparticles sinter within a fraction of a second under an electron beam at 'room temperature' as long as classical models of thermal equilibrium apply. Images exhibit crystal planes that change in orientation with time as if the particle was undergoing melting and resolidification processes. We explore whether these dynamical effects are the result of heating or transformation effects in the electron microscope or quantum fluctuations in small systems.
Target Surface Area Effects on Hot Electron Dynamics from High Intensity Laser-Plasma Interactions
2016-08-19
field Abstract Reduced surface area targets were studied using an ultra- high intensity femtosecond laser in order to determine the effect of electron...New J. Phys. 18 (2016) 063020 doi:10.1088/1367-2630/18/6/063020 PAPER Target surface area effects on hot electron dynamics from high intensity laser...the higher intensity interaction, asymmetric electron current around the hexagonal loop (b)was attributed to field induced current along parallel wire
Measuring Conformational Dynamics of Single Biomolecules Using Nanoscale Electronic Devices
NASA Astrophysics Data System (ADS)
Akhterov, Maxim V.; Choi, Yongki; Sims, Patrick C.; Olsen, Tivoli J.; Gul, O. Tolga; Corso, Brad L.; Weiss, Gregory A.; Collins, Philip G.
2014-03-01
Molecular motion can be a rate-limiting step of enzyme catalysis, but motions are typically too quick to resolve with fluorescent single molecule techniques. Recently, we demonstrated a label-free technique that replaced fluorophores with nano-electronic circuits to monitor protein motions. The solid-state electronic technique used single-walled carbon nanotube (SWNT) transistors to monitor conformational motions of a single molecule of T4 lysozyme while processing its substrate, peptidoglycan. As lysozyme catalyzes the hydrolysis of glycosidic bonds, two protein domains undergo 8 Å hinge bending motion that generates an electronic signal in the SWNT transistor. We describe improvements to the system that have extended our temporal resolution to 2 μs . Electronic recordings at this level of detail directly resolve not just transitions between open and closed conformations but also the durations for those transition events. Statistical analysis of many events determines transition timescales characteristic of enzyme activity and shows a high degree of variability within nominally identical chemical events. The high resolution technique can be readily applied to other complex biomolecules to gain insights into their kinetic parameters and catalytic function.
Dynamics of Dissociative Electron Attachment to Uracil and Furane
NASA Astrophysics Data System (ADS)
Fonseca Dos Santos, Samantha; Douguet, Nicolas; Orel, Ann; Rescigno, Thomas
2016-05-01
We present the results of a theoretical study of dissociative electron attachment (DEA) to Uracil and Furan. In both cases we will present calculated angular distributions based on analysis of the entrance amplitudes obtained from the results of complex Kohn scattering calculations. For uracil, we will compare our results with available experimentally measured angular distributions obtained using the COLTRIMS method.
Dynamics of a single-atom electron pump.
van der Heijden, J; Tettamanzi, G C; Rogge, S
2017-03-15
Single-electron pumps based on isolated impurity atoms have recently been experimentally demonstrated. In these devices the Coulomb potential of an atom creates a localised electron state with a large charging energy and considerable orbital level spacings, enabling robust charge capturing processes. In contrast to the frequently used gate-defined quantum dot pumps, which experience a strongly time-dependent potential, the confinement potential in these single-atom pumps is hardly affected by the periodic driving of the system. Here we describe the behaviour and performance of an atomic, single parameter, electron pump. This is done by considering the loading, isolating and unloading of one electron at the time, on a phosphorous atom embedded in a silicon double gate transistor. The most important feature of the atom pump is its very isolated ground state, which is populated through the fast loading of much higher lying excited states and a subsequent fast relaxation process. This leads to a substantial increase in pumping accuracy, and is opposed to the adverse role of excited states observed for quantum dot pumps due to non-adiabatic excitations. The pumping performance is investigated as a function of dopant position, revealing a pumping behaviour robust against the expected variability in atomic position.
Dynamics of a single-atom electron pump
NASA Astrophysics Data System (ADS)
van der Heijden, J.; Tettamanzi, G. C.; Rogge, S.
2017-03-01
Single-electron pumps based on isolated impurity atoms have recently been experimentally demonstrated. In these devices the Coulomb potential of an atom creates a localised electron state with a large charging energy and considerable orbital level spacings, enabling robust charge capturing processes. In contrast to the frequently used gate-defined quantum dot pumps, which experience a strongly time-dependent potential, the confinement potential in these single-atom pumps is hardly affected by the periodic driving of the system. Here we describe the behaviour and performance of an atomic, single parameter, electron pump. This is done by considering the loading, isolating and unloading of one electron at the time, on a phosphorous atom embedded in a silicon double gate transistor. The most important feature of the atom pump is its very isolated ground state, which is populated through the fast loading of much higher lying excited states and a subsequent fast relaxation process. This leads to a substantial increase in pumping accuracy, and is opposed to the adverse role of excited states observed for quantum dot pumps due to non-adiabatic excitations. The pumping performance is investigated as a function of dopant position, revealing a pumping behaviour robust against the expected variability in atomic position.
Quantum ergodicity breaking in semi-classical electron transfer dynamics.
Goychuk, Igor
2017-01-25
Can the statistical properties of single-electron transfer events be correctly predicted within a common equilibrium ensemble description? This fundamental in nanoworld question of ergodic behavior is scrutinized within a very basic semi-classical curve-crossing problem. It is shown that in the limit of non-adiabatic electron transfer (weak tunneling) well-described by the Marcus-Levich-Dogonadze (MLD) rate the answer is yes. However, in the limit of the so-called solvent-controlled adiabatic electron transfer, a profound breaking of ergodicity occurs. Namely, a common description based on the ensemble reduced density matrix with an initial equilibrium distribution of the reaction coordinate is not able to reproduce the statistics of single-trajectory events in this seemingly classical regime. For sufficiently large activation barriers, the ensemble survival probability in a state remains nearly exponential with the inverse rate given by the sum of the adiabatic curve crossing (Kramers) time and the inverse MLD rate. In contrast, near to the adiabatic regime, the single-electron survival probability is clearly non-exponential, even though it possesses an exponential tail which agrees well with the ensemble description. Initially, it is well described by a Mittag-Leffler distribution with a fractional rate. Paradoxically, the mean transfer time in this classical on the ensemble level regime is well described by the inverse of the nonadiabatic quantum tunneling rate on a single particle level. An analytical theory is developed which perfectly agrees with stochastic simulations and explains our findings.
Dynamics of a single-atom electron pump
van der Heijden, J.; Tettamanzi, G. C.; Rogge, S.
2017-01-01
Single-electron pumps based on isolated impurity atoms have recently been experimentally demonstrated. In these devices the Coulomb potential of an atom creates a localised electron state with a large charging energy and considerable orbital level spacings, enabling robust charge capturing processes. In contrast to the frequently used gate-defined quantum dot pumps, which experience a strongly time-dependent potential, the confinement potential in these single-atom pumps is hardly affected by the periodic driving of the system. Here we describe the behaviour and performance of an atomic, single parameter, electron pump. This is done by considering the loading, isolating and unloading of one electron at the time, on a phosphorous atom embedded in a silicon double gate transistor. The most important feature of the atom pump is its very isolated ground state, which is populated through the fast loading of much higher lying excited states and a subsequent fast relaxation process. This leads to a substantial increase in pumping accuracy, and is opposed to the adverse role of excited states observed for quantum dot pumps due to non-adiabatic excitations. The pumping performance is investigated as a function of dopant position, revealing a pumping behaviour robust against the expected variability in atomic position. PMID:28295055
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.
An open-source framework for analyzing N-electron dynamics. I. Multideterminantal wave functions.
Pohl, Vincent; Hermann, Gunter; Tremblay, Jean Christophe
2017-06-30
The aim of the present contribution is to provide a framework for analyzing and visualizing the correlated many-electron dynamics of molecular systems, where an explicitly time-dependent electronic wave packet is represented as a linear combination of N-electron wave functions. The central quantity of interest is the electronic flux density, which contains all information about the transient electronic density, the associated phase, and their temporal evolution. It is computed from the associated one-electron operator by reducing the multideterminantal, many-electron wave packet using the Slater-Condon rules. Here, we introduce a general tool for post-processing multideterminant configuration-interaction wave functions obtained at various levels of theory. It is tailored to extract directly the data from the output of standard quantum chemistry packages using atom-centered Gaussian-type basis functions. The procedure is implemented in the open-source Python program detCI@ORBKIT, which shares and builds on the modular design of our recently published post-processing toolbox (Hermann et al., J. Comput. Chem. 2016, 37, 1511). The new procedure is applied to ultrafast charge migration processes in different molecular systems, demonstrating its broad applicability. Convergence of the N-electron dynamics with respect to the electronic structure theory level and basis set size is investigated. This provides an assessment of the robustness of qualitative and quantitative statements that can be made concerning dynamical features observed in charge migration simulations. © 2017 Wiley Periodicals, Inc. © 2017 Wiley Periodicals, Inc.
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
NASA Astrophysics Data System (ADS)
Lara-Astiaso, Manuel; Palacios, Alicia; Decleva, Piero; Tavernelli, Ivano; Martín, Fernando
2017-09-01
We present a theoretical study of charge dynamics initiated by an attosecond XUV pulse in the glycine molecule, which consists in delocalized charge fluctuations all over the molecular skeleton. For this, we have explicitly used the actual electron wave packet created by such a broadband pulse. We show that, for the chosen pulse, charge dynamics in glycine is barely affected by nuclear motion or non adiabatic effects during the first 8 fs, and that the initial electronic coherences do not dissipate during the first 20 fs. In contrast, small variations in the initial nuclear positions, compatible with the geometries expected in the Franck-Condon region, lead to noticeable changes in this dynamics.
Probing lattice dynamics in silicon with laser-wakefield accelerated electrons
NASA Astrophysics Data System (ADS)
Nees, John; He, Z.-H.; Thomas, A. G. R.; Krushelnick, Karl; Scott, S.; Legally, M.; Beaurepaire, B.; Gallé, G.; Faure, J.
2016-10-01
Laser wakefield acceleration is the key technology in a new breed of electron and photon beam sources that operate in the ultrafast domain. We show that the spatial and temporal properties of wakefield-generated electron beams can be manipulated to enable them interrogate ultrafast lattice dynamics in freestanding single-crystal silicon membranes, while maintaining spatial resolution on the atomic scale. In particular, picosecond resolution of Si lattice dynamics is obtained by recording streaked electron diffraction peaks using static magnetic fields. We will also discuss the role of wave front control in establishing optimal beam characteristics and the significance of single-shot measurements. Michigan support from NSF PHY-1535628.
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)
Enhanced Raman spectrum of pyrazine with the aid of resonant electron dynamics in a nearby cluster
NASA Astrophysics Data System (ADS)
Noda, Masashi; Yasuike, Tomokazu; Nobusada, Katsuyuki; Hayashi, Michitoshi
2012-10-01
Considerable enhancement of the electric dipole excitation in a pyrazine molecule is computationally demonstrated even under the nonresonant condition with the aid of resonant electron dynamics in a nearby linear Na4 cluster. A real-time and real-space electron dynamics simulation based on time-dependent density functional theory illustrates the details of the enhanced electric dipole excitation through analysis of the time-dependent dipole moment induced in the pyrazine molecule. Specific vibrational normal modes in the molecular plane of pyrazine are found to effectively couple with the photoinduced electronic oscillation of Na4.
NASA Astrophysics Data System (ADS)
Sato, Shunsuke A.; Yabana, Kazuhiro
2014-06-01
We propose an efficient basis expansion for electron orbitals to describe real-time electron dynamics in crystalline solids. Although a conventional grid representation in the three-dimensional Cartesian coordinates works robustly, it requires a large amount of computational resources. To reduce computational costs, we consider basis expansion methods employing eigenstates of the ground state Hamiltonian with a truncation. We have found that adding occupied eigenstates of nearby k points to the truncated basis functions composed of eigenstates of the original k point is crucially important. We demonstrate the usefulness of the method for linear and nonlinear electron dynamics calculations in crystalline SiO2.
Single-molecule interfacial electron transfer dynamics manipulated by an external electric current.
Zhang, Guofeng; Xiao, Liantuan; Chen, Ruiyun; Gao, Yan; Wang, Xiaobo; Jia, Suotang
2011-08-14
Interfacial electron transfer (IET) dynamics in a 1,1'-dioctadecyl-3,3,3',3'-tetramethylindodicarbocyanine (DiD) dye molecule/indium tin oxide (ITO) film system have been probed at the ensemble and single-molecule levels. By comparing the difference in the external electric current (EEC) dependence of the fluorescence intensities and lifetimes of the ensembles and single molecules, it is shown that the single-molecule probe can effectively demonstrate IET dynamics. The backward electron transfer and electron transfer from the ground state induce single-molecule fluorescence quenching when an EEC is applied to the DiD/ITO film system.
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.
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.
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.
Electron dynamics following photoionization: Decoherence due to the nuclear-wave-packet width
NASA Astrophysics Data System (ADS)
Vacher, Morgane; Steinberg, Lee; Jenkins, Andrew J.; Bearpark, Michael J.; Robb, Michael A.
2015-10-01
The advent of attosecond techniques opens up the possibility to observe experimentally electron dynamics following ionization of molecules. Theoretical studies of pure electron dynamics at single fixed nuclear geometries in molecules have demonstrated oscillatory charge migration at a well-defined frequency but often neglecting the natural width of the nuclear wave packet. The effect on electron dynamics of the spatial delocalization of the nuclei is an outstanding question. Here, we show how the inherent distribution of nuclear geometries leads to dephasing. Using a simple analytical model, we demonstrate that the conditions for a long-lived electronic coherence are a narrow nuclear wave packet and almost parallel potential-energy surfaces of the states involved. We demonstrate with numerical simulations the decoherence of electron dynamics for two real molecular systems (paraxylene and polycyclic norbornadiene), which exhibit different decoherence time scales. To represent the quantum distribution of geometries of the nuclear wave packet, the Wigner distribution function is used. The electron dynamics decoherence result has significant implications for the interpretation of attosecond spectroscopy experiments since one no longer expects long-lived oscillations.
Designing a dynamic path guidance system based on electronic maps by using Q-learning
NASA Astrophysics Data System (ADS)
Zou, Liang; Xu, Jianmin; Zhu, Lingxiang
2005-11-01
Shortest path problem from one origin node to one destination node in non-FIFO (First In First Out) dynamic networks is an unsolved hard problem in dynamic path guidance system. A new approach based on Q-learning is adopted to solve the problem based on electronic maps in this paper. The approach uses geographical information on electronic maps to define Q-learning's value function. Q-learning algorithm's strategy train learning method and training process on path searching are presented. Finally based on Guangzhou City's electronic map, we randomly generate a dynamic network containing 20000 nodes, 40000 links and 144 time intervals, which do not satisfy FIFO to test the approach proposed in this paper. The approach is implemented with this dynamic network and its computational performance is analyzed experimentally. The experimental results prove the effectiveness of the approach.
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
Dynamics of electrons in ammonia cages: the discovery system of solvation.
Lee, I-Ren; Lee, Wonchul; Zewail, Ahmed H
2008-01-11
Two centuries ago solvated electrons were discovered in liquid ammonia and a century later the concept of the solvent cage was introduced. Here, we report a real time study of the dynamics of size-selected clusters, n=20 to 60, of electrons in ammonia, and, for comparison, that of electrons in water cages. Unlike the water case, the observed dynamics for ammonia indicates the formation, through a 100 fs temperature jump, of a solvent collective motion in a 500 fs relaxation process. The agreement of the experimental results-obtained for a well-defined n, gated electron kinetic energy, and time delay-with molecular dynamics theory suggests the critical and different role of the kinetic energy and the librational motions involved in solvation.
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. Copyright © 2015 The Author. Published by Elsevier B.V. All rights reserved.
Electron-phonon thermalization in a scalable method for real-time quantum dynamics
Rizzi, Valerio; Todorov, Tchavdar N.; Kohanoff, Jorge J.; ...
2016-01-27
Here, we present a quantum simulation method that follows the dynamics of out-of-equilibrium many-body systems of electrons and oscillators in real time. Its cost is linear in the number of oscillators and it can probe time scales from attoseconds to hundreds of picoseconds. Contrary to Ehrenfest dynamics, it can thermalize starting from a variety of initial conditions, including electronic population inversion. While an electronic temperature can be defined in terms of a nonequilibrium entropy, a Fermi-Dirac distribution in general emerges only after thermalization. These results can be used to construct a kinetic model of electron-phonon equilibration based on the explicitmore » quantum dynamics.« less
Ultrafast extreme-ultraviolet ARPES studies of electronic dynamics in two-dimensional materials
NASA Astrophysics Data System (ADS)
Buss, Jan Heye; Maklar, Julian; Joucken, Frédéric; Wang, He; Xu, Yiming; Mo, Sung-Kwan; Lanzara, Alessandra; Kaindl, Robert A.
2017-02-01
The intriguing electronic properties of two-dimensional materials motivates experiments to resolve their rapid, microscopic interactions and dynamics across momentum space. Essential insight into the electronic momentum-space dynamics can be obtained directly via time- and angle-resolved photoemission spectroscopy (trARPES). We discuss the development of a high-repetition rate trARPES setup that employs a bright source of narrowband, extreme-UV harmonics around 22.3 eV, and its application to sensitive studies of materials dynamics. In the bulk transition-metal dichalcogenide MoSe2 momentum-space quasiparticle scattering is observed after resonant excitation at the K-point exciton line, resulting in the time-delayed buildup of electrons at the Σ-point conduction band minimum. We will discuss this and other aspects of the non-equilibrium electronic response accessible with the extreme-UV trARPES probe.
Electron dynamics of a He atom in strong, oscillating magnetic fields
NASA Astrophysics Data System (ADS)
Sadhukhan, M.; Deb, B. M.
2014-04-01
The present numerical, time-dependent density-functional study of a He atom interacting with strong, oscillating magnetic fields shows that this scenario is quite different from the case of a laser electric field-He atom interaction. Signatures of sluggish electron dynamics are found in this study, while through a mechanical analogy the flow of electron density under such conditions has been explained. These calculations take into account both exchange and correlation. Through several calculated dynamical quantities, we have shown that, in contrast to the case of the (one-electron) H atom studied earlier, the nonlinear dependence of interelectronic repulsions (a combination of Coulomb, exchange and correlation terms) on the magnetic field plays a significant role in this strong-field electron dynamics in the He atom, which cannot be explained by a perturbative approach.
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)
Kanekal, S. G.; Selesnick, R. S.; Baker, D. N.; Blake, J. B.
2007-05-01
Models of energization of electrons in the Earth's outer radiation belts invoke two classes of processes, radial transport and in-situ wave-particle interactions. Temporal evolution of electron spectra and flux isotropization during energization events provide useful observational constraints on models of electron energization. Events dominated by radial diffusion result in pancake type pitch angle distributions whereas some in-situ wave-particle energization mechanisms include pitch angle scattering leading to rapid flux isotropization. We present a survey of flux isotrpization time scales and electron spectra during relativstic electron enhancement events. We will use data collected by detectors onboard SAMPEX in low earth orbit and Polar which measures electron fluxes at higher altitude to measure flux isotropization. Electron spectra are obtained by pulse height analyzed data from the PET detector onboard SAMPEX.SAMPEX measurements cover the entire outer zone for more than a decade from mid 1992 to mid 2004 and Polar covers the time period from mid 1996 to the present.
Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium
NASA Astrophysics Data System (ADS)
Zürch, Michael; Chang, Hung-Tzu; Borja, Lauren J.; Kraus, Peter M.; Cushing, Scott K.; Gandman, Andrey; Kaplan, Christopher J.; Oh, Myoung Hwan; Prell, James S.; Prendergast, David; Pemmaraju, Chaitanya D.; Neumark, Daniel M.; Leone, Stephen R.
2017-06-01
Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 1020 cm-3. Separate electron and hole relaxation times are observed as a function of hot carrier energies. A first-order electron and hole decay of ~1 ps suggests a Shockley-Read-Hall recombination mechanism. The simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.
Direct and simultaneous observation of ultrafast electron and hole dynamics in germanium
Zurch, Michael; Chang, Hung -Tzu; Borja, Lauren J.; ...
2017-06-01
Understanding excited carrier dynamics in semiconductors is crucial for the development of photovoltaics and efficient photonic devices. However, overlapping spectral features in optical pump-probe spectroscopy often render assignments of separate electron and hole carrier dynamics ambiguous. Here, ultrafast electron and hole dynamics in germanium nanocrystalline thin films are directly and simultaneously observed by ultrafast transient absorption spectroscopy in the extreme ultraviolet at the germanium M4,5 edge. We decompose the spectra into contributions of electronic state blocking and photo-induced band shifts at a carrier density of 8 × 1020 cm–3. Separate electron and hole relaxation times are observed as a functionmore » of hot carrier energies. A first-order electron and hole decay of ~1 ps suggests a Shockley–Read–Hall recombination mechanism. Furthermore, the simultaneous observation of electrons and holes with extreme ultraviolet transient absorption spectroscopy paves the way for investigating few- to sub-femtosecond dynamics of both holes and electrons in complex semiconductor materials and across junctions.« less
Dynamics of electron currents in nanojunctions with time-varying components and interactions
NASA Astrophysics Data System (ADS)
Cuansing, Eduardo C.; Bayocboc, Francis A.; Laurio, Christian M.
2017-08-01
We study the dynamics of the electron current in nanodevices where there are time-varying components and interactions. These devices are a nanojunction attached to heat baths and with dynamical electron-phonon interactions, and a nanojunction with photon beams incident and reflected at the channel. We use the two-time nonequilibrium Green's functions technique to calculate the time-dependent electron current flowing across the devices. We find that whenever a sudden change occurs in the device, the current takes time to react to the abrupt change, overshoots, oscillates, and eventually settles down to a steady value. With dynamical electron-phonon interactions, the interaction gives rise to a net resistance that reduces the flow of current across the device when a source-drain bias potential is attached. In the presence of dynamical electron-photon interactions, the photons drive the electrons to flow. The direction of flow, however, depends on the frequencies of the incident photons. Furthermore, the direction of electron flow in one lead is exactly opposite to the direction of flow in the other lead thereby resulting in no net change in current flowing across the device.
Correlated electron-nuclear dynamics with conditional wave functions.
Albareda, Guillermo; Appel, Heiko; Franco, Ignacio; Abedi, Ali; Rubio, Angel
2014-08-22
The molecular Schrödinger equation is rewritten in terms of nonunitary equations of motion for the nuclei (or electrons) that depend parametrically on the configuration of an ensemble of generally defined electronic (or nuclear) trajectories. This scheme is exact and does not rely on the tracing out of degrees of freedom. Hence, the use of trajectory-based statistical techniques can be exploited to circumvent the calculation of the computationally demanding Born-Oppenheimer potential-energy surfaces and nonadiabatic coupling elements. The concept of the potential-energy surface is restored by establishing a formal connection with the exact factorization of the full wave function. This connection is used to gain insight from a simplified form of the exact propagation scheme.
Counting statistics for electron capture in a dynamic quantum dot.
Fricke, Lukas; Wulf, Michael; Kaestner, Bernd; Kashcheyevs, Vyacheslavs; Timoshenko, Janis; Nazarov, Pavel; Hohls, Frank; Mirovsky, Philipp; Mackrodt, Brigitte; Dolata, Ralf; Weimann, Thomas; Pierz, Klaus; Schumacher, Hans W
2013-03-22
We report noninvasive single-charge detection of the full probability distribution P(n) of the initialization of a quantum dot with n electrons for rapid decoupling from an electron reservoir. We analyze the data in the context of a model for sequential tunneling pinch-off, which has generic solutions corresponding to two opposing mechanisms. One limit considers sequential "freeze-out" of an adiabatically evolving grand canonical distribution, the other one is an athermal limit equivalent to the solution of a generalized decay cascade model. We identify the athermal capturing mechanism in our sample, testifying to the high precision of our combined theoretical and experimental methods. The distinction between the capturing mechanisms allows us to derive efficient experimental strategies for improving the initialization.
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.
Electron Dynamics in a Subproton-Gyroscale Magnetic Hole
NASA Technical Reports Server (NTRS)
Gershman, Daniel J.; Dorelli, John C.; Vinas, Adolfo F.; Avanov, Levon A.; Gliese, Ulrik B.; Barrie, Alexander C.; Coffey, Victoria; Chandler, Michael; Dickson, Charles; MacDonald, Elizabeth A.;
2016-01-01
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.
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.
Electron impact ionization dynamics of para-benzoquinone
NASA Astrophysics Data System (ADS)
Jones, D. B.; Ali, E.; Ning, C. G.; Colgan, J.; Ingólfsson, O.; Madison, D. H.; Brunger, M. J.
2016-10-01
Triple differential cross sections (TDCSs) for the electron impact ionization of the unresolved combination of the 4 highest occupied molecular orbitals (4b3g, 5b2u, 1b1g, and 2b3u) of para-benzoquinone are reported. These were obtained in an asymmetric coplanar geometry with the scattered electron being observed at the angles -7.5°, -10.0°, -12.5° and -15.0°. The experimental cross sections are compared to theoretical calculations performed at the molecular 3-body distorted wave level, with a marginal level of agreement between them being found. The character of the ionized orbitals, through calculated momentum profiles, provides some qualitative interpretation for the measured angular distributions of the TDCS.
An electronic prosthesis mimicking the dynamic vestibular function.
Shkel, Andrei M; Zeng, Fan-Gang
2006-01-01
This paper presents a functional architecture, system level design, and electronic evaluation of a unilateral vestibular prosthesis. The sensing unit of the prosthesis is a custom-designed one-axis micro-electromechanical system (MEMS) gyroscope. Similar to the natural semicircular canal, the MEMS gyroscope senses angular motion of the head and generates voltages proportional to the corresponding angular acceleration. The voltage is then converted into electric current pulses according to the physiological data relating angular acceleration to the spike count in the vestibular nerve. The current pulses can be delivered to stimulate the corresponding vestibular nerve branch. Electronic properties of the vestibular prosthesis prototype have been systematically evaluated and found to meet the design specifications. A unique feature of the present vestibular implant prototype is the scalability: the sensing unit, pulse generator, and the current source can be potentially implemented on a single chip using integrated MEMS technology.
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.
Spin Interactions and Spin Dynamics in Electronic Nanostructures
2007-11-02
and of nanomagnet dynamics excited by spin polarized currents. Major accomplishments achieved during this project include the development and...Reversal Induced by a Spin - Polarized Current,” E. B Myers, F. J. Albert, J. C. Sankey, E. Bonet, R. A. Buhrman, and D. C. Ralph, Phys. Rev. Lett. 89...196801 (2002). 4. “Using single quantum states as spin filters to study spin polarization in ferromagnets,” Mandar M. Deshmukh and D. C. Ralph, Phys
Dynamics of Electronically Excited Species in Gaseous and Condensed Phase
1989-12-01
1987). 3 D. McQuarrie , " Statistical Mechanics " (Harper and Row, 1976). 4. C. Chabalowsky, J. 0. Jensen, D. R. Yariony, and B. H. Lengsfield Ill, J. Chem...initio, lattice dynamical, and statistical mechanical approaches, helium has long attracted many researchers because it constitutes a fundamental system...modelling MTGLE parameters for realistic quenching studies (e.g., in He-He* matrix studies). This involves certain approximate statistical mechanical
Electronic Spectra from Molecular Dynamics: A Simple Approach.
1983-10-01
to the measured contours. This method and others such as the methods of Lax, Lee, Tellinghuisen and Moeller and the Landau - Zener - Stuckleberg...dynamic binning spectra, and his semi- classical Franck-Condon spectra are approximated by our harmonic quantum correction. The Landau - Zener ...depends on our assumption of two degrees of freedom, and Eq. (3.6) is gen- eral. B. Equivalence with Landau - Zener - Stuckelberg, Tully - Preston (LZSTP
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.
Intermittent Single-Molecule Interfacial Electron Transfer Dynamics
Biju, Vasudevan P.; Micic, Miodrag; Hu, Dehong; Lu, H. Peter
2004-08-04
We report on single molecule studies of photosensitized interfacial electron transfer (ET) processes in Coumarin 343 (C343)-TiO2 nanoparticle (NP) and Cresyl Violet (CV+)-TiO2 NP systems, using time-correlated single photon counting coupled with scanning confocal fluorescence microscopy. Fluorescence intensity trajectories of individual dye molecules adsorbed on a semiconductor NP surface showed fluorescence fluctuations and blinking, with time constrants distributed from sub-milliseconds to several seconds.
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.
Proton Dynamics on Goethite Nanoparticles and Coupling to Electron Transport
Zarzycki, Piotr P.; Smith, Dayle MA; Rosso, Kevin M.
2015-04-14
The surface chemistry of metal oxide particles is governed by the charge that develops at the interface with aqueous solution. Mineral transformation, biogeochemical reactions, remediation, and sorption dynamics are profoundly affected in response. Here we report implementation of replica-exchange constant-pH molecular dynamics simulations that use classical molecular dynamics for exploring configurational space and Metropolis Monte Carlo walking through protonation space with a simulated annealing escape route from metastable configurations. By examining the archetypal metal oxide, goethite (α-FeOOH), we find that electrostatic potential gradients spontaneously arise between intersecting low-index crystal faces and across explicitly treated oxide nanoparticles at a magnitude exceeding the Johnson–Nyquist voltage fluctuation. Fluctuations in adsorbed proton density continuously repolarize the surface potential bias between edge-sharing crystal faces, at a rate slower than the reported electron–polaron hopping rate in goethite interiors. This suggests that these spontaneous surface potential fluctuations will control the net movement of charge carriers in the lattice.
Single-molecule interfacial electron transfer dynamics in solar energy conversion
NASA Astrophysics Data System (ADS)
Dhital, Bharat
This dissertation work investigated the parameters affecting the interfacial electron transfer (ET) dynamics in dye-semiconductor nanoparticles (NPs) system by using single-molecule fluorescence spectroscopy and imaging combined with electrochemistry. The influence of the molecule-substrate electronic coupling, the molecular structure, binding geometry on the surface and the molecule-attachment surface chemistry on interfacial charge transfer processes was studied on zinc porphyrin-TiO2 NP systems. The fluorescence blinking measurement on TiO2 NP demonstrated that electronic coupling regulates dynamics of charge transfer processes at the interface depending on the conformation of molecule on the surface. Moreover, semiconductor surface charge induced electronic coupling of molecule which is electrostatically adsorbed on the semiconductor surface also predominantly alters the ET dynamics. Furthermore, interfacial electric field and electron accepting state density dependent ET dynamics has been dissected in zinc porphyrin-TiO2 NP system by observing the single-molecule fluorescence blinking dynamics and fluorescence lifetime with and without applied bias. The significant difference in fluorescence fluctuation and lifetime suggested the modulation of charge transfer dynamics at the interface with external electric field perturbation. Quasi-continuous distribution of fluorescence intensity with applied negative potential was attributed to the faster charge recombination due to reduced density of electron accepting states. The driving force and electron accepting state density ET dependent dynamics has also been probed in zinc porphyrin-TiO2 NP and zinc porphyrin-indium tin oxide (ITO) systems. Study of a molecule adsorbed on two different semiconductors (ITO and TiO2), with large difference in electron densities and distinct driving forces, allows us to observe the changes in rates of back electron transfer process reflected by the suppressed fluorescence blinking of
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.
Beleggia, Marco; Pozzi, Giulio
2008-10-01
We present an alternative interpretation of the holographic phase dislocation loops revealed by Shindo et al. [J. Electron Microsc. 56(1): 1-5 (2007)] around a charged sample. Our interpretation does not involve the motion of secondary electrons around a charged object. It relates, instead, to fluctuating charges on the sample and to the resulting Moiré-type patterns in the hologram.
Spin relaxations in 2D electron gas determined by the memory in the carrier dynamics.
NASA Astrophysics Data System (ADS)
Sherman, Eugene; Glazov, Mikhail
2007-03-01
The effects of long memory, in carrier dynamics in a magnetic field, on spin polarization evolution in 2D electron gas are investigated qualitatively and quantitatively. As examples we consider (i) systems with random Rashba-type SO coupling and (ii) quantum wells with rigid short-range scatterers (antidotes) and regular Dresselhaus SO coupling. In both cases the spin dynamics is strongly non-Markovian. In the system with the random SO coupling the time dependence of the spin polarization shows Gaussian rather than exponential behavior with the cusps corresponding to the electron revolutions. The relaxation speeds up with the increase of the magnetic field. In the system with antidotes scattering, the spin polarization shows a long-tail behavior with the relaxation rate determined by inelastic electron-phonon and electron-electron collisions and demonstrates unusual field dependence.
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.
Time-dependent density-functional theory method in the electron nuclear dynamics framework
NASA Astrophysics Data System (ADS)
Ajith Perera, S.; McLaurin, Patrick M.; Grimes, Thomas V.; Morales, Jorge A.
2010-08-01
A time-dependent density-functional theory (DFT) dynamics method in the electron nuclear dynamics (END) framework is presented. This time-dependent variational method treats simultaneously the nuclei and electrons of a system without utilizing predetermined potential energy surfaces. Like the simplest-level END, this method adopts a classical-mechanics description for the nuclei and a Thouless single-determinantal representation for the electrons. However, the electronic description is now expressed in a Kohn-Sham DFT form that provides electron correlation effects absent in the simplest-level END. Current implementation of this method employs the adiabatic approximation in the exchange-correlation action and potential. Simulations of molecular vibrations and proton-molecule reactions attest to the accuracy of the present method.
Electron nuclear dynamics for a zig-zag chain of nitrogen atoms
NASA Astrophysics Data System (ADS)
Pohl, Anna; Calais, Jean-Louis
1995-02-01
We study the nitrogen zig-zag chain with two atoms per unit cell within the electron nuclear dynamics (END) formalism. This amounts to an approximate solution of the time-dependent Schrödinger equation for all the particles in the system. In the present approximation the nuclei are treated classically. The time dependence of the electronic motion is brought in through time-dependent linear combinations of fixed Bloch sums. This implies that the immediate mutual interaction between electronic and nuclear motion is taken into account. We investigate in particular the long-range terms of the interaction so as to arrive at convergent lattice sums. Before going to the general case when electronic and nuclear motion is coupled, we investigate the special cases of END traditional lattice dynamics and the random phase approximation (RPA) for the electrons.
New algorithm for dynamical friction of ions in a magnetized electron beam
NASA Astrophysics Data System (ADS)
Bruhwiler, David L.; Webb, Stephen D.
2017-03-01
Relativistic magnetized electron cooling in untested parameter regimes is essential to achieve the ion luminosity requirements of proposed electron-ion collider designs. Therefore, accurate calculations of magnetized dynamic friction are required, with the ability to include all relevant physics that might increase the cooling time, including space charge forces, field errors and complicated phase space distributions of imperfectly magnetized electron beams. We present a fundamentally new analytic treatment of momentum transfer from a single magnetized electron to a drifting ion, with arbitrary initial conditions and arbitrary interaction time. The map describing such collisions, which is derived from a Hamiltonian and conserves momentum, removes any need to numerically integrate the complicated Larmor trajectories. This important result, made possible by effectively exploiting the perturbative nature of the problem, will enable rapid semi-analytic calculations of dynamic friction on ions in magnetized cooling systems for arbitrary electron distributions.
Communication: Adiabatic and non-adiabatic electron-nuclear motion: Quantum and classical dynamics.
Albert, Julian; Kaiser, Dustin; Engel, Volker
2016-05-07
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.
Zhou, Yueming; Huang, Cheng; Tong, Aihong; Liao, Qing; Lu, Peixiang
2011-01-31
We have investigated the correlated electron dynamics in nonsequential double ionization (NSDI) of helium by the orthogonally polarized two-color pulses that consisted of an 800-nm and a 400-nm laser fields using the classical ensemble model. Depending on the relative phase of the two-color field, the electron momentum distributions along the polarization direction of the 800-nm field exhibit a surprisingly strong anticorrelated or correlated behavior. Back analysis reveals that recollisions eventually leading to NSDI are concentrated in a time window as short as several hundreds attoseconds with this scheme. By changing the relative phase of the two-color field, the revisit time of recolliding electron wave packet has been controlled with attosecond precision, which is responsible for the various correlated behaviors of the two electrons. Our results reveal that the orthogonally polarized two-color field can serve as a powerful tool to control the correlated electron dynamics in NSDI.
Andrews, David Q; Solomon, Gemma C; Van Duyne, Richard P; Ratner, Mark A
2008-12-24
Molecular electronics is partly driven by the goal of producing active electronic elements that rival the performance of their solid-state counterparts, but on a much smaller size scale. We investigate what constitutes an ideal switch or molecular device, and how it can be designed, by analyzing transmission plots. The interference features in cross-conjugated molecules provide a large dynamic range in electron transmission probability, opening a new area for addressing electronic functionality in molecules. This large dynamic range is accessible through changes in electron density alone, enabling fast and stable switching. Using cross-conjugated molecules, we show how the width, depth, and energetic location of the interference features can be controlled. In an example of a single molecule transistor, we calculate a change in conductance of 8 orders of magnitude with an applied gate voltage. Using multiple interference features, we propose and calculate the current/voltage behavior of a molecular rectifier with a rectification ratio of >150,000. We calculate a purely electronic negative differential resistance behavior, suggesting that the large dynamic range in electron transmission probability caused by quantum interference could be exploited in future electronic devices.
4D scanning ultrafast electron microscopy: visualization of materials surface dynamics.
Mohammed, Omar F; Yang, Ding-Shyue; Pal, Samir Kumar; Zewail, Ahmed H
2011-05-25
The continuous electron beam of conventional scanning electron microscopes (SEM) limits the temporal resolution required for the study of ultrafast dynamics of materials surfaces. Here, we report the development of scanning ultrafast electron microscopy (S-UEM) as a time-resolved method with resolutions in both space and time. The approach is demonstrated in the investigation of the dynamics of semiconducting and metallic materials visualized using secondary-electron images and backscattering electron diffraction patterns. For probing, the electron packet was photogenerated from the sharp field-emitter tip of the microscope with a very low number of electrons in order to suppress space-charge repulsion between electrons and reach the ultrashort temporal resolution, an improvement of orders of magnitude when compared to the traditional beam-blanking method. Moreover, the spatial resolution of SEM is maintained, thus enabling spatiotemporal visualization of surface dynamics following the initiation of change by femtosecond heating or excitation. We discuss capabilities and potential applications of S-UEM in materials and biological science.
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.
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.
Dissociation dynamics of transient anion formed via electron attachment to sulfur dioxide
NASA Astrophysics Data System (ADS)
Gope, K.; Prabhudesai, V. S.; Mason, N. J.; Krishnakumar, E.
2017-08-01
We report the molecular dynamics of dissociative electron attachment to sulfur dioxide (SO2) by measuring the momentum distribution of fragment anions using the velocity slice imaging technique in the electron energy range of 2-10 eV. The S- channel results from symmetric dissociation which exhibits competition between the stretch mode and bending mode of vibration in the excited parent anion. The asymmetric dissociation of parent anions leads to the production of O- and SO- channels where the corresponding neutral fragments are formed in their ground as well as excited electronic states. We also identify that internal excitation of SO- is responsible for its low yield at higher electron energies.
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.
Ultrafast structural and electronic dynamics of the metallic phase in a layered manganite.
Piazza, L; Ma, C; Yang, H X; Mann, A; Zhu, Y; Li, J Q; Carbone, F
2014-01-01
The transition between different states in manganites can be driven by various external stimuli. Controlling these transitions with light opens the possibility to investigate the microscopic path through which they evolve. We performed femtosecond (fs) transmission electron microscopy on a bi-layered manganite to study its response to ultrafast photoexcitation. We show that a photoinduced temperature jump launches a pressure wave that provokes coherent oscillations of the lattice parameters, detected via ultrafast electron diffraction. Their impact on the electronic structure are monitored via ultrafast electron energy loss spectroscopy, revealing the dynamics of the different orbitals in response to specific structural distortions.
Xiao, H. Y.; Weber, W. J.; Zhang, Y.; Zu, X. T.; Li, S.
2015-01-01
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, electron and ion irradiations. PMID:25660219
Bound electron dynamics: Exact solution for a one-dimensional oscillator-string model
NASA Astrophysics Data System (ADS)
Dekker, H.
1984-11-01
The dynamical problem of a harmonically bound electron with standard dipole model coupling to the electromagnetic field in a finite one-dimensional space is solved exactly in a simple manner. It is easily shown that in this model the coupling between the electron and the field is “rigid”, in the sense of and in complete analogy with a recent treatment of a purely mechanical particle on a string. As a consequence the electron's quantum mechanical momentum fluctuations exhibit a logarithmic ultraviolet divergence. In the limit of infinite spatial extension of the field, and apart from quantal noise, the electron behaves exactly as a simple linearly damped harmonic oscillator.
Dissociation dynamics of transient anion formed via electron attachment to sulfur dioxide.
Gope, K; Prabhudesai, V S; Mason, N J; Krishnakumar, E
2017-08-07
We report the molecular dynamics of dissociative electron attachment to sulfur dioxide (SO2) by measuring the momentum distribution of fragment anions using the velocity slice imaging technique in the electron energy range of 2-10 eV. The S(-) channel results from symmetric dissociation which exhibits competition between the stretch mode and bending mode of vibration in the excited parent anion. The asymmetric dissociation of parent anions leads to the production of O(-) and SO(-) channels where the corresponding neutral fragments are formed in their ground as well as excited electronic states. We also identify that internal excitation of SO(-) is responsible for its low yield at higher electron energies.
Electronic dynamics under effect of a nonlinear Morse interaction and a static electric field
NASA Astrophysics Data System (ADS)
Ranciaro Neto, A.; de Moura, F. A. B. F.
2016-11-01
Considering non-interacting electrons in a one-dimension alloy in which atoms are coupled by a Morse potential, we study the system dynamics in the presence of a static electric field. Calculations are performed assuming a quantum mechanical treatment for the electronic transport and a classical Hamiltonian model for the lattice vibrations. We report numerical evidence of the existence of a soliton-electron pair, even when the electric field is turned on, and we offer a description of how the existence of such a phase depends on the magnitude of the electric field and the electron-phonon interaction.
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.
Liu, Jinxiang; Cukier, Robert I; Bu, Yuxiang
2013-11-12
We report an ab initio molecular dynamics simulation study of the solvation and dynamics of an excess electron in liquid acetonitrile (ACN). Four families of states are observed: a diffusely solvated state and three ACN core-localized states with monomer core, quasi-dimer (π*-Rydberg mode) core, and dual-core/dimer core (a coupled dual-core). These core localized states cannot be simply described as the corresponding anions because only a part of the excess electron resides in the core molecule(s). The quasi-dimer core state actually is a mixture that features cooperative excess electron capture by the π* and Rydberg orbitals of two ACNs. Well-defined dimer anion and solvated electron cavity were not observed in the 5-10 ps simulations, which may be attributed to slow dynamics of the formation of the dimer anion and difficulty of the formation of a cavity in such a fluxional medium. All of the above observed states have near-IR absorptions and thus can be regarded as the solvated electron states but with different structures, which can interpret the experimentally observed IR band. These states undergo continuous conversions via a combination of long-lasting breathing oscillation and core switching, characterized by highly cooperative oscillations of the electron cloud volume and vertical detachment energy. The quasi-dimer core and diffusely solvated states dominate the time evolution, with the monomer core and dual-core/dimer core states occurring occasionally during the breathing and core switching processes, respectively. All these oscillations and core switchings are governed by a combination of the electron-impacted bending vibration of the core ACN molecule(s) and thermal fluctuations.
NASA Astrophysics Data System (ADS)
Krylov, A. I.; Gerber, R. B.; Gaveau, M. A.; Mestdagh, J. M.; Schilling, B.; Visticot, J. P.
1996-03-01
Molecular Dynamics simulations using a surface-hopping method for transitions between different electronic states are employed to study the dynamics following photoexcitation of the Ba(Ar)125 cluster. The results are used to interpret spectroscopic experiments on large, size-distributed Ba(Ar)n clusters. The dynamics of the coupled electronic-nuclear motions in the cluster involves transitions between three potential energy surfaces, corresponding to the nearly-degenerate p-states of the excited Ba atom. Ejection of excited Ba atoms, adsorbed on the surface of the cluster, can take place. The focus in comparing theory and experiment is on the emission spectrum from the excited clusters, on the polarization of this radiation, and on the polarization of light emitted by excited Ba atoms ejected from the cluster. Based on the good agreement found between theory and experiment, a comprehensive picture of the excited state dynamics is given. It is found that upon excitation, energy is rapidly redistributed in the cluster and no direct ejection of Ba occurs. Electronic relaxation to the lowest P-state occurs, and the latter dominates the cluster emission spectrum and polarization. The electronic state relaxation is mostly complete within t≲10 ps. Ejection of Ba atoms occurs as a rare and delayed event when a dynamical fluctuation creates a ``hot spot'' at the Ba site, with a non-adiabatic excitation to the highest electronic level. The results show the feasibility of near-quantitative understanding of non-adiabatic processes in large clusters.
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.
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.
Dynamical exchange-correlation potentials for the electron liquid
NASA Astrophysics Data System (ADS)
Qian, Zhixin; Vignale, Giovanni
2002-03-01
The imaginary parts of the exchange-correlation kernels f_xc^L,T(q=0, ω) in the linear density-density and transverse current-current response functions of a homogeneous electron liquid are calculated exactly at low frequency, to leading order in the Coulomb interaction. Combining these new results with the previously known high-frequency behaviors of Im f_xc^L,T(q=0, ω) and with the compressibility and the third frequency moment sum rules, we construct simple interpolation for Im f_xc^L,T(q=0, ω) in 3- and 2- dimensions. A novel feature of our interpolation formulas is that they explicitly take into account the two-plasmon component of the excitation spectrum: our longitudinal spectrum Im f_xc^L(q=0, ω) is thus intermediate between the Gross-Kohn interpolation, which ignores the two-plasmon contribution, and a recent approximate calculation by Nifosi, Conti, and Tosi, which probably overestimates it. Numerical results for both the real and imaginary parts of the exchange-correlation kernels at typical electron densities are presented, and compared with those obtained from previous approximations.
Electronic dynamics and plasmons of sodium under compression
Mao, Ho-Kwang; Ding, Yang; Xiao, Yuming; Chow, Paul; Shu, Jinfu; Lebègue, Sébastien; Lazicki, Amy; Ahuja, Rajeev
2011-01-01
Sodium, which has long been regarded as one of the simplest metals, displays a great deal of structural, optical, and electronic complexities under compression. We compressed pure Na in the body-centered cubic structure to 52 GPa and in the face-centered cubic structure from 64 to 97 GPa, and studied the plasmon excitations of both structures using the momentum-dependent inelastic X-ray scattering technique. The plasmon dispersion curves as a function of pressure were extrapolated to zero momentum with a quadratic approximation. As predicted by the simple free-electron model, the square of the zero-momentum plasmon energy increases linearly with densification of the body-centered cubic Na up to 1.5-fold. At further compressions and in face-centered cubic Na above 64 GPa, the linear relation curves progressively toward the density axis up to 3.7-fold densification at 97 GPa. Ab initio calculations indicate that the deviation is an expected behavior of Na remaining a simple metal. PMID:22143758
Hamiltonian magnetic reconnection with parallel electron heat flux dynamics
NASA Astrophysics Data System (ADS)
Grasso, D.; Tassi, E.
2015-10-01
> We analyse, both analytically and numerically, a two-dimensional six-field fluid model for collisionless magnetic reconnection, accounting for temperature and heat flux fluctuations along the direction of the magnetic guide field. We show that the model possesses a Hamiltonian structure with a non-canonical Poisson bracket. This bracket is characterized by the presence of six infinite families of Casimirs, associated with Lagrangian invariants. This reveals that the model can be reformulated as a system of advection equations, thus generalizing previous results obtained for Hamiltonian isothermal fluid models for reconnection. Numerical simulations indicate that the presence of heat flux and temperature fluctuations yields slightly larger growth rates and similar saturated island amplitudes, with respect to the isothermal models. For values of the sonic Larmor radius much smaller than the electron skin depth, heat flux fluctuations tend to be suppressed and temperature fluctuations follow density fluctuations. Increasing the sonic Larmor radius results in an increasing fraction of magnetic energy converted into heat flux, at the expense of temperature fluctuations. In particular, heat flux fluctuations tend to become relevant along the magnetic island separatrices. The qualitative structures associated with the electron field variables are also reinterpreted in terms of the rotation of the Lagrangian invariants of the system.
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.
Electronic dynamics and plasmons of sodium under compression.
Mao, Ho-Kwang; Ding, Yang; Xiao, Yuming; Chow, Paul; Shu, Jinfu; Lebègue, Sébastien; Lazicki, Amy; Ahuja, Rajeev
2011-12-20
Sodium, which has long been regarded as one of the simplest metals, displays a great deal of structural, optical, and electronic complexities under compression. We compressed pure Na in the body-centered cubic structure to 52 GPa and in the face-centered cubic structure from 64 to 97 GPa, and studied the plasmon excitations of both structures using the momentum-dependent inelastic X-ray scattering technique. The plasmon dispersion curves as a function of pressure were extrapolated to zero momentum with a quadratic approximation. As predicted by the simple free-electron model, the square of the zero-momentum plasmon energy increases linearly with densification of the body-centered cubic Na up to 1.5-fold. At further compressions and in face-centered cubic Na above 64 GPa, the linear relation curves progressively toward the density axis up to 3.7-fold densification at 97 GPa. Ab initio calculations indicate that the deviation is an expected behavior of Na remaining a simple metal.
Study of dynamic grain growth by electron microscopy and EBSD.
Rofman, O V; Bate, P S; Brough, I; Humphreys, F J
2009-03-01
The effect of hot deformation on fully recrystallized aluminium-copper alloys (Al-4wt%Cu and Al-33wt%Cu) with different volume fractions of CuAl(2) has been studied. The alloys are Zener pinned systems with different superplastic properties. Strain-induced grain growth, observed in both alloys, was quantitatively estimated by means of electron microscopy and EBSD and compared with the rate of static grain growth. Surface marker observations and in situ hot-deformation experiments combined with EBSD were aimed at clarifying the mechanisms responsible for the changes in the deformed microstructures. A sequence of secondary and backscattered electron images and EBSD maps was obtained during in situ SEM deformation with different testing conditions. Overlaying EBSD maps for the Al-4wt%Cu with channelling contrast images showed that grain boundary motion occurred during deformation, creating a layered structure and leading to an increase in size of some grains and shrinkage of others. Of a particular interest are results related to behaviour of CuAl(2) in superplastic Al-33wt%Cu during deformation, including several problems with the use of EBSD in this alloy.
Electron-Nuclear Dynamics of atomic and molecular collisions: Charge exchange and energy loss
NASA Astrophysics Data System (ADS)
Cabrera-Trujillo, Remigio; Sabin, John R.; Ohrn, Yngve; Deumens, Erik
2004-05-01
Processes like electron exchange (capture and loss), bond breaking, and chemical reactions are difficult to visualize and treat in a time-independent approach. In this work, we present the Electron-Nuclear Dynamics (END) method for the study of time-dependent scattering processes. The END is a general approach for treating time-dependent problems which includes the dynamics of electrons and nuclei simultaneously by considering the full electron-nuclear coupling in the system and thus eliminates the necessity of constructing potential-energy surfaces. The theory approximates the time dependent Schrödinger equation starting from the time dependent variational principle (TDVP) by deriving a Hamiltonian dynamical system for time dependent nuclear and electronic wave function parameters. The wave function is described in a coherent state manifold, which leads to a system of Hamilton's equations of motion. The resulting system of coupled, first order, ordinary differential equations approximates the Schrödinger equation. A detailed analysis of the END equations is given for the case of a single-determinantal state for the electrons and a classical treatment of the nuclei. Emphasis is put on electron exchange, differential cross section and energy loss (stopping cross section) of collision of ions, atoms and molecules involving H, He, C, N, O, and Ne atoms. We compare our results to available experimental data.
NASA Astrophysics Data System (ADS)
Walbran, Sean Michael
We have carried out simulation studies of the electrode electrolyte interface using quantum mechanical electronic structure direct dynamics and classical molecular dynamics methods. We have obtained a complete description of the electrostatic response of the copper/water interface including electronic structure of the electrode, molecular structure of the Stern layer, and a continuum treatment of the electrolyte ions. We have furthered the investigation of chlorine adsorbtion and electron transfer reactions at the interface by refining and exploring electronic structure techniques. While these techniques are currently too expensive for use in electron transfer studies, we were able to study the cuprous/cupric reaction at a copper electrode in water by incorporating features of more detailed simulations into classical molecular dynamics models. In contrast with earlier studies of ferrous/ferric electron transfer, we find that the cuprous/cupric reaction proceeds adiabatically. Results on the electron transfer rates are in reasonable agreement with new experiments carried out by out collaborators at Argonne National Laboratory.
Dynamics and pathway of electron tunneling in repair of damaged DNA by photolyase
NASA Astrophysics Data System (ADS)
Liu, Zheyun; Guo, Xunmin; Tan, Chuang; Li, Jiang; Kao, Ya-Ting; Wang, Lijuan; Sancar, Aziz; Zhong, Dongping
2013-03-01
Through electron tunneling, photolyase, a photoenzyme, restores damaged DNA into normal bases. Here, we report our systematic characterization and analyses of three electron transfer processes in thymine dimer restoration by following the entire dynamical evolution during enzymatic repair with femtosecond resolution. Using (deoxy)uracil and thymine as dimer substrates, we unambiguously determined the electron tunneling pathways for the forward electron transfer to initiate repairing and for the final electron return to restore the active cofactor and complete the repair photocycle. Significantly, we found that the adenine moiety of the unusual bent cofactor is essential to mediating all electron-transfer dynamics through a super-exchange mechanism, leading to a delicate balance of time scales. The active-site structural integrity, unique electron tunneling pathways and the critical role of adenine assure these elementary dynamics in synergy in this complex photorepair machinery to achieve the maximum repair efficiency close to unity. The authors thank Drs. Chaitanya Sexana, Yi Yang, and Chen Zang for the initial help with experiment, and Prof. Sherwin Singer and Dr. Ali Hassanali for discussion.
Understanding Dynamic Competitive Technology Diffusion in Electronic Markets
NASA Astrophysics Data System (ADS)
Zhang, Cheng; Song, Peijian; Xu, Yunjie; Xue, Ling
The extant literature on information technology (IT) diffusion has largely treated technology diffusion as a generic and independent process. This study, in contrast, examines the diffusion of different IT products with brand differentiation and competition. Drawing upon existing theories of product diffusion, we propose a research model to capture the dynamics of the competitive diffusion of web-based IT products and validate it with longitudinal field data of e-business platforms. Our findings suggest that IT product diffusion can be better predicted by a competitive model than by an independent-diffusion-process model. This research extends IT research to the context of competitive diffusion and provides practitioners an effective model to predict the dissemination of their products. The research also suggests the existence of asymmetric interactions among competing products, prompting scholars and practitioners to pay attention to the influence of competing products when making forecast of their product market.
[The innovative dynamic of the mechanics, electronics and materials subsystem].
Maldonado, José; Gadelha, Carlos Augusto Grabois; Costa, Laís Silveira; Vargas, Marco
2012-12-01
The mechanics, electronics and materials subsystem, one of the subsystems of the health care productive complex, encompasses different activities, usually clustered in what is called the medical, hospital and dental equipment and materials industry. This is a strategic area for health care, since it represents a continuous source of changes in care practices, and influences the provision of health care services. It has, moreover, potential for promoting the progress of Brazil's system of innovation and for increasing the competitiveness of the industry as a whole, given that it articulates future technologies. Despite the significant growth of this industry in Brazil in recent years, such equipment and materials have been presenting a growing deficit in the balance of trade. This incompatibility between national health care needs and the productive and innovative basis of the industry points to structural fragilities in the system. Using the framework of political economy, the article aims to discuss the development of this industry in Brazil and its challenges.
Ultrafast structural dynamics of boron nitride nanotubes studied using transmitted electrons.
Li, Zhongwen; Sun, Shuaishuai; Li, Zi-An; Zhang, Ming; Cao, Gaolong; Tian, Huanfang; Yang, Huaixin; Li, Jianqi
2017-08-31
We investigate the ultrafast structural dynamics of multi-walled boron nitride nanotubes (BNNTs) upon femtosecond optical excitation using ultrafast electron diffraction in a transmission electron microscope. Analysis of the time-resolved (100) and (002) diffraction profiles reveals highly anisotropic lattice dynamics of BNNTs, which can be attributed to the distinct nature of the chemical bonds in the tubular structure. Moreover, the changes in (002) diffraction positions and intensities suggest that the lattice response of BNNTs to the femtosecond laser excitation involves a fast and a slow lattice dynamic process. The fast process with a time constant of about 8 picoseconds can be understood to be a result of electron-phonon coupling, while the slow process with a time constant of about 100 to 300 picoseconds depending on pump laser fluence is tentatively associated with an Auger recombination effect. In addition, we discuss the power-law relationship of a three-photon absorption process in the BNNT nanoscale system.
Nonadiabatic Electron Dynamics in Orthogonal Two-Color Laser Fields with Comparable Intensities.
Geng, Ji-Wei; Xiong, Wei-Hao; Xiao, Xiang-Ru; Peng, Liang-You; Gong, Qihuang
2015-11-06
We theoretically investigate the nonadiabatic subcycle electron dynamics in orthogonally polarized two-color laser fields with comparable intensities. The photoelectron dynamics is simulated by exact solution to the 3D time-dependent Schrödinger equation, and also by two other semiclassical methods, i.e., the quantum trajectory Monte Carlo simulation and the Coulomb-corrected strong field approximation. Through these methods, we identify the underlying mechanisms of the subcycle electron dynamics and find that both the nonadiabatic effects and the Coulomb potential play very important roles. The contribution of the nonadiabatic effects manifest in two aspects, i.e., the nonadiabatic ionization rate and the nonzero initial velocities at the tunneling exit. The Coulomb potential has a different impact on the electrons' trajectories for different relative phases between the two pulses.
NASA Astrophysics Data System (ADS)
Lee, J.; Lee, E.; Kim, K. H.; Lee, D. H.; Lee, J.; Spence, H. E.
2015-12-01
Earth's outer radiation belt varies dynamically under the variations of the solar wind. In this study, we investigated the variations of energetic electrons in the outer radiation belt caused by an enhancement of the solar wind dynamic pressure associated with an interplanetary shock using the measurements from the Van Allen Probes (VAP) satellites. The enhanced dynamic pressure lasted for about 24 hours, but magnetic storm was not occurred. The impact of the interplanetary shock on 13 April 2013 produced dipolarization of the magnetic field for a few minutes, which was simultaneously observed by VAP A and B moving in the nightside region. The enhancement of the electron fluxes with E < ~600 keV coincidentally occurred during the dipolarization. Later, drift echoes with energy dispersion and ULF-like modulations were observed. By comparing the measurements from VAP A and B we will discuss spatial and temporal characteristics of the enhancement of the energetic electron fluxes.
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.
NASA Astrophysics Data System (ADS)
Lee, P.; Maynard, G.; Audet, T. L.; Cros, B.; Lehe, R.; Vay, J.-L.
2016-11-01
The dynamics of electron acceleration driven by laser wakefield is studied in detail using the particle-in-cell code WARP with the objective to generate high-quality electron bunches with narrow energy spread and small emittance, relevant for the electron injector of a multistage accelerator. Simulation results, using experimentally achievable parameters, show that electron bunches with an energy spread of ˜11 % can be obtained by using an ionization-induced injection mechanism in a mm-scale length plasma. By controlling the focusing of a moderate laser power and tailoring the longitudinal plasma density profile, the electron injection beginning and end positions can be adjusted, while the electron energy can be finely tuned in the last acceleration section.
Lee, Patrick; Maynard, G.; Audet, T. L.; ...
2016-11-16
The dynamics of electron acceleration driven by laser wakefield is studied in detail using the particle-in-cell code WARP with the objective to generate high-quality electron bunches with narrow energy spread and small emittance, relevant for the electron injector of a multistage accelerator. Simulation results, using experimentally achievable parameters, show that electron bunches with an energy spread of ~11% can be obtained by using an ionization-induced injection mechanism in a mm-scale length plasma. By controlling the focusing of a moderate laser power and tailoring the longitudinal plasma density profile, the electron injection beginning and end positions can be adjusted, while themore » electron energy can be finely tuned in the last acceleration section.« less
Dynamics of boundary layer electrons in laser driven wakefields (Conference Presentation)
NASA Astrophysics Data System (ADS)
Chen, Min
2017-05-01
The dynamics of electrons forming the boundary layer of a highly nonlinear laser wakefield is investigated using computational simulations. It is shown that when the driver pulse intensity increases or the focal spot size decreases, a significant amount of electrons initially pushed by the laser pulse can detach from the bubble structure at its tail, middle, or front and form particular classes of waves locally with high densities, referred to as the tail wave, lateral wave, and bow wave. Simulation results show that the tail and bow waves correspond to real electron trajectories, while the lateral wave does not. The detached electrons can be ejected transversely, containing considerable energy, and reducing the efficiency of the laser wakefield accelerator. Some of the transversely emitted electrons may obtain MeV level energy. These electrons can be used for wake evolution diagnosis and producing high frequency radiation.
Eliasson, B; Shukla, P K
2006-10-01
We consider nonlinear interactions between two colliding laser beams in an electron plasma, accounting for the relativistic electron mass increase in the laser fields and radiation pressure driven electron-acoustic (EA) perturbations that are supported by hot and cold electrons. By using the hydrodynamic and Maxwell equations, we obtain the relevant equations for nonlinearly coupled laser beams and EA perturbations. The coupled equations are then Fourier analyzed to obtain a nonlinear dispersion relation. The latter is numerically solved to show the existence of new classes of the parametric instabilities in the presence of two colliding laser beams in a two-electron plasma. The dynamics of nonlinearly coupled laser beams in our electron plasma is also investigated. The results should be useful in understanding the nonlinear propagation characteristics of multiple electromagnetic beams in laser-produced plasmas as well as in space plasmas.
NASA Astrophysics Data System (ADS)
Tang, C. L.; Wang, Y. X.; Ni, B.; Zhang, J.-C.; Reeves, G. D.; Su, Z. P.; Baker, D. N.; Spence, H. E.; Funsten, H. O.; Blake, J. B.
2017-05-01
Using the particle data measured by Van Allen Probe A from October 2012 to March 2016, we investigate in detail the radiation belt seed population and its association with the relativistic electron dynamics during 74 geomagnetic storms. The period of the storm recovery phase was limited to 72 h. The statistical study shows that geomagnetic storms and substorms play important roles in the radiation belt seed population (336 keV electrons) dynamics. Based on the flux changes of 1 MeV electrons before and after the storm peak, these storm events are divided into two groups of "large flux enhancement" and "small flux enhancement." For large flux enhancement storm events, the correlation coefficients between the peak flux location of the seed population and those of relativistic electrons (592 keV, 1 MeV, 1.8 MeV, and 2.1 MeV) during the storm recovery phase decrease with electron kinetic energy, being 0.92, 0.68, 0.49, and 0.39, respectively. The correlation coefficients between the peak flux of the seed population and those of relativistic electrons are 0.92, 0.81, 0.75, and 0.73. For small flux enhancement storm events, the correlation coefficients between the peak flux location of the seed population and those of relativistic electrons are relatively smaller, while the peak flux of the seed population is well correlated with those of relativistic electrons (correlation coefficients >0.84). It is suggested that during geomagnetic storms there is a good correlation between the seed population and ≤1 MeV electrons and the seed population is important to the relativistic electron dynamics.
Hammes-Schiffer, Sharon
2011-06-16
Proton-coupled electron transfer (PCET) reactions play an important role in a wide range of biological and chemical processes. The motions of the electrons, transferring protons, solute nuclei, and solvent nuclei occur on a wide range of timescales and are often strongly coupled. As a result, the theoretical description of these processes requires a combination of quantum and classical methods. This perspective discusses three of the current theoretical challenges in the field of PCET. The first challenge is the calculation of electron-proton nonadiabatic effects, which are significant for these reactions because the hydrogen tunneling is often faster than the electronic transition. The second challenge is the modeling of electron transfer coupled to proton transport along hydrogen-bonded networks. The third challenge is the simulation of the ultrafast dynamics of nonequilibrium photoinduced PCET reactions in solution. Insights provided by theoretical studies may assist in the design of more effective catalysts for energy conversion processes. The proton relay portion of this review is based upon work supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences.
Hammes-Schiffer, Sharon
2011-06-16
Proton-coupled electron transfer (PCET) reactions play an important role in a wide range of biological and chemical processes. The motions of the electrons, transferring protons, solute nuclei, and solvent nuclei occur on a wide range of time scales and are often strongly coupled. As a result, the theoretical description of these processes requires a combination of quantum and classical methods. This Perspective discusses three of the current theoretical challenges in the field of PCET. The first challenge is the calculation of electron proton nonadiabatic effects, which are significant for these reactions because the hydrogen tunneling is often faster than the electronic transition. The second challenge is the modeling of electron transfer coupled to proton transport along hydrogen-bonded networks. The third challenge is the simulation of the ultrafast dynamics of nonequilibrium photoinduced PCET reactions in solution. Insights provided by theoretical studies may assist in the design of more effective catalysts for energy conversion processes. The proton relay portion of this review is based upon work supported as part of the Center for Molecular Electrocatalysis, an Energy Frontier Research Center funded by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences.
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.
Equilibrium, dynamic, and trapping properties of an excess electron in dense helium
NASA Astrophysics Data System (ADS)
Sheu, Sheh-Yi; Cukier, R. I.
1991-06-01
The equilibrium, dynamic, and trapping properties of an excess electron in dense helium are simulated. An adiabatic simulation method is used whereby the Schrödinger equation for the electron in the presence of a fixed, classical solvent configuration is solved. The solvent configuration is advanced by molecular dynamics with the force on a particular helium atom arising from the classical helium-helium potential and the expectation value of the electron-helium potential. The equilibrium properties of the electron are contrasted with those obtained by Coker and Berne [D. F. Coker and B. F. Berne, J. Chem. Phys. 89, 2128 (1988)] using a different procedure for generating helium configurations. The diffusion coefficient of the electron is obtained and, for ρ*=ρσ 3=0.9, is De=5.0×10-3 cm2 s-1. This is an order of magnitude greater than the diffusion coefficient of the helium atoms and corresponds to a very mobile electron. The distribution of times for an electron to move between donor and acceptor sites inserted in the system is obtained and shown to yield an average diffusion coefficient consistent with that obtained from the mean square displacement. The ability of the electron to move between the donor and acceptor sites by electron transfer is assessed by evaluating the reorganization energy of the solvent and using conventional electron transfer theory. If the sites are sufficiently far apart, then electron transport via detrapping from the donor site followed by transport to the acceptor site can be competitive with electron transfer as a charge transport mechanism.
NASA Astrophysics Data System (ADS)
Dietl, Tomasz
2015-03-01
A physically transparent and mathematically simple semiclassical model is employed to examine dynamics in the central-spin problem. The results reproduce previous findings obtained by various quantum approaches and, at the same time, provide information on the electron spin dynamics and Berry's phase effects over a wider range of experimentally relevant parameters than available previously. This development is relevant to dynamics of bound magnetic polarons and spin dephasing of an electron trapped by an impurity or a quantum dot, and coupled by a contact interaction to neighboring localized magnetic impurities or nuclear spins. Furthermore, it substantiates the applicability of semiclassical models to simulate dynamic properties of spintronic nanostructures with a mesoscopic number of spins.
Verlet-like algorithms for Car-Parrinello molecular dynamics with unequal electronic occupations.
Castañeda Medina, Arcesio; Schmid, Rochus
2017-09-21
The ab initio molecular dynamics simulations of metallic, charged, and electrochemical systems require, in principle, the inclusion of unequally occupied electronic states. In this contribution, the general approach to work with fixed but arbitrary occupations within the Car-Parrinello molecular dynamics scheme is revisited, focusing on the procedure which is required to maintain the orthonormality constraints in the commonly used position-Verlet integrator. Expressions to constrain also the orbital velocities, as it is demanded by a velocity-Verlet integrator, are then derived. The generalized unequal-occupation SHAKE algorithm is compared with the standard procedure for damped dynamics (energy optimization) of systems including fully unoccupied electronic states. In turn, the proposed unequal-occupation RATTLE algorithm is validated by the corresponding microcanonical ensemble simulations. It is shown that only with the proper orthogonalization method, a correct ordering of states and energy conserving dynamics can be achieved.
Nonlinear dynamics and bifurcation mechanisms in intense electron beam with virtual cathode
NASA Astrophysics Data System (ADS)
Frolov, Nikita S.; Kurkin, Semen A.; Koronovskii, Alexey A.; Hramov, Alexander E.
2017-07-01
In this paper we report on the results of investigations of nonlinear dynamics and bifurcation mechanisms in intense electron beam with virtual cathode in micrometer-scaled source of sub-THz electromagnetic radiation. The numerical analysis is provided by means of 3D electromagnetic particle-in-cell (PIC) simulation. We have studied evolution of the system dynamics with the change of beam current value by means of Fourier and bifurcation analysis. The bifurcation diagram has identified a number of the alternating regions of beam current with regular or chaotic regimes of system dynamics. The study of spatiotemporal dynamics of formed electron structures in the beam has revealed the physical mechanisms responsible for the regimes switchings in the system.
Impact of two-electron dynamics and correlations on high-order-harmonic generation in He
NASA Astrophysics Data System (ADS)
Artemyev, Anton N.; Cederbaum, Lorenz S.; Demekhin, Philipp V.
2017-03-01
The interaction of a helium atom with an intense, short, 800-nm, laser pulse is studied theoretically beyond the single-active-electron approximation. For this purpose, the time-dependent Schrödinger equation for a two-electron wave packet driven by a linearly polarized infrared pulse is solved by the time-dependent restricted-active-space configuration-interaction method in the dipole velocity gauge. By systematically extending the space of active configurations, we investigate the role of the collective two-electron dynamics in the strong-field ionization and high-order-harmonic generation processes. Our numerical results demonstrate that allowing both electrons in He to be dynamically active results in a considerable extension of the computed high-order-harmonic generation spectrum.
Simulations of one- and two-electron systems by Bead-Fourier path integral molecular dynamics
NASA Astrophysics Data System (ADS)
Ivanov, Sergei D.; Lyubartsev, Alexander P.
2005-07-01
The Bead-Fourier path integral molecular dynamics technique introduced earlier [S. D. Ivanov, A. P. Lyubartsev, and A. Laaksonen, Phys. Rev. E 67 066710 (2003)] is applied for simulation of electrons in the simplest molecules: molecular hydrogen, helium atom, and their ions. Special attention is paid to the correct description of electrons in the core region of a nucleus. In an attempt to smooth the Coulomb potential at small distances, a recipe is suggested. The simulation results are in excellent agreement with the analytical solution for the "harmonic helium atom", as well as with the vibrational potential of the H2 molecule and He ionization energies. It is demonstrated, that the Bead-Fourier path integral molecular dynamics technique is able to provide the accuracy required for the description of electron structure and chemical bonds in cases when electron exchange effects need not be taken into account.